CN113151852A - Electrooxidation and hydrogen evolution device and application - Google Patents
Electrooxidation and hydrogen evolution device and application Download PDFInfo
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- CN113151852A CN113151852A CN202110311991.5A CN202110311991A CN113151852A CN 113151852 A CN113151852 A CN 113151852A CN 202110311991 A CN202110311991 A CN 202110311991A CN 113151852 A CN113151852 A CN 113151852A
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- hydrogen evolution
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- 239000001257 hydrogen Substances 0.000 title claims abstract description 37
- 229910052739 hydrogen Inorganic materials 0.000 title claims abstract description 37
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 title claims abstract description 36
- 238000006056 electrooxidation reaction Methods 0.000 title claims abstract description 23
- 229910052799 carbon Inorganic materials 0.000 claims abstract description 60
- 239000007789 gas Substances 0.000 claims abstract description 50
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 48
- 238000009792 diffusion process Methods 0.000 claims abstract description 31
- 239000012528 membrane Substances 0.000 claims abstract description 28
- 238000007731 hot pressing Methods 0.000 claims abstract description 22
- 239000011230 binding agent Substances 0.000 claims abstract description 18
- 239000010411 electrocatalyst Substances 0.000 claims abstract description 17
- 239000005518 polymer electrolyte Substances 0.000 claims abstract description 10
- 239000011248 coating agent Substances 0.000 claims abstract description 8
- 238000000576 coating method Methods 0.000 claims abstract description 8
- JRZJOMJEPLMPRA-UHFFFAOYSA-N olefin Natural products CCCCCCCC=C JRZJOMJEPLMPRA-UHFFFAOYSA-N 0.000 claims abstract description 6
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical group [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 61
- ATUOYWHBWRKTHZ-UHFFFAOYSA-N Propane Chemical compound CCC ATUOYWHBWRKTHZ-UHFFFAOYSA-N 0.000 claims description 60
- 239000003054 catalyst Substances 0.000 claims description 56
- 239000001294 propane Substances 0.000 claims description 30
- 238000007254 oxidation reaction Methods 0.000 claims description 27
- 230000003647 oxidation Effects 0.000 claims description 26
- 238000011068 loading method Methods 0.000 claims description 21
- 229910052697 platinum Inorganic materials 0.000 claims description 17
- 238000005868 electrolysis reaction Methods 0.000 claims description 15
- 229920000557 Nafion® Polymers 0.000 claims description 14
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 claims description 12
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical group C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims description 12
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- 239000003792 electrolyte Substances 0.000 claims description 6
- 229910052703 rhodium Inorganic materials 0.000 claims description 6
- 239000010948 rhodium Substances 0.000 claims description 6
- MHOVAHRLVXNVSD-UHFFFAOYSA-N rhodium atom Chemical compound [Rh] MHOVAHRLVXNVSD-UHFFFAOYSA-N 0.000 claims description 6
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- 150000001336 alkenes Chemical class 0.000 claims description 5
- 239000004020 conductor Substances 0.000 claims description 5
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- 229910052692 Dysprosium Inorganic materials 0.000 claims description 3
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 claims description 3
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- 238000005275 alloying Methods 0.000 claims description 3
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- 239000011651 chromium Substances 0.000 claims description 3
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- 239000002131 composite material Substances 0.000 claims description 3
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- 239000010949 copper Substances 0.000 claims description 3
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- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 claims description 3
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- 239000003014 ion exchange membrane Substances 0.000 claims description 3
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- 229910052741 iridium Inorganic materials 0.000 claims description 3
- GKOZUEZYRPOHIO-UHFFFAOYSA-N iridium atom Chemical compound [Ir] GKOZUEZYRPOHIO-UHFFFAOYSA-N 0.000 claims description 3
- 229910052742 iron Inorganic materials 0.000 claims description 3
- 229910052746 lanthanum Inorganic materials 0.000 claims description 3
- FZLIPJUXYLNCLC-UHFFFAOYSA-N lanthanum atom Chemical compound [La] FZLIPJUXYLNCLC-UHFFFAOYSA-N 0.000 claims description 3
- WPBNNNQJVZRUHP-UHFFFAOYSA-L manganese(2+);methyl n-[[2-(methoxycarbonylcarbamothioylamino)phenyl]carbamothioyl]carbamate;n-[2-(sulfidocarbothioylamino)ethyl]carbamodithioate Chemical compound [Mn+2].[S-]C(=S)NCCNC([S-])=S.COC(=O)NC(=S)NC1=CC=CC=C1NC(=S)NC(=O)OC WPBNNNQJVZRUHP-UHFFFAOYSA-L 0.000 claims description 3
- 229910052759 nickel Inorganic materials 0.000 claims description 3
- 229940005657 pyrophosphoric acid Drugs 0.000 claims description 3
- 229910052707 ruthenium Inorganic materials 0.000 claims description 3
