CN117117225A - Direct organic liquid fuel cell based on liquid hydrogen storage material - Google Patents
Direct organic liquid fuel cell based on liquid hydrogen storage material Download PDFInfo
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- 239000007788 liquid Substances 0.000 title claims abstract description 122
- 239000001257 hydrogen Substances 0.000 title claims abstract description 102
- 229910052739 hydrogen Inorganic materials 0.000 title claims abstract description 102
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 title claims abstract description 99
- 239000000446 fuel Substances 0.000 title claims abstract description 31
- 239000011232 storage material Substances 0.000 title claims abstract description 18
- 239000003054 catalyst Substances 0.000 claims abstract description 89
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 claims abstract description 37
- 125000004435 hydrogen atom Chemical group [H]* 0.000 claims abstract description 8
- 229910052707 ruthenium Inorganic materials 0.000 claims abstract description 7
- 229910052709 silver Inorganic materials 0.000 claims abstract description 7
- 230000005611 electricity Effects 0.000 claims abstract description 4
- 239000012528 membrane Substances 0.000 claims description 55
- 238000009792 diffusion process Methods 0.000 claims description 32
- 239000007789 gas Substances 0.000 claims description 32
- UQSQSQZYBQSBJZ-UHFFFAOYSA-N fluorosulfonic acid Chemical group OS(F)(=O)=O UQSQSQZYBQSBJZ-UHFFFAOYSA-N 0.000 claims description 27
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Substances [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 25
- BLRHMMGNCXNXJL-UHFFFAOYSA-N 1-methylindole Chemical compound C1=CC=C2N(C)C=CC2=C1 BLRHMMGNCXNXJL-UHFFFAOYSA-N 0.000 claims description 7
- OXQOBQJCDNLAPO-UHFFFAOYSA-N 2,3-Dimethylpyrazine Chemical compound CC1=NC=CN=C1C OXQOBQJCDNLAPO-UHFFFAOYSA-N 0.000 claims description 7
- CAWHJQAVHZEVTJ-UHFFFAOYSA-N methylpyrazine Chemical compound CC1=CN=CC=N1 CAWHJQAVHZEVTJ-UHFFFAOYSA-N 0.000 claims description 7
- QRRKZFCXXBFHSV-UHFFFAOYSA-N 1-ethylindole Chemical compound C1=CC=C2N(CC)C=CC2=C1 QRRKZFCXXBFHSV-UHFFFAOYSA-N 0.000 claims description 6
- PBMFSQRYOILNGV-UHFFFAOYSA-N pyridazine Chemical compound C1=CC=NN=C1 PBMFSQRYOILNGV-UHFFFAOYSA-N 0.000 claims description 6
- KYQCOXFCLRTKLS-UHFFFAOYSA-N Pyrazine Chemical compound C1=CN=CC=N1 KYQCOXFCLRTKLS-UHFFFAOYSA-N 0.000 claims description 5
- 150000002894 organic compounds Chemical class 0.000 claims description 5
- KEOWKZFSSBVUIW-UHFFFAOYSA-N 1h-cyclopenta[b]pyrazine Chemical compound C1=CNC2=CC=CC2=N1 KEOWKZFSSBVUIW-UHFFFAOYSA-N 0.000 claims description 4
- LCZUOKDVTBMCMX-UHFFFAOYSA-N 2,5-Dimethylpyrazine Chemical compound CC1=CN=C(C)C=N1 LCZUOKDVTBMCMX-UHFFFAOYSA-N 0.000 claims description 4
- PCNDJXKNXGMECE-UHFFFAOYSA-N Phenazine Natural products C1=CC=CC2=NC3=CC=CC=C3N=C21 PCNDJXKNXGMECE-UHFFFAOYSA-N 0.000 claims description 3
- 239000000463 material Substances 0.000 claims description 3
- 239000001934 2,5-dimethylpyrazine Substances 0.000 claims description 2
- 150000004678 hydrides Chemical class 0.000 claims description 2
- 125000004433 nitrogen atom Chemical group N* 0.000 claims description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 27
- 229910052799 carbon Inorganic materials 0.000 description 27
- 238000000034 method Methods 0.000 description 20
- 238000012360 testing method Methods 0.000 description 17
- 230000000052 comparative effect Effects 0.000 description 16
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 12
- 229910052719 titanium Inorganic materials 0.000 description 12
- 239000010936 titanium Substances 0.000 description 12
- 238000006356 dehydrogenation reaction Methods 0.000 description 10
- 239000001301 oxygen Substances 0.000 description 10
- 229910052760 oxygen Inorganic materials 0.000 description 10
- 238000006555 catalytic reaction Methods 0.000 description 7
- 238000006243 chemical reaction Methods 0.000 description 6
- -1 on the other hand Substances 0.000 description 6
- 230000008569 process Effects 0.000 description 6
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 5
- 238000010248 power generation Methods 0.000 description 5
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 4
- 229910021126 PdPt Inorganic materials 0.000 description 4
- 238000005516 engineering process Methods 0.000 description 4
- 150000002431 hydrogen Chemical class 0.000 description 3
- 238000007086 side reaction Methods 0.000 description 3
- 239000000126 substance Substances 0.000 description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 3
- UJOBWOGCFQCDNV-UHFFFAOYSA-N 9H-carbazole Chemical compound C1=CC=C2C3=CC=CC=C3NC2=C1 UJOBWOGCFQCDNV-UHFFFAOYSA-N 0.000 description 2
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 2
- SMWDFEZZVXVKRB-UHFFFAOYSA-N Quinoline Chemical compound N1=CC=CC2=CC=CC=C21 SMWDFEZZVXVKRB-UHFFFAOYSA-N 0.000 description 2
- 230000009471 action Effects 0.000 description 2
- 230000006978 adaptation Effects 0.000 description 2
- 230000009286 beneficial effect Effects 0.000 description 2
- 230000003197 catalytic effect Effects 0.000 description 2
- 238000002485 combustion reaction Methods 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 238000002474 experimental method Methods 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 229910052757 nitrogen Inorganic materials 0.000 description 2
