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A main chain type sulfonated polyquinoxaline prepared by post-sulfonation method and its proton exchange membrane

A technology of sulfonated polyquinoxaline and main chain type, applied in the field of proton exchange membrane

Active Publication Date: 2020-10-30
BEIJING INSTITUTE OF TECHNOLOGYGY
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

However, most of them fail to meet the high proton conductivity at high operating temperature, strong hydrolytic stability and long-lasting stability required by high-performance proton exchange membranes [Asano N, Aoki M, Suzuki S, Miyatake K, Uchida H, Watanabe M. J Am Chem Soc 2006; 128:1762–9]

Method used

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  • A main chain type sulfonated polyquinoxaline prepared by post-sulfonation method and its proton exchange membrane
  • A main chain type sulfonated polyquinoxaline prepared by post-sulfonation method and its proton exchange membrane
  • A main chain type sulfonated polyquinoxaline prepared by post-sulfonation method and its proton exchange membrane

Examples

Experimental program
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Effect test

Embodiment 1

[0034] In this embodiment, the tetraamine (1) skeleton is used as an example to synthesize sulfonated polyquinoxaline from the monomer (4) of the polyquinoxaline structural unit (a) before sulfonation, and the structure is as follows:

[0035]

[0036] The specific preparation method is:

[0037] (1) Polymerization

[0038] Weigh 1.2052g of 4,4'-bis(4-(2-(4-phenyl)acyl)phenoxy)biphenyl and 0.4285g of 3,3',4,4'-tetraaminobiphenyl respectively, and mix Then pour it into a flask, add m-cresol to dissolve, react at room temperature for about 24 hours under a nitrogen atmosphere, pour the solution into ethanol to precipitate the polymer, wash repeatedly until it is clean, filter, collect the solid, and dry it in vacuum to obtain polymer fibers.

[0039] (2) Sulfonation

[0040] Pour the polymer fibers into a flask, add fuming sulfuric acid at a ratio of 10-15wt% solid content, react under a nitrogen atmosphere, pour the liquid into water, the sulfonated product is precipitated...

Embodiment 2

[0044] In this embodiment, the monomer (4) of the polyquinoxaline structural unit (a) and the monomer (3) of the structural unit (b) before sulfonation are used as raw materials to synthesize sulfonated polyquinoxaline with the tetraamine (1) skeleton Taking morphine as an example, the structure is as follows (wherein x:y=3:1):

[0045]

[0046] The specific preparation method is:

[0047] (1) Polymerization

[0048] Weigh 0.9039g of 4,4'-bis(4-(2-(4-phenyl)acyl)phenoxy)biphenyl, 4,4'-bis(2-(4-phenyl)acyl) Diphenyl ether 0.2172g and 3,3',4,4'-tetraaminobiphenyl 0.4285g, add m-cresol to dissolve, react at room temperature under nitrogen atmosphere for about 24h, after the reaction, pour the solution into ethanol to make the polymer The precipitates are washed repeatedly until they are clean, filtered, and dried to obtain polymer fibers.

[0049] (2) Sulfonation

[0050] React the obtained polymer with concentrated sulfuric acid, pour the solution into water after the react...

Embodiment 3

[0054] In this embodiment, the tetraamine (3) skeleton is used as the raw material to synthesize the sulfonated polyquinoxaline monomer (1) of the structural unit (a) and the monomer (1) of the structural unit (b) before sulfonation. Taking quinoxaline as an example, the structure is as follows (wherein x:y=3:1):

[0055]

[0056] The specific preparation method is:

[0057] (1) Polymerization

[0058] Weigh 0.7898g of 1,4-bis(4-(2-(4-phenyl)acyl)phenoxy)benzene, 0.2092g of biphenylil and 3,3',4,4'-tetraaminobis 0.4605g of phenylene ether was dissolved by adding m-cresol, and reacted at room temperature under nitrogen atmosphere for about 24 hours. After the reaction, the solution was poured into ethanol to precipitate the polymer, washed repeatedly until it was cleaned, filtered, and dried to obtain polymer fibers.

[0059] (2) Sulfonation

[0060] Pour the polymer fibers into a flask, add fuming sulfuric acid at a ratio of 10-15wt% solid content, react under a nitrogen...

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Abstract

The invention discloses a preparation method of a main chain type sulfonated polyquinoxaline and a proton exchange membrane, and belongs to the field of proton exchange membranes. The preparation method is invented to solve the problem that when an aromatic sulfonated polymer is taken as a proton exchange membrane, the requirements of high proton conductivity and high chemical stability at a highoperating temperature are impossible to satisfy. According to the preparation method, the main chain type sulfonated polyquinoxaline is prepared through copolymerizing of a di-acyl monomer, a non-sulfonated di-acyl monomer, and different tetramine monomers according to different molar ratios, and mild post-sulfonation method is adopted to obtain the main chain type sulfonated polyquinoxaline whichis clear in sulfonation positions, predictable in ion exchange capacity and repeatable in results. According to the preparation process of sulfonated polyquinoxaline, the sulfonation degree is controllable, the reaction conditions are mild, and the obtained proton exchange membrane has good proton conductivity, excellent hydrolytic stability, dimensional stability and good fuel cell performance,and has a wide application prospect as a fuel cell proton exchange membrane.

Description

[0001] (1) Technical field [0002] The invention belongs to the field of proton exchange membranes, in particular to a main chain type sulfonated polyquinoxaline proton exchange membrane. [0003] (2) Background technology [0004] The past decades have seen considerable interest in the development of proton exchange membrane fuel cells (PEMFCs), as they can achieve higher efficiencies at lower environmental costs than current conventional fossil fuel power sources. The proton exchange membrane (PEM) plays a key role in the fuel cell system, both to isolate the fuel gas between the two electrodes and to transfer protons from the anode to the cathode [Feixiang Gong, Nanwen Li, Su obo Zhang. Synthesis and properties of novel sulfonated poly(phenylquinoxaline)s as proton exchange membranes [J]. Polymer. 50(2009) 6001–6008]. At present, perfluorosulfonic acid PEM is the only commercialized proton exchange membrane, the most advanced of which is the Nafion series PEM in the United...

Claims

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Application Information

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IPC IPC(8): C08G73/06C08L79/04C08J5/22H01M8/1088
CPCC08G73/0694C08J5/2256C08J2379/04H01M8/1088Y02E60/50
Inventor 陈康成刘璐陈星
Owner BEIJING INSTITUTE OF TECHNOLOGYGY
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