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Branched block polymer for proton exchange membrane, preparation method and application

A proton exchange membrane and polymer technology, applied in the field of branched block type polymers and preparation, can solve the problems of inability to balance proton conductivity and mechanical properties, etc.

Active Publication Date: 2021-09-14
SHENZHEN UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0006] In view of the above-mentioned deficiencies in the prior art, the object of the present invention is to provide a branched block polymer for proton exchange membranes and its preparation method and application, aiming to solve the problem of proton conductivity and mechanical problems of existing proton exchange membranes. The problem of not being able to balance performance

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  • Branched block polymer for proton exchange membrane, preparation method and application
  • Branched block polymer for proton exchange membrane, preparation method and application
  • Branched block polymer for proton exchange membrane, preparation method and application

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preparation example Construction

[0056] The present invention also provides a preferred embodiment of the preparation method of the branched block polymer such as formula (I), including the following:

[0057] Step A1. In a protective atmosphere, sequentially add 3,3'-diaminobenzidine, 1,3,5-tris(4-carboxyphenyl)benzene and 1,4-benzenedioic acid to the 130-150°C In polyphosphoric acid (PPA), keep stirring for 1.5-2.5h, then raise the temperature to 165-175°C for pre-polymerization for 20-60min, then raise the temperature to 210-230°C for 40min-1.5h to obtain the intermediate product (Brp-PBI- Am);

[0058] Step B1, cooling the reacted mixture in step A1 to 130-150°C, and then adding 3,3'-diaminobenzidine and 2,2-bis(4-carboxyphenyl)hexafluoropropane in sequence, And keep stirring for 1.5-2.5h, then raise the temperature to 210-230°C for 3-5h;

[0059] Step C1, cooling the reacted mixture in step B1 to 20-40°C, soaking in saturated sodium bicarbonate solution, filtering, and washing the precipitate to obtain...

Embodiment 1

[0071] Example 1 Synthesis of the polymer of formula (I) (branched poly-p-phenylene bibenzimidazole block fluorine-containing polybenzimidazole)

[0072] (1) Install a 100 mL three-necked flask with a condensing device on a magnetic stirrer, and place the flask in an oil bath.

[0073] (2) Add 45 g of polyphosphoric acid into the three-necked flask in a nitrogen atmosphere, raise the temperature to 140 °C, and keep it warm for 2 hours until the magnetron proceeds smoothly under the condition of high rotation speed.

[0074] (3) Add 0.4543 g 3,3'-diaminobenzidine (2.12 mmol), 0.1052 g 1,3,5-tris(4-carboxyphenyl)benzene (0.24 mmol) and 0.2725 g 1 , 4-phthalic acid (1.64 mmol), the molar ratio of the three is 53:6:41.

[0075] (4) Stir at 140 °C for 2 h, then heat up to 170 °C for 0.5 h of prepolymerization, and then react at 220 °C for 1 h to obtain the intermediate product Brp-PBI-Am.

[0076] (5) Cool the reacted mixture to 140 °C, add 0.4285 g 3,3'-diaminobenzidine (2 mmol)...

Embodiment 2

[0080] Example 2 Synthesis of the polymer of formula (II) (branched fluorine-containing polybenzimidazole block poly-p-phenylene bibenzimidazole)

[0081] (1), (2) steps are the same as in Example 1.

[0082] (3) Add 0.4285 g of 3,3'-diaminobenzidine (2 mmol) and 0.3522 g of 1,4-phthalic acid (2.12 mmol) to the three-necked flask in sequence, with a molar ratio of 1:1.06.

[0083] (4) The steps are the same as in Example 1 to obtain the intermediate product p-PBI-Ac.

[0084] (5) Cool the reacted mixture to 140 °C, add 0.4543 g 3,3'-diaminobenzidine (2.12 mmol), 0.1052 g 1,3,5-tris(4-carboxybenzene base) benzene (0.24 mmol) and 0.6433 g 2,2-bis(4-carboxyphenyl)hexafluoropropane (1.64 mmol), the molar ratio of the three is 53:6:41.

[0085]Steps (6), (7), and (8) are the same as in Example 1, and finally a branched fluorine-containing polybenzimidazole block poly-p-phenylene bibenzimidazole polymer (BrF6-PBI-b-p-PBI) is obtained , the yield was 91%, and the degree of branchi...

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Abstract

The invention discloses a branched block polymer used in a proton exchange membrane, a preparation method and an application thereof, wherein the molecular structure of the polymer is similar to a "core-shell" structure, and the core structure is branched poly-p-phenylene biphenyl and imidazole, the shell structure is fluorine-containing polybenzimidazole; or the core structure is branched fluorine-containing polybenzimidazole, and the shell structure is poly-p-phenylene bibenzimidazole. Due to the introduction of a branched structure, a large number of protrusions and microcavities can be formed in the membrane made of polymer, which increases the free volume in the membrane, facilitates the absorption of phosphoric acid, and promotes the improvement of proton conductivity; at the same time, the block The structure of the membrane forms a microphase separation channel that is beneficial to the transport of protons. The two work together to make the phosphoric acid-doped polymer membrane of the present invention greatly improve the proton conductivity performance.

Description

technical field [0001] The invention relates to the field of fuel cells, in particular to a branched block polymer used for proton exchange membranes, a preparation method and application. Background technique [0002] Hydrogen-oxygen proton exchange membrane fuel cell (PEMFC) generates electricity through the catalysis of metal Pt, fuel and oxygen reaction, high energy utilization rate (60-70%), fast start-up speed, high energy density, and low environmental pollution. A promising device for efficient and clean energy utilization. Proton exchange membrane (PEM) is the core component in PEMFC, which has three major functions in fuel cells: (1) isolate fuel; (2) support catalyst; (3) conduct protons. [0003] Among PEMs, polybenzimidazole (PBI) and its derivatives have been extensively studied. Since this type of polymer contains benzimidazole rings in the main chain, it can be doped with non-volatile high-boiling phosphoric acid (PA) to get rid of the dependence on water a...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): H01M8/103H01M8/1072C08G73/18
CPCC08G73/18H01M8/103H01M8/1072Y02E60/50
Inventor 王雷王立潘成军
Owner SHENZHEN UNIV
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