CN114481164B - Non-pure water solution electrolytic hydrogen production device, system and method based on liquid phase moisture absorption - Google Patents
Non-pure water solution electrolytic hydrogen production device, system and method based on liquid phase moisture absorption Download PDFInfo
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- CN114481164B CN114481164B CN202210184170.4A CN202210184170A CN114481164B CN 114481164 B CN114481164 B CN 114481164B CN 202210184170 A CN202210184170 A CN 202210184170A CN 114481164 B CN114481164 B CN 114481164B
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- 239000001257 hydrogen Substances 0.000 title claims abstract description 187
- 229910052739 hydrogen Inorganic materials 0.000 title claims abstract description 187
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 title claims abstract description 184
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- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 17
- 229910052799 carbon Inorganic materials 0.000 claims description 15
- 239000003054 catalyst Substances 0.000 claims description 13
- 229910000510 noble metal Inorganic materials 0.000 claims description 10
- 239000007789 gas Substances 0.000 claims description 9
- 239000012528 membrane Substances 0.000 claims description 9
- 229910045601 alloy Inorganic materials 0.000 claims description 7
- 239000000956 alloy Substances 0.000 claims description 7
- 239000004810 polytetrafluoroethylene Substances 0.000 claims description 6
- 229920001343 polytetrafluoroethylene Polymers 0.000 claims description 6
- 239000011148 porous material Substances 0.000 claims description 6
- 238000006555 catalytic reaction Methods 0.000 claims description 5
- 239000008151 electrolyte solution Substances 0.000 claims description 4
- 239000002245 particle Substances 0.000 claims description 4
- 230000009471 action Effects 0.000 claims description 3
- HTXDPTMKBJXEOW-UHFFFAOYSA-N dioxoiridium Chemical compound O=[Ir]=O HTXDPTMKBJXEOW-UHFFFAOYSA-N 0.000 claims description 3
- 239000004744 fabric Substances 0.000 claims description 3
- 150000002431 hydrogen Chemical class 0.000 claims description 3
- 239000002608 ionic liquid Substances 0.000 claims description 3
- 229910000457 iridium oxide Inorganic materials 0.000 claims description 3
- DZQBLSOLVRLASG-UHFFFAOYSA-N iridium;methane Chemical compound C.[Ir] DZQBLSOLVRLASG-UHFFFAOYSA-N 0.000 claims description 3
- NCPHGZWGGANCAY-UHFFFAOYSA-N methane;ruthenium Chemical compound C.[Ru] NCPHGZWGGANCAY-UHFFFAOYSA-N 0.000 claims description 3
- 229910001925 ruthenium oxide Inorganic materials 0.000 claims description 3
- WOCIAKWEIIZHES-UHFFFAOYSA-N ruthenium(iv) oxide Chemical compound O=[Ru]=O WOCIAKWEIIZHES-UHFFFAOYSA-N 0.000 claims description 3
- 239000002033 PVDF binder Substances 0.000 claims description 2
- DSVGQVZAZSZEEX-UHFFFAOYSA-N [C].[Pt] Chemical compound [C].[Pt] DSVGQVZAZSZEEX-UHFFFAOYSA-N 0.000 claims description 2
- 239000003929 acidic solution Substances 0.000 claims description 2
- 239000012670 alkaline solution Substances 0.000 claims description 2
- 239000003011 anion exchange membrane Substances 0.000 claims description 2
- 239000000919 ceramic Substances 0.000 claims description 2
- 239000004205 dimethyl polysiloxane Substances 0.000 claims description 2
- 235000013870 dimethyl polysiloxane Nutrition 0.000 claims description 2
- 229910021389 graphene Inorganic materials 0.000 claims description 2
- 150000004767 nitrides Chemical class 0.000 claims description 2
- CXQXSVUQTKDNFP-UHFFFAOYSA-N octamethyltrisiloxane Chemical compound C[Si](C)(C)O[Si](C)(C)O[Si](C)(C)C CXQXSVUQTKDNFP-UHFFFAOYSA-N 0.000 claims description 2
- 238000004987 plasma desorption mass spectroscopy Methods 0.000 claims description 2
- 229920000435 poly(dimethylsiloxane) Polymers 0.000 claims description 2
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- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 3
- 238000000926 separation method Methods 0.000 description 3
- ZXLOSLWIGFGPIU-UHFFFAOYSA-N 1-ethyl-3-methyl-1,2-dihydroimidazol-1-ium;acetate Chemical compound CC(O)=O.CCN1CN(C)C=C1 ZXLOSLWIGFGPIU-UHFFFAOYSA-N 0.000 description 2
- 230000002378 acidificating effect Effects 0.000 description 2
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- SCVFZCLFOSHCOH-UHFFFAOYSA-M potassium acetate Chemical compound [K+].CC([O-])=O SCVFZCLFOSHCOH-UHFFFAOYSA-M 0.000 description 2
- 238000003860 storage Methods 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- ZAMOUSCENKQFHK-UHFFFAOYSA-N Chlorine atom Chemical compound [Cl] ZAMOUSCENKQFHK-UHFFFAOYSA-N 0.000 description 1
- KWYUFKZDYYNOTN-UHFFFAOYSA-M Potassium hydroxide Chemical compound [OH-].[K+] KWYUFKZDYYNOTN-UHFFFAOYSA-M 0.000 description 1
- NRTRXITURRQSMN-UHFFFAOYSA-N [Pt].[Ir].[C] Chemical compound [Pt].[Ir].[C] NRTRXITURRQSMN-UHFFFAOYSA-N 0.000 description 1
- 230000008859 change Effects 0.000 description 1
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Images
Classifications
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B1/00—Electrolytic production of inorganic compounds or non-metals
- C25B1/01—Products
- C25B1/02—Hydrogen or oxygen
- C25B1/04—Hydrogen or oxygen by electrolysis of water
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B15/00—Operating or servicing cells
- C25B15/08—Supplying or removing reactants or electrolytes; Regeneration of electrolytes
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/36—Hydrogen production from non-carbon containing sources, e.g. by water electrolysis
Abstract
