Device and method for electrochemical decomposition of consumable two-dimensional layered semiconductor or conductor material
By using a mesh and/or belt feeding system in the electrolytic cell, the problem of low electrolytic stripping efficiency of two-dimensional layered semiconductor or conductor materials in the prior art is solved, realizing efficient and continuous electrochemical decomposition and improving yield and decomposition quality.
Patent Information
- Authority / Receiving Office
- CN · China
- Patent Type
- Applications(China)
- Current Assignee / Owner
- SIXONIA TECH GMBH
- Filing Date
- 2024-09-26
- Publication Date
- 2026-04-28
AI Technical Summary
Existing technologies for producing two-dimensional layered semiconductor or conductor materials suffer from low efficiency, low yield, and easy re-aggregation of materials. In particular, it is difficult to achieve high-quality graphene production during the electrolytic stripping process.
An apparatus and method are employed, the apparatus comprising an electrolytic cell, a power supply, and a feeding system, wherein consumable two-dimensional layered semiconductor or conductor material is delivered into an electrolyte via a feed system consisting of a mesh and/or a belt, ensuring constant current and distance, reducing ohmic losses, avoiding short circuits, and achieving continuous electrochemical decomposition.
It improves the electrochemical decomposition efficiency and yield of two-dimensional layered semiconductor or conductor materials, reduces material fracture and re-aggregation, and achieves a highly efficient decomposition process.
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Figure CN121941801A_ABST
Abstract
Description
[0001] The present invention relates to an apparatus and method for the electrochemical decomposition of consumable two-dimensional layered semiconductor or conductor materials, comprising at least one electrolytic cell and a feeding system for delivering the consumable two-dimensional layered semiconductor or conductor material into an electrolyte.
[0002] For many years, the separation of monolayers from two-dimensional structured or layered semiconductor or conductor materials has been a subject of considerable interest, particularly due to the significant performance improvements and high efficiency that these materials bring to electronic components. An example of such separated layers in two-dimensional structured or layered materials is graphene, which represents a monolayer—a single atom layer of graphite, a naturally occurring form of carbon. However, graphene also refers to materials in which some of these monolayers are stacked on top of each other. Graphene can be understood as a two-dimensional network of chain-like benzene rings, which, among other things, possesses tremendous electrical conductivity. Its applications in numerous technological fields are attracting considerable attention due to its electronic, thermal, optical, and mechanical properties.
[0003] Graphene is produced in part under challenging process conditions using high-boiling-point solvents such as dimethylformamide and N-methyl-2-pyrrolidone.
[0004] Graphene can also be produced by reducing graphene oxide, for example, via the so-called Hummers method (Hummers et al., 1958). Graphene oxide exhibits excellent dispersibility in a variety of solvents, particularly water, which greatly facilitates its application on a larger scale. It can also be redispersed after complete drying. However, a drawback of the reduction method is that oxide groups and other defects, such as pores or non-six-membered rings, are retained within the material. These structural defects severely limit the electronic and thermal properties of graphene produced from graphene oxide (Gómez-Navarro et al., 2007).
[0005] Alternatively, monolayers or thin layers of conductive materials such as graphene are produced by electrolytic exfoliation of a base material (such as graphite) with a two-dimensional layered structure. Graphene layers as sheets have been separated from solid graphite (e.g., see Novoselov et al., 2011) or liquid phase (e.g., see Xia et al., 2013) as the base material.
[0006] So-called liquid-phase graphite exfoliation utilizes purely physical shear forces in primarily organic solvents and allows for the production of graphene with significantly fewer defects than graphene synthesized from graphene oxide. However, a disadvantage is that this results only in low yields of exfoliated graphene and very small lateral layer sizes (Coleman, 2013). Furthermore, after exfoliation, the lamellar crystals tend to re-aggregate (stack). The use of surfactants or other additives to prevent this effect is unavoidable. However, these additives are difficult to remove and significantly reduce the conductivity of the product.
[0007] Recently, anodic exfoliation has emerged as a promising method for the large-scale, low-cost production of high-quality graphene in aqueous solutions. The two-dimensional base material can be used as the anode in an aqueous solution of an ionic liquid, inorganic acid, or inorganic salt. Under the influence of an electric current, electrons are separated from the two-dimensional base material (e.g., graphite) and leave a positive charge on the anode. Anions from the electrolyte can then be readily pushed between the layers of the base material (e.g., graphite) and separate them. However, graphene produced in this manner suffers from a high proportion of oxygen-containing radicals. This is due to oxygen radicals such as HO· or O·, which are formed and added to the graphene layers during the production process through water splitting (Rao et al., 2015).
[0008] Furthermore, the exfoliated layers re-adhere after drying and are difficult to redisperse. One way to increase the dispersibility of graphene layers is to functionalize them with small molecules or polymers. Ejigu et al. described the cathodic exfoliation of graphite in organic solvents and the simultaneous, in-situ functionalization of graphene layers with diazonium salts (Ejigu et al., 2017). Diazonium salts generate free radicals and functionalize the surface through a reduction reaction at the cathode.
[0009] Chen et al. described a method for producing highly crystalline graphene by electrolytic exfoliation of melamine in 0.65 M sulfuric acid at concentrations ranging from 10 g / 100 ml to 200 g / 100 ml of electrolyte solution (Chen et al., 2015), in which graphene layers are exfoliated from a graphite electrode and influenced by melamine molecules. These in-situ applied protective layers prevent further oxidation of the graphene layers, resulting in larger graphene microcrystals. Residual melamine is then washed away from the collected graphene with water, and after drying, low-density oxygen vacancies are observed.
[0010] Another possibility for producing functionalized graphene is the use of ionic liquids (Liu et al., 2008).
[0011] CN 113 830 760 A describes a method for producing graphene oxide by stable electrolysis, particularly by using a two-phase liquid comprising an insulating protective solution (preferably paraffin) and an electrolyte (preferably an aqueous solution of sulfuric acid with a concentration of 70 wt.%), wherein the graphite electrode is first immersed in the insulating protective solution after intercalation, and then gradually immersed in the electrolyte solution. Cleaning and deacidification are then performed. CN 113 830 760 A discloses that the graphite electrode is gradually introduced into the electrolyte through the insulating and protective solution at a rate ranging from 0.01 mm to 100 mm / min, preferably 1 mm / min.
[0012] US 2021 / 078863 A1 describes a method for exfoliating graphene sheets from a graphite sample, comprising compressing the graphite sample in an electrochemical reactor and applying a voltage between the graphite sample and an electrode in an electrochemical cell. US2021 / 078863 A1 discloses pressing the graphite sample onto a cathode through a ceramic membrane, particularly a movable permeable ceramic membrane, and preferably applying a counterweight to the movable permeable ceramic membrane, wherein the ceramic membrane is permeable to an electrolyte.