- KZUNJOHGWZRPMI-UHFFFAOYSA-N samarium atom Chemical compound [Sm] KZUNJOHGWZRPMI-UHFFFAOYSA-N 0.000 claims description 3
- GZCRRIHWUXGPOV-UHFFFAOYSA-N terbium atom Chemical compound [Tb] GZCRRIHWUXGPOV-UHFFFAOYSA-N 0.000 claims description 3
- 229910052718 tin Inorganic materials 0.000 claims description 3
- 239000011135 tin Substances 0.000 claims description 3
- 238000002360 preparation method Methods 0.000 abstract description 9
- QTBSBXVTEAMEQO-UHFFFAOYSA-N Acetic acid Chemical compound CC(O)=O QTBSBXVTEAMEQO-UHFFFAOYSA-N 0.000 description 24
- 238000003756 stirring Methods 0.000 description 20
- 238000006243 chemical reaction Methods 0.000 description 19
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 18
- KFZMGEQAYNKOFK-UHFFFAOYSA-N Isopropanol Chemical compound CC(C)O KFZMGEQAYNKOFK-UHFFFAOYSA-N 0.000 description 18
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 17
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 16
- 238000010438 heat treatment Methods 0.000 description 15
- 238000002156 mixing Methods 0.000 description 15
- 238000001035 drying Methods 0.000 description 14
- 238000000227 grinding Methods 0.000 description 14
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- HQABUPZFAYXKJW-UHFFFAOYSA-N butan-1-amine Chemical compound CCCCN HQABUPZFAYXKJW-UHFFFAOYSA-N 0.000 description 12
- 238000000034 method Methods 0.000 description 11
- 229910052786 argon Inorganic materials 0.000 description 9
- 238000004502 linear sweep voltammetry Methods 0.000 description 9
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- 239000002105 nanoparticle Substances 0.000 description 9
- 238000011056 performance test Methods 0.000 description 9
- FQNHWXHRAUXLFU-UHFFFAOYSA-N carbon monoxide;tungsten Chemical group [W].[O+]#[C-].[O+]#[C-].[O+]#[C-].[O+]#[C-].[O+]#[C-].[O+]#[C-] FQNHWXHRAUXLFU-UHFFFAOYSA-N 0.000 description 8
- 238000001548 drop coating Methods 0.000 description 8
- 230000002209 hydrophobic effect Effects 0.000 description 8
- JVTAAEKCZFNVCJ-UHFFFAOYSA-N lactic acid Chemical compound CC(O)C(O)=O JVTAAEKCZFNVCJ-UHFFFAOYSA-N 0.000 description 8
- 238000010408 sweeping Methods 0.000 description 8
- 238000009210 therapy by ultrasound Methods 0.000 description 8
- WRIDQFICGBMAFQ-UHFFFAOYSA-N (E)-8-Octadecenoic acid Natural products CCCCCCCCCC=CCCCCCCC(O)=O WRIDQFICGBMAFQ-UHFFFAOYSA-N 0.000 description 7
- QGLWBTPVKHMVHM-KTKRTIGZSA-N (z)-octadec-9-en-1-amine Chemical compound CCCCCCCC\C=C/CCCCCCCCN QGLWBTPVKHMVHM-KTKRTIGZSA-N 0.000 description 7
- LQJBNNIYVWPHFW-UHFFFAOYSA-N 20:1omega9c fatty acid Natural products CCCCCCCCCCC=CCCCCCCCC(O)=O LQJBNNIYVWPHFW-UHFFFAOYSA-N 0.000 description 7
- QSBYPNXLFMSGKH-UHFFFAOYSA-N 9-Heptadecensaeure Natural products CCCCCCCC=CCCCCCCCC(O)=O QSBYPNXLFMSGKH-UHFFFAOYSA-N 0.000 description 7
- 239000005642 Oleic acid Substances 0.000 description 7
- ZQPPMHVWECSIRJ-UHFFFAOYSA-N Oleic acid Natural products CCCCCCCCC=CCCCCCCCC(O)=O ZQPPMHVWECSIRJ-UHFFFAOYSA-N 0.000 description 7
- QXJSBBXBKPUZAA-UHFFFAOYSA-N isooleic acid Natural products CCCCCCCC=CCCCCCCCCC(O)=O QXJSBBXBKPUZAA-UHFFFAOYSA-N 0.000 description 7
- ZQPPMHVWECSIRJ-KTKRTIGZSA-N oleic acid Chemical compound CCCCCCCC\C=C/CCCCCCCC(O)=O ZQPPMHVWECSIRJ-KTKRTIGZSA-N 0.000 description 7
- 239000000843 powder Substances 0.000 description 7
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 6
- 239000000956 alloy Substances 0.000 description 6
- 229910045601 alloy Inorganic materials 0.000 description 6
- 239000011259 mixed solution Substances 0.000 description 6
- 238000010992 reflux Methods 0.000 description 6
- KLFRPGNCEJNEKU-FDGPNNRMSA-L (z)-4-oxopent-2-en-2-olate;platinum(2+) Chemical compound [Pt+2].C\C([O-])=C\C(C)=O.C\C([O-])=C\C(C)=O KLFRPGNCEJNEKU-FDGPNNRMSA-L 0.000 description 5
- 239000004310 lactic acid Substances 0.000 description 4
- 235000014655 lactic acid Nutrition 0.000 description 4
- CMHKGULXIWIGBU-UHFFFAOYSA-N [Fe].[Pt] Chemical compound [Fe].[Pt] CMHKGULXIWIGBU-UHFFFAOYSA-N 0.000 description 3
- WBLJAACUUGHPMU-UHFFFAOYSA-N copper platinum Chemical compound [Cu].[Pt] WBLJAACUUGHPMU-UHFFFAOYSA-N 0.000 description 3
- WTDPMEQSZXQVDG-UHFFFAOYSA-N lanthanum platinum Chemical compound [La].[Pt] WTDPMEQSZXQVDG-UHFFFAOYSA-N 0.000 description 3
- 238000004519 manufacturing process Methods 0.000 description 3
- 229910000510 noble metal Inorganic materials 0.000 description 3
- 239000003960 organic solvent Substances 0.000 description 3
- 239000000243 solution Substances 0.000 description 3
- SMZOUWXMTYCWNB-UHFFFAOYSA-N 2-(2-methoxy-5-methylphenyl)ethanamine Chemical compound COC1=CC=C(C)C=C1CCN SMZOUWXMTYCWNB-UHFFFAOYSA-N 0.000 description 2
- NIXOWILDQLNWCW-UHFFFAOYSA-N 2-Propenoic acid Natural products OC(=O)C=C NIXOWILDQLNWCW-UHFFFAOYSA-N 0.000 description 2
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 2
- 239000011149 active material Substances 0.000 description 2
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 239000001301 oxygen Substances 0.000 description 2
- 229910052760 oxygen Inorganic materials 0.000 description 2
- 239000010970 precious metal Substances 0.000 description 2
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- 239000002243 precursor Substances 0.000 description 2
- MBVAQOHBPXKYMF-LNTINUHCSA-N (z)-4-hydroxypent-3-en-2-one;rhodium Chemical compound [Rh].C\C(O)=C\C(C)=O.C\C(O)=C\C(C)=O.C\C(O)=C\C(C)=O MBVAQOHBPXKYMF-LNTINUHCSA-N 0.000 description 1
