Capillary-based electrosynthesis or electrical energy gas-liquid cells

Abstract

An electrosynthesis or electric energy battery and method of operation are disclosed, which includes a first gas diffusion electrode configured to generate a first gas and contact and be adjacent to a first gas containing the first gas, and a second gas diffusion electrode configured to generate a second gas and contact and be adjacent to a second gas containing the second gas. A porous capillary spacer is positioned between the first gas diffusion electrode and the second gas diffusion electrode. The porous capillary spacer is filled with a liquid electrolyte and configured to confine the liquid electrolyte to the porous capillary spacer by capillary effect, such that the liquid electrolyte has a maximum column height of greater than 0.4 cm.

Description

[Technical Field]

[0001] The present invention broadly relates to, for example, electrosynthesis cell or electrical energy cell Used as an electrochemical cell More particularly, example embodiments of the present invention are inherently energy efficient and employ molecular-level capillary, diffusion, and / or osmotic effects to achieve electrochemical cell Zero-gap electrochemistry minimizes the need for external macro-level control cell Regarding structure. [Background technology]

[0002] Electrical Energy cell means uninterrupted or continuous for an infinite period of time, cell Electrochemical to generate electricity for use outside the cell Electrical energy cell is galvanic in that it may be necessary to provide a constant external supply of reactants during operation. cell The products of electrochemical reactions are also generally cell Unlike batteries, electrical energy is constantly removed from cell does not store chemical or electrical energy internally.

[0003] Electrosynthesis cell Similarly, uninterrupted or continuous for an infinite period of time, cell Electrochemicals that produce one or more chemicals that are used outside the cell Chemicals can be in gas, liquid, or solid form. Electrical energy cell As in, electrosynthesis cell Electrosynthesis also requires a constant supply of reactants and a constant removal of products during operation. cell generally also require a constant input of electrical energy.

[0004] Electrical Energy cell or electrosynthesis cellDue to the large amount of electrical energy involved in their operation, a major issue in their development is making them as energy efficient as possible during operation. This can be achieved in part by minimizing electrical impedance. Impedance is the ratio of a voltage applied to a current. cell The resistance presented by a circuit. One way to minimize impedance is to cell The anode and cathode electrodes are positioned as close as possible to each other, facing each other, without contact (contact would cause a short circuit). cell The gap between the two electrodes should also be occupied by an electrolyte with the highest possible ionic conductivity.

[0005] For this purpose, electrosynthesis or electrical energy cell Various "zero gap" cell Structures have been developed in which two electrodes are tightly sandwiched against either side of a thin membrane that may have intrinsic high ionic conductivity or may be saturated with a liquid electrolyte that has high ionic conductivity. This type of zero-gap membrane is generally called a zero-gap cell The thickness is less than 2 mm. cell Some example structures are provided in R. Phillips and CW Dunnill, "Zero gap alkaline electrolysis cell design for renewable energy storage as hydrogen gas," RSC Advances (2016), Vol. 6, pp. 100643-100651.

[0006] Electrosynthesis or Electrical Energy cell Another characteristic of such reactors is the large amount of reactants and products that are typically involved in their operation. cell can always be supplied with a substantial amount of reactants, while at the same time a substantial amount of product is cell Ideally, reactant feed and product removal should be completely separate processes, so that cell reactants independently of the products being removed from cell and these processes do not interfere with each other. cell Supply of reactants to cell Removal of the product from the electrochemical reaction should not interfere with or limit the electrochemical reaction.

[0007] For example, the most well-known zero-gap cell One of them is hydrogen-oxygen polymer electrolyte membrane (PEM) fuel. cell Such cell is typically a thin proton (H) membrane formed of a sulfonated tetrafluoroethylene-based fluorinated polymer-copolymer, such as a Nafion® membrane supplied by Chemours, sandwiched between two gas-porous electrodes (also known as "gas diffusion electrodes"). + ) conductive membranes are employed. Nafion® membranes can typically be about 0.183 mm thick (e.g., when using a Nafion® 117 membrane) or about 0.125 mm thick (e.g., when using a Nafion® 115 membrane). cell In a catalytic converter, reactant hydrogen (H2) gas is introduced through one of the gas diffusion electrodes ("hydrogen electrode") and converted to protons at the gas diffusion electrode. The protons are transported through a Nafion® membrane to the other electrode ("oxygen electrode"). Oxygen (O2) gas is introduced through the gas diffusion "oxygen" electrode and reacts with the protons that have permeated the Nafion® membrane to produce water (H2O). The water formed at the oxygen electrode typically evaporates by gravity or evaporation. cell is removed from cell The electrochemical reaction at the electrode generates a current or voltage in an attached external circuit.

[0008] this cell The key to its operation is the transfer of protons (H +The ability of the Nafion® membrane to facilitate oxygen conduction is key. To perform this function, the Nafion® membrane must be partially or fully saturated (i.e., hydrated) with water. However, maintaining the required hydration level can be difficult because water is also a product of the reaction produced at the oxygen electrode. Most commonly, PEM fuels cell The hydration level of the Nafion® membrane in a FCFC is managed by humidifying the input (reactant) hydrogen gas. This must be carefully controlled, as excessive moisture can condense into water and accumulate at one of the gas diffusion electrodes, blocking the input gas and terminating the reaction. This phenomenon, known as "flooding," is particularly dangerous at the oxygen electrode, where the reaction product, water, is also formed. However, insufficient humidification can lead to partial drying of the Nafion® membrane, reducing proton conductivity and slowing the reaction. This is particularly dangerous at the hydrogen electrode, because during operation, electrophoretic drift causes water molecules to leave the hydrogen electrode and migrate across the Nafion® membrane to the oxygen electrode. Therefore, the process of providing the reactant (hydrogen) is intimately connected to the process of removing the product (water), making this type of fuel difficult to handle. cell In many cases, active management is required, involving modification of the humidity content of the input gas by a responsive, monitored, real-time electronic feedback system.

[0009] Much electrical energy or electrical synthesis cell requires some form of control, including active control, during operation because the processes involved in the supply of reactants are closely related to and not independent of the product removal processes. cellThis arises because the molecular-level processes that deliver reactants to and / or remove products from the active sites of the electrochemical reaction are not separate and independent within the electrode itself. Moreover, they are not controlled by the electrochemical reaction. Therefore, this molecular-level deficiency must be addressed by macroscale management of indirect, surrogate control processes that (i) deliver reactants to the electrodes and / or (ii) remove products from the electrodes, and / or (iii) control critical intermediates or critical processes between the electrodes.

[0010] This problem can be stated more conceptually to clarify the issue: essentially all zero-gap electrical energy or electrical synthesis cell Within the membrane, reactions and molecular transport occur at the molecular level, under the control of electrochemical reactions, largely in the "cross-plane" axis at the electrodes and between the electrodes within the interelectrode membrane. Reactants must generally migrate from the exterior of the membrane to this cross-plane axis, a process that may not be under the control of the electrochemical reaction. Similarly, the products of the electrochemical reaction must typically migrate from the cross-plane axis, a process that may not be under the control of the electrochemical reaction. The same is true for all other critical processes and the specific materials involved. As the degree of control over the execution of these processes decreases, cell Within the electrochemical reaction system itself, there can be a molecular-level decoupling between reactant supply / product removal to / from the reaction site and the rate of the electrochemical reaction itself. It is this molecular-scale decoupling that generally necessitates challenging external macro-scale control, including active control. That is, the need for control is due to the interaction between the electrochemical reaction and cell This can arise from the disconnect between the bulk of the material that must be fed to or removed from the electrochemical reaction within itself. If all such transport were better controlled, this would cell The need to manage cell This may eliminate the need to actively manage Summary of the Invention [Problem to be solved by the invention]

[0011] Some electrosynthesis or electrical energy zero gaps involve gas-to-liquid or liquid-to-gas conversions cell The problem is the molecular level migration of liquid phase material towards or away from the intersecting plane axis. For example, as mentioned above, zero gap PEM fuel cell In the case of ZnO, water migration in / out of the intersecting planar axis can interfere with gas-phase reactant access to the electrodes, thereby requiring active management. cell So, it is the molecular-level movement of the base material into or out of the intersecting planar axes that can be problematic and require active management. For example, zero-gap water electrolysis cell The gas bubbles generated in often have to be actively swept away from the electrodes by constantly pumping liquid electrolyte over the electrodes to provide access to the electrode surface for the water reactant. cell Not only does this increase the cost of the system (due to additional piping, tanks, and other equipment, including pressure management equipment), it also increases the "crossover" of gas from one electrode to the other, thereby cell The electrochemical efficiency of the device would be significantly reduced, potentially posing a safety issue.

[0012] Such cell So, the question is, what is the electrochemical mechanism where a chemical species with one phase of matter (e.g., a liquid) flows in a direction and place that opposes and counteracts the flow of another chemical species with a different phase of matter (e.g., a gas)? cell This can be summarized as involving internal molecular-level flows. This type of flow can be called "multiphase counterflow." In interfering with and hindering each other, such multiphase counterflows: cell This can reduce the performance of the system and create inefficiencies that require energy to overcome.

[0013] Electrosynthesis or Electrical Energy cell The existence of such multiphase backflow in water electrolysis is well known. However, in many cases, eliminating or minimizing multiphase backflow is not straightforward, as there are other important considerations that must be addressed. For example, as mentioned above, cellIn a conventional electrocatalyst, the flow of liquid-phase reactants (e.g., water molecules and ions) toward the electrodes resists the flow of gas-phase products (e.g., gas bubbles) away from the electrodes. This resistance is often amplified by the inter-electrode membrane. The primary function of the inter-electrode membrane is to prevent gas crossover between the electrodes. For this reason, the inter-electrode membrane is typically non-porous and must have a Nafion® 115 membrane thickness of 0.125 mm or greater. If the inter-electrode membrane is fully porous, the pores must be as small as possible to prevent gas bubbles from entering and passing through the inter-electrode membrane. Such properties are not suitable for the continuous supply of large amounts of liquid-phase reactants, such as water molecules. In fact, these properties of known inter-electrode membranes can impede, minimize, or even prevent the mobility of liquid-phase water within the inter-electrode membrane. This is necessary to minimize gas crossover through the membrane. [Means for solving the problem]

[0014] In summary, e.g., electrosynthesis cell or electrical energy cell New and improved electrochemistry used as cell or zero-gap electrochemistry cell Alternatively or additionally, new and improved zero-gap electrical energy cell and / or electrosynthesis cell Alternatively or additionally, in instances where management may be required, zero-gap electrical energy cell and / or electrosynthesis cell There is also a need for new and improved means of managing the operation of electrical energy. cell and electrosynthesis cell New and improved electrochemical methods for promoting gas-to-liquid and liquid-to-gas conversion cell or zero-gap electrochemistry cell is particularly needed.

[0015] Reference herein to any prior publication (or information derived therefrom) or any known matter is not, and should not be construed as, an acknowledgment, admission, or any form of suggestion that the prior publication (or information derived therefrom) or known matter forms part of the common general knowledge in the field of endeavor to which this specification pertains.

[0016] This Summary is provided to introduce a selection of concepts in a simplified form that are further described below in the Detailed Description. This Summary is not intended to identify all key or essential features of the claimed subject matter, nor is it intended to be used to limit the scope of the claimed subject matter.

[0017] In various example aspects, embodiments may utilize molecular-level capillary action, diffusion, and / or osmosis. cell We hire internally, cell Electrochemistry with minimal need for macro-level external control cell Structure, especially zero-gap electrochemistry cell Preferably, these molecular level processes are essentially cell Preferably, these molecular-level processes are cell are separate and independent for the various liquid and gas phase reactants and / or products. Preferably, each such molecular-level process includes: cell Preferably, the fresh reactants or excess products are cell During operation, the liquid and gas are separately supplied to or removed from the liquid and gas. Preferably, this supply or removal is cell Each liquid or gas within the chamber is separately linked to an external storage and supply / removal system via an airtight / liquid-tight conduit.

[0018] Example embodiments are particularly directed to zero-gap electrosynthesis or electrical energy facilitating gas-to-liquid or liquid-to-gas processes. cell Regarding such celloperates uninterruptedly or continuously for an indefinite period of time, consuming reactants; cell It may produce a product that is too bulky to be contained within and instead may be supplied or removed by an external storage and supply / removal system. Preferably, the example embodiment is inherently energy efficient.

[0019] In one embodiment, an electrosynthesis or electrical energy converter is provided that includes a first gas diffusion electrode, a second electrode, and a porous capillary spacer positioned between the first gas diffusion electrode and the second electrode. cell Preferably, the porous capillary spacer is capable of filling itself with liquid electrolyte when an end of the porous capillary spacer is in liquid contact with the liquid electrolyte in the reservoir. Preferably, the first gas diffusion electrode is located outside the reservoir. Preferably, the second electrode is also located outside the reservoir. Optionally, cell Electrosynthetic water electrolysis cell is.

[0020] In one embodiment, the first gas diffusion electrode is in direct contact with the first gas. In another embodiment, the porous capillary spacer is filled with a liquid electrolyte. In another embodiment, the porous capillary spacer has an average pore size of more than 2 μm. In another embodiment, the first gas diffusion electrode is in contact with and adjacent to the first gas. In another embodiment, the second electrode is a second gas diffusion electrode that is in contact with and adjacent to the second gas.

[0021] In another embodiment, electrosynthesis or electrical energy cell a reservoir for containing a liquid electrolyte; a first gas diffusion electrode located outside the reservoir; a second electrode located outside the reservoir; and a porous capillary spacer located between the first gas diffusion electrode and the second electrode, the porous capillary spacer having an end extending into the reservoir, the porous capillary spacer being capable of filling itself with the liquid electrolyte when the end of the porous capillary spacer is in liquid contact with the liquid electrolyte in the reservoir. cell is provided.

[0022] In another embodiment, electrosynthetic water electrolysis cell an electrosynthetic water electrolysis device comprising: a first gas diffusion electrode configured to generate a first gas and to be in direct contact with a first gas containing the first gas; a second electrode; and a porous capillary spacer filled with a liquid electrolyte and configured to be positioned between the first gas diffusion electrode and the second electrode, wherein the porous capillary spacer has an average pore size of greater than 2 μm. cell is provided.

[0023] In another embodiment, electrosynthesis or electrical energy cell a first gas diffusion electrode configured to generate a first gas and to be in contact with and adjacent to a first gas comprising the first gas; a second gas diffusion electrode configured to generate a second gas and to be in contact with and adjacent to a second gas comprising the second gas; and a porous capillary spacer located between the first gas diffusion electrode and the second gas diffusion electrode, wherein the porous capillary spacer is filled with a liquid electrolyte and configured to confine the liquid electrolyte in the porous capillary spacer by capillary effect, whereby the liquid electrolyte has a maximum column height of greater than 0.4 cm. cell is provided.

[0024] In another embodiment, electrosynthesis or electrical energy cell A laminate of the first electrosynthesis or electrical energy cell and a first electrosynthesis or electrical energy cell a second electrosynthetic or electrical energy source electrically connected to the cell and each electrosynthesis or electric energy cell is disclosed herein cell A laminate is provided, which is an example of the above.

[0025] In another embodiment, electrosynthesis or electrical energy for carrying out electrochemical reactions cell A method of operation of cell is disclosed herein cellIn one example of a method, the method includes applying or generating a voltage between a first gas diffusion electrode and a second electrode.

[0026] In another embodiment, electrosynthesis or electrical energy for carrying out electrochemical reactions cell A method of operating the stack of the present invention is provided, comprising electrosynthesizing or electrical energy cell The laminate of the present invention can be electrosynthesized or electrochemically cell The method is an example of a laminate of cell Applying a voltage between the first gas diffusion electrode and the second electrode in each stack of the cell generating a voltage between the first gas diffusion electrode and the second electrode in each stack of the stack.

[0027] In another embodiment, electrosynthesis or electrical energy for carrying out electrochemical reactions cell A method of operation is provided for electrosynthesis or electrical energy cell The present invention provides a method for a battery comprising a vessel containing a liquid electrolyte, a first gas diffusion electrode, a second electrode, and a porous capillary spacer positioned between the first gas diffusion electrode and the second electrode, the porous capillary spacer being positioned within the vessel and having an end in liquid contact with the liquid electrolyte. The method includes contacting the first gas diffusion electrode and the second electrode with the liquid electrolyte, and applying or generating a voltage between the first gas diffusion electrode and the second electrode.

[0028] Illustrative embodiments will now be described, by way of non-limiting example, with reference to the accompanying drawings, in which: Various example embodiments will become apparent from the following description, given by way of example only, of at least one preferred but non-limiting embodiment, which is illustrated in connection with the accompanying drawings, in which: [Brief explanation of the drawings]

[0029] [Figure 1]1 shows in schematic form a cross-sectional view of an electrosynthesis or electrical energy cell having a separate liquid reservoir that is not in direct contact with either electrode. [Figure 2] 1 shows a schematic cross-sectional view of an example of an electrosynthesis or electrical energy cell in which the liquid in the reservoir is in direct contact with at least one electrode. [Figure 3] 1 shows a schematic cross-sectional view of an example of an electrosynthesis or electrical energy cell in which the reservoir is integrated into a porous capillary spacer. [Figure 4] 1 shows in schematic form an enlarged cross-sectional view of a central portion of an electrode-spacer-electrode assembly of an example electrosynthesis or electrical energy cell. [Figure 5] Graphs of measured (black dots) and modeled (hollow squares) flow rates for porous capillary spacers composed of polyethersulfone material filters with average pore sizes of (a) 0.45 μm, (b) 1.2 μm, (c) 5 μm, and (d) 8 μm filled with 6 M KOH liquid electrolyte are shown. [Figure 6] 10 shows an alternative example of a tank configuration. [Figure 7] 1 shows an electrode-spacer-electrode assembly that can be used to implement an example electrosynthesis or electrical energy cell. [Figure 8] An example of an electrosynthesis or electrical energy cell incorporating an electrode-spacer-electrode assembly of the type shown in FIG. 7 is shown. [Figure 9] FIG. 8 shows an example of an electrosynthesis or electrical energy cell stack and a possible cell configuration that can be used. [Figure 10] FIG. 8 shows an example of an electrosynthesis or electrical energy cell stack and a possible cell configuration using four impregnation chambers in a cell stack of four individual cells. [Figure 11]1 shows polarization curves at 80°C for (a) an example embodiment of a water electrolysis cell having the structure of FIG. 1 in which a gas-handling structure is incorporated into the oxygen-generating electrode; (b) an example embodiment of a water electrolysis cell similar to (a) above, but without a gas-handling structure incorporated into the oxygen-generating electrode; (c) an equivalent water electrolysis cell using the same electrodes and porous capillary spacers as (a) and (b), but where the cell is completely filled with liquid electrolyte and gas is generated in the form of bubbles in the liquid electrolyte; (d) the most energy-efficient commercially available alkaline water electrolysis cell for which data is published; and (d) the most energy-efficient commercially available PEM water electrolysis cell for which data is published. [Figure 12] The polarization curve (a) shows the current produced by the cell of Figure 11 when the cell voltage is fixed at 1.47 V at 80°C, which is equivalent to 100% energy efficiency due to the higher heating value (HHV) of hydrogen. [Figure 13] (a) Potential of the oxygen electrode in Figure 11 at polarization curve (a) and (b) equivalent potential of an oxygen electrode coated with a thin hydrophilic layer of the same catalyst, which promotes capillary-induced migration of a thin film of 6 M KOH liquid electrolyte along the surface of the electrode to the surface of the electrode. [Figure 14] 1 shows a schematic cross-sectional view of a further example of a gas-free electrosynthesis or electrical energy cell. [Figure 15] 1 shows a schematic cross-sectional view of a further example of an electrosynthesis or electrical energy cell in which the liquid electrolyte is replenished / maintained via a non-interfering vapor phase pathway via a gas. [Figure 16] 1 shows a schematic cross-sectional view of a further example of an electrosynthesis or electrical energy cell in which the headspace above one electrode is occupied by a liquid electrolyte and the headspace above the other electrode is occupied by a gas. [Figure 17] FIG. 1 shows a schematic cross-sectional view of a further example of an electrosynthesis or electrical energy cell in which the headspace above one electrode and above the other electrode is occupied by gas. [Figure 18] 1 shows a schematic cross-sectional view of a further example of an electrosynthesis or electrical energy cell in which the liquid electrolyte is replenished / maintained via a non-interfering vapor phase pathway via a gas. [Figure 19]FIG. 1 shows a schematic cross-sectional view of a further example of an electrosynthesis or electrical energy cell in which a liquid electrolyte held in a porous capillary spacer prevents gas crossover between gases. [Figure 20] FIG. 1 shows a schematic cross-sectional view of a further example of an electrosynthesis or electrical energy cell in which one electrode is in contact with a first gas only above the electrode (in the headspace) and the other electrode is in contact with a second gas only above the electrode (in the headspace). [Figure 21] FIG. 1 shows a schematic cross-sectional view of a further example of an electrosynthesis or electrical energy cell in which a liquid electrolyte held in a porous capillary spacer prevents gas crossover between a first gas and a second gas, one electrode contacts the first gas only at the top of the electrode (in the headspace), and the other electrode incorporates a gas handling structure filled with a gas (collectively forming the second gas) in contiguous with the headspace. [Figure 22] FIG. 1 shows a schematic cross-sectional view of a further example of an electrosynthesis or electrical energy cell incorporating a ring structure of gas-hands filled with a first electrode (collectively forming a first gas) in continuity with the headspace. [Figure 23] FIG. 1 shows a schematic cross-sectional view of a further example of an electrosynthesis or electrical energy cell in which one electrode is in contact with a first gas only at the top of the electrode (in the headspace), and the other electrode is adjacent to a gas capillary structure filled with a gas (collectively forming a second gas) that is continuous with the headspace. [Figure 24] 1 shows a schematic cross-sectional view of a further example of an electrosynthesis or electrical energy cell in which one electrode is adjacent to a gas capillary structure filled with a gas (collectively forming a first gas) in continuity with the headspace, and the other electrode is adjacent to another gas capillary structure filled with a gas (collectively forming a second gas) in continuity with the headspace. [Figure 25] FIG. 1 shows a schematic cross-sectional view of a further example of an electrosynthesis or electrical energy cell in which one electrode has an attached or incorporated gas capillary or gas handling structure that extends through the liquid electrolyte above the electrode into the headspace. [Figure 26]FIG. 1 shows a schematic cross-sectional view of a further example of an electrosynthesis or electrical energy cell in which the gas capillary or gas handling structure is filled with a gas (collectively forming a first gas) that is continuous with the headspace gas, and the other electrode is in contact with a second gas only at the top (in the headspace). [Figure 27] The other electrode also shows a schematic cross-sectional view of a further example of an electrosynthesis or electrical energy cell having an attached or incorporated gas capillary or gas handling structure that extends through the liquid electrolyte above the other electrode into the headspace, the gas capillary or gas handling structure being filled with a gas (collectively forming a second gas) that is continuous with the headspace gas. [Figure 28] 1 shows a schematic cross-sectional view of a further example of an electrosynthesis or electrical energy cell in which one electrode has an attached or incorporated gas capillary or gas handling structure that releases bubble / gas volume through the liquid electrolyte, and the other electrode has an attached or incorporated gas capillary or gas handling structure that releases bubble gas volume through the liquid electrolyte. [Figure 29] 1 shows a schematic cross-sectional view of a further example of an electrosynthesis or electrical energy cell in which one electrode has an attached or incorporated gas capillary or gas handling structure that releases bubble / gas volume through the liquid electrolyte, and the other electrode has an attached or incorporated gas capillary or gas handling structure that releases bubble gas volume through the liquid electrolyte. [Figure 30] 1 shows a schematic cross-sectional view of a further example of an electrosynthesis or electrical energy cell in which a first gas is in gaseous communication with a body conduit and an external gas storage system, and a second gas is in gaseous communication with an external conduit and an external gas storage system. [Figure 31] Figure 1 shows a schematic cross-sectional view of a further example of an electrosynthesis or electrical energy cell in which a gas capillary or gas handling structure receives a volume of gas bubbles / gas from an external gas conduit along a first path through a liquid electrolyte, and another gas capillary or gas handling structure receives a volume of gas bubbles / gas from an external gas conduit along a second path through a liquid electrolyte. [Figure 32] Figure 1 shows a schematic cross-sectional view of a further example of an electrosynthesis or electrical energy cell in which a gas capillary or gas handling structure receives a volume of gas bubbles / gas from an external gas conduit along a first path through a liquid electrolyte, and another gas capillary or gas handling structure receives a volume of gas bubbles / gas from an external gas conduit along a second path through a liquid electrolyte. [Figure 33] 1 shows a schematic cross-sectional view of a further example of an electrosynthesis or electrical energy cell in which one electrode has an attached or incorporated gas capillary or gas handling structure containing a first gas 125 therein in gaseous communication with an external conduit and an external gas storage system, and the other electrode has an attached or incorporated gas capillary or gas handling structure containing a second gas therein in gaseous communication with an external conduit and an external gas storage system. [Figure 34] FIG. 1 shows a schematic cross-sectional view of a further example of an electrosynthesis or electrical energy cell in which electrode gas generation dynamically generates gases associated with each electrode, each gas being in separate gas communication with an external conduit and external gas storage system. [Figure 35] 1 shows a schematic cross-sectional view of a further example of an electrosynthesis or electrical energy cell exhibiting one or more of a set of physical attributes characteristic of an "independent pathway cell." DETAILED DESCRIPTION OF THE INVENTION

[0030] To provide a more thorough understanding of the spirit of the preferred embodiment or embodiments, the following aspects, features, or aspects are described, given by way of example only.

[0031] definition A "reservoir" is a portion of a device in which a liquid is held. A "reactant" is a chemical consumed during an electrochemical reaction. A "product" is a chemical produced during an electrochemical reaction. A "liquid electrolyte" is a liquid containing ions in solution capable of conducting electricity. A "conduit" is a channel, tube, chamber, or trough for conveying a fluid. A "manifold" is one or more pipes with multiple openings, one or more tubes, one or more chambers, or one or more channels for conveying a fluid. "Room temperature" is defined as 21°C.

[0032] "Liquid-Gas" cell refers to an electrochemical reaction having at least one liquid phase reactant or product and at least one gas phase reactant or product. cell is defined as:

[0033] "Electric energy cell " means, cell Electrochemical power generation that produces electricity uninterruptedly or continuously for an indefinite period of time for outdoor use cell Electrical energy cell During operation, the products of the electrochemical reaction may also require an external supply of reactants. cell Electrical energy can always be removed from cell is liquid-gas cell Electrical energy cell An example of a hydrogen-oxygen fuel is cell This example is also a liquid-gas cell is.

[0034] "Electrosynthesis" cell What is that? cell Electrochemical processes that produce one or more chemicals continuously or uninterruptedly for an indefinite period of time for outdoor use cell The chemicals can be in gas, liquid, or solid form. Electrical energy cell As in, in operation, electrosynthesis cell However, it may be necessary to constantly supply reactants and remove products. cellGenerally, they may also require a constant input of electrical energy during operation. cell is liquid-gas cell Electrosynthesis cell An example of this is water electrolysis. cell This example is also a liquid-gas cell is.

[0035] Electrical Energy cell and electrosynthesis cell contains all / some of the reactants needed to operate and all / some of the products produced during operation. cell It is not built into the device itself, unlike other types of electrochemical devices such as batteries and sensors. cell Instead, they are always cell carried into, or cell For example, electrical energy can be removed cell is Galvanic cell are the reactants and products cell Galvanic in that it is stored within the body cell Unlike batteries, they are cell Similarly, some electrochemical sensors consume reactants and generate products in limited amounts during sensing operation, but some / all of these cell It is stored within the body itself.

[0036] "Zero-gap" electrochemistry cell means that there is no gap between the electrode and the inter-electrode spacer. cell That is, "zero gap" cell In the interelectrode spacer, the electrodes are closely spaced on both sides of the interelectrode spacer or abut on both sides.

[0037] A "porous material" is a solid material that contains open space ("interstitial" space) that is not occupied by the main backbone of atoms or molecules that make up the structure of the solid.

[0038] The "porosity" of a porous material is defined as the ratio, expressed as a percentage, of the volume of the interstitial space divided by the total volume of the porous material.

[0039] "Capillaries" or "pores" are microscopic structures within a porous material through which liquids or gases can pass.

[0040] The "pore size" of a pore in a porous material is the ideal diameter of the pore.

[0041] The "average pore size" of the pores in a porous material is the idealized average diameter of the pores present in the porous material, routinely measured using a gas porometer.

[0042] "Capillary action" involves the drawing, retention, and induction of a liquid into a narrow space without or against the aid of an external force such as gravity. In drawings, liquids can be seen being drawn up and retained between the bristles of a paintbrush, in a thin tube, or in porous materials such as paper or plaster. Such capillary action is typically driven by intermolecular forces between the liquid and the surrounding solid surface. Within porous materials, capillary action occurs due to a combination of surface tension (created by cohesion within the liquid) and attractive forces between the liquid and the container wall. Once drawn up, a liquid can typically be retained indefinitely up to a height known as the maximum column height.

[0043] Capillary pressure is the external pressure that must be applied to totally oppose capillary action; that is, the pressure that, when applied to a liquid drawn up by capillary action, causes the liquid to return to the position it would occupy if capillary action did not occur. Capillary pressure can also be thought of as the pressure that causes such liquid to be held within the pores or capillaries of the material that exerts capillary action.

[0044] The "capillary pressure" of a porous material containing a liquid is defined as the gas pressure required to force the liquid out of a mean diameter capillary within the porous material, as measured using a gas porometer.

[0045] The "bubble point" of a porous material containing a liquid is defined as the gas pressure required to force the liquid out of the largest capillary in the porous material, as measured using a gas porometer.

[0046] A "porous capillary spacer" of example embodiments is a porous material that uses capillary action to draw liquid electrolyte into itself and maintain a column height of liquid electrolyte, which forms the column height and is trapped within the volume of the porous capillary spacer, exhibiting capillary pressure. It should be understood that a "porous capillary spacer" may alternatively be described as a "porous spacer," "porous electrode spacer," "porous capillary electrode spacer," "porous spacer with flow channels," "porous electrode spacer with flow channels," "porous capillary separator," "porous separator," "porous electrode separator," "porous capillary electrode separator," "porous separator with flow channels," or "porous electrode separator with flow channels."