[0013] CN 112 607 729 A describes an apparatus and method for exfoliating graphene using an alternating electric field. The apparatus includes a feeding unit, an intercalation unit, and an exfoliation unit. The exfoliation unit includes an electrolytic cell, a temperature sensor placed in an electrolyte, a temperature controller, and AC and DC power supplies. Graphite strips are fed through the feeding unit and sequentially enter the intercalation unit and the exfoliation unit. Two electrode plates are arranged on both sides of the electrolyzer containing the electrolyte and connected to the AC and DC power supplies. CN 112607 729 A describes the feeding unit as including one conductive roller and five non-conductive rollers. The conductive and non-conductive rollers are driven by a motor, the speed of which determines the feeding speed and conveys the graphite strips to the intercalation unit and the exfoliation unit.
[0014] EP 3 732 315 A1 and US 2021 / 078865 A1 disclose a method for preparing surfactant-free functionalized semiconductor or conductor material dispersions from two-dimensional layered carbon-based materials by electrolytic stripping, the method using an aqueous and / or alcoholic electrolyte solution comprising sulfuric acid and / or at least one salt selected from sulfate and / or hydrogen sulfate and / or perchlorate and / or persulfate.
[0015] EP 3 434 645 B1 and US 2019 / 112195 A1 describe a method for the continuous preparation of graphene oxide nanosheets, comprising the steps of: providing a flexible graphite paper roll as a graphite raw material; and a two-step process of sequential electrochemical intercalation in a first apparatus and electrolytic oxidative exfoliation in a second apparatus, driven by a feeding device (particularly a roller feed device). EP 3 434 645 B1 and US 2019 / 112195 A1 disclose a continuous supply of graphite or carbon fiber, particularly a graphite material feed rate in the range of 1 mm / min to 10 m / min, preferably from 10 mm / min to 10 cm / min. A disadvantage of this arrangement is that the flexible graphite paper needs to be conveyed using rollers to prevent any contact between the graphite paper and the counter electrode to prevent short circuits. Therefore, the intercalation and exfoliation steps need to be performed in two separate apparatuses, thus reducing the efficiency of the method.
[0016] Therefore, the task is to provide a method with improved efficiency and / or yield.
[0017] According to the present invention, this task is solved by the apparatus and method described in the independent claim. Advantageous embodiments of the invention are specified in the dependent claims.
[0018] A first aspect of the present invention provides an apparatus for the electrochemical decomposition of a consumable two-dimensional layered semiconductor or conductor material, the apparatus comprising:
[0019] i. At least one electrolytic cell, the at least one electrolytic cell comprising
[0020] - At least one electrode pair consisting of at least one first electrode and one second electrode, and
[0021] - Containers used for electrolyte solutions,
[0022] ii. Power supply,
[0023] iii. A feeding system for conveying consumable two-dimensional layered semiconductor or conductor material into an electrolyte, the feeding system comprising at least one mesh and / or belt.
[0024] The first electrode is in contact with a consumable two-dimensional layered semiconductor or conductor material.
[0025] The second electrode is a counter electrode, which is disposed between at least one inner side of the consumable two-dimensional layered semiconductor or conductor material and the container.
[0026] The first and second electrodes are connected to a power source.
[0027] Advantageously, the apparatus according to the invention is capable of continuously electrochemically decomposing consumable two-dimensional layered semiconductor or conductor materials with improved efficiency or yield. Advantageously, according to the invention, the electrochemical decomposition of consumable two-dimensional layered semiconductor or conductor materials is achieved in one step or in one apparatus. By using a feeding system comprising a mesh and / or a belt, apparatus and methods with improved efficiency or yield are provided because the mesh and / or belt ensure a constant distance from the counter electrode, thereby providing a constant current when feeding the consumable two-dimensional layered semiconductor or conductor material into the electrolyte.
[0028] Advantageously, the distance between at least one second electrode and the consumable two-dimensional layered semiconductor or conductor material (raw material delivered by the feeding system) can be reduced to a very small extent, so that ohmic losses (due to the resistance of the electrolyte) can be minimized (these losses are lost as heat in the process) without the risk of a short circuit between the second electrode and the raw material.
[0029] Without a mesh and / or belt (e.g., if only rollers are used as the feeding system), the distance between the consumable two-dimensional layered semiconductor or conductor material and at least one second electrode may change, leading to altered peeling, particularly reduced or locally accelerated peeling. As a result, dissolution of the two-dimensional layered semiconductor or conductor material in the electrolyte may cause material breakage / interruption, thus interrupting peeling of the corresponding portion. This would result in larger, unpeeled clumps of initial material entering the electrolyte, for example, clogging the system's overflow or drain ports, leading to process interruption.
[0030] As used herein, the term “electrolytic cell” refers to a battery that uses an external power source to force a chemical reaction, particularly a voltage applied between at least two electrodes.
[0031] As used in this article, the term "electrolyte solution" (also referred to as electrolyte) refers to a solution containing ions that conduct electricity through the movement of those ions but not electrons.
[0032] As used herein, the term "feeding system" refers to a unit or device for continuously or intermittently conveying two-dimensional layered semiconductor or conductor material into and / or through a container for an electrolyte solution. Suitably, the movement of the feeding system (particularly the movement of a net and / or belt) is preferably by means of the rotation of pulleys or drums to draw the two-dimensional layered semiconductor or conductor material into the electrolyte.
[0033] As used herein, the term "consumable" refers to material that is decomposed through electrolytic stripping.
[0034] As used herein, the term "two-dimensional layered material" refers to a material consisting of at least one layer of covalently bonded atoms of at least one element. In embodiments, the two-dimensional layered material comprises at least two layers of covalently bonded atoms of at least one element, wherein these layers are parallel or nearly parallel to each other.
[0035] As used herein, the term "conducting material" refers to a class of materials that allow electric charge (current) to flow in one or more directions, such as metals.
[0036] As used herein, the term "semiconductor material" refers to a class of materials whose electrical conductivity values are between those of conductors and insulators (such as glass), such as Si, Ge, Se, α-Sn, B, Te, C (fullerene), GaP, GaAs, InP, InSb, InAs, GaSb, GaN, AlN, or InN.
[0037] In the embodiments, the semiconductor or conductor material is selected from graphene, graphene derivatives, carbon-based semiconductor or conductor polymers and / or layered chalcogenides of the general formula MQ2, wherein M is Ti, Zr, Hf, V, Nb, Ta, Mo or W, and wherein Q is O, S, Se or Te.
[0038] In the embodiments, the consumable two-dimensional layered semiconductor or conductor material is selected from graphite, carbon-based two-dimensional layered semiconductor or conductor polymers, and / or layered chalcogenides. Graphite may be naturally occurring or synthetic.
