Self-coupling of electron acceptor units in conjugated microporous polymers strengthening local donor-acceptor interaction for improving photocatalytic activity

IF 4.7 2区化学 Q2 CHEMISTRY, PHYSICAL Applied Catalysis A: General Pub Date : 2024-07-17 DOI:10.1016/j.apcata.2024.119888

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Abstract

The partial self-coupling of donor or acceptor unit during donor-acceptor (D-A) type CMPs synthesis is often overlooked for the effect on photocatalytic activity. Herein, we developed three D-A type CMPs, named SATE-CMP-n (n=1–3), which were constructed from triazine (TEPT) unit (A) and three salen units (D). With the rigidity of salen units increasing (the rigidity: salen-1 < salen-2 < salen-3), the self-coupling proportion of TEPT decreases. The experiments and DFT calculations reveal that salen-1 has the stronger electron-donating ability compared to salen-2 and salen-3, and that the self-coupling of TEPT units also enhances the electron-accepting ability. Therefore, SATE-CMP-1 exhibits the strongest D-A interaction and the highest separation and transfer efficiency of charge carriers, and has been used a photocatalyst for S−S and S−N coupling reactions. This work proves that the self-coupling of monomers in the construction of CMPs is not overlooked for adjusting the photocatalytic activity of catalyst.

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共轭微孔聚合物中电子受体单元的自偶联加强了局部供体与受体之间的相互作用，从而提高了光催化活性

在供体-受体（D-A）型 CMPs 合成过程中，供体或受体单元的部分自偶联对光催化活性的影响往往被忽视。在此，我们开发了三种 D-A 型 CMP，命名为 SATE-CMP-n（n=1-3），它们由三嗪（TEPT）单元（A）和三个沙仑单元（D）构建而成。随着沙仑单元刚性的增加（沙仑-1 < 沙仑-2 < 沙仑-3），TEPT 的自偶联比例降低。实验和 DFT 计算表明，与 salen-2 和 salen-3 相比，salen-1 具有更强的电子供能能力，TEPT 单元的自偶联也增强了电子接受能力。因此，SATE-CMP-1 具有最强的 D-A 相互作用和最高的电荷载流子分离和转移效率，已被用作 S-S 和 S-N 偶联反应的光催化剂。这项工作证明，在构建 CMP 时，单体的自偶联对于调节催化剂的光催化活性是不可忽视的。

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来源期刊

Applied Catalysis A: General 化学-环境科学

CiteScore

9.00

自引率

5.50%

发文量

415

审稿时长

24 days

期刊介绍： Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications. Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.