Piezocatalytic overall water splitting (OWS) is a promising way to harvest hydrogen energy, but the search for efficient piezocatalysts is still challenging. The rational structure design for a piezocatalyst is one of the important strategies to improve the piezocatalytic performance. Inspired by 2D piezoelectric materials and the electron donor–acceptor (D–A) structure that can produce a built-in electric field to induce a charge pull–push effect, we target to explore the piezocatalytic properties of 2D conjugated microporous polymers (CMPs) with D–A structure for OWS. Herein, two D–A type CMPs with different D–A interactions, Zn-Salen-TEPT and Zn-Salen-TEPB, are rationally synthesized, and the piezocatalytic tests under ultrasonic irradiation show that they can efficiently catalyze OWS into H₂ and H₂O₂, with the H₂ yield rates of 3260.2 for Zn-Salen-TEPT and 1816.7 μmol g^–1 h^–1 for Zn-Salen-TEPB. Experimental results and theoretical calculations show that the strong D–A interactions can effectively construct the built-in electric field which enhances the separation and migration of intrinsic charge carriers for the catalyst and improves the piezoelectric properties of CMPs. The stronger D–A interaction in Zn-Salen-TEPT results in the higher yield rates of H₂ relative to Zn-Salen-TEPB. The high sensitivity of these piezocatalysts to mechanical forces and their piezocatalytic performance for the OWS are also attributed to the combined effect of their large specific surface area, intrinsic dipoles, high flexibility, and abundant active sites. Thus, exploring the effect of the D–A structure on the piezoelectric properties of CMPs is a meaningful attempt to present a high economic value process for generating H₂ and H₂O₂ directly from pure water.

中文翻译：

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具有供体-受体结构的共轭微孔聚合物的整体水分解的压电催化性能

压电催化整体水分解（OWS）是一种很有前景的获取氢能的方法，但寻找高效的压电催化剂仍然具有挑战性。压电催化剂的合理结构设计是提高压电催化性能的重要策略之一。受二维压电材料和电子供体-受体（D-A）结构的启发，电子供体-受体（D-A）结构可以产生内置电场以诱导电荷拉推效应，我们的目标是探索二维共轭微孔聚合物（CMP）的压电催化性能OWS 具有 D-A 结构。本文合理合成了两种具有不同D-A相互作用的D-A型CMPs Zn-Salen-TEPT和Zn-Salen-TEPB，超声辐照下的压电催化测试表明它们可以有效地将OWS催化成H ₂和H ₂ O ₂，​​Zn-Salen-TEPT 的 H ₂产率为 3260.2， Zn-Salen-TEPB 的H 2产率为 1816.7 μmol g ^–1 h ^–1 。实验结果和理论计算表明，强的D-A相互作用可以有效地构建内建电场，增强催化剂本征载流子的分离和迁移，提高CMPs的压电性能。 Zn-Salen-TEPT 中更强的 D-A 相互作用导致相对于 Zn-Salen-TEPB更高的 H ₂产率。这些压电催化剂对机械力的高敏感性及其对OWS的压电催化性能也归因于它们大的比表面积、固有偶极子、高灵活性和丰富的活性位点的综合作用。因此，探索D-A结构对CMP压电性能的影响是一种有意义的尝试，旨在提出一种直接从纯水中产生H ₂和H ₂ O _{2 的高经济价值工艺。}