Hydrogen Production System

Abstract

A system and method for producing hydrogen gas. The system includes at least one reformer reactor, at least one separator, at least one separator transport line, at least one regenerator reactor, at least one regenerator transport line, and at least one recycle line. The reformer reactor is configured to convert spent adsorbent A into a regenerator. * The reformer reactor is configured to accommodate a sorbent A that captures CO forming H2 and CO2 and to reform a feedstock B and steam C to produce a reformed gas mixture comprising H2 and CO2. The reformer reactor includes a reformer inlet for supplying at least one of B and C to the reformer reactor, and a reformer inlet for supplying H2 and CO2 to the reformer reactor. * and a reformer outlet for discharging H2. * The separator is configured to separate H2 and A from H2. * a separator inlet for supplying the separated A * and a separator outlet for discharging the separator. The separator conveying line is * and H2 are transported from the reformer outlet to the separator inlet. The regenerator reactor is * The regenerator power source is configured to receive at least a portion of the A to regenerate the sorbent by allowing the release of CO2. * The regenerator outlet discharges the regenerated adsorbent. The regenerator conveying line is configured to supply sufficient energy to the * The recycle line is arranged to transport at least a portion of the regenerated adsorbent from the regenerator outlet to the reformer reactor. The regenerator transport line transports the A stream transported to the regenerator inlet. * The flow regulator is configured to regulate the flow rate of the

Description

[Technical field]

[0001] The present invention relates to hydrogen production and methods thereof. More particularly, the present invention relates to a system and method for producing hydrogen gas in which a sorbent is used to capture carbon dioxide produced during a reforming reaction in a reformer reactor, and the spent sorbent is separated and controllably fed to a regenerator reactor. [Background technology]

[0002] As the use of hydrogen fuel as an energy carrier is rapidly increasing, the supply of hydrogen to industrial users has become a major business worldwide.

[0003] Hydrogen can be extracted from fossil fuels or biomass, from water, or from a mixture of both. Currently, the primary source for hydrogen production is natural gas.

[0004] Currently, hydrogen fuel is produced in a variety of ways. The most common methods are natural gas / methane reforming, coal gasification, and electrolysis. Other methods include solar-driven and bioprocesses. See, for example, https: / / www.energy.gov / eere / fuelcells / hydrogen-fuel-basics

[0005] [Conventional SMR] In conventional steam methane reforming (SMR), steam reacts with methane in the presence of a catalyst at high temperature (800-1000 °C) and pressure (15-20 bar) to produce a gas mixture consisting of hydrogen (H2) and carbon monoxide (CO), see reaction (2.1). Carbon monoxide is then reacted with steam over a catalyst in the water-gas shift reaction (2.2) to produce carbon dioxide (CO2) and additional hydrogen in a low temperature (300-400 °C) environment. The hydrogen gas is then separated from the CO2 in multiple steps, for example by pressure swing adsorption, until the desired hydrogen purity is achieved.

[0006] The main reactions in a conventional SMR are as follows: Reformation: CH4(g)+H2O(g) ⇔ CO(g)+3H2(g) (2.1) Shift: CO(g) + H2O(g) ⇔ CO2(g) + H2(g) (2.2) Total: CH4(g)+2H2O(g) ⇔ CO2(g)+4H2(g) (2.3)

[0007] Conventional SMRs suffer from several drawbacks, including the need for a large fixed bed to minimize pressure drop, catalyst deactivation due to carbon formation, and the need to maintain high reactor temperatures because only a portion of the heat of combustion is used directly in the process.

[0008] [Sorption-enhanced SMR (SE-SMR)] The sorption-enhanced steam methane reforming (SE-SMR) process reduces the processing steps by adding a CO2 sorbent, such as calcium oxide (CaO) or dolomite, to the reformer reactor along with the catalyst. When the sorbent is added to the reactor, the CO2 is converted to solid carbonate (CaCO3) in an exothermic calcination reaction (2.4), so that the product gas from the reformer consists mainly of H2 and H2O with small amounts of CO, CO2 and unconverted CH4 (fuel gas). Thus, the addition of the sorbent shifts reactions (2.1)-(2.3) in the forward direction, improving methane conversion and hydrogen yield. The exothermic reaction results in a mostly self-heating process with temperatures ranging from 550°C to 650°C.

[0009] The main reactions in SE-SMR are, in addition to reactions (2.1)-(2.2), the following: Carbonation: CaO(s) + CO2(g) ⇔ CaCO3(s) (2.4) Total: CH4(g)+2H2O(g)+CaO(s) ⇔ CaCO3(s)+4H2(g) (2.5)

[0010] In continuous production, the carbonate sorbent saturated with CO2 is then delivered to the regenerator reactor and subjected to high temperatures to ensure the endothermic calcination reaction (2.6) occurs. Calcination / regeneration: CaCO3(s) ⇔ CaO(s) + CO2(g) (2.6)

[0011] Depending on the reactor configuration, the saturated sorbent is heated to approximately 900° C. due to the endothermic reaction that releases CO2 from the carbonated limestone, CaCO3.

[0012] The resulting regenerated sorbent (CaO) is then returned to the reformer reactor and the CO2 released from the spent sorbent is transported to an external location (typically a CO2 processing or storage facility).

[0013] The heat supplied to the regenerator reactor must raise the temperature of the saturated sorbent entering the bed while providing enough excess heat for the calcination reaction to take place. The heat source may be, for example, waste heat from a solid oxide fuel cell (SOFC). The sorbent saturated with CO2 is usually referred to as "spent sorbent".

[0014] The above SE-SMR can be carried out in both fixed bed and fluidized bed reactors. However, the use of a fluidized bed reactor is believed to be advantageous due to the possibility of continuous fluid / particulate feed and withdrawal (thus allowing for a higher degree of continuous operation), efficient and near isothermal heat distribution, efficient mixing of the chemical reactants, greater suitability for large scale operation, low pressure drop, and high heat transfer between the bed and the immersion body.

[0015] The fluidizing medium for the SE-SMR regenerator can in principle be any gas that can be easily separated from the CO2. Steam condenses at a much higher temperature than CO2, so in this respect water vapor seems ideal. The fluidizing medium for the SE-SMR reformer is usually a mixture of water vapor and hydrocarbon gas, with the ratio S / C between water vapor and hydrocarbon gas being between 2.5 / 1 and 4 / 1.

