CN114000171A - Electrolytic hydrogen production system and method with hydrogen-oxygen recombination reactor - Google Patents
Electrolytic hydrogen production system and method with hydrogen-oxygen recombination reactor Download PDFInfo
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- CN114000171A CN114000171A CN202111229234.XA CN202111229234A CN114000171A CN 114000171 A CN114000171 A CN 114000171A CN 202111229234 A CN202111229234 A CN 202111229234A CN 114000171 A CN114000171 A CN 114000171A
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- 239000001257 hydrogen Substances 0.000 title claims abstract description 180
- 229910052739 hydrogen Inorganic materials 0.000 title claims abstract description 180
- 239000001301 oxygen Substances 0.000 title claims abstract description 149
- 229910052760 oxygen Inorganic materials 0.000 title claims abstract description 149
- 238000005215 recombination Methods 0.000 title claims abstract description 77
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- 238000004519 manufacturing process Methods 0.000 title claims abstract description 56
- 238000000034 method Methods 0.000 title abstract description 7
- 239000007788 liquid Substances 0.000 claims abstract description 158
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims abstract description 122
- 239000003513 alkali Substances 0.000 claims abstract description 58
- 239000003054 catalyst Substances 0.000 claims abstract description 52
- 239000007789 gas Substances 0.000 claims abstract description 34
- 239000000203 mixture Substances 0.000 claims abstract description 33
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 23
- 238000006555 catalytic reaction Methods 0.000 claims abstract description 18
- 238000006243 chemical reaction Methods 0.000 claims abstract description 10
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 claims description 24
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 24
- 238000005868 electrolysis reaction Methods 0.000 claims description 16
- 238000010438 heat treatment Methods 0.000 claims description 16
- 230000002093 peripheral effect Effects 0.000 claims description 13
- 238000005192 partition Methods 0.000 claims description 12
- 229910052697 platinum Inorganic materials 0.000 claims description 12
- 229910052763 palladium Inorganic materials 0.000 claims description 11
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 10
- 239000011148 porous material Substances 0.000 claims description 7
- 229910052684 Cerium Inorganic materials 0.000 claims description 5
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims description 5
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- GWXLDORMOJMVQZ-UHFFFAOYSA-N cerium Chemical compound [Ce] GWXLDORMOJMVQZ-UHFFFAOYSA-N 0.000 claims description 5
- 229910052759 nickel Inorganic materials 0.000 claims description 5
- 229910052703 rhodium Inorganic materials 0.000 claims description 5
- 239000010948 rhodium Substances 0.000 claims description 5
- MHOVAHRLVXNVSD-UHFFFAOYSA-N rhodium atom Chemical compound [Rh] MHOVAHRLVXNVSD-UHFFFAOYSA-N 0.000 claims description 5
- 229910052719 titanium Inorganic materials 0.000 claims description 5
- 239000010936 titanium Substances 0.000 claims description 5
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- 238000010586 diagram Methods 0.000 description 2
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- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 1
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- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 description 1
- 229920002647 polyamide Polymers 0.000 description 1
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- HBMJWWWQQXIZIP-UHFFFAOYSA-N silicon carbide Chemical compound [Si+]#[C-] HBMJWWWQQXIZIP-UHFFFAOYSA-N 0.000 description 1
- 229910010271 silicon carbide Inorganic materials 0.000 description 1
- 229910052814 silicon oxide Inorganic materials 0.000 description 1
- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 description 1
- 238000001179 sorption measurement Methods 0.000 description 1
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- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 description 1
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- 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
- C25B9/00—Cells or assemblies of cells; Constructional parts of cells; Assemblies of constructional parts, e.g. electrode-diaphragm assemblies; Process-related cell features
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B13/00—Oxygen; Ozone; Oxides or hydroxides in general
- C01B13/02—Preparation of oxygen
- C01B13/0229—Purification or separation processes
- C01B13/0233—Chemical processing only
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
- C01B3/50—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification
- C01B3/56—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification by contacting with solids; Regeneration of used solids
- C01B3/58—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification by contacting with solids; Regeneration of used solids including a catalytic reaction
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B5/00—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
- 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
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- 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
- C25B15/083—Separating products
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- 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
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- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Engineering & Computer Science (AREA)
- Inorganic Chemistry (AREA)
- Electrochemistry (AREA)
- Materials Engineering (AREA)
- Metallurgy (AREA)
- Combustion & Propulsion (AREA)
- General Chemical & Material Sciences (AREA)
- Analytical Chemistry (AREA)
- Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
Abstract
The invention provides an electrolytic hydrogen production system with an oxyhydrogen reunion reactor and a method, wherein the electrolytic hydrogen production system comprises an electrolytic bath, a hydrogen gas-liquid separator, an oxygen gas-liquid separator, a hydrogen drier and an oxygen drier; an alkali liquor and hydrogen mixture outlet of the electrolytic cell is sequentially communicated with an inlet of the hydrogen gas-liquid separator and an inlet of the hydrogen dryer; an alkali liquor and oxygen mixture outlet of the electrolytic cell is sequentially communicated with an inlet of the oxygen gas-liquid separator and an inlet of the oxygen dryer; the hydrogen gas-liquid separator and the oxygen gas-liquid separator both internally comprise an oxyhydrogen recombination catalysis layer for recombination reaction of hydrogen and oxygen. According to the electrolytic hydrogen production system with the hydrogen-oxygen recombination reactor, the hydrogen-oxygen recombination catalyst layer is added in the hydrogen-gas-liquid separator and the oxygen separator of the electrolytic hydrogen production system, and a small amount of impurity gas is combined with the product gas and converted into water again by using catalytic reaction, so that the product purity is improved.