[0047] "Column height" is the cell The term "height" is defined as the height of the column of liquid trapped within the porous capillary spacer by capillary action, including during operation of the porous capillary spacer. The term "height" is defined as the height above the surface of the liquid bath in which the porous capillary spacer is immersed. If the porous capillary spacer is not immersed in the liquid bath, it is defined as the height above the bottom (distal) end of the porous capillary spacer.

[0048] "Maximum column height" is defined as the maximum "height" of a column of liquid that can be maintained within a porous capillary spacer by capillary action if the porous capillary spacer itself were hypothetically of infinite height. The term "height" is defined as the height above the surface of the liquid bath in which the porous capillary spacer is immersed. If the porous capillary spacer is not immersed in the liquid bath, it is defined as the height above the bottom (distal) end of the porous capillary spacer.

[0049] The actual "column height" of the liquid in the porous capillary material is cell Note that the "column height" may be limited by the height of the porous capillary spacer that reaches the top of the column. That is, the "column height" may be less than the "maximum column height" if the porous capillary material itself has a height less than the "maximum column height." cell So, "Maximum column height" is cell This is because the porous capillary spacer cell It may be necessary to ensure that the liquid is completely filled at all points within the cavity, which may then be necessary to prevent gas crossover (see definition below for "gas crossover").

[0050] "Flow rate" is defined as the mass of liquid per unit time flowing through a 1 cm wide strip of porous capillary spacer fully saturated with liquid under the influence of capillaries alone. Due to gravity, "flow rate" typically decreases as the height of the porous capillary spacer increases. "Flow rate" at a particular "height" is defined as the flow rate at a height above the surface of the liquid bath in which the porous capillary spacer is immersed, measured using the technique employed to collect the measured data in Figure 5. If the porous capillary spacer is not immersed in the liquid bath, it is defined as the "flow rate" at a height above the bottom (distal) end of the porous capillary spacer.

[0051] "Diffusion" is the spontaneous net movement of liquid or gas phase molecules from a region of higher concentration to a region of lower concentration, with a tendency to equalize the concentrations in both regions.

[0052] "Osmosis" is the spontaneous movement of water molecules from a region of low solute concentration to a region of high solute concentration, typically under conditions where the solute itself is not as free to move in the opposite direction (e.g., when there is a membrane between the two regions that is impermeable or poorly permeable to the solute).

[0053] electrochemistry cellis "self-regulating" if the rate of reactant supply and / or product removal from the reaction zone at the electrode essentially adjusts itself according to or in response to the electrochemical reaction rate. That is, faster electrochemical reaction rates spontaneously lead to faster reactant supply and product removal, while slower electrochemical reaction rates lead to slower reactant supply to and product removal from the reaction zone.

[0054] The term "multiphase counterflow" refers to an electrochemical reaction in which a chemical species having one phase of matter (e.g., liquid) moves (flows) in a direction and place opposite to the movement (flow) of another chemical species having a different phase of matter (e.g., gas). cell This refers to internal molecular-level flows. In interfering with and hindering each other, such counteracting multiphase flows can create inefficiencies that require energy to overcome.

[0055] "Independent Path cell "teeth, cell a gas-liquid electrochemical system that provides at least one pathway that is separate and independent from the movement (flow) of each individual liquid-phase and gas-phase reactant and product within the system, and that does not interfere with or impede one another; cell is defined as:

[0056] "Electrode compression" or "electrode pressure" as used herein refers to the pressure that compresses two electrodes against either side of an intervening porous capillary spacer. Such compression is cell or cell by springs or washers on tie rods that compress the stack; or cell The delivery may be by a spring mounted within the

[0057] A "gas capillary structure" is a structure that employs the capillary effect to spontaneously draw gas from a liquid and exhibits a measurable capillary pressure associated with gas uptake. As used herein, the capillary pressure in a gas capillary structure is defined as "measurable" if repeated measurements and calculations reproducibly produce a capillary pressure of greater than 10 mbar.

[0058] A "gas handling structure" is a structure that has physical properties that facilitate the movement of gases without necessarily utilizing the gas capillary effect.

[0059] Gas diffusion layer and porous transport layer are terms sometimes used in other fields of electronics. It should be understood that "gas diffusion layers," "porous transport layers," and / or such type structures may be "gas capillary structures" if they spontaneously draw gas from a liquid and exhibit a measurable capillary pressure associated with gas uptake. They are "gas handling structures" if they do not spontaneously draw gas from a liquid or exhibit a measurable capillary pressure associated with gas uptake, but assist in gas movement / transport to or from the electrodes.

[0060] As used herein, an electrode is defined as "bubble-free" if, during operation, the formation of bubbles on at least a portion of its surface cannot be discerned using the human eye.

[0061] Electrosynthesis cell "Energy efficiency" of a chemical product, as used herein, refers to the ratio, expressed as a percentage, of the net energy present in a single unit of output of a chemical product to the amount of energy required to produce the same unit of output of that chemical product. cell is defined as the net energy consumed divided by the net energy consumed. cell The "energy efficiency" of a cell The energy generated by cell It is defined as the theoretical maximum energy that can be generated by

[0062] "Gas crossover" is the phenomenon in which a portion of a first gas on a first side of a porous capillary spacer containing a liquid electrolyte migrates through the porous capillary spacer to a second gas on the opposite side of the porous capillary spacer. "Benchmark gas crossover" is expressed as a percentage: cell is a constant 150mA / cm at room temperature and atmospheric pressure 2It is defined as the volume of a first gas present in a second gas divided by the volume of the second gas after 30 minutes under operating conditions.

[0063] Electrosynthesis or Electrical Energy of the Preferred Embodiments cell Has a separate layer that does not contact any of the electrodes cell Examples FIG. 1 illustrates the electrosynthesis or electrical energy of a preferred embodiment. cell The structure of 10 is shown schematically. cell 10 is zero-gap electrosynthesis or electrical energy cell Preferably, cell 10 comprises a reservoir 140 for containing a liquid electrolyte, a first gas diffusion electrode 120 located outside the reservoir, a second electrode 130 located outside the reservoir, and a porous capillary spacer 110 located between the first gas diffusion electrode 120 and the second electrode 130, the porous capillary spacer 110 having an end extending into the reservoir, the porous capillary spacer 110 being capable of filling itself with the liquid electrolyte 100 when the end of the porous capillary spacer 150 is in liquid contact with the liquid electrolyte 100 in the reservoir 140. The assembly of the first electrode 120, the porous capillary spacer 110, and the second electrode 130 is cell 10 "electrode-spacer-electrode" assemblies 139 are constructed.

[0064] The porous capillary spacer comprises a porous material capable of drawing liquid electrolyte into itself using capillary action and maintaining the liquid electrolyte at a column height, the liquid electrolyte forming the column height being trapped within the volume of the porous capillary spacer and exhibiting a capillary pressure. It will be understood that a "porous capillary spacer" may alternatively be described as a "porous spacer," "porous electrode spacer," "porous capillary electrode spacer," "porous spacer with flow channels," "porous electrode spacer with flow channels," "porous capillary separator," "porous separator," "porous electrode separator," "porous capillary electrode separator," "porous separator with flow channels," or "porous electrode separator with flow channels."

[0065] Preferably, the end of the porous capillary spacer is located in the reservoir. Preferably, a reservoir 140 is provided that contains or is capable of containing the liquid electrolyte 100, and an end 150, e.g., a distal end (or equivalently, an end portion or a distal end portion) of the electrolyte-filled porous capillary spacer 110 is located in the reservoir 140, which may contain the liquid electrolyte 100, i.e., is immersed in the reservoir 140. Preferably, the reservoir is configured to be filled with the liquid electrolyte, and the end of the porous capillary spacer is configured to be in contact with the liquid electrolyte. Preferably, the porous capillary spacer draws the liquid electrolyte into the porous capillary spacer by capillary action and maintains a column height of the liquid electrolyte. Preferably, the maximum column height of the liquid electrolyte is at least equal to or greater than the height of the first gas diffusion electrode. Preferably, the porous capillary spacer is configured to transport the liquid electrolyte along the porous capillary spacer by at least capillary action. Preferably, cell is configured to include filling the porous capillary spacer with liquid electrolyte from a reservoir by at least capillary action. cell The method is configured to include filling the porous capillary spacer with liquid electrolyte before the end of the porous capillary spacer is positioned within the reservoir.

[0066] Preferably, cell 10 may be configured such that the first gas diffusion electrode 120 is separated from the liquid electrolyte 100 in the reservoir 140 when the reservoir 140 contains a liquid electrolyte. cell The porous capillary spacer 110 may be further configured such that, when the reservoir 140 contains the liquid electrolyte 100, the second electrode 130 is separated from the liquid electrolyte 100 in the reservoir 140. Preferably, the first gas diffusion electrode 120 and the second electrode 130 are spaced apart from the reservoir 140. That is, preferably, the liquid electrolyte 100 contained in the reservoir 140 may not be in direct contact with either the first electrode 120 or the second electrode 130. Preferably, the direct contact area between the porous capillary spacer 110 and the first gas diffusion electrode 120 is outside the reservoir 140, and the direct contact area between the porous capillary spacer 110 and the second electrode 130 is outside the reservoir 140. Preferably, cell The method includes contacting a first gas diffusion electrode and a second electrode with a liquid electrolyte after the liquid electrolyte has been transported along a porous capillary spacer.

[0067] Optionally, but preferably, the end 150 of the porous capillary spacer 110 extends beyond the first electrode 120 and the second electrode 130. In this example, the end 150 of the porous capillary spacer 110 may extend along its length beyond the end of the first electrode 120 (e.g., the distal end of the first electrode 120) and the end of the second electrode 130 (e.g., the distal end of the second electrode 130), such that the end 150 of the porous capillary spacer 110 extends into the liquid electrolyte 100 in the reservoir 140. The reservoir 140 can be a body cavity, chamber, tank, housing, pipe, conduit, etc. suitable for containing the liquid electrolyte 100. One or more reservoirs can be used, and in one example, one or more reservoirs can supply liquid electrolyte to the same porous capillary spacer.

[0068] Preferably, the porous capillary spacer has a plurality of pores that provide flow paths between the first gas diffusion electrode, the second electrode, and the reservoir. Preferably, the porous capillary spacer is fluidly connected to the reservoir. Preferably, during operation, the porous capillary spacer remains filled with liquid electrolyte.

[0069] Optionally, the porous capillary spacer 110 is filled with the liquid electrolyte 100 before the end 150 of the porous capillary spacer 110 extends into the reservoir 140. Preferably, cell is configured to contact the first gas diffusion electrode 120 and the second electrode 130 only after first being transported along the porous capillary spacer 110 from the reservoir 140 during operation. cellis configured such that during operation, a surface area covered by the liquid electrolyte in the porous capillary spacer is at least equal to or greater than a surface area of ​​the first gas diffusion electrode facing the porous capillary spacer. Preferably, the first gas diffusion electrode is configured to generate a first gas forming a first gas, with a first side of the porous capillary spacer adjacent to a first side of the first gas diffusion electrode, a second side of the porous capillary spacer adjacent to a first side of the second electrode, and a second side of the first gas diffusion electrode adjacent to the first gas.

[0070] cell ,for example cell During operation of 10, at the molecular level, liquid-phase materials produced or consumed by the electrochemical reactions spontaneously migrate from or to the reaction zones of the electrodes along the length of the inter-electrode spacer to or from the reservoir, in the liquid electrolyte within the inter-electrode spacer. That is, the liquid-phase reactants or products migrate "in-plane" through the liquid electrolyte along the length of the inter-electrode spacer to or from the reservoir. The liquid-phase materials do so under capillary, diffusion, and / or osmotic control, and are "self-regulated" by the concentration differences present in the liquid electrolyte. As a result of these self-regulated migrations, the liquid-phase reactants can be regulated by adding fresh liquid-phase reactants to the reservoir. cell and the liquid phase product can be replenished by removing the liquid phase product from the tank. cell Preferably, cell is working, cell The porous capillary spacer is configured such that liquid phase reactants or products of an electrochemical reaction in the porous capillary spacer follow a liquid phase path in the liquid electrolyte inside the porous capillary spacer. Preferably, during the electrochemical reaction, the liquid electrolyte in the porous capillary spacer promotes migration of one or more liquid phase materials along the length of the porous capillary spacer. Preferably, the porous capillary spacer is configured to transport the liquid electrolyte along the porous capillary spacer by capillary action, diffusion, and / or osmosis. Preferably, migration of one or more liquid phase materials along the length of the porous capillary spacer is under the control of liquid phase capillary action, diffusion, and / or osmosis. Preferably, cell is working, cellis configured to be self-regulated by capillary action, diffusion, and / or osmosis occurring within the porous capillary spacer. Preferably, the electrochemical reaction is electrosynthesis or electrochemical reaction using electrical energy. cell Preferably, the movement of the liquid phase material from the intersecting planar axis is self-regulated by the composition of the liquid electrolyte in the reservoir. Preferably, the liquid phase capillary, diffusion, and / or osmosis is regulated by (i) constantly replenishing one or more liquid phase materials consumed within the liquid electrolyte; (ii) constantly removing one or more liquid phase materials formed within the liquid electrolyte; It acts in the porous capillary spacer in the same way.

[0071] cell 10 may optionally be encased in a liquid- and gas-impermeable outer housing 151. The outer housing 151 may incorporate a liquid conduit 152 forming one inlet / outlet or separate inlets and outlets (not shown) for the reservoir 140, or one or more liquid conduits (i.e., the outer housing 151 provides at least one external liquid conduit 152) for supplying make-up or excess liquid-phase reactants and / or products and / or liquid electrolyte 100. cell The at least one external liquid conduit 152 may allow for external ingress or egress, i.e., the liquid electrolyte, along with the associated liquid-phase reactants and / or products of the reaction, is transported into or out of the vessel 140 via at least one external liquid conduit 152. The liquid conduit 152 may be in direct connection with, or in direct or indirect communication with, a liquid storage system 153, preferably an external liquid storage system 153, which may contain make-up or excess liquid-phase reactants and / or products or liquid electrolyte 100. That is, the at least one external liquid conduit 152 is in direct or indirect communication with the external liquid storage system 153 for external storage / supply / removal of the liquid electrolyte 100 and / or liquid-phase reactants or products. Preferably, cell teeth, cell and an outer housing providing at least one external liquid conduit. cell teeth cellThe external housing includes an external housing having at least one external liquid conduit, and the liquid electrolyte is transported into or out of the reservoir via the at least one external liquid conduit. cell During operation, liquid electrolyte cell The liquid-phase reactants and / or products of the electrochemical reaction are delivered via at least one external liquid conduit. cell The at least one external fluid conduit is configured for fluid transfer within or to an external fluid storage system.

[0072] The reservoir 140 may further include an opening 145 through which the porous capillary spacer 110 passes. The opening 145 can be a slit, a gap, an orifice, or the like. The reservoir 140 can be formed of two halves, such as two cavities in different bodies, that abut together to form the reservoir 140, each body including a groove or notch through which the porous capillary spacer 110 can pass to be in liquid contact with the liquid electrolyte 100 in the reservoir 140. The housing or walls of the reservoir 140 prevent the liquid electrolyte 100 in the reservoir 140 from coming into direct contact with the first electrode 120 or the second electrode 130. Thus, as described above, the liquid electrolyte 100 can only contact the first electrode 120 and the second electrode 130 after the liquid electrolyte 100 has first been transported from the reservoir 140 along the porous capillary spacer 110. The area of ​​direct contact between the porous capillary spacer 110 and the first electrode 120 can be external to the reservoir 140. Similarly, the area of ​​direct contact between the porous capillary spacer 110 and the second electrode 130 can be external to the reservoir 140. In one embodiment, the first electrode 120 and the second electrode 130 are spaced apart from the reservoir 140. In one embodiment, the first electrode 120 and the second electrode 130 are physically separated from the reservoir 140. In one embodiment, the first electrode 120 and the second electrode 130 are located away from the reservoir 140. In one embodiment, the first electrode 120 and the second electrode 130 are located completely external to the reservoir 140.

[0073] In one example, an additional barrier layer 155 may optionally be provided to help prevent the liquid electrolyte 100 in layer 140 from directly contacting the first electrode 120 and the second electrode 130. The barrier layer 155 includes gaps or openings 145 through which the porous capillary spacers 110 pass. The barrier layer 155 may be integrated as part of the layer 140 or may be provided as a separate, separate layer. The barrier layer 155 may be formed of a material that is impermeable to the liquid electrolyte 100. Preferably, the layer includes openings through which the porous capillary spacers pass.

[0074] As a result of the presence of (i) a single opening, slit, gap, or orifice 145, etc., and / or (ii) an additional barrier layer 155 that contains only a single opening that is completely filled with the porous capillary spacer 110, cell may be unaffected or partially unaffected by orientation effects. That is, if there is only one opening at the end of the reservoir nearest the electrode, and that opening is filled with a porous capillary spacer 110, and the reservoir is mostly filled with liquid electrolyte 100, for example, the reservoir may be cell in any orientation, including on top of cell It may be possible to get it to work successfully.

[0075] Optionally, the second electrode is a second gas diffusion electrode. Preferably, the second gas diffusion electrode is configured to generate a second gas forming a second gas, and a second side of the second gas diffusion electrode is adjacent to the second gas. Preferably, the second electrode is configured to generate the second gas and to be in direct contact with the second gas containing the second gas. Thus, in cases where both the first electrode 120 and the second electrode 130 are gas diffusion electrodes, the two gases, first gas 125 containing the first gas (associated with the first electrode 120) and second gas 135 containing the second gas (associated with the second electrode 130), preferably reside on opposite sides of the electrolyte-filled porous capillary spacer 110. The first side of the porous capillary spacer 110 is adjacent to the first side of the first electrode 120. The second side of the porous capillary spacer 110 is adjacent to the first side of the second electrode 130. The second side of the first electrode 120 is adjacent to the first gas 125. The second side of the second electrode 130 is adjacent to the second gas 135. Preferably, cell are configured such that during operation, at least a portion of the second side of the first gas diffusion electrode is in direct gas-phase contact with the first gas, and at least a portion of the second side of the second gas diffusion electrode is in direct gas-phase contact with the second gas. That is, at least a portion of the second side of the first electrode 120 is in direct gas-phase contact with the first gas 125. At least a portion of the second side of the second electrode 130 is in direct gas-phase contact with the second gas 135.

[0076] At the molecular level, gas-phase materials produced or consumed by electrochemical reactions migrate perpendicular (90°) to the liquid-phase materials along continuous gas-phase pathways that are distinct from and do not interfere with the liquid-phase pathways. That is, gas molecules or atoms migrate to and from each macroscopic gas through associated interfaces to and from the gas diffusion electrodes and interelectrode spacers, i.e., into or out of the reaction zone within or around the interelectrode spacers. These interfaces can be further engineered (e.g., by incorporating gas capillaries or gas handling structures) to modify gas migration rates. Such migration preferably occurs under capillary and / or diffusion control along continuous gas-phase pathways connecting each electrode to each gas. Thus, gas-phase materials (reactants or products) also exhibit self-regulation. Because each gas migration pathway does not overlap or interfere with other gas migration pathways or liquid migration pathways, gas migration is independently self-regulated, separate from the self-regulation of liquid migration. That is, different gas-phase and liquid-phase reactants or products each undergo their own self-regulation that does not interfere with the migration of other reactants or products.

[0077] Preferably, the gas capillary structure promotes gas migration into or out of the intersecting planar axis under the influence of gas phase capillaries. Examples of gas capillary structures include, but are not limited to: i. porous deaeration plate, ii. a porous hydrophobic membrane, and / or iii. Porous or narrow-porous hydrophobic structures and / or other gas capillary structures that spontaneously draw gas from a liquid and exhibit a measurable capillary pressure associated with gas uptake. There is.

[0078] Preferably, the gas handling structures facilitate gas migration into or out of the intersecting planar axis. Examples of gas handling structures include, but are not limited to: (a) Having a surface area with low surface energy, e.g., a gas that has a measurable capillary pressure, which facilitates or accelerates gas transport without the involvement of capillary effects. 1. Materials with low surface energy such as polytetrafluoroethylene (PTFE), fluorinated polymers, Nafion®, etc. 2. Surface structures with low surface energy, such as nanoscale superhydrophobic structures or a material or structure in which gases tend to selectively coalesce and migrate, such as those comprising or consisting of (b) Materials or structures with super-anaerobic surface regions that promote desorption of coalescing gases, such as super-hydrophilic or "super-wetting" materials or structures. There is.

[0079] Preferably, the gas present within such gas capillary structures or gas handling structures is or will be continuous with an adjacent gas, such as the first gas or the second gas. Optionally, the gas present within such gas handling structures is independently in gaseous communication with an external gas conduit and / or an external gas storage system.

[0080] Preferably, cell comprises a gas capillary structure located at least partially within or on the second side of the first gas diffusion electrode. cell comprises a gas handling structure located at least partially within or on the second side of the first gas diffusion electrode. cell comprises a gas capillary structure located at least partially within or on the second side of the second gas diffusion electrode. cell comprises a second gas handling structure located at least partially within or on a second side of the second gas diffusion electrode. cell comprises a gas handling structure located between the first gas diffusion electrode and the porous capillary spacer, within the first gas diffusion electrode, at or near the first gas diffusion electrode, and / or on a portion of the first gas diffusion electrode. cell includes a second gas handling structure located between the second gas diffusion electrode and the porous capillary spacer, within the second gas diffusion electrode, at or near the second gas diffusion electrode, and / or on a portion of the second gas diffusion electrode.

[0081] Preferably, cellis configured such that, during operation, the first gas follows a first vapor phase path to the first gas diffusion electrode, the first vapor phase path being separate from the liquid phase path. cell is configured such that during operation, the second gas of the second gas follows a second vapor phase path to the second gas diffusion electrode, the second vapor phase path being separate from the liquid phase path. Preferably, the migration paths of the liquid and vapor phase materials into and out of the intersecting planar axis are directed differently. Preferably, cell is configured such that during operation, a continuous gas phase path exists between the active surface of the first gas diffusion electrode and the first gas in the intersecting planar axis, whereby no visible bubbles of the first gas are generated on at least a portion of the active surface of the first gas diffusion electrode. cell is configured such that during operation, no gas bubbles are visible at least in part of the first gas diffusion electrode or at least in part of the second gas diffusion electrode. cell is configured such that, during operation, the first gas diffusion electrode is covered with a thin film of liquid electrolyte less than 0.125 mm thick, preferably less than 0.11 mm thick, more preferably less than 0.10 mm thick. cell is configured such that during operation, a continuous gas phase path exists between the active surface of the second gas diffusion electrode and the second gas at the intersecting plane, whereby no visible bubbles of the second gas are generated on at least a portion of the active surface of the second gas diffusion electrode. cell is configured such that, during operation, the second gas diffusion electrode is covered with a thin film of liquid electrolyte that is less than 0.125 mm thick, preferably less than 0.11 mm thick, and more preferably less than 0.10 mm thick.

[0082] Thus, the first gas (associated with the first electrode 120 ) can be a reactant consumed at the first electrode 120 or a product produced by the first electrode 120 . cell During operation, the first gas 125 needs to be replenished with a first gas (in the case of a reactant) or the first gas needs to be removed from the first gas 125 (in the case of a product). The second gas (associated with the second electrode 130) can be a reactant consumed at the second electrode 130 or a product produced by the second electrode 130. cellDuring operation, the second gas 135 needs to be replenished with a second gas (in the case of a reactant) or the second gas needs to be removed from the second gas 135 (in the case of a product).

[0083] The first gas in the first gas body 125, in various examples, is connected to and gaseously communicates with, can be contained within, or can be transported into or out of, at least one external first gas conduit 127, which can be one or more pipes, one or more conduits, a common gas manifold, a chamber, etc., through the external housing 151. The second gas in the second gas body 135, in various examples, is connected to and gaseously communicates with, can be contained within, or can be transported into or out of, at least one external second gas conduit 137, which can be one or more pipes, one or more conduits, a common gas manifold, a chamber, etc., through the external housing 151. The at least one external first gas conduit 127 and / or the at least one external second gas conduit 137 may be provided in addition to the at least one external liquid conduit 152 or may be provided without the at least one external liquid conduit 152; or cell Not included in 10, cell10 may include only at least one external liquid conduit 152. The external first gas conduit 127 may be connected to or in gaseous communication with a first gas storage system 128, preferably the external first gas storage system 128. The external second gas conduit 137 may be connected to or in gaseous communication with a second gas storage system 138, preferably the external second gas storage system 138. The external first gas storage system 128 and the external first gas conduit 127, i.e., associated pipes, conduits, manifolds, and chambers, may allow a first gas in the first gas medium 125 to be supplied to or removed from a region adjacent to the first electrode 120. The external second gas storage system 138 and the external second gas conduit 137, i.e., associated pipes, conduits, manifolds, and chambers, may allow a second gas in the second gas medium 135 to be supplied to or removed from a region adjacent to the second electrode 130. That is, the external housing 151 may provide at least one external first gas conduit 127, and / or the external housing 151 may provide at least one external second gas conduit 137. A first gas (if present) may be transported in or out of the first gas body 125 via the at least one external first gas conduit 127, and / or a second gas (if present) may be transported in or out of the second gas body 135 via the at least one external second gas conduit 137. In other words, the at least one external first gas conduit 127 is in gaseous communication with the external first gas storage system 128 for externally storing the first gas, and / or the at least one external second gas conduit 137 is in gaseous communication with the external second gas storage system 138 for externally storing the second gas.

[0084] Generally, a separate supply system and a separate removal system are used. cell 10, and each reactant is independently controlled during operation. cell Supply to cell 10. Each such system preferably includes: cell Reactants are fed to, or products are removed from, separate gas or liquid reservoirs within the reactor, and the gas or liquid reservoirs are cell Reactants are delivered to or products are removed from associated electrodes within the reactor.

[0085] Preferably, cell comprises an external housing, the external housing providing at least one external first gas conduit, and the first gas being transported into or out of the first gas storage system via the at least one external first gas conduit. Preferably, the external housing provides at least one external gas conduit in gaseous communication with the first gas. Preferably, the at least one external first gas conduit is in gaseous communication with an external first gas storage system. Preferably, the external housing further provides at least one external first gas conduit, and is configured such that, during operation, the first gas is transported into or out of the first gas storage system via the at least one external first gas conduit. Preferably, cell The external housing further includes an external first gas conduit, and the first gas is transported into or out of the first gas chamber via the external first gas conduit. Thus, for example, an external first reactant source (i.e., cell 10) supplies the first reactant to the first electrode 120 via one or more first reactant pipes or conduits. Optionally, the external housing further provides at least one external second gas conduit, and is configured such that, during operation, a second gas is transported in or out of the second gas storage system via the at least one external second gas conduit. Preferably, the at least one external second gas conduit is in gaseous communication with an external second gas storage system. Preferably, the external housing further includes providing at least one external second gas conduit, and the second gas is transported in or out of the second gas storage system via the at least one external second gas conduit. Optionally, an external second reactant source supplies the second reactant to the first electrode 120 or the second electrode 130 via one or more second reactant pipes or conduits. Additionally, optionally, an external additional reactant source supplies additional reactants to the first electrode 120 or the second electrode 130 via one or more additional reactant pipes or conduits. cell10) receives a first product produced at first electrode 120 via one or more first product pipes or conduits. Optionally, an external second product tank or reservoir receives a second product produced at first electrode 120 or second electrode 130 via one or more second product pipes or conduits. Further, optionally, an external further product tank or reservoir receives further products produced at first electrode 120 or second electrode 130 via one or more further product pipes or conduits.

[0086] Preferably, the liquid electrolyte 100 within the porous capillary spacer 110 and the capillary pressure that the liquid electrolyte 100 maintains within the porous capillary spacer 110 separate the first gas 125 and the second gas 135, preventing the first gas 125 and the second gas 135 from physically contacting each other, or at least minimizing the extent to which each contaminates the other. In one example, the porous capillary spacer 110 is filled with the liquid electrolyte 110 before the end 150 of the porous capillary spacer is positioned within the reservoir 140. In another example, the liquid electrolyte 100 is first transported from the reservoir 140 along the porous capillary spacer 110 before contacting the first electrode 120 and the second electrode 130. Preferably, cell During operation of the system 10, at least a portion of the porous capillary spacer 110 adjacent to all of the first electrodes 120 and at least a portion of the porous capillary spacer 110 adjacent to all of the second electrodes 130 remain filled with the liquid electrolyte 100. Preferably, when the porous capillary spacer is filled with the liquid electrolyte, the porous capillary spacer is configured to prevent or impede mixing of the first gas with the second gas, maintaining a benchmark gas crossover of less than 2%.

[0087] To equalize, or keep as close as possible, the pressures of the two gases 125 and 135 and the liquid electrolyte 100, a pipe, conduit, well, or chamber 149 may be incorporated into the top of the reservoir 140. Such a pipe, conduit, well, or chamber 149 may provide a direct interface between each gas 125 and 135 and the liquid electrolyte in the reservoir 140, thereby ensuring that their pressures are equal. Preferably, the pipe, conduit, well, or chamber 149 extends upward from the top of the reservoir some way into the gases 125 and 135. This minimizes the likelihood that liquid electrolyte temporarily displaced from the reservoir due to a transient pressure difference will spill into the gas chamber occupied by the gases 125 and 135. Furthermore, if any liquid electrolyte spills into the gas chamber, it will be physically disconnected and separated from the liquid electrolyte in the rest of the reservoir.

[0088] Preferably, but not exclusively, cell is configured such that, during operation, the first gas has a pressure of greater than 3 bar gauge, preferably greater than 4 bar gauge, more preferably greater than 5 bar gauge. cell is configured such that during operation the second gas has a pressure above 3 bar gauge.

[0089] In cases where only one of the first electrode 120 and the second electrode 130 is a gas diffusion electrode, there may be only one gas, which is the first gas 125 (if the first electrode 120 is a GDE) and the second gas 135 (if the second electrode 130 is a GDE).

[0090] The first electrode 120 and the second electrode 130 are connected to an external electrical circuit 180 by a first electrical connection 160 and a second electrical connection 170, respectively. The first electrical connection 160, the second electrical connection 170, or the external electrical circuit 180 itself preferably penetrates the external housing 151 without compromising its gas and liquid impermeability. The external electrical circuit 180 transmits electrical energy cell 10 (e.g., electrosynthesis) cell (In the case of ). Alternatively, cellThe electrical energy generated by 10 may be supplied to an external electrical circuit 180 (e.g., electrical energy cell in the case of).