[0016] SE-SMR is known in the art. See, for example, WO 2016 / 191678, which discloses a hydrogen production system by sorption-enhanced reforming. In this prior art system, the sorbent material CaO in the reformer reactor acts to adsorb CO2 to form spent sorbent in the form of CaCO3. The spent sorbent is further guided to a regenerator reactor at atmospheric pressure, which heats the spent sorbent to desorb CO2 from the spent sorbent, thereby producing regenerated sorbent that is recycled to the reformer reactor. Other examples of sorption-enhanced SMR are described in U.S. Pat. No. 8,241,374, WO 2018 / 162675 search report, WO 2018 / 148514, and U.S. Patent Application Publication No. 2019 / 0112188.

[0017] None of the systems described in the above mentioned patent publications provide any information regarding the control of the flow rate of the spent adsorbent between the reformer reactor and the regenerator reactor.

[0018] It is therefore an object of the present invention to enable control of the flow rate of spent sorbent within the system. Summary of the Invention

[0019] The invention is set forth and characterized in the independent claims, with further characteristic features of the invention being set forth in the dependent claims.

[0020] In a first aspect, the present invention relates to a system for producing hydrogen gas, H2.

[0021] The system includes at least one reformer reactor, at least one separator, at least one separator transport line, at least one regenerator reactor, at least one regenerator transport line, and at least one recycle line.

[0022] The reformer reactor(s) may be configured to convert the spent sorbent A into a gas when conditions exist for capturing carbon dioxide, such as a minimum pressure and / or a minimum temperature and / or a minimum amount per volume unit. * The reformer reactor has an enclosed volume for housing an adsorbent A that captures carbon dioxide forming a carbon dioxide gas. The reformer reactor is configured to enable reforming of a feedstock B (such as a hydrocarbon fuel) with steam C (i.e., primarily water in the gas phase) to produce a reformed gas mixture comprising hydrogen gas H2 and carbon dioxide CO2. The reformer reactor has at least one reformer inlet for supplying at least one of the feedstock B and the steam C to the reformer reactor, and a spent adsorbent A that captures carbon dioxide forming a carbon dioxide gas. * and at least one reformer outlet for discharging hydrogen gas H2. More preferably, the reformer reactor includes at least two reformer inlets including a feed inlet and a steam inlet. The reformer reactor may include an additional inlet for supplying a carbon dioxide capturing sorbent to the reformer reactor.

[0023] The separator(s), e.g., a cyclone, separates the spent adsorbent A * The separator(s) is configured to separate the hydrogen gas H2 and the used adsorbent A. * at least one separator inlet for supplying the separated spent adsorbent A to the separator(s); * and at least one separator outlet for discharging the separator.

[0024] The separator conveying line(s) conveys the spent adsorbent A. * and is suitable for transporting hydrogen gas H2 from the reformer outlet to the separator inlet.

[0025] In a preferred configuration, the reformer reactor has two reformer outlets and one reformer outlet located at the top of the reformer reactor for discharging gas (mainly hydrogen gas H2) and a reformer outlet located at the top of the reformer reactor for discharging mainly spent adsorbent A. * and one reformer outlet located at the bottom of the reformer reactor for discharging the hydrogen gas H2 and the spent adsorbent A. In this configuration, *The hydrogen gas H2 stream and the spent adsorbent A are mixed in the separator conveying line(s) and flow into the separator(s). * If vertical transport is required, it may be advisable to install a dedicated vertical transport device such as a transport riser. An example of such a transport riser may be a section of piping with a diameter that ensures particle entrainment by the transport gas (i.e., the gas velocity is high enough) and with a lower portion that prevents or limits particle deposition.

[0026] Further, the regenerator reactor(s) may be configured to regenerate the spent adsorbent A separated in the separator(s). * at least one regenerator inlet for receiving at least a portion of the spent adsorbent A; * at least one regenerator power source configured to supply energy to the adsorbent A to enable the release of carbon dioxide CO2, thereby regenerating the adsorbent A; at least one regenerator outlet for discharging the regenerated adsorbent A; and * from the separator outlet(s) to the regenerator inlet(s), and at least one recycle line configured to transport at least a portion of the regenerated adsorbent A from the regenerator outlet(s) to the reformer reactor(s), e.g., via one or more reformer inlets or via one or more dedicated recycle inlets.

[0027] The regenerator conveying line, or each of the regenerator conveying lines, advantageously conveys the spent adsorbent A to the regenerator inlet. * Flow rate R A* [m 3 The device may include at least one flow regulator configured to adjust the flow rate [ / s (sec) or kg / s].

[0028] In one exemplary configuration of the present invention, the regenerator transport line is configured to transport the separated spent adsorbent A *The method further comprises at least one tank for containing the separator, at least one first regenerator conveying line having one end coupled to the separator outlet(s) and the other end coupled to at least one tank inlet of the tank, and at least one second regenerator conveying line having one end coupled to at least one tank outlet of the tank and the other end coupled to the regenerator inlet. One or more measuring devices(s) are connected to the tank for measuring the amount of spent adsorbent A stored in the tank. * The amount of can be measured.

[0029] In another exemplary configuration of the present invention, the regenerator transport line(s) may include a regenerator transport line(s) for transporting the separated spent adsorbent A through the regenerator transport line(s). * The valve(s) may be located in the first regenerator transfer line, for example, to stop or open the flow to the tank(s).

[0030] In yet another exemplary configuration of the present invention, the flow control device(s) may include a flow control device for controlling the flow of spent adsorbent A to the regenerator reactor(s). * Flow rate R A* Adjustable rotation speed to adjust the V r The conveyor includes at least one screw conveyor arranged to rotate at a speed of about 10000 rpm. A screw conveyor is generally a mechanism that uses rotating, helical screw blades that allow the movement of liquids and / or solids, such as particulate matter.

[0031] The screw conveyor is preferably arranged such that the screw conveyor has a higher rotation speed v r;H and lower rotation speed v r,L When the two are rotating at the same speed, the used adsorbent A * but at higher flow rates R A*,H and lower flow rate R A*,L to the regenerator reactor.

[0032] Furthermore, the flow rate adjusting device is preferably rotatably connected to the screw conveyor, whereby said adjustable rotation speed v r and a variable speed drive / frequency converter connected to the motor and enabling control of the rotational speed of the motor and thereby the rotational speed of the screw conveyor.

[0033] In yet another exemplary configuration of the present invention, the system further includes an automatic controller in signal communication with the flow regulator (e.g., a variable speed drive) and / or directly with the motor. In this exemplary configuration, the controller automatically controls operation of the flow regulator to thereby reduce or increase the flow rate R based on at least one of the following: A* The control circuitry may be designed and programmed to automatically control: the flow rate of feed B entering the reformer reactor; Flow rate of steam C entering the reformer reactor Flow rate of the mixture of feedstock B and steam C entering the reformer reactor Spent adsorbent A flows between the reformer outlet and the regenerator inlet * Flow rate of, A flow rate of at least carbon dioxide CO2, and preferably also carbon monoxide CO, flowing between the reformer and the regenerator inlet - Flow rate of gas (mainly hydrogen gas) exiting the separator.

