Ultrafast charge transfer channels induced by alkynyl bridge in novel covalent organic frameworks for boosting photocatalytic hydrogen evolution

IF 4.8 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General Pub Date : 2025-06-26 DOI:10.1016/j.apcata.2025.120418

Shidong Wang , Wei Luo , Yeqin Chen , Tingfang Liu , Yu Huang , Xueqin Zhu , Zhiwei Cai , Minjian Yang

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引用次数: 0

Abstract

The development of efficient photocatalysts for hydrogen evolution is pivotal for sustainable energy conversion. Herein, two novel covalent organic frameworks (COFs), COF-TFPPy and COF-TAEPy, were synthesized via Schiff-base condensation, distinguished by their C–C and CC bridging units, respectively. Structural and photophysical characterizations revealed that the alkynyl-bridged COF-TAEPy exhibited enhanced π-conjugation, reduced bandgap, and superior charge transfer kinetics compared to COF-TFPPy. Under visible light, COF-TAEPy demonstrated a remarkable hydrogen evolution rate of 75.2 mmol h⁻¹ g⁻¹ , twofold higher than COF-TFPPy (37.5 mmol h⁻¹ g⁻¹). This performance stems from alkynyl-induced ultrafast charge separation, prolonged exciton lifetimes, and minimized recombination losses. Our findings highlight the critical role of alkynyl bridges in tailoring COFs for high-efficiency photocatalytic applications, providing a strategic blueprint for designing advanced energy conversion materials.

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新型共价有机骨架中炔基桥诱导的超快电荷转移通道促进光催化析氢

开发高效的析氢光催化剂是实现可持续能源转化的关键。本文通过希夫碱缩合合成了两种新型共价有机框架（COFs）： COF-TFPPy和COF-TAEPy，它们分别以C-C和CC桥接单元进行区分。结构和光物理表征表明，与COF-TFPPy相比，烷基基桥接的COF-TAEPy具有增强的π共轭性、减小的带隙和优越的电荷转移动力学。在可见光下，COF-TAEPy显示出惊人的氢发展速度：75.2 mmol h⁻¹ g⁻¹ ，比COF-TFPPy（37.5 mmol h⁻¹）高两倍。这种性能源于烷基基诱导的超快电荷分离，延长激子寿命，最小化复合损失。我们的研究结果强调了炔基桥在为高效光催化应用定制COFs方面的关键作用，为设计先进的能量转换材料提供了战略蓝图。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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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.