- 229910052697 platinum Inorganic materials 0.000 description 2
- 231100000572 poisoning Toxicity 0.000 description 2
- 230000000607 poisoning effect Effects 0.000 description 2
- 230000002441 reversible effect Effects 0.000 description 2
- PLAZXGNBGZYJSA-UHFFFAOYSA-N 9-ethylcarbazole Chemical compound C1=CC=C2N(CC)C3=CC=CC=C3C2=C1 PLAZXGNBGZYJSA-UHFFFAOYSA-N 0.000 description 1
- SDFLTYHTFPTIGX-UHFFFAOYSA-N 9-methylcarbazole Chemical compound C1=CC=C2N(C)C3=CC=CC=C3C2=C1 SDFLTYHTFPTIGX-UHFFFAOYSA-N 0.000 description 1
- 239000004215 Carbon black (E152) Substances 0.000 description 1
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 1
- XDTMQSROBMDMFD-UHFFFAOYSA-N Cyclohexane Chemical compound C1CCCCC1 XDTMQSROBMDMFD-UHFFFAOYSA-N 0.000 description 1
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 1
- 229910021124 PdAg Inorganic materials 0.000 description 1
- GLUUGHFHXGJENI-UHFFFAOYSA-N Piperazine Chemical compound C1CNCCN1 GLUUGHFHXGJENI-UHFFFAOYSA-N 0.000 description 1
- 239000011865 Pt-based catalyst Substances 0.000 description 1
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical group [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 description 1
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 1
- 150000001336 alkenes Chemical class 0.000 description 1
- 150000001345 alkine derivatives Chemical class 0.000 description 1
- 125000006615 aromatic heterocyclic group Chemical group 0.000 description 1
- 150000004945 aromatic hydrocarbons Chemical class 0.000 description 1
- 125000003118 aryl group Chemical group 0.000 description 1
- 229910002092 carbon dioxide Inorganic materials 0.000 description 1
- 239000001569 carbon dioxide Substances 0.000 description 1
- 229910002091 carbon monoxide Inorganic materials 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 239000000571 coke Substances 0.000 description 1
- 238000013329 compounding Methods 0.000 description 1
- 230000009849 deactivation Effects 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 238000003487 electrochemical reaction Methods 0.000 description 1
- 238000004146 energy storage Methods 0.000 description 1
- 238000003912 environmental pollution Methods 0.000 description 1
- 150000002391 heterocyclic compounds Chemical class 0.000 description 1
- 229930195733 hydrocarbon Natural products 0.000 description 1
- 239000012535 impurity Substances 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 229910052763 palladium Inorganic materials 0.000 description 1
- 230000010287 polarization Effects 0.000 description 1
- 238000006116 polymerization reaction Methods 0.000 description 1
- 238000012545 processing Methods 0.000 description 1
- 238000010926 purge Methods 0.000 description 1
- 125000003373 pyrazinyl group Chemical group 0.000 description 1
- 238000004064 recycling Methods 0.000 description 1
- 238000000926 separation method Methods 0.000 description 1
- 239000004332 silver Substances 0.000 description 1
- 230000000087 stabilizing effect Effects 0.000 description 1
- 239000000758 substrate Substances 0.000 description 1
- 230000001131 transforming effect Effects 0.000 description 1
- 229910052723 transition metal Inorganic materials 0.000 description 1
- 150000003624 transition metals Chemical class 0.000 description 1
Classifications
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/90—Selection of catalytic material
- H01M4/92—Metals of platinum group
- H01M4/925—Metals of platinum group supported on carriers, e.g. powder carriers
- H01M4/926—Metals of platinum group supported on carriers, e.g. powder carriers on carbon or graphite
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/90—Selection of catalytic material
- H01M4/92—Metals of platinum group
- H01M4/921—Alloys or mixtures with metallic elements
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/10—Fuel cells with solid electrolytes
- H01M8/1009—Fuel cells with solid electrolytes with one of the reactants being liquid, solid or liquid-charged
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/10—Fuel cells with solid electrolytes
- H01M8/1016—Fuel cells with solid electrolytes characterised by the electrolyte material
- H01M8/1018—Polymeric electrolyte materials
- H01M8/1039—Polymeric electrolyte materials halogenated, e.g. sulfonated polyvinylidene fluorides
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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Materials Engineering (AREA)
- Life Sciences & Earth Sciences (AREA)
- Manufacturing & Machinery (AREA)
- Sustainable Development (AREA)
- Sustainable Energy (AREA)
- Fuel Cell (AREA)
- Inert Electrodes (AREA)
Abstract
The application provides a direct organic liquid fuel cell based on a liquid hydrogen storage material, which belongs to the technical field of liquid hydrogen storage and liquid fuel cells, and uses an anode catalyst containing palladium element to catalyze hydrogen-rich organic liquid so that the hydrogen-rich organic liquid is oxidized to generate hydrogen protons and electrons for generating electricity, wherein the anode catalyst is in the form of PdXC, wherein X is one of Ru, pt and Ag, and the mass ratio of PdX to C is 0.25-1.5:1, the mass ratio of Pd to X is 0.25-4:1, the application can achieve higher power density.