[0091] For example, the external circuit may include a power supply that applies a voltage between the first electrode and the second electrode in operation. Many examples of power supplies are commercially available, all of which may be used to apply a voltage across two terminals, each of which may be separately connected to the first electrode and the second electrode. In another example, the external circuit may include a power supply that supplies, for example, electrical energy cell The device may include a power receiving and modulating device such as a DC / AC converter that regulates the amount of power received and generates an external voltage when attached to the electrodes of the device. Many examples of power receiving devices are commercially available, all of which have terminals that receive electrical energy. cell When separately connected to the first and second electrodes of the power supply, they can be used to generate an external voltage. A variety of voltages, such as greater than 0.5 V, greater than 2 V, greater than 5 V, greater than 10 V, greater than 20 V, greater than 50 V, greater than 100 V, greater than 250 V, greater than 500 V, greater than 1000 V, greater than 5000 V, or greater than 10,000 V, can be applied by those power sources or received by such a power receiving device.

[0092] Preferably, the external circuit includes a power source or power receiving device capable of applying or generating a voltage between the first gas diffusion electrode and the second electrode.

[0093] Further exemplary embodiments are shown for electrosynthesis employing thin porous capillary spacers 110 (less than 0.45 mm thick) as inter-electrode spacers. cell or electrical energy cell Preferably, cell is zero gap cellThus, the porous capillary spacer 110 is less than 0.45 mm thick, preferably less than 0.30 mm thick, and more preferably less than 0.13 mm thick. A non-limiting example of such a thin porous capillary spacer 110 is a thin porous polyethersulfone material filter having an average pore size of 8 μm supplied by Pall Corporation. The thin porous material utilizes capillary exchange to draw and retain the liquid electrolyte in the inter-electrode spacer. Two electrodes are sandwiched on either side of the inter-electrode spacer. At least one or both of the electrodes may be porous to gas, i.e., a gas diffusion electrode. The bottom end of the inter-electrode spacer may optionally be immersed in a liquid electrolyte reservoir that may be separate from the electrodes, or the reservoir may contact either or both of the two electrodes, or the reservoir may be entirely incorporated within the porous capillary spacer. If both electrodes are gas diffusion electrodes, the gas diffusion electrodes are in fluid contact with the gas on one or both sides of the electrode-spacer-electrode assembly. The sealed (liquid-tight and / or gas-tight) external conduits and storage volumes connected separately to the gas and / or reservoir are cell In other examples, the porous capillary spacer 110 is less than 0.35 mm thick, less than 0.2 mm thick, less than 0.1 mm thick, less than 0.05 mm thick, or less than 0.025 mm thick.

[0094] Preferably, the porous capillary spacer has an average pore size of more than 2 μm and less than 400 μm. Preferably, the porous capillary spacer has an average pore size of more than 4 μm and less than 400 μm, more than 6 μm and less than 400 μm, more than 8 μm and less than 400 μm, more than 10 μm and less than 400 μm, more than 20 μm and less than 400 μm, or more than 30 μm and less than 400 μm. Preferably, the porous capillary spacer has an average pore size of about 3 μm, about 4 μm, about 5 μm, about 6 μm, about 7 μm, about 8 μm, about 9 μm, or about 10 μm. Preferably, the porous capillary spacer has an average pore size of less than 400 μm. Optionally, the porous capillary spacer is more than 60% porous, preferably more than 70% porous, and most preferably more than 80% porous. Preferably, the porous capillary spacer is filled with a liquid electrolyte and has a resistivity of 140 mΩ cm at room temperature. 2Preferably, the first gas diffusion electrode and the second electrode are compressed against the porous capillary spacer at more than 2 bar, preferably more than 3 bar, more preferably more than 4 bar. Preferably, the first gas diffusion electrode and the second gas diffusion electrode are compressed against the porous capillary spacer at more than 2 bar, preferably more than 3 bar, more preferably more than 4 bar. Preferably, the liquid electrolyte is aqueous, and when the porous capillary spacer is filled with the liquid electrolyte, the liquid electrolyte in the porous capillary spacer flows at a rate of more than 0.0014 g of water per minute at a height of more than 8 cm.

[0095] Preferably, the first gas diffusion electrode and the second electrode each have a thickness of 10 cm 2 Preferably, the first gas diffusion electrode comprises a metal mesh, a metal foam, and / or a metal perforated plate. Preferably, the second gas diffusion electrode comprises a metal mesh, a metal foam, and / or a metal perforated plate. Preferably, cell is operated using a current of 1 Amp or greater, preferably 1.5 Amp or greater, more preferably 2 Amp or greater, and more preferably 2.5 Amp or greater through the first gas diffusion electrode and the second electrode. cell operates continuously for at least 24 hours.

[0096] Such electrosynthesis or electrical energy cell For uninterrupted or continuous operation over an indefinite period of time, the thin porous capillary spacer 110 preferably comprises, among other things: i) drawing in liquid electrolyte and maintaining itself completely filled with liquid electrolyte, thereby cell maintaining a column height of liquid electrolyte within a porous capillary spacer extending to the top of the ii) preferably providing a flow rate of fluid electrolyte within the porous capillary spacer sufficient to sustain the electrochemical reaction at all times and under all operating conditions; iii) At the interface of the porous capillary spacer with the electrodes, release sufficient liquid electrolyte to adequately wet the electrodes for reaction under all operating conditions. It is possible.

[0097] Preferably, cell is electrosynthesis cell The electrochemical reaction is cell Preferably, the enzyme produces a chemical product that is transported away from the enzyme and to the outside. cell is electrical energy cell and electrochemical reactions are cell generates energy that is transported away from the

[0098] Both the liquid and vapor phase migration pathways are self-regulating; cell can operate continuously without external supervision. This is different from many conventional electrosynthetic or electrical energy converters that typically require active supervision. cell constitutes a significant advantage over

[0099] The bath liquid comes into direct contact with the electrodes cell Examples Another embodiment of zero-gap electrosynthesis or electrical energy cell 20 is shown schematically in FIG. cell 20 in that the wall of the vessel closest to the electrode may be absent and there may be no barrier 155 between the vessel and the electrode. cell 10. Thus, the liquid 100 in the reservoir may be in direct contact with one or both electrodes 120 or 130. The degree of contact may be relatively small (e.g., 5-10% of the outer electrode area, as shown in FIG. 2A) or relatively large (e.g., 50-70% of the outer electrode area, as shown in FIG. 2B). However, the degree of contact between the liquid electrolyte and the electrodes may vary. cell It should be understood that A and B may be constant or may change rapidly, slowly, temporarily, or permanently during operation, and that the specific values ​​of A and B may be anywhere between 0% and 100%, inclusive.

[0100] Optionally, the values ​​of A and / or B are small. Preferably, cellWhen the reservoir contains a liquid electrolyte, the first gas diffusion electrode is configured to contact the liquid electrolyte at the edge of the reservoir. cell When the reservoir contains a liquid electrolyte, the second electrode is configured to contact the liquid electrolyte at the edge of the reservoir. cell 20 is the same as in Figure 1 cell 10. In other respects, cell 20 is the same as in Figure 1 cell It may have one or more of the same components with the same properties and characteristics as the 10 components.

[0101] The example embodiment shown in FIG. cell In this embodiment, gases 125 and 135 may be adjacent to and in contact with a smaller percentage of the outer surface area of ​​electrodes 120 and 130, respectively, than in the embodiment shown in Figure 2. For example, the degree of contact may be relatively small (e.g., 30-50% of the outer surface area of ​​the electrodes, as shown for gas 135 in Figure 2), or relatively large (e.g., 90-95% of the outer surface area of ​​the electrodes, as shown for gas 125 in Figure 2). However, these values ​​may be cell It should be understood that the value may be constant or may change rapidly, slowly, temporarily, or permanently during operation, and may range anywhere from 0% to 100%, inclusive.

[0102] Although a smaller percentage of contact between the electrodes 120 or 130 and the gases 125 and 135, respectively, is typical, many of the features and advantages of the preferred embodiments may nevertheless still apply, either fully or partially.

[0103] Further, the example embodiments of this class cell (i.e. cell 20) is another preferred embodiment of cell These may provide features and advantages that are less common or not observed in other systems. cell This includes the ability of the relative liquid levels in 20 to physically vary, i.e., the variation of the relative values ​​of A and B. cell Such a change in relative liquid level in (i) Rapid and spontaneous equalization of gas pressures in gases 125 and 135 with compensatory movement of liquid to new A and / or B values; (ii) improving the maintenance of the porous capillary spacer 110 being completely filled with liquid electrolyte at all times; and / or (iii) Improved maintenance of fully wet electrodes during operation This may make it possible.

[0104] Furthermore, the ability of the electrodes to be in physical contact with the liquid electrolyte means that capillary action at the electrodes can be employed to assist the capillary action of the porous capillary spacer 110. That is, capillary action at the electrodes can be used to transport the liquid electrolyte to the reaction zones at the electrodes or between the electrodes. In fact, the liquid electrolyte may be induced to migrate to the capillary at the electrode and along the capillary to the porous capillary spacer 110 or the electrode 120 or 130, thereby (i) cell Porous capillary spacers 110 filled with liquid electrolyte at all times, including at locations above (ii) in operation; cell Electrodes that are thoroughly wet at all times, including the upper areas within the This can help maintain

[0105] Of course, capillary-induced movement of liquid electrolyte onto and above the electrode surfaces can typically interfere with, or even prevent, gas transfer between the electrodes 120 or 130 and the gas 125 or 135, respectively. cell 20 energy efficiency. However, it has been discovered that if such transport is configured to involve only a very thin layer of liquid electrolyte moving along the surface of the electrode, there is no interference with gas transport. That is, if capillary-induced transport of liquid electrolyte can be designed to avoid flooding of the electrode and its pores, this may provide an alternative, advantageous, non-interfering method of transporting liquid electrolyte to the reaction zone that also undergoes self-regulation.

[0106] Preferably, cellis configured such that, during operation, the first gas diffusion electrode is covered with a thin film of liquid electrolyte less than 0.125 mm thick, preferably less than 0.11 mm thick, more preferably less than 0.10 mm thick. cell is configured such that, during operation, the second gas diffusion electrode is covered with a thin film of liquid electrolyte that is less than 0.125 mm thick, preferably less than 0.11 mm thick, and more preferably less than 0.10 mm thick.

[0107] Having a reservoir built into a porous capillary spacer cell Examples FIG. 3 illustrates an alternative embodiment of zero-gap electrosynthesis or electrical energy storage in which the reservoir is incorporated into the porous capillary spacer 110 itself, such that a distinct liquid reservoir separate from the porous capillary spacer may not be discernible. cell Shows 30.

[0108] cell 30 may be used, for example, when the reactants and products are purely gas-phase materials and liquid electrolyte is not consumed, produced, or in any way affected by the electrochemical reaction. For example, rare, expensive, or exotic liquid electrolytes that do not readily vaporize, such as "ionic liquids," may be employed. In such cases, it may be most practical to minimize the amount of liquid electrolyte present by minimizing the size of the reservoir and incorporating the reservoir into the porous capillary spacer 110.

[0109] The resulting cell30 may be capable of viably promoting new electrochemical reactions that cannot currently be performed on an industrial scale. The ability to promote electrical energy or electrosynthesis conversion using small amounts of rare, expensive, or exotic liquid electrolytes may open up new electrochemical reactions to industrial manufacturing that can currently only be performed using such electrolytes. Gas phase reactants and / or products may be supplied to or removed from gases 125 and / or 135 via external pipes 127, 137a, and / or 137b to / from first gas storage system 128, second gas storage system 138a, and / or third gas storage system 138b. Two gas storage systems (second gas storage system 138a and third gas storage system 138b) are shown in FIG. 3 to introduce reactants and / or cell 1 shows a situation where gas is circulated through a gas (135 in this illustrative case) to remove products from the

[0110] The use of rare, expensive, or exotic materials that do not readily vaporize, such as "ionic liquids," is not shown in FIG. 3. cell It should be understood that the present invention is not limited to the structure of such an electrolyte. cell It can be used in.

[0111] In another example embodiment, the porous capillary spacer 110 is filled with an aqueous liquid electrolyte, and the reservoir is entirely incorporated into the porous capillary spacer 110. In this case, the aqueous electrolyte within the porous capillary spacer 110 may be replenished or maintained by introducing or removing water vapor into the gases 125 and / or 135, some of which condenses in the porous capillary spacer 110 or evaporates from the porous capillary spacer 110.

[0112] As previously mentioned, using gas-phase vapor to replenish or maintain a liquid-phase material, such as water, in the inter-electrode separator may typically interfere with or prevent the transfer of gas-phase reactants or products between the electrodes 120 or 130 and the gas 125 or 135, respectively. cell This can reduce the energy efficiency of the system.

[0113] However, it has been discovered that the situation may be different when a porous capillary spacer 110 filled with a liquid electrolyte held within the spacer by capillary forces is employed as the inter-electrode separator. It may be possible to replenish or maintain the liquid electrolyte by introducing or removing water vapor from one or both gases (i.e., the first gas 125 and / or the second gas 135) without interfering with the other existing gas-phase pathways (of gaseous reactants or products to / from the electrodes). In operation, a voltage may be applied or generated between the first electrode 120 and the second electrode 130.

[0114] That is, under some circumstances, a vapor phase pathway can be created that does not interfere with or impede the vapor phase pathway of gaseous reactants or products to / from the electrodes to replenish or maintain the liquid phase electrolyte.

[0115] This may be particularly possible when the porous capillary spacer 110 is used as an inter-electrode separator because a continuum of liquid electrolyte may be confined within the porous capillary spacer. Such a continuum of liquid electrolyte may not be present in other inter-electrode separators. Water vapor may preferably condense in such a continuum of liquid or vaporize from such a continuum of liquid. Furthermore, the liquid is held within the spacer by capillary forces, thereby ensuring that any water vapor that condenses in the liquid is confined to the porous capillary spacer 110 by capillary forces, thereby not overflowing or blocking the electrodes from access by gas reactants / products.

[0116] Preferably, cell During operation, the liquid electrolyte in the porous capillary spacer cell Preferably, the electrode is configured to contain only a continuum of liquid electrolyte within the electrode. cell does not include an external liquid conduit, and the liquid electrolyte and / or liquid-phase reactants and / or products are in vapor form within the gas stream. cellThe porous capillary spacer is configured to be transported in or out of the porous capillary spacer, and the vapor liquefies in or evaporates from the liquid electrolyte in the porous capillary spacer. cell In the present invention, there is no external liquid conduit and the liquid electrolyte, liquid-phase reactants, and / or products are in vapor form within the gas stream. cell Preferably, the reservoir is integrated as part of the porous capillary spacer, and the vapor is condensed in or evaporated from the liquid electrolyte in the porous capillary spacer.

[0117] In other respects, cell 30 is the same as in Figure 1 cell 10 or Fig. 2 cell 20. In other respects, cell 30 is the same as in Figure 1 cell 10 or Fig. 2 cell It may have one or more of the same components with the same properties and characteristics as the 20 components.

[0118] Further Example Embodiments Beyond the above embodiment examples, cell Various other example embodiments of structures may be utilized, including, but not limited to, other structures described herein.

[0119] In further example embodiments, electrosynthesis or electrical energy cell The stack is provided with a first electrochemical or electrical energy cell and a first electrosynthesis or electrical energy cell a second electrosynthetic or electrical energy cell Each electrosynthesis or electric energy cellThe present invention relates to a battery comprising a reservoir for containing a liquid electrolyte, a first gas diffusion electrode located outside the reservoir, a second electrode located outside the reservoir, and a porous capillary spacer located between the first gas diffusion electrode and the second electrode, the porous capillary spacer having an end extending into the reservoir, the porous capillary spacer being capable of filling itself with the liquid electrolyte when the end of the porous capillary spacer is in liquid contact with the liquid electrolyte in the reservoir.

[0120] Preferably, electrosynthesis or electrical energy cell In the stack of the first electrosynthesis or electrical energy cell is an example embodiment described herein. cell and the second electrosynthesis or electrical energy cell is an example embodiment described herein. cell Preferably, electrosynthesis or electrical energy cell In the laminate of the first electrosynthesis or electrical energy cell and second electrosynthesis or electrical energy cell are connected in series.

[0121] In a further embodiment, electrosynthesis or electrical energy for carrying out electrochemical reactions cell A method of operation of cell The present invention relates to a method for manufacturing a liquid electrolyte battery, the method comprising: a reservoir for containing a liquid electrolyte; a first gas diffusion electrode located outside the reservoir; a second electrode located outside the reservoir; and a porous capillary spacer located between the first gas diffusion electrode and the second electrode, the porous capillary spacer having an end extending into the reservoir, the porous capillary spacer being capable of filling itself with the liquid electrolyte when the end of the porous capillary spacer is in liquid contact with the liquid electrolyte in the reservoir; and the method includes applying a voltage between the first gas diffusion electrode and the second electrode.

[0122] In a further embodiment, a method for electrosynthesis or electrical energy conversion for carrying out an electrochemical reaction includes applying a voltage between a first gas diffusion electrode and a second electrode. cell A method of operation is provided.

[0123] In a further embodiment, the first electrosynthesis or electrical energy cell and second electrosynthesis or electrical energy cell applying a voltage between each of the first gas diffusion electrodes and the second electrode to generate an electrosynthesis or electrical energy for carrying out an electrochemical reaction; cell A method of operating the stack is provided.

[0124] In a further example embodiment, electrosynthetic water electrolysis cell is provided, cell is configured to generate a first gas, and comprises a first gas diffusion electrode configured to be in direct contact with a first gas containing the first gas, a second electrode, and a porous capillary spacer filled with a liquid electrolyte and configured to be positioned between the first gas diffusion electrode and the second electrode, wherein the porous capillary spacer has an average pore size greater than 2 μm.

[0125] In a further example, multiple cell whereby a plurality of cell are electrically connected to each other.

[0126] In a further example embodiment, electrosynthetic water electrolysis cell The stack is provided with a first electrosynthetic water electrolysis cell and the first electrosynthetic water electrolysis cell a second electrosynthetic water electrolysis system electrically connected to the cell Each electrosynthetic water electrolysis cell The present invention relates to a fuel cell comprising: a first gas diffusion electrode configured to generate a first gas and to be in direct contact with a first gas containing the first gas; and a porous capillary spacer filled with a liquid electrolyte and configured to be positioned between the first gas diffusion electrode and a second electrode, wherein the porous capillary spacer has an average pore size of greater than 2 μm.

[0127] Preferably, electrosynthetic water electrolysis cell In the stack of the first electrosynthetic water electrolysis cell is an example embodiment described herein. cell The second electrosynthetic water electrolysis cell is an example embodiment described herein. cell Preferably, electrosynthetic water electrolysis cell In the stack of the first electrosynthetic water electrolysis cell and second electrosynthetic water electrolysis cell are connected in series.

[0128] In a further embodiment, an electrosynthetic water electrolysis device is provided for performing water electrolysis. cell A method of operation of cell The present invention relates to a fuel cell comprising a first gas diffusion electrode configured to generate a first gas and to be in direct contact with a first gas comprising the first gas, a second electrode, and a porous capillary spacer filled with a liquid electrolyte and configured to be positioned between the first gas diffusion electrode and the second electrode, wherein the porous capillary spacer has an average pore size greater than 2 μm, and the method includes applying a voltage between the first gas diffusion electrode and the second electrode.

[0129] In a further embodiment, a method for performing water electrolysis includes applying a voltage between a first gas diffusion electrode and a second electrode. cell A method of operation is provided.

[0130] In a further embodiment, an electrosynthetic water electrolysis device is provided for performing water electrolysis. cell A method of operating the stack of the present invention is provided, the method comprising: applying a voltage to a first electrode to synthesize water electrolysis cell and second electrosynthetic water electrolysis cell The method includes applying a voltage between each of the first gas diffusion electrodes and the second electrode.

[0131] In a further embodiment, electrosynthesis or electrical energy cella first gas diffusion electrode configured to generate a first gas and be in adjacent contact with a first gas comprising the first gas; a second gas diffusion electrode configured to generate a second gas and be in direct contact with a second gas comprising the second gas; and a porous capillary spacer configured to be located between the first gas diffusion electrode and the second gas diffusion electrode, the porous capillary spacer being filled with a liquid electrolyte and configured to confine the liquid electrolyte in the porous capillary spacer by capillary effect, whereby the liquid electrolyte has a maximum column height of greater than 0.4 cm. cell is provided.

[0132] Optionally, cell may include a reservoir containing a liquid electrolyte and configured to underlie the porous capillary spacer during operation, with at least a distal end of the porous capillary spacer contacting the liquid electrolyte in the reservoir. Preferably, the liquid electrolyte has a maximum column height of greater than 0.4 cm.

[0133] In a further example, multiple cell whereby a plurality of cell are electrically connected to form an electrocomposite or electrical energy multi-cell stack.

[0134] In a further example, electrosynthesis or electrical energy cell The stack is provided with a first electrochemical or electrical energy cell and a first electrosynthesis or electrical energy cell a second electrosynthetic or electrical energy source electrically connected to the cell Each electrosynthesis or electric energy cellThe present invention relates to a gas diffusion device comprising: a first gas diffusion electrode configured to generate a first gas and to be in contact with and adjacent to a first gas comprising the first gas; a second gas diffusion electrode configured to generate the first gas and to be in contact with and adjacent to a second gas comprising a second gas; and a porous capillary spacer located between the first gas diffusion electrode and the second gas diffusion electrode, the porous capillary spacer being filled with a liquid electrolyte and configured to confine the liquid electrolyte in the porous capillary spacer by capillary effect, whereby the liquid electrolyte has a maximum column height of greater than 0.4 cm.

[0135] In a further example, electrosynthesis or electrical energy cell A laminate of the above is provided, and a first electrochemical or electrical energy cell is an example embodiment described herein. cell and the second electrosynthesis or electrical energy cell is an example embodiment described herein. cell is.

[0136] In a further example, the first electrosynthesis or electrical energy cell and second electrosynthesis or electrical energy cell are connected in series, electrosynthesis or electrical energy cell A laminate of the following is provided.

[0137] In a further embodiment, electrosynthesis or electrical energy for carrying out electrochemical reactions cell A method of operation of cella first gas diffusion electrode configured to generate a first gas and be in direct contact with a first gas comprising the first gas; a second gas diffusion electrode configured to generate a second gas and be in direct contact with a second gas comprising the second gas; and a porous capillary spacer configured to be located between the first gas diffusion electrode and the second gas diffusion electrode, the porous capillary spacer being filled with a liquid electrolyte and configured to confine the liquid electrolyte in the porous capillary spacer by capillary effect, whereby the liquid electrolyte has a maximum column height of greater than 0.4 cm; and the method includes applying a voltage between the first gas diffusion electrode and the second gas diffusion electrode.

[0138] In a further embodiment, a method for electrosynthesis or electrical energy conversion for carrying out an electrochemical reaction includes applying a voltage between a first gas diffusion electrode and a second gas diffusion electrode. cell A method of operation is provided.

[0139] In a further embodiment, the first electrosynthesis or electrical energy cell and second electrosynthesis or electrical energy cell applying a voltage between each of the first gas diffusion electrode and the second gas diffusion electrode to generate an electrosynthesis or electrical energy for carrying out an electrochemical reaction; cell A method of operating the stack is provided.

[0140] In further example embodiments, electrosynthesis or electrical energy for carrying out electrochemical reactions cell A method of operation of the electrosynthesis or electrical energy cell The method includes a vessel containing a liquid electrolyte, a first gas diffusion electrode, a second electrode, and a porous capillary spacer positioned between the first gas diffusion electrode and the second electrode, the porous capillary spacer being positioned within the vessel and having an end in liquid contact with the liquid electrolyte. The method includes contacting the first gas diffusion electrode and the second electrode with the liquid electrolyte and applying or generating a voltage between the first gas diffusion electrode and the second electrode.

[0141] In a further embodiment, the electrochemical reaction produces ammonia from nitrogen and hydrogen. In a further embodiment, the electrochemical reaction produces electricity from ammonia and oxygen. In a further embodiment, the electrochemical reaction produces hydrogen and nitrogen from ammonia. In a further embodiment, the electrochemical reaction produces NO as a reactant. X In a further embodiment, the electrochemical reaction produces chlorine, hydrogen, and caustic from brine. In a further embodiment, the electrochemical reaction produces chlorine and caustic from brine. In a further embodiment, the electrochemical reaction produces chlorine and hydrogen from hydrochloric acid. In a further embodiment, the electrochemical reaction produces electrical energy from hydrogen and oxygen. In a further embodiment, the electrochemical reaction produces hydrogen and oxygen from water. In a further embodiment, the electrochemical reaction extracts pure hydrogen from a gas mixture containing hydrogen.

[0142] In a further example, electrosynthesis or electrical energy cell is provided, cell The present invention relates to a method for producing an electrochemical cell comprising: a reservoir containing a liquid electrolyte; a first gas diffusion electrode; a second electrode; and a porous capillary spacer positioned between the first gas diffusion electrode and the second electrode, the porous capillary spacer being positioned within the reservoir and having an end in liquid contact with the liquid electrolyte, the porous capillary spacer being adapted to produce an electrochemical cell using electrosynthesis or electrical energy. cell may be configured to operate according to any example method described herein.

[0143] In a further example, the first electrosynthesis or electrical energy cell and second electrosynthesis or electrical energy cell Electrosynthesis or electrical energy cell A laminate of the following is provided.

[0144] In a further embodiment, the first electrosynthesis or electrical energy cell and second electrosynthesis or electrical energy cell are connected in series, electrosynthesis or electrical energy cell A laminate of the following is provided.

[0145] In a further embodiment, electrosynthesis or electrical energy is provided that includes two or more porous capillary spacers. Preferably, but not exclusively, zero-gap electrosynthesis or electrical energy includes two or more porous capillary spacers (preferably each less than 0.45 mm thick). cell has liquid electrolyte drawn into and continuously retained in the porous capillary spacers by capillary forces from two or more reservoirs of liquid electrolyte in which the ends of each porous capillary spacer are immersed.

[0146] In a further embodiment, an electrosynthesis or electrical energy system is provided that includes two or more reservoirs configured to contain a liquid electrolyte. cell is provided, wherein a distal end of each of the two or more porous capillary spacers is located within one of the two or more reservoirs.

[0147] In another embodiment, the reservoir may be configured to create, employ, or utilize an osmotic effect, preferably to increase the maximum column height of the liquid electrolyte in the porous capillary spacer and / or to increase the flow rate of components of the liquid electrolyte within the porous capillary spacer during the electrochemical reaction.

[0148] Preferably, the reservoir comprises a first volume configured to contain a first liquid, a second volume configured to contain a second liquid, and a semi-permeable membrane separating the first and second volumes. Optionally, the distal end of the porous capillary spacer is located in the first volume, and during operation, the first liquid is a liquid electrolyte and the second liquid is configured to be different from the first liquid.

[0149] In another embodiment, an electrosynthetic or electrical energy multi-cell stack is provided, the stack comprising a plurality of cell During operation, multiple cell Each of the second liquids is a plurality of cell The second volumes of the respective liquids are arranged to communicate with each other through a common supply or removal pipe connected to the second volumes of the respective liquids.

[0150] In a further embodiment, electrosynthesis or electrical energy cellis provided, wherein the porous capillary spacer is at least partially composed of one or more materials selected from the group including PVDF, PTFE, tetrafluoroethylene, fluorinated polymers, polyimides, polyamides, nylons, nitrogen-containing materials, glass fibers, silicon-containing materials, polyvinyl chloride, chloride-containing polymers, cellulose acetate, cellulose nitrate, cellophane, ethyl cellulose, cellulose-containing materials, polycarbonates, carbonate-containing materials, polyethersulfones, polysulfones, polyphenylsulfones, sulfone-containing materials, polyphenylene sulfide, sulfide-containing materials, polypropylene, polyethylene, polyolefins, olefin-containing materials, asbestos, titanium-based ceramics, zirconium-based ceramics, ceramic materials, polyvinyl chloride, vinyl-based materials, rubber, porous battery separators, and clays.

[0151] Additional Embodiments In another embodiment, zero-gap electrosynthesis or electrical energy cell is provided, cell consists of the following elements: (1) Two electrodes, at least one of which is gas permeable (i.e., a gas diffusion electrode), sandwiched on either side of a porous capillary spacer less than 0.45 mm thick (in other examples, less than 0.30 mm thick or less than 0.13 mm thick); (2) a porous capillary spacer containing a liquid electrolyte drawn therein by capillary action and held continuously therein; (3) optionally, an end of a porous capillary spacer, optionally spaced or separated from the electrode-spacer-electrode assembly described in (1) and (2) above, immersed in liquid electrolyte or otherwise in liquid contact with a reservoir of liquid electrolyte, optionally the porous capillary spacer being itself or incorporating a reservoir; (4) one or more gases on one or both sides of the electrode-spacer-electrode assembly, optionally the one or more gases being separated from the reservoir of liquid electrolyte, the one or more gases being in gaseous communication with each electrode; (5) cellSealed (liquid-tight / gas-tight) external conduits and storage volumes separately connected to the first gas, the second gas, and / or the reservoir for supplying reactants and removing products during operation.

[0152] Preferably, the porous capillary spacer is formed of or includes a porous material. Preferably, during the electrochemical reaction, the porous capillary spacer draws in the liquid electrolyte by capillary action to maintain a maximum column height of the liquid electrolyte within the porous capillary spacer. Preferably, the maximum column height exceeds either or both electrodes sandwiched against the porous capillary spacer. Preferably, the maximum column height of the liquid electrolyte is at least equal to or greater than the height of the first gas diffusion electrode. Preferably, the maximum column height is cell Preferably, the liquid electrolyte forming the column height is confined within the volume of the porous capillary spacer. Preferably, the liquid electrolyte within the porous capillary spacer is cell Preferably, the liquid electrolyte within the porous capillary spacer prevents or inhibits mixing of the first gas with the second gas.

[0153] Preferably, cell Liquid-phase reactants or products of the electrochemical reaction in the porous capillary spacer follow a liquid-phase pathway within the liquid electrolyte within the porous capillary spacer. Preferably, during the electrochemical reaction, the liquid electrolyte within the porous capillary spacer promotes migration of liquid-phase material by "in-plane" migration along the length of the porous capillary spacer to or from a reservoir of liquid electrolyte under the influence and control of liquid-phase capillary action, diffusion, and / or osmosis. Optionally, at least one electrode promotes migration of a thin film of liquid electrolyte along and / or above the electrode surface under the influence and control of liquid-phase capillary action. Preferably, a first gas of the first gas follows a first vapor-phase pathway to the first gas diffusion electrode, the first vapor-phase pathway being separate from the liquid-phase pathway. Preferably, a second gas of the second gas follows a second vapor-phase pathway to the second gas diffusion electrode, the second vapor-phase pathway being separate from the liquid-phase pathway.