[0039] As used herein, the term “electrode pair” refers to a pair of at least one cathode and at least one anode.
[0040] In one embodiment, the first electrode is connected to the power source as the anode, and the second electrode is connected to the power source as the cathode.
[0041] As used herein, the term "anode" refers to the electrode of a polarizing device through which conventional current enters the device. The anode accepts electrons.
[0042] As used herein, the term "cathode" refers to an electrode of a device through which conventional current leaves the device. The cathode provides electrons.
[0043] In one embodiment, the first electrode is arranged such that it does not come into contact with the electrolyte during use of the device.
[0044] Appropriately, the second electrode is arranged such that it is in contact with the electrolyte during use of the device.
[0045] In this embodiment, the second electrode is a non-consumable counter electrode.
[0046] In the embodiments, at least the first electrode and / or the second electrode are non-consumable electrodes, which are preferably composed of at least one metal or metal alloy, particularly preferably platinum (Pt), gold (Au), silver (Ag), copper (Cu), aluminum (Al), titanium (Ti) or stainless steel.
[0047] In the embodiments, at least the first electrode and / or the second electrode are in the form of foil, plate, sheet, rod, bar, or sponge.
[0048] In one embodiment, at least one first electrode is arranged in the electrolytic cell such that it does not come into contact with the electrolyte during the electrochemical decomposition of the consumable two-dimensional layered semiconductor or conductor material. In another embodiment, at least one second electrode is arranged in the electrolytic cell such that it comes into at least partial contact with the electrolyte during the electrochemical decomposition of the consumable two-dimensional layered semiconductor or conductor material.
[0049] In an embodiment, the distance between at least one electrode pair (particularly the first electrode and the second electrode) is in the range of 1 mm to 100 cm.
[0050] In an embodiment, the distance between at least one second electrode and the consumable two-dimensional layered semiconductor or conductor material is in the range of 1 mm to 100 cm.
[0051] Suitable, at least one electrode pair (particularly the first and second electrodes) is arranged in any possible manner between the two electrodes, preferably the electrodes are arranged parallel or inclined to each other.
[0052] Appropriately, in the inclined arrangement, the distance between the electrodes decreases in the direction toward the bottom of the container. Advantageously, this arrangement counteracts the effect of reduced conductivity of the consumable two-dimensional layered semiconductor or conductor material due to decomposition (especially thinning and / or perforation).
[0053] In an embodiment, the apparatus further includes at least one unit for collecting and / or separating electrochemically decomposed semiconductor or conductor material from the electrolyte solution.
[0054] As used herein, the term "collection and / or separation unit" is a unit or apparatus for separating solid particles from a liquid solution. A collection and / or separation unit may be a filter, a centrifuge, or any other apparatus capable of increasing the particle concentration or separating particles in a suspension containing electrochemically decomposed semiconductor or conductor materials and an electrolyte solution.
[0055] In this embodiment, the collection and / or separation unit is located inside or outside the container for the electrolyte solution.
[0056] In an embodiment, the apparatus includes at least one unit inside a container for an electrolyte solution for collecting and / or separating electrochemically decomposed semiconductor or conductor material from the electrolyte solution, and at least one unit outside the container for an electrolyte solution for collecting and / or separating electrochemically decomposed semiconductor or conductor material from the electrolyte solution.
[0057] In an embodiment, the collection and / or separation unit is selected from filters and / or centrifuges and / or scrapers (preferably rotating screws) and / or pumps and / or air nozzles.
[0058] Suitablely, the filter and / or centrifuge and / or pump are located outside the container for the electrolyte solution. Suitablely, the scraper (preferably a rotating screw) and / or air nozzle are located inside the container for the electrolyte solution.
[0059] In an embodiment, the collection and / or separation unit is at least one filter.
[0060] In an embodiment, the apparatus includes at least one filter outside the container for the electrolyte solution and at least one scraper and at least one air nozzle inside the container for the electrolyte solution, for collecting and / or separating electrochemically decomposed semiconductor or conductor materials from the electrolyte solution.
[0061] As used herein, the term "scraper" refers to a unit with at least a single blade for scraping material from a surface. In embodiments, the scraper is arranged such that electrochemically decomposed semiconductor or conductor material can be scraped together and conveyed from the surface of the electrolyte solution or the bottom of the container to the container's outlet. Suitably, the scraper may be a rotating screw, preferably located at the bottom of the container.
[0062] In this embodiment, the air nozzle is directed toward the top of the electrolyte solution to facilitate the movement of floating particles toward the container edge (particularly toward the overflow port). Advantageously, the air nozzle prevents the accumulation of electrochemically decomposed semiconductor or conductor material on the electrolyte solution surface, which could lead to a potential short circuit between the semiconductor or conductor material and the counter electrode.
[0063] In an embodiment, the apparatus includes at least three units for separating electrochemically decomposed semiconductor or conductor materials from an electrolyte solution, preferably selected from a filter, a scraper, and an air nozzle.
[0064] In an embodiment, the apparatus further includes at least one additional separation unit (washing unit) for washing the electrochemically decomposed semiconductor or conductor material. Suitably, the washing unit is used, for example, to remove the electrolyte solution and / or exchange the solvent of the suspension of the electrochemically decomposed semiconductor or conductor material from the electrochemically decomposed semiconductor or conductor material using an aqueous solution and / or an organic solvent.
[0065] In this embodiment, the washing unit is selected from a filter or a centrifuge.
[0066] In one embodiment, the apparatus further includes at least one "processing unit".
[0067] As used herein, the term "processing unit" refers to a unit that processes electrochemically decomposed semiconductor or conductor materials into liquid formulations (particularly suspensions, preferably inks, coatings, pastes, slurries, sludge) and / or solid formulations (particularly powders, granules, or tablets).
[0068] As used herein, the term “suspension” refers to a heterogeneous mixture of liquids containing solid particles.
[0069] As used herein, the terms “ink” or “coating” refer to a suspension containing electrochemically decomposed semiconductor or conductor material and used to coat a surface.
[0070] As used herein, the term "paste" refers to a solid-liquid mixture (suspension) with a high solids content.
[0071] As used herein, the term "slurry" refers to a solid-liquid mixture (suspension) in which a relatively dense solid is suspended in at least one liquid, particularly water. As used herein, the term "sludge" refers to a semi-solid slurry.
[0072] In an embodiment, the processing unit is a device that applies shear force to the electrochemically decomposed semiconductor or conductor material.
[0073] In one embodiment, the processing unit includes an ultrasonic processor. Suitably, the ultrasonic processor is used to disperse electrochemically decomposed semiconductor or conductor materials into a low viscosity (typically within 10). -4 Up to 100 0 The dispersion, particularly ink, is within the Pa·s range. In embodiments, the processing unit further includes at least one separation unit, particularly a centrifuge and / or belt filter. Suitablely, the separation unit (particularly the centrifuge and / or belt filter) is used to separate poorly dispersed particles from the dispersion.