Description
Technical Field
The application relates to the technical field of liquid hydrogen storage and liquid fuel cells, in particular to a direct organic liquid fuel cell based on a liquid hydrogen storage material.
Background
With the ever-decreasing reserves of fossil energy and the increasing carbon emissions, it is urgent to find alternatives to fossil energy. Hydrogen energy is one of the highest green energy sources of the call, and meets the opportunity of vigorous development. The method has very important practical significance in the current economic situation how to realize reasonable and efficient utilization of hydrogen energy. The amount of heat released during the combustion of hydrogen is much, and the amount of heat released is about 3 times that of the same-quality gasoline, 3.9 times that of alcohol and 4.5 times that of coke. And the product in the combustion process is water, so that zero emission of carbon dioxide can be realized, the problems of energy crisis and environmental pollution can be relieved, but hydrogen has certain dangers: easy leakage, inflammability, explosiveness, etc., and hamper the large-scale application of hydrogen.
The hydrogen storage technology for organic liquid is characterized in that alkene, alkyne, carbocycle aromatic hydrocarbon and heterocyclic compound with conjugated structure are subjected to reversible reaction with hydrogen under the action of a catalyst, on one hand, hydrogen-poor organic liquid can react with hydrogen to store hydrogen in the organic liquid, on the other hand, hydrogen-rich organic liquid can release hydrogen through chemical reaction, and the hydrogen-poor organic liquid is obtained for recycling. The organic liquid hydrogen storage technology is essentially used for transforming high-risk dangerous chemical hydrogen transportation into common chemical transportation, greatly increasing the safety in the hydrogen transportation process and being beneficial to popularization of large-scale use of hydrogen.
However, the conventional dehydrogenation reaction of the existing LOHC has the problems of low dehydrogenation speed, high reaction temperature, catalyst deactivation, side reaction and the like, and prevents the large-scale application of the organic liquid hydrogen storage technology. Conventional thermochemical dehydrogenation generally requires a significant heat input, for example, dehydrogenation temperatures typically up to about 270 ℃ to meet the reaction of the dehydrogenation catalyst. Therefore, a relatively large energy loss is caused, and the economy is poor. In addition, the hydrogen produced after thermochemical dehydrogenation is used as a hydrogen source by the steps of relaxation, drying and the like, which results in a complicated hydrogen utilization process and a rapid increase in the use cost.
There are researchers to put forward direct liquid organic hydrogen carrier fuel cells, DLFC for short, that is, the direct organic liquid fuel cells are prepared by utilizing the principle that a hydrogen-rich organic carrier is anodized, so as to reduce the temperature required by the hydrogen discharge reaction, and improve the overall energy utilization rate, for example, patent application of 2012, cheng Hansong and other inventors disclose related patents of DLFC, and two patent publications CN102800878B and CN102800877B are entitled to direct fuel cell energy storage and supply systems, wherein the organic liquid used by DLFC is mostly multi-element mixed unsaturated heterocyclic aromatic hydrocarbon, the components of the organic liquid are complex, and the organic liquid is generally required to enter the fuel cell device to work in a liquid form through a low-temperature co-fusion technology, and in the process, the problems of multiple side reactions such as electro-polymerization, poor electrochemical reaction kinetics, low power density and the like exist.
In a fuel cell with a single organic liquid function, such as that disclosed in patent CN111834640a with cyclohexane as fuel, the temperature reaches 80 ℃, with a ternary transition metal catalyst, the power density of the cell is only 5mW/cm 2 Its power is to be increased.
Disclosure of Invention
In view of this, the present application provides a direct organic liquid fuel cell based on a liquid hydrogen storage material capable of achieving higher power density.
In order to solve the technical problems, the application provides a direct organic liquid fuel cell based on a liquid hydrogen storage material, which uses an anode catalyst containing palladium element to catalyze hydrogen-rich organic liquid, so that the hydrogen-rich organic liquid is oxidized to generate hydrogen protons and electrons to generate electricity;
the anode catalyst is in the form of PdXC, wherein X is one of Ru, pt and Ag, and the mass ratio of PdX to C is 0.25-1.5:1, the mass ratio of Pd to X is 0.25-4:1.
further, the hydrogen-rich organic liquid is an azacyclic organic compound, the number of N atoms in the molecular formula of the azacyclic organic compound is 1-2, and the purity of the azacyclic organic compound is more than or equal to 99.5%.
The hydrogen-rich organic liquid is in a liquid state at normal temperature, namely 20 ℃.
The hydrogen-rich organic liquid provided by the application has high purity, few impurities and less possibility of side reaction to influence dehydrogenation efficiency and poisoning catalyst.
Further, the hydrogen-rich organic liquid is N-ethylindole, N-methylindole, pyrazine, 2, 3-dimethylpyrazine, 2, 5-dimethylpyrazine, 2-methylpyrazine, pyridazine or cyclopentapyrazine perhydrides or partial hydrides.
Further, the direct organic liquid fuel cell adopts a PEMFC structure, and the PEMFC structure comprises an anode plate, an anode gas diffusion layer, an anode catalyst layer, a proton exchange membrane, a cathode plate, a cathode gas diffusion layer and a cathode catalyst layer.
Further, an anode catalyst is coated on the anode catalyst layer.
Further, the anode catalyst is used in an amount of 0.1 to 5mg/cm on the anode catalyst layer 2 。
Further, a cathode catalyst is coated in the cathode catalyst layer, and the cathode catalyst exists in the form of PtC, wherein the mass ratio of Pt to C is 0.25-1.5:1.