[0154] Preferably, during the electrochemical reaction, liquid-phase capillary, diffusion, and / or osmosis actions operate within the electrolyte-filled porous capillary spacer to (i) constantly replenish one or more liquid-phase materials consumed within the liquid electrolyte, or (ii) constantly remove one or more liquid-phase materials produced within the liquid electrolyte, or (iii) constantly introduce / remove one or more liquid-phase materials that would otherwise be directly or peripherally involved in the electrochemical reaction. That is, preferably, the electrochemical reaction is carried out by electrosynthesis or electrical energy. cell Optionally, during the electrochemical reaction, liquid phase capillary action involving a thin film of liquid electrolyte migrating over the surface of the electrode acts to (i) constantly replenish one or more liquid phase materials consumed in the liquid electrolyte, or (ii) constantly remove one or more liquid phase materials produced in the liquid electrolyte, or (iii) constantly introduce / remove one or more liquid phase materials that would otherwise be directly or peripherally involved in the electrochemical reaction. That is, preferably, the electrochemical reaction is electrosynthesis or electrical energy cell It self-regulates in this way.

[0155] Preferably, during the electrochemical reaction, the flow rate induced within the porous capillary spacer by said liquid-phase capillary, diffusion, and / or osmosis is sufficient to sustain the electrochemical reaction. Optionally, during the electrochemical reaction, the flow rate by liquid-phase capillary action involving a thin film of liquid electrolyte moving over the surface of the electrode is sufficient to sustain the electrochemical reaction.

[0156] Another non-limiting embodiment is zero-gap electrosynthesis or electrical energy synthesis. cell The present invention provides a method for producing electricity using a chemical product or power, the method comprising: (1) Two electrodes, at least one of which is gas porous (i.e., a gas diffusion electrode), (2) Consists of a porous capillary spacer (less than 0.45 mm thick) narrowed to both sides; (3) the porous capillary spacer contains a liquid electrolyte therein that is drawn therein by capillary action from a reservoir of liquid electrolyte and is constantly retained therein; (4) The end of the porous capillary spacer is immersed in a bath of electrolyte, or alternatively, The porous capillary spacer may incorporate a reservoir, or there may be no reservoir, and the liquid electrolyte within the porous capillary spacer may be cell contains only continuous liquid in (5) Gas is present on one or both sides of some of the electrode-spacer-electrode assemblies; (6) liquid phase materials involved in the electrochemical reaction migrate by "in-plane" movement within the porous capillary spacer along the length of the porous capillary spacer to or from the reservoir / body under the influence and control of capillary, diffusion, and / or osmotic forces; and / or A liquid phase material involved in the electrochemical reaction migrates in a thin film on the surface of at least one electrode to or from the reservoir / body under the influence and control of capillaries; (7) cell During operation, reactants are introduced through external conduits and storage volumes that separately connect to the first gas, the second gas, and / or the reservoir. cell The product is constantly supplied / replenished from outside. cell It is constantly removed externally.

[0157] Feature combinations According to various non-limiting example embodiments, the following points are considered in various cell , multi-cell stacks, example systems, and / or combinations of features that provide example methods of operation are disclosed.

[0158] 1. An electrosynthesis or electrical energy converter comprising a first gas diffusion electrode, a second electrode, and a porous capillary spacer positioned between the first gas diffusion electrode and the second electrode. cell .

[0159] 2. The porous capillary spacer is capable of filling itself with liquid electrolyte when the end of the porous capillary spacer is in liquid contact with the liquid electrolyte in the reservoir, as described in point 1. cell .

[0160] 3. The first gas diffusion electrode according to point 1 or 2 is located outside the cell cell .

[0161] 4. The method according to any of the preceding points, wherein the second electrode is located outside the vessel. cell .

[0162] 5. cell Electrosynthetic water electrolysis cell as described in any of the preceding points, cell .

[0163] 6. The method according to any of the preceding points, wherein the first gas diffusion electrode is in direct contact with the first gas. cell .

[0164] 7. The porous capillary spacer is filled with a liquid electrolyte, as described in any of the preceding points. cell .

[0165] 8. According to any of the preceding points, the porous capillary spacer has an average pore size of more than 2 μm. cell .

[0166] 9. The method of any of the preceding points, wherein the first gas diffusion electrode is in contact with and adjacent to the first gas. cell .

[0167] 10. The method of any of the preceding points, wherein the second gas diffusion electrode is in contact with and adjacent to the second gas. cell .

[0168] 11. The method of any of the preceding points, wherein the liquid electrolyte is confined in a porous capillary spacer by capillary effect, and the liquid electrolyte has a maximum column height of more than 0.4 cm. cell .

[0169] 12. Electrosynthesis or Electrical Energy cella reservoir for containing a liquid electrolyte; a first gas diffusion electrode located external to the reservoir; and a second electrode located external to the reservoir. a porous capillary spacer located between the first gas diffusion electrode and the second electrode, the porous capillary spacer having an end extending into the reservoir, the porous capillary spacer being capable of filling itself with the liquid electrolyte when the end of the porous capillary spacer is in liquid contact with the liquid electrolyte in the reservoir; cell .

[0170] 13. Electrosynthetic Water Electrolysis cell an electrosynthetic water electrolysis device comprising: a first gas diffusion electrode configured to generate a first gas and to be in direct contact with a first gas comprising the first gas; a second electrode; and a porous capillary spacer filled with a liquid electrolyte and configured to be located between the first gas diffusion electrode and the second electrode, wherein the porous capillary spacer has an average pore size of greater than 2 μm. cell .

[0171] 14. Electrosynthesis or Electrical Energy cell a first gas diffusion electrode configured to generate a first gas and be in direct contact with a first gas comprising the first gas; a second gas diffusion electrode configured to generate a second gas and be in contact with a second gas comprising the second gas and be adjacent to the second gas; and a porous capillary spacer located between the first gas diffusion electrode and the second gas diffusion electrode, the porous capillary spacer being filled with a liquid electrolyte and configured to confine the liquid electrolyte in the porous capillary spacer by capillary effect, whereby the liquid electrolyte has a maximum column height of more than 0.4 cm. cell .

[0172] 15. The method of any of the preceding points for carrying out an electrochemical reaction, comprising contacting a first gas diffusion electrode and a second electrode with a liquid electrolyte, and applying or generating a voltage between the first gas diffusion electrode and the second electrode. cell How it works.

[0173] 16. cell 10. The method of claim 9, further comprising providing at least one external liquid conduit to the fluid passage. cell Or method.

[0174] 17. The method according to any of the preceding points, wherein, when the reservoir contains a liquid electrolyte, the first gas diffusion electrode is configured to be separated from the liquid electrolyte in the reservoir. cell Or method.

[0175] 18. The method according to any of the preceding points, wherein, when the reservoir contains a liquid electrolyte, the first gas diffusion electrode is configured to contact the liquid electrolyte at the edge of the reservoir. cell Or method.

[0176] 19. The method according to any of the preceding points, wherein the second electrode is configured to be separated from the liquid electrolyte in the reservoir when the reservoir contains a liquid electrolyte. cell Or method.

[0177] 20. The method according to any of the preceding points, wherein, if the bath contains a liquid electrolyte, the second electrode is configured to contact the liquid electrolyte at the edge of the bath. cell Or method.

[0178] 21. The method of any of the preceding points, wherein the porous capillary spacer is filled with liquid electrolyte before the end of the porous capillary spacer extends into the reservoir. cell Or method.

[0179] 22. The method according to any of the preceding points, wherein during operation, the liquid electrolyte is configured to contact the first gas diffusion electrode and the second electrode only after first being transported from the reservoir along the porous capillary spacer. cell Or method.

[0180] 23. The method according to any of the preceding points, wherein the first gas diffusion electrode and the second electrode are spaced apart from the vessel. cell Or method.

[0181] 24. The method according to any of the preceding points, wherein the area of ​​direct contact between the porous capillary spacer and the first gas diffusion electrode is outside the vessel, and the area of ​​direct contact between the porous capillary spacer and the second electrode is outside the vessel. cell Or method.

[0182] 25. The method according to any of the preceding points, wherein the reservoir includes an opening through which the porous capillary spacer passes. cell Or method.

[0183] 26. According to any of the preceding points, the surface area covered by the liquid electrolyte in the porous capillary spacer is configured to be at least equal to or exceed the surface area of ​​the first gas diffusion electrode facing the porous capillary spacer during operation. cell Or method.

[0184] 27. The first gas diffusion electrode and the second electrode are each 10 cm 2 1. The method according to claim 1, further comprising: cell Or method.

[0185] 28. The method of any of the preceding points, wherein the first gas diffusion electrode comprises a metal mesh, a metal foam, and / or a metal perforated plate. cell Or method.

[0186] 29. The device according to any of the preceding points, wherein the first gas diffusion electrode is configured to generate a first gas forming a first gas, a first side of the porous capillary spacer is adjacent to a first side of the first gas diffusion electrode, a second side of the porous capillary spacer is adjacent to a first side of the second electrode, and a second side of the first gas diffusion electrode is adjacent to the first gas. cell Or method.

[0187] 30. The method according to any of the preceding points, wherein the second electrode is a second gas diffusion electrode. cell Or method.

[0188] 31. The method of any of the preceding points, wherein the second gas diffusion electrode comprises a metal mesh, a metal foam, and / or a metal perforated plate. cell Or method.

[0189] 32. The method of any preceding point, wherein the second gas diffusion electrode is configured to generate a second gas that forms a second gas, and the second side of the second gas diffusion electrode is adjacent to the second gas. cell Or method.

[0190] 33. The method of any preceding point, wherein during operation, at least a portion of the second side of the first gas diffusion electrode is configured to be in direct gas-phase contact with a first gas, and at least a portion of the second side of the second gas diffusion electrode is configured to be in direct gas-phase contact with a second gas. cell Or method.

[0191] 34. The method of any of the preceding points, comprising a gas capillary structure located at least partially within or on the second side of the first gas diffusion electrode. cell Or method.

[0192] 35. The method of any of the preceding points, including a second gas capillary structure located at least partially within or on the second side of the second gas diffusion electrode. cell Or method.

[0193] 36. cell is zero gap cell and whereby the porous capillary spacer is less than 0.45 mm thick, preferably less than 0.30 mm thick, more preferably less than 0.13 mm thick. cell Or method.

[0194] 37. The method according to any of the preceding points, wherein the porous capillary spacer has an average pore size of more than 2 μm and less than 400 μm. cell Or method.

[0195] 38. The method according to any of the preceding points, wherein the average pore size of the porous capillary spacer is greater than 4 μm and less than 400 μm, greater than 6 μm and less than 400 μm, greater than 8 μm and less than 400 μm, greater than 10 μm and less than 400 μm, greater than 20 μm and less than 400 μm, or greater than 30 μm and less than 400 μm. cell Or method.

[0196] 39. The method of any of the preceding points, wherein the porous capillary spacer includes a plurality of holes that provide flow paths between the first gas diffusion electrode, the second electrode, and the reservoir. cell Or method.

[0197] 40. The porous capillary spacer according to any of the preceding points, wherein the porous capillary spacer is fluidly connected to a reservoir. cell Or method.

[0198] 41. The porous capillary spacer of any of the preceding points, wherein the porous capillary spacer is at least partially composed of one or more materials selected from the group including PVDF, PTFE, tetrafluoroethylene, fluorinated polymers, polyimides, polyamides, nylons, nitrogen-containing materials, glass fibers, silicon-containing materials, polyvinyl chloride, chloride-containing polymers, cellulose acetate, cellulose nitrate, cellophane, ethyl cellulose, cellulose-containing materials, polycarbonates, carbonate-containing materials, polyethersulfones, polysulfones, polyphenylsulfones, sulfone-containing materials, polyphenylene sulfide, sulfide-containing materials, polypropylene, polyethylene, polyolefins, olefin-containing materials, asbestos, titanium-based ceramics, zirconium-based ceramics, ceramic materials, polyvinyl chloride, vinyl-based materials, rubber, porous battery separators, and clays. cell Or method.

[0199] 42. The method further includes: cell and / or cell 10. The method of claim 9, further comprising providing at least one external liquid conduit for removing liquid from the cell Or method.

[0200] 43. The method of any of the preceding points, further comprising an external housing providing at least one external gas conduit in gaseous communication with the first gas. cell Or method.

[0201] 44. The liquid electrolyte is aqueous, and when the porous capillary spacer is filled with the liquid electrolyte, the liquid electrolyte in the porous capillary spacer flows at a flow rate of more than 0.0014 g of water per minute at a height of more than 8 cm, as described in any of the preceding points. cell Or method.

[0202] 45. The method of any of the preceding points, wherein during operation, the first gas is configured to have a pressure of more than 3 bar gauge, preferably more than 4 bar gauge, more preferably more than 5 bar gauge. cell Or method.

[0203] 46. ​​The method according to any of the preceding points, wherein the first gas diffusion electrode and the second electrode are compressed against the porous capillary spacer at more than 2 bar, preferably more than 3 bar, more preferably more than 4 bar. cell Or method.

[0204] 47. The porous capillary spacer according to any of the preceding points, wherein the porous capillary spacer has a porosity of more than 60%, preferably more than 70%, and most preferably more than 80%. cell Or method.

[0205] 48. The method of any of the preceding points, wherein during operation, a continuous gas phase path exists between the active surface of the first gas diffusion electrode and the first gas in the cross-sectional axis, such that no visible bubbles of the first gas are generated on at least a portion of the active surface of the first gas diffusion electrode. cell Or method.

[0206] 49. A gas handling structure comprising: Between the first gas diffusion electrode and the porous capillary spacer; in the first gas diffusion electrode, at or near the first gas diffusion electrode, and / or A portion of the first gas diffusion electrode 10. The gas handling structure of claim 1, further comprising: cell Or method.

[0207] 50. The method of any of the preceding points, wherein the second electrode is configured to generate a second gas and to be in direct contact with a second atmosphere containing the second gas. cell Or method.

[0208] 51. The method of any preceding point, wherein the porous capillary spacer is configured to inhibit or prevent mixing of the first gas with the second gas when the porous capillary spacer is filled with a liquid electrolyte, maintaining a benchmark gas crossover of less than 2%. cell Or method.

[0209] 52. A second gas handling structure, comprising: Between the second gas diffusion electrode and the porous capillary spacer; in the second gas diffusion electrode, at or near the second gas diffusion electrode, and / or Part of the second gas diffusion electrode 10. The method of claim 1, further comprising: cell Or method.

[0210] 53. During operation, the liquid electrolyte in the porous capillary spacer cell 1. The method according to claim 1, further comprising the step of: cell Or method.

[0211] 54. cell does not include an external liquid conduit, and the liquid electrolyte and / or liquid-phase reactants and / or products are in vapor form within the gas stream. cell According to any of the preceding points, the vapor is condensed into or evaporated from the liquid electrolyte in the porous capillary spacer. cell Or method.

[0212] 55. The end of the porous capillary spacer is located in the tank, as described in any of the preceding points. cell Or method.

[0213] 56. The method according to any of the preceding points, wherein the reservoir is configured to be filled with a liquid electrolyte and the end of the porous capillary spacer is configured to contact the liquid electrolyte. cell Or method.

[0214] 57. The porous capillary spacer according to any of the preceding points, wherein the porous capillary spacer is configured to transport the liquid electrolyte along the porous capillary spacer by at least capillary action. cell Or method.

[0215] 58. The method of any of the preceding points, wherein the porous capillary spacer is configured to transport the liquid electrolyte along the porous capillary spacer by capillary action, diffusion, and / or osmosis. cell Or method.

[0216] 59. In operation, cell is self-regulated by capillary action, diffusion, and / or osmosis occurring within the porous capillary spacer. cell Or method.

[0217] 60. The porous capillary spacer is filled with a liquid electrolyte and has a resistance of 140 mΩ cm at room temperature. 2 3. The method of claim 1, wherein the ionization resistance is less than cell Or method.

[0218] 61. A method according to any of the preceding points, wherein the first gas diffusion electrode is configured such that during operation it is covered with a thin film of liquid electrolyte less than 0.125 mm thick, preferably less than 0.11 mm thick, more preferably less than 0.10 mm thick. cell Or method.

[0219] 62. The method according to any of the preceding points, wherein the porous capillary spacer has an average pore size of less than 400 μm. cell Or method.

[0220] 63. The method according to any of the preceding points, wherein the porous capillary spacer has an average pore size of about 3 μm, about 4 μm, about 5 μm, about 6 μm, about 7 μm, about 8 μm, about 9 μm, or about 10 μm. cell Or method.

[0221] 64. Any of the preceding points cell It contains multiple cell are electrically connected, preferably electrically connected in series.

[0222] 65. The method of any preceding point, further comprising: a reservoir containing a liquid electrolyte and configured to underlie the porous capillary spacer during operation, wherein at least a distal end of the porous capillary spacer is in contact with the liquid electrolyte in the reservoir. cell Or method.

[0223] 66. The method of any of the preceding points, further comprising an external housing, the external housing providing at least one external liquid conduit. cell Or method.

[0224] 67. In operation, cell a liquid electrolyte, a liquid-phase reactant of an electrochemical reaction, and / or a liquid-phase product of an electrochemical reaction, through at least one external liquid conduit; cell 10. The method of claim 9, wherein the liquid supply system is configured to be transported in or out of the liquid supply system and wherein at least one external liquid conduit is configured to communicate with an external liquid storage system. cell Or method.

[0225] 68. In operation, cell 10. The method of claim 9, wherein the liquid-phase reactants or products of the electrochemical reaction within the porous capillary spacer are configured to follow a liquid-phase path within the liquid electrolyte within the porous capillary spacer. cell Or method.

[0226] 69. The method of any of the preceding points, wherein during operation, the first gas follows a first gas phase path to the first gas diffusion electrode, the first gas phase path being separate from the liquid phase path. cell Or method.

[0227] 70. The method of any of the preceding points, wherein during operation, the second gas follows a second gas phase path to the second gas diffusion electrode, the second gas phase path being separate from the liquid phase path. cell Or method.

[0228] 71. The method of any of the preceding points, wherein the porous capillary spacer is configured to prevent or impede mixing of the first gas with the second gas when the porous capillary spacer is filled with a liquid electrolyte, maintaining a benchmark gas crossover of less than 2%. cell Or method.

[0229] 72. The method according to any of the preceding points, wherein during operation, gas bubbles are not visible at least in part of the first gas diffusion electrode or at least in part of the second gas diffusion electrode. cell Or method.

[0230] 73. The method according to any of the preceding points, wherein the external housing further provides at least one external first gas conduit, and wherein during operation the first gas is configured to be transported into or out of the first gas chamber via the at least one external first gas conduit. cell Or method.

[0231] 74. The method of any of the preceding points, wherein at least one external first gas conduit is in gaseous communication with an external first gas storage system. cell Or method.

[0232] 75. The method of any of the preceding points, wherein the external housing further provides at least one external second gas conduit, and wherein during operation, the second gas is configured to be transported into or out of the second gas via the at least one external second gas conduit. cell Or method.

[0233] 76. The method according to any of the preceding points, wherein at least one external second gas conduit is in gaseous communication with an external second gas storage system. cell Or method.

[0234] 77. The method of any preceding point, wherein the reservoir comprises a first volume configured to contain a first liquid, a second volume configured to contain a second liquid, and a semi-permeable membrane separating the first volume and the second volume. cell Or method.

[0235] 78. The method of any preceding point, wherein the distal end of the porous capillary spacer is located in a first volume, and wherein, during operation, the first liquid is a liquid electrolyte and the second liquid is configured to be different from the first liquid. cell Or method.

[0236] 79. According to any of the preceding points, including two or more porous capillary spacers cell Or method.

[0237] 80. The method of any of the preceding points, comprising two or more reservoirs configured to contain a liquid electrolyte, wherein a distal end of each of the two or more porous capillary spacers is located within one of the two or more reservoirs. cell Or method.

[0238] 81. Any of the preceding points cell Contains multiple, active, multiple cell Each of the second liquids is a plurality of cell The electrosynthetic or electrical energy multi-cell stack is configured to communicate a liquid through a common supply or removal pipe connected to each second volume of the stack.

[0239] 82. The method according to any of the preceding points, comprising filling the porous capillary spacer with liquid electrolyte from the layer by at least capillary action. cell Or method.

[0240] 83. The method of any of the preceding points, comprising filling the porous capillary spacer with liquid electrolyte before the end of the porous capillary spacer is positioned in the reservoir. cell Or method.

[0241] 84. The method of any of the preceding points, comprising contacting the first gas diffusion electrode and the second electrode with the liquid electrolyte after the liquid electrolyte has been transported along the porous capillary spacer. cell Or method.

[0242] 85. During operation, the porous capillary spacer remains filled with liquid electrolyte, as described in any of the preceding points. cell Or method.

[0243] 86. cell is electrosynthesis cell The electrochemical reaction is cell 3. The method according to claim 1, wherein the chemical product is transported away from the cell Or method.

[0244] 87. cell and the external housing provides at least one external liquid conduit, and the liquid electrolyte is transported into or out of the reservoir via the at least one external liquid conduit. cell Or method.

[0245] 88. The device according to any of the preceding points, further comprising an external housing providing at least one external first gas conduit, wherein the first gas is transported into or out of the first gas chamber via the at least one external first gas conduit. cell Or method.

[0246] 89. cell 10. The method of claim 9, further comprising providing an external housing for the first gas supply system, the external housing providing at least one external first gas conduit, the first gas being transported into or out of the first gas supply system via the at least one external first gas conduit. cell Or method.

[0247] 90. The device according to any of the preceding points, further comprising an external housing providing at least one external second gas conduit, wherein the second gas is transported into or out of the second gas chamber via the at least one external second gas conduit. cell Or method.

[0248] 91. In a gas turbine engine, there is no external liquid conduit and the liquid electrolyte, liquid-phase reactants, and / or products are in vapor form within the gas stream. cell 10. The method of claim 1, further comprising transporting the device in or out of the device. cell Or method.

[0249] 92. The method according to any of the preceding points, wherein the reservoir is integrated as part of the porous capillary spacer, and the vapor is condensed in or evaporated from the liquid electrolyte in the porous capillary spacer. cell Or method.

[0250] 93. cell According to any of the preceding points, the device is operated using a current of 1 Amp or more, preferably 1.5 Amp or more, more preferably 2 Amp or more, and more preferably 2.5 Amp or more through the first gas diffusion electrode and the second electrode. cell Or method.

[0251] 94. cell operates continuously for at least 24 hours, cell Or method.

[0252] 95. The porous capillary spacer according to any of the preceding points, wherein the porous capillary spacer draws liquid electrolyte into the porous capillary spacer by capillary action and maintains the liquid electrolyte at the column height. cell Or method.

[0253] 96. The method according to any of the preceding points, wherein the maximum column height of the liquid electrolyte is at least equal to or greater than the height of the first gas diffusion electrode. cell Or method.

[0254] 97. During an electrochemical reaction, the liquid electrolyte in the porous capillary spacer promotes migration of one or more liquid phase materials along the length of the porous capillary spacer, as described in any of the preceding points. cell Or method.

[0255] 98. The method according to any of the preceding points, wherein the migration of one or more liquid phase materials along the length of the porous capillary spacer is under the control of liquid phase capillary action, diffusion, and / or osmosis. cell Or method.

[0256] 99. Electrochemical reactions are reactions that involve electrosynthesis or electrical energy. cell 5. The method according to claim 1, wherein the cell Or method.

[0257] 100. The method according to any of the preceding points, wherein the movement of the liquid phase material from the intersecting plane axis is self-regulated by the composition of the liquid electrolyte in the bath. cell Or method.

[0258] 101. The migration paths of the liquid and gas phase materials into and out of the intersecting plane axes are directed differently, as described in any of the preceding points. cell Or method.

[0259] 102. Liquid-phase capillary, diffusion, and / or osmosis are (i) constantly replenishing one or more liquid phase materials consumed within the liquid electrolyte; (ii) constantly removing one or more liquid phase materials formed within the liquid electrolyte; As described in any of the preceding points, acting in a porous capillary spacer cell Or method.

[0260] 103. The electrochemical reaction described in any of the preceding points produces ammonia from nitrogen and hydrogen. cell Or method.

[0261] 104. The electrochemical reaction described in any of the preceding points produces electricity from ammonia and oxygen. cell Or method.

[0262] 105. The electrochemical reaction described in any of the preceding points produces hydrogen and nitrogen from ammonia. cell Or method.

[0263] 106. Electrochemical reactions involve NO as a reactant. X Use the cell Or method.

[0264] 107. The electrochemical reaction described in any of the preceding points produces chlorine, hydrogen, and caustic from brine. cell Or method.

[0265] 108. The electrochemical reaction described in any of the preceding points produces chlorine and caustic from brine. cell Or method.

[0266] 109. The electrochemical reaction described in any of the preceding points produces chlorine and hydrogen from hydrochloric acid. cell Or method.

[0267] 110. The electrochemical reaction described in any of the preceding points produces electrical energy from hydrogen and oxygen. cell Or method.

[0268] 111. The electrochemical reaction described in any of the preceding points produces hydrogen and oxygen from water. cell Or method.

[0269] 112. The electrochemical reaction described in any of the preceding points extracts pure hydrogen from a hydrogen-containing gas mixture. cell Or method.

[0270] cellExamples include: (1) ammonia production, (2) chlorine production via the chlor-alkali process and its variants (e.g., including the oxygen-depolarized chlor-alkali process and the HCl recycle reaction), and (3) fuel for electricity. cell It can be used in several major industrial processes, including hydrogen production, (4) hydrogen production with aqueous electrolytes, and (5) hydrogen purification.

[0271] Electrosynthesis or Electrical Energy cell To be useful in industry, cell In the example, electrodes 125 and 135 are cell During operation, currents of 1 ampere or more may be passed. To achieve such currents, electrodes 125 and 135 are spaced apart by 10 cm. 2 In order to be energy efficient and maintain low electrical resistance during operation, the electrodes 125 and 135 may comprise current carriers capable of conducting high current with low electrical resistance, such as metal mesh, metal foam, and / or metal perforated plate. That is, the first gas diffusion electrode 120 may comprise metal mesh, metal foam, and / or metal perforated plate, and / or the second gas diffusion electrode 130 may comprise metal mesh, metal foam, and / or metal perforated plate. To be useful in industry, such electrodes must be made of a material with a low electrical resistance and a high electrical current capacity. cell is capable of operating uninterrupted or continuously for at least 24 hours at a time.

[0272] Preferred embodiments cell Features that may be present in Separate liquid and gas phase molecular level transport into and out of the reaction zone / intersecting plane axis Figure 4 shows cell 10, etc., an example of electrosynthesis or electrical energy cell 1 shows an enlargement of a portion of the electrode-spacer-electrode assembly 139 in FIG. cell The electrochemical reaction within 10 occurs at or between first electrode 120 and second electrode 130. In the example of Figure 4, first electrode 120 and second electrode 130 are both gas diffusion electrodes - i.e., they are porous and permeable to gases.

[0273] At each location along an electrode surface that is adjacent to, abutting, sandwiched, or laminated with the porous capillary spacer 110, electrochemical reactions occur at the electrode, and liquid-phase ions, intermediates, or molecules exchanged by the electrode travel along, within, or are largely confined to a pathway 180 between the first electrode 120 and the second electrode 130. A plurality of such pathways 180 exist down the entire length of the two electrodes 120, 130. For clarity, FIG. 4 shows only a few of the many pathways 180. As can be seen, these pathways 180 follow a "cross-plane" direction, i.e., perpendicular to the plane of the porous capillary spacer 110 and largely within the porous capillary spacer 110. Thus, cell The cumulative combination of all paths 180 in is said to constitute the "intersection plane" axis (also called the "reaction zone").

[0274] Electrochemical reactions typically consume reactants and produce products at the intersecting planar axis. That is, reactants are generally consumed and products are produced within the accumulation pathway 180. Once consumed, reactants must be replenished to maintain the electrochemical reaction. To achieve replenishment, new reactants must be moved from outside the intersecting planar axis to the intersecting planar axis. This movement must occur continuously if the electrochemical reaction is to be maintained. Similarly, products produced at the intersecting planar axis must be moved away from it to maintain the electrochemical reaction. If products accumulate at the intersecting planar axis, the electrochemical reaction may be impeded or may stop entirely.

[0275] In a preferred embodiment, liquid-phase reactants or products (or similarly other liquid-phase materials involved in electrochemical reactions) may move in or out of the intersecting planar axis by migration within the liquid electrolyte 100 present in the porous capillary spacer 110, following a path 190. Such migration may be to or from the reservoir 140. That is, the liquid-phase reactants or products may follow a path 190 in an "in-plane" direction, the path 190 being within the liquid electrolyte 100 inside the porous capillary spacer 110.

[0276] Such migration may occur spontaneously under the influence or control of capillary, diffusion, and / or osmosis, which are typically driven by differences in the concentration and composition of the electrolyte in the intersecting planar axis relative to the concentration and composition of the remainder of the electrolyte, which may primarily comprise the liquid electrolyte in reservoir 140. Reservoir 140 may comprise the vast majority of the liquid electrolyte in the system, such that in preferred embodiments, its composition and concentration are effectively (i) capillary, diffusion, and / or osmosis controls the rate at which changes to the electrolyte concentration and composition in the intersecting planar axes caused by the electrochemical reaction are counteracted; (ii) When the electrochemical reaction stops, including within the intersecting plane axis, cell Determine the final equilibrium state of the liquid electrolyte throughout In effect, the presence of liquid electrolyte 100 in reservoir 140 and the presence of continuous liquid connection (via porous capillary spacer 110) to the intersecting planar axis can control and regulate the movement of liquid phase material into and out of the intersecting planar axis.