- QTBSBXVTEAMEQO-UHFFFAOYSA-M Acetate Chemical compound CC([O-])=O QTBSBXVTEAMEQO-UHFFFAOYSA-M 0.000 description 1
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 description 1
- YRKCREAYFQTBPV-UHFFFAOYSA-N acetylacetone Chemical class CC(=O)CC(C)=O YRKCREAYFQTBPV-UHFFFAOYSA-N 0.000 description 1
- 230000002378 acidificating effect Effects 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- ORTQZVOHEJQUHG-UHFFFAOYSA-L copper(II) chloride Chemical compound Cl[Cu]Cl ORTQZVOHEJQUHG-UHFFFAOYSA-L 0.000 description 1
- 125000000113 cyclohexyl group Chemical group [H]C1([H])C([H])([H])C([H])([H])C([H])(*)C([H])([H])C1([H])[H] 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 238000003487 electrochemical reaction Methods 0.000 description 1
- 229960002089 ferrous chloride Drugs 0.000 description 1
- 239000000446 fuel Substances 0.000 description 1
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- 150000002431 hydrogen Chemical class 0.000 description 1
- 239000012535 impurity Substances 0.000 description 1
- 229910052809 inorganic oxide Inorganic materials 0.000 description 1
- NMCUIPGRVMDVDB-UHFFFAOYSA-L iron dichloride Chemical compound Cl[Fe]Cl NMCUIPGRVMDVDB-UHFFFAOYSA-L 0.000 description 1
- ICAKDTKJOYSXGC-UHFFFAOYSA-K lanthanum(iii) chloride Chemical compound Cl[La](Cl)Cl ICAKDTKJOYSXGC-UHFFFAOYSA-K 0.000 description 1
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- 239000002184 metal Substances 0.000 description 1
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- 239000002135 nanosheet Substances 0.000 description 1
- 239000002077 nanosphere Substances 0.000 description 1
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- 150000004767 nitrides Chemical class 0.000 description 1
- JKDRQYIYVJVOPF-FDGPNNRMSA-L palladium(ii) acetylacetonate Chemical compound [Pd+2].C\C([O-])=C\C(C)=O.C\C([O-])=C\C(C)=O JKDRQYIYVJVOPF-FDGPNNRMSA-L 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
-
- 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 an electrooxidation and hydrogen evolution device, which comprises a current collector, a gas diffusion electrode and two flow field plates, wherein the gas diffusion electrode is positioned between the two flow field plates and comprises an anode, a cathode and a polymer electrolyte membrane; the anode is formed by coating an anode electrocatalyst and a binder on the surface of carbon paper; the cathode is formed by coating a cathode electrocatalyst and a binder on the surface of carbon paper; the gas diffusion electrode is formed by sequentially stacking the anode, the polymer electrolyte membrane and the cathode and then hot-pressing, and low-carbon alkane or low-carbon olefin is introduced into the anode side of the flow field plate. The electrooxidation and hydrogen evolution device has high energy efficiency in the hydrogen preparation process.
Description
Technical Field
The invention relates to an electrooxidation and hydrogen evolution device and application, belonging to the technical field of electrolysis.
Background
The electrooxidation and hydrogen evolution device is commonly used for preparing high-purity hydrogen by electrolyzing water, direct current is introduced into an electrolytic cell filled with electrolyte, water molecules generate electrochemical reaction on an electrode, under an acidic condition, oxygen is generated at an anode, and hydrogen is generated at a cathode. Compared with the hydrogen production by reforming natural gas, the hydrogen production technology by water electrolysis does not produce CO impurities, so the method is more suitable for the next step of fuel cell electrochemical conversion of hydrogen, and the large-scale preparation of high-purity hydrogen by the water electrolysis technology has wide application prospect. However, because the hydrogen evolution reaction is slow, conventional water electrolysis reactions require a large cell pressure (>1.5V) to accelerate the hydrogen evolution reaction, resulting in low energy efficiency in the hydrogen production process and a commercially insignificant product of oxygen produced on the anode side.
Disclosure of Invention
The invention provides an electrooxidation and hydrogen evolution device and application thereof, which can effectively solve the problems.
The invention is realized by the following steps:
an electrooxidation and hydrogen evolution device comprises a current collector, a gas diffusion electrode and two flow field plates, wherein the gas diffusion electrode is positioned between the two flow field plates and comprises an anode, a cathode and a polymer electrolyte membrane; the anode is formed by coating an anode electrocatalyst and a binder on the surface of carbon paper; the cathode is formed by coating a cathode electrocatalyst and a binder on the surface of carbon paper; the gas diffusion electrode is formed by sequentially stacking the anode, the polymer electrolyte membrane and the cathode and then hot-pressing, and low-carbon alkane or low-carbon olefin is introduced into the anode side of the flow field plate.
As a further refinement, the anode electrocatalyst is a Pt-based catalyst.
As a further improvement, the alloying element of the Pt-based catalyst is selected from platinum, ruthenium, rhodium, palladium, iridium, gold, nickel, iron, manganese, cobalt, copper, chromium, tin, lanthanum, cerium, samarium, terbium, dysprosium, or thulium.