[0074] In embodiments, the processing unit includes a high-shear mixer, particularly a dissolver, a rotor-stator mixer, a high-pressure liquid jet micronizer (wet jet mill), a two-roll or three-roll mill, and / or a kneader. Suitably, the high-shear mixer is used to disperse electrochemically decomposed semiconductor or conductor materials into a form with high viscosity (typically above 10). -4 Up to 10 3 A uniform dispersion (within the range of Pa·s), especially a uniform ink, coating, paste or slurry.
[0075] In embodiments, the processing unit includes drying devices, particularly filter presses, drying racks, air knife dryers, belt dryers, drying cabinets, vacuum dryers, dehumidifiers, fluidized bed dryers, freeze dryers, and / or supercritical point dryers.
[0076] Appropriately, drying equipment is used to process electrochemically decomposed semiconductor or conductor materials into solid formulations.
[0077] In embodiments, the apparatus further includes at least one waste treatment unit. Suitably, the waste treatment unit is used to treat waste products generated during the operation of the apparatus, particularly used or excess electrolyte solutions, liquids or solids from washing and / or purification processes, particularly supernatants or precipitates from centrifugation, and / or condensates from drying processes. Advantageously, the waste treatment unit can be used to recover or regenerate waste products as segregants, particularly water or other liquids, such as electrolyte solutions or solvents that can be reused during apparatus operation. Further advantageously, by recovering or regenerating waste products, a circular material flow is achieved to improve the overall efficiency of the apparatus and reduce operating costs and waste, thereby minimizing potential environmental impact.
[0078] In one embodiment, the waste treatment unit includes at least one separation unit, particularly a filter or centrifuge. In another embodiment, the waste treatment unit includes at least one adsorption unit, particularly a filter column, preferably an activated carbon column.
[0079] In an embodiment, the device further includes at least one storage unit for storing segregated materials (particularly consumable two-dimensional layered semiconductor or conductor materials), raw materials (particularly electrolyte components), or waste.
[0080] In an embodiment, the container for the electrolyte solution includes at least one inlet and at least one outlet, wherein the outlet is connected to the inlet via at least one connecting element, and wherein a separation device is located between the outlet and the inlet. Advantageously, the electrolyte solution can be reused in the system after the decomposed semiconductor or conductor material is separated from the electrolyte solution.
[0081] In an embodiment, at least one outlet of the container is configured as an overflow outlet and / or located on the side or bottom of the container.
[0082] As used in this article, the term "overflow port" refers to a notch on the top edge of a container.
[0083] Advantageously, the overflow port ensures that the electrolyte solution is discharged above a certain height level and / or prevents the accumulation of electrochemically decomposed semiconductor or conductor materials on the surface of the electrolyte solution, which could lead to a potential short circuit between the semiconductor or conductor materials and the counter electrode.
[0084] As used herein, the term "mesh" (also referred to as a mesh or grid) refers to a barrier unit made of interconnected strands of fibers or other flexible material. Advantageously, the mesh is permeable and allows ions to pass through. In embodiments, the mesh is impermeable to particles larger than 1 µm. Advantageously, the mesh prevents particle accumulation between the consumable two-dimensional layered semiconductor or conductor material and the counter electrode in the electrolyte-containing container, thereby minimizing the risk of short circuits.
[0085] Appropriately, the size of the mesh is selected based on the size of the consumable two-dimensional layered semiconductor or conductor material.
[0086] In embodiments, the mesh includes holes or openings, particularly spaced holes or openings, with diameters ranging from 1 µm to 20 cm, preferably from 10 µm to 10 cm, and most preferably from 50 µm to 5 cm.
[0087] As used herein, the term "belt" refers to a conveyor belt that includes at least two pulleys (also called drums) and has a closed loop of a carrier belt that rotates around them.
[0088] Appropriately, the net or belt is made of mechanically and chemically stable, electrically insulating materials.
[0089] In the embodiments, the net or belt is made of polyethylene or polypropylene.
[0090] In one embodiment, the feeding system is arranged such that the mesh or strip is at least partially in contact with the consumable two-dimensional layered semiconductor or conductor material. In another embodiment, the feeding system is arranged such that the mesh or strip is at least partially immersed in the electrolyte during the electrochemical decomposition of the consumable two-dimensional layered semiconductor or conductor material.
[0091] In one embodiment, the feeding system includes at least two meshes, wherein the holes or openings of the meshes are staggered from each other.
[0092] In one embodiment, the feeding system includes at least two mesh-like, insulating strips placed on either side of a consumable two-dimensional layered semiconductor or conductor material, the consumable two-dimensional layered semiconductor or conductor material being at least partially arranged in a container such that it is at least partially surrounded by an electrolyte solution.
[0093] In one embodiment, the feeding system includes at least two mesh-like, insulating strips placed on either side of a consumable two-dimensional layered semiconductor or conductor material, the consumable two-dimensional layered semiconductor or conductor material being completely arranged in the container such that it is completely surrounded by an electrolyte solution.
[0094] In this embodiment, the mesh or belt is driven by a motor and / or operated by process control.
[0095] In one embodiment, the electrolytic cell includes another counter electrode (third electrode), wherein a consumable two-dimensional layered semiconductor or conductor material is arranged between the two counter electrodes.
[0096] In one embodiment, the electrolytic cell includes at least two parallel electrode pairs. In another embodiment, the electrolytic cell includes multiple parallel electrode pairs.
[0097] In an embodiment, the apparatus further includes at least one cooling unit, wherein the cooling unit is disposed in or connected to at least one first electrode and / or at least one second electrode and / or a container for an electrolyte solution and / or between at least one inlet and at least one outlet of the container.
[0098] As used herein, the term "cooling unit arranged in at least one first and / or second electrode" refers to an electrode designed to allow coolant to flow through it.
[0099] As used herein, the term "cooling unit arranged in a container for an electrolyte solution" refers to a container designed such that coolant can flow through at least one of its walls in contact with the electrolyte. In embodiments, the container for the electrolyte solution is a double-walled container connected to a cooling system.
[0100] In an embodiment, the electrolytic cell includes at least two (especially multiple) parallel electrode pairs, wherein a cooling unit is arranged in each of at least one electrode.
[0101] In an embodiment, the device further includes at least one sensor for monitoring at least one process parameter, preferably selected from temperature, conductivity, current, voltage and / or ultraviolet / visible light absorption.
[0102] In this embodiment, the sensors used to monitor the temperature are a temperature sensor and a temperature controller. Suitablely, the temperature sensor is used to measure and / or control the electrolyte temperature in the container, and to monitor and / or control the cooling water temperature, particularly at the container's inlet and / or outlet.