[0277] Important Note Regarding Diffusion and Osmosis: The terms "diffusion" and "osmosis" have been used interchangeably herein to describe processes that result in net movement of liquid-phase material within a porous capillary spacer, such as porous capillary spacer 110. The reason for this equivalence is that in some example porous capillary spacers, which are porous materials, solute diffusion may have fewer degrees of freedom than water diffusion. That is, in some example porous capillary spacers, water movement may be more favorable than solute movement, potentially resulting in osmosis rather than a diffusion effect. To encompass this possibility and be descriptively inclusive, we have not distinguished between diffusion and / or osmosis that result in movement of liquid-phase material within a porous capillary spacer. Conversely, solute and water movement generally always have equal degrees of freedom within a bath of liquid electrolyte.

[0278] For example, hydrogen-oxygen fuel according to an example embodiment cellIn the case of argon, water may be produced as a product at the intersecting plane axis. As water is formed, it typically gradually dilutes the electrolyte at the intersecting plane axis, thereby increasing the ionic resistance, thereby cell However, because of the continuity of the liquid electrode 100 in the porous capillary spacer 110, by connecting the intersecting planar axis with, for example, the reservoir 140, capillary, diffusion, and / or osmosis spontaneously counteract the effects of dilution. That is, by capillary, diffusion, and / or osmosis, excess water in the intersecting planar axis may spontaneously migrate downward from the porous capillary spacer 110 toward the reservoir 140, while solutes in the porous capillary spacer 110 and the reservoir 140 migrate upward toward the intersecting planar axis. These processes may be driven by the difference in the concentration and composition of the electrolyte in the intersecting planar axis relative to the concentration and composition of the remainder of the electrolyte, which is mostly composed of the liquid electrolyte in the reservoir 140. The greater the dilution that occurs in the intersecting planar axis, the faster these processes may proceed. In this manner, the movement of liquid phase products from the intersecting planar axis may be “self-regulating” by the concentration and / or composition of the liquid electrolyte within the porous capillary spacer 110 and any associated reservoir 140 .

[0279] Similarly, capillary, diffusion, and osmosis can counteract, in a self-regulating manner, any other changes that occur in the composition and concentration of the electrolyte in the intersecting planar axis due to electrochemical reactions, including, for example, consumption of liquid phase materials and chemical changes to liquid phase materials in the electrolyte in the intersecting planar axis.

[0280] Conversely, gas-phase transport can occur in a direction perpendicular to liquid transport. When the first electrode 120 and the second electrode 130 are both porous gas diffusion electrodes, gas-phase reactants or products (or other gas-phase materials involved in the electrochemical reaction) can move in or out of the intersecting planar axis by migration to or from the continuous gases 125 and 135, respectively, across the first interface 126 and the second interface 136, respectively, between the gases 125 and 135 and the porous capillary spacer 110. These migrations follow paths 200. There can be multiple such paths 200 down the length of the electrodes 120, 130. These migrations can occur spontaneously under the influence and control of capillary forces and / or diffusion to and from the gases 125, 135 through the first electrode 120 and the second electrode 130, respectively.

[0281] Gases are known to spontaneously diffuse from regions of higher partial pressure to regions of lower partial pressure, with the rate of diffusion driven by the partial pressure difference. The diffusion process typically continues until the partial pressures are equalized at both locations, with the rate depending on the partial pressure difference. Thus, the supply of gas reactants to an electrode reaction zone and the removal of gas products from the electrode reaction zone can occur separately from the movement of liquid-phase reactants or products and can be independently "self-regulating." Furthermore, the supply of gas reactants to or the removal of gas products from a reaction zone associated with one electrode can occur separately from the supply of gas reactants to or the removal of gas products from the reaction zone associated with the other electrode and can also be independently "self-regulating."

[0282] In providing pathways to separate the reactants and products in the gas and liquid phases from each other and to prevent them from interfering with each other, the preferred embodiment cell Many electrochemical cell It is also possible to avoid or minimize the phenomenon of "multiphase backflow" that occurs in cell This involves the molecular-level movement of liquid-phase species that opposes the flow of gas-phase species within the electrolyte. cell In this case, the movement of liquid-phase reactants (water) toward the electrode surface can oppose and resist the movement of gas-phase products (e.g., hydrogen and oxygen) away from the electrode surface. The resulting multiphase backflow is cellThis can create serious operational complications. For example, it can produce bubbles or foam of the gas-liquid mixture, and the two phases of material must be disentangled in a gas-liquid separator tank. This type of multiphase counterflow can also create mass transport limitations, insofar as, for example, electrodes can be starved of reactants or products can accumulate excessively at the electrodes, depending on the strength of the countervailing flows. These types of inefficiencies can lead to inefficient cell It can lead to movement and require energy to resolve.

[0283] At least one distinct, independent, and non-interfering path cell Gas-liquid interaction occurs at the molecular level (flow) of reactants and products in the gas and liquid phases. cell is an "independent pathway" cell In order to avoid or minimize multiphase backflow, independent paths cell This also avoids or minimizes the inefficiencies created by multiphase backflow. cell is an independent path cell It could be.

[0284] cell Movement can be "self-regulating" Thus, gas consumed or produced at electrode 120 or 130 may be in direct vapor-phase contact with gases 125 and 135, respectively, along path 200. Because gases 125 and 135 comprise the majority of each gas in the system, the composition and pressure of gases 125 and 135 may control and regulate the rate of gas transport to and from each electrode 120 and 130. Capillary and diffusion may operate in a self-regulating manner to counteract changes that occur in gas composition and concentration at the electrodes and intersecting planar axes due to electrochemical reactions.

[0285] Conversely, liquid phase material may move in and out of the intersecting planar axis along a path 190 that is perpendicular (i.e., inclined by 90°) to and separate from the path 200 along which gas phase material may move in and out of the intersecting planar axis.

[0286] Additionally, pathway 190 may involve a continuous liquid phase, which is the phase best suited to controlling the migration of liquid phase materials, while pathway 200 may involve a continuous vapor phase, which is the phase best suited to controlling the migration of vapor phase materials.

[0287] Thus, an important feature of example embodiments is that the migration paths of liquid and vapor phase materials into and out of the intersecting planar axis may be separate, distinct, and independent, and may involve phases of matter best suited to controlling and regulating migration, and in so doing may avoid interference with one another and, as a result, be subject to independent regulation.

[0288] Another important feature is that the movement of liquid and vapor phase materials into and out of the intersecting planar axes along paths 190 and 200, respectively, is cell essentially, including changes in conditions within cell The capillary, diffusion, and osmotic processes share the common property of being able to change spontaneously in response to existing concentration and partial pressure differences. These processes can therefore be "self-regulating," which is cell The whole thing can be made self-regulating.

[0289] For example, if there is insufficient reactant needed to be consumed during an electrochemical reaction, this may manifest as a larger concentration difference or partial pressure difference, automatically increasing the reactant supply required for such a process. Conversely, if there is sufficient reactant, the concentration difference or partial pressure difference may decrease, thereby decreasing the reactant supply.

[0290] Capillary-induced migration of electrolyte can be promoted upward along the electrode While well-separated, non-interfering liquid and gas phase pathways are a feature of preferred embodiments, it should be understood that such pathways need not be strictly within the porous capillary spacer 110 (liquid phase) or at the interface between the gases (125 and 135) and the corresponding electrodes (120 and 130, respectively) (gas phase). Any separate, non-interfering liquid or gas phase pathways are within preferred embodiments and may be advantageously employed. If such pathways are separate and non-interfering, they may still be self-regulating.

[0291] Thus, for example, in a preferred embodiment having the structure shown in FIG. 2, as described above, the liquid electrolyte within the reservoir can be in physical contact with the electrolyte and can be induced to travel upward along the electrodes to the reaction zone.

[0292] Capillary action of the above type generally fills and floods the electrode and its pores, thereby hindering / interfering with gas transport to or from the electrode; cell This often significantly reduces the energy efficiency of the system.

[0293] However, it has surprisingly been discovered that porous electrodes (e.g., gas diffusion electrodes) with a relatively open structure / large pores can promote capillary-induced migration of only a thin layer of liquid electrolyte on the electrode surface. Such a layer can be thin enough to avoid impingement on the gas migration (reaction dependent). That is, such migration can constitute a non-interfering liquid phase pathway that has beneficial effects, for example, in improving the wettability of the electrode and helping to maintain the liquid electrolyte within the porous capillary spacer 110.

[0294] Furthermore, it has been discovered that electrode surfaces can be modified by coating them with thin hydrophilic or superhydrophilic layers that promote upward capillary-guided migration of thin layers of liquid electrolyte. In some cases, it has been shown that exceptionally rapid upward flow rates and maximum column heights can be achieved. This improves the wettability of the electrode, cell This can be particularly advantageous for helping to maintain the liquid electrolyte within the porous capillary spacer 110 in place above the

[0295] Furthermore, such a hydrophilic or superhydrophilic layer can be made of a catalyst. That is, the hydrophilic or superhydrophilic layer can also be the catalytic layer of the electrode. When covered with only a thin layer of the liquid electrode, such a catalytic layer can exhibit several advantageous effects. For example, gas can be generated by the catalytic layer without generating bubbles. This is known as "bubble-free" gas generation and will be described in more detail below.

[0296] Furthermore, such hydrophilic or superhydrophilic layers may be fabricated to incorporate "gas handling structures" that facilitate gas transport into or out of the reaction zone via independent, non-interfering pathways. Gas handling structures are described in more detail below.

[0297] Thus, the liquid electrolyte induced to migrate as a thin film up the capillaries within the electrodes to the porous capillary spacer 110 or the electrodes 120 or 130 (i) cell Porous capillary spacers 110 filled with liquid electrolyte at all times, including at locations above (ii) in operation; cell Electrodes that are thoroughly wet at all times, including the upper areas within the These may constitute a non-interfering liquid phase pathway that helps maintain

[0298] In preferred embodiments, the "thin layer" of liquid may be less than 0.125 mm thick. In other examples, it may be less than 1.5 mm, less than 1.0 mm, less than 0.7 mm, less than 0.5 mm, less than 0.3 mm, or less than 0.2 mm thick. In other examples, it may be less than 0.1 mm, less than 0.05 mm, less than 0.025 mm, less than 0.01 mm, less than 0.005 mm, less than 0.001 mm, less than 0.00001 mm, or less than 0.000001 mm thick.

[0299] Thus, an electrode 120 or 130 is provided that promotes the movement of liquid electrolyte 100 over the electrode surface by capillary action, preferably at a rate greater than 0.5 cm per minute. In other examples, the movement rate can be greater than 1 cm per minute, greater than 1.5 cm per minute, greater than 2 cm per minute, greater than 2.5 cm per minute, greater than 3 cm per minute, greater than 3.5 cm per minute, greater than 4 cm per minute, or greater than 5 cm per minute.

[0300] Using the porous capillary spacer 110, a non-interfering gas phase path for liquid replenishment / maintenance may be possible As also mentioned above, the vapor pathway for replenishing / maintaining the liquid electrolyte typically interferes with other vapor pathways that are present, but surprisingly does not when the porous capillary spacer 110 is used.

[0301] Thus, the type shown in Figure 3 cell In the 30 embodiment, it has been discovered that when porous capillary spacer 110 is employed as the inter-electrode separator, it may be possible to separately and uninterferingly replenish or maintain the liquid electrolyte by introducing water vapor or removing water vapor from one or both of gases 125 or 135.

[0302] This may be because the porous capillary spacer 110 includes a continuum of liquid electrolyte trapped within the porous capillary spacer. Other inter-electrode separators may not have such a continuous, trapped liquid of liquid electrolyte present. Water vapor may preferably condense in the liquid continuum or vaporize from the liquid continuum. Furthermore, any water vapor that condenses in the aqueous electrolyte continuum may be trapped in the spacer 110 by capillary forces, thereby ensuring that it does not overflow the gas reactants / products or block the electrodes from access by the gas reactants / products.

[0303] It is therefore also possible to replenish / maintain the liquid electrolyte within the porous capillary spacer 110 via separate, non-interfering pathways by which water vapor is introduced to / removed from the gas 125 or 135. If the pathway created is truly separate and does not interfere with other liquid or gas phase pathways, it should still be self-regulating.

[0304] Wetting of the electrode can involve electrode capillary action and compression of the electrode against a porous capillary spacer. As mentioned above, the embodiment cell A preferred feature of the method is that sufficient liquid electrolyte 100 is released from the porous capillary spacer 110 at its interface 126a or 136a with the electrode 120 or 130, respectively, to wet that electrode 120 or 130 for reaction. This may require that the electrode 120 or 130 exhibits a capillary action at its interface 126a or 136a towards the liquid electrolyte 100 that is stronger than the capillary action of the porous capillary spacer 110 towards the liquid electrolyte 100. That is, the porous capillary spacer 110 employs capillary action to draw in the liquid electrolyte 100 and fill itself with the liquid electrolyte 100. An electrode 120 or 130 sandwiched against the porous capillary spacer 110 may require stronger capillary action at the interface 126a or 136a to draw in the liquid electrolyte 100 and wet itself with the liquid electrolyte 100 held within the porous capillary spacer 110.

[0305] Thus, electrode 120 or 130 may also exhibit capillary action toward liquid electrolyte 100. Capillary action may include a capillary pressure greater than the capillary pressure of porous capillary spacer 100 filled at interface 126a or 136a. Preferably, the capillary pressure of electrode 120 or 130 is at least 10 mbar greater than the capillary pressure of porous capillary spacer 100 at interface 126a or 136a, respectively. Other examples include greater than 20 mbar, greater than 50 mbar, greater than 75 mbar, greater than 100 mbar, greater than 200 mbar, greater than 500 mbar, greater than 1 bar, or greater than 2 bar.

[0306] It has further been discovered that electrode wetting can be promoted by compressing the electrodes 120 and 130 against the porous capillary spacer 110. This type of electrode compression can help generate and maintain electrode wetting by ensuring intimate contact between the electrodes 120 or 130 and the porous capillary spacer 110 at the interfaces 126a and 136a, respectively. That is, it can avoid disruption of the liquid-phase pathway along which liquid-phase species travel from the porous capillary spacer 110 to the electrodes 120 or 130, respectively. Experiments using pressure-sensitive thin films indicate that this type of electrode compression is preferably in the range of 8 to 20 bar. In other examples, the electrode compression can be in the range of 6 to 8 bar, 4 to 6 bar, or 2 to 6 bar. In other examples, the electrode compression can be in the range of 20 to 25 bar, 25 to 30 bar, 30 to 35 bar, or 35 to 50 bar.

[0307] Gas capillaries or gas handling structures in, at, or near electrodes Although less well known, capillary action can also be observed in gas-phase materials. In such cases, gas can be induced to spontaneously flow into narrow spaces that would normally be expected to be filled with liquid. This can be seen, for example, when a capillary tube is immersed in a pool of mercury. The meniscus of liquid mercury inside the tube typically moves to a height lower than the height of the mercury outside the tube. In more practical applications, it can also be seen in the spontaneous extraction of gas from a solution, for example, by a degassing plate or a porous hydrophobic membrane. Any structure that spontaneously draws gas from a liquid and exhibits a measurable capillary pressure associated with gas uptake can be called a gas-capillary structure.

[0308] The gas capillary structure is cellThe gas capillary structures that facilitate gas movement into or out of the intersecting planar axis may be incorporated within or at least partially within the first electrode 120 and / or within or at least partially within the second electrode 130, adjacent to / near, at, or into the first electrode 120 or second electrode 130, or at, near, or into, for example, the electrode-gas (liquid-gas) boundary 126 b or 136 b or the electrode-spacer boundary 126 a or 136 a. cell may optionally include a gas capillary structure located in or at the first gas diffusion electrode and optionally a gas capillary structure located in or at the second gas diffusion electrode. The gas capillary structure, when indicating a capillary pressure for gas uptake, may include, but is not limited to, any of the following: - closely spaced hydrophobic surfaces; - Hydrophobic body with closely spaced perforations, - Deaeration board, or - Porous hydrophobic membrane. Examples may include, but are not limited to, those described in the section entitled "Breathable (bubble-free) electrodes" in the chemical publication entitled "The prospects of developing a highly energy efficient water electrolyser by eliminating or mitigating bubble effects" published in Sustainable Energy and Fuels, 2021, Vol. 5, p. 1280, which is incorporated herein by reference.

[0309] A feature of gas capillary structures is that they can contain one or more gases within them due to their affinity for gases, and such gases can persist as separate entities from the bulk gas even when the gas capillary structure is fully immersed in a liquid electrolyte.

[0310] In example embodiments, such gas within a gas capillary structure may be an adjacent gas or may become continuous with an adjacent gas. For example, a gas capillary structure within, at least partially at, adjacent to, at, or near electrode 120 may contain a gas that is gas 125 or that becomes continuous with gas 125. Similarly, a gas capillary structure within, at least partially at, adjacent to, at, or near electrode 130 may contain a gas that is gas 135 or that becomes continuous with gas 135. In such cases, the gas within a gas capillary structure may form part of a larger gas. For example, a gas within a gas capillary structure that is gas 125 or that becomes continuous with gas 125 may form part of gas 125. Gas 125 may be in gaseous communication with an external gas conduit (e.g., 127) and / or a gas storage system 128. Similarly, gas within a gas capillary structure that is or becomes continuous with gas 135 may form part of gas 135. Gas 135 may be in gaseous communication with an external gas conduit (e.g., 137) and / or a gas storage system (e.g., 138). In one example, a first side of the porous capillary spacer is adjacent to a first side of a first gas diffusion electrode, a second side of the porous capillary spacer is adjacent to a first side of a second gas diffusion electrode, a second side of the first gas diffusion electrode is adjacent to a first gas, and a second side of the second gas diffusion electrode is adjacent to a second gas. The gas capillary structure is at least partially located within the first gas diffusion electrode or on the second side of the first gas diffusion electrode. The second gas capillary structure may be located at least partially within the second gas diffusion electrode or on a second side of the second gas diffusion electrode.

[0311] Alternatively, the gas within the gas capillary structure may itself be a bulk gas that is in independent gaseous communication with an external gas conduit or storage system. For example, a gas capillary structure within, adjacent to, or near electrode 120 may contain an internal gas that is gas 125 and in direct gaseous communication with an external gas conduit (e.g., 127) or storage system (e.g., 128). Similarly, a gas capillary structure within, adjacent to, or near electrode 130 may contain an internal gas that is gas 135 and in direct gaseous communication with an external gas conduit (e.g., 137) or storage system (e.g., 138).

[0312] An alternative to the use of gas capillary structures in or near the electrodes is to incorporate "gas handling" structures that have physical properties that facilitate gas movement without necessarily utilizing the gas capillary effect. The pathways for gas movement in the gas handling structures can also be cell It does not interfere with and can be independent of other molecular-level liquid and gas phase movements within the polymer.

[0313] Optionally, the first gas diffusion electrode 120 may include a gas handling structure located within, at, or near the first gas diffusion electrode 120, for example, at or near boundary 126a or 126b. Also optionally, the second gas diffusion electrode 130 may include a gas handling structure within boundary 136a or 136b, or may include a gas handling structure located at or near boundary 136a or 136b. Examples of gas handling structures include, but are not limited to: (a) Having a surface area with low surface energy, e.g., a gas that has a measurable capillary pressure, which facilitates or accelerates gas transport without the involvement of capillary effects. 1. Materials with low surface energy such as polytetrafluoroethylene (PTFE), fluorinated polymers, Nafion®, etc. 2. Surface structures with nanoscale superhydrophobic structures, etc. Materials or structures in which gases tend to selectively coalesce and migrate, such as those containing or consisting of There is. Examples may include, but are not limited to, those described in the section entitled "Hydrophobic islands" in the chemistry publication entitled "The prospects of developing a highly energy efficient water electrolyser by eliminating or mitigating bubble effects" published in Sustainable Energy and Fuels, 2021, Vol. 5, p. 1280, which is incorporated herein by reference. Examples of gas handling structures include, but are not limited to: (b) Materials or structures with super-anaerobic surface regions that promote desorption of coalescing gases, such as super-hydrophilic or "super-wetting" materials or structures. Examples may include, but are not limited to, those described in the section entitled "Superwetting electrodes" in the chemistry publication entitled "The prospects of developing a highly energy efficient water electrolyser by eliminating or mitigating bubble effects," published in Sustainable Energy and Fuels, 2021, Vol. 5, p. 1280, which is incorporated herein by reference.

[0314] A feature of the gas handling structure is that it can contain one or more gases within itself due to its affinity for gases, and such gases can persist as separate entities from the bulk gas even when the gas capillary structure is fully immersed in a liquid electrolyte.

[0315] In example embodiments, such gas within a gas handling structure may be an adjacent gas or may become continuous with an adjacent gas. For example, gas handling structures within, adjacent to, or near electrode 120 may contain a gas that is gas 125 or that will be continuous with gas 125. Similarly, gas handling structures within, adjacent to, or near electrode 130 may contain a gas that is gas 135 or that will be continuous with gas 135. In such cases, the gas within the gas handling structure may form part of a larger gas. For example, gas within a gas handling structure that is, or that will be continuous with gas 125, may form part of gas 125. Gas 125 may be in gaseous communication with an external gas conduit (e.g., 127) and / or gas storage system 128. Similarly, gas within the gas handling structure that is or becomes continuous with gas 135 may form part of gas 135. Gas 135 may be in gaseous communication with an external gas conduit (e.g., 137) and / or a gas storage system (e.g., 138).

[0316] Alternatively, the gas within the gas handling structure may itself be bulk gas in independent gaseous communication with an external gas conduit or storage system. For example, gas handling structure within, adjacent to, or near electrode 120 may contain internal gas that is gas 125 and in direct gaseous communication with an external gas conduit (e.g., external gas conduit 127) or storage system (e.g., storage system 128). Similarly, gas handling structure within, adjacent to, or near electrode 130 may contain internal gas that is gas 135 and in direct gaseous communication with an external gas conduit (e.g., external gas conduit 137) or storage system (e.g., storage system 138).

[0317] “Bubble-free” electrode Generate gas at one or more of the electrodes cellAn example feature is the ability to generate bulk gas directly from a liquid electrolyte without forming visible bubbles in the electrolyte. Such "bubble-free" gas generation is different from conventional gas generation, which generates gas in the form of bubbles within a liquid electrolyte. cell These advantages may include greater energy efficiency due to avoiding the energy required to form bubbles, and the ability to keep the electrode surface bubble-free and available for electrochemical reaction. In particular, cracks, fissures, and imperfections on the surface, where bubbles first form and where they are most tenaciously attached yet generally the most active catalytic sites, may remain free and available for catalytic reaction. When the electrode active surface is covered with bubbles, such obstructions can lead to gas generation. cell The energy efficiency of the system may be reduced.

[0318] Therefore, for example, water electrolysis cell In conventional electrolysis, liquid water is electrochemically converted to hydrogen gas at the active surface of the cathode electrode and to oxygen gas at the active surface of the anode electrode. cell In the water electrolysis of the preferred embodiment, however, these gases are produced in the form of bubbles surrounded by a liquid electrolyte. cell In the case where the first electrode 120 and the second electrode 130 are both gas diffusion electrodes, the gas may merge directly with the associated gases 125 and 135, respectively, without forming any visible bubbles. That is, a continuous gas phase pathway may exist between the active surfaces of the electrodes 120 and 130 at the intersecting planar axis and the gases 125 and 135, respectively. Newly formed gas on the electrode active surfaces may merge into this continuous gas phase pathway without ever forming any bubbles.

[0319] Historically, it was only possible to achieve bubble-free gas production at electrodes using gas capillary structures such as porous hydrophobic membranes.

[0320] However, a feature of example embodiments is that bubble-free gas generation may be produced in other ways that do not rely on or require the presence of gas capillary structure microstructures and nanostructures. cell This structure allows for bubble-free gas generation by the electrodes. This can be done in several ways.

[0321] In some examples, the surface of the gas diffusion electrode (e.g., the gas diffusion electrode 120 or the second gas diffusion electrode 130) is cell During operation, the electrode may be covered with only a thin layer of liquid electrolyte. Gas generated at the electrode surface may dissolve in the electrolyte and migrate through the thin layer to the surface, where it may interact with an adjacent gas (first gas 125 or second gas 135). The gas may then transfer to the gas (first gas 125 or second gas 135), thereby avoiding bubble formation.

[0322] In doing so, the gas may move away from the electrode in a manner that does not interfere with the movement of water and liquid phase ions on the surface of the electrode. That is, the water may always have unimpeded access and path to the surface of the electrode, avoiding bubble formation. There may be no multiphase backflow, where gas bubbles moving away from the electrode counteract and counteract the movement of water to the electrode.

[0323] The gas can also be released at very low partial pressures required to nucleate bubbles, thereby avoiding the high voltages required to create excessive partial pressures.

[0324] Incorporating gas handling structures at or near the electrodes can also help create a direct, bubble-free gas-phase pathway from the electrode active surface to the respective gas 125 and / or 135. Such a pathway may be separate and independent from, and do not interfere with, the movement of water and liquid-phase ions on the electrode surface. In such cases, newly formed gas may dissolve in the electrolyte and then coalesce with the low-energy surfaces of the gas handling structures and be removed. Such gas may then migrate further along these low-energy surfaces away from the electrodes to the respective gases 125 and 135 without forming bubbles. This type of bubble-free operation may be facilitated by the capillary pressure of the porous capillary spacer 110, which may inhibit bubble formation by raising the high partial pressure required for bubble nucleation from dissolved gas. That is, in the porous capillary spacer 110, a nucleating bubble not only needs to push itself up, but also push the liquid held therein within the capillary with significant capillary pressure.

[0325] Of course, bubble-free gas generation can also be achieved by incorporating a gas capillary structure, such as a porous hydrophobic membrane, at or near the electrode. In such a case, newly formed gas can be spontaneously drawn from the liquid electrolyte by gas capillary action and through the gas capillary structure before bubbles form, thereby producing a gas phase transport that is separate, independent, and uninterfering from the transport of water and liquid phase ions on the electrode surface.

[0326] Although effective, the use of gas capillary structures at or near the electrodes has the disadvantage that such structures are generally not electrically conductive. Therefore, electrical connections to the electrodes must bypass the gas capillary structures. The resulting need for long electrical connection paths makes them unsuitable for commercial construction. cellWhen multiple layers are stacked, additional electrical resistance is created that accumulates. The additional resistance typically counteracts and negates the benefits of bubble-free operation. This issue is discussed in the section relating to Figure 17 in the science publication entitled "The prospects of developing a highly energy efficient water electrolyser by eliminating or mitigating bubble effects," published in Sustainable Energy and Fuels, 2021, Vol. 5, p. 1280, which is incorporated herein by reference.

[0327] Conversely, this problem does not exist in embodiments that achieve bubble-free operation without the use of gas capillary structures. In such embodiments, electrical connections can be made directly to the (full) surface of the electrode via the shortest possible path. In doing so, the limitations on additional resistance that counteracts the benefits of bubble-free operation can be lifted, allowing the benefits of bubble-free operation to be fully utilized. cell can be significantly more energy efficient.

[0328] Foam-free example embodiments may preferably exhibit greater than 0.5% energy efficiency than their foamed counterparts. In other examples, the improvement in energy efficiency may be greater than 1%, greater than 2%, greater than 5%, greater than 10%, greater than 15%, or greater than 20%.

[0329] Preferred embodiments cell is an "independent pathway" that indicates increased energy efficiency. cell " can be constructed Preferred embodiments cell Many of the features in cell It will be appreciated that the present invention provides separate, independent, non-interfering molecular level pathways for the movement (flow) of gas or liquid phase species within the gas phase. cell is "independent pathway" cell " It can be.

[0330] "Independent Path cell "teeth, cellGas-phase electrochemistry that provides at least one separate and independent pathway for the movement (flow) of each of the individual liquid and gas-phase reactants and products within cell and wherein such pathways do not interfere with or hinder each other. cell is defined as:

[0331] The pathway, in this context, requires sufficient reactants cell If provided externally and sufficient product is available cell When removed externally, it is possible to maintain an electrochemical reaction indefinitely. cell It is defined as a route or set of routes at the molecular level within a molecule.

[0332] This type of flow of separate and independent liquid phase reactants and products is inherently efficient in that they do not interfere with or obstruct one another. cell is an equivalent electrochemical process in which not all of the gas and liquid phase reactant and product streams are separate and independent. cell Such higher energy efficiency can be achieved by utilizing a system in which not all of the gas-phase and liquid-phase reactant and product streams are separate and independent. cell Compared with the electrosynthesis under uniform conditions, cell The voltage (applied between the first and second electrodes) required is lower or the electrical energy cell This can be manifested as a higher voltage being generated (generated between the first and second electrodes).

[0333] Independent pathways cell may utilize all or some of the following features to achieve higher energy efficiency: (1) separate and independent liquid or gas phase molecular level migration into and out of the reaction zone / intersecting planar axis; (2) non-interfering capillary-guided migration along or above the electrodes; (3) cell(4) capillary-induced electrode wettability involving a non-interfering path, (5) capillary-induced electrode wettability involving a non-interfering path created by compression of the electrode against a porous capillary spacer, (6) non-interfering gas phase transport through the gas handling or gas capillary structure, and / or (7) non-interfering gas and liquid phase transport over a bubble-free electrode. Increased energy efficiency can be cumulatively attributed to some or all of these effects.

[0334] In the example embodiment, cell " preferably refers to a similar or equivalent flow in which at least one reactant or product stream intervenes. cell In other examples, the improvement in energy efficiency may be greater than 1%, greater than 2%, greater than 5%, greater than 10%, greater than 15%, or greater than 20%.

[0335] Capillary-related features of porous capillary spacer 110 A further feature of preferred embodiments is capillary action in the porous spacer 110. That is, the porous capillary spacer 110 contains a liquid electrolyte that is held tightly within the porous capillary spacer by capillary forces. For example, the previously mentioned example of a porous capillary spacer 110, a polyethersulfone material filter having an average pore size of 8 μm supplied by Pall Corporation, can draw in a liquid electrolyte, e.g., an aqueous electrolyte, and hold the electrolyte within the material by capillary forces.

[0336] To operate uninterruptedly or continuously for an indefinite period of time, the porous capillary spacer 110 may require sufficient capillary action to keep itself uninterruptedly or continuously filled with the liquid electrolyte 100.