Further, the cathode catalyst is used in an amount of 0.05-2mg/cm on the cathode catalyst layer 2 。
Furthermore, the proton exchange membrane adopts a perfluorosulfonic acid proton exchange membrane.
Further, the thickness of the proton exchange membrane is 100-190 mu m.
The beneficial effects of the application are as follows:
the application is characterized in that the anode catalyst containing palladium element is used for catalyzing the hydrogen-rich organic liquid, the anode catalyst containing palladium element has low cost and better poisoning resistance, so that the dehydrogenation performance of the anode catalyst is better than that of the Pt-based catalyst in the background art, and the battery has higher power density aiming at the proton separation and higher carbon monoxide tolerance in the hydrogen-rich organic liquid.
By combining the anode catalyst and the hydrogen-rich organic liquid for power generation, taking N-ethylindole as an example, 8H-N-ethylindole is dehydrogenated under the catalysis of PdX/C to generate N-ethylindole and H + And electrons（e - ）；H + Through the proton exchange membrane to the cathode, and through the external circuit to the cathode, the electrons react with oxygen to produce water under the catalysis of Pt/C.
The hydrogen-rich organic liquid used in the application is an organic liquid which cannot be catalyzed by a Pt-based anode catalyst in the prior art, is a substance which can be catalyzed and generated only by the anode catalyst containing palladium element, has high dehydrogenation efficiency, has no pretreatment in a hydrogen utilization process compared with the traditional thermochemical process, has high economic value, and the dehydrogenation products of the hydrogen-rich organic liquid can be recycled, and is environment-friendly and pollution-free.
Drawings
FIG. 1 is a schematic diagram of a complete power generation and power utilization architecture of the present application;
fig. 2 is a schematic view of a first structure of the PEMFC device of the present application;
fig. 3 is a schematic view showing a second structure of the PEMFC device of the present application.
Reference numerals:
1. a hydrogen-rich organic liquid storage tank; 2. a hydrogen-depleted organic liquid storage tank; 3. a PEMFC device; 4. a thermal control module; 5. an air pump; 6. a feed pump; 7. an anode plate; 8. an anode gas diffusion layer; 9. an anode catalyst layer; 10. a proton exchange membrane; 11. a cathode plate; 12. a cathode gas diffusion layer; 13. a cathode catalyst.
Detailed Description
In order to make the objects, technical solutions and advantages of the embodiments of the present application more clear, the technical solutions of the embodiments of the present application will be clearly and completely described below with reference to fig. 1 to 3 of the embodiments of the present application. It will be apparent that the described embodiments are some, but not all, embodiments of the application. All other embodiments, which are obtained by a person skilled in the art based on the described embodiments of the application, fall within the scope of protection of the application.
The following describes the use of the direct organic liquid fuel cell and the liquid hydrogen storage material according to the embodiments of the present application.
The hydrogen storage material is an organic liquid capable of storing hydrogen through reversible reaction in a conjugated structure, hydrogen protons are removed by using the organic liquid under the catalysis of an anode catalyst, oxygen is taken as a cathode to be reduced into oxygen anions, then the hydrogen protons react with the oxygen anions, and electrons form a loop through an external circuit to generate electric energy, namely the use mode of the direct organic liquid fuel cell and the liquid hydrogen storage material thereof in the following embodiment.
In this document PdXC means three elements, pd is palladium element, X means upper expression shorthand of Ru, pt and Ag, i.e., X may be any one of Ru, pt and Ag, ru is ruthenium element, pt is platinum element, ag is silver element, and C means carbon element; ptC means two elements, pt is platinum element, and C means carbon element; PEMFCs refer to proton exchange membrane fuel cells.
As shown in fig. 1, the complete power generation and electric energy utilization structure of the present application is composed of a PEMFC device 3, a hydrogen-rich organic liquid storage tank 1, a feed pump 6, a hydrogen-poor organic liquid storage tank 2, an air pump 5, and a thermal control module 4.
In fig. 1, the solid line is a material flow line, and the dotted line is a current line.
Wherein the hydrogen-rich organic liquid as a key point of the present application is stored inside the hydrogen-rich organic liquid storage tank 1 and enters the PEMFC device 3 through the feed pump 6 to react, while the anode catalyst containing palladium element of the present application is located inside the PEMFC device 3, as shown in fig. 2 and 3, the PEMFC device 3 itself comprises an anode plate 7, an anode gas diffusion layer 8, an anode catalyst layer 9, a proton exchange membrane 10, a cathode plate 11, a cathode gas diffusion layer 12, and a cathode catalyst layer 13, and the anode catalyst is coated on the anode catalyst layer 9.
Anode: the hydrogen-rich organic liquid is incompletely oxidatively dehydrogenated to generate aromatic ring molecules and protons.
And (3) cathode: oxygen is reduced to produce oxyanions, and hydrogen protons react with the oxyanions to produce water.
In this case, the hydrogen-rich organic liquid is subjected to the action of the anode catalyst to remove hydrogen protons; the cathode oxygen is reduced to generate oxygen anions, hydrogen protons and oxygen ions react, and electrons form a loop through an external circuit to generate electric energy, so that the purpose of directly and conveniently using the hydrogen-rich organic liquid is achieved.
The anode catalyst exists in a form of PdX/C, wherein the X element is one of Ru, pt and Ag, and the mass ratio of PdX to C is 0.25-1.5:1, the mass ratio of Pd to X is 0.25-4:1, the power density of the single cell can be greatly improved under the proportion, and the optimal power density can be achieved under the condition of limited catalyst.
