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通过串联缩聚法制备用于光催化产氢和质子传导的共价嘧啶骨架

Covalent Pyrimidine Frameworks via a Tandem Polycondensation Method for Photocatalytic Hydrogen Production and Proton Conduction.

作者信息

Zhong Yifei, Li Chao, Yang Fan, Guan Lijiang, Jin Shangbin

机构信息

School of Chemical Engineering and Technology, Xi'an Jiaotong University, Xianning Road 28, Xi'an, Shaanxi, 710049, China.

出版信息

Small. 2023 Apr;19(14):e2204515. doi: 10.1002/smll.202204515. Epub 2023 Jan 12.

DOI:10.1002/smll.202204515
PMID:36635041
Abstract

The development of heteroaromatic conjugated porous polymers (H-CPPs) have received enormous research interests, because of the important functional roles of the heteroatoms in photocatalysis and proton conduction. However, due to the synthetic challenges deriving from the stable structures, the structural diversity and synthetic methods of them are still limited. Herein, a new type of H-CPPs, covalent pyrimidine frameworks (CPFs), via an efficient tandem polycondensation reaction between aldehyde, acetyl, and amidine monomers is reported. The resulting CPFs are bridged by pyrimidine units, rich of nitrogen atoms and can be structurally regulated on demand. The CPFs are shown to be active photocatalysts for hydrogen evolution from methanol via a photo-thermo-catalysis process, achieving an excellent hydrogen evolution rate of 5282.8 µmol h  g . The CPFs can be further processed into a mixed matrix membrane, displaying an excellent proton conductivity of 1.30 × 10  S cm at 413 K under anhydrous condition.

摘要

由于杂原子在光催化和质子传导中具有重要的功能作用,杂芳族共轭多孔聚合物(H-CPPs)的发展受到了极大的研究关注。然而,由于其稳定结构带来的合成挑战,它们的结构多样性和合成方法仍然有限。在此,报道了一种新型的H-CPPs,即共价嘧啶骨架(CPFs),其通过醛、乙酰基和脒单体之间的高效串联缩聚反应制备而成。所得的CPFs由富含氮原子的嘧啶单元桥连,并且可以根据需要进行结构调控。结果表明,CPFs通过光热催化过程对甲醇析氢具有活性,实现了5282.8 μmol h g的优异析氢速率。CPFs可以进一步加工成混合基质膜,在无水条件下于413 K时显示出1.30×10 S cm的优异质子传导率。

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