Description
Technical Field
The invention belongs to the technical field of hydrogen energy, and particularly relates to an electrolytic hydrogen production system with an oxyhydrogen reunion reactor and a method.
Background
The water electrolysis hydrogen production is the only commercially available technical means for green hydrogen production at present. The existing water electrolysis hydrogen production system consists of an electrolytic cell and an auxiliary system, water is decomposed into hydrogen and oxygen through electrochemical reaction in the electrolytic cell, the hydrogen production reaction and the oxygen production reaction respectively occur on the cathode side and the anode side of the electrolytic cell, and the generated gas is collected after passing through a gas-liquid separator. The hydrogen product has certain requirements on the purity, the purity of the hydrogen produced by the electrolytic cell can generally reach 99.8%, and the oxygen purity can reach about 98%. The purity of hydrogen for the current fuel cell reaches 99.97 percent, the purity of pure hydrogen is 99.99 percent in national standard, and the purity of pure oxygen is 99.99 percent. In order to improve the use value of the product, a hydrogen and oxygen purification system is required to be added after the electrolytic cell. At present, a three-tower purification system is generally adopted for hydrogen and oxygen purification, three towers circularly carry out purification, temperature rise and regeneration operation, the heat consumption is large, the consumption of an adsorbent is large, the adaptability of purification to inlet gas flow change is poor, and the requirement of flexible operation under the input of a fluctuating power supply is difficult to meet.
Disclosure of Invention
In view of the above, a first object of the present invention is to provide an electrolytic hydrogen production system with an oxyhydrogen recombination reactor, in which an oxyhydrogen recombination catalyst layer is added in both a hydrogen gas-liquid separator and an oxygen gas separator of the electrolytic hydrogen production system, and a small amount of impurity gas is recombined with product gas and converted into water again by using catalytic reaction, so as to improve product purity, eliminate hydrogen and oxygen purification units in the system, reduce system floor space and complexity, and save overall investment.
The second purpose of the invention is to provide a method for producing hydrogen by water electrolysis.
In order to achieve the above object, an embodiment of the first aspect of the present invention provides an electrolytic hydrogen production system with an oxyhydrogen recombination reactor, comprising: the device comprises an electrolytic bath, a hydrogen gas-liquid separator, an oxygen gas-liquid separator, a hydrogen drier and an oxygen drier; an alkali liquor and hydrogen mixture outlet of the electrolytic cell is sequentially communicated with an inlet of the hydrogen gas-liquid separator and an inlet of the hydrogen dryer; an alkali liquor and oxygen mixture outlet of the electrolytic cell is sequentially communicated with an inlet of the oxygen gas-liquid separator and an inlet of the oxygen dryer; the hydrogen gas-liquid separator and the oxygen gas-liquid separator both internally comprise an oxyhydrogen recombination catalysis layer for recombination reaction of hydrogen and oxygen; the oxyhydrogen recombination catalysis layer is a carrier filling layer loaded with a gas combination catalyst, and the load amount of the gas combination catalyst is 5-10 wt%.
According to the electrolytic hydrogen production system with the hydrogen-oxygen recombination reactor, provided by the embodiment of the invention, the hydrogen-oxygen recombination catalyst layer is added in the hydrogen-gas-liquid separator and the oxygen separator of the electrolytic hydrogen production system, and a small amount of impurity gas is combined with the product gas and converted into water again by using catalytic reaction, so that the product purity is improved, a hydrogen and oxygen purification unit in the system can be omitted, the floor area and the complexity of the system are reduced, and the overall investment is saved.
In addition, the electrolytic hydrogen production system with the hydrogen-oxygen recombination reactor proposed according to the above embodiment of the present invention may also have the following additional technical features:
in one embodiment of the invention, a first clapboard and a second clapboard which can be used for the gas-liquid mixture to pass through are arranged in the hydrogen gas-liquid separator and the oxygen gas-liquid separator at a certain interval; the hydrogen and oxygen recombination catalysis layer is arranged between the first clapboard and the second clapboard.