The cathode catalyst is present in the form of PtC, wherein the mass ratio of Pt to C is 0.25-1.5:1, and the amount of the cathode catalyst used on the cathode catalyst layer 13 is 0.05-2mg/cm 2 The corresponding protons released by the anode are matched to release cathode oxygen ions, so that stable current is formed.
The proton exchange membrane 10 adopts the perfluorosulfonic acid proton exchange membrane 10, the thickness of the proton exchange membrane 10 is 100-190 mu m, and the damage of the hydrogen-rich organic liquid to the proton exchange membrane 10 can be prevented under the thickness, and the durability of the PEMFC device 3 can be improved, so that the catalysis of the anode catalyst containing palladium element to the hydrogen-rich organic liquid is facilitated, and the higher power density is ensured.
As shown in fig. 3, the organic liquid which is dehydrogenated once and flows out of the PEMFC device contains organic liquid which is partially and incompletely dehydrogenated, the organic liquid which is incompletely dehydrogenated and flows out of the anode can be pumped into the anode of the PEMFC device again through a pipeline, and the hydrogen in the hydrogen-rich organic liquid can be ensured to be completely used after a plurality of times.
The method for testing the power density of the single cell is as follows:
the electronic load is enabled to work in a constant current mode by using a fuel cell test platform software control system, load current is continuously changed to measure output voltage values of single cells under different current densities, then an I-V curve of the single cells can be obtained through data processing and plotting, in the experimental process, the cells are heated by a temperature control system, hydrogen-rich organic liquid is heated by an oven, and the I-V curve test is carried out when the hydrogen-rich organic liquid is heated to a set value. Setting the fuel flow to be 2mL/min, the oxygen flow to be 0.6mL/min, setting the current initial value to be 0A, setting the current final value to be based on the output voltage value to be 0.1V, stabilizing each group of load current for about 3min corresponding to the test time under the current load for 10s, and taking one group of data every 2 s. According to the characteristics of the polarization curve, the current density is selected as gradient change, the load current value is sequentially increased until the voltage of the single cell is reduced to about 0.1V, an I-V curve is obtained by arrangement, and the output power of the cell is increased under different temperature conditions of the catalyst; after the experiment is completed, the test platform is closed, the hydrogen-rich organic liquid in the pipeline is discharged, nitrogen is introduced into the cathode of the single cell for purging, and the nitrogen is closed after the cell is cooled to room temperature.
Example 1
The anode catalyst used in this example was PdRu/C, wherein the mass ratio of PdRu to C was 1.2:1, and the mass ratio of pd to Ru was 0.4:0.8, the dosage is 1.2mg/cm 2 The method comprises the steps of carrying out a first treatment on the surface of the The hydrogen-rich organic liquid used in combination with the anode catalyst is perhydrogenated pyridazine with purity of more than 99.5%.
The PEMFC device 3 shown in figure 2 is adopted for assembly, the anode plate 7 and the cathode plate 11 are made of metallic titanium, the anode gas diffusion layer 8 is made of carbon paper, the cathode gas diffusion layer 12 is made of carbon paper with a microporous layer, wherein the proton exchange membrane 10 is made of perfluorosulfonic acid proton exchange membrane 10, the thickness of the perfluorosulfonic acid proton exchange membrane 10 is 100 mu m, ptC is used at the corresponding cathode, the mass ratio of Pt to C is 0.3:1, and the use amount is 2mg/cm 2 。
After the setting is finished, the test is carried out, the working temperature is controlled to be 100 ℃, and the power density of the single cell is measured to be 55 mW/cm 2 。
Example two
The present embodiment differs from the first embodiment in that Pd in the anode catalyst is changed: ru: c, and converting the hydrogen-rich organic liquid into perhydrogenated 2-methyl pyrazine.
The specific changes are as follows:
the anode catalyst used in this example was PdRu/C, wherein PdRu: the mass ratio of C is 1.5:1, and the mass ratio of Pd to Ru is 0.6:0.9, the dosage is 5mg/cm 2 The method comprises the steps of carrying out a first treatment on the surface of the The hydrogen-rich organic liquid used in combination with the anode catalyst has high purity99.5% of 2-methylpyrazine.
The PEMFC device 3 shown in figure 2 is adopted for assembly, the anode plate 7 and the cathode plate 11 are made of metallic titanium, the anode gas diffusion layer 8 is made of carbon paper, the cathode gas diffusion layer 12 is made of carbon paper with a microporous layer, wherein the proton exchange membrane 10 is made of perfluorosulfonic acid proton exchange membrane 10, the thickness of the perfluorosulfonic acid proton exchange membrane 10 is 183 mu m, ptC is used at the corresponding cathode, the mass ratio of Pt to C is 0.5:1, and the use amount is 2mg/cm 2 。
After the setting is finished, the test is carried out, the working temperature is controlled to be 100 ℃, and the power density of the single cell is measured to be 85 mW/cm 2 。
Example III
The present embodiment differs from the first embodiment in that Pd in the anode catalyst is changed: ru: c, and converting the hydrogen-rich organic liquid into perhydrogenated N-methylindole.
The specific changes are as follows:
the anode catalyst used in this example was PdRu/C, wherein PdRu: the mass ratio of C is 0.8:1, and the mass ratio of Pd to Ru is 0.6:0.2, the dosage is 4mg/cm 2 The method comprises the steps of carrying out a first treatment on the surface of the The hydrogen-rich organic liquid used in combination with the anode catalyst is perhydrogenated N-methylindole with purity of more than 99.5 percent.
