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High-temperature-resistant composite proton exchange membrane and preparation method thereof

A proton exchange membrane and composite technology, which can be used in the manufacture of final products, sustainable manufacturing/processing, fuel cells, etc., can solve the problems of limiting proton conductivity, reducing membrane toughness, and detrimental to the comprehensive performance of high temperature proton exchange membranes. Wide applicability, improved mechanical strength, and easy mass production

Inactive Publication Date: 2019-07-02
DALIAN INST OF CHEM PHYSICS CHINESE ACAD OF SCI
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

Traditional small-molecule cross-linking agents have a significant effect in improving the tensile strength, but reduce the toughness of the membrane, which limits the phosphoric acid doping content and proton conductivity of the phosphoric acid-doped polybenzimidazole membrane, which is not conducive to high-temperature proton exchange membranes. Overall Performance Improvement

Method used

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  • High-temperature-resistant composite proton exchange membrane and preparation method thereof
  • High-temperature-resistant composite proton exchange membrane and preparation method thereof
  • High-temperature-resistant composite proton exchange membrane and preparation method thereof

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0039] Blend 0.06mol 3,4-dimethylphenyl-p-benzoquinone, 0.06mol 4,4-dihydroxydiphenyl sulfone, 0.12mol 4,4'-difluorobenzophenone and 0.15mol potassium carbonate in Under a nitrogen atmosphere, use 100ml sulfolane as a solvent and 30ml toluene as a water-carrying agent, heat up to 140°C with water for 3 hours, then distill off the toluene, and then heat up to 180°C for 4 hours. After the reaction, the mixed solution was poured into deionized water to obtain a white strip polymer. Break the strip polymer into a powder with a tissue grinder, boil and wash it with acetone several times to remove the solvent, and wash it repeatedly with distilled water to remove the salt, and then put it in an oven for 24 hours at 60°C to obtain a pure white powder. The solid, that is, side-chain dimethylphenyl type polyarylether (dmPA, the structure of which is shown below), was 46.3 g, and the yield was 94%.

[0040]

[0041] Weigh 8.20g of DMPA obtained above, 4.45g (0.025mol) of N-bromosucc...

Embodiment 2

[0045] Use the same method as in Example 1 to prepare dmPA to synthesize side chain p-methylphenyl type polyarylether (mPA, its structure is as follows), except that 0.06mol p-methylphenyl-p-benzoquinone is used to replace 0.06mol 3,4 -Dimethylphenyl-p-benzoquinone, the yield of mPA obtained is 44.5 g, the yield is 92%.

[0046]

[0047] The same method as in Example 1 to prepare BrdmPA is used to prepare side chain-containing benzyl bromide p-methylphenyl type polyarylether—BrmPA, the difference is that 8.06g mPA is used to replace 8.20g dmPA, and the resulting BrmPA output is 8.50g, with an average per The mole benzyl position contains 0.92 mole bromine.

[0048] The method for preparing BrdmPA-c-PBI in Example 1 is used to prepare the side chain-containing benzyl bromide p-methylphenyl type polyarylether and polybenzimidazole composite cross-linked membrane (BrmPA-c-PBI), the difference is that BrmPA replaces BrdmPA.

[0049] Adopt the method for preparing PA / BrdmPA-c-PB...

Embodiment 3

[0051] Weigh 30g of mPBI solution (10wt% solid content), pour the solution onto a glass plate, cast it on a glass plate and dry it thoroughly in an oven at 80°C, continue heating at 150°C for 5h, and finally remove it from the glass plate to obtain a PBI film.

[0052] Take a 4*4cm PBI membrane and soak it in 85wt% phosphoric acid solution, soak it at 80°C for 24 hours, remove excess phosphoric acid on the surface with filter paper, and obtain a phosphoric acid doped membrane using polybenzimidazole (PA / PBI). The phosphoric acid doping level was 12.0.

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Abstract

A high-temperature-resistant composite proton exchange membrane is formed by compositing polybenzimidazole and an aromatic polymer with benzyl halide in side chains to form a composite cross-linking membrane and impregnating the composite cross-linking membrane in phosphoric acid. The mass fraction of the heterocyclic aromatic polymer containing benzyl halide in the composite cross-linking membrane is 0.01-99.99wt%. The mass fraction of the phosphoric acid doped in the composite proton exchange membrane is 1-99%. Compared with the existing phosphoric acid doped high-temperature proton exchangemembrane, the high-temperature-resistant composite proton exchange membrane of the invention has the advantages as follows: the glass transition temperature of the aromatic polymer with benzyl halidein side chains is high, which ensures the stability of the composite proton exchange membrane at high temperature; and each molecular chain contains multiple benzyl bromide groups and forms a covalent bond with multiple polybenzimidazole molecular chains, which improves the dimensional stability of the composite membrane; the composite proton exchange membrane has a high phosphoric acid doping level and good mechanical performance, and is a high-temperature proton exchange membrane with excellent comprehensive performance; and the preparation method is simple, and the composite proton exchange membrane has wide applications and is convenient for large-scale production.

Description

technical field [0001] The invention relates to a high-temperature fuel cell composite proton exchange membrane and a preparation method thereof, in particular to a method for preparing a high-temperature proton exchange membrane by using a polymer as a crosslinking agent to modify polybenzimidazole. Background technique [0002] A fuel cell is an electrochemical conversion device that converts chemical energy into electrical energy, and is one of the most competitive power generation technologies in the 21st century. Among many fuel cell systems, high-temperature proton exchange membrane fuel cells (PEMFCs) have become a hotspot in the research and development of fuel cells in the world because of their (1) strong CO resistance capability and (2) simple system. [0003] Due to its high glass transition temperature, polybenzimidazole is relatively mature in the field of high-temperature proton exchange membrane fuel cells. The conductivity of the phosphoric acid-doped polyb...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): H01M8/1044H01M8/1072
CPCH01M8/1044H01M8/1072Y02E60/50Y02P70/50
Inventor 王素力马文佳孙公权
Owner DALIAN INST OF CHEM PHYSICS CHINESE ACAD OF SCI
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