In one embodiment of the invention, the first separator and the second separator are both rigid porous plates.
In one embodiment of the present invention, each of the first separator and the second separator is composed of a porous body and a peripheral connecting portion, and the pores on the porous body are uniformly distributed.
In one embodiment of the invention, the top parts of the hydrogen gas-liquid separator and the oxygen gas-liquid separator are both provided with gas outlets, and the bottom parts of the hydrogen gas-liquid separator and the oxygen gas-liquid separator are both provided with inlets for gas-liquid mixture to enter; in the hydrogen gas-liquid separator and the oxygen gas-liquid separator, respective oxyhydrogen recombination catalytic layers, the first partition plate and the second partition plate are arranged in parallel with the horizontal plane.
In one embodiment of the invention, heating units are arranged outside the hydrogen gas-liquid separator and the oxygen gas-liquid separator and at positions corresponding to the hydrogen and oxygen recombination catalytic layers respectively.
In one embodiment of the present invention, the support is an inorganic material or an organic material having a regular pore structure; the gas combination catalyst is an alloy formed by one or more than two of platinum, palladium, rhodium, titanium, zirconium, cerium and nickel.
In one embodiment of the invention, the electrolytic hydrogen production system with the hydrogen-oxygen recombination reactor further comprises an alkali liquor circulating pump, an alkali liquor filter and an alkali liquor cooler; the liquid outlet of the hydrogen gas-liquid separator and the liquid outlet of the oxygen gas-liquid separator are communicated with an alkali liquor circulating pump, an alkali liquor filter, an alkali liquor cooler and an electrolytic bath in sequence to form an alkali liquor circulating loop.
In order to achieve the above purpose, the second aspect of the invention provides a method for producing hydrogen by water electrolysis, which adopts the system for producing hydrogen by water electrolysis as described above to produce hydrogen by water electrolysis.
Additional aspects and advantages of the invention will be set forth in part in the description which follows and, in part, will be obvious from the description, or may be learned by practice of the invention.
Drawings
The foregoing and/or additional aspects and advantages of the present invention will become apparent and readily appreciated from the following description of the embodiments, taken in conjunction with the accompanying drawings of which:
FIG. 1 is a schematic diagram of a simple configuration of an electrolytic hydrogen production system with an oxyhydrogen recombination reactor according to one embodiment of the invention;
FIG. 2 is a simplified schematic front cross-sectional view of a hydrogen gas-liquid separator or an oxygen gas-liquid separator in an electrolytic hydrogen production system with an oxyhydrogen recombination reactor according to one embodiment of the present invention;
FIG. 3 is a top view of a first separator in a hydrogen gas-liquid separator or an oxygen gas-liquid separator in an electrolytic hydrogen production system with an oxyhydrogen recombination reactor according to one embodiment of the invention;
FIG. 4 is a top view of a second separator in a hydrogen gas-liquid separator or an oxygen gas-liquid separator in an electrolytic hydrogen production system with an oxyhydrogen recombination reactor according to one embodiment of the invention.
Reference numerals:
1-an electrolytic cell; 2-a hydrogen gas-liquid separator; 3-an oxygen gas-liquid separator; 4-a hydrogen dryer; 5-an oxygen dryer; 6-alkali liquor circulating pump; 7-an alkali liquor filter; 8-an alkali liquor cooler; 100-hydrogen and oxygen are combined with the catalyst layer; 200-a first separator; 2001-first separator porous body; 2002-a first separator plate peripheral connection; 300-a second separator; 3001-a second separator porous body; 3002-a second separator peripheral connection; 400-heating unit.
Detailed Description
Reference will now be made in detail to embodiments of the present invention, examples of which are illustrated in the accompanying drawings. The embodiments described below with reference to the drawings are illustrative and intended to be illustrative of the invention and are not to be construed as limiting the invention.
An electrolytic hydrogen production system with an oxyhydrogen recombination reactor according to an embodiment of the present invention will be described with reference to the accompanying drawings.
FIG. 1 is a schematic diagram of a simple configuration of an electrolytic hydrogen production system with an oxyhydrogen recombination reactor according to one embodiment of the invention.
As shown in fig. 1, an electrolytic hydrogen production system with an oxyhydrogen recombination reactor comprises an electrolytic bath 1, a hydrogen gas-liquid separator 2, an oxygen gas-liquid separator 3, a hydrogen dryer 4 and an oxygen dryer 5; an alkali liquor and hydrogen mixture outlet of the electrolytic cell 1 is sequentially communicated with an inlet of the hydrogen gas-liquid separator 2 and an inlet of the hydrogen dryer 4; an alkali liquor and oxygen mixture outlet of the electrolytic cell 1 is sequentially communicated with an inlet of the oxygen gas-liquid separator 3 and an inlet of the oxygen dryer 5; as shown in fig. 2, the hydrogen gas-liquid separator 2 and the oxygen gas-liquid separator 3 each include therein a hydrogen-oxygen recombination catalyst layer 100 for generating recombination reaction between hydrogen gas and oxygen gas. The oxyhydrogen recombination catalyst layer 100 is a carrier-packed layer loaded with a gas-combined catalyst, and the load amount of the gas-combined catalyst is 5 to 10 wt%.
