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A kind of hyperbranched polybenzimidazole-polysiloxane block copolymer and its preparation method and application

A technology of polybenzimidazole block and polysiloxane block is applied in the field of hyperbranched polybenzimidazole-polysiloxane block copolymer and its preparation, and can solve the problem of decreased proton conductivity, loss of phosphoric acid, etc. problem, to achieve the effect of promoting the formation of

Active Publication Date: 2022-03-01
ZHUHAI COSMX BATTERY CO LTD
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0004] The study found that the current benzimidazole polymers used as proton exchange membrane materials have the problems of obtaining higher proton conductivity under the condition of low phosphoric acid doping level and the decrease of proton conductivity caused by the loss of phosphoric acid.

Method used

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  • A kind of hyperbranched polybenzimidazole-polysiloxane block copolymer and its preparation method and application
  • A kind of hyperbranched polybenzimidazole-polysiloxane block copolymer and its preparation method and application
  • A kind of hyperbranched polybenzimidazole-polysiloxane block copolymer and its preparation method and application

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preparation example Construction

[0089] [Preparation method of block copolymer]

[0090] The present invention also provides a kind of preparation method of above-mentioned block copolymer, it comprises the steps:

[0091] The block copolymer is prepared by dissolving carboxyl group-containing hyperbranched benzimidazole polymer and double-terminal amino group-containing polysiloxane in an organic solvent and reacting at high temperature.

[0092] Wherein, the reaction is carried out under the heating condition of 120-160° C. under the protection of inert gas; specifically, the reaction time is 10-24 hours.

[0093] Wherein, the organic solvent is one or more combinations of the following: DMF (N,N-dimethylformamide), DMAc (N,N-dimethylacetamide), DMSO (dimethylmethylene sulfone), NMP (N,N-dimethylpyrrolidone), polyphosphoric acid, methanesulfonic acid, TFA (trifluoroformic acidsulfonic acid), preferably DMF or DMAc.

[0094] Wherein, the molar ratio of the carboxyl-containing hyperbranched benzimidazole po...

Embodiment 1

[0136] (1) Add polyphosphoric acid (PPA) 378.38g in a dry three-necked flask, then add 3,3-diaminobenzidine (DAB) 2.142g and trimellitic acid ( BTA) 1.68g, the reaction solid content was 1.0%. The temperature was raised to 150°C and maintained in a nitrogen atmosphere for 3h, and then heated to 200°C for 8h.

[0137] (2) Lower the temperature of the above solution to 120°C, then add 0.346g of o-phenylenediamine (the molar ratio to BTA is 0.4:1), heat up to 190°C for 4 hours, then precipitate with deionized water, and mix with Carboxyl-containing HBPBI was obtained by washing with deionized water multiple times;

[0138] Its structure is as described in formula (b):

[0139]

[0140] (3) Take 2.46g of HBPBI (Mv=4.1kDa) from step (2) and dissolve it in DMAc (5wt%), then add 0.2g of double-terminal amino PDMS (shown in formula (a), Mn=10k, 0.02mmol) , and then inert gas argon was introduced and the temperature was raised to 160° C. for 8 h. After the reaction, the solid co...

Embodiment 2

[0145] (1) Same as Example 1, except adding 2.142g of DAB and 1.89g of BTA with a molar ratio of 1:0.9.

[0146] (2) Same as Example 1, except that 0.606 g of o-phenylenediamine was added (the molar ratio to BTA was 0.62:1).

[0147] (3) Same as Example 1, 2.88g of HBPBI (Mv=7.2kDa) from step (2) was dissolved in DMAc (5wt%), and then 0.34g of double-terminal amino PDMS (Mn=17k, 0.02mmol) was added.

[0148] After testing and calculation, the storage modulus of the polymer film not impregnated with phosphoric acid is 558MPa at 180°C, the ADL of the film impregnated with phosphoric acid is 10.73, the proton conductivity is 0.0791S / cm, and the proton conductivity per unit phosphoric acid doping level 0.00737S / cm, 0.0561S / cm proton conductivity after 10 immersions in deionized water, and 70.9% proton conductivity retention.

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Abstract

The invention relates to the field of block copolymers, in particular to a hyperbranched polybenzimidazole-polysiloxane block copolymer and its preparation method and application. The block copolymer has amphiphilicity, and the block copolymer forms a soft-hard, hydrophilic-hydrophobic structure due to the combination of the soft segment of PDMS and the hard segment of HBPBI, and the hydrophobic segment of PDMS and the hydrophilic segment of HBPBI. Phase separation structure, the proton transport channel is constructed through the phase separation structure of the two chain segments. In addition, the hyperbranched structure of HBPBI can accommodate more phosphoric acid, and finally obtain high proton conductivity (up to 0.085S / cm, the test temperature reaches 180°C), high proton conductivity retention rate (up to 85.1%), high storage modulus (767MPa, test temperature 180°C) block copolymer.

Description

technical field [0001] The invention relates to the field of block copolymers, in particular to a hyperbranched polybenzimidazole-polysiloxane block copolymer and its preparation method and application. Background technique [0002] Benzimidazole polymers (PBIs) are polymers containing benzimidazole rings in the main chain structure, which have excellent physical and chemical properties such as chemical stability, thermal stability, flame retardancy and mechanical properties, and are widely used Used in high temperature resistant fabrics, fire retardant materials and filter materials for industrial products, etc. With the rise of fuel cell research, the commonly used perfluorosulfonic acid proton exchange membrane cannot meet the operation of fuel cells under high temperature and low humidity conditions due to defects such as the decrease of proton conductivity and mechanical properties under high temperature and low humidity conditions. Researchers began to look for and st...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): C08G77/452C08G73/18H01M8/1048H01M8/1037H01M8/103H01M8/1072H01M8/124
CPCC08G77/452C08G73/18H01M8/1048H01M8/1037H01M8/103H01M8/1072H01M8/124Y02E60/50
Inventor 莫肇华李素丽李俊义徐延铭
Owner ZHUHAI COSMX BATTERY CO LTD
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