[0034] In yet another exemplary configuration of the present invention, the system further includes an automatic controller in signal communication with the flow regulator, the controller automatically controlling operation of the flow regulator to thereby reduce the flow rate R based on at least one of the following: A* is configured to automatically control The composition ratio of feed material B to the total flow rate of steam C and feed material B flowing into the reformer reactor The composition ratio of the liquid compounds (typically H2, CO, CO2, and CH4) flowing between the reformer outlet and the regenerator inlet The gas composition ratio between carbon monoxide (CO) and unreacted fuel gas (typically CH4) flowing between the reformer outlet and the regenerator inlet The gas composition ratio between carbon dioxide (CO2) and unreacted fuel gas (typically CH4) flowing between the reformer outlet and the regenerator inlet Measurement of the general gas composition in the hydrogen line, for example to detect degradation of CO2 capture in the reformer reactor (200)

[0035] Measurement of the gas composition can be accomplished by several known measurement techniques, such as gas chromatography.

[0036] In yet another exemplary configuration of the present invention, the regenerator reactor encloses an internal volume and contains spent adsorbent A * The regenerator further includes a regenerator vessel into which the heat exchanger gas may flow. In this configuration, a regenerator power source is disposed outside the regenerator vessel and is capable of providing power within the interior volume.

[0037] The regenerator power source located outside the vessel may be a heat source such as a burner or waste heat, for example from a high temperature solid oxide fuel cell (SOFC), thereby ensuring the release of carbon dioxide from the spent sorbent by indirectly supplying heat through the vessel wall. The burner may be a gas burner, a coal burner, an oxy-fuel burner and / or an oil burner. Indirect heat exchange between the power source and the regenerator may require the incorporation of a high temperature heat exchanger in the regenerator bed to transfer heat from the power source to the regenerator bed material.

[0038] Alternatively or additionally, at least a portion of the power source or an additional power source may be located inside the regenerator vessel, typically at the bottom of the vessel, whereby energy such as hot gases is converted into spent adsorbent A. *The combustion products from the internal power source (e.g., from an oxy-fuel burner) may be used for other purposes, such as fluidizing the regenerator bed. If the power source is an oxy-fuel burner, direct heat transfer between the power source and the regenerator may require the use of an air separation unit to supply oxygen to the oxy-fuel burner.

[0039] In yet another exemplary configuration of the present invention, the system comprises: * and at least one hydrogen transfer line for transferring the separated hydrogen gas H2 stream from the at least one second separator outlet to one or more external locations. The at least one external location may be a location including equipment for purifying at least a portion of the hydrogen gas H2 stream.

[0040] In yet another exemplary configuration of the present invention, the system comprises: * and at least one CO2 transport line for transporting the carbon dioxide CO2 stream released from the at least one second regenerator outlet to one or more external locations. The at least one external location may be a location including a facility for storing at least a portion of the carbon dioxide CO2 stream.

[0041] In a second aspect, the invention relates to a system, as described above, in which the reformer reactor comprises a quantity of feedstock B and a quantity of steam C. Feedstock B may comprise one or more of the following: a hydrocarbon-containing fuel, such as natural gas, methane-rich gas, synthesis gas, a mixture of methane-rich gas and synthesis gas, gas from the gasification of organic matter, such as biomass or carbon / hydrocarbons, and gas hydrates.

[0042] In an exemplary configuration of the second aspect of the present invention, the reformer reactor includes a quantity of adsorbent A. Adsorbent A may be a metal oxide such as calcium oxide, and the spent adsorbent A may be a * may be a metal carbonate such as calcium carbonate.

[0043] In another exemplary configuration of the second aspect of the present invention, the reformer reactor(s) and / or the regenerator reactor(s) comprise a fluidized bed, thereby achieving several advantages, such as, for example, a larger contact surface area between the adsorbent A and the reformed gas mixture B, C, enhanced or improved temperature uniformity, and / or increased heat transfer.

[0044] In another exemplary configuration of the second aspect of the present invention, the reformer reactor comprises: i) a reformer reactor configured to support sorption-enhanced steam methane reforming; ii) a reformer reactor configured to support a sorption-enhanced water-gas shift; or iii) a combination of i) and ii).

[0045] In a third aspect, the present invention relates to a method for producing hydrogen gas H2 using the system described above.

[0046] The method comprises the following steps: A. introducing a feedstock B (such as a hydrocarbon fuel) and steam C into a reformer reactor(s) via one or more reformer inlets, the reformer reactor(s) including an adsorbent A for capturing carbon dioxide CO2; B. Reforming the feedstock B and steam C in the reformer reactor(s) to produce a reformed gas mixture comprising hydrogen gas H2 and carbon dioxide CO2, wherein the adsorbent A captures the carbon dioxide CO2 and converts it into spent adsorbent A. * reforming feed B and steam C to form C. Used adsorbent A * and at least a portion of the hydrogen gas H2 from the reformer reactor(s) to a separator(s) via a separator conveying line(s); D. Separator (s) is operated to separate spent adsorbent A. * from hydrogen gas H2; E. By operating the adjustment device, used adsorbent A * Flow rate R A* While adjusting the amount of used adsorbent A, * from the separator to a regenerator reactor via a regenerator transfer line; F. Spent adsorbent A in regenerator reactor(s) * The purpose of the present invention is to supply energy such as heat to the used adsorbent A. * providing energy to release at least a portion of the carbon dioxide CO2 captured by the adsorbent A of step A, thereby at least partially regenerating the adsorbent A of step A; G. Recycling at least a portion of the regenerated adsorbent A of step F by conveying the regenerated adsorbent A from the regenerator reactor(s) to the reformer reactor(s) via a recycle line(s); Includes.

[0047] The adsorbent A may be a metal oxide such as calcium oxide, and the spent adsorbent A * may be a metal carbonate such as calcium carbonate.

[0048] The heat provided by the regenerated sorbent A recycled via the recycle line(s) may be sufficient to ensure the desired process in the reformer reactor to produce reformed gas and capture carbon dioxide CO2 in the sorbent A. However, the reformer reactor may also be equipped with a separate power source, such as an external heat source.