As a further improvement, the polymer electrolyte membrane is selected from a Nafion membrane, a PBI membrane or an oxide proton conductor membrane.
As a further improvement, the binder is selected from Nafion, PBI, ionic liquids, pyrophosphoric acid composite electrolytes, oxide proton conducting or alkaline ion exchange membrane binders.
As a further improvement, the lower alkane or lower alkene is selected from methane, ethane, propane or propylene.
As a further improvement, the mass ratio of the anode electrocatalyst to the binder is 1: 0.3 to 0.9.
As a further improvement, the cathode electrocatalyst is a carbon-supported platinum catalyst.
As a further improvement, the loading capacity of the Pt-based catalyst on the anode is 1-5 mgPt/cm2。
The electrolysis method using the electrooxidation and hydrogen evolution device is characterized in that the electrolysis temperature is 60-400 ℃, the pressure of an electrolytic cell working tank is 0.3-1.4V, and the operating pressure is 0.1-10 Mpa.
The invention has the beneficial effects that:
the electrooxidation and hydrogen evolution device realizes that the current density of electrolysis can reach 333mA/cm when the cell voltage is lower than 1.5V2And the energy conversion efficiency is higher when electrolysis is carried out at a lower tank pressure compared with the traditional water electrolysis technology.
The anode reaction of the electrooxidation and hydrogen evolution device comprises the steps of preparing methanol by methane oxidation, preparing acetic acid by ethane oxidation, preparing lactic acid by propane oxidation and preparing acrylic acid and lactic acid by propylene oxidation, can convert low-carbon hydrocarbons into products with additional values, and has great application prospect.
Drawings
In order to more clearly illustrate the technical solutions of the embodiments of the present invention, the drawings that are required to be used in the embodiments will be briefly described below, it should be understood that the following drawings only illustrate some embodiments of the present invention and therefore should not be considered as limiting the scope, and for those skilled in the art, other related drawings can be obtained according to the drawings without inventive efforts.
Fig. 1 is a schematic structural diagram of an electrooxidation and hydrogen evolution apparatus according to an embodiment of the present invention.
FIG. 2 is a graph showing a potential-current curve in example 1. In the figure: as can be seen from the figure, the peak current density of the oxidation of propane catalyzed by the carbon-supported platinum catalyst can reach 220mA/cm2。
FIG. 3 is a graph showing a potential-current curve in example 2. In the figure: as can be seen from the figure, the peak current density of the oxidation of propane catalyzed by the carbon-supported palladium catalyst can reach 72mA/cm2。
FIG. 4 is a graph showing a potential-current curve in example 3. In the figure: as can be seen from the figure, the peak current density of the oxidation of propane catalyzed by the carbon-supported rhodium catalyst can reach 27mA/cm2。
FIG. 5 is a graph showing a potential-current curve in example 4. In the figure: as can be seen from the figure, the carbon-supported platinum-iron catalyst of the invention can catalyze propane to oxidize with peak current density of 118mA/cm2。
FIG. 6 is a graph showing a potential-current curve in example 5. In the figure: as can be seen from the figure, the peak current density of the oxidation of propane catalyzed by the carbon-supported platinum copper catalyst can reach 113mA/cm2。
FIG. 7 is a graph showing a potential-current curve in example 6. In the figure: as can be seen from the figure, the carbon-supported platinum lanthanum catalyst of the invention can catalyze propane to oxidize with peak current density of 101mA/cm2。
FIG. 8 is a graph showing a potential-current curve in example 7. In the figure: as can be seen from the figure, the peak current density of the oxidation of propane using PBI as the electrolyte in the present case can reach 100mA/cm2。
FIG. 9 is the potential-current of example 8The graph is schematic. In the figure: as can be seen from the figure, the peak current density of the oxidation of propane using the oxide proton conductor as the electrolyte in the present case can reach 230mA/cm2。
FIG. 10 is a graph showing a potential-current curve in example 9. In the figure: as can be seen from the figure, the maximum current density of the carbon-supported platinum catalyst for catalyzing the oxidation of propylene can reach 335mA/cm2。
Detailed Description
In order to make the objects, technical solutions and advantages of the embodiments of the present invention more apparent, the technical solutions of the embodiments of the present invention will be described clearly and completely with reference to the accompanying drawings of the embodiments of the present invention, and it is obvious that the described embodiments are some, but not all embodiments of the present invention. All other embodiments, which can be obtained by a person skilled in the art without any inventive step based on the embodiments of the present invention, are within the scope of the present invention. Thus, the following detailed description of the embodiments of the present invention, presented in the figures, is not intended to limit the scope of the invention, as claimed, but is merely representative of selected embodiments of the invention. All other embodiments, which can be obtained by a person skilled in the art without any inventive step based on the embodiments of the present invention, are within the scope of the present invention.
In the description of the present invention, the terms "first" and "second" are used for descriptive purposes only and are not to be construed as indicating or implying relative importance or implying any number of technical features indicated. Thus, a feature defined as "first" or "second" may explicitly or implicitly include one or more of that feature. In the description of the present invention, "a plurality" means two or more unless specifically defined otherwise.
Referring to fig. 1, an embodiment of the present invention provides an electrooxidation and hydrogen evolution apparatus, including a current collector, a gas diffusion electrode and two flow field plates, wherein the gas diffusion electrode is located between the two flow field plates, and the gas diffusion electrode includes an anode, a cathode and a polymer electrolyte membrane; the anode is formed by coating an anode electrocatalyst and a binder on the surface of carbon paper; the cathode is formed by coating a cathode electrocatalyst and a binder on the surface of carbon paper; the gas diffusion electrode is formed by sequentially stacking the anode, the polymer electrolyte membrane and the cathode and then hot-pressing, and low-carbon alkane or low-carbon olefin is introduced into the anode side of the flow field plate. The anode of the reactor generates electrocatalytic oxidation reaction of low-carbon alkane and olefin to convert the low-carbon alkane and olefin into a multi-carbon product with additional value; the cathode generates hydrogen precipitation reaction and is converted into high-purity hydrogen.