The hydrogen and oxygen purifying unit is saved, the occupied area and the complexity of the system are reduced, only a simple dryer is needed, the existing hydrogen production system is simplified, and the overall investment is saved. Meanwhile, the traditional physical adsorption impurity removal mode is abandoned, the impurities in the gas are removed by means of the hydrogen and oxygen combined with the catalyst layer through catalytic reaction, the impurity removal effect is more reliable, the gas purity is high, the safety of the electrolytic hydrogen production system is improved, and the product quality is improved.
Optionally, a first partition plate 200 and a second partition plate 300 which are capable of allowing the gas-liquid mixture to pass through are further arranged in the hydrogen gas-liquid separator 2 and the oxygen gas-liquid separator 3 at a certain interval; the hydrogen and oxygen recombination catalyst layer 100 is disposed between the first separator 200 and the second separator 300.
It is understood that the above-described first separator and second separator have at least a function of supporting the hydrogen-oxygen recombination catalytic layer and restricting the positions of the hydrogen-oxygen recombination catalytic layer in the hydrogen gas-liquid separator 2 and the oxygen gas-liquid separator 3, in addition to passing the gas-liquid mixture from the electrolyzer. For this reason, optionally, the first separator 200 and the second separator 300 may both adopt hard porous plates, the porous plates may adopt materials with good oxidation resistance, corrosion resistance and high hardness, such as stainless steel, and the like, and the aperture of the hard porous plates is suitable for allowing gas-liquid mixture to pass through, and further may cause leakage of materials, such as catalyst of hydrogen-oxygen recombination catalyst layer, and the like.
Alternatively, as shown in fig. 3 and 4, each of the first separator 200 and the second separator 300 may have a structure including a porous body (a first separator porous body represented by 2001 in fig. 3 and a second separator porous body represented by 3001 in fig. 4) and a peripheral connecting portion (a first separator peripheral connecting portion represented by 2002 in fig. 3 and a second separator peripheral connecting portion represented by 3002 in fig. 4) provided outside the porous body to surround the entire porous body therebetween, and the porous body and the peripheral connecting portion may be integrally formed or may be fixed together by means of screw coupling or the like. Further alternatively, the porous body and the peripheral connecting portion may be formed in a flat plate shape as a whole. Preferably, the first and second separators 200 and 300 have shapes and sizes corresponding to those of the hydrogen gas-liquid separator 2 and the oxygen gas-liquid separator 3 at the locations where they are installed, so that the first and second separators 200 and 300 can be fixed to the inner walls of the hydrogen gas-liquid separator 2 and the oxygen gas-liquid separator 3 by welding or the like through peripheral connection portions.
It can be understood that, in the hydrogen electrolysis production system with the oxyhydrogen recombination reactor according to the embodiment of the present invention, the impurities in the gas are removed by the catalytic reaction by means of the oxyhydrogen recombination catalyst layer in the hydrogen gas-liquid separator and the oxygen gas-liquid separator, and the efficiency of the catalytic reaction is related to the contact area between the reactant and the catalyst, and in order to improve the efficiency of the catalytic reaction, the contact area between the gas-liquid mixture and the oxyhydrogen recombination catalyst layer is required to be larger, and therefore, the first separator and the second separator also have at least the function of dispersing the gas-liquid mixture, which requires the pores on the first separator and the second separator to be uniformly distributed, that is, the pores on the porous main body portion to be uniformly distributed (as shown in fig. 3 and fig. 4), and the porous main body to be ensured to correspond to the arrangement position of the oxyhydrogen recombination catalyst layer (as shown in fig. 2).
Preferably, in order to ensure sufficient contact between the gas-liquid mixture and the hydrogen-oxygen recombination catalyst layer, as shown in fig. 2, the shape and area of the first separator 200 and the second separator 300 are the same as the shape and area of the hydrogen-oxygen recombination catalyst layer 100, and both sides of the hydrogen-oxygen recombination catalyst layer 100 are respectively attached to the first separator 200 and the second separator 300.
Optionally, as shown in fig. 2, the hydrogen gas-liquid separator 2 and the oxygen gas-liquid separator 3 include a housing, the top of the housing is provided with a gas outlet, and the bottom of the housing is provided with an inlet for a gas-liquid mixture to enter; in the housing of the hydrogen gas-liquid separator 2 and the oxygen gas-liquid separator 3, the respective oxyhydrogen recombination catalyst layer 100, the first partition plate 200 and the second partition plate 300 are all arranged in parallel with the horizontal plane, and the first partition plate 200, the oxyhydrogen recombination catalyst layer 100 and the second partition plate 300 are all arranged in sequence from top to bottom and are positioned between the gas outlet and the inlet for the gas-liquid mixture to enter.