[0049] In an exemplary process of the third aspect of the present invention, the flow rate control device includes at least one screw conveyor, and the flow rate R in step E is A* The adjustment is done by adjusting the rotation speed of the screw conveyor v r This is achieved by adjusting

[0050] In another exemplary process of the third aspect of the present invention, in step E, the rotation speed v of the screw conveyor(s) is r Adjusting the amount of used adsorbent A* one or more higher flow rates R A*,H The screw conveyor(s) are rotated at one or more higher rotational speeds vr ,H and the used adsorbent A * one or more lower flow rates R A*,L The screw conveyor(s) are rotated at one or more lower rotational speeds v to convey the regenerator reactor(s) at r,L and adjusting the

[0051] In yet another exemplary process of the third aspect of the present invention, the flow regulator further comprises at least one motor rotatably connected to the screw conveyor(s) and at least one variable speed drive connected to the motor(s).

[0052] In this exemplary method, the rotation speed v of the screw conveyor(s) in step E r The step of adjusting the motor(s) may include operating a variable speed drive to vary the rotational speed(s) of the motor(s), thereby adjusting the rotational speed v of the screw conveyor(s) connected to the motor(s). r The method may further include adjusting the

[0053] In yet another exemplary process of the third aspect of the present invention, the regenerator transport line(s) further comprises at least one valve, and step E comprises: * and further operating the valve(s) to open or stop the flow(s).

[0054] In yet another exemplary process of the third aspect of the present invention, the regenerator transport line(s) is / are transported through the separated spent adsorbent A. *at least one tank for containing the separated spent adsorbent A; at least one first regenerator transfer line having one end coupled to the separator outlet(s) and the other end coupled to the tank inlet(s) of the tank(s); and at least one second regenerator transfer line having one end coupled to the tank outlet(s) of the tank(s) and the other end coupled to the regenerator inlet(s); and step E comprises transferring the separated spent adsorbent A * The system further includes filling the tank(s) to a predetermined minimum amount(s) of spent sorbent A stored in the tank(s). * The method may further comprise at least one measuring device for measuring the amount(s) of.

[0055] The valve(s) mentioned above can be located, for example, in the first regenerator transfer line to stop or open the flow(s) to the tank(s) described below.

[0056] In yet another exemplary process of the third aspect of the present invention, the regenerator reactor(s) is / are used to regenerate the spent adsorbent A. * In this exemplary process, the regenerator power source(s) may be located outside the regenerator vessel to provide indirect heating to the regenerator vessel, and the spent adsorbent A in the regenerator reactor may be heated to 1000° C. and 1000° C. in the regenerator reactor. * The step F of providing energy to the regenerator may include transporting energy, such as heat, from the regenerator power source(s) into the regenerator vessel.

[0057] In yet another exemplary process of the third aspect of the present invention, the step of reforming the feedstock (B) and steam (C) comprises reforming using a reformer reactor (100) selected from the group consisting of: i) a reformer reactor configured to support sorption enhanced steam methane reforming, ii) a reformer reactor configured to support sorption enhanced water gas shift, or iii) a combination of i) and ii).

[0058] In yet another exemplary process of the third aspect of the present invention, the reformer reactor(s) is operated at a pressure of at least 1.1 bar absolute, more preferably at least 1.3 bar absolute.

[0059] In yet another exemplary process of the third aspect of the present invention, the regenerator reactor(s) is operated at a pressure of at least 1.1 bar (absolute), more preferably at least 1.3 bar (absolute).

[0060] In yet another exemplary process of the third aspect of the present invention, the method further comprises, during step D, separating spent adsorbent A in separator(s). * The method further includes conveying the separated hydrogen gas H2 stream from the separator(s) via the second separator outlet(s) to external location(s).

[0061] In yet another exemplary process of the third aspect of the present invention, the external location(s) may be a location that includes an arrangement for purifying at least a portion of the stream(s) of hydrogen gas H. The purification step may include pressure swing adsorption.

[0062] In yet another exemplary process of the third aspect of the present invention, the method further comprises, during step F, removing spent adsorbent A from the regenerator vessel. * The method further includes conveying the stream of carbon dioxide CO2 released from the regenerator reactor to an external location via a dedicated CO2 outlet.

[0063] In yet another exemplary process of the third aspect of the present invention, the external location may be a location that includes facilities for processing and / or storing at least a portion of the carbon dioxide CO2 stream.

[0064] In the hydrogen production system using the SE-SMR described above, used adsorbent A * Flow rate R A* By being able to control the amount of heat generated, several advantages are achieved.

[0065] By adjusting the flow rate control device (e.g., the rotation speed of the screw conveyor), the used adsorbent A transported through the regenerator transport line is * Flow rate R A* By controlling the flow rate regulator, the amount of solids / used sorbent flowing into the regenerator reactor can be controlled. And since the regenerated sorbent A in the regenerator reactor is returned to the reformer reactor, by adjusting the flow rate regulator, a high degree of control is achieved over the circulation flow rate of the particles involved in the sorbent looping process, and thus a high degree of control of the amount of CO2 captured and released in the sorbent looping process. By adjusting the flow rate regulator, it is possible to switch between a feedstock containing little or no carbon dioxide (CO2) and a feedstock (B) containing a significant amount of initial carbon dioxide (CO2), thereby feeding a variable amount of sorbent to the reformer reactor in response to variations in the CO2 content in the feedstock (B).

[0066] Furthermore, both the reformer and regenerator reactors can only hold a certain amount of solids: if the maximum amount of solids in one reactor is exceeded, the excess solids will continue to flow in the system loop to the other reactor due to their direct connection to each other, assuming the beds in the reactors are fluidized and smoothed.

[0067] If the circulation rate is too low, the reformer reactor does not receive enough regenerated sorbent, such as CaO, compared to the amount of CO2 available in the gas produced in the reforming process (see reaction (2.2) - water-gas shift). Therefore, if the circulation continues, eventually, only the spent sorbent (saturated solid) A will remain in the reformer reactor. * again resulting in little or no capture / absorption of CO2.

[0068] As CO2 capture in the reformer reactor stops due to lack of (unused) sorbent A, more CO2 will exit the reformer reactor in gas phase. This increase in CO2 emissions can be monitored by measuring the reformate composition as described above, for example by gas chromatography. Furthermore, due to the looped coupling between the reactors, monitoring the reduction in CO2 exiting in gas phase from the regenerator reaction provides an indication of the reduction in CO2 capture in the reformer reactor, since no CO2 is added to the system loop.

[0069] It is therefore believed to be highly advantageous to have sufficient sorbent (e.g., CaO) flowing from the regenerator reactor to the reformer reactor at any given time to ensure optimal operation of the system.