The invention provides a non-pure water solution electrolytic hydrogen production device based on liquid phase moisture absorption, and belongs to the technical field of electrochemical hydrogen production. The device comprises an electrolyte layer, a water vapor mass transfer layer and an oxygen evolution catalytic layer, wherein the water vapor mass transfer layer and the oxygen evolution catalytic layer are attached to two sides of the electrolyte layer, the device further comprises a hydrogen evolution catalytic layer and an ion exchange membrane positioned between the oxygen evolution catalytic layer and the hydrogen evolution catalytic layer, the oxygen evolution catalytic layer is provided with an anode electrode, and the hydrogen evolution catalytic layer is provided with a cathode electrode. The invention also provides a system and a method for producing hydrogen by electrolysis of the non-pure water solution based on liquid phase moisture absorption. The device and the system can obtain clean hydrogen energy by using the non-pure water solution, can supply power through an external power supply in an energy conversion system of areas such as a future offshore floating island, a desert river coast and the like, directly obtain pure water without impurity ions through an electrolyte layer attached to a water-vapor mass transfer layer, and prepare hydrogen by using a catalytic electrolysis principle, thereby realizing high-efficiency hydrogen energy acquisition.
Description
Technical Field
The invention belongs to the technical field of electrochemical hydrogen production, and particularly relates to a non-pure water solution electrolytic hydrogen production device, system and method based on liquid phase moisture absorption.
Background
The existing hydrogen production technology is mainly focused on the electrolysis of fresh water obtained by desalination/purification of non-pure water solution, and extra desalination cost is needed, but direct electrolysis of the non-pure water solution is difficult, because the existence of a large amount of ions in the non-pure water solution influences membrane materials or electrodes in an electrolysis system, so that the electrolysis efficiency is reduced, such as the competition problem of oxygen and chlorine separation reaction and the electrode corrosion problem in the seawater electrolysis process. However, in global water resources, 97% is sea, 2% is river and lake, some groundwater which is difficult to utilize and the like, the reserve is extremely large, and if the non-pure water solution can be directly electrolyzed, a great amount of manpower, material resources, equipment investment and energy consumption required for desalting/purifying the water are saved, and the subverted influence is generated on the hydrogen production industry.
Disclosure of Invention
The invention aims to provide a device, a system and a method for producing hydrogen by electrolysis of a non-pure water solution based on liquid phase moisture absorption. According to the invention, an external power supply is used for supplying energy, liquid water in the non-pure water solution is directly obtained through the interface pressure difference between the non-pure water solution and the electrolyte, and the collected water molecules are directly used for hydrogen production in an electrolysis mode, so that impurity ions contained in the non-pure water solution can be fundamentally removed, and the method is beneficial to providing strong technical support for the development of hydrogen energy.
The aim of the invention is achieved by the following technical scheme:
an apparatus for producing hydrogen by electrolysis of a non-pure water solution based on liquid phase moisture absorption, comprising: an outer electrolyte layer, a water vapor mass transfer layer attached to one side of the outer electrolyte layer; an inner electrolyte layer attached to an oxygen evolution catalytic layer on one side of the inner electrolyte layer; a peristaltic pump between the outer electrolyte layer and the inner electrolyte layer; the device further comprises a hydrogen evolution catalytic layer, an ion exchange membrane or diaphragm positioned between the oxygen evolution catalytic layer and the hydrogen evolution catalytic layer, wherein the oxygen evolution catalytic layer is provided with an anode electrode, and the hydrogen evolution catalytic layer is provided with a cathode electrode.
In the hydrogen production device, the outer electrolyte layer is taken as an accommodating vessel of the outer electrolyte by a cuboid solution tank, an opening at one side of the solution tank is attached to the water vapor mass transfer layer, so that the outer electrolyte is convenient to directly contact with the water vapor mass transfer layer, and the electrolyte absorbs water vapor permeated in the non-pure water solution under the action of the interface pressure difference between the non-pure water solution and the outer electrolyte. The outer electrolyte layer continuously absorbs the water in the non-pure water solution and simultaneously continuously passes into the inner electrolyte layer through the peristaltic pump. The inner electrolyte layer is formed by taking a cuboid solution tank as an accommodating vessel of the inner electrolyte, wherein an opening at one side of the solution tank is in direct contact with the oxygen evolution catalytic layer, and the oxygen evolution catalytic layer is subjected to electrolytic oxidation reaction to generate oxygen, and the hydrogen evolution catalytic layer is subjected to hydrogen evolution reaction to generate hydrogen. During electrolysis, water in the inner electrolyte is consumed, and meanwhile, the inner electrolyte continuously enters the outer electrolyte layer through a peristaltic pump, so that water in the non-pure water solution is further obtained, the concentration of the electrolyte is kept constant, and a reciprocating cycle is formed, so that a stable hydrogen production process is formed.