The PEMFC device 3 shown in figure 2 is adopted for assembly, the anode plate 7 and the cathode plate 11 are made of metallic titanium, the anode gas diffusion layer 8 is made of carbon paper, the cathode gas diffusion layer 12 is made of carbon paper with a microporous layer, wherein the proton exchange membrane 10 is made of perfluorosulfonic acid proton exchange membrane 10, the thickness of the perfluorosulfonic acid proton exchange membrane 10 is 50 mu m, ptC is used at the corresponding cathode, the mass ratio of Pt to C is 0.5:1, and the use amount is 2mg/cm 2 。
After the setting is finished, the test is carried out, the working temperature is controlled to be 100 ℃, and the power density of the single cell is measured to be 90 mW/cm 2 。
Example IV
The present embodiment differs from the first embodiment in that Pd in the anode catalyst is changed: ru: c, and converting the hydrogen-rich organic liquid to the use of partially hydrogenated N-methylindole.
The specific changes are as follows:
the anode catalyst used in this example was PdRu/C, wherein PdRu: the mass ratio of C is 1.5:1, and the mass ratio of Pd to Ru is 0.6:0.9, the dosage is 5mg/cm 2 The method comprises the steps of carrying out a first treatment on the surface of the The hydrogen-rich organic liquid used in combination with the anode catalyst is partially hydrogenated N-methylindole with a purity of more than 99.5%, i.e. 4-hydrogenated N-methylindole.
The PEMFC device 3 shown in figure 2 is adopted for assembly, the anode plate 7 and the cathode plate 11 are made of metallic titanium, the anode gas diffusion layer 8 is made of carbon paper, the cathode gas diffusion layer 12 is made of carbon paper with a microporous layer, wherein the proton exchange membrane 10 is made of perfluorosulfonic acid proton exchange membrane 10, the thickness of the perfluorosulfonic acid proton exchange membrane 10 is 137 mu m, ptC is used at the corresponding cathode, the mass ratio of Pt to C is 0.5:1, and the use amount is 2mg/cm 2 。
After the setting is finished, the test is carried out, the working temperature is controlled to be 100 ℃, and the power density of the single cell is measured to be 78 mW/cm 2 。
Example five
The present embodiment differs from the first embodiment in that the X element in the anode catalyst is changed, and Pd is used: pt: c, and converting the hydrogen-rich organic liquid to the use of perhydrogenated N-ethylindole.
The specific changes are as follows:
the anode catalyst used in this example was PdPt/C, where PdPt: the mass ratio of C is 1.2:1, and the mass ratio of Pd to Pt is 1:2, the usage amount is 5mg/cm 2 The method comprises the steps of carrying out a first treatment on the surface of the The hydrogen-rich organic liquid used in combination with the anode catalyst is N-ethylindole with purity of more than 99.5 percent.
The PEMFC device 3 shown in figure 2 is adopted for assembly, the anode plate 7 and the cathode plate 11 are made of metallic titanium, the anode gas diffusion layer 8 is made of carbon paper, the cathode gas diffusion layer 12 is made of carbon paper with a microporous layer, wherein the proton exchange membrane 10 is made of perfluorosulfonic acid proton exchange membrane 10, the thickness of the perfluorosulfonic acid proton exchange membrane 10 is 100 mu m, ptC is used at the corresponding cathode, and the mass ratio of Pt to C is 0.5:1, so thatThe dosage is 2mg/cm 2 。
After the setting is finished, the test is carried out, the working temperature is controlled to be 100 ℃, and the power density of the single cell is measured to be 65 mW/cm 2 。
Example six
The present embodiment is different from embodiment five in that Pd in the anode catalyst is changed: pt: c, and converting the hydrogen-rich organic liquid into perhydro pyrazine.
The specific changes are as follows:
the anode catalyst used in this example was PdPt/C, where PdPt: the mass ratio of C is 1.5:1, and the mass ratio of Pd to Pt is 2:1.5, the dosage is 3mg/cm 2 The method comprises the steps of carrying out a first treatment on the surface of the The hydrogen-rich organic liquid used in combination with the anode catalyst is pyrazine with a purity of more than 99.5%.
The PEMFC device 3 shown in figure 2 is adopted for assembly, the anode plate 7 and the cathode plate 11 are made of metallic titanium, the anode gas diffusion layer 8 is made of carbon paper, the cathode gas diffusion layer 12 is made of carbon paper with a microporous layer, wherein the proton exchange membrane 10 is made of perfluorosulfonic acid proton exchange membrane 10, the thickness of the perfluorosulfonic acid proton exchange membrane 10 is 100 mu m, ptC is used at the corresponding cathode, the mass ratio of Pt to C is 0.5:1, and the use amount is 2mg/cm 2 。
After the setting is finished, the test is carried out, the working temperature is controlled to be 100 ℃, and the power density of the single cell is measured to be 82 mW/cm 2 。
Example seven
The present embodiment differs from the first embodiment in that the X element in the anode catalyst is changed, and Pd is used: ag: c, and converting the hydrogen-rich organic liquid into perhydrogenated 2, 3-dimethyl pyrazine.
The specific changes are as follows:
the anode catalyst used in this example was PdAG/C, where PdAG: the mass ratio of C is 1.5:1, and the mass ratio of Pd to Ag is 0.6:0.9, the dosage is 5mg/cm 2 The method comprises the steps of carrying out a first treatment on the surface of the The hydrogen-rich organic liquid used in combination with the anode catalyst is 2, 3-dimethyl pyrazine with purity of more than 99.5 percent.