As a further refinement, the anode electrocatalyst is a Pt-based catalyst. The Pt-based catalyst is designed into a morphology regulation and alloying method, and comprises nanospheres, nanocubes, nano octahedrons, nanosheets, nanowires, nano truncated octahedrons and nano icosahedrons.
As a further improvement, the polymer electrolyte membrane is selected from a Nafion membrane, a PBI membrane or an oxide proton conductor membrane.
As a further improvement, the binder is selected from Nafion, PBI, ionic liquids, pyrophosphoric acid composite electrolytes, oxide proton conducting or alkaline ion exchange membrane binders. The mass concentration of the binder is 2-8 wt%, and preferably 5 wt%.
As a further improvement, the lower alkane or lower alkene is selected from methane, ethane, propane or propylene. The anode reaction comprises methane oxidation to prepare methanol, ethane oxidation to prepare acetic acid, propane oxidation to prepare lactic acid and propylene oxidation to prepare acrylic acid and lactic acid; the cathode reaction is water electrolysis hydrogen precipitation reaction; the overall reaction is exemplified by propane oxidation
As a further improvement, the mass ratio of the anode electrocatalyst to the binder is 1: 0.3 to 0.9.
As a further improvement, the cathode electrocatalyst is a carbon-supported platinum catalyst, and is a commercial carbon-supported platinum catalyst.
As a further improvement, the loading capacity of the Pt-based catalyst on the anode is 1-5 mgPt/cm2。
The electrolysis method applying the electrooxidation and hydrogen evolution device is characterized in that the electrolysis temperature is 60-400 ℃, the pressure of an electrolytic cell working tank is 0.3-1.4V, and the operating pressure is 0.1-10 Mpa. Preferably, the temperature of the electrolytic reaction is 60-150 ℃, the pressure of the working tank of the electrolytic cell is 0.6-1.2V, and the operating pressure is 0.1-0.5 Mpa.
As a further improvement, the flow rate of the electrolysis gas is 200-500 sccm.
The preparation method of the Pt-based catalyst comprises the following steps:
s1, stirring and dissolving a precursor of the noble metal or the alloy thereof by using oleylamine and oleic acid, heating to 130 ℃, adding tungsten hexacarbonyl, heating to 230-250 ℃, and reacting for 30-60 min; preferably, tungsten hexacarbonyl is added, and then the mixture is heated to 235-245 ℃ to react for 40-50 min. In this example, the reaction was carried out for 40min by heating to 240 ℃. The precursor of the metal or the alloy thereof is acetylacetone salt, acetate or chloride of platinum, ruthenium, rhodium, palladium, iridium, gold, nickel, iron, manganese, cobalt, copper, chromium, tin, lanthanum, cerium, samarium, terbium, dysprosium and thulium. Preferably: platinum acetylacetonate.
S2, centrifugally washing after reaction, drying in vacuum, grinding, dissolving the prepared powder with an organic solvent, adding a carrier, mixing, performing ultrasonic treatment, stirring, and continuously reacting for 12 hours to obtain carrier/precious metal or alloy nanoparticles thereof; the material of the carrier is carbon, inorganic nitride, inorganic carbide or inorganic oxide. Preferably: carbon, titanium dioxide.
S3, centrifugally washing the prepared carrier/precious metal or alloy nano particles thereof, drying and grinding to obtain a target catalyst, wherein the target catalyst comprises a carrier and an active material loaded on the carrier; the active material is a noble metal or an alloy thereof. In addition, the support/noble metal or alloy nanoparticles thereof are washed centrifugally with an organic solvent. Preferably, the organic solvent is cyclohexane or ethanol. In this example, ethanol was used.
Example 1
Preparation of carbon-supported platinum catalyst:
dispersing 20mg of platinum acetylacetonate in a mixed solution of 2mL of oleic acid and 8mL of oleylamine, and heating to 130 ℃ under vigorous stirring in an Ar atmosphere; adding 50mg of tungsten hexacarbonyl, stirring at a slow speed, raising the temperature to 240 ℃, and keeping the temperature for 40 min; centrifugally washing after reaction, drying in vacuum, grinding, dispersing the prepared powder by using butylamine, adding 10mg of carbon carrier, mixing, performing ultrasonic treatment for 2 hours, and stirring to continue reacting for 12 hours; heating and refluxing the prepared nano-particle acetic acid for 12h, centrifugally washing with ethanol, drying in vacuum, and grinding to obtain the target catalyst.
Preparing an anode: mixing 5 wt% of nafion and a carbon-supported platinum catalyst according to a mass ratio of 0.4: 1 preparing catalyst ink, taking isopropanol and water as a mixed solvent, dispersing for 1 hour by ultrasonic treatment, dripping the catalyst ink on the surface of commercial carbon paper (Ballard 3260) by adopting a dripping method, and controlling the Pt loading capacity of an anode to be 1mgPt/cm2. Preparing a cathode: commercial carbon paper (Ballard 3260) loaded with commercial Pt/C catalyst was selected, and the Pt loading was 0.4mgPt/cm2. The carbon paper needs to be subjected to surface hydrophobic treatment.
And sequentially stacking the anode, the nafion211 membrane and the cathode, and preparing the gas diffusion electrode in a hot pressing mode, wherein the hot pressing condition is 130 ℃ and 2 min. And a gas diffusion electrode is arranged between the two flow field plates to assemble an electrolytic cell. The temperature of the electrolytic cell is controlled to be 110 ℃, propane gas with 95 ℃ humidification is introduced into the anode, and argon gas with 95 ℃ humidification is introduced into the cathode. The cathode was used as a counter electrode and a reference electrode, and the propane oxidation performance test was performed by linear sweep voltammetry, sweeping at a sweep rate of 5mV/s, and recording the current-potential curve.