[0070] Too high a circulation rate, due to too much sorbent (CaO) in the reformer reactor, is considered less problematic than too low a circulation rate. However, circulation rates above a certain threshold are considered undesirable, since they risk reducing the residence time of the CO2 in the regenerator reactor, and thus reducing the CO2 emitted from the regenerator reactor. To ensure sufficient regeneration, the power supplied to the spent sorbent may have to be increased. [Brief description of the drawings]

[0071] In order to facilitate an understanding of the invention, the following drawings are included, which illustrate embodiments of the invention and are described herein by way of example only:

[0072] [Figure 1] FIG. 1 is a diagram illustrating a system for producing hydrogen gas using an adsorbent according to a first embodiment of the present invention. [Diagram 2] FIG. 2 is a diagram of the system of FIG. 1 with typical compositions, flows, and temperatures illustrated. [Diagram 3]FIG. 3 shows details of the dosing system including the flow regulator and control system. [Figure 4] FIG. 4 is a diagram illustrating a system for producing hydrogen gas using an adsorbent according to a second embodiment of the present invention. DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS

[0073] In the following, embodiments of the invention will be described in more detail with reference to the accompanying drawings, in which it will be understood, however, that the drawings are not intended to limit the invention to the subject matter shown in the drawings.

[0074] In particular, with reference to FIGS. 1 and 2, a system 1 of the present invention for the production of hydrogen gas includes at least two reactors, a reformer reactor 100 and a regenerator reactor 200 .

[0075] First, a fluidized bed such as a bubbling fluidized bed (BFB), a catalyst such as a nickel catalyst, and an adsorbent A such as calcium oxide (CaO) are introduced into the reformer reactor 100 .

[0076] To control the temperature of the fluidized bed, a heat exchanger may be inserted into the reactor to deliver cooling or heating fluid to the bed. However, as will be further explained below, such a heat exchanger may be omitted in this particular system, since the reformer reactor temperature required to ensure the desired reaction in the reactor may be achieved by feedback of the heated regenerated adsorbent A.

[0077] A fuel / feedstock B, such as natural gas / methane (CH4) flowing through the fuel feedstock line 3, and a gas separable from CO2, such as steam C flowing through the steam line 2, are guided as a mixture D to a common feed line 4. The mixture D then enters the reformer reactor 100 via the reformer inlet 130. The temperature of the mixture D is typically between 200°C and 300°C, for example 250°C. The pressure and flow rate of the mixture D can be between 1.0 bar (absolute) and 1.4 bar (absolute), typically 1.2 bar (absolute), and between 375 kg / h and 425 kg / h, typically 392 kg / h, respectively.

[0078] Additionally, typical values ​​of temperature, pressure and flow rate in the fuel material line 3 and the steam line 2 are 120°C (±20°C) / 1.4 bar (absolute) (±0.4 bar (absolute)) / 73 kg / h (±15 kg / h) and 120°C (±20°C) / 1.4 bar (absolute) (±0.4 bar (absolute)) / 318 kg / h (±50 kg / h), respectively.

[0079] Alternatively, fuel material B and gas C can enter the reformer reactor 100 through separate inlets.

[0080] When exemplary fluids and particulates are used, the following reactions occur in the reformer reactor 100: Reformation: CH4(g)+H2O(g) ⇔ CO(g)+3H2(g) (2.1) Shift: CO(g) + H2O(g) ⇔ CO2(g) + H2(g) (2.2) Carbonation: CaO(s) + CO2(g) ⇔ CaCO3(s) (2.4)

[0081] The reforming and shift reactions are endothermic and exothermic reactions, respectively, and the carbonation reaction is an exothermic reaction. Total: CH4(g)+2H2O(g)+CaO(s) ⇔ CaCO3(s)+4H2(g) (2.5)

[0082] Thus, the CO2 gas is captured by the adsorbent A (here in the form of CaO particles) in the fluidized bed, and the spent adsorbent A * (here in the form of CaCO3 particles).

[0083] Produced H2 gas and used adsorbent A * is further conducted through separator conveying lines / pipes 150 via reformer outlet 155 and separator inlet 304 to one or more separators 300 .

[0084] The separator 300 separates at least H2 gas into spent adsorbent A. * from the spent adsorbent A, preferably using centrifugation as the driving separation force. * from the gas. Other separators known in the art, such as electrostatic separators, can also accomplish the desired separation.

[0085] During operation, the separated H2 gas is continuously discharged to the hydrogen line 310 via the hydrogen outlet 315 located at the top of the separator 300. Meanwhile, the separated spent adsorbent A * is continuously discharged through a spent adsorbent outlet 305 located at the bottom of the separator 300 into a first regenerator transfer line 320 .

[0086] The separated H2 gas may be directed to a facility for further purification, for example, using pressure swing adsorption, electrochemical purification, or catalytic recombination. Typical temperatures, pressures, and flow rates in the hydrogen line 310 during operation are 600° C. (±100° C.), 1.2 bar absolute (±0.4 bar absolute), and 208 kg / h (±40 kg / h). As described further below, the gas discharge to the hydrogen line 310 can also include non-reacted gases from the reformer reactor 100, such as CO, CO2, and fuel gas B (e.g., CH4), in addition to H2 gas.

[0087] Separated used adsorbent A *is guided from the spent adsorbent outlet 305 to a feed system 400 configured to control the flow rate through the first regenerator transfer line 320. Typical values ​​of temperature, pressure and flow rate in the first regenerator transfer line 320 during operation are 600° C. (±100° C.), 1.2 bar absolute (±0.4 bar absolute) and 2000 kg / h (±600 kg / h).

[0088] The feed system 400 feeds the spent adsorbent A from the separator 300. * and from tank 410 to receive used sorbent A * The tank 410 may include one or more tank inlets 405 and one or more tank outlets 415, respectively, for discharging the liquid.

[0089] The supply system 400 is a * The tank 410 may include a tank gauging device 411 to allow monitoring of operational parameters such as the amount of CO, the presence and composition of other chemical species such as CO, CO2 and / or CH4, the degree of moisture, etc. In Figures 1-4, such a tank gauging device 411 is shown directly coupled to the tank 410. However, measurements may be performed anywhere along the spent sorbent transport line 320, 430 as long as the desired parameters can be achieved. One example of such a tank gauging device 411 is a level gauging device that may continuously monitor the volume of solids present in the tank 410.

[0090] Used adsorbent A * After being discharged from the tank 410 via the tank outlet 415, it is further guided to the regenerator reactor 200 through the second regenerator conveying line 430, 430', and the spent adsorbent A * is regenerated / calcined back into Adsorbent A and CO2 gas. Typical temperatures, pressures and flow rates of the inflow (mainly Adsorbent A) to the regenerator reactor 200 are 850°C (±100°C), 1.2 bar(absolute) (±0.4 bar(absolute)), and 296 kg / h (±50 kg / h), respectively.