According to the non-pure water solution electrolytic hydrogen production device based on liquid phase moisture absorption, pure water vapor in the non-pure water solution is directly absorbed through the outer electrolyte layer attached to the water vapor mass transfer layer, no extra energy is required for desalting or purifying the non-pure water solution, and in-situ capture of the water vapor without impurity ions is directly realized by means of interface pressure difference between the outer electrolyte layer and the non-pure water solution. Pure water vapor in the non-pure water solution is directly obtained by adopting an outer electrolyte layer close to the water vapor mass transfer layer, impurity ions contained in the non-pure water solution are removed, hydrogen is prepared by a chemical principle of catalytic electrolysis, and a plurality of technologies are coupled to form a complete non-pure water solution hydrogen production system.
The hydrogen production flow based on the catalytic electrolysis of the non-pure water solution of the device is as follows: the water vapor mass transfer layer is close to the external electrolyte solution, under the action of the interface pressure difference between the non-pure water solution and the external electrolyte, the water vapor permeates the water vapor mass transfer layer, the aggregated water, the contained impurity ions and the like are removed, the external electrolyte layer rapidly absorbs and captures the water vapor, meanwhile, the water vapor continuously flows into the internal electrolyte layer through the peristaltic pump, the oxidation reaction is carried out on the oxygen evolution catalytic layer to continuously produce oxygen, the hydrogen evolution reaction is carried out on the hydrogen evolution catalytic layer to continuously produce hydrogen, and H produced in the process + Or OH (OH) - Transfer is performed through an ion exchange membrane. The water in the inner electrolyte is consumed by electrolysis, and simultaneously the inner electrolyte continuously enters the outer electrolyte layer through a peristaltic pump, so that the water in the non-pure water solution is further obtained, the concentration of the electrolyte is kept constant, and the reciprocating circulation is formed, so that a stable hydrogen production process is formed.
In the device, the water vapor mass transfer layer only allows gases such as water vapor and the like to pass through, but does not allow aggregated water to pass through, so that the permeation of ions is prevented, and the problem of competition between impurity ions in non-pure water solution and oxygen evolution reaction is fundamentally solved. The outer electrolyte layer attached to the water vapor mass transfer layer is used for quickly absorbing water vapor without impurity ions, and can realize continuous and stable hydrogen production process by coupling electrolysis.
Under the pushing of the interfacial pressure difference between the non-pure water solution and the external electrolyte layer, the device promotes the water vapor in the non-pure water solution to diffuse through the water vapor mass transfer layer, meanwhile, impurity ions in the non-pure water solution are repelled outside by the water vapor mass transfer layer, the external electrolyte layer rapidly absorbs the permeated water vapor, the internal circulation hydrogen production of the device consumes water, the interfacial pressure difference is continuously maintained inside and outside the water vapor mass transfer layer, and therefore, the water vapor is stably and continuously diffused to the external electrolyte side from the outside of the water vapor mass transfer layer, and the process continuously and rapidly obtains pure water vapor without impurities. Meanwhile, based on the catalytic electrolysis hydrogen production principle, oxygen is generated by electrolyzing moisture in an electrolyte layer in an anode side, hydrogen is generated by a cathode side, and H is generated in the process + Or OH (OH) - Transfer occurs through an ion exchange membrane or diaphragm. The water in the inner electrolyte is consumed by electrolysis, meanwhile, the inner electrolyte continuously enters the outer electrolyte layer through the peristaltic pump, water vapor penetrating through the water vapor mass transfer layer is further obtained and continuously returns to the inner electrolyte layer through the peristaltic pump, and further electrolytic reaction is carried out, so that a stable hydrogen production process is formed.
Further, the anode electrode arranged on the oxygen evolution catalytic layer can be buried inside the oxygen evolution catalytic layer in a wrapping manner, and can also be arranged between the oxygen evolution catalytic layer and the inner electrolyte layer.
Further, the cathode electrode arranged on the hydrogen evolution catalytic layer can be buried inside the hydrogen evolution catalytic layer in a wrapping manner, and can also be arranged outside the hydrogen evolution catalytic layer.
Further, the water vapor mass transfer layer is a porous water vapor mass transfer layer prepared by one of a TPU film, PDMS film and PTFE film with the aperture of 0.1-100 um or graphene, PVDF particles and PTFE particles through spraying, screen printing and electrostatic adsorption.
Further, the electrolyte layer is one of an acidic solution (sulfuric acid solution and the like) with the concentration of 15-50 wt%, an alkaline solution (potassium acetate solution, potassium hydroxide solution and the like) with the concentration of 15-50 wt% and an ionic liquid (1-ethyl-3-methylimidazole acetate and the like), and the hydrogen evolution catalytic layer is one of a non-noble metal alloy, a non-noble metal phosphide, a non-noble metal nitride and a noble metal alloy catalyst; the oxygen evolution catalytic layer is one of iridium carbon, ruthenium carbon, niFe-LDH, niFeCu alloy, iridium oxide, ruthenium oxide and iridium platinum carbon catalyst. In hydrogen evolution, a combination of noble metal catalyst and carbon (e.g., pt/c) is used in an acidic environment, and one or more of other non-noble metals or carbon is used in an alkaline environment; during oxygen evolution, iridium carbon, ruthenium carbon, iridium oxide and ruthenium oxide are used in an acidic environment, and NiFe-LDH, niFeCu alloy and platinum carbon catalyst can be used in an alkaline environment.