Example 2
Preparation of a palladium on carbon catalyst:
dispersing 20mg of palladium acetylacetonate in a mixed solution of 2mL of oleic acid and 8mL of oleylamine, and heating to 130 ℃ by vigorous stirring in an Ar atmosphere; adding 50mg of tungsten hexacarbonyl, stirring at a slow speed, raising the temperature to 240 ℃, and keeping the temperature for 40 min; centrifugally washing after reaction, drying in vacuum, grinding, dispersing the prepared powder by using butylamine, adding 10mg of carbon carrier, mixing, performing ultrasonic treatment for 2 hours, and stirring to continue reacting for 12 hours; heating and refluxing the prepared nano-particle acetic acid for 12h, centrifugally washing with ethanol, drying in vacuum, and grinding to obtain the target catalyst.
Preparing an anode: mixing 5 wt% of nafion and a carbon-supported palladium catalyst according to a mass ratio of 0.4: 1 preparing catalyst ink, taking isopropanol and water as a mixed solvent, and ultrasonically dispersing for 1 h. Catalyst ink was drop coated onto the surface of commercial carbon paper (Ballard 3260) using a drop coating process, with the anode Pt loading controlled to 1mgPt/cm2. Preparing a cathode: commercial Pt/C loaded carbon paper is selected, and the Pt loading capacity is 0.4mgPt/cm2. The carbon paper needs to be subjected to surface hydrophobic treatment.
And sequentially stacking the anode, the nafion211 membrane and the cathode, and preparing the gas diffusion electrode in a hot pressing mode, wherein the hot pressing condition is 130 ℃ and 2 min. And arranging a gas diffusion electrode between the two flow field plates to assemble an electrolytic cell. The temperature of the electrolytic cell is controlled to be 110 ℃, propane gas with 95 ℃ humidification is introduced into the anode, and argon gas with 95 ℃ humidification is introduced into the cathode. The cathode was used as a counter electrode and a reference electrode, and the propane oxidation performance test was performed by linear sweep voltammetry, sweeping at a sweep rate of 5mV/s, and recording the current-potential curve.
Example 3
Preparation of carbon supported rhodium catalyst:
dispersing 20mg of rhodium acetylacetonate in a mixed solution of 2mL of oleic acid and 8mL of oleylamine, and heating to 130 ℃ under vigorous stirring in an Ar atmosphere; adding 50mg of tungsten hexacarbonyl, stirring at a slow speed, raising the temperature to 240 ℃, and keeping the temperature for 40 min; centrifugally washing after reaction, drying in vacuum, grinding, dispersing the prepared powder by using butylamine, adding 10mg of carbon carrier, mixing, performing ultrasonic treatment for 2 hours, and stirring to continue reacting for 12 hours; heating and refluxing the prepared nano-particle acetic acid for 12h, centrifugally washing with ethanol, drying in vacuum, and grinding to obtain the target catalyst.
Preparing an anode: mixing 5 wt% of nafion with a carbon-supported rhodium catalyst according to a mass ratio of 0.4: 1 preparing catalyst ink, taking isopropanol and water as a mixed solvent, and ultrasonically dispersing for 1 h. Catalyst ink was drop coated onto the surface of commercial carbon paper (Ballard 3260) using a drop coating process, with the anode Pt loading controlled to 1mgPt/cm2. Preparing a cathode: commercial Pt/C loaded carbon paper is selected, and the Pt loading capacity is 0.4mgPt/cm2. The carbon paper needs surface thinningAnd (6) water treatment.
And sequentially stacking the anode, the nafion211 membrane and the cathode, and preparing the gas diffusion electrode in a hot pressing mode, wherein the hot pressing condition is 130 ℃ and 2 min. And arranging a gas diffusion electrode between the two flow field plates to assemble an electrolytic cell. The temperature of the electrolytic cell is controlled to be 110 ℃, propane gas with 95 ℃ humidification is introduced into the anode, and argon gas with 95 ℃ humidification is introduced into the cathode. The cathode was used as a counter electrode and a reference electrode, and the propane oxidation performance test was performed by linear sweep voltammetry, sweeping at a sweep rate of 5mV/s, and recording the current-potential curve.
Example 4
Preparation of carbon-supported platinum-iron catalyst:
dispersing 20mg of platinum acetylacetonate and 5mg of ferrous chloride tetrahydrate in a mixed solution of 2mL of oleic acid and 8mL of oleylamine, and violently stirring and heating to 130 ℃ in an Ar atmosphere; adding 50mg of tungsten hexacarbonyl, stirring at a slow speed, raising the temperature to 240 ℃, and keeping the temperature for 40 min; centrifugally washing after reaction, drying in vacuum, grinding, dispersing the prepared powder by using butylamine, adding 10mg of carbon carrier, mixing, performing ultrasonic treatment for 2 hours, and stirring to continue reacting for 12 hours; heating and refluxing the prepared nano-particle acetic acid for 12h, centrifugally washing with ethanol, drying in vacuum, and grinding to obtain the target catalyst.
Preparing an anode: mixing 5 wt% of nafion with a carbon-supported platinum-iron catalyst according to a mass ratio of 0.4: 1 preparing catalyst ink, taking isopropanol and water as a mixed solvent, and ultrasonically dispersing for 1 h. Catalyst ink was drop coated onto the surface of commercial carbon paper (Ballard 3260) using a drop coating process, with the anode Pt loading controlled to 1mgPt/cm2. Preparing a cathode: commercial Pt/C loaded carbon paper is selected, and the Pt loading capacity is 0.4mgPt/cm2. The carbon paper needs to be subjected to surface hydrophobic treatment.