[0091] The regeneration reaction CaCO3(s) ⇔ CaO(s)+CO2(g) (2.6) is an endothermic reaction that requires the supply of energy, usually in the form of added heat. At typical pressures of 1.1 to 1.4 bar (absolute), a temperature range of 800°C to 1100°C may be sufficient to initiate and sustain the regeneration reaction.

[0092] The regenerator reactor 200 comprises: - a regenerator vessel 201 having an internal volume with a fluidized bed (usually a BFB); -Used adsorbent A * a regenerator power source 220 for providing thermal energy to the - the second regenerator transfer line 430' to the regenerator vessel 201 used adsorbent A * one or more regenerator inlets 205 for allowing the inflow of one or more CO2 outlets 235 for discharging CO2 from the regenerator vessel 201 to one or more CO2 lines 240; one or more steam inlets 225 for allowing the inflow of C (such as steam C introduced from steam line 2) from one or more steam regenerator lines 230 into the regenerator vessel 201 to fluidize the bed of the regenerator reactor; one or more adsorbent outlets 215 for allowing discharge of hot regenerated adsorbent A from the regenerator vessel 201; It is equipped with:

[0093] After being discharged from the regenerator vessel 201 , the hot adsorbent A is directed back to the reformer reactor 100 through the recycle line 210 via one or more adsorbent inlets 120 .

[0094] Steam C entering regenerator vessel 201 from steam line 2 is preheated and has a typical temperature, pressure and flow rate of 750° C. (±75° C.), 1.2 bar absolute (±0.4 bar absolute), and 112 kg / h (±20 kg / h). Upstream, steam line 2 branches into flows towards feed line 4 and steam regenerator line 230, steam C having a typical temperature, pressure and flow rate of 120° C., 1.2 bar absolute (±0.4 bar absolute), and 430 kg / h (±75 kg / h).

[0095] CO2 line 240 directs the exhausted CO2 to an external location, typically a CO2 storage facility 600. Typical temperatures, pressures, and flow rates in CO2 line 240 are 850°C (±75°C), 1.2 bar absolute (±0.4 bar absolute), and 296 kg / h (±75 kg / h).

[0096] Additionally, the supply system 400 may be configured to supply the spent sorbent A to and / or from the tank 410. * The fluid may include a valve (not shown), such as a one-way valve, configured to open or stop the flow of fluid.

[0097] It is known that both the kinetics of the sorbent and the operating pressure have a significant effect on the production efficiency of SE-SMR in a fluidized bed reactor [see literature such as Wang, YF; Chao, ZX; Jakobsen, HA 3D Simulation of bubbling fluidized bed reactors for sorption enhanced steam methane reforming processes. J. Nat. Gas Sci. Eng. 2010, 2, 105-113 and publication Wang, YF; Chao, ZX; Jakobsen, HA SE-SMR process performance in CFB reactors: Simulation of the CO2 adsorption / desorption process with CaO based sorbents. Int. J. Greenhouse Gas Control 2011, 5, 489-497].

[0098] Therefore, the inventors have determined that during the hydrogen production process, in particular the capture efficiency of the adsorbent A and / or the amount of the used adsorbent A * Flow rate R A* The present inventors have realized that it would be highly advantageous to have the ability to monitor and control the

[0099] FIG. 3 illustrates one exemplary configuration of the feed system 400 of FIGS. 1 and 2, which feeds the spent adsorbent A discharged from the separator 300. * Flow rate R A* and a flow rate regulator 440 for controlling the flow rate R A* and a control system 500 for controlling various operating parameters such as the capture efficiency of adsorbent A.

[0100] Flow rate R A*To control this, the flow regulator 440, in the illustrated exemplary configuration, includes a screw conveyor 450 that forms part of the second regenerator conveying line 430, thereby dividing the conveying line into an upstream conveying line section 430 and a downstream conveying line section 430'. A motor 460 is rotatably coupled to an end of the screw conveyor 450 to impart rotational motion to the screw conveyor 450. The ability to adjust the rotational speed is also achieved by connecting a variable speed drive / frequency converter 470 to the motor 460.

[0101] The illustrated control system 500 is configured in signal communication with the variable speed drive 470 for both digital control and monitoring.

[0102] In the exemplary configuration shown in Figures 1-4, the control system 500 can further receive and / or send operational signals from one or more of the other dynamics / components of system 1 involved in the looped hydrogen production process, as follows: receiving via a fuel feed measurement line 501a a signal indicative of the flow rate of fuel feed B (usually CH4) through the fuel feed line 3 in order to measure the flow rate and / or composition of the fuel feed B to the reformer reactor 100; receiving, via a water steam measurement line 501c, a signal indicative of the flow rate and / or composition of water steam C (or other gas that can be separated from CO2, see above) entering the reformer reactor 100 through the water steam line 2; receiving, via a water vapor measurement line 501d, a signal indicative of the flow rate and / or composition of water vapor C (or other gas that can be separated from CO2, see above) entering the regenerator reactor 200 through the water vapor line 2; receiving, via a feed inlet measurement line 501b, a signal indicative of the flow rate and / or composition of mixture D entering the reformer reactor 100 through the feed line 4; receiving a signal indicative of the volume and / or composition of gas and / or solids in the reformer reactor 100 via reformer measurement line 501e; - The fluid flowing in the second regenerator conveying line 430 upstream and / or downstream 430' of the flow control device 440 (mainly the separated spent adsorbent A * receiving a signal indicative of the flow rate and / or composition of the adsorbent via a spent adsorbent measurement line 502; receiving, via a CO2 measurement line 505, a signal indicative of the flow rate and / or composition of the gas (mainly CO2 and water vapor) discharged from the regenerator vessel 201 to the CO2 line; - Used adsorbent A in regenerator vessel 201 * to the regenerator power source 220 via heat adjustment measurement line 504 to set a desired power output for heating the - Used adsorbent A in regenerator vessel 201 * receiving a signal indicative of the operating power provided to the regenerator via a heat regulation measurement line 504 or via a separate measurement line from the regenerator power source 220; receiving a signal via a thermal measurement line 506 from the regenerator vessel 201 to monitor the temperature of the fluid in the regenerator vessel 201; receiving, via a regenerator sorbent measurement line 507, a signal indicative of the flow rate and / or composition of the fluid (mainly the regenerator sorbent A) discharged from the regenerator vessel 201 to the recycle line 210; -Solid / spent sorbent A * receiving a signal indicative of an operating parameter of the tank 410, such as the volume and / or weight of the tank 410, via the tank measurement line 508 or via another measurement line directly from the tank 410; Receiving a signal via gas measurement line 509 indicative of the flow rate and / or composition of the gas flowing in the hydrogen line 310.