Further, the anode electrode is made of carbon paper, carbon cloth or a porous material with electrical conductivity, and the cathode electrode is made of carbon paper, carbon cloth or a porous material with electrical conductivity.
Further, the ion exchange membrane is a proton exchange membrane (nafion membrane) or an anion exchange membrane, and the membrane is a ceramic membrane.
The system comprises the device, an external power supply which is connected with an anode electrode and a cathode electrode and provides electric energy for hydrogen production reaction, a hydrogen scrubber, a hydrogen dryer and a hydrogen collecting bottle which are sequentially communicated with a hydrogen evolution catalytic layer, and an oxygen scrubber, an oxygen dryer and an oxygen collecting bottle which are sequentially communicated with an oxygen evolution catalytic layer.
The invention discloses a non-pure water solution electrolytic hydrogen production system based on liquid phase moisture absorption, which realizes the whole non-pure water solution electrolytic hydrogen production process by three main processes of supplying energy through an external power supply, directly obtaining water vapor without impurity ions from the non-pure water solution through an external electrolyte layer and producing hydrogen through electrolytic catalysis. Firstly, an external power supply is utilized to provide energy for electrolytic hydrogen production; secondly, the water vapor mass transfer layer can block impurity ions in the non-pure water solution and permeate water vapor, the outer electrolyte layer is arranged on the other side, and through interface pressure difference, the water vapor without the impurity ions is continuously absorbed by the outer electrolyte layer after permeating the water vapor mass transfer layer, and the outer electrolyte continuously enters the inner electrolyte layer through a peristaltic pump to provide pure water for electrolytic hydrogen production; finally, hydrogen and oxygen are generated by electrolysis on the catalytic layers (oxygen evolution catalytic layer and hydrogen evolution catalytic layer) on the inner electrolyte layer side. The water in the inner electrolyte layer is consumed by electrolysis, and meanwhile, the inner electrolyte continuously enters the outer electrolyte layer through a peristaltic pump, so that the pure water of the non-pure water solution is further obtained, the concentration of the electrolyte is kept constant, and the hydrogen is continuously generated in a reciprocating cycle.
A method for preparing hydrogen by electrolysis of non-pure water solution based on liquid phase moisture absorption adopts the system, and comprises the following steps:
the external power supply is connected with the cathode electrode and the anode electrode and is used for providing electric energy for hydrogen production reaction;
the water vapor mass transfer layer is close to the outer electrolyte layer and is directly contacted with the non-pure water solution, so that the non-pure water solution vapor is directly diffused through the water vapor mass transfer layer, the outer electrolyte layer directly absorbs the vapor diffused from the water vapor mass transfer layer, the outer electrolyte continuously enters the inner electrolyte layer through the peristaltic pump while continuously absorbing moisture, and an oxygen evolution reaction occurs on the surface of the oxygen evolution catalytic layer and a hydrogen evolution reaction occurs on the surface of the hydrogen evolution catalytic layer; the water in the inner electrolyte is consumed by electrolysis, and simultaneously the inner electrolyte continuously enters the outer electrolyte layer through a peristaltic pump to further obtain the water in the non-pure water solution, so that the concentration of the electrolyte is kept constant, and a reciprocating cycle is formed;
oxygen generated by the oxygen evolution reaction enters an oxygen collecting bottle after passing through an oxygen scrubber and an oxygen dryer, and hydrogen generated by the hydrogen evolution reaction passes through a hydrogen scrubber and hydrogenAnd the dryer is used for removing water vapor entrained in the hydrogen and then entering a hydrogen collecting bottle for storage and next utilization. H generated in this process + Or OH (OH) - Transfer occurs through an ion exchange membrane or diaphragm.
Compared with the prior art, the invention has the following beneficial effects:
the device and the system can obtain clean hydrogen energy through the non-pure water solution, can supply power through an external power supply in the energy conversion system of areas such as a floating island, a river and a lake in the future, directly obtain pure water vapor without impurity ions through the electrolyte layer attached to the water vapor mass transfer layer, and prepare hydrogen by utilizing the catalytic electrolysis principle, thereby realizing high-efficiency hydrogen energy acquisition.
The device and the system can be designed into an integrated device which is simply carried according to the hydrogen production requirement, can also be designed into an integrated device which is prepared on a large scale, can be used for carrying out non-intermittent hydrogen production operation in any places capable of producing water molecules, such as water gathering places of glaciers, rivers, waste water and the like, and is not limited by time and space.
The invention utilizes the difficult-to-treat substances such as sulfuric acid, and the like, and simultaneously has low cost and low price of the electrolyte. The device is simple and convenient in whole and easy to assemble and operate.
The electrolyte used in the invention can be replaced by solid electrolyte with moisture absorption capability, such as PVA, PAMPS and the like.