With the PEMFC device 3 as shown in fig. 2The anode plate 7 and the cathode plate 11 are assembled by adopting metallic titanium as a substrate material, the anode gas diffusion layer 8 adopts carbon paper, the cathode gas diffusion layer 12 adopts carbon paper with a microporous layer, wherein the proton exchange membrane 10 adopts a perfluorosulfonic acid proton exchange membrane 10, the thickness of the perfluorosulfonic acid proton exchange membrane 10 is 100 mu m, ptC is adopted at the corresponding cathode, the mass ratio of Pt to C is 0.5:1, and the use amount is 2mg/cm 2 。
After the setting is finished, the test is carried out, the working temperature is controlled to be 100 ℃, and the power density of the single cell is measured to be 77 mW/cm 2 。
Example eight
The present embodiment differs from embodiment seven in that Pd in the anode catalyst is changed: ag: c, and converting the hydrogen-rich organic liquid to use perhydrogenated cyclopentapyrazine.
The specific changes are as follows:
the anode catalyst used in this example was PdRu/C, where PdAg: the mass ratio of C is 1.5:1, and the mass ratio of Pd to Ag is 1.5:2, the usage amount is 4mg/cm 2 The method comprises the steps of carrying out a first treatment on the surface of the The hydrogen-rich organic liquid used in combination with the anode catalyst is cyclopentapyrazine with a purity of greater than 99.5%.
The PEMFC device 3 shown in figure 2 is adopted for assembly, the anode plate 7 and the cathode plate 11 are made of metallic titanium, the anode gas diffusion layer 8 is made of carbon paper, the cathode gas diffusion layer 12 is made of carbon paper with a microporous layer, wherein the proton exchange membrane 10 is made of perfluorosulfonic acid proton exchange membrane 10, the thickness of the perfluorosulfonic acid proton exchange membrane 10 is 100 mu m, ptC is used at the corresponding cathode, the mass ratio of Pt to C is 0.5:1, and the use amount is 2mg/cm 2 。
After the setting is finished, the test is carried out, the working temperature is controlled to be 100 ℃, and the power density of the single cell is measured to be 63 mW/cm 2 。
Comparative example one
This comparative example differs from example one in that catalytic power generation was performed using an anode catalyst without palladium element.
The specific changes are as follows:
anodes used in this comparative exampleThe catalyst is Pt/C, wherein the mass ratio of Pt to C is 0.8:1, and the using amount is 4mg/cm 2 The method comprises the steps of carrying out a first treatment on the surface of the The hydrogen-rich organic liquid used in combination with the anode catalyst is perhydrogenated pyridazine with purity of more than 99.5%.
The PEMFC device 3 shown in figure 2 is adopted for assembly, the anode plate 7 and the cathode plate 11 are made of metallic titanium, the anode gas diffusion layer 8 is made of carbon paper, the cathode gas diffusion layer 12 is made of carbon paper with a microporous layer, wherein the proton exchange membrane 10 is made of perfluorosulfonic acid proton exchange membrane 10, the thickness of the perfluorosulfonic acid proton exchange membrane 10 is 100 mu m, ptC is used at the corresponding cathode, the mass ratio of Pt to C is 0.3:1, and the use amount is 2mg/cm 2 。
After the setting is finished, the test is carried out, the working temperature is controlled to be 100 ℃, and the power density of the single cell is measured to be 13 mW/cm 2 。
Comparative example two
This comparative example differs from example one in that a different hydrogen-rich organic liquid was used for catalytic power generation.
The specific changes are as follows:
the anode catalyst used in this comparative example was PdRu/C, where the mass ratio of PdRu to C was 1.2:1, and the mass ratio of pd to Ru was 0.4:0.8, the dosage is 1.2mg/cm 2 The method comprises the steps of carrying out a first treatment on the surface of the The hydrogen-rich organic liquid used in combination with the anode catalyst is a mixture of carbazole: N-methyl carbazole: N-ethyl carbazole: quinoline=4:3:5:1.
The PEMFC device 3 shown in figure 2 is adopted for assembly, the anode plate 7 and the cathode plate 11 are made of metallic titanium, the anode gas diffusion layer 8 is made of carbon paper, the cathode gas diffusion layer 12 is made of carbon paper with a microporous layer, wherein the proton exchange membrane 10 is made of perfluorosulfonic acid proton exchange membrane 10, the thickness of the perfluorosulfonic acid proton exchange membrane 10 is 100 mu m, ptC is used at the corresponding cathode, the mass ratio of Pt to C is 0.3:1, and the use amount is 2mg/cm 2 。
After the setting is finished, the test is carried out, the working temperature is controlled to be 100 ℃, and the power density of the single cell is measured to be 26 mW/cm 2 。
Comparative example three
The present comparative example differs from the first example in that the proton exchange membrane 10 was thinned to a thickness of 50 μm.
The specific changes are as follows:
the anode catalyst used in this comparative example was PdRu/C, where the mass ratio of PdRu to C was 1.2:1, and the mass ratio of pd to Ru was 0.4:0.8, the dosage is 1.2mg/cm 2 The method comprises the steps of carrying out a first treatment on the surface of the The hydrogen-rich organic liquid used in combination with the anode catalyst is perhydrogenated pyridazine with purity of more than 99.5%.