[0103] The control system 500 can receive and / or transmit signals wirelessly to one or more of the above-mentioned components by installing the necessary transmitters / receivers, thereby eliminating the corresponding measurement line(s).

[0104] Additionally, the control system 500 may be connected to other portions of the system 1 to enable monitoring and / or control of those portions.

[0105] The flow and composition measurements can be performed by a shared measurement system in the control system 500 including the necessary measurement means such as mass flow meters in the case of spent adsorbent and regenerated adsorbent A flow measurements, and by a shared measurement system in the control system 500 including the necessary measurement means such as gas chromatographs, diode laser spectrometers and / or combo-probes in the case of gas composition measurements. Alternatively or additionally, the measurements can be performed by measurement systems dedicated to the individual measurement lines. As shown in FIG. 3, at least one of the flow measurements may require cooling 510 before measurement.

[0106] When the system 1 is equipped with the control system 500 described above, various advantageous diagnostic results can be obtained.

[0107] For example, considering the reactions occurring in a typical SE-SMR process, CH4 and CO are consumed by the reforming reaction (2.1) and the gas shift reaction (2.2) to produce CO2 and H2.

[0108] Therefore, when the ability of the adsorbent A to capture CO2 decreases, the spent adsorbent A flows out of the reformer reactor 100 and into the separator 300. * 3. Increasing the amount of CO, CH4 and CO2 separated from the hydrogen gas and released into the hydrogen line 310.

[0109] Thus, the degradation of the ability of sorbent A to capture CO2 during hydrogen production can be monitored by measuring the gas composition entering the hydrogen line 310. If the measurements show a gradual increase in at least one of the following gases: CO, CH4, and CO2, this can be interpreted as a degradation in the ability of the sorbent to capture / adsorb CO2 in the reformer reactor 100.

[0110] As mentioned above, such gas composition measurements can be performed by installing a suitable gas composition measurement device, such as a gas chromatograph (not shown). The measurement signal is sent via gas measurement line 509 to the automatic control device 500, which can display the measurement result on a display (not shown) and / or the measurement signal can be a function of the energy supply from the regenerator power source 220 (via heat measurement line 504) or the rotation speed v of the screw conveyor 450 (via flow rate adjustment measurement line 503). r The above parameters are then used to calculate (via a processor within the controller 500) new settings for the parameters.

[0111] In the preceding description, various aspects of the system according to the present invention have been described with reference to exemplary embodiments. For purposes of explanation, specific numbers, systems and configurations have been set forth to provide a thorough understanding of the system and its operation. However, this description is not intended to be construed in a limiting sense. Various modifications and variations of the illustrated embodiments, as well as other embodiments of the system, that are apparent to those skilled in the art to which the disclosed subject matter pertains, are deemed to be within the scope of the present invention. [Explanation of symbols]

[0112] 1 Hydrogen production system 2. Steam line 3 Fuel material line 4 Supply Line 100 Reformer reactor 120 Adsorbent inlet 130 Reformer inlet for mixture D of feedstock B and steam C 150 Separator conveying line 155 Reformer outlet 200 Regenerator Reactor 201 Regenerator container 205 Regenerator inlet 210 Recycling Line 215 Adsorbent outlet 220 Regenerator power source / Regenerator heat source 225 Steam inlet 230 Steam Regenerator Line 235 CO2 outlet 240 CO2 Line 300 separator 304 Separator inlet 305 Spent adsorbent outlet 310 Hydrogen Line 315 Hydrogen Outlet 320 First regenerator transfer line 400 Supply System 405 Tank inlet 410 Tank 411 Tank Gauge Device 415 Tank outlet 430 Second regenerator conveying line (upstream of 440) 430 Second regenerator conveying line (downstream of 440) 440 Flow rate adjustment device 450 Screw Conveyor 460 Motor / Electric Motor 470 Variable Speed ​​Drive / Frequency Converter 500 Control Systems / Automatic Control Devices 501a Supply inlet measurement line 501b Fuel Materials Measurement Line 501c Water vapor measurement line (reformer reactor) 501d Water vapor measurement line (regenerator reactor) 501e Reformer Measurement Line 502 Used adsorbent measurement line 503 Flow Control Measurement Line 504 Heat Control Measurement Line 505 CO2 measurement line 506 Heat Measurement Line 507 Regenerated Adsorbent Measurement Line 508 Tank Gauging Line 509 Gas Measurement Line 510 Cooling System 600 CO2 storage (storage / reservoir) A Adsorbent, CaO A * Used adsorbent, CaCO3 B Feedstock / Natural Gas C. Water vapor D feed mixture R A* Spent sorbent flow rate R A*,H Higher spent adsorbent flow rate R A*,L Lower spent adsorbent flow rate v r Screw conveyor rotation speed v r,H Higher screw conveyor rotation speed v r,L Lower screw conveyor rotation speed Q Fever

Claims

1. 1. A system for producing hydrogen gas, comprising: - used adsorbent (A ＊ a reformer reactor (100) for containing an adsorbent (A) for capturing carbon dioxide to form hydrogen gas (H), said reformer reactor (100) allows for the reforming of a feedstock (B) and steam (C) to form hydrogen gas (H ２ ) and carbon dioxide (CO ２ a reformer inlet (130) for supplying at least one of the feedstock (B) and the steam (C) to the reformer reactor (100); and a second outlet (140) for supplying the spent adsorbent (A) to the reformer reactor (100). ＊ ) and the hydrogen gas (H ２ a reformer outlet (155) for discharging the sulphur dioxide; - the used adsorbent (A ＊ ) to the hydrogen gas (H ２ ), wherein the separator (300) is configured to separate the hydrogen gas (H ２ ) and the used adsorbent (A ＊ a separator inlet (304) for feeding the separated spent adsorbent (A ＊ a separator outlet (305) for discharging the condensed water; - the used adsorbent (A ＊ ) and the hydrogen gas (H ２ a separator transfer line (150) for transferring the reformer from the reformer outlet (155) to the separator inlet (304); - the spent adsorbent (A) separated in the separator (300) ＊ a regenerator inlet (205) for receiving at least a portion of the spent adsorbent (A ＊ ) to carbon dioxide (CO ２ a regenerator reactor (200) comprising a regenerator power source (220) configured to provide sufficient energy to enable the release of the adsorbent (A) to regenerate said adsorbent (A), and a regenerator outlet (215) for discharging the regenerated adsorbent (A); - the used adsorbent (A ＊ a regenerator transfer line (320, 430, 430') for transferring the stream of (I) from the separator outlet (305) to the regenerator inlet (205); a recycle line (210) arranged to convey at least a portion of said regenerated adsorbent (A) from said regenerator outlet (215) to said reformer reactor (100); Equipped with The regenerator conveying line (320, 430) conveys the used adsorbent (A) to the regenerator inlet (205). ＊ ) flow rate (R Ａ＊ a flow control device (440) configured to adjust the flow rate of the flowing fluid; and an automatic control device (500) in signal communication with the flow control device (440), The automatic control device (500) the flow rate of the feedstock (B) entering the reformer reactor (100); the flow rate of steam (C) entering the reformer reactor (100); the flow rate of the mixture of feedstock (B) and steam (C) entering said reformer reactor (100); the flow rate of the spent adsorbent (A*) flowing between the reformer outlet (155) and the regenerator inlet (205); the flow rate of at least carbon dioxide (CO2) flowing between the reformer outlet (155) and the regenerator inlet (205); and The flow rate of the hydrogen gas (310) leaving the separator (300) The flow rate adjusting device (440) is configured to automatically control the operation of the flow rate adjusting device (440) based on at least one of the following: system.