Drawings
FIG. 1 is a schematic diagram showing the structure of a non-pure water solution electrolytic hydrogen production apparatus based on liquid phase moisture absorption in example 1;
FIG. 2 is a schematic diagram showing the structure of a system for producing hydrogen by electrolysis of a non-pure water solution based on liquid phase moisture absorption in example 1;
FIG. 3 is a graph of sulfuric acid-induced water migration over time for example 1;
FIG. 4 is the result of direct constant voltage electrolysis of sulfuric acid in example 1;
FIG. 5 is a schematic diagram showing the structure of a non-pure water solution electrolytic hydrogen production apparatus based on liquid phase moisture absorption in accordance with example 2;
FIG. 6 is a schematic diagram showing the structure of a system for producing hydrogen by electrolysis of a non-pure water solution based on liquid phase moisture absorption in accordance with example 2;
FIG. 7 is a schematic diagram showing the structure of a system for producing hydrogen by electrolysis of a non-pure water solution based on liquid phase moisture absorption in accordance with example 3;
reference numerals: 1. an external power supply; 2. a hydrogen production reactor; 3. a water vapor mass transfer layer; 4. an outer electrolyte layer; 5. a first peristaltic pump; 6. a second peristaltic pump; 7. an inner electrolyte layer; 8. an anode electrode; 9. an oxygen evolution catalytic layer; 10. an oxygen scrubber; 11. an oxygen dryer; 12. an oxygen collection bottle; 13. an ion exchange membrane; 14. a hydrogen evolution catalytic layer; 15. a cathode electrode; 16. a hydrogen scrubber; 17. a hydrogen dryer; 18. a hydrogen collection bottle; 19. electrolyte layer.
Detailed Description
The present invention will be described in further detail with reference to the following examples in order to make the objects, technical solutions and advantages of the present invention more apparent. It should be understood that the specific embodiments described herein are for purposes of illustration only and are not intended to limit the scope of the invention.
Example 1
The non-pure water solution electrolytic hydrogen production device based on liquid phase moisture absorption in this embodiment is shown in fig. 1, and comprises: the hydrogen production reactor 2, the hydrogen production reactor 2 comprises an outer electrolyte layer 4, a water vapor mass transfer layer 3 attached to one side of the outer electrolyte layer 4, an inner electrolyte layer 7, an anode electrode 8 attached to the inner electrolyte layer 7 and sequentially arranged, an oxygen evolution catalytic layer 9, an ion exchange membrane 13, a hydrogen evolution catalytic layer 14 and a cathode electrode 15.
In the above device, the water vapor transfer layer 3 is a PTFE film having a pore diameter of 1 μm, the inner electrolyte layer 7 and the outer electrolyte layer 4 are solution tanks (sulfuric acid concentration of 20 wt%) for supporting a sulfuric acid solution having hygroscopicity, the anode electrode 8 is carbon paper having gas diffusivity, the oxygen evolution catalyst layer 9 is Ir/C, the ion exchange membrane 13 is a nafion film, the cathode electrode 15 is carbon paper having gas diffusivity, the hydrogen evolution catalyst layer 14 is Pt/C, and the ion exchange membrane 13 is a nafion film.
In the hydrogen production device of the embodiment, the outer electrolyte layer 4 is formed by a cuboid solution tank as a container of the outer electrolyte, and an opening at one side of the solution tank is attached to the water vapor mass transfer layer 3, so that the outer electrolyte is convenient to directly contact with the water vapor mass transfer layer 3, and water vapor permeated in the non-pure water solution is absorbed. The external electrolyte continuously absorbs water vapor and continuously enters the internal electrolyte layer 7 through the first peristaltic pump 5, the internal electrolyte layer 7 is taken as a containing vessel of the internal electrolyte by a cuboid solution tank, an opening at one side of the solution tank is in direct contact with the anode electrode 8 and generates electrolytic oxidation reaction on the anode to generate oxygen, and electrolytic hydrogen evolution reaction on the cathode to generate hydrogen. During electrolysis, the water of the inner electrolyte is consumed, and simultaneously the inner electrolyte continuously enters the outer electrolyte layer 4 through the second peristaltic pump 6 to further absorb the water of the non-pure water solution so as to maintain the concentration of the electrolyte constant, thereby forming a reciprocating cycle.
The system for producing hydrogen by electrolysis of non-pure water solution based on liquid phase moisture absorption in this embodiment is shown in fig. 2, and comprises the hydrogen production device, an external power supply 1 connected with an anode electrode 8 and a cathode electrode 15 for providing electric energy for hydrogen production reaction, a hydrogen scrubber 16, a hydrogen dryer 17, a hydrogen collecting bottle 18, an oxygen scrubber 10, an oxygen dryer 11 and an oxygen collecting bottle 12, wherein the hydrogen scrubber 16, the hydrogen dryer 17, the hydrogen collecting bottle 18, the oxygen scrubber 10, the oxygen dryer 11 and the oxygen collecting bottle 12 are sequentially communicated with the oxygen separation catalytic layer 9.
The specific working process of the non-pure water solution electrolytic hydrogen production system based on liquid phase moisture absorption in the embodiment is as follows:
the external power supply 1 is connected with the cathode electrode 15 and the anode electrode 8 and is used for providing electric energy for hydrogen production reaction; the water vapor mass transfer layer 3 is close to the outer electrolyte layer 4 and is directly contacted with the non-pure water solution, so that the non-pure water solution vapor is directly diffused through the water vapor mass transfer layer 3, the outer electrolyte layer 4 directly absorbs the vapor diffused from the water vapor mass transfer layer 3, meanwhile, the outer electrolyte continuously enters the inner electrolyte layer 7 through the first peristaltic pump 5, and the moisture in the inner electrolyte is subjected to oxidation reaction at an anode formed by the anode electrode 8 and the oxygen evolution catalytic layer 9 to generate oxygen; the inner electrolyte, which is consumed by electrolysis, continuously enters the outer electrolyte layer 4 through the second peristaltic pump 6, and further absorbs the moisture in the non-pure water solution to maintain the concentration of the electrolyte constant, thereby forming a reciprocating cycle.