The PEMFC device 3 shown in figure 2 is adopted for assembly, the anode plate 7 and the cathode plate 11 are made of metallic titanium, the anode gas diffusion layer 8 is made of carbon paper, the cathode gas diffusion layer 12 is made of carbon paper with a microporous layer, wherein the proton exchange membrane 10 is made of perfluorosulfonic acid proton exchange membrane 10, the thickness of the perfluorosulfonic acid proton exchange membrane 10 is 50 mu m, ptC is used at the corresponding cathode, the mass ratio of Pt to C is 0.3:1, and the use amount is 2mg/cm 2 。
After the setting is finished, testing is carried out, the working temperature is controlled to be 100 ℃, and the condition of liquid leakage occurs after the operation for 3 hours, and the power density of the single cell is measured to be 25mW/cm 2 。
Comparative example four
The difference between the comparative example and the comparative example I is that the X element in the anode catalyst is eliminated, and Pd element and C element are directly matched for use, and the specific changes are as follows:
the anode catalyst used in this comparative example was Pd/C in a mass ratio of Pd to C of 1.2:1 in an amount of 1.2mg/cm 2 The method comprises the steps of carrying out a first treatment on the surface of the The hydrogen-rich organic liquid used in combination with the anode catalyst is perhydrogenated pyridazine with purity of more than 99.5%.
The PEMFC device 3 shown in figure 2 is adopted for assembly, the anode plate 7 and the cathode plate 11 are made of metallic titanium, the anode gas diffusion layer 8 is made of carbon paper, the cathode gas diffusion layer 12 is made of carbon paper with a microporous layer, wherein the proton exchange membrane 10 is made of perfluorosulfonic acid proton exchange membrane 10, the thickness of the perfluorosulfonic acid proton exchange membrane 10 is 100 mu m, ptC is used at the corresponding cathode, the mass ratio of Pt to C is 0.3:1, and the use amount is 2mg/cm 2 。
After the setting is finished, testing is carried out, the working temperature is controlled to be 100 ℃, and the condition of liquid leakage occurs after the operation for 3 hours, and the power density of the single cell is measured to be 33mW/cm 2 。
The following data table was made according to the above examples and the changes and data of the comparative examples:
according to the embodiment to the eighth embodiment, it can be seen that in the application, after the anode catalyst containing palladium element is adopted, the corresponding hydrogen-rich organic liquid is matched for generating electricity, and the power density of the finally obtained single cell is greatly improved, and the better generating effect is achieved by matching with other corresponding devices.
It can be seen from examples one and comparative example one that the absence of palladium has a great influence on the catalysis of the hydrogen-rich organic liquid of the present application, directly resulting in a decrease in the power density of the unit cell.
It can be seen from examples one and two that the anode catalyst of the present application does not achieve a better cell power density for hydrogen-rich organic liquids containing various complex contents, only the hydrogen-rich organic liquid of the present application can have a higher power density.
According to the first embodiment and the third embodiment, it can be seen that the thickness of the proton exchange membrane can ensure the normal operation of the single cell, and the too thin proton exchange membrane cannot support the long-time operation of the cell.
Experiments on the fourth comparative example show that the application can promote the catalysis of palladium element by compounding some X elements, and the catalysis effect of palladium element on hydrogen-rich organic liquid is improved.
While the foregoing is directed to the preferred embodiments of the present application, it will be appreciated by those skilled in the art that various modifications and adaptations can be made without departing from the principles of the present application, and such modifications and adaptations are intended to be comprehended within the scope of the present application.
Claims (10)
1. A direct organic liquid fuel cell based on a liquid hydrogen storage material is characterized in that an anode catalyst containing palladium element is used for catalyzing hydrogen-rich organic liquid, so that the hydrogen-rich organic liquid is oxidized to generate hydrogen protons and electrons to generate electricity;
the anode catalyst is in the form of PdXC, wherein X is one of Ru, pt and Ag, and the mass ratio of PdX to C is 0.25-1.5:1, the mass ratio of Pd to X is 0.25-4:1.
2. the direct organic liquid fuel cell based on a liquid hydrogen storage material according to claim 1, wherein the hydrogen-rich organic liquid is an azacyclic organic compound having a number of N atoms of 1 to 2 in the molecular formula, and the azacyclic organic compound has a purity of 99.5% or more.
3. The direct organic liquid fuel cell based on a liquid hydrogen storage material according to claim 2, wherein the hydrogen rich organic liquid is a perhydride or a partial hydride of N-ethylindole, N-methylindole, pyrazine, 2, 3-dimethylpyrazine, 2, 5-dimethylpyrazine, 2-methylpyrazine, pyridazine or cyclopentapyrazine.
4. The direct organic liquid fuel cell based on a liquid hydrogen storage material according to claim 1, wherein the direct organic liquid fuel cell adopts a PEMFC structure including an anode plate (7), an anode gas diffusion layer (8), an anode catalyst layer (9), a proton exchange membrane (10), a cathode plate (11), a cathode gas diffusion layer (12), and a cathode catalyst layer (13).
5. The direct organic liquid fuel cell based on a liquid hydrogen storage material according to claim 4, wherein the anode catalyst is coated on the anode catalyst layer (9).
6. The liquid-based storage of claim 5A direct organic liquid fuel cell of hydrogen material, characterized in that the anode catalyst is used in an amount of 0.1-5mg/cm on the anode catalyst layer (9) 2 。
7. The direct organic liquid fuel cell based on liquid hydrogen storage material according to claim 4, wherein the cathode catalyst layer (13) is internally coated with a cathode catalyst, which is present in the form of PtC, wherein the mass ratio of Pt to C is in the range of 0.25-1.5:1.
8. The direct organic liquid fuel cell based on a liquid hydrogen storage material according to claim 7, wherein the amount of the cathode catalyst used on the cathode catalyst layer (13) is 0.05-2mg/cm 2 。
9. The direct organic liquid fuel cell based on a liquid hydrogen storage material according to claim 4, wherein the proton exchange membrane (10) is a perfluorosulfonic acid proton exchange membrane (10).
10. Direct organic liquid fuel cell based on liquid hydrogen storage material according to claim 9, characterized in that the proton exchange membrane (10) has a thickness of 100-190 μm.
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