物理化学学报

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氰基调控助催化剂电子结构用于高效光催化析氢

尹树杰1, 许家超1, 蔡政宇1, 钟威2, 王国宏1, 吴新鹤1   

  1. 1 污染物分析与资源化技术湖北省重点实验室，湖北师范大学化学化工学院，湖北 黄石 435002;
    2 深圳技术大学新材料与新能源学院，广东 深圳 518118
  • 收稿日期:2026-08-09 修回日期:2026-08-20 录用日期:2026-08-23
  • 通讯作者: 许家超, 钟威, 吴新鹤Jiachao Xu, Wei Zhong, Xinhe Wu E-mail:xujiachao@hbnu.edu.cn;zhongwei@sztu.edu.cn;wuxinhe@hbnu.edu.cn
  • 基金资助:
    本工作得到了国家自然科学基金(22302061和22578106)以及2025年国家级大学生创新创业训练计划项目(202510513002和S202510513061)资助。

Cyano-induced electronic structure regulation of co-catalysts toward high-efficiency photocatalytic hydrogen evolution

Shujie Yin1, Jiachao Xu1, Zhengyu Cai1, Wei Zhong2, Guohong Wang1, Xinhe Wu1   

  1. 1 Hubei Key Laboratory of Pollutant Analysis and Reuse Technology, College of Chemistry and Chemical Engineering, Hubei Normal University, Huangshi 435002, Hubei Province, China;
    2 College of New Materials and New Energies, Shenzhen Technology University, Shenzhen 518118, Guangdong Province, China
  • Received:2026-08-09 Revised:2026-08-20 Accepted:2026-08-23

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摘要： 调控半导体催化剂载体与负载型助催化剂之间的界面电子相互作用，是一种精准调控助催化剂活性中心电子态、进而提升催化性能的有效策略。本文合成了铂纳米颗粒负载的富氰基晶化氮化碳纳米片(Pt-CCNS)光催化剂，实现Pt纳米颗粒高度均匀分散并同时增强了Pt助剂与g-C3N4之间的界面电子耦合作用。相较于传统Pt纳米颗粒改性g-C3N4 (Pt-CN)，Pt‑CCNS当中引入的氰基具不仅能够让Pt助催化剂均匀锚定在晶化g-C3N4表面，还可以加速电荷由g-C3N4载体向活性Pt活性位点迁移。该电子传输过程优化了氢反应中间体在Pt活性位点上的吸附行为。得益于优化后的Pt助剂电子结构以及高效的界面电荷传输，最优样品Pt-CCNS0.1的光催化产氢速率可达596.7 μmol h−1，是Pt-CN材料的2.8倍、纯g-C3N4的29.6倍。本研究阐明了助催化剂改性光催化体系中的界面电子作用机制，为高效光催化材料的合理构筑提供了可靠思路。

关键词: 光催化, 产氢, 晶化氮化碳, 氰基, 电子结构调控

Abstract: Tailoring the electronic interaction at the interface between semiconductor catalyst supports and deposited cocatalysts affords a refined strategy to precisely manipulate the electronic states of the active centers residing in the cocatalysts, and concomitantly promote their catalytic efficacy. Herein, we report the fabrication of Pt‑CCNS, a model system consisting of Pt nanoparticles supported on cyano-rich crystalline g-C3N4 nanosheet, which manifests highly uniform Pt dispersion and a strengthened interfacial electronic interaction with the underlying g-C3N4. Compared with conventional Pt nanoparticle-modified g-C3N4 (Pt-CN), the introduced cyano groups in Pt‑CCNS play a dual role. They not only enable uniform dispersion of Pt cocatalysts on the crystalline g‑C3N4 surface, but also effectively promote charge transfer from the g-C3N4 substrate to Pt sites. This enhanced electron flow consequently optimizes the adsorption behavior of hydrogen reaction intermediates on the Pt active centers. Benefiting from the optimized electronic structure and interfacial charge transfer, the optimized Pt-CCNS0.1 photocatalyst delivers a prominent hydrogen-evolution rate of 596.7 μmol h−1, outperforming Pt‑CN by a factor of 2.8 and pristine g-C3N4 by a factor of 29.6. This investigation elucidates the intricate interfacial electronic interactions in cocatalyst-modified photocatalytic systems and, more importantly, establishes a robust paradigm for the rational construction of high-efficiency photocatalysts.

Key words: Photocatalysis, Hydrogen evolution, Crystalline g-C3N4, Cyano group, Electronic structure regulation