Oxygen generated by the oxygen evolution reaction enters an oxygen collecting bottle after passing through an oxygen scrubber 10 and an oxygen dryer 1112, hydrogen generated by the hydrogen evolution reaction passes through a hydrogen scrubber 16 and a hydrogen dryer 17, and water vapor carried in the hydrogen is removed and then enters a hydrogen collecting bottle 18 for storage and next utilization. H generated in this process + Or OH (OH) - Transfer occurs through the ion exchange membrane 13 or separator.
The change graph of the migration amount of the sulfuric acid-induced water molecules with time is shown in fig. 3, which shows that sulfuric acid with different concentrations has a certain moisture absorption effect. The direct constant voltage electrolysis result of sulfuric acid is shown in fig. 4, which shows that the sulfuric acid after moisture absorption can generate electrolysis reaction to produce hydrogen and has certain stability.
Example 2
The apparatus for producing hydrogen by electrolysis of non-pure water solution based on liquid phase moisture absorption in this embodiment is shown in fig. 5, and comprises: an outer electrolyte layer 4, a water vapor mass transfer layer 3 attached to one side of the outer electrolyte layer 4, an inner electrolyte layer 7, an oxygen evolution catalytic layer 9 attached to the inner electrolyte layer 7 and arranged in this way, an ion exchange membrane 13 and a hydrogen evolution catalytic layer 14; the oxygen evolution catalyst layer 9 is embedded with an anode electrode 8, and the hydrogen evolution catalyst layer 14 is embedded with a cathode electrode 15.
In the device, the water vapor mass transfer layer 3 is a TPU film with the aperture of 1 mu m, the inner electrolyte layer 7 is a solution tank loaded with 1-ethyl-3 methylimidazole acetate ionic liquid, the anode electrode 8 is hydrophilic carbon paper with gas diffusivity, the oxygen evolution catalytic layer 9 is Ir/C, the ion exchange film 13 is a nafion film, the cathode electrode 15 is hydrophilic carbon paper with gas diffusivity, the hydrogen evolution catalytic layer 14 is Pt/C, and the ion exchange film 13 is a nafion film.
In the hydrogen production device of the embodiment, the outer electrolyte layer 4 is formed by a cuboid solution tank as a container of the outer electrolyte, and an opening at one side of the solution tank is attached to the water vapor mass transfer layer 3, so that the outer electrolyte is convenient to directly contact with the water vapor mass transfer layer 3, and water vapor permeated in the non-pure water solution is absorbed. The external electrolyte continuously absorbs water vapor and continuously enters the internal electrolyte layer 7 through the first peristaltic pump 5, the internal electrolyte layer 7 is formed by a cuboid solution tank as a container of the internal electrolyte, an opening at one side of the solution tank is in direct contact with the anode electrode 8 and generates electrolytic oxidation reaction on the anode to generate oxygen, and hydrogen evolution reaction occurs on the cathode to generate hydrogen. During electrolysis, the water of the inner electrolyte is consumed, and simultaneously the inner electrolyte continuously enters the outer electrolyte layer 4 through the second peristaltic pump 6, and further absorbs the water of the non-pure water solution to maintain the constant electrolysis concentration, thereby forming a reciprocating cycle.
The system for producing hydrogen by electrolysis of non-pure water solution based on liquid phase moisture absorption in this embodiment is shown in fig. 6, and comprises the hydrogen production device, an external power supply 1 connected with an anode electrode 8 and a cathode electrode 15 for providing electric energy for hydrogen production reaction, a hydrogen scrubber 16, a hydrogen dryer 17, a hydrogen collecting bottle 18, an oxygen scrubber 10, an oxygen dryer 11 and an oxygen collecting bottle 12, wherein the hydrogen scrubber 16, the hydrogen dryer 17, the hydrogen collecting bottle 18, the oxygen scrubber 10, the oxygen dryer 11 and the oxygen collecting bottle 12 are sequentially communicated with the oxygen separation catalytic layer 9.
The specific working process of the non-pure water solution electrolytic hydrogen production system based on liquid phase moisture absorption in the embodiment is as follows:
the external power supply 1 is connected with the cathode electrode 15 and the anode electrode 8 and is used for providing electric energy for hydrogen production reaction; the water vapor mass transfer layer 3 is close to the outer electrolyte layer 4 and is directly contacted with the non-pure water solution, so that the water vapor of the non-pure water solution is directly diffused through the water vapor mass transfer layer 3, the outer electrolyte layer 4 directly absorbs the water vapor diffused from the water vapor mass transfer layer 3, meanwhile, the outer electrolyte continuously enters the inner electrolyte layer 7 through the first peristaltic pump 5, and the moisture in the inner electrolyte layer is subjected to oxidation reaction in the oxygen-separating catalytic layer 9 (Ir/C, anode) embedded with the anode electrode 8 to generate oxygen; the inner electrolyte which is electrolyzed and consumes water continuously enters the outer electrolyte layer 4 through the second peristaltic pump 6, and further absorbs the water in the non-pure water solution to maintain the constant concentration of the electrolyte, so that a reciprocating cycle is formed;
oxygen generated by the oxygen evolution reaction enters an oxygen collecting bottle 12 after passing through an oxygen scrubber 10 and an oxygen dryer 11, hydrogen generated by the hydrogen evolution reaction enters a hydrogen collecting bottle 18 after being dehydrated by a hydrogen scrubber 16 and a hydrogen dryer 17, and is stored and utilized in the next step. The H+ or OH-generated in this process is transferred through the ion exchange membrane 13 or separator.