Optionally, as shown in fig. 2, in order to provide heat for the oxyhydrogen recombination reaction, the oxyhydrogen recombination reaction temperature can be conveniently controlled (i.e., the reaction temperature can be flexibly controlled) to improve the reaction efficiency, so that the requirement on the reaction catalyst is reduced, a non-noble metal catalyst can be used to reduce the overall cost, and the heating units 400 are respectively disposed at the positions outside the hydrogen gas-liquid separator 2 and the oxygen gas-liquid separator 3 (i.e., on the outer surface of the housing) corresponding to the respective oxyhydrogen recombination catalyst layers 100. Alternatively, the heating unit 400 may select one of heating jackets, coil heating, and the like, with a heating jacket being preferred. Further, in order to secure the heating effect, it is preferable that the heating unit 400 is highly uniform with the hydrogen-oxygen recombination catalyst layer 100.
Optionally, the carrier is an inorganic material or an organic material with a regular pore structure, for example, the carrier may be one or more of silicon carbide, silicon oxide, aluminum oxide, titanium oxide, a molecular sieve, graphene, a metal-organic framework (MOF) material, a high molecular polymer material (polyethylene, polypropylene, polyamide, polyethersulfone, and the like), and the like. The gas-bonding catalyst is selected from platinum, palladium, rhodium, titanium, zirconium, cerium or nickel, and also can adopt a multi-element alloy formed by more than two of platinum, palladium, rhodium, titanium, zirconium, cerium or nickel. When a multi-component alloy of two or more of platinum, palladium, rhodium, titanium, zirconium, cerium, and nickel is used as the composite catalyst, the metals in the composite catalyst may be mixed at any molar ratio, and for convenience, the metals in the composite catalyst are usually mixed at an equal molar ratio, for example, when a binary alloy of platinum and palladium is used as the gas-bonding catalyst, the molar ratio of platinum and palladium in the composite catalyst is 1: 1.
it should be noted that, in the hydrogen gas-liquid separator and the oxygen gas-liquid separator of the electrolytic hydrogen production system with the hydrogen-oxygen recombination reactor described in the above embodiment, impurities of gas species are removed by catalytic reaction, rich catalytic active sites are provided by using the porous catalytic layer, the catalytic effect is good, the gas purity is high, the safety of the electrolytic hydrogen production system is increased, and the product quality is improved. Meanwhile, compared with a conventional purification unit, the purification unit has abundant active sites, is simple to operate, does not need regeneration, and has stronger adaptability to fluctuating power supply input. When the reactor is used, on one hand, impurities are removed through the catalytic reaction of hydrogen and oxygen reunited with the catalyst layer, and on the other hand, gas-liquid separation is realized under the action of gravity, so that the hydrogen gas-liquid separator and the oxygen gas-liquid separator respectively form a gas-liquid separation-hydrogen and oxygen reunion reactor.
Optionally, in order to realize recycling of the alkali liquor, the electrolytic hydrogen production system with the hydrogen-oxygen recombination reactor further comprises an alkali liquor circulating pump 6, an alkali liquor filter 7 and an alkali liquor cooler 8; the liquid outlet of the hydrogen gas-liquid separator 2 and the liquid outlet of the oxygen gas-liquid separator 3 are communicated with an alkali liquor circulating pump 6, an alkali liquor filter 7, an alkali liquor cooler 8 and the electrolytic bath 1 in sequence to form an alkali liquor circulating loop.
In addition, a commercially available electrolytic cell for hydrogen production by electrolysis having a heating function may be used as the electrolytic cell 1. Thus, in addition to heating the alkali liquor by the electrolytic bath, the circulating alkali liquor can be heated by a heating unit (such as a heating jacket) outside the hydrogen gas-liquid separator and the oxygen gas-liquid separator, and the starting time is shortened.