[0337] Such a porous capillary spacer 110 may also need to exhibit other properties, including: (1) Capillary Pressure and "Bubble Point": The capillary pressure, or more specifically, the "bubble point," of the porous capillary spacer 110 may need to be appropriately large (within reason and taking into account other considerations discussed herein). The capillary pressure represents the gas pressure required to force the liquid electrolyte 100 out of the average capillary in the porous capillary spacer 110. The bubble point represents the gas pressure required to force the liquid electrolyte 100 out of the largest capillary in the porous capillary spacer 110. These pressures may need to be high enough to help ensure that small or temporary pressure differences in the gases 125 and 135 cannot force the liquid electrolyte 100 out of or down the porous capillary spacer 110. For example, in the case of a porous capillary spacer of the type shown in FIGS. 1-3, cell Loss of liquid electrolyte within the porous capillary spacer 110 at any point can slow or stop the electrochemical reaction (when there is no liquid electrolyte at any point between the electrodes) and / or lead to gas crossover (when there is no liquid at any point in the spacer to act as a barrier between the gases present). (2) Maximum Column Height: As mentioned above, the porous capillary spacer 110 may be required to indefinitely maintain a column height of liquid electrolyte 100 within itself. This column height is the maximum column height in one example embodiment. cell , so that the porous capillary spacer 110 cell This ensures that all points within the cell The height can be guaranteed only if it is less than or equal to the maximum column height of the porous capillary spacer 110, which is the maximum column height of the liquid electrolyte 100 that can be maintained by the porous capillary spacer 110 if the porous capillary spacer 110 has a hypothetical infinite height. That is, in order for the liquid electrolyte 100 to always be present between the electrodes at all locations of the electrode-spacer-electrode assembly 139, the maximum column height of the liquid electrolyte 100 in the porous capillary spacer 110 must be cell above the highest point, i.e., at the location of the porous capillary spacer cell The height of the example embodiment may need to be equal to or greater than the height of the example embodiment. cellIn the case of a porous capillary spacer 110, the porous capillary spacer 110 and the liquid electrolyte 100 within the spacer may be between gases, such as gases 125 and 135 in FIGS. 1-3. In that case, the liquid electrolyte 100 within the porous capillary spacer 110 may be necessary to prevent gases from, for example, gases 125 in FIGS. 1-3 from crossing and mixing with gases in gas 135, and vice versa. cell In the prior art, this phenomenon is known as "gas crossover" and can lead to loss of energy efficiency, production or consumption of impure gases, and / or safety hazards. The maximum column height must also be greater than the height of the first electrode 120 and the second electrode 130. (3) Flow Rate: The upward flow rate of the liquid electrolyte 100 moving inside the filled porous capillary spacer 110 under the influence of the capillary is: cell It may be necessary to ensure that the porous capillary spacer remains filled with the liquid electrolyte 100 at all times, including during operation. For example, with the structure shown in FIG. 1 or FIG. 2, where the electrochemical reaction consumes water as a reactant, cell Then, the capillary-driven flow rate at all heights within the porous capillary spacer is cell It must be possible to replenish the water consumed when the pump is operating at maximum rate.

[0338] Specific Capillary Characteristics of Porous Capillary Spacer 110 - Capillary Pressure and Bubble Point Capillary pressure is defined as the pressure difference across the meniscus in a capillary; that is, the pressure required to force a liquid electrolyte out of the capillary. The most common mathematical expression for capillary pressure is the Young-Laplace equation:

number

[0339] Using this equation, the capillary pressure for 6M KOH electrolyte for a series of exemplary porous capillary spacers 110, i.e., porous polyethersulfone material filters supplied by Pall Corporation having average pore sizes of 0.45 μm, 1.2 μm, 5 μm, and 8 μm, was calculated to be 1.66 atm (for 0.45 μm average pore size), 1.08 atm (for 1.2 μm average pore size), 0.27 atm (for 5 μm average pore size), and 0.22 atm (for 8 μm average pore size).

[0340] Equation (2) indicates that the larger the pore radius / pore size, the lower the pressure required to displace a liquid within the pores. Therefore, the most important type of capillary pressure in a porous capillary spacer is the "bubble point." This is the pressure required to displace a liquid through the largest pore in the porous capillary spacer. The bubble points of the above series of porous polyethersulfone material filters were measured using a capillary flow porometer and found to be 0.91 atm (for a 0.45 μm average pore size), 0.48 atm (for a 1.2 μm average pore size), 0.13 atm (for a 5 μm average pore size), and 0.11 atm (for an 8 μm average pore size).

[0341] As mentioned above, a high bubble point helps ensure that small or temporary pressure differences in the gas, such as gas 125 or 135 in Figures 1-3, cannot push the liquid electrolyte out or down through the porous capillary spacer. Thus, if the structure shown in Figure 1 cell When 6 M KOH was used as the liquid electrolyte 100 and a porous polyethersulfone material filter having a specified average pore size of about 8 μm was used as the porous capillary spacer 110, cellThe capillary spacer 110 must be designed to ensure that neither gas 125 nor gas 135 has a pressure more than 0.11 atm higher than the pressure of the liquid or other gas during operation (otherwise the liquid electrolyte 100 would be forced out of its largest pores). However, when a porous polyethersulfone material filter with a specified average pore size of 0.45 μm is used as the porous capillary spacer 110, a pressure difference of up to 0.91 atm can be maintained without initiating the extrusion of the liquid electrolyte 100 from the porous capillary spacer 110.

[0342] The above trend in bubble point can be modeled as a power law, with the bubble point for large average pore sizes being 0.5086 × (average pore size) -0.772 From this measurement, it can be expected that a 400 μm average pore size in a porous capillary spacer 110 of polyethersulfone material will produce a bubble point of 0.005 atm (5 mbar), which is cell It is the low pressure difference between gases 125 and 135 that can be considered to provide a threshold above which it is practically difficult to guarantee independence within the gases.

[0343] An average pore size of 400 μm in a porous capillary spacer 110 made of polyethersulfone material corresponds to a capillary pressure of 0.011 atm (11 mbar) by extrapolation of the above trend in capillary pressure.

[0344] Thus, when filled with liquid electrolyte, example embodiments of porous capillary spacer 110 preferably have a capillary pressure greater than 11 mbar. In other examples, porous capillary spacer 110 may have a capillary pressure greater than 15 mbar, greater than 20 mbar, greater than 30 mbar, greater than 50 mbar, greater than 80 mbar, greater than 100 mbar, greater than 500 mbar, greater than 1 bar, or greater than 2 bar.

[0345] Thus, when filled with liquid electrolyte, example embodiments of porous capillary spacer 110 may preferably have a bubble point greater than 5 mbar. In other examples, porous capillary spacer 110 may have a bubble point greater than 10 mbar, greater than 15 mbar, greater than 20 mbar, greater than 50 mbar, greater than 100 mbar, greater than 250 mbar, greater than 500 mbar, greater than 1 bar, or greater than 2 bar.

[0346] Specific Capillary Characteristics of Porous Capillary Spacer 110 - Maximum Column Height Without wishing to be bound by theory, the maximum column height of liquid electrolyte that can be supported by a hypothetical capillary of infinite height can be given by Jurin's law:

number

[0347] As can be seen, Jurin's law dictates that the smaller the pore size and the lower the contact angle between the liquid electrolyte and the porous capillary spacer, the higher the column height of the liquid electrolyte 100 that can be maintained within the porous capillary spacer 110.

[0348] The maximum column heights that could be maintained by the series of porous capillary spacer 110 examples, i.e., porous polyethersulfone material filters with average pore sizes of 0.45 μm, 1.2 μm, 5 μm, and 8 μm supplied by Pall Corporation, were measured. The filters were hydrophilic, exhibiting contact angles of 66.6° with Class II deionized water and 70.3° with 6M KOH alkaline solution. Measurements showed that the polyethersulfone material filter with an average pore size of 8 μm maintained the lowest maximum column heights of the filters, which were 19.6 cm with Class II deionized water and 16.6 cm with 6M KOH. Filters with smaller average pore sizes maintained higher maximum column heights, including much higher maximum column heights.

[0349] Thus, a porous polyethersulfone material filter with an average pore size of about 8 μm has the structure shown in FIG. cell In the example, when porous capillary spacers 110 were used, together with 6M KOH as the liquid electrolyte 100, cell The porous capillary spacer, including the first electrode 120 and the second electrode 130, could be safely extended to a height of approximately 16.4-16.5 cm. That is, the porous capillary spacer could be safely employed as a barrier to gas crossover at heights up to 16.4-16.5 cm. Smaller pore materials provide higher maximum column heights, including much higher maximum column heights. There is no limit on the width of the porous capillary spacer and electrodes, as long as the porous capillary spacer, i.e., the polyethersulfone porous capillary spacer, has access to 6 M KOH at all points along its width.

[0350] As noted in the previous section, an average pore size of about 400 μm in a porous capillary spacer 110 of polyethersulfone material would be expected to produce a bubble point of 0.005 atm (5 mbar), which is indeed cell It is the low pressure differential between gas 125 and gas 135 that can provide a threshold that is difficult to guarantee indefinitely.

[0351] To determine the maximum column height that can accommodate such a 400 μm average pore size, the maximum column height of a polyethersulfone material filter with an average pore size of 8 μm was scaled by the discrepancy factor predicted by Jurin's law. From this measurement, a porous capillary spacer 110 made of polyethersulfone material with an average pore size of approximately 400 μm, packed with 6 M KOH, can be expected to have a maximum column height 0.4 cm above its end 150. This corresponds to a very small capillary effect.

[0352] Thus, in example embodiments, the maximum column height of the liquid electrolyte within the porous capillary spacer 110 may preferably be greater than 0.4 cm. In other examples, the maximum column height of the liquid electrolyte may be greater than 1 cm, greater than 3 cm, greater than 6 cm, greater than 8 cm, greater than 10 cm, greater than 12 cm, greater than 14 cm, greater than 16 cm, greater than 18 cm, greater than 20 cm, greater than 25 cm, greater than 30 cm, greater than 50 cm, or greater than 100 cm.

[0353] Specific Capillary Characteristics of Porous Capillary Spacer 110 - Flow Rate The rate at which the liquid electrolyte flows upwards inside the already filled porous capillary spacer under the influence of capillary action is given by Darcy's law:

number

[0354] In a widely accepted study by L.J. Klinkenberger entitled "The Permeability of Porous Media to Liquids and Gases," American Petroleum Institute, Drilling and Production Practice, pp. 200-213, New York, January 1941, the Poiseuille equation, which describes the flow rate of liquids through porous media, is:

number

[0355] Then, the permeability (k) of a porous material and its porosity (φ) can be expressed as:

number

[0356] therefore,

number

[0357] Furthermore, the pressure difference across the meniscus is given by the Young-Laplace equation:

number

[0358] Substituting into Darcy's equation, we get

number

[0359] For porous capillary spacers 110 containing the above polyethersulfone material filters with pore sizes of 0.45 μm, 1.2 μm, 5 μm, and 8 μm and filled with 6 M KOH as the liquid electrolyte: the cross-sectional area (A) of the porous capillary spacer 110 can be measured using a microscope; The porosity (φ) of the porous capillary spacer 110 can be measured as follows: the empty porous capillary spacer 110 is weighed, then filled with liquid electrolyte and weighed again. The difference provides the weight of the liquid filling the interstitial volume of the porous capillary spacer 110. That weight is converted to volume and then compared to the net volume of the porous capillary spacer measured under a microscope. The mean pore radius (r) of the porous capillary spacer 110 may be measured using a capillary flow porometer. The surface tension of 6M KOH electrolyte at the relevant temperature can be obtained from published data (see the scientific paper by P. Ripoche and M. Rolin in Bull. Soc. Chem. France, Part 1. 1980, Vol. 9-10, pp. 1386-139, which is incorporated herein by reference). The contact angle (θ) of 6M KOH electrolyte with the polyethersulfone material of the porous capillary spacer 110 may be measured using a standard laboratory goniometer instrument. The viscosity (μ) of 6M KOH electrolyte at the relevant temperature can be obtained from published data (see graph 7 in the Caustic Potash Handbook, March 2018, Occidental Chemical Corporation, USA, which is incorporated herein by reference). The height (L) above the reservoir (or above the bottom end of the porous capillary spacer if there is no reservoir) can be measured.

[0360] Therefore, it is possible to model the capillary flow rate in the porous capillary spacer 110 at a particular height using equation (8) along with the tortuosity factor 1 / m, which describes the percentage of pores participating in the flow, determined by comparing the predicted flow rate with the measured flow rate.

[0361] To measure the flow rate of one of the polyethersulfone material filters at a specific height, a 1 cm-wide dry filter sample was cut to the selected length and suspended from a scale capable of measuring the weight change of a suspended object. An absorbent pad was attached to the top of the filter and secured to the scale. The filter and absorbent pad were then wrapped in parafilm to prevent any liquid evaporation during the experiment. The bottom end of the filter was then immersed in a bath of 6 M KOH, allowing the filter to fill by capillary action. Data on weight change over time was collected. From the point at which the filter was fully filled, the data was analyzed for flow rate; after the filter was fully filled, the weight vs. time data became linear. Flow rate was measured as weight change per unit time.

[0362] Figure 5 shows a graph of this measured flow rate (black dots) and modeled flow rate (open squares) for 6M KOH liquid electrolyte at room temperature in porous capillary spacers 110 constructed with porous polyethersulfone material filters having pore sizes of 0.45 μm, 1.2 μm, 5 μm, and 8 μm. The coefficient 1 / m = 1 / 1.7 = 58.8% was found to provide the best fit for all samples tested. As can be seen, the modeled results provide good agreement with the measured results for each of the porous capillary spacers 110 constructed with porous polyethersulfone material filters.

[0363] As noted above, the capillary flow rate within the porous capillary spacer 110 is important insofar as it may need to be sufficient to keep the porous capillary spacer 110 filled with liquid electrolyte 100 indefinitely, including during operation. For example, if the electrochemical reaction consumes water as a reactant, the capillary-driven flow rate may be: cell When operating at maximum rate, it may be necessary to be able to replenish the water consumed. cell may not be able to operate indefinitely.

[0364] However, as can be seen in the graph of Figure 5, the flow rate through the porous capillary spacer 110 generally decreases with increasing height. Thus, the flow rate required by the electrochemical reaction (and external factors such as evaporation) may determine the maximum height of the electrode.

[0365] This can be illustrated by the following example: Zero-gap alkaline water electrolysis with the structure shown in FIG. cell Zero gap that consumes water during electrochemical reactions, such as cell In this case, a total current of 10 A corresponds to a total consumption of 0.056 g of water per minute. 2 size (i.e. cell is a current density of 0.25A / cm 2 ) the porous capillary spacer is 1 cm of the electrode-spacer-electrode assembly 139. 2This means that the electrode must be able to supply 0.056 / 40 = 0.0014 g of water per minute. 2 Including up to.

[0366] Referring to the graph in FIG. 5(d), when a porous polyethersulfone material filter with an average pore size of 8 μm filled with 6M KOH is used as the porous capillary spacer 110, a feed rate of 0.0014 g of water per minute can only be sustained up to a maximum electrode height of about 20 cm. Thus, a 20 cm high electrode-spacer-electrode assembly 139 can be expected to operate indefinitely. cell is 20cm high and 2cm wide (total area 40cm 2 ) Wider assemblies 139 less than 20 cm in height can also operate indefinitely.

[0367] However, when a porous polyethersulfone material filter with an average pore size of 5 μm filled with 6 M KOH is used as the porous capillary spacer 110, a feed rate of 0.0014 g of water per minute can only be sustained indefinitely up to a maximum electrode height of about 15 cm (as shown in FIG. 5(c)). cell The electrodes within the chamber must be no more than 15cm high to function indefinitely.

[0368] Furthermore, when a porous polyethersulfone material filter with an average pore size of 1.5 μm filled with 6 M KOH is used as the porous capillary spacer 110, a feed rate of 0.0014 g of water per minute can only be sustained indefinitely up to a maximum electrode height of about 6 cm (as shown in FIG. 5(d)). cell If it is to operate indefinitely, it can only be about 6 cm.

[0369] Furthermore, when a porous polyethersulfone material filter with an average pore size of 0.45 μm filled with 6 M KOH is used as the porous capillary spacer 110, a feed rate of 0.0014 g of water per minute can only be maintained indefinitely up to a maximum electrode height of approximately 4 cm (as shown in FIG. 5(d)). In that case, the maximum electrode height is approximately 4 cm. Electrodes with heights greater than 4 cm cannot indefinitely maintain the required flow rate of 0.0014 g of water per minute at the maximum electrode height.

[0370] Therefore, the high capillary flow rate in the porous capillary spacer 110 allows cell The effect on the diameter of the high flow porous capillary spacer 110 can potentially be limited. cell This may provide greater freedom in terms of design.

[0371] From a practical industrial point of view, electrodes higher than 8 cm are preferred, therefore a porous capillary spacer 110 capable of providing a flow rate of 0.0014 g of water per minute at heights greater than 8 cm is preferred.

[0372] The average pore size of such a porous capillary spacer 110 can be determined by plotting the maximum height as a function of the average pore size. Such a plot indicates that the average pore size must be greater than 2 μm. That is, a porous capillary spacer 110 capable of providing a flow rate of 0.0014 g of water per minute at a height greater than 8 cm is calculated to have an average pore size greater than 2 μm.

[0373] Thus, preferred embodiments of the porous capillary spacer 110 preferably have an average pore size greater than 2 μm. In another example, the average pore size is less than 400 μm. In another example, the average pore size can be greater than 2 μm and less than 400 μm. In other examples, the average pore size can be greater than 4 μm, greater than 6 μm, greater than 8 μm, greater than 10 μm, greater than 20 μm, or greater than 30 μm. In other examples, the average pore size can be greater than 4 μm and less than 400 μm, greater than 6 μm and less than 400 μm, greater than 8 μm and less than 400 μm, greater than 10 μm and less than 400 μm, greater than 20 μm and less than 400 μm, or greater than 30 μm and less than 400 μm. In other examples, the average pore size of the porous capillary spacer can be about 3 μm, about 4 μm, about 5 μm, about 6 μm, about 7 μm, about 8 μm, about 9 μm, or about 10 μm.

[0374] Note that the above measured and calculated graphs describe the flow rate under the influence of capillary action only at room temperature. Therefore, they do not include the effects of diffusion or osmosis, both of which may contribute to higher flow rates. Furthermore, equation (8) shows a direct relationship with surface tension and contact angle, but an inverse relationship with viscosity. Viscosity typically decreases rapidly with increasing temperature, while surface tension and contact angle show much smaller changes, so flow rates can be much higher at higher temperatures. Therefore, these flow rates are for operation above room temperature, cell can reasonably be considered a minimum value for design purposes.

[0375] Capillary action can affect the porous capillary spacer 110, which has very low ionic resistance and / or very high ionic conductivity. A porous capillary spacer 110 constructed from a polyethersulfone material filter of the type described above had a uniform thickness of approximately 145 μm. Measurements showed that the ionic resistance of such a porous capillary spacer between two closely spaced electrodes, when filled with 6 M KOH electrolyte, was 33-53 mΩ cm at room temperature. 2 These values ​​are 1 / 4 to 1 / 8 of the ionic resistance of conventional commercially available interelectrode membrane separators. cell At a typical operating temperature of 80°C, this is 15-23mΩcm2 decreased to the same extent.

[0376] The low ionic resistance of these polyethersulfone material filters was found to result from their 75-85% porosity and the pore (void) volume being occupied by the highly conductive 6M KOH electrolyte, which is tightly held within the spacer by capillary action. The ionic resistance of a 145 μm thick layer of 6M KOH was only about 22 mΩ cm at room temperature. 2 and approximately 10 mΩ cm at 80°C. 2 Therefore, when drawn into the porous capillary material and held there by capillary forces, the 6M KOH electrolyte imparted a very low ionic resistance to the porous capillary material. The higher the porosity of the porous capillary material, the greater the proportion occupied by 6M KOH, and the lower its overall ionic resistance. Thus, the porous polyethersulfone material filter with the greatest porosity (84.6%) exhibited the lowest ionic resistance when saturated with 6M KOH electrolyte (33 mΩ cm at room temperature). 2 and 15mΩcm at 80℃ 2 ).

[0377] In comparison, Agfa's Zirfon PERL® membranes have much lower porosity and therefore much higher ionic resistance. Chemours' Nafion® 115 and 117 membrane separators are inherently ionically conductive and not porous at all. Their ionic resistance is a function of the polymer structure, which contains ionic groups that facilitate transport through the membrane.

[0378] Therefore, in the example embodiment cell is a conventional zero-gap electrosynthesis or electrical energy cell These improvements may be derived from the capillary action of the porous capillary spacer 110, which takes advantage of the low ionic resistance of the electrolyte.

[0379] In example embodiments, the porous capillary spacer may preferably have a porosity of greater than 60%. In other examples, the porous capillary spacer may have a porosity of greater than 70%, greater than 80%, or greater than 90%.

[0380] The porous capillary spacer 110 of the preferred embodiment filled with liquid electrolyte 100 has a resistivity of 140 mΩcm at room temperature. 2 In another example, the ionic resistance may be less than 270 mΩ cm. 2 Less than 200mΩcm 2 Less than 180mΩcm 2 Less than 160mΩcm 2 Less than or 150mΩcm 2 In another example, the ionic resistance may be less than 130 mΩ cm at room temperature. 2 Less than 120mΩcm 2 Less than 110mΩcm 2 Less than 100mΩcm 2 Less than 90mΩcm 2 Less than 80mΩcm 2 Less than 70mΩcm 2 Less than 60mΩcm 2 Less than 50mΩcm 2 Less than 40mΩcm 2 Less than 30mΩcm 2 It may be less than.

[0381] Capillary action within the porous capillary spacer 110 can lead to very low gas crossover In many electrochemical reactions, it is crucial to minimize the migration of gas associated with one electrode (e.g., first gas 125 in FIGS. 1-3) across the porous capillary spacer to the opposite side of the porous capillary spacer, where it mixes with gas associated with the other electrode (e.g., second gas 135 in FIGS. 1-3), and vice versa. As noted above, this phenomenon is known as "gas crossover," and its occurrence is proportional to cell The energy efficiency of a particular cell It also poses potential safety issues.

[0382] For example, a zero-gap water electrolysis device having the structure shown in FIGS. cell In this case, the hydrogen gas produced at the cathode is preferably kept as free as possible from contamination by the oxygen gas produced at the anode, and vice versa. This is because hydrogen containing >4.6% or hydrogen with >3.8% is an explosive mixture (such electrolysis). cell This is because the normal operating temperature is 80°C.

[0383] Conventional zero-gap water electrolysis cell In such systems, gas is generated as bubbles in the liquid electrolyte (i.e., in the anolyte and catholyte) on either side of the interelectrode separator membrane. In such systems, gas crossover can occur by two possible mechanisms: (A) diffusion of gas dissolved in the liquid electrolyte through the interelectrode separator membrane to the other side (referred to as "diffusion-based crossover") and (B) physical movement of liquid containing gas and bubbles between the two sides (referred to as "cross-permeation-based crossover"). Cross-permeation-based crossover can occur due to transient, fluctuating pressure differentials across the separator, including those resulting from bubble formation and release.

[0384] Commercially available alkaline electrolytic capacitors typically employ Zirfon PERL® interelectrode separators. cell In conventional zero-gap alkaline electrolysis, cross-permeation-based crossover is by far the predominant mechanism. Even with extremely small pressure differences between the two sides (i.e., anolyte and catholyte), cell For example, if the pressure difference between the two sides of a thin Zirfon PERL® membrane can be limited to only 1%, a 200 mA / cm2 flow rate can be achieved with a total pressure of 6 bar. 2When operating at 1000 K, the cross-permeation-based crossover of hydrogen into the oxygen product stream is ∼2%, while the concomitant diffusion-based crossover is only ∼0.3%. This is why Zirfon PERL® separators have relatively small pores, with an average pore size of only ∼0.14 μm. These small pores minimize the mobility of the liquid electrolyte, typically aqueous 6 M KOH, in and through the membrane to minimize gas crossover (as taught by HILee et al., “The Synthesis of a Zirfon PERL®-type Porous Separator with Reduced Gas Crossover for Alkaline Electrolyzer,” Int J. Energy Res. 2020, Vol. 44, pp. 1875-1885). The level of diffusion-based crossover is very low because of the high levels of K in 6 M KOH. + and OH - This is because the ions "salt out" the dissolved gases. That is, 6M KOH has very low solubility for dissolved gases such as hydrogen and oxygen. The diffusivity of dissolved oxygen and hydrogen in 6M KOH is also very low.

[0385] Conversely, commercially available PEM electrolysis cell In the case of Nafion®, a material typically employed by Chemours, it is non-porous. This eliminates cross-permeation crossover as a gas crossover mechanism because cell This is because the deionized water used in PEM electrolysis cannot freely permeate the membrane at all. However, diffusion-based crossover is still possible, and because the combined solubility and diffusivity of gases such as hydrogen and oxygen is about 40-120 times greater in deionized water at 80°C, diffusion-based crossover transports high levels of gas across the membrane. Therefore, commercial PEM electrolysis cell generally have higher gas crossover than commercially available alkaline membranes.

[0386] Example embodiments such as those shown in FIG. cell Alkaline electrolysis cell and PEM electrolysis cell, without any of their drawbacks. Thus, the cross-transmission based cross-over of the example embodiment cell This is essentially impossible in the example embodiment because there is no free liquid electrolyte volume outside the electrodes: their volumes are occupied by gas 125 and 135, respectively. Instead, the liquid electrolyte is supplied from below along the porous capillary spacer 110. cell There is no anolyte or catholyte present in the porous capillary spacer 110, and therefore no liquid electrolyte body that can freely permeate from one side to the other through the porous capillary spacer 110. In fact, it is this feature that allows the use of porous capillary spacers with high porosity.

[0387] Furthermore, in using an electrolyte having a high ion concentration, cell also benefits from the very low solubility and diffusivity of gases such as oxygen and hydrogen in 6M KOH, and therefore the resulting diffusion-based crossover is low.

[0388] Therefore, in the example embodiment cell is comparable to a commercially available alkaline or PEM electrolytic solution under comparable conditions. cell It shows a much lower gas crossover than

[0389] This largely eliminates the constraints imposed by gas crossing on the selection and design of the inter-electrode separator. cell The porous capillary spacer 110 may employ large pore sizes that produce high flow rates within the porous capillary spacer 110 without significant gas crossover. As noted above, the porous capillary spacer 110 of the embodiment preferably has an average pore size greater than 2 μm, while the average pore size for Zirfon PERL® is only 0.14 μm. This is unexpected and contrary to teachings in the field of conventional interelectrode separators (as noted above). However, unique cell By structure, the embodiment cell It is possible.

[0390] Example embodiment cell of cellThe structure not only allows for the use of large average pore sizes in the porous capillary spacer 110, but also leads to very low ionic resistance, as noted in the previous section.

[0391] It also maximizes the mobility of liquid water within the porous capillary spacer. In doing so, it overcomes the problem noted in the background section that conventional inter-electrode separators typically severely limit the mobility of electrolyte within the separator in order to minimize gas crossover. For this reason, zero-gap water electrolysis cell The electrodes within the separator may need to draw water reactants from outside the electrodes, thereby creating a multiphase backflow where liquid water moving towards the electrodes counteracts the gas bubbles moving away from the electrodes. In example embodiments, the porous capillary spacer 110 is specifically adapted to supply the required water and ionic reactants from within the separator, thereby avoiding such multiphase backflow and doing so without significant gas crossover. cell By construction, the porous capillary spacers of the example embodiments are able to avoid multiphase backflow that can occur in conventional zero gap water electrolysis devices, which is the essence of the present invention and its novelty.

[0392] Another advantage of low gas crossover is that it is more efficient than conventional alkaline electrolysis. cell The advantage of this approach is that it allows for successful operation at higher total absolute pressures than would be possible with an equivalent conventional pump, as absolute pressure increases, until a safety limit is reached. cell This is because there may be room for much higher crossover growth than in the case of

[0393] "Benchmark gas intersection" cell is room temperature, atmospheric pressure, fixed 200mA / cm 2 This is the degree of gas crossing after 30 minutes under specific operating conditions.

[0394] In embodiment porous capillary spacer 110, preferably, the liquid electrolyte within the porous capillary spacer prevents or inhibits mixing of first gas 125 with second gas 135 to maintain a benchmark gas crossover of less than 2%. In other examples, the benchmark gas crossover can be less than 1%, less than 0.8%, less than 0.6%, less than 0.4%, less than 0.2%, less than 0.1%, less than 0.05%, or less than 0.01%.

[0395] The capillary action in the porous capillary spacer 110 makes the porous capillary spacer 110 a very good bubble barrier. Some preferred embodiments cell Although the present invention does not have visible bubbles, tiny invisible micro- or nano-bubbles may still be present. In other embodiments, visible bubbles may also be formed. Bubbles are, by definition, non-conductive gaps, and their presence in the inter-electrode spacer increases the electrical resistance (i.e., impedance) between the electrodes, cell Furthermore, over time, an increasing number of bubbles may become increasingly lodged within the spacer, eventually forming a single continuous gas path that bridges or partially bridges the porous capillary spacer. Such bridges typically result in excessively high levels of gas crossover, cell This type of problem can occur with some conventional inter-electrode spacers.

[0396] The capillary action of the porous capillary spacer 110 may encourage the porous capillary spacer 110 to act as a better barrier to gas bubbles, including microbubbles or nanobubbles, especially to microbubbles or nanobubbles, than conventional inter-electrode separators.

[0397] As noted above, bubbles will nucleate inside the porous capillary spacer 110 only if newly formed gas at the electrodes creates a bubble with an internal pressure that overcomes the capillary pressure within the porous capillary spacer 110. This is unlikely to occur in example embodiments because the first electrode 120 and second electrode 130 may be in direct contact with the associated first gases 125 and 135, respectively, and there is no additional capillary pressure to overcome. Therefore, bubble formation may be preferentially directed away from the porous capillary spacer 110 and to electrode locations at or near the interface with the gases 125 or 135. In such cases, the porous capillary spacer 110 may be utilized to achieve zero-gap cell This would be a much more effective bubble barrier than would be the case with a conventional inter-electrode spacer.

[0398] In preferred embodiments, the porous capillary spacer 110 can prevent bubbles greater than 1 μm in diameter from being transported between the electrodes. In other examples, it can prevent bubbles greater than 2 μm in diameter, greater than 5 μm in diameter, greater than 10 μm in diameter, greater than 25 μm in diameter, greater than 50 μm in diameter, or greater than 100 μm in diameter.