2. The regenerator conveying line (320, 430) - the separated used adsorbent (A ＊ a tank (410) for containing the a first regenerator transfer line (320) connected at one end to the separator outlet (305) and at the other end to the tank inlet (405) of the tank (410); a second regenerator conveying line (430, 430') connected at one end to the tank outlet (415) of said tank (410) and at the other end to said regenerator inlet (205); The system of claim 1 , comprising:

3. The flow control device (440) controls the amount of the spent adsorbent (A ＊ ) flow rate (R Ａ＊ ) to adjust the rotation speed (v ｒ 2. The system of claim 1, further comprising a screw conveyor (450) arranged to rotate at a speed of 1000 rpm.

4. The screw conveyor (450) is rotated at a higher rotational speed (v ｒ，Ｈ ) and lower rotation speeds (v ｒ，Ｌ ) respectively, the used adsorbent (A ＊ ) has a higher flow rate (R Ａ＊，Ｈ ) and lower flow rates (R Ａ＊，Ｌ 4. The system of claim 3, wherein the regenerator reactor (200) is configured to transport the gas therethrough.

5. The flow rate adjusting device (440) a motor (460) rotatably connected to said screw conveyor (450); a variable speed drive (470) connected to said motor (460) and enabling the rotational speed of said motor (460) to be controlled; The system of claim 3 , comprising:

6. The automatic control device (500) the composition ratio of the feedstock (B) to the total flow rate of steam (C) entering the reformer reactor (100); the composition ratio of compounds in the fluid flowing between the reformer outlet (155) and the regenerator inlet (205); the gas composition ratio between carbon monoxide (CO) and unconverted fuel gas flowing between the reformer outlet (155) and the regenerator inlet (205); Carbon dioxide (CO ) flowing between the reformer outlet (155) and the regenerator inlet (205) ２ ) and the unconverted fuel gas, and Measurement of the gas composition in the hydrogen line (310) The system of any one of claims 1 to 5, configured to automatically control operation of the flow regulator (440) based on at least one of:

7. 6. The system of claim 1, wherein the reformer reactor (100) comprises a quantity of the feedstock (B), a quantity of the steam (C), and a quantity of the adsorbent (A), and the feedstock (B) comprises a hydrocarbon-containing fuel.

8. The system of any one of claims 1 to 5, wherein at least one of the reformer reactor (100) and the regenerator reactor (200) comprises a fluidized bed.

9. The system according to any one of claims 1 to 5 is used to generate hydrogen gas (H ２ ), a method for producing A. The feedstock (B) and the steam (C) are fed through one or more of the reformer inlets (130) to form carbon dioxide (CO ２ into said reformer reactor (100) containing an adsorbent (A) for capturing B. The hydrogen gas (H ２ ) and the carbon dioxide (CO ２ reforming the feedstock (B) and the steam (C) in the reformer reactor (100) to produce a reformed gas mixture comprising carbon dioxide (CO ２ ) to capture the used adsorbent (A ＊ reforming the feedstock (B) and the steam (C) to form C. The used adsorbent (A ＊ ) and at least a portion of the hydrogen gas (H ２ ) from the reformer reactor (100) to the separator (300) through the separator transfer line (150); D. Operating at least one of the separators (300) to remove the spent adsorbent (A ＊ ) to the hydrogen gas (H ２ ) and E. By operating the flow control device (440), the used adsorbent (A ＊ ) of the flow rate (R Ａ＊ ) while adjusting the used adsorbent (A ＊ ) from the separator (300) to the regenerator reactor (200) through a regenerator transfer line (320, 430, 430'); F. The spent adsorbent (A) in the regenerator reactor (200) ＊ ) to supply energy to the used adsorbent (A ＊ ) to carbon dioxide (CO ２ ), thereby at least partially regenerating the adsorbent (A) of step A; G. Recycling at least a portion of the regenerated adsorbent (A) of step F by conveying the regenerated adsorbent (A) from the regenerator reactor (200) to the reformer reactor (100) through the recycle line (210); A method comprising:

10. The flow rate adjusting device (440) is provided with a screw conveyor (450), and the flow rate (R Ａ＊ ) is adjusted to the rotation speed (v ｒ 10. The method of claim 9, wherein the method is achieved by adjusting

11. In step E, the rotation speed (v ｒ ) can be adjusted, The used adsorbent (A ＊ ) at a higher flow rate (R Ａ＊，Ｈ ) to the regenerator reactor (200). ｒ，Ｈ ) and The used adsorbent (A ＊ ) at a lower flow rate (R Ａ＊，Ｌ ) to the regenerator reactor (200), the screw conveyor is rotated at a lower rotational speed (v ｒ，Ｌ ) and The method of claim 10, comprising:

12. The flow rate adjusting device (440) a motor (460) rotatably connected to said screw conveyor (450); a variable speed drive (470) connected to said motor (460) to enable control of the rotational speed of said motor (460); Furthermore, In step E, the rotation speed (v ｒ ) includes operating the variable speed drive (470) to vary the rotational speed of the motor (460). The method of claim 10.

13. The regenerator conveying line (320, 430, 430') - the separated used adsorbent (A ＊ a tank (410) for containing the a first regenerator transfer line (320) connected at one end to the separator outlet (305) and at the other end to the tank inlet (405) of the tank (410); a second regenerator conveying line (430, 430') connected at one end to the tank outlet (415) of said tank (410) and at the other end to said regenerator inlet (205); Equipped with Step E: Transfer the tank (410) to the separated spent adsorbent (A ＊ ) to a predetermined minimum amount of 10. The method of claim 9.

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