Example 3
The apparatus for producing hydrogen by electrolysis of non-pure water solution based on liquid phase moisture absorption in this embodiment is shown in fig. 7, and comprises: an electrolyte layer 19, a water vapor mass transfer layer 3 attached to one side of the electrolyte layer 19, an anode electrode 8 attached to the electrolyte layer 19 and arranged in sequence, an oxygen evolution catalytic layer 9, an ion exchange membrane 13, a hydrogen evolution catalytic layer 14 and a cathode electrode 15.
In the above device, the water vapor mass transfer layer 3 is a PTFE membrane having a pore diameter of 1 μm, the electrolyte layer 19 is a solution tank (sulfuric acid concentration of 20 wt%) for supporting a sulfuric acid solution having hygroscopicity, the anode electrode 8 is carbon paper having gas diffusivity, the oxygen evolution catalyst layer 9 is Ir/C, the ion exchange membrane 13 is a nafion membrane, the cathode electrode 15 is carbon paper having gas diffusivity, the hydrogen evolution catalyst layer 14 is Pt/C, and the ion exchange membrane 13 is a nafion membrane.
In the hydrogen production device of this embodiment, the electrolyte layer 19 is a container for static electrolyte in a rectangular solution tank, and an opening at one side of the solution tank is attached to the water vapor mass transfer layer 3, so that the electrolyte is in direct contact with the water vapor mass transfer layer 3, and water vapor permeated in the non-pure water solution is absorbed. The electrolyte continuously absorbs water vapor, the opening on the other side of the electrolyte tank is in direct contact with the anode electrode 8, electrolytic oxidation reaction occurs on the anode to generate oxygen, and reduction reaction occurs on the cathode electrode 15 to generate hydrogen. During electrolysis, the water of the electrolyte is consumed, and the electrolyte further absorbs the water of the non-pure water solution through the water vapor mass transfer layer 3 to maintain the concentration of the electrolyte constant, thereby forming a reciprocating cycle.
The system for producing hydrogen by electrolysis of non-pure water solution based on liquid phase moisture absorption in this embodiment is shown in fig. 7, and comprises the hydrogen production device, an external power supply 1 connected with an anode electrode 8 and a cathode electrode 15 for providing electric energy for hydrogen production reaction, a hydrogen scrubber 16, a hydrogen dryer 17, a hydrogen collecting bottle 18, an oxygen scrubber 10, an oxygen dryer 11 and an oxygen collecting bottle 12, wherein the hydrogen scrubber 16, the hydrogen dryer 17, the hydrogen collecting bottle 18, the oxygen scrubber 10, the oxygen dryer 11 and the oxygen collecting bottle 12 are sequentially communicated with the hydrogen evolution catalytic layer 14.
The specific working process of the non-pure water solution electrolytic hydrogen production system based on liquid phase moisture absorption in the embodiment is as follows:
the external power supply 1 is connected with the cathode electrode 15 and the anode electrode 8 and is used for providing electric energy for hydrogen production reaction; the water vapor mass transfer layer 3 is close to one side of the electrolyte layer 19 and is directly contacted with the non-pure water solution, so that the non-pure water solution vapor is directly diffused through the water vapor mass transfer layer 3, the electrolyte layer 19 directly absorbs the vapor diffused from the water vapor mass transfer layer 3, meanwhile, the moisture in the electrolyte generates oxygen through the oxidation reaction at an anode formed by the anode electrode 8 and the oxygen evolution catalytic layer 9, and generates hydrogen through the hydrogen evolution reaction at a cathode; the electrolyte of the consumed water further absorbs the water in the non-pure water solution to maintain the concentration of the electrolyte constant, thereby forming a reciprocating cycle.
Oxygen generated by the oxygen evolution reaction enters an oxygen collecting bottle 12 after passing through an oxygen scrubber 10 and an oxygen dryer 11, hydrogen generated by the hydrogen evolution reaction enters a hydrogen collecting bottle 18 after being dehydrated by a hydrogen scrubber 16 and a hydrogen dryer 17, and is stored and utilized in the next step. H generated in this process + Or OH (OH) - Transfer occurs through the ion exchange membrane 13 or separator.
The foregoing description of the preferred embodiments of the invention is not intended to be limiting, but rather is intended to cover all modifications, equivalents, and alternatives falling within the spirit and principles of the invention.