[0399] The capillary action in the porous capillary spacer 110 causes the “dry cell " structure can be advantageous. The capillary action of the porous spacer and its ability to draw in and retain liquid electrolyte while the external environment is dry and liquid-free allows the use of the example embodiment. cell The interelectrode spacer is typically a so-called "dry" conductive material. cell At the same time, the example embodiment cell The dry electrolyte can also take advantage of the liquid electrolyte, which can be much more conductive than solid-state conductive materials. cell The advantages of this structure can be combined with those of a liquid electrolyte structure while avoiding the disadvantages of each. cell is usually a zero-gap electrochemical or electrical energy cell This may avoid the need for external engineering systems that may be required for management, including active management of the

[0400] Capillary action in the porous capillary spacer 110 may enable the use of expensive / exotic / rare electrolytes In a further embodiment, electrosynthesis or electrical energy synthesis employs a class of liquid electrolytes that are versatile and have useful properties for promoting electrochemical reactions. cell Such electrolytes may be expensive, rare, and / or exotic, and may be, by way of example only, ionic liquids. An example embodiment employing such a liquid electrolyte is cell This may be practically feasible due to the small amount of electrolyte required in the porous capillary spacer and reservoir. cell may enable the industrialization of electrochemical reactions that have not previously been commercially viable.

[0401] Electrosynthesis or Electrical Energy cell How it works In another embodiment, electrosynthesis or electrical energy for carrying out electrochemical reactions cellA method of operation of the present invention is provided. The method includes filling a porous capillary spacer 110 with a liquid electrolyte 100 and contacting the liquid electrolyte 100 with a first electrode 120, e.g., a first gas diffusion electrode, and a second electrode 130, e.g., a second gas diffusion electrode. In another alternative, the method includes transporting the liquid electrolyte 100 along the porous capillary spacer 110 from a reservoir 140 by at least capillary action, and contacting the liquid electrolyte 100, after being transported along the porous capillary spacer 110, with the first gas diffusion electrode 120 and the second electrode 130, which may also be a gas diffusion electrode. In another example, the method includes filling the porous capillary spacer 110 with the liquid electrolyte 100 from the reservoir 140 by at least capillary action. In another example, the method includes filling the porous capillary spacer 110 with liquid electrolyte 100 before the end 150 of the porous capillary spacer 110 is positioned within the reservoir 140. In another example, the method includes maintaining the porous capillary spacer 110 filled with liquid electrolyte 100 during operation. In another example, the method includes maintaining the porous capillary spacer 110 filled with liquid electrolyte 100 during operation by migration of the liquid electrolyte 100 from the reservoir 140 under capillary / diffusion / osmosis. In another example, the method includes maintaining the porous capillary spacer 110 filled with liquid electrolyte 100 during operation by migration of the liquid electrolyte 100 from the reservoir 140 in a thin film upward along the electrode surfaces 120 and / or 130. In another example, the method includes: cell 10 is electrosynthetic cell and the electrochemical reaction is cell Electrosynthesis away from 10 cell In another example, the method includes maintaining the porous capillary spacer 110 filled with the liquid electrolyte 100 due to vapor in the gases 125 and / or 135 condensing in or vaporizing from the liquid electrolyte 100 in the porous capillary spacer 110 during operation. cell 10 is electrical energy cell and the electrochemical reaction is cellIn another example, the method includes, during operation, generating power that can be used to provide work external to the reactor. cell External supply / replenishment and / or products cell and removing the first gas, the second gas, and / or the reservoir to the outside, where the transfer occurs within sealed (liquid-tight and / or gas-tight) external conduits and housings separately connected to each of the first gas, second gas, and / or reservoir.

[0402] In one example, the porous capillary spacer draws in the liquid electrolyte by capillary action and maintains a column height of the liquid electrolyte within the porous capillary spacer. In another example, the maximum column height of the liquid electrolyte is at least equal to or exceeds the height of the first gas diffusion electrode. In another example, the maximum column height of the liquid electrolyte is cell The top and cell In another example, the electrodes draw a thin film of liquid electrolyte along or above their surfaces. In another example, the liquid electrolyte in the porous capillary spacer is replenished / maintained by vapor of the liquid present in the gas phase pathway condensing in or evaporating from the liquid electrolyte in the porous capillary spacer.

[0403] Preferably, during the electrochemical reaction, the liquid electrolyte within the porous capillary spacer promotes the migration of one or more liquid phase materials along the length of the porous capillary spacer. Alternatively, during the electrochemical reaction, the liquid electrolyte promotes the migration of one or more liquid phase materials along the surface of the electrode. Also preferably, the migration of one or more liquid phase materials along the length of the porous capillary spacer is under the control of liquid capillary action, diffusion, and / or osmosis. In another example, the electrochemical reaction is carried out by electrosynthesis or electrical energy. cell In yet another example, the movement of liquid phase material off the intersecting planar axis is self-regulated by the composition of the liquid electrolyte in the reservoir.

[0404] Preferably, the migration paths of liquid and vapor phase materials into and out of the intersecting planar axis are differently directed and distinct. In another example, liquid capillary, diffusion, and / or osmosis act within the porous capillary spacer to (i) constantly replenish one or more liquid phase materials consumed within the liquid electrolyte, or (ii) constantly remove one or more liquid phase materials produced within the liquid electrolyte. In another example, this is achieved by liquid capillary movement along the electrode surface that does not interfere with the vapor phase pathway.

[0405] For example, in the preferred embodiment cell PEM fuel cell In another example, the need for a gas humidification system, along with all the associated engineering components and electronic control circuitry, typically required in a preferred embodiment may be avoided. cell may avoid the need for a liquid electrolyte circulation system that may be required in a water electrolysis device, along with all the associated pipes, pumps, and other engineering and electronic components.

[0406] In another example, vapor present in the gas condenses in or vaporizes from the liquid electrolyte in the porous capillary spacer to (i) continuously replenish one or more liquid phase materials consumed within the liquid electrolyte, or (ii) continuously remove one or more liquid phase materials produced within the liquid electrolyte, which in another example is achieved by a non-interfering vapor phase pathway.

[0407] Permeation chamber configuration that amplifies the maximum column height and flow rate of liquid electrolyte in a porous capillary spacer and allows automation of its operation If the capillary action of the porous capillary spacer 110 provides an insufficient maximum column height and / or flow rate of the liquid electrolyte 100 in the porous capillary spacer 110, the reservoir 140 and porous capillary spacer 110 may be configured as a permeation system to enhance the maximum column height and / or flow rate. Figure 6 shows an example of such an alternative permeation configuration of the reservoir 141.

[0408] The reservoir 141 may be confined, and preferably sealed, within a fixed-volume cavity within which the porous capillary spacer 110 is located, as shown in FIG. 6 . The reservoir 141 may have a membrane 145 sealed across it, thereby selectively dividing the reservoir 141 into two fixed, confined volumes: a first volume 142 and a second volume 143. The membrane 145 may be permeable to water but not ions; i.e., the membrane 145 may be a “semi-permeable” membrane of the type common in osmotic systems. The porous capillary spacer 110 may be located within, immersed in, or otherwise communicate with the liquid electrolyte 100 (i.e., first liquid) contained in the first volume 142, while the second volume 143 on the opposite side of the membrane 145 contains, for example, pure water (i.e., second liquid 146). That is, the porous capillary spacer 110 may be located within a first volume 142, the first liquid may be the liquid electrolyte 100, and the second liquid 146 may be different from the first liquid.

[0409] Such a configuration can create an osmotic pressure that is transmitted from the second volume 143 through the semi-permeable membrane 145 to the first volume 142. The osmotic pressure can drive the liquid electrolyte 100 up the porous capillary spacer 110 more than would be possible due solely to capillary action in the porous capillary spacer 110. The osmotic pressure can also amplify the rate at which the liquid electrolyte 100 and its components can flow upward along the porous capillary spacer 110.

[0410] The maximum column height of liquid electrolyte 100 and its flow rate within porous capillary spacer 110 due to osmotic effects may typically depend on the composition of liquid electrolyte 100 relative to pure water (i.e., second liquid 146) and the total amount of liquid electrolyte 100 relative to the total amount of pure water 146. That is, by adjusting the chamber size of volume 142 and the chamber size of volume 143 relative to the volume of liquid electrolyte 100 in porous capillary spacer 110, and taking into account the composition of electrolyte 100 relative to pure water (i.e., second liquid 146), it may be possible to control and adjust the maximum additional column height and additional flow rate of liquid electrolyte 100 within porous capillary spacer 110 imparted by the osmotic pressure created.

[0411] Therefore, an alternative embodiment reservoir configuration 141 is provided that may employ the osmotic effect to help amplify the maximum column height and flow rate of the liquid electrolyte 100 within the porous capillary spacer 110 .

[0412] This configuration allows water to be the sole product produced by the electrochemical reaction or the sole reactant consumed by the electrochemical reaction. cell This also aids in automating the example embodiment. That is, the vessel of the structure 141 can be used to generate hydrogen-oxygen fuel in the example embodiment. cell (Water is the only reaction product) or water electrolysis of the example embodiment cell It can also be employed to automate the removal or addition of water, respectively (where water is the only reactant consumed).

[0413] Such an example embodiment cell In the example embodiment, an osmotic equilibrium may exist between the pure water (i.e., second liquid 146) in the second volume 143 and the liquid electrolyte 100 in the first volume 142 and the porous capillary spacer 110. cell The formation of additional new water due to electrochemical reactions within the first volume 142 may dilute the liquid electrolyte 100. This may shift the equilibrium, causing additional pure water to migrate from the first volume 142 through the semi-permeable membrane 145 into the second volume 143 until the equilibrium is restored. The additional pure water entering the second volume 143 may be removed by periodically opening a valve between the second volume 143 and a pure water pipe attached to the second volume 143. The valve may be configured to automatically open whenever the amount of pure water in the second volume 143 exceeds a certain amount. In this manner, tank management may be automated, thereby allowing the hydrogen-oxygen fuel of the example embodiment to be pumped without human intervention. cell Water produced as the sole product within the reactor can be automatically removed via a tank 141 that provides a permeation system.

[0414] Water electrolysis in one embodiment cellIn the electrochemical reaction, water is the sole reactant consumed by the reaction. The effect of consuming water is to make the liquid electrolyte 100 more concentrated, shifting the equilibrium, but in the opposite direction. That is, pure water can be induced to flow from the second volume 143 through the semi-permeable membrane 145 to the first volume 142 and the porous capillary spacer 110 until equilibrium is restored. Additional pure water flowing out of the second volume 143 can be replenished by periodically opening a valve between the second volume 143 and a pure water pipe attached to the second volume 143. The valve can be configured to automatically open whenever the amount of pure water in the second volume 143 falls below a certain amount. In this manner, cell management can be automated, whereby, without human intervention, water consumed as the sole reactant in the example embodiment water electrolysis device can be automatically replenished via the cell 141 providing the osmotic system.

[0415] Examples of porous capillary spacers and liquid electrolytes While the above examples employed porous capillary spacers 110 comprised of porous polyethersulfone material filters having average pore sizes of 0.45 μm, 1.2 μm, 5 μm, and 8 μm supplied by Pall Corporation, it should be understood that a wide range of other porous thin materials capable of incorporating liquid electrolyte therein may be employed as porous capillary spacers 110, including, but not limited to: Included are thin films of various types, combinations of types, or hybrids of different types, including, but not limited to, PVDF, PTFE, tetrafluoroethylene, various types of fluorinated polymers, polyimides, polyamides, nylons, various types of nitrogen-containing materials, glass fibers, various types of silicon-containing materials, polyvinyl chloride, various types of chloride-containing polymers, cellulose acetate, cellulose nitrate, cellophane, ethyl cellulose, various types of cellulose-containing materials, polycarbonates, various types of carbonate-containing materials, polyethersulfones, polysulfones, polyphenylsulfones, various types of sulfone-containing materials, polyphenylene sulfide, various types of sulfide-containing materials, polypropylene, polyethylene, polyolefins, various types of olefin-containing materials, asbestos, titanium-based ceramics, zirconium-based ceramics, various types of ceramic materials, polyvinyl chloride, various types of vinyl-based materials, various types of rubbers, various types of porous battery separators, and various types of clays.

[0416] The above example uses 6M KOH solution as the liquid electrolyte 100, but is not limited thereto. - Not limited to 0.001 to 14M Na + , K. + , Ca 2+ , Mg 2+ , O.H. - , SO4 2- , HSO4 - , Cl - , NO3 - , ClO4 - , phosphate (HPO4 - including carbonate (HCO3 - PF6 - , BF4 - , (CF3SO2)2N - or polyelectrolytes, including polymers with functional groups, such as, but not limited to, polystyrene sulfonic acid, DNA, polypeptides, and the like, water containing one or more dissolved ions; - a non-aqueous liquid containing a solute, for example but not limited to, a propylene carbonate liquid, a dimethoxyethane liquid, or a propionitrile liquid containing a solute, for example but not limited to, LiClO4 or Bu4NPF6; Conductive liquids, for example and without limitation, room temperature molten salts or ionic liquids composed of alkyl-substituted ammonium, imidazolium, or pyridinium cations paired with suitable anions; - Gels that are conductive and can act as electrolytes It should be understood that a wide variety of other liquids or gels may be employed as the electrolyte 100, including

[0417] Particularly suitable are electrolytes that are versatile or useful in facilitating electrochemical reactions, but may be expensive and / or rare. The very small amounts of electrolyte that may be present in the thin, porous capillary spacer (and reservoir) allow for the use of the preferred embodiment. cell is electrosynthesis or electrical energy cell This could enable widespread use of such electrolytes in various applications. Examples in this regard include, but are not limited to, ionic liquids, which have often been found to be particularly useful, but which currently are not feasible for practical use. Despite their great technological versatility and utility in electrochemical reactions, many ionic liquids have to date been restricted from use in electrosynthesis or electrical energy synthesis due to their high cost and scarce availability. cell It has not been widely used as an electrolyte in electrolytes.

[0418] Simple engineering design cell Examples The following promotes a variety of different electrochemical reactions and has the structure shown in Figure 1. cell Examples are provided. To provide a reproducible illustration, the engineering design is simple and easily reproduced. cell This design is an example of an embodiment. cell It is one of many possible designs for cell It is understood that the examples are within the scope of the present invention.

[0419] Figures 5 and 6 cell Fabrication of an Example: An electrode-spacer-electrode assembly 139 was prepared by mounting the assembly inside a specially cut plastic laminate that hardens after heat treatment by passing it through a stationery store laminator.

[0420] As shown in FIG. 7 , a laser cutter was used to cut a clear plastic laminate to the design of the cutout 500. The cutout 500 incorporated two 3.2 cm × 3.2 cm electrode windows 501 and two 5 cm wide × 2 cm high cell windows 502. The porous capillary spacer 110 was cut to dimensions of 6.5 × 6.5 cm. A 3.25 cm × 3.25 cm gas-porous fine-mesh metal mesh current carrier 320 was incorporated into or onto a 3.3 × 3.3 cm first electrode 120, which was incorporated as a gas diffusion electrode, to form an electrode-current carrier assembly 420. A 3.25 × 3.25 cm second gas-porous fine-mesh metal mesh current carrier 330 was incorporated into or onto a 3.3 × 3.3 cm second electrode 130, which was incorporated as a gas diffusion electrode, to form a second electrode-current carrier assembly 430.

[0421] Cutout 500 was a transparent laminate that was folded in two, as shown as folded cutout 510. Within the fold, porous capillary spacer 110 was inserted with electrode-current carrier assembly 420 on the front side and electrode-current carrier assembly 430 on the back side. Electrode-current carrier assembly 420 and electrode-current carrier assembly 430 each had their current carriers 320 and 330, respectively, facing outward, away from porous capillary spacer 110. Electrode-current carrier assembly 420 and electrode-current carrier assembly 430 each had their first electrode 120 and second electrode 130, respectively, facing inward, in direct contact with porous capillary spacer 110. The porous capillary spacer was positioned to cover both the entire window 501 and the entire window 502. Electrode-current carrier assemblies 420 and 430 were positioned so that they only covered window 501 on each side. The assembly so produced was then passed through a stationery store laminator to adhere and cure the two inner surfaces of the folded cutout 510 to one another, thereby forming the current carrier-electrode-spacer-electrode-current carrier assembly 520.

[0422] An exploded view of assembly 520 is shown in the lower right of Figure 7, showing how the components inside assembly 520 are aligned with the windows 501 and 502 on each side. The front face 511 of the stack formed the front of assembly 520. The rear face 512 of the stack formed the rear of assembly 520. A porous capillary spacer 110 was positioned between the front face 511 and rear face 512 of the stack. The porous capillary spacer 110 was aligned with and covered both the upper and lower windows on each of the front face 511 and rear face 512 of the stack (shown as dashed lines on the porous capillary spacer 110 in the lower right of Figure 7). An electrode-current carrier assembly 430 was positioned on the front face of the porous capillary spacer 110, with its electrode side facing the porous capillary spacer 110 and its current carrier side facing the stack cover on the front face 511. Assembly 430 was aligned with the top window on the front surface 511 of the stack. The current carrier 330 in electrode-current carrier assembly 430 covered the entire top window on the front surface 511 of the stack. On the rear surface of porous capillary spacer 110 was positioned electrode-current carrier assembly 420, with its electrode side facing porous capillary spacer 110 and its current carrier side 320 facing rear surface 512 of the stack. Assembly 420 was aligned with the top window at 512. The current carrier covered the entire top window on rear surface 512 of the stack at 420.

[0423] As can be seen from FIG. 7 , the height of the porous capillary spacer 110 was at least equal to or greater than the height of the first electrode 120 and the height of the second electrode 130. Similarly, the surface area of ​​the porous capillary spacer 110 overlaps and is at least equal to or greater than the surface area of ​​the first electrode 120 and the surface area of ​​the second electrode 130. Therefore, the maximum column height of the liquid electrolyte 100 within the porous capillary spacer 110 exceeds the height of the first electrode 120 and the height of the second electrode 130. Preferably, the maximum column height of the liquid electrolyte is at least equal to or greater than the height of the first gas diffusion electrode. The maximum column height is: cellSimilarly, this allows the surface area covered by the liquid electrolyte 100 in the porous capillary spacer 110 to be at least equal to or greater than the surface area of ​​the first electrode 120 facing the porous capillary spacer and the surface area of ​​the second electrode 130 facing the porous capillary spacer.

[0424] FIG. 8 shows a current carrier-electrode-spacer-electrode-current carrier assembly 520 assembled using the cell An exploded view of the above is shown.

[0425] Two cell The halves 600 were machined from stainless steel. cell 600 is half cell It contained a stepped window 610 connected to a pipe 611 exiting the top of 600. cell 600 also contained a grooved rectangular well 615 measuring 5 cm wide x 2 cm high x 1 cm deep. cell It was connected to two pipes 621 coming out of the top of 600.

[0426] Conductive metal flow fields 620, 630 are formed on each half cell The flow fields 620, 630 were placed in specially designed grooves in the upper window 610 of the catalyst carrier 600. Each flow field 620, 630 contained a porous central area measuring 3.2 cm x 3.2 cm. Various designs can be used for the porous section of the flow fields 620, 630. In the example shown in Figure 8, the flow fields 620, 630 are closely packed with cylindrical voids running from front to back. Where possible, electrodes 120 and 130 were welded to their respective current carriers 320 and 330 and / or their respective flow fields 620 and 630 before incorporating the catalyst.

[0427] As shown in FIG. 8, the assembly 520 is then configured such that current carriers external to the assembly 520 are cell In intimate contact with the conductive flow fields 620, 630 at 600, cell It was narrowly spaced 600 meters apart. cell600 are securely screwed together using non-conductive polymer bolts that pass through seven edge-arranged holes that run the entire thickness of the assembly. cell 700, which is shown in the lower right of FIG. 8 in perspective (left) and cross-sectional (right) views.

[0428] The liquid electrolyte is then cell Half of each within 700 cell It flows down one of the pipes 621 on 600 and cell 600 fills the reservoir cavities 615 in the assembly 520. The liquid in those reservoirs 615 passes through windows 502 on either side of the assembly 520 and is drawn up between the first electrode 120 and the second electrode 130 in the porous capillary spacer 110 if both the first electrode 120 and the second electrode 130 are gas diffusion electrodes.

[0429] A conductive bus bar 640 is provided on each half to provide electrical connection to the electrodes 120, 130. cell The electrical currents flowed through a window 610 in the housing 600 and were compressed against the conductive flow fields 620, 630. These were then compressed against the conductive current carriers 320, 330 embedded in the first electrode 120 and second electrode 130, respectively. Compression was provided by two bolts that were twisted against the busbar to deliver the desired electrode compression. In some embodiments, the busbar 640 was replaced with a stainless steel bolt threaded through the housing 600 at the same location (i.e., 610), which was twisted to provide the desired electrode compression. The applied pressure delivered by twisting the bolt can be checked using a pressure-sensitive membrane. The two ends 641, 642 of the busbar 640 served as connection points to an external electrical circuit. The busbar 640 (or the stainless steel bolts) were connected to each half cell The flow field 320, 330 at 600 is constructed to allow for flow between the flow field 320, 330 and the pipe 611.

[0430] cell The gas connection to cellThe gas flow was conducted through pipes 611 above each of the electrodes 600. The gas flowing in and out of these pipes 611 was connected to the first electrode 120 and the second electrode 130 via flow fields 620, 630 and gas porous current carriers 320, 330, respectively.

[0431] the above cell simply removes the polymer between the voids 501 and 502 in the laminate 500 (see FIG. 7), cell 600 (see FIG. 8) can be adapted to have the structure shown in FIG. 2 by removing the metal barrier between chambers 615 and 610 and then ensuring that the liquid in reservoir 615 has a high enough level to touch at least one of electrodes 120 or 130.

[0432] the above cell 5 simply cuts the voids 502 into the laminate 500 (see FIG. 7) and cell 600 (see FIG. 8) can also be adapted to have the structure shown in FIG. 3 by not cutting chamber 615. cell There is no tank inside.

[0433] Multi-cell laminate example Referring to FIG. 9, at least a first electrosynthesis or electrical energy cell and second electrosynthesis or electrical energy cell Providing multiple individual cell 700 is laminated and cell One end 642 of the external bus bar 640 is connected to the cell 640 of the multi-cell stack. cell 9 shows such a stack 750, which may be, for example, eight individual cell 700 (i.e., the first cell , second cell , third cell , 4th cell , 5th cell , 6th cell , 7th cell, 8th cell ) and cell There are seven electrical connections 710 between them. Each electrical connection 710 cell The end 642 of the bus bar 640 of 700 is cell 9. This involved contacting the ends 641 of the bus bars 640 of 700. An external electrical circuit was then connected across the open end 642 on the left side of FIG. 9 and the open end 641 on the right side of FIG.

[0434] Many conventional zero-gap electrochemistries cell Advantages of this multi-cell configuration compared to include, but are not limited to:

[0435] (1) Elimination of shunt current: "Shunt" current (also called "parasitic" or "bypass" current) is a current that is generated by electrochemical cell This can be a problem in stacks. cell All or several of the laminates cell This occurs when connecting the electrodes to the stack and a common conductive liquid electrolyte is present between them. The presence of such a common electrolyte can cause unwanted currents to flow between the different individual electrodes in the stack. cell Such "shunt" currents interfere with the desired current path, resulting in significant efficiency losses as well as corrosion and non-uniformity. cell The shunt current can cause problems with the performance of each individual cell but, cell Any other individual cell This can only be totally avoided by ensuring that there is no conductive or physical contact with the liquid electrolyte.

[0436] For example cell The stack 750 meets this requirement: at least a first electrochemical or electrical energy cell and second electrosynthesis or electrical energy cell Each individual provides cell 700 has its own individual liquid electrolyte 100 in its own porous capillary spacer 110 and its own reservoir 140, and each liquid electrolyte 100 cellAny other individual components within the stack 750 cell There is no physical contact with the liquid electrolyte 100 in 700. cell All or more of the layers in the stack 750 cell 700 and the common conductive liquid electrolyte that is common to them is cell Not present in stack 750.

[0437] (2) A single water supply / removal system can be used to maintain multiple individual tanks without splitting the water flow, and the system can be automated: This allows multiple individual tanks to be maintained without splitting the water flow through a single common water supply or removal system. cell This raises the question of whether it is possible and practical to automate the maintenance of multiple individual vessels within stack 750. That is, is it feasible to manage multiple individual vessels from a single water supply or removal system and still avoid split currents? (As noted in FIG. 6 and the associated text, the use of Type 141 vessels allows water to be the sole product of an electrochemical reaction (e.g., hydrogen-oxygen fuel). cell ), or is the sole reactant that is consumed (e.g., in water electrolysis) cell ) of individual embodiments cell (It may be possible to automate bath maintenance in

[0438] To answer this question, Figure 10 shows an example of four individual cell Consisting of 700 cell Four vessels of type 141 are shown schematically and exemplarily in stack 750. Within each vessel, a second volume 143 containing pure water 146 has a pressure or volume sensitive valve 148 connecting them to a single common water supply or removal pipe 147 containing pure water 146. In operation, the valves open and close automatically individually to allow for the flow of (hydrogen-oxygen fuel) cell The water produced (in the electrolysis system) can be removed or the water consumed (in the electrolysis system) can be replenished. cell The second liquid 146, in this example pure water, cellThe two valves may communicate with each other through a common supply or removal pipe 147 connected to the second volume 143 of the first valve. Since the valves operate independently, it is obvious that there exists the possibility that the two valves may be open simultaneously at any time. In such a case, the two individual valves cell However, the pure water in the pipe 147 and the pure water in the two temporarily opened second volumes 143 are pure water 146, which is non-conductive, so no split flow is possible. That is, the connection between the individual tanks and the common water supply / removal system is via the non-conductive pure water, so no split flow is possible.

[0439] Thus, in the example embodiment having a type 141 tank: cell teeth cell The tanks may be arranged in a stack 750, with each tank connected to a single common water supply / removal system 147 without the possibility of splitting. cell All of the serious problems that can be caused to the laminate 750 can be completely eliminated.

[0440] (3) Within the laminate cell Eliminates number constraints: No shunt currents allow for feasible integration into a single high voltage stack cell Many conventional electrochemical cell That is, the example embodiment can eliminate the constraints that exist in the stack. cell The number can be adjusted to the voltage output of the most efficient and / or lowest cost power supply available. This is currently the case for many conventional electrochemical devices that often require the use of custom power supplies which can be relatively inefficient and costly. cell is not possible.

[0441] (4) Gas supply or removal can be done directly using a single common gas manifold: cell Another feature of the laminate 750 is that cell Within the stack 750 cell700 to a single common gas manifold, thereby allowing the gases in gas manifold 125 to be distributed through a single external fitting. cell Supply to stack 750 or cell can be removed from the stack 750. cell Each in the stack 750 cell Each gas 135 in 700 may be connected to a single common gas manifold, allowing gases in gas 135 to be delivered through a single external fitting. cell Supply to stack 750 or cell The stack 750 can be removed. Furthermore, by using a single gas manifold for each of the gases 125, 135, the gases within these manifolds can be pressurized, effectively removing any gases within the stack, including the reservoir. cell The gases 125, 135 may be pressurized together (if an aperture such as 149 in FIG. 1 is present) to the same pressure or to different pressures below the bubble point of the electrolyte-infused porous capillary spacer 110 during operation. Furthermore, gases supplied or removed through such a single gas manifold may be pressurized to different pressures. cell This allows for direct vapor-phase contact with the intersecting planar axes of the gases, improving control and allowing for self-adjustment of the control.

[0442] (5) Eliminates the need for foam management systems: many conventional electrochemical cell In such a case, gas is produced in the form of bubbles. cell Many have foam management systems. For example, many cell The foam management system constantly pumps and circulates electrolyte across the electrodes to remove bubbles as they form. cell Within the laminate cell As the number increases, it can become increasingly complex and expensive (e.g., because of the need to avoid transient pressure differences at all points in such a system, even if large amounts of bubbles must be collected and separated in a gas-liquid separator). cellThe stack may avoid the need for a foam management system and all the complications that it brings, as any gas produced travels directly to the gases 125, 135 along the gas phase path 200.

[0443] Examples of various reactions cell The following examples provide a more detailed discussion of the embodiments. The examples are for illustrative purposes only and are not intended to limit the scope of the invention.

[0444] Materials: The following materials were employed (suppliers): porous polyethersulfone material filters (0.03 μm, 0.45 μm, 1.2 μm, 5 μm, and 8 μm pore sizes; supplied by Pall Corporation), carbon black (AkzoNobel), 10% Pt on Vulcan XC-72 (Premetek Co. #P10A100), 20% Pt-Pd on Vulcan XC-72 (Premetek Co. #P13A200), nanoparticle Ni (average diameter 20 nm) (American Elements; SDC Materials, Inc. Tampa, AZ), PTFE dispersion (as binder or gas handling structure) (60 wt% dispersion in alcohol / HO; Sigma-Aldrich #665800), PTFE fine powder (Alfa Aesar, A12613, 15-25 μm particle size), Nafion® dispersion (5% in alcohol / water; Sigma-Aldrich #527084), Sigracet™ carbon paper (Fuel Cell Store, 29BC), KOH 90%, flakes (Sigma-Aldrich #484016), H2SO4 95-98% (Sigma-Aldrich #320501), Ni mesh, 200 LPI (Century Woven, Beijing) (cleaned with isopropyl alcohol before use), Ni foam (Goodfellows; TMax Battery Equipment, 1 mm thick, 97% porosity, density: 350 ± 20 g / m 2), a polypropylene-based Preveil™ expanded PTFE (ePTFE) Gortex membrane with an average pore size of 0.2 μm manufactured by General Electric Energy, and Ti mesh (Goodfellows).

