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A kind of phosphonated (polyolefin-g-hyperbranched polybenzimidazole) graft copolymer and its preparation method and application

A technology of graft copolymer and benzimidazole, which is applied in the field of phosphonated graft copolymer and its preparation, can solve the problems of phosphoric acid loss, reduction of proton conductivity, decrease of mechanical properties, etc., to promote migration and improve proton conductivity. efficiency, high proton conductivity

Active Publication Date: 2022-03-18
ZHUHAI COSMX BATTERY CO LTD
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0003] In the field of high-temperature proton exchange membranes, the proton conductivity of PBIs-based proton exchange membranes is heavily dependent on its phosphoric acid doping level (ADL, per mole of polymer repeating units combined phosphoric acid mole number), in order to make this type of membrane have high proton conductivity, a large amount of phosphoric acid needs to be mixed in, which will lead to a significant decline in the mechanical properties of the membrane, so it is necessary to take into account the balance between proton conductivity and mechanical properties; in addition, More phosphoric acid is also easy to lose with the water generated by the cathode during use, which will reduce the proton conductivity of the membrane

Method used

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  • A kind of phosphonated (polyolefin-g-hyperbranched polybenzimidazole) graft copolymer and its preparation method and application
  • A kind of phosphonated (polyolefin-g-hyperbranched polybenzimidazole) graft copolymer and its preparation method and application
  • A kind of phosphonated (polyolefin-g-hyperbranched polybenzimidazole) graft copolymer and its preparation method and application

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preparation example Construction

[0088]

[0089] The present invention also provides a kind of preparation method of above-mentioned graft copolymer, it comprises the steps:

[0090] (1) Mixing the olefinic polymer containing carboxyl group in the side chain and the phosphonic acid containing amino group, and reacting to obtain the partially phosphonated olefinic polymer containing carboxyl group in the side chain;

[0091] (2) dissolving amino group-containing hyperbranched benzimidazole polymers, side chain carboxyl-containing partially phosphonated olefin polymers and carboxyl-containing phosphonic acids in an organic solvent, reacting under heating conditions to prepare the described graft copolymer.

[0092] In a specific embodiment of the present invention, in step (1), the olefinic polymer containing carboxyl groups in the side chain is selected from, for example, polyacrylic acid (PAA), polymethacrylic acid (PMAA), carboxylated polystyrene at least one of .

[0093] In a specific embodiment of the ...

Embodiment 1

[0128] (1) Add 1219g of polyphosphoric acid (PPA) to a dry three-necked flask and heat up to 120°C, then add 3,3-diaminobenzidine (DAB) 3.43g and 2- Phosphonic acid butane-1,2,4-tricarboxylic acid (PBTCA) 2.70g, solid content accounted for 0.5% of the total solution, stirred at this temperature for 4h to fully dissolve the solid. The temperature was raised to 150°C and maintained in a nitrogen atmosphere for 3h, and then heated to 200°C for 20h. After the reaction stopped, the solution was precipitated in water, washed twice with deionized water, then added with sodium bicarbonate to make it alkaline, and then washed with deionized water until neutral. The solid was collected and dried under vacuum at 60° C. to obtain hyperbranched polybenzimidazole (HBPBI) with amino as the end group.

[0129] (2) Dissolve 0.3 g of polyacrylic acid (PAA) in DMAc, then add 0.986 g of alendronic acid (accounting for 95% of the carboxyl moles), react at 150° C. for 12 h under the protection of ...

Embodiment 2

[0134] (1) Other operations are the same as in Example 1, the difference is: add polyphosphoric acid (PPA) 1219g to a dry three-necked flask and heat up to 120°C, then add DAB 3.86g and PBTCA 2.70 at the same time with a molar ratio of 1.8:1 g, the solid content accounted for 0.8% of the total solution, stirred at this temperature for 4 hours to fully dissolve the solid. The temperature was raised to 150°C and maintained in a nitrogen atmosphere for 3h, and then heated to 200°C for 20h.

[0135] (2) Dissolve 0.45g of PAA in DMAc, then add 1.090g of alendronic acid (accounting for 70% of the carboxyl moles), react at 150°C for 12h under the protection of nitrogen, and then dry by rotary evaporation of the solvent to obtain partially phosphonated PAA (LPAA).

[0136] (3) According to the mass ratio of 1.75:1, the total mass of 4.01 g of HBPBI in (1) and LPAA in (2) were dissolved in DMAc to obtain solution a. 1.502 g of phosphonoacetic acid was dissolved in DMF to obtain solut...

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Abstract

The invention relates to the field of graft copolymers, in particular to a phosphonated (polyolefin-g-hyperbranched polybenzimidazole) graft copolymer and its preparation method and application. The material of the present invention uses polyolefins as the main chain and uses HBPBI as the branch to synthesize the graft copolymer. The polymers with two properties will undergo microscopic phase separation to construct proton transport channels, thereby improving the proton conductivity; in addition, at high temperatures, the flexible main chain drives the movement of HBPBI branch chains to reduce the activation energy of proton migration and promote the migration of phosphoric acid or protons , to increase the proton conductivity. Utilizing the hyperbranched structure can not only accommodate more phosphoric acid, but also a large number of active sites in the hyperbranched structure can be grafted with a large amount of organic phosphonic acid, which can reduce the loss of phosphoric acid and improve the retention rate of proton conductivity through a two-pronged approach. High proton conductivity (0.09S / cm) can be obtained at a lower phosphoric acid doping level (ADL<9).

Description

technical field [0001] The invention relates to the field of graft copolymers, in particular to a phosphonated (polyolefin-g-hyperbranched polybenzimidazole) graft 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 ...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): C08G81/02C08F8/40C08F120/06C08G73/18H01M8/18H01M8/1041H01M8/1088H01M8/1072
CPCC08G81/024C08F8/40C08G73/18H01M8/188H01M8/1041H01M8/1088H01M8/1072H01M2300/0082C08F120/06Y02E60/50
Inventor 莫肇华李素丽李俊义徐延铭
Owner ZHUHAI COSMX BATTERY CO LTD