Claims (8)
1. A non-pure water solution electrolytic hydrogen production device based on liquid phase moisture absorption, which is characterized by comprising: an outer electrolyte layer (4) attached to the water vapor mass transfer layer (3) on one side of the outer electrolyte layer (4); an inner electrolyte layer (7) attached to an oxygen evolution catalyst layer (9) on one side of the inner electrolyte layer (7); a first peristaltic pump (5) and a second peristaltic pump (6) between the outer electrolyte layer (4) and the inner electrolyte layer (7); the device further comprises a hydrogen evolution catalytic layer (14), an ion exchange membrane (13) or a diaphragm positioned between the oxygen evolution catalytic layer (9) and the hydrogen evolution catalytic layer (14), wherein the oxygen evolution catalytic layer (9) is provided with an anode electrode (8), and the hydrogen evolution catalytic layer (14) is provided with a cathode electrode (15);
the water vapor mass transfer layer (3) is one of a TPU film, a PDMS film and a PTFE film with the aperture of 0.1-100 um, or is a porous water vapor mass transfer layer (3) prepared by spraying, screen printing and electrostatic adsorption of graphene, PVDF particles and PTFE particles;
the inner electrolyte layer (7) and the outer electrolyte layer (4) are one of an acidic solution with the concentration of 15-50 wt%, an alkaline solution with the concentration of 15-50 wt% and an ionic liquid.
2. The non-pure water solution electrolytic hydrogen production device based on liquid phase moisture absorption as claimed in claim 1, wherein the anode electrode (8) arranged on the oxygen evolution catalysis layer (9) can be embedded in the oxygen evolution catalysis layer (9) in a wrapping manner, and can be arranged between the oxygen evolution catalysis layer (9) and the inner electrolyte.
3. The non-pure water solution electrolytic hydrogen production device based on liquid phase moisture absorption as claimed in claim 1, wherein the cathode electrode (15) arranged on the hydrogen evolution catalytic layer (14) can be embedded in the hydrogen evolution catalytic layer (14) in a wrapping manner, and can be arranged outside the hydrogen evolution catalytic layer (14).
4. The non-pure water solution electrolytic hydrogen production device based on liquid phase moisture absorption as claimed in claim 1, wherein the hydrogen evolution catalytic layer (14) is one or a combination of several of non-noble metal alloy, non-noble metal phosphide, non-noble metal nitride, noble metal alloy catalyst and carbon; the oxygen evolution catalysis layer (9) is one of iridium carbon, ruthenium carbon, niFe-LDH, niFeCu alloy, iridium oxide, ruthenium oxide and platinum carbon catalyst.
5. A non-pure water solution electrolytic hydrogen production apparatus based on liquid phase moisture absorption as claimed in claim 1, wherein said anode electrode (8) is carbon paper or carbon cloth having gas diffusion property or porous material having electric conductivity, and said cathode electrode (15) is made of porous material having gas diffusion property and electric conductivity.
6. The non-pure water solution electrolytic hydrogen production device based on liquid phase moisture absorption as claimed in claim 1, wherein the ion exchange membrane (13) is a proton exchange membrane or an anion exchange membrane (13), and the diaphragm is a ceramic diaphragm.
7. A non-pure water solution electrolytic hydrogen production system based on liquid phase moisture absorption, which is characterized by comprising the device as claimed in any one of claims 1 to 6, an external power supply (1) connected with an anode electrode (8) and a cathode electrode (15) for providing electric energy for hydrogen production reaction, a hydrogen scrubber (16), a hydrogen dryer (17) and a hydrogen collecting bottle (18) which are sequentially communicated with a hydrogen evolution catalytic layer (14), and an oxygen scrubber (10), an oxygen dryer (11) and an oxygen collecting bottle (12) which are sequentially communicated with an oxygen evolution catalytic layer (9).
8. A method for producing hydrogen by electrolysis of a non-pure water solution based on liquid phase moisture absorption, characterized in that the method adopts the system of claim 7 to produce hydrogen, and comprises the following steps:
the external power supply (1) is connected with the cathode electrode (15) and the anode electrode (8) and is used for providing electric energy for hydrogen production reaction;
the water vapor mass transfer layer (3) is close to the outer electrolyte layer (4) and is directly contacted with the non-pure water solution, water molecules in the non-pure water solution migrate from the non-pure water solution to the outer electrolyte layer (4) under the action of interface pressure difference between the non-pure water solution and the outer electrolyte solution at two sides of the water vapor mass transfer layer (3), the outer electrolyte solution is continuously converged into the inner electrolyte layer (7) through the first peristaltic pump (5), the inner electrolyte solution generates oxygen evolution reaction on the surface of the oxygen evolution catalytic layer (9), and hydrogen evolution reaction occurs on the surface of the hydrogen evolution catalytic layer (14); the water in the inner electrolyte is consumed by electrolysis, and simultaneously the inner electrolyte continuously enters the outer electrolyte layer (4) through a second peristaltic pump (6), so that the water in the non-pure water solution is further obtained, the concentration of the electrolyte is kept constant, and a reciprocating cycle is formed, so that a stable hydrogen production process is formed;
oxygen generated by the oxygen evolution reaction enters an oxygen collecting bottle (12) after passing through an oxygen scrubber (10) and an oxygen dryer (11), hydrogen generated by the hydrogen evolution reaction enters a hydrogen collecting bottle (18) after passing through a hydrogen scrubber (16) and a hydrogen dryer (17) to remove water vapor carried in the hydrogen, and the hydrogen is stored and utilized in the next step.
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| CN115466968A (en) * | 2022-09-02 | 2022-12-13 | 四川大学 | Electrolysis hydrogen production system without pure water |
| CN115323399A (en) * | 2022-09-02 | 2022-11-11 | 四川大学 | Non-pure water solution desalination-free in-situ direct electrolysis hydrogen production device and use method |
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