And sequentially stacking the anode, the nafion211 membrane and the cathode, and preparing the gas diffusion electrode in a hot pressing mode, wherein the hot pressing condition is 130 ℃ and 2 min. And arranging a gas diffusion electrode between the two flow field plates to assemble an electrolytic cell. The temperature of the electrolytic cell is controlled to be 110 ℃, propane gas with 95 ℃ humidification is introduced into the anode, and argon gas with 95 ℃ humidification is introduced into the cathode. The cathode was used as a counter electrode and a reference electrode, and the propane oxidation performance test was performed by linear sweep voltammetry, sweeping at a sweep rate of 5mV/s, and recording the current-potential curve.
Example 5
Preparation of carbon-supported platinum-copper catalyst:
dispersing 20mg of platinum acetylacetonate and 10mg of copper chloride in a mixed solution of 2mL of oleic acid and 8mL of oleylamine, and heating to 130 ℃ by vigorous stirring in an Ar atmosphere; adding 50mg of tungsten hexacarbonyl, stirring at a slow speed, raising the temperature to 240 ℃, and keeping the temperature for 40 min; centrifugally washing after reaction, drying in vacuum, grinding, dispersing the prepared powder by using butylamine, adding 10mg of carbon carrier, mixing, performing ultrasonic treatment for 2 hours, and stirring to continue reacting for 12 hours; heating and refluxing the prepared nano-particle acetic acid for 12h, centrifugally washing with ethanol, drying in vacuum, and grinding to obtain the target catalyst.
Preparing an anode: mixing 5 wt% of nafion with a carbon-supported platinum-copper catalyst according to a mass ratio of 0.4: 1 preparing catalyst ink, taking isopropanol and water as a mixed solvent, and ultrasonically dispersing for 1 h. Catalyst ink was drop coated onto the surface of commercial carbon paper (Ballard 3260) using a drop coating process, with the anode Pt loading controlled to 1mgPt/cm2. Preparing a cathode: commercial Pt/C loaded carbon paper is selected, and the Pt loading capacity is 0.4mgPt/cm2. The carbon paper needs to be subjected to surface hydrophobic treatment.
And sequentially stacking the anode, the nafion211 membrane and the cathode, and preparing the gas diffusion electrode in a hot pressing mode, wherein the hot pressing condition is 130 ℃ and 2 min. And arranging a gas diffusion electrode between the two flow field plates to assemble an electrolytic cell. The temperature of the electrolytic cell is controlled to be 110 ℃, propane gas with 95 ℃ humidification is introduced into the anode, and argon gas with 95 ℃ humidification is introduced into the cathode. The cathode was used as a counter electrode and a reference electrode, and the propane oxidation performance test was performed by linear sweep voltammetry, sweeping at a sweep rate of 5mV/s, and recording the current-potential curve.
Example 6
Preparation of carbon-supported platinum lanthanum catalyst:
dispersing 20mg of platinum acetylacetonate and 10mg of lanthanum chloride in a mixed solution of 2mL of oleic acid and 8mL of oleylamine, and heating to 130 ℃ by vigorous stirring in an Ar atmosphere; adding 50mg of tungsten hexacarbonyl, stirring at a slow speed, raising the temperature to 240 ℃, and keeping the temperature for 40 min; centrifugally washing after reaction, drying in vacuum, grinding, dispersing the prepared powder by using butylamine, adding 10mg of carbon carrier, mixing, performing ultrasonic treatment for 2 hours, and stirring to continue reacting for 12 hours; heating and refluxing the prepared nano-particle acetic acid for 12h, centrifugally washing with ethanol, drying in vacuum, and grinding to obtain the target catalyst.
Preparing an anode: mixing 5 wt% of nafion with a carbon-supported platinum-lanthanum catalyst according to a mass ratio of 0.4: 1 preparing catalyst ink, taking isopropanol and water as a mixed solvent, and ultrasonically dispersing for 1 h. Catalyst ink was drop coated onto the surface of commercial carbon paper (Ballard 3260) using a drop coating process, with the anode Pt loading controlled to 1mgPt/cm2. Preparing a cathode: commercial Pt/C loaded carbon paper is selected, and the Pt loading capacity is 0.4mgPt/cm2. The carbon paper needs to be subjected to surface hydrophobic treatment.
And sequentially stacking the anode, the nafion211 membrane and the cathode, and preparing the gas diffusion electrode in a hot pressing mode, wherein the hot pressing condition is 130 ℃ and 2 min. And arranging a gas diffusion electrode between the two flow field plates to assemble an electrolytic cell. The temperature of the electrolytic cell is controlled to be 110 ℃, propane gas with 95 ℃ humidification is introduced into the anode, and argon gas with 95 ℃ humidification is introduced into the cathode. The cathode was used as a counter electrode and a reference electrode, and the propane oxidation performance test was performed by linear sweep voltammetry, sweeping at a sweep rate of 5mV/s, and recording the current-potential curve.
Example 7
The carbon supported platinum catalyst was prepared as in example 1.
Preparing an anode: mixing 5 wt% of nafion and a carbon-supported platinum catalyst according to a mass ratio of 0.4: 1 preparing catalyst ink, taking isopropanol and water as a mixed solvent, and ultrasonically dispersing for 1 h. Catalyst ink was drop coated onto the surface of commercial carbon paper (Ballard 3260) using a drop coating process, with the anode Pt loading controlled to 1mgPt/cm2. Preparing a cathode: commercial Pt/C loaded carbon paper is selected, and the Pt loading capacity is 0.4mgPt/cm2. The carbon paper needs to be subjected to surface hydrophobic treatment.