[0103] The term "temperature controller" is understood as an element that uses a sensor to detect the actual value of the temperature and compares it with a setpoint value, thereby allowing the desired temperature to be input via an actuator.
[0104] In a preferred embodiment, the sensor used to monitor temperature is a thermometer with a thermistor or thermocouple for contact measurement or a non-contact infrared thermometer.
[0105] As used herein, the term "conductivity sensor" refers to a sensor that uses conductivity to measure the ion content of an aqueous solution. Appropriately, conductivity sensors are used to monitor the conductivity of electrolytes in a container, monitor the conductivity of a washing solution, and particularly as a quality standard for container inputs and / or as an indicator of washing process efficiency.
[0106] In one embodiment, the sensor used to monitor conductivity is a 2- or 4-electrode conductivity cell, preferably made of graphite or platinum. In another embodiment, the conductivity sensor includes a chemically resistant glass body.
[0107] In this embodiment, the sensor used to monitor conductivity measures conductivity non-contactly, particularly using an eddy current sensor. Suitablely, the non-contact conductivity sensor is used to determine the solids content of the filtered or washed material during and / or after the washing process.
[0108] In a further embodiment, the conductivity sensor includes an integrated temperature sensor.
[0109] As used herein, the term "current sensor" refers to a sensor that measures current. Suitablely, a current sensor is used to measure the current flowing into the stripping system as a control variable for the stripping speed. In embodiments, the sensor used to monitor the current is selected from shunt resistors, current transformers, Rogowski coils, and magnetic field-based sensors.
[0110] As used herein, the term "voltage sensor" refers to a sensor that measures voltage in transmission lines and / or electronic circuits. Suitablely, voltage sensors are used to measure and / or regulate voltage at a power source because the voltage between a consumable electrode (a two-dimensional layered semiconductor or conductor material) and its counter electrode affects the quality of the electrochemically decomposed semiconductor or conductor material. In embodiments, the sensor used to monitor voltage is a voltage transformer.
[0111] As used herein, the term "UV / Vis sensor" refers to a sensor that measures the absorption or reflection (particularly the intensity of light after passing through the sample) of the electromagnetic spectrum in at least a portion of the UV and / or visible light regions. Appropriately, UV / Vis sensors are used to monitor electrolytes and / or washing solutions, particularly to monitor the efficiency of the washing process.
[0112] In this embodiment, the sensor used to monitor ultraviolet / visible light absorption is an ultraviolet / visible light probe (preferably a rod-shaped probe) with a hydrophobic coating (especially silicone or fluorinated polymer). In this embodiment, the light source of the ultraviolet / visible light sensor is a laser, a diode, an incandescent lamp, or a fluorescent tube.
[0113] In a further embodiment, the ultraviolet / visible light sensor includes an integrated temperature sensor.
[0114] In an embodiment, the device further includes at least one sensor for monitoring at least one gas (particularly hydrogen, oxygen, carbon monoxide, and / or carbon dioxide). Suitably, the hydrogen sensor measures the hydrogen concentration and controls the power supply to ensure that dangerous hydrogen concentrations are not reached. Suitably, the carbon monoxide and / or carbon dioxide sensors measure carbon monoxide and / or carbon dioxide in the air to ensure a harmless working environment.
[0115] In embodiments, the apparatus further includes at least one flow sensor, particularly a liquid or gas flow sensor. Suitably, the liquid flow sensor measures and / or regulates the amount of cooling water, electrolyte, washing solution, and / or solvent exchange, particularly to ensure that clogging does not occur. Suitably, the gas flow sensor measures and / or controls the exhaust gas flow, particularly to prevent hazardous gas concentrations.
[0116] In one embodiment, the device further includes at least one leak sensor. Suitable for monitoring faults, particularly leaks and / or spills.
[0117] In embodiments, the device further includes an automated electrolyte remetering unit and / or at least one quantity sensor. Suitablely, the quantity sensor (particularly a scale or level sensor for containers or storage containers) is used to measure the production, addition, consumption, and / or remetering of the electrolyte and / or the addition, consumption, and / or refilling of consumable two-dimensional layered semiconductor or conductor material.
[0118] In one embodiment, the device further includes at least one camera. Suitable for enabling remote diagnostics in the event of a malfunction. In another embodiment, the camera is connected to a movable unit to view different areas.
[0119] In one embodiment, the movable unit includes means for positioning in three-dimensional space. In another embodiment, the means for positioning in three-dimensional space is designed as a robotic arm, a triangular robot, a multi-axis system, or a hexapod robot.
[0120] In this embodiment, the device for positioning in three-dimensional space is designed as a combination of a robotic arm, a triangular robot, or a hexapod robot. This means that the movable unit can be positioned as needed; for example, the system can move in the XY direction using a hexapod robot and position itself in the Z direction using a robotic arm.
[0121] In this embodiment, the device for positioning in three-dimensional space is designed with a combination of axes, linear actuators, and / or rotary actuators, whose operating modes and degrees of freedom are coordinated to allow for the positioning of a movable unit in the X, Y, and Z directions with the desired accuracy and speed. Appropriately, information regarding the X, Y, and Z directions refers to axes in a Cartesian coordinate system.
[0122] In an embodiment, the apparatus further includes at least one metering system for re-metering the electrolyte or adjusting the electrolyte composition.
[0123] In embodiments, the apparatus further includes at least one collection hood and / or venting device. Suitably, the collection hood almost completely covers the container. In embodiments, the collection hood is segmented, including a section covering at least one first electrode and / or a feed system for conveying consumable two-dimensional layered semiconductor or conductor material into the electrolyte, and a section covering at least one second electrode. Advantageously, at least one collection hood and / or venting device is capable of collecting (preferably separately) gases (e.g., oxygen or hydrogen) generated at the anode and cathode.
[0124] In one embodiment, a collection hood and / or an exhaust device are connected to a waste treatment unit. Suitably, the waste treatment unit is used to treat the gases collected in the collection hood and / or exhaust device. These gaseous byproducts and waste gases include hydrogen and oxygen.
[0125] In one embodiment, a waste treatment unit (particularly a palladium membrane and / or activated carbon column) purifies the gas. In another embodiment, the system includes at least one fuel cell. Suitable for this purpose, the purified gas is fed into the fuel cell to generate electricity, which is then used to at least partially operate the device and reduce its overall power consumption.
[0126] In an embodiment, the apparatus further includes at least one unit for connecting consumable two-dimensional layered semiconductor or conductor material (particularly connecting one roll of consumable two-dimensional layered semiconductor or conductor material to another roll), wherein the end of the first roll is connected to the beginning of the other roll. In an embodiment, the connection is made by adhesive (particularly with conductive adhesive) or mechanical connection (particularly by folding or stamping).