When the hydrogen production system with the hydrogen-oxygen recombination reactor is used for water electrolysis hydrogen production (namely water electrolysis hydrogen production), the electrolytic tank 1 is filled with alkali liquor and gas mixture (including hydrogen and oxygen), the alkali liquor and hydrogen mixture enters the bottom of the hydrogen gas-liquid separator 2 from one end of the electrolytic tank 1, and the alkali liquor and oxygen mixture enters the bottom of the oxygen gas-liquid separator 3 from the other end of the electrolytic tank 1. Inside the hydrogen gas-liquid separator 2 and the oxygen gas-liquid separator 3, after the gas-liquid mixture is uniformly distributed from the second separator 300, the hydrogen and the oxygen are sequentially recombined with the catalyst layer 100 and the first separator 200. On the surface of the hydrogen-oxygen recombination catalyst layer 100 of the hydrogen gas-liquid separator 2, the trace oxygen contained in the hydrogen gas and the main hydrogen gas are recombined to react to generate water; on the surface of the oxyhydrogen recombination catalyst layer 100 of the oxygen gas-liquid separator 3, the trace hydrogen contained in the oxygen and the main oxygen are recombined to react to generate water; in the hydrogen gas-liquid separator 2 and the oxygen gas-liquid separator 3, the gas-liquid mixture is separated by gravity, the liquid is in the lower portion, the gas is in the upper portion, and the gas separated from the first partition 200 is a high purity gas containing water. The liquid at the lower parts of the hydrogen gas-liquid separator 2 and the oxygen gas-liquid separator 3 returns to the electrolytic bath 1 from the middle part of the electrolytic bath 1 through an alkali liquor circulating pump 6, an alkali liquor filter 7 and an alkali liquor cooler 8 to form alkali liquor circulation. The gas at the upper parts of the hydrogen gas-liquid separator 2 and the oxygen gas-liquid separator 3 respectively passes through a hydrogen drier 4 and an oxygen drier 5 to generate hydrogen and oxygen products. In the whole process, in order to enable the catalyst layer to be completely soaked by liquid, the liquid levels in the hydrogen gas-liquid separator 2 and the oxygen gas-liquid separator 3 are required to be over the respective hydrogen and oxygen, and then the hydrogen and oxygen are combined with the catalyst layer for 1001-2 cm.
The electrolytic hydrogen production system and method with an oxyhydrogen recombination reactor according to the present invention will be further described with reference to a specific example.
As shown in figure 1, an electrolytic hydrogen production system with an oxyhydrogen reunion reactor comprises an electrolytic bath 1, a hydrogen gas-liquid separator 2, an oxygen gas-liquid separator 3, a hydrogen drier 4, an oxygen drier 5, an alkali liquor circulating pump 6, an alkali liquor filter 7 and an alkali liquor cooler 8; an alkali liquor and hydrogen mixture outlet of the electrolytic cell 1 is sequentially communicated with an inlet of the hydrogen gas-liquid separator 2 and an inlet of the hydrogen dryer 4; an alkali liquor and oxygen mixture outlet of the electrolytic cell 1 is sequentially communicated with an inlet of the oxygen gas-liquid separator 3 and an inlet of the oxygen dryer 5; the liquid outlet of the hydrogen gas-liquid separator 2 and the liquid outlet of the oxygen gas-liquid separator 3 are communicated with an alkali liquor circulating pump 6, an alkali liquor filter 7, an alkali liquor cooler 8 and the electrolytic bath 1 in sequence to form an alkali liquor circulating loop. As shown in fig. 2, each of the hydrogen gas-liquid separator 2 and the oxygen gas-liquid separator 3 includes a cylindrical housing, the top of the housing is provided with a gas outlet, and the bottom of the housing is provided with an inlet and a liquid outlet for gas-liquid mixture to enter; the lower part of the middle in the shell is sequentially provided with a first clapboard 200, a hydrogen-oxygen recombination catalysis layer 100 and a second clapboard 300 from top to bottom, the first clapboard, the hydrogen-oxygen recombination catalysis layer 100 and the second clapboard 300 are all arranged in parallel with the horizontal plane, and the adjacent two are tightly attached. As shown in fig. 3 and 4, each of the first separator 200 and the second separator 300 is an integrally formed stainless steel porous plate, which has a porous body in the middle (the first separator porous body represented by 2001 in fig. 3 and the second separator porous body represented by 3001 in fig. 4), and a plurality of through holes are uniformly distributed; the periphery of the stainless steel porous body is a peripheral joint (a first diaphragm peripheral joint represented by 2002 in fig. 3 and a second diaphragm peripheral joint represented by 3002 in fig. 4), and the side wall thereof is welded to the inner wall of the casing. The shape of the first separator 200 and the second separator 300 is the same as the shape of the hydrogen-oxygen recombination catalyst layer 100, and both are circular, and the areas of the three are the same.
The oxyhydrogen recombination catalyst layer 100 in the hydrogen gas-liquid separator 2 and the oxygen gas-liquid separator 3 is a graphene filling layer loaded with a platinum and palladium binary alloy, and the molar ratio of platinum to palladium in the platinum and palladium binary alloy is 1: 1 and the total loading of platinum and palladium was 10 wt%.
As shown in fig. 2, heating jackets are installed on the outer surfaces of the respective housings of the hydrogen gas-liquid separator 2 and the oxygen gas-liquid separator 3 at positions corresponding to the respective hydrogen-oxygen recombination catalyst layers 100.
Wherein, the electrolytic tank 1 adopts a commercial electrolytic tank for hydrogen production by electrolysis with heating function.