And sequentially stacking the anode, the PBI membrane and the cathode, and preparing the gas diffusion electrode in a hot pressing mode, wherein the hot pressing condition is 130 ℃ and 2 min. And arranging a gas diffusion electrode between the two flow field plates to assemble an electrolytic cell. The temperature of the electrolytic cell is controlled to be 150 ℃, dry propane gas is introduced into the anode, and dry argon gas is introduced into the cathode. The cathode was used as a counter electrode and a reference electrode, and the propane oxidation performance test was performed by linear sweep voltammetry, sweeping at a sweep rate of 5mV/s, and recording the current-potential curve.
Example 8
The carbon supported platinum catalyst was prepared as in example 1.
Preparing an anode: catalyst ink is prepared by using a carbon-supported platinum catalyst, isopropanol and water are used as mixed solvents, and ultrasonic dispersion is carried out for 1 hour. Catalyst ink was drop coated onto the surface of commercial carbon paper (Ballard 3260) using a drop coating process, with the anode Pt loading controlled to 1mgPt/cm2. Preparing a cathode: commercial Pt/C loaded carbon paper is selected, and the Pt loading capacity is 0.4mgPt/cm2. The carbon paper needs to be subjected to surface hydrophobic treatment.
And sequentially stacking the anode, the oxide proton conductor membrane and the cathode, and preparing the gas diffusion electrode in a hot pressing mode, wherein the hot pressing condition is 130 ℃ and 2 min. And arranging a gas diffusion electrode between the two flow field plates to assemble an electrolytic cell. The temperature of the electrolytic cell is controlled to be 400 ℃, dry propane gas is introduced into the anode, and dry argon gas is introduced into the cathode. The cathode was used as a counter electrode and a reference electrode, and the propane oxidation performance test was performed by linear sweep voltammetry, sweeping at a sweep rate of 5mV/s, and recording the current-potential curve.
Example 9
The carbon supported platinum catalyst was prepared as in example 1.
Preparing an anode: mixing 5 wt% of nafion and a carbon-supported platinum catalyst according to a mass ratio of 0.4: 1 preparing catalyst ink, taking isopropanol and water as a mixed solvent, and ultrasonically dispersing for 1 h. Catalyst ink was drop coated onto the surface of commercial carbon paper (Ballard 3260) using a drop coating process, with the anode Pt loading controlled to 1mgPt/cm2. Preparing a cathode: commercial Pt/C loaded carbon paper is selected, and the Pt loading capacity is 0.4mgPt/cm2. The carbon paper needs to be subjected to surface hydrophobic treatment.
And sequentially stacking the anode, the nafion211 membrane and the cathode, and preparing the gas diffusion electrode in a hot pressing mode, wherein the hot pressing condition is 130 ℃ and 2 min. And arranging a gas diffusion electrode between the two flow field plates to assemble an electrolytic cell. The temperature of the electrolytic cell is controlled to be 110 ℃, propylene gas with 95 ℃ humidification is introduced into the anode, and argon gas with 95 ℃ humidification is introduced into the cathode. The cathode is used as a counter electrode and a reference electrode, the propylene oxidation performance test is carried out by linear sweep voltammetry, scanning is carried out at the sweep rate of 5mV/s, and a current-potential curve is recorded.
The above description is only a preferred embodiment of the present invention and is not intended to limit the present invention, and various modifications and changes may be made by those skilled in the art. Any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention should be included in the protection scope of the present invention.
Claims (10)
1. An electrooxidation and hydrogen evolution device comprises a current collector, a gas diffusion electrode and two flow field plates, wherein the gas diffusion electrode is positioned between the two flow field plates; the anode is formed by coating an anode electrocatalyst and a binder on the surface of carbon paper; the cathode is formed by coating a cathode electrocatalyst and a binder on the surface of carbon paper; the gas diffusion electrode is formed by sequentially stacking the anode, the polymer electrolyte membrane and the cathode and then hot-pressing, and low-carbon alkane or low-carbon olefin is introduced into the anode side of the flow field plate.
2. The electro-oxidation and hydrogen evolution device of claim 1, wherein the anode electrocatalyst is a Pt-based catalyst.
3. The electrical oxidation and hydrogen evolution device according to claim 2, wherein the alloying element of the Pt-based catalyst is selected from platinum, ruthenium, rhodium, palladium, iridium, gold, nickel, iron, manganese, cobalt, copper, chromium, tin, lanthanum, cerium, samarium, terbium, dysprosium, or thulium.
4. The electro-oxidation and hydrogen evolution device according to claim 2, characterized in that the polymer electrolyte membrane is selected from the group consisting of Nafion membrane, PBI membrane or oxide proton conductor membrane.
5. The electro-oxidation and hydrogen evolution device of claim 1, wherein the binder is selected from the group consisting of Nafion, PBI, ionic liquids, pyrophosphoric acid composite electrolytes, oxide proton conducting or alkaline ion exchange membrane binders.
6. The electrooxidation and hydrogen evolution device of claim 1 wherein the lower alkane or lower alkene is selected from methane, ethane, propane or propylene.
7. The electrooxidation and hydrogen evolution device of claim 1 wherein the mass ratio of the anode electrocatalyst to binder is 1: 0.3 to 0.9.
8. The electrooxidation and hydrogen evolution device of claim 1 wherein the cathode electrocatalyst is a carbon supported platinum catalyst.
9. The electrooxidation and hydrogen evolution device of 1, characterized in that the loading capacity of the Pt-based catalyst on the anode is 1-5 mgPt/cm2。
10. An electrolysis method using the electro-oxidation and hydrogen evolution apparatus according to any one of claims 1 to 9, wherein the electrolysis temperature is 60 to 400 ℃, the pressure of the working tank of the electrolytic cell is 0.3 to 1.4V, and the operating pressure is 0.1 to 10 MPa.
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| US5607785A (en) * | 1995-10-11 | 1997-03-04 | Tanaka Kikinzoku Kogyo K.K. | Polymer electrolyte electrochemical cell and process of preparing same |
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