[0127] In one embodiment, the apparatus further includes at least one raw material reservoir (particularly a rotating rack) having a membrane of consumable two-dimensional layered semiconductor or conductor material. Advantageously, the raw material reservoir can be used (particularly by a robot) to automatically remove new membranes and store empty membrane cores.
[0128] In one embodiment, the device is enclosed by a housing (e.g., a shipping container).
[0129] In an embodiment, the housing includes at least one connector for supplying electrical power, at least one air inlet and exhaust outlet, at least one line for electrolyte solution, water and / or other liquids, and / or at least one output for decomposed semiconductor or conductor materials and / or waste, such as used or excess electrolyte solution, liquids or solids from washing and / or purification processes, particularly from supernatants or precipitates from centrifugation and / or condensates from drying processes.
[0130] In one embodiment, the housing is equipped with a solar panel and / or a wind turbine. Suitable, the solar panel and / or wind turbine can supply electrical energy to the device.
[0131] In one embodiment, the housing is equipped with an inlet port or connection for manually replenishing raw materials or removing waste.
[0132] In embodiments, the apparatus includes at least one other movable unit for replacing the completed roll of consumable two-dimensional layered semiconductor or conductor material and / or transporting the consumable two-dimensional layered semiconductor or conductor material to a feeding system, particularly an actuator or robotic system.
[0133] As used herein, the term "actuator" refers to a device that generates motion (particularly linear or rotational motion) by converting energy and signals supplied to a system.
[0134] In an embodiment, the movable unit includes means for positioning in three-dimensional space, which is designed as a robotic arm, a triangular robot, a multi-axis system, or a hexapod robot.
[0135] In embodiments, the device for positioning in three-dimensional space is designed as a combination of a robotic arm, a triangular robot, or a hexapod robot. In embodiments, the device for positioning in three-dimensional space is designed with a combination of axes, linear actuators, and / or rotary actuators, whose operating modes and degrees of freedom are coordinated to allow for the positioning of movable units in the X, Y, and Z directions with the required accuracy and speed.
[0136] In an embodiment, at least one actuator and / or robot system is operated and / or controlled by a control unit or manually operated by an operator.
[0137] In one embodiment, the device further includes a control unit, which includes a processor configured to cause it to:
[0138] - Adjust the power supply, especially the voltage and / or current between at least one first electrode and the second electrode.
[0139] - The rate at which consumable two-dimensional layered semiconductor or conductor material is delivered into the electrolyte solution via a feeding system, and / or
[0140] - Supply and discharge of electrolyte solutions.
[0141] Any program-controlled data processing device is considered a control unit. In embodiments, a control unit has one or more hardware components and / or one or more software components. In embodiments, the control unit includes a cloud computing system, a computer network, a computer, a tablet computer, a smartphone, or a combination thereof.
[0142] In this embodiment, the hardware interacts with the software and / or can be configured using the software. The software is executed using the hardware appropriately. In this embodiment, the hardware is a memory system, a field-programmable gate array (FPGA) system, an application-specific integrated circuit (ASIC) system, a microcontroller system, a processor system, or a combination thereof.
[0143] In one embodiment, the control unit calculates the voltage between at least one first electrode and a second electrode and / or the rate at which consumable two-dimensional layered semiconductor or conductor material is delivered into the electrolyte solution based on measured conductivity, current or voltage and calibration values stored in the processor.
[0144] Advantageously, the device can operate autonomously using a control unit that monitors and processes sensor inputs and / or controls and / or continuously adjusts the feed rate of raw materials and other media.
[0145] In this embodiment, the device (particularly the control unit) is connected to the Internet and can be remotely accessed, operated, and maintained.
[0146] Another aspect of the present invention is a method for the electrochemical decomposition of consumable two-dimensional layered semiconductor or conductor materials, comprising:
[0147] a) Electrolytic stripping of consumable two-dimensional layered semiconductor or conductor materials in an electrolytic cell, the electrolytic cell comprising:
[0148] - At least one electrode pair consisting of at least one first electrode and one second electrode, and
[0149] - Containers used for electrolyte solutions,
[0150] By contacting at least one second electrode and a consumable two-dimensional layered semiconductor or conductor material with an electrolyte solution, and applying a voltage between at least one first electrode and the second electrode using a power source,
[0151] The first electrode is in contact with a consumable two-dimensional layered semiconductor or conductor material.
[0152] The second electrode is a counter electrode, disposed between at least one inner side of a consumable two-dimensional layered semiconductor or conductor material and a container for the electrolyte solution.
[0153] The first and second electrodes are connected to a power source.
[0154] b) Using a feeding system comprising at least one mesh and / or belt, continuously or intermittently deliver consumable two-dimensional layered semiconductor or conductor material into an electrolyte solution.
[0155] c) Separate the decomposed semiconductor or conductor material from the electrolyte solution.
[0156] In the embodiments, the consumable two-dimensional layered semiconductor or conductor material is a carbon-based material, preferably selected from graphite, graphite derivatives, carbon-based semiconductor or conductor polymers.
[0157] Appropriately, consumable two-dimensional layered semiconductor or conductor materials are in the form of foils, sheets, or mixtures thereof.
[0158] Preferably, the consumable two-dimensional layered semiconductor or conductor material is graphite foil.
[0159] In this embodiment, the electrolyte solution is an aqueous solution. In this embodiment, the electrolyte solution contains at least one polar organic solvent, such as propylene carbonate or acetonitrile.
[0160] In the embodiments, the electrolyte solution contains at least one dissolved salt or at least one dissolved salt and sulfuric acid, wherein the at least one salt is selected from sulfates, bisulfates, persulfates and / or perchlorates.
[0161] In this embodiment, when electrolytic stripping begins in step a), the first and second electrodes are periodically reversed. The polarity is reversed by applying an alternating voltage between the first and second electrodes.
[0162] In this embodiment, the voltage in step a) is in the range of 1 V to 20 V. In this embodiment, the voltage is in the range of + / - 2 V to + / - 20 V, preferably in the range of + / - 5 V to + / - 15 V.
[0163] In an embodiment, step b) involves delivering the consumable two-dimensional layered semiconductor or conductor material into the electrolyte solution by applying a constant rate or by maintaining a constant current (possibly at a varying rate, preferably a constant current).
[0164] In an embodiment, step b) involves feeding the consumable two-dimensional layered semiconductor or conductor material into the electrolyte solution at a feed rate depending on the thickness of the consumable two-dimensional layered semiconductor or conductor material and the applied current. In another embodiment, step b) involves feeding the consumable two-dimensional layered semiconductor or conductor material into the electrolyte solution at a feed rate ranging from 0.1 mm / min to 10 cm / min.
[0165] In an embodiment, the method further includes washing, processing, and / or drying the decomposed semiconductor or conductor material.