When the hydrogen production system with the hydrogen-oxygen recombination reactor of the embodiment is used for water electrolysis hydrogen production (namely water electrolysis hydrogen production), the electrolytic cell 1 is filled with alkali liquor and gas mixture (including hydrogen and oxygen), the alkali liquor and hydrogen mixture enters the bottom of the hydrogen gas-liquid separator 2 from one end of the electrolytic cell 1, and the alkali liquor and oxygen mixture enters the bottom of the oxygen gas-liquid separator 3 from the other end of the electrolytic cell 1. Inside the hydrogen gas-liquid separator 2 and the oxygen gas-liquid separator 3, after the gas-liquid mixture is uniformly distributed from the second separator 300, the hydrogen and the oxygen are sequentially recombined with the catalyst layer 100 and the first separator 200. On the surface of the hydrogen-oxygen recombination catalyst layer 100 of the hydrogen gas-liquid separator 2, the trace oxygen contained in the hydrogen gas and the main hydrogen gas are recombined to react to generate water; on the surface of the oxyhydrogen recombination catalyst layer 100 of the oxygen gas-liquid separator 3, the trace hydrogen contained in the oxygen and the main oxygen are recombined to react to generate water; in the hydrogen gas-liquid separator 2 and the oxygen gas-liquid separator 3, the gas-liquid mixture is separated by gravity, the liquid is in the lower portion, the gas is in the upper portion, and the gas separated from the first partition 200 is a high purity gas containing water. The liquid at the lower parts of the hydrogen gas-liquid separator 2 and the oxygen gas-liquid separator 3 returns to the electrolytic bath 1 from the middle part of the electrolytic bath 1 through an alkali liquor circulating pump 6, an alkali liquor filter 7 and an alkali liquor cooler 8 to form alkali liquor circulation. The gas at the upper parts of the hydrogen gas-liquid separator 2 and the oxygen gas-liquid separator 3 respectively passes through a hydrogen drier 4 and an oxygen drier 5 to generate hydrogen and oxygen products. In the whole process, the liquid levels in the hydrogen gas-liquid separator 2 and the oxygen gas-liquid separator 3 are controlled to be over 1001.5 cm in combination with the catalytic layer after passing through respective hydrogen and oxygen.
After the electrolytic hydrogen production system with the hydrogen and oxygen reunion reactor is used for producing hydrogen by electrolyzing water, a chromatograph is used for analyzing the content of trace impurities in hydrogen and oxygen. The specific surface area of the hydrogen and oxygen recombination catalytic layer is 1340m2(g, bulk density)Is 1.2g/cm3The platinum and palladium loading of the catalyst was 10 wt%; the space velocity of the hydrogen and oxygen recombination catalyst layer is 0.1s-1. Gas purity was analyzed periodically as shown in table 1:
TABLE 1 Hydrogen and oxygen purities
| Time, h | 0 | 1 | 2 | 3 | 4 | 5 |
| Oxygen in hydrogen,%) | 0.001 | 0.001 | 0.001 | 0.001 | 0.001 | 0.001 |
| Hydrogen in oxygen,% | 0.003 | 0.002 | 0.002 | 0.002 | 0.003 | 0.002 |
Note: in Table 1, "%" represents volume fraction.
In the description of the present invention, it is to be understood that the terms "central," "longitudinal," "lateral," "length," "width," "thickness," "upper," "lower," "front," "rear," "left," "right," "vertical," "horizontal," "top," "bottom," "inner," "outer," "clockwise," "counterclockwise," "axial," "radial," "circumferential," and the like are used in the orientations and positional relationships indicated in the drawings for convenience in describing the invention and to simplify the description, and are not intended to indicate or imply that the referenced devices or elements must have a particular orientation, be constructed and operated in a particular orientation, and are therefore not to be considered limiting of the invention.
Furthermore, the terms "first", "second" and "first" are used for descriptive purposes only and are not to be construed as indicating or implying relative importance or implicitly indicating the number of technical features indicated. Thus, a feature defined as "first" or "second" may explicitly or implicitly include at least one such feature. In the description of the present invention, "a plurality" means at least two, e.g., two, three, etc., unless specifically limited otherwise.
In the present invention, unless otherwise expressly stated or limited, the terms "mounted," "connected," "secured," and the like are to be construed broadly and can, for example, be fixedly connected, detachably connected, or integrally formed; may be mechanically coupled, may be electrically coupled or may be in communication with each other; they may be directly connected or indirectly connected through intervening media, or they may be connected internally or in any other suitable relationship, unless expressly stated otherwise. The specific meanings of the above terms in the present invention can be understood by those skilled in the art according to specific situations.
In the present invention, unless otherwise expressly stated or limited, the first feature "on" or "under" the second feature may be directly contacting the first and second features or indirectly contacting the first and second features through an intermediate. Also, a first feature "on," "over," and "above" a second feature may be directly or diagonally above the second feature, or may simply indicate that the first feature is at a higher level than the second feature. A first feature being "under," "below," and "beneath" a second feature may be directly under or obliquely under the first feature, or may simply mean that the first feature is at a lesser elevation than the second feature.
