物理化学学报 >> 2025, Vol. 41 >> Issue (12): 100168.doi: 10.1016/j.actphy.2025.100168

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基于分子水平调控的供体-π-受体型石墨相氮化碳光催化体系的制备及其高效生产H2O2

王佳瑶1,†, 潘桂旭1,†, 王宁1,*(), 王诗涵1, 朱耀麟2,*(), 李云锋1,*()   

  1. 1 西安工程大学环境与化学工程学院, 功能性纺织材料及制品教育部重点实验室, 陕西 西安 710048
    2 西安工程大学电子信息学院, 陕西 西安 710048
  • 收稿日期:2025-07-19 修回日期:2025-08-17 录用日期:2025-08-18 发布日期:2025-10-23
  • 通讯作者: Email: liyf377@nenu.edu.cn (李云锋)20070802@xpu.edu.cn (朱耀麟)ninaw2018@163.com (王宁)
  • 作者简介:

    †These authors contributed equally to this work.

  • 基金资助:
    国家自然科学基金(22008185); 国家自然科学基金(21872023); 陕西省重点研发计划(2022GY-166); 陕西省重点研发计划(2024SF-YBXM-593); 陕西省教育厅青年创新团队研究计划项目(24JP072); 陕西省教育厅科研计划项目(23JC033); 西安市科技计划项目(24GXFW0021)

Preparation of donor-π-acceptor type graphitic carbon nitride photocatalytic systems via molecular level regulation for high-efficient H2O2 production

Jiayao Wang1, Guixu Pan1, Ning Wang1,*(), Shihan Wang1, Yaolin Zhu2,*(), Yunfeng Li1,*()   

  1. 1 College of Environmental and Chemical Engineering, Key Laboratory of Functional Textile Material and Product of the Ministry of Education, Xi'an Polytechnic University, Xi'an 710048, Shannxi Province, China
    2 School of Electronics and Information, Xi'an Polytechnic University, Xi'an 710048, Shannxi Province, China
  • Received:2025-07-19 Revised:2025-08-17 Accepted:2025-08-18 Published:2025-10-23
  • Contact: Email: liyf377@nenu.edu.cn (Yunfeng Li)20070802@xpu.edu.cn (Yaolin Zhu)ninaw2018@163.com (Ning Wang)
  • Supported by:
    the National Natural Science Foundation of China(22008185); the National Natural Science Foundation of China(21872023); the Shaanxi Provincial Key Research and Development Program(2022GY-166); the Shaanxi Provincial Key Research and Development Program(2024SF-YBXM-593); the Shaanxi Provincial Department of Education Youth Innovation Team Research Plan Project(24JP072); Scientific Research Program Funded by Shaanxi Provincial Education Department(23JC033); the Xi'an Science and Technology Planning Project(24GXFW0021)

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摘要：

供体-π-受体(D-π-A)共轭聚合物是一类新兴材料，其结构特征为交替排列的电子供体(D)、π桥(π)和电子受体(A)单元，在增强可见光吸收及优化电荷分离与再分布方面展现出显著潜力。为克服石墨相氮化碳(g-C3N4)的局限性并发挥D-π-A体系的结构优势，本研究通过精确的分子水平调控，设计合成了一系列4-芳香胺衍生物修饰的g-C3N4光催化剂，以实现特定的局域电子离域化。该策略可系统研究电子离域程度与光催化H2O2生成之间的构效关系。此外，调控电子离域的吸电子诱导效应显著增强了光生电子向表面活性位点的转移效率。最优催化剂表现出卓越的H2O2生成性能，其产率是原始g-C3N4的30.44倍。机理研究表明，D-π-A型g-C3N4的光催化H2O2生成主要通过双电子氧还原反应(ORR)路径实现。

关键词: 光催化, g-C3N4, D-π-A结构, 超分子自组装, H2O2生产

Abstract:

Donor-π-Acceptor (D-π-A) conjugated polymers represent an emerging class of materials featuring alternating electron donor (D), π-bridge (π), and electron acceptor (A) units, which exhibit significant potential in enhancing visible-light absorption and optimizing charge separation and redistribution. To overcome the limitations of graphitic carbon nitride (g-C3N4) while capitalizing on the structural merits of D-π-A systems, a series of 4-aromatic amine derivatives modified g-C3N4 photocatalysts was designed and synthesized through precise molecular level regulation with tailored local electron delocalization. This strategy allows for a systematic investigation of the relationship between electron delocalization extent and photocatalytic H2O2 production. Furthermore, the electron-withdrawing induction effect for regulating electron delocalization results in a substantial enhancement of photoinduced electron transfer to surface reactive sites. The as-synthesized optimum photocatalyst exhibits a remarkable H2O2 production performance, which is 30.44 times higher than that of the pristine g-C3N4. The mechanism study reveals that the photocatalytic H2O2 production in D-π-A-type g-C3N4 proceeds primarily via a two-electron oxygen reduction reaction (ORR).

Key words: Photocatalysis, g-