[0445] 1. To produce ammonia from nitrogen and hydrogen, ammonia is decomposed into hydrogen and nitrogen, and NO X Electrosynthetic nitrogen reduction for cleanup cell Example of ammonia fuel for generating electricity from ammonia cell Examples The porous capillary spacer 110 is a porous polyethersulfone material filter having an average pore size of 1.2 μm, and the nitrogen reduction of the embodiment having the structure shown in FIGS. cell The liquid electrolyte 100 was the ionic liquid trihexyl(tetradecyl)phosphonium tris(pentafluoroethyl)trifluorophosphate ([P6,6,6,14][eFAP]) or the ionic liquid 1-butyl-1-methylpyrrolidinium tris(pentafluoroethyl)trifluorophosphate ([C4mpyr][eFAP]). The ionic liquid electrolyte 100 was acidified. The electrode-current carrier assembly 420 included an Fe catalyst deposited on a stainless steel cloth, as described in Zhou, F. et al. (2017), Electro-Synthesis of Ammonia from Nitrogen at Ambient Temperature and Pressure in Ionic Liquids, Energy & Environmental Science, 10(12), 2516-2520, which is incorporated herein by reference. The stainless steel cloth served as the current carrier 320. The counter electrode 130 comprised a Sgracet™ carbon paper substrate onto which a thin catalyst layer of 10% Pt on Vulcan XC-72 with PTFE (from a PTFE dispersion) as a binder had been sprayed on the micro-hole side. The electrode 130 was compressed against a Ni mesh that served as the current carrier 330, thereby providing an electrode-current carrier assembly 430. cellThe inner flow fields 620 and 630 were Ni foam. The conductive busbar 640 was Ni coated stainless steel. The nitrogen flow was cell passed through. cell While in operation, nitrogen cell During the passage of cell The gases in the gas 125 coming out of the reactor also contained ammonia and hydrogen. Pure hydrogen was released as gas 135. cell In an alternative embodiment, oxygen or air-oxygen is introduced as gas 135. cell (with a suitable catalyst at the associated electrode). The ammonia produced was removed from the exiting gas 125 by means known in the art.

[0446] cell The very small total amount of liquid electrolyte required in the synthesis of ionic liquids has made it practically possible to use ionic liquids as electrolytes. cell Therefore, it is generally not feasible to use ionic liquids as electrolytes due to scarcity and high cost.

[0447] In an alternative embodiment, cell The action of ammonia can be reversed. cell and decomposes it into hydrogen and nitrogen, i.e., produces hydrogen and nitrogen. Using the same catalyst and a suitable applied voltage, cell produced hydrogen from ammonia.

[0448] In an alternative embodiment, cell No X Can be used for cleanup, i.e. NO X was used as a reactant, and NO X The contained gas is removed. In an alternative embodiment, cell The process can be reversed, with ammonia as one of the gases. cell oxygen or air-oxygen as other gases cell was introduced to cell generates electricity.

[0449] 2. Electrosynthetic chlor-alkali to produce chlorine, hydrogen, and caustic from saltwater cell Examples cell 1-2 , an example embodiment of a chlor-alkali for producing chlorine, caustic, and hydrogen from brine using a three-layer porous capillary spacer 110 tightly compressed together into a whole and consisting of, from one side to the other, (i) Layer 1: a GLA-5000 polyvinyl chloride (PVC) material filter (Pall Corp) with an average pore size of 5 μm, having one end immersed in a liquid bath containing an aqueous solution of 280 g / L NaCl (brine) acidified to pH 3; (ii) Layer 2: an industry-standard perfluorinated sodium exchange membrane; and (iii) Layer 3: a polyethersulfone material filter with an average pore size of 8 μm, having one end immersed in a second, separate liquid bath containing an aqueous solution of 35% NaOH. cell The chlorine generation electrode 120 consisted of a commercially available dimensionally stable anode (Permascand) and also served as the electrode-current carrier assembly 420. The hydrogen generation electrode 130 included a Sgracet™ carbon paper substrate onto which a thin catalyst layer of 10% Pt on Vulcan XC-72 was sprayed on the micro-hole side using PTFE (from a PTFE dispersion) as the binder. The electrode 130 was compressed against a Ni mesh, which served as the current carrier 330, thereby providing the electrode-current carrier assembly 430. Overall cell The flow fields 620 and 630 in the figure were Ti mesh and Ni foam, respectively. The conductive bus bars 640 were Ti-coated and Ni-coated stainless steel, respectively. Chlorine was used as gas 125. cell while hydrogen is produced as gas 135 cell Sodium chloride (brine) was consumed from the acidified NaCl-containing tank, while caustic (sodium hydroxide) was produced in the NaOH-containing tank. Continuous replenishment and removal of these materials from each tank could be accomplished by means known to those skilled in the art.

[0450] 3. Electrosynthetic oxygen depolarized chlorine alkali to produce chlorine and caustic from saltwater cell Examples cell 1-2 , an example embodiment of an oxygen-depolarized chlorine-alkali filter for producing chlorine and caustic from brine, using a three-layer porous capillary spacer 110 tightly compressed together into a whole and consisting of, from one side to the other, (i) Layer 1: a GLA-5000 polyvinyl chloride (PVC) material filter (Pall Corp) with an average pore size of 5 μm, having one end immersed in a liquid bath containing an aqueous solution of 280 g / L NaCl (brine) acidified to pH 3; (ii) Layer 2: an industry-standard perfluorosodium exchange membrane; and (iii) Layer 3: a polyethersulfone material filter with an average pore size of 8 μm, having one end immersed in a second, separate liquid bath containing an aqueous solution of 35% NOH. cell The chlorine generating electrode 120 consisted of a commercially available dimensionally stable anode (Permascand) and also served as the electrode-current carrier assembly 420. The oxygen depolarized counter electrode 130 comprised a Sgracet™ carbon paper substrate onto which a thin catalytic layer of 10% Pt on Vulcan XC-72 was sprayed on the microhole side using PTFE (from a PTFE dispersion) as the binder. The electrode 130 was compressed against a Ni mesh, which served as the current carrier 330, thereby providing the electrode-current carrier assembly 430. Overall cell The flow fields 620 and 630 in the figure were Ti mesh and Ni foam, respectively. The conductive bus bars 640 were Ti-coated and Ni-coated stainless steel, respectively. Chlorine was used as gas 125. cell while oxygen is produced as gas 135 cell Sodium chloride (brine) was consumed from the acidified NaCl-containing tank, while caustic (sodium hydroxide) was produced in the NaOH-containing tank. Continuous replenishment and removal of these materials from each tank could be accomplished by means known to those skilled in the art.

[0451] 4. Electrosynthesis to generate chlorine and hydrogen by recycling hydrochloric acid cell Examples 1 or 2, using a GLA-5000 polyvinyl chloride (PVC) material filter (Pall Corp) with an average pore size of 5 μm as the porous capillary spacer 110. cell The liquid electrolyte 100 was aqueous 1 M HCl. The chlorine generation electrode 120 consisted of a commercially available dimensionally stable anode (Permascand), which also served as the electrode-current carrier assembly 420. The hydrogen generation electrode 130 included a Sgracet™ carbon paper substrate onto which a thin catalyst layer of 10% Pt on Vulcan XC-72 was sprayed on the micro-hole side using PTFE (from a PTFE dispersion) as the binder. The electrode 130 was compressed against a Ni mesh, which served as the current carrier 330, thereby providing the electrode-current carrier assembly 430. Overall cell The flow fields 620 and 630 in the figure were Ti mesh and Ni foam, respectively. The conductive bus bars 640 were Ti-coated and Ni-coated stainless steel, respectively. Chlorine was used as gas 125. cell while hydrogen is produced as gas 135 cell The hydrochloric acid was depleted from tank 140, which may be constantly replenished with hydrochloric acid by means known to those skilled in the art.

[0452] 5. Electrical energy fuel that generates electrical energy from hydrogen and oxygen cell Examples Example embodiment hydrogen-oxygen fuel having the structure shown in FIG. 1 or FIG. 2 cell was fabricated using a polyethersulfone material filter with an average pore size of 8 μm as the porous capillary space 110. The liquid electrode 100 was aqueous 6M KOH. The first electrode 120 and second electrode 130 were both composed of a mixture of 20% Pd / Pt, carbon black, and PTFE (from a 60% PTFE dispersion) on Vulcan XC-72 deposited on and compressed into a Ni mesh, which served as the current carriers 320 and 330, respectively, thereby providing electrode-current carrier assemblies 420 and 430, respectively. Complete cellThe internal flow fields 620 and 630 were Ni foam. The conductive busbar 640 was Ni-coated stainless steel. Oxygen was used as gas 125. cell while hydrogen is introduced as gas 135 cell was introduced.

[0453] In one alternative example, electrode-current carrier assemblies 420 and 430 were fabricated as described in Wagner, K., Tiwari, P., Swiegers, GF & Wallace, GG, "Alkaline Fuel Cells with Novel Gortex-Based Electrodes are Powered Remarkably Efficiently by Methane Containing 5% Hydrogen," Advanced Energy Materials, 8(7), 1702285-1-1702285-10, which is incorporated herein by reference. Because the resulting electrode-current carrier assemblies 420 and 430 had a non-conductive Gortex membrane backing, flow fields 620 and 630 were cut with sharp protrusions on the sides facing the electrodes. These protrusions cut through the Gortex backing on 420 and 430, thereby establishing electrical connections between the first electrode 120 and second electrode 130 and the respective flow fields 420 and 430.

[0454] These examples represent variations in the electrode-spacer interfaces 126 and 136 to modify, better control, or accelerate the capillary and / or diffusion processes by which liquid phase material moves along path 200, as described with reference to FIG. 4.

[0455] fuel cell operates as described in the scientific paper cited above. Water was produced as a reaction product in vessel 140. Water could be continuously removed from vessel 140 by various means known to those skilled in the art.

[0456] Having the structure shown in FIG. cellcan also be fabricated by the same process, where the liquid electrolyte in the porous capillary spacer is maintained non-interferingly by vaporizing water and humidifying the hydrogen and / or oxygen gas stream. cell Circulate through cell The container was dried on the outside to remove evaporated water.

[0457] 6. Electrosynthetic water electrolysis to generate hydrogen and oxygen from water cell Examples Water electrolysis of the embodiment having the structure shown in FIG. 1 or FIG. 2 cell was made using a polyethersulfone material filter with an average pore size of 8 μm as the porous capillary space 110. The liquid electrode 100 was aqueous 6 M KOH.

[0458] The hydrogen generating electrode 130 was manufactured in accordance with the method described in "An Alkaline Water Electrolyzer with Sustained Water" by Z. Liu, S.D. Sajjad, Yan Gao, J.J. Kaczur, and R.I. Masel. TM Membranes: 1A / cm 2 at 1.9V with Base Metal Catalysts,” ECS Transactions (2017) 77(9), 71-73, which is incorporated herein by reference. This procedure was used to fabricate 10% Pt (Pt 0.5 mg / cm) on Vulcan XC-72 using 5% Nafion® as the binder (26 wt%). 2 The electrode 130 was compressed against a Ni mesh that served as a current carrier 330, thereby providing an electrode-current carrier assembly 430.

[0459] The oxygen-producing electrode 120 was composed of a fine-mesh nickel mesh (200 LPI) onto which a NiFe catalyst was electrodeposited, as taught in the scientific paper "Novel NiFe / NiFe-LDH Composites as Competitive Catalysts for Clean Energy Purposes" by A.M. Sakata, E. Valles, R. Della, and A.V. Benedetti, Applied Surface Science 447 (2018) 107-116, which is incorporated herein by reference. The nickel mesh was placed in an electrodeposition solution composed of a 3:1 mixture of NiCl (0.075 M) and FeCl (0.025 M) (according to Figures 8(c) and 1(a) of the same paper) with a 1 M KCl supporting electrolyte (according to Figure 8(b) of the same paper). The nickel mesh was immersed in the electrodeposition solution and coated with NiFe by cycling between -1.0 V and -0.2 V at 10 mV / s using cyclic voltammetry (according to Figure 1 of the same paper). A low voltage of −1.0 V was chosen to allow inclusion of the gas handling material without forming precipitates, as described in the next paragraph. A high voltage of −0.2 V provided the best performing resulting catalyst. The coating was deposited at a charge of 16.6 C (over a geometric area of ​​1 cm). 2 The Ni mesh itself served as the current carrier 320, thereby providing an electrode-current carrier assembly 420. cell The inner flow fields 620 and 630 were Ni foam. The conductive busbars 640 were nickel. Oxygen was used as the gas 125. cell while hydrogen is produced as gas 135 cell Generated by.

[0460] Having the structure shown in FIG. cell can also be fabricated by the same process, where the liquid electrolyte within the porous capillary spacer is maintained non-interferingly by liquefying water from the humidification of hydrogen and / or oxygen gas streams. cell Circulate through cellThe external humidification promotes condensation of the vapor in the porous capillary spacer.

[0461] 6.1 Example: Introducing a gas handling structure into an electrode The electrode 120 was modified to include a gas handling structure constructed from polytetrafluoroethylene (PTFE), a low surface energy material. As described above, PTFE has the property of trapping dissolved gases and causing them to coalesce on its surface. The gases can then migrate further along the surface into the gas 125 without forming bubbles in the liquid electrolyte. The PTFE gas handling structure was incorporated into the electrode 120 by dispersing PTFE in the electrodeposition solution (60 wt % dispersion in alcohol / HO). The fabrication procedure was otherwise described above.

[0462] 6.2 Example: fully flooded cell Comparison with For comparison purposes, the electrode-spacer-electrode assembly (139) was flooded with liquid electrolyte. cell Such a cell corresponds to the structure shown in Figure 2, and A and B are both cell That is, the electrodes were entirely covered with liquid electrolyte and there was no gas 125 or 135 present. cell The traditional cell The gas is generated in the form of bubbles in the liquid electrolyte. cell The bubbles are formed within cell rises to the top of the

[0463] 6.3 Embodiments cell Demonstration of energy efficiency improvements through 11(a) and 11(b) are the same as those in FIG. cell 6 shows the polarization curves at 80° C. of the resulting water electrolysis device having the structure. Note that these curves are not corrected for internal resistance, i.e., they include the resistance imparted by the busbar 640 and the conductive flow fields 620, 630.

[0464] Curve (a) of FIG. 11 shows the results when the oxygen generating electrode (120 / 320 / 420) described above incorporates the PTFE gas handling structure. cell The polarization curve of this cell is not corrected for internal resistance, 118.2 Ω cm 2 and low overall cell The resistance was the lowest of any tested or indeed known by the inventors. cell However, the oxygen generating electrodes (120 / 320 / 420) described above did not incorporate the PTFE gas handling structures described above. cell The polarization curve of

[0465] Curve (c) of FIG. 11 employs the same porous capillary spacer and the same electrodes as described above, but cell is an equivalent water electrolysis system completely filled with liquid electrolyte. cell This shows the polarization curve of water electrolysis. cell The traditional cell In this configuration, gas is generated in the form of bubbles in the liquid electrolyte. Figure 11 shows the results of the best commercially available alkaline water electrolysis devices and PEM water electrolysis devices for which data is available. cell The equivalent polarization curves (d)-(e) at 80 °C are shown.

[0466] In curves (a) and (b) of FIG. 11, the same electrodes and porous capillary spacers are used, but the gas is generated in the form of bubbles in the liquid electrolyte. cell This shows a significant improvement over the previous cell Improved compared to the structure of the example embodiment cell The energy efficiency of the structure was demonstrated.

[0467] Curves (a) and (b) in Figure 11 show the best commercially available alkaline water electrolysis cell (Curve (d) in Figure 11) and commercial PEM water electrolysis cell This is a significant improvement over the curve (e) in Figure 11. This is especially true for the curves (a) and (b) in Figure 11. cellHowever, in particular, the type of PEM water electrolysis shown in Figure 11(e) cell Alkaline water electrolysis is significantly cheaper, more durable, and has a much longer lifespan than alkaline water electrolysis cell Considering that, in the example embodiment cell It is shown that the structure improves energy efficiency.

[0468] Alkaline electrolysis cell The curve (c) in Figure 11, which involves the best commercially available alkaline water electrolysis cell It is also worth noting that this is a dramatic improvement from curve (d) in Figure 11. This is because, under comparable conditions, both A and B cell The structure shown in FIG. 2 extending to the top of FIG. 11(a) and FIG. 11(b) also cell Although the improvement is smaller than that of Fig. 11(c), it still provides efficiency improvement. cell "Independent Pathway" cell "This is because...

[0469] Therefore, for example, a current density of 0.7 A / cm 2 in its ability to produce hydrogen at cell Comparing the - Curve (a) in Figure 11 cell Only 1.536V (point A) is required, which is equivalent to an energy efficiency of 96% of the higher heating value (HHV) of hydrogen. - Curve (b) in Figure 11 cell Only 1.568V (point B) is required, which is equivalent to an energy efficiency of 94% of the higher heating value (HHV) of hydrogen. - Curve (c) in Figure 11 cell requires 1.655V (point C), which is equivalent to an energy efficiency of 89% of the higher heating value (HHV) of hydrogen. - The best commercially available alkaline water electrolysis shown in Figure 11, curve (d) cell requires 1.84V (point D), which is equivalent to an energy efficiency of 80% of the higher heating value (HHV) of hydrogen. - The best commercially available PEM water electrolysis in Figure 11, curve (e) cellrequires 1.61V (point E), which is equivalent to an energy efficiency of 91% of the higher heating value (HHV) of hydrogen.

[0470] The ability to improve energy efficiency is further illustrated by FIG. 12, which shows a constant voltage of 1.47V at 80° C. representing 100% energy efficiency (HHV). cell When the voltage is held at the cell This shows the performance over time. cell is a constant 300mA / cm at 100% energy efficiency (HHV). 2 (=0.3A / cm 2 On the other hand, commercially available alkaline electrolytic cell The best publicly reported current at 80°C and 1.47V is approximately 0.1A / cm 2 and commercially available PEM electrolysis cell The current due to this is about 0.2mA / cm 2 is.

[0471] 6.4 Example: Demonstration of low interelectrode resistance Curve (a) in Figure 11 cell There were several reasons for the improved energy efficiency of the PVDF. These included the lower resistance of the porous capillary spacer, curve (a) of Figure 11, which was approximately 130 mΩ cm at 80°C for the Zirfon PERL® separator membrane, curve (d) of Figure 11. 2 and about 74 mΩcm at 80°C for the Nafion® 115 separator membrane, curve (e) of Figure 11. 2 22 mΩ cm at 80°C compared to 2 The effect was as shown in curve (d) of Figure 11. cell 11 curve (e) cell The difference is about 0.052 V compared to the curve (a) in Figure 11. cell at 1A / cm 2 The goal was to reduce the voltage required in

[0472] 6.5 Example: Demonstration of Gas Crossover Degradation Curve (a) in Figure 11 cellhad a low benchmark gas crossover, with % hydrogen in oxygen ranging from 0.04 to 0.14% and % oxygen in hydrogen ranging from 0.00%. In comparison, Zirfon PERL® was found to be superior to comparable fulminated alkaline water electrolysis systems. cell When used in this way, it is considered to exhibit a benchmark gas crossover of 0.22% or greater.

[0473] 6.6 Example: Demonstration of energy efficiency improvements resulting from inclusion of gas handling structures in electrodes As can be seen, curve (a) in Figure 11 is an improvement over curve (b) in Figure 11, demonstrating the beneficial effect of including a PTFE gas handling structure in the oxygen generating electrode. The gas handling structure helps newly formed gas exit the electrode without forming visible bubbles. The gas handling structure does so by lowering the surface energy of the path along which the gas leaves.

[0474] 6.7 Example: Demonstration of improved energy efficiency due to "foam-free" electrodes Therefore, another major contributor to the improved energy efficiency of curve (a) in Figure 11 was the absence of visible bubbles in either electrode, which significantly improved the energy efficiency of the electrolyte and reduced the voltage required across the electrolyte, as shown by comparison with curve (c) in Figure 11.

[0475] In this example, a thin layer (less than 0.125 mm thick) of liquid electrolyte appears to be drawn from the porous capillary spacer 110 onto the catalytic surface of the electrode. As gas is then produced by the electrode, it migrates from the thin layer of electrolyte to the adjacent outer surface and combines with gases 125 and 135 across the interface. Alternatively or optionally, within the oxygen-producing electrode 120, newly formed oxygen gas coalesces on the PTFE surface present on the electrode and migrates along the PTFE surface to combine with oxygen gas 125.

[0476] Thus, there was no need to release gas by forming bubbles on or near the electrode surface. As a result, the electrode was not masked with bubbles, as may be the case in conventional bubble systems. Furthermore, the liquid electrolyte near the electrode surface did not need to be supersaturated with gas to nucleate bubble formation. In doing so, the additional voltage that may be required to create such supersaturation was avoided. Furthermore, bubbles tend to form in (and often strongly attach to) cracks, cracks, and imperfections on the electrode surface where the most catalytically active sites are also located, but such sites were largely unaffected and operated at their highest catalytic activity in the absence of bubble formation. Thus, the catalytic surface of the electrode was more fully utilized at any given time.

[0477] 6.8 Example: Water electrolysis cell is an "independent pathway" that indicates improved energy efficiency. cell " The ability of the porous capillary spacer 110 to infinitely supply the liquid phase reactants necessary for the electrodes 120 and 130 to sustain the reaction while the gas products move away from the electrodes in a direction that complements the liquid phase movement means that multiphase backflow is avoided and at least one separate, independent, non-interfering path is provided. cell It is shown that the individual liquid and gas phase reactants and products are transported (flowed) within the reactor.

[0478] Therefore, in Figs. 11(a) and 11(b), cell is "independent pathway" cell ", which was basically the reason for the higher energy efficiency. cell Independent pathways cell However, the energy efficiency was lower due to bubble formation: the energy required to overcome the inefficiencies associated with multiphase backflow was avoided, but the energy required to overcome the inefficiencies associated with bubble formation was not avoided.

[0479] In Fig. 11(a) and Fig. 11(b), cellThe bubble-free operation of the electrode enhanced the efficiency of the pathway for gas removal from the bubble-free electrode. The inclusion of a gas-handling structure in the oxygen electrode provided a particularly improved pathway for gas removal from that electrode. The effect was cell improves the efficiency of molecular movements within the cell The key to success was improving the energy efficiency of the system.

[0480] Therefore, this example is a disjoint path cell But other cell We have shown that it is possible to achieve higher energy efficiencies than conventional methods. We also show that the improvement in energy efficiency can be substantial.

[0481] 6.9 Example: Demonstration of high energy efficiency after modifying the electrode surface to promote capillary-guided movement of electrolyte up the electrode As mentioned above, capillary-induced movement of liquid electrolyte along and up the electrodes can typically interfere with, or even prevent, gas transport between the electrodes and the associated gases. cell This can reduce the energy efficiency of the system.

[0482] However, if such transport is designed to be limited to a very thin layer of liquid electrolyte moving over the electrode surface, there may be no interference or impediment to gas transport, and thus no detrimental impact on energy efficiency.

[0483] Such capillary-induced transport of a thin film of liquid electrolyte deposits a thin hydrophobic layer on the electrode surface, as described below, resulting in a thin hydrophobic layer, as shown in Figure 2. cell It can be designed by adopting a design.

[0484] Nickel foam was used as a substitute oxygen electrode in the water electrolysis device. The nickel foam was sonicated in ethanol for 10 minutes to remove any organic residue, then rinsed with water, and further sonicated in 3M HCl for 20 minutes, then rinsed with water and dried. The Ni foam was then immersed in an autoclave containing an aqueous solution of 43 mM NiNO, 14.3 mM FeNO, and 0.28 M urea, and heated at 120°C for 12 hours. The resulting electrode was rinsed with water and air-dried.

[0485] Thin layers of NiFe layered double hydroxide (LDH) deposited using this method were both strongly hydrophilic and good catalysts for the production of oxygen from water. Their high hydrophilicity appeared to facilitate capillary-based upward migration of a thin layer of 6 M KOH liquid electrolyte on the electrode surface at rates exceeding 5 cm / min. This was significantly faster than that exhibited by a porous capillary spacer 110 containing a polyethersulfone material filter with an 8 μm pore size.

[0486] During catalytic oxygen production, the NiFe-coated Ni foam also exhibited high energy efficiency comparable to that of the oxygen electrode shown in curve (a) of Figure 11. (a) Curve (a) in Figure 11 cell Oxygen electrode and (b) Curve (a) in Figure 11 cell The NiFe-coated Ni foam when used as an oxygen electrode in Figure 1 shows a comparison of electrode potential vs. current density for the oxygen electrodes of NiFe and NiFe. As can be seen, the performance of the two electrodes is very similar, indicating that capillary-induced migration on the surface of the NiFe-coated Ni foam electrode did not significantly reduce energy efficiency.

[0487] 6.10 Example: Incorporation of gas handling structures into surface-modified electrodes The Ni foam electrodes described above can also be modified to incorporate PTFE gas handling structures during surface modification.

[0488] This was achieved as follows: an aqueous solution of 43 mM NiNO, 14.3 mM FeNO, and 0.28 M urea was heated in an autoclave at 120 °C for 12 hours. The resulting NiFe-LDH catalyst was collected, washed three times with deionized water by centrifugation, and then dried in a vacuum oven at room temperature. A dispersion of the resulting NiFe powder was prepared in a solution containing isopropanol and water (4:1 vol%) with the addition of Nafion® (10 g / L). The NiFe-LDH dispersion was then airbrushed onto pre-cleaned Ni foam or Ni mesh to obtain a NiFe-LDH-coated electrode of the desired weight / thickness.

[0489] 6.11 Example: Inclusion of a gas capillary structure in an electrode In one alternative example, electrode-current carrier assemblies 420 and 430 were fabricated to incorporate a gas capillary structure, in this case a hydrophobic Gore-Tex™ membrane (i.e., a hydrophobic membrane comprising expanded polytetrafluoroethylene (ePTFE)), with the PTFE side tightly positioned against the outside of electrode-current carrier assemblies 420 and 430. cell In the example, the outside of the electrodes, which comprised a Gore-Tex™ membrane, was then in contact with each flow field 620 and 630. A generic version of the Gore-Tex™ membrane is known as a "Gor...

Claims

1. 1. An electrochemical cell comprising: a first gas diffusion electrode configured to generate a first gas and to be in contact with and adjacent to a first gas stream containing the first gas; a second gas diffusion electrode configured to generate a second gas and to be in contact with and adjacent to a second gas stream containing the second gas; a porous capillary spacer located between the first gas diffusion electrode and the second gas diffusion electrode, the porous capillary spacer being filled with a liquid electrolyte and configured to confine the liquid electrolyte in the porous capillary spacer by capillary effect; Equipped with the porous capillary spacer is less than 0.2 mm thick; The electrochemical cell is an electrosynthesis cell.

2. 10. The electrochemical cell of claim 1, further comprising a reservoir configured to contain a liquid electrolyte and to underlie the porous capillary spacer during operation, wherein at least a tip of the porous capillary spacer contacts the liquid electrolyte in the reservoir.

3. 10. The electrochemical cell of claim 1, wherein the first gas diffusion electrode and the second gas diffusion electrode are compressed against the porous capillary spacer at greater than 2 bar.

4. 10. The electrochemical cell of claim 1, wherein the porous capillary spacer is less than 0.13 mm thick.

5. 10. The electrochemical cell of claim 1, configured such that during operation, no gas bubbles are visible on at least a portion of the first gas diffusion electrode or at least a portion of the second gas diffusion electrode.

6. 10. The electrochemical cell of claim 1, further comprising an external housing providing at least one external first gas conduit, wherein the electrochemical cell is configured such that during operation, the first gas is transported into or out of the first gas body via the at least one external first gas conduit.

7. 7. The electrochemical cell of claim 6, wherein the external housing further provides at least one external second gas conduit, and wherein during operation, the second gas is configured to be transported into or out of the second gas body via the at least one external second gas conduit.

8. 3. The electrochemical cell of claim 2, wherein the reservoir comprises a first volume configured to contain a first liquid, a second volume configured to contain a second liquid, and a semi-permeable membrane separating the first volume and the second volume.

9. 9. The electrochemical cell of claim 8, wherein the tip of the porous capillary spacer is located in the first volume, and wherein during operation, the first liquid is the liquid electrolyte and the second liquid is configured to be different from the first liquid.

10. The porous capillary spacer is filled with a liquid electrolyte and has a resistivity of 140 mΩcm at room temperature. ２ 10. The electrochemical cell of claim 1, configured to have an ionic resistance of less than 1000 .mu.m.

11. 10. The electrochemical cell of claim 1, comprising two or more porous capillary spacers.

12. 12. The electrochemical cell of claim 11, comprising two or more reservoirs configured to contain the liquid electrolyte, wherein a distal end of each of the two or more porous capillary spacers is located within one of the two or more reservoirs.

13. 10. An electrochemical multi-cell stack comprising a plurality of electrochemical cells according to claim 1, whereby said plurality of electrochemical cells are electrically connected.

14. 10. An electrochemical multi-cell stack comprising a plurality of electrochemical cells according to claim 8, wherein during operation, the second liquid of each of the plurality of electrochemical cells is fluidly communicated through a common supply or removal pipe connected to the second volume of each of the plurality of electrochemical cells.

15. 1. A stack of electrochemical cells, comprising: a first electrochemical cell; a second electrochemical cell electrically connected to the first electrochemical cell; Equipped with Each electrochemical cell is a first gas diffusion electrode configured to generate a first gas and to be in contact with and adjacent to a first gas stream containing the first gas; a second gas diffusion electrode configured to generate a second gas and to be in contact with and adjacent to a second gas stream containing the second gas; a porous capillary spacer located between the first gas diffusion electrode and the second gas diffusion electrode, the porous capillary spacer being filled with a liquid electrolyte and configured to confine the liquid electrolyte in the porous capillary spacer by capillary effect; wherein the porous capillary spacers are less than 0.2 mm thick and the electrochemical cells are electrosynthesis cells.

16. 1. A method of operating an electrochemical cell to carry out an electrochemical reaction, the electrochemical cell comprising: a first gas diffusion electrode configured to generate a first gas and to be in contact with and adjacent to a first gas comprising the first gas; a second gas diffusion electrode configured to generate a second gas and to be in contact with and adjacent to a second gas comprising the second gas; and a porous capillary spacer positioned between the first gas diffusion electrode and the second gas diffusion electrode, the porous capillary spacer being filled with a liquid electrolyte and configured to confine the liquid electrolyte in the porous capillary spacer by capillary effect, the porous capillary spacer being less than 0.2 mm thick; the electrochemical cell being an electrosynthesis cell; and the method of operating comprising applying a voltage between the first gas diffusion electrode and the second gas diffusion electrode.

17. 10. A method of operating an electrochemical cell according to claim 1 to carry out an electrochemical reaction, comprising applying a voltage between the first gas diffusion electrode and the second gas diffusion electrode.

18. 10. The electrochemical cell of claim 1, wherein the porous capillary spacer has an average pore size greater than 2 μm.

19. 10. The electrochemical cell of claim 1, wherein the porous capillary spacer comprises a plurality of pores that provide a flow path between the first gas diffusion electrode and the second gas diffusion electrode.

20. 10. The electrochemical cell of claim 1, wherein the liquid electrolyte has a maximum column height of greater than 0.4 cm.

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