In the present disclosure, the terms "one embodiment," "some embodiments," "an example," "a specific example," or "some examples" and the like mean that a specific feature, structure, material, or characteristic described in connection with the embodiment or example is included in at least one embodiment or example of the present disclosure. In this specification, the schematic representations of the terms used above are not necessarily intended to refer to the same embodiment or example. Furthermore, the particular features, structures, materials, or characteristics described may be combined in any suitable manner in any one or more embodiments or examples. Furthermore, various embodiments or examples and features of different embodiments or examples described in this specification can be combined and combined by one skilled in the art without contradiction.
Although embodiments of the present invention have been shown and described above, it is understood that the above embodiments are exemplary and should not be construed as limiting the present invention, and that variations, modifications, substitutions and alterations can be made to the above embodiments by those of ordinary skill in the art within the scope of the present invention.
Claims (10)
1. An electrolytic hydrogen production system with an oxyhydrogen recombination reactor, comprising: an electrolytic bath (1), a hydrogen gas-liquid separator (2), an oxygen gas-liquid separator (3), a hydrogen drier (4) and an oxygen drier (5);
an alkali liquor and hydrogen mixture outlet of the electrolytic cell (1) is sequentially communicated with an inlet of the hydrogen gas-liquid separator (2) and an inlet of the hydrogen dryer (4); an alkali liquor and oxygen mixture outlet of the electrolytic cell (1) is sequentially communicated with an inlet of the oxygen gas-liquid separator (3) and an inlet of the oxygen dryer (5);
the hydrogen gas-liquid separator (2) and the oxygen gas-liquid separator (3) both internally comprise a hydrogen-oxygen recombination catalysis layer (100) for recombination reaction of hydrogen and oxygen; the oxyhydrogen recombination catalysis layer (100) is a carrier filling layer loaded with a gas combination catalyst, and the load amount of the gas combination catalyst is 5-10 wt%.
2. The system for electrolytic hydrogen production with an oxyhydrogen recombination reactor according to claim 1, wherein a first partition (200) and a second partition (300) for allowing a gas-liquid mixture to pass through are further arranged in the hydrogen gas-liquid separator (2) and the oxygen gas-liquid separator (3) at intervals; the hydrogen and oxygen recombination catalysis layer (100) is arranged between the first separator (200) and the second separator (300).
3. The system for electrolytic hydrogen production with an oxyhydrogen recombination reactor according to claim 2, wherein the first separator (200) and the second separator (300) are both rigid porous plates.
4. The system for electrolytic hydrogen production with an oxyhydrogen recombination reactor according to claim 2, wherein the first separator (200) and the second separator (300) are each composed of a porous body and a peripheral connection part, and the pores on the porous body are uniformly distributed.
5. The system for electrolytic hydrogen production with an oxyhydrogen recombination reactor according to any one of claims 2 to 4, wherein the top of the hydrogen gas-liquid separator (2) and the top of the oxygen gas-liquid separator (3) are both provided with a gas outlet, and the bottom of the hydrogen gas-liquid separator is both provided with an inlet for the entry of a gas-liquid mixture; in the hydrogen gas-liquid separator (2) and the oxygen gas-liquid separator (3), the respective oxyhydrogen recombination catalyst layer (100), the first clapboard (200) and the second clapboard (300) are all arranged in parallel with the horizontal plane.
6. The system for electrolytic hydrogen production with an oxyhydrogen recombination reactor according to claim 1, wherein the hydrogen gas-liquid separator (2) and the oxygen gas-liquid separator (3) are provided with heating units (400) at positions corresponding to the respective oxyhydrogen recombination catalyst layers (100) outside.
7. The system for electrolytic hydrogen production with an oxyhydrogen recombination reactor according to claim 1, wherein the carrier is an inorganic material or an organic material with a regular pore structure.
8. The system for electrolytic hydrogen production with an oxyhydrogen recombination reactor according to claim 1 or 7, wherein the gas-bonding catalyst is an alloy of one or more of platinum, palladium, rhodium, titanium, zirconium, cerium and nickel.
9. The system for electrolytic hydrogen production with an oxyhydrogen recombination reactor according to claim 1, further comprising an alkali circulation pump (6), an alkali filter (7) and an alkali cooler (8); the liquid outlet of the hydrogen gas-liquid separator (2) and the liquid outlet of the oxygen gas-liquid separator (3) are communicated with an alkali liquor circulating pump (6), an alkali liquor filter (7), an alkali liquor cooler (8) and an electrolytic bath (1) in sequence to form an alkali liquor circulating loop.
10. A method for producing hydrogen by water electrolysis, characterized in that hydrogen is produced by water electrolysis by using the hydrogen production electrolysis system according to any one of claims 1 to 9.
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