[0166] In this embodiment, the method, particularly steps a) and / or b), is performed manually by a field operator.
[0167] In this embodiment, step a) and / or step b) are regulated by the control unit.
[0168] It also includes a computer program product comprising instructions that, when executed by a computer, cause the computer to perform steps a) and / or b) of the method.
[0169] In this embodiment, the computer program product is designed to be loaded into the processor of the control unit.
[0170] This invention is not limited to the specific combination of features described, but can also be defined by any other combination of all the individual features disclosed, provided that the individual features are not mutually exclusive, or that the individual features of a particular combination are not explicitly excluded.
[0171] The project for which this application was submitted has been funded by the EU Research and Innovation Programme 2020 under Funding Agreement No. 649953.
[0172] The invention will be explained in more detail below by way of examples. These examples are intended to describe the invention but not to limit it.
[0173] Embodiments of the present invention will be described by way of example only with reference to the accompanying drawings, wherein:
[0174] Figure 1 The system according to the invention is shown in a side view (narrow side). A consumable two-dimensional layered semiconductor or conductor material 1 (particularly graphite foil) is conveyed by a feeding system 3 (particularly a mesh or belt) in a container 2 for an electrolyte solution, wherein an electrode pair 4, consisting of at least one first electrode and a second electrode, is connected to a power source 7. The first electrode is in contact with the consumable two-dimensional layered semiconductor or conductor material 1 via a sliding contact 6 and is not in contact with the electrolyte solution. The second electrode is a non-consumable counter electrode arranged between the consumable two-dimensional layered semiconductor or conductor material 1 and at least one inner side of the container 2.
[0175] Figure 2 The system according to the invention is shown in a side view (longitudinal side). A consumable two-dimensional layered semiconductor or conductor material 1 (particularly graphite foil) is conveyed by a feeding system 3 (particularly a mesh or belt) in a container 2 for an electrolyte solution. A first electrode is in contact with the consumable two-dimensional layered semiconductor or conductor material 1 via a sliding contact 6 and not with the electrolyte solution. A second electrode, a non-consumable counter electrode, is arranged between at least one inner side of the consumable two-dimensional layered semiconductor or conductor material 1 and the container 2. After electrolysis of the consumable two-dimensional layered semiconductor or conductor material 1 (particularly graphite foil), the electrochemically decomposed semiconductor or conductor material on the surface of the electrolyte solution is removed through an outlet (particularly an overflow port 5).
[0176] Figure 3An automated, autonomous system according to the invention, integrated into a housing 23, is illustrated: a consumable two-dimensional layered semiconductor or conductor material 1 (particularly graphite foil) is conveyed by a feeding system 3 (particularly a mesh or belt) in a container 2 for an electrolyte solution. The container 2 includes an electrode pair 4 consisting of at least one first electrode and a second electrode, an outlet 5 (particularly an overflow port), a sliding foil contact 6, and is connected to a power source 7. An electrolyte stream continuously enters the container, supplied by an electrolyte recovery system 8 and an electrolyte feeding system 9. A mixture 10 of electrochemically decomposed semiconductor or conductor material and attached electrolyte is conveyed to a separation unit 11, where a concentrated slurry 12 of the electrochemically decomposed semiconductor or conductor material and the electrolyte 8 are separated. The concentrated electrochemically decomposed semiconductor or conductor material is then transferred to a washing unit 13, which uses washing water 14 to produce purified electrochemically decomposed semiconductor or conductor material 15 and wastewater 16. The wastewater is treated in a waste treatment unit 17, which feeds clean water 18 back to the electrolyte recovery and feeding systems 8 and 9 and discharges residual waste 19. The purified electrochemically decomposed semiconductor or conductor material 15 is then fed into a processing unit 20, which produces processed electrochemically decomposed semiconductor or conductor material 21. In this example, the entire system is housed in a housing 23, which is equipped with various inlets and outlets for the necessary raw materials, waste, and product streams, including an exhaust port 22 for process gases, and is autonomously operated by a control unit 24.
[0177] according to Figure 1 and Figure 2The system enables a method for the electrochemical decomposition of a consumable two-dimensional layered semiconductor or conductor material (particularly graphite foil 1), comprising electrolytic stripping of the graphite foil in an electrolytic cell comprising an electrode pair 4 consisting of a first electrode and a second electrode made of titanium and a container for an electrolyte solution 2 (25 mM sulfuric acid solution), by contacting the second electrode and the graphite foil 1 with the electrolyte solution and applying a voltage of 10 V between the first electrode and the second electrode using a power supply 7, wherein the first electrode is in contact with the graphite foil 1 but not with the electrolyte solution, wherein the second electrode is a non-consumable counter electrode arranged between the graphite foil 1 (the distance between the counter electrode and the graphite foil is approximately 5 cm) and at least one inner side of the container for the electrolyte solution, wherein the first electrode and the second electrode are connected to the power supply 7. Subsequently, graphite foil 1 is continuously or intermittently (preferably semi-continuously) fed into the electrolyte solution using a feeding system 3 at a constant current or a speed of approximately 10 cm / h. The feeding system comprises two mesh-like, insulated strips made of polypropylene placed on either side of the graphite foil. The feeding system is arranged in a container such that its upper roller is above the electrolyte solution and its lower part is immersed in the electrolyte solution. Decomposed graphite foil particles (graphene aggregates) are separated from the electrolyte solution using a filter; in particular, graphene on the surface of the electrolyte solution is removed from the system through an overflow port and then removed from the electrolyte solution through a filter. The electrolyte can be returned to the container after filtration, particularly through at least one connecting element (e.g., a hose) to the inlet. Alternatively, the electrolyte can be re-metered.
[0178] In a further example, the device also includes a scraper at the bottom of the container that scrapes together the electrochemically decomposed semiconductor or conductor material. Cited non-patent literature Chen CH, Yang SW, Chuang MC, Woon WY, Su CY (2015) Towards the continuous production of high crystallinity graphene via electrochemical exfoliation with molecular in situ encapsulation. Nanoscale 7, 15362–15373. Coleman JN (2013) Liquid Exfoliation of Defect-Free Graphene. Accounts of Chemical Research 46(1), 14-22. Ejigu A, Kinloch IA, Dryfe RAW (2017) Single Stage Simultaneous Electrochemical Exfoliation and Functionalization of Graphene. ACS Applied Materials & Interfaces 9(1), 710-721. Gómez-Navarro C, Weitz RT, Bittner AM, Scolari M, Mews A, Burghard M, Kern K. (2007) Electronic transport properties of individual chemically reduced graphene oxide sheets. NanoLett. 7(11), 3499-3503. Hummers WS, Offeman RE (1958) Preparation of Graphitic Oxide. Journal of the American Chemical Society 80(6), 1339-1339. Liu N, Luo F, Wu H, Liu Y, Zhang C, Chen J (2008) One-Step Ionic-Liquid-Assisted Electrochemical Synthesis of Ionic-Liquid-Functionalized Graphene Sheets Directly from Graphite. Adv. Funct. Mater. 18, 1518–1525. Novoselov KS, Geim AK, Morozov SV, Jiang D, Zhang Y, Dubonos SV, Grigorieva IV, Firsov AA (2004) Electric Field Effect in Atomically ThinCarbon Films. Science 306, 666-669. Rao KS, Sentilnathan J, Cho HW, Wu JJ, Yoshimura M (2015) Soft Processing of Graphene Nanosheets by Glycine-Bisulfate Ionic-Complex-Assisted Electrochemical Exfoliation of Graphite for Reduction Catalysis. Adv. Funct. Mater. 25, 298-305. Xia ZY, Pezzini S, Treossi E, Giambastiani G, Corticelli F, Morandi V, Zanelli A, Bellani V, Palermo V (2013) The Exfoliation of Graphene in Liquids by Electrochemical, Chemical, and Sonication-Assisted Techniques: A Nanoscale Study. Adv. Funct. Mater. 23, 4684-4693. List of reference numerals 1. Consumable two-dimensional layered semiconductor or conductor materials, especially graphite foil. 2 Electrolyte container 3. Feeding systems, particularly mesh belts or conveyor belts, for conveying consumable two-dimensional layered semiconductor or conductor materials into an electrolyte. 4. An electrode pair consisting of at least one first electrode and one second electrode. 5. Outlets, especially overflow outlets 6. Sliding foil contact 7 Power Supply 8 Electrolyte Circulation System 9 Electrolyte Supply System 10. A mixture of electrolyte and dissociated semiconductor or conductor material. 11 Separation Unit 12. Paste of dissociated semiconductor or conductor material 13 Washing Units 14 Washing water 15. Purified dissociated semiconductor or conductor materials 16 Wastewater 17 Wastewater Treatment Unit 18 Purified Water 19 Waste Discharge Outlets 20 processing units 21. Processed dissociated semiconductor or conductor materials 22 Exhaust port 23. Housing / Chassis 24 Control Unit
Claims
1. An apparatus for the electrochemical decomposition of an energy-consuming two-dimensional layered semiconductor or conductor material (1), said apparatus comprising: i. At least one electrolytic cell, said electrolytic cell comprising - At least one electrode pair consisting of at least one first electrode and a second electrode (4), and - Container for electrolyte solution (2) ii. Power supply (7), iii. A feeding system (3) for conveying energy-consuming two-dimensional layered semiconductor or conductor material into an electrolyte, said feeding system (3) comprising at least one mesh and / or belt, The first electrode is in contact with the energy-consuming two-dimensional layered semiconductor or conductor material (1). The second electrode is a counter electrode, which is disposed between at least one inner side of the energy-consuming two-dimensional layered semiconductor or conductor material (1) and the container (2). The first electrode and the second electrode are connected to the power supply (7).
2. The apparatus according to claim 1, wherein, The first electrode is connected to the power supply (7) as an anode, and the second electrode is connected to the power supply (7) as a cathode.
3. The apparatus according to claim 1 or 2 further comprises at least one unit for collecting and / or separating (11) electrochemically decomposed semiconductor or conductor material from the electrolyte solution.
4. The apparatus according to claim 3, wherein, The collection and / or separation unit (11) is selected from filters, centrifuges, scrapers, pumps and / or air nozzles.
5. The apparatus according to any one of claims 1 to 4, wherein, The container for the electrolyte solution includes at least one inlet and at least one outlet (5), wherein the outlet is connected to the inlet via at least one connecting element, and The separation unit (11) is located between the outlet (5) and the inlet.
6. The apparatus according to any one of claims 1 to 5, wherein, At least one outlet (5) of the container is configured as an overflow outlet and / or located on the side or bottom of the container (2).
7. The apparatus according to any one of claims 1 to 6, wherein, The feeding system (3) includes at least two mesh-like non-conductive strips placed on both sides of the consumable two-dimensional layered semiconductor or conductor material (1). The energy-consuming two-dimensional layered semiconductor or conductor material is arranged at least partially in the container (2) such that it is at least partially surrounded by the electrolyte solution.
8. The apparatus according to any one of claims 1 to 7, wherein, The net or belt is made of polyethylene or polypropylene.
9. The apparatus according to any one of claims 1 to 8, wherein, The electrolytic cell includes another counter electrode, wherein the consumable two-dimensional layered semiconductor or conductor material (1) is arranged between the two counter electrodes.
10. The apparatus according to any one of claims 1 to 9, further comprising at least one cooling unit, wherein, The cooling unit is arranged in or connected to the at least one first electrode, the at least one second electrode, the container (2) for the electrolyte solution, and / or between the at least one inlet and at least one outlet (5) of the container.
11. The apparatus according to any one of claims 1 to 10, further comprising at least one sensor for monitoring at least one process parameter, said at least one process parameter preferably selected from temperature, conductivity, current, voltage and / or ultraviolet / visible light absorption.
12. A method for the electrochemical decomposition of an energy-consuming two-dimensional layered semiconductor or conductor material, the method comprising: a) Electrolytically stripping energy-consuming two-dimensional layered semiconductor or conductor material (1) in an electrolytic cell, said electrolytic cell comprising... - At least one electrode pair consisting of at least one first electrode and a second electrode (4), and - A container for the electrolyte solution (2), By contacting at least one second electrode and the energy-consuming two-dimensional layered semiconductor or conductor material (1) with an electrolyte solution, and applying a voltage between the at least one first electrode and the second electrode using a power source (7), The first electrode is in contact with the energy-consuming two-dimensional layered semiconductor or conductor material (1). The second electrode is a counter electrode, which is disposed between at least one inner side of the consumable two-dimensional layered semiconductor or conductor material (1) and the container for the electrolyte solution (2). The first electrode and the second electrode are connected to the power supply (7). b) Using a feeding system (3) comprising at least one mesh and / or belt, the energy-consuming two-dimensional layered semiconductor or conductor material (1) is continuously or intermittently fed into the electrolyte solution. c) Separating the decomposed semiconductor or conductor material from the electrolyte solution.
13. The method according to claim 12, wherein, The energy-consuming two-dimensional layered semiconductor or conductor material (1) is a carbon-based material, preferably selected from graphite, graphite derivatives, carbon-based semiconductor or conductor polymers.
14. The method according to claim 12 or 13, wherein, The voltage in step a) is in the range of 1 V to 20 V, and / or wherein the delivery of the energy-consuming two-dimensional layered semiconductor or conductor material (1) into the electrolyte solution in step b) is performed by applying a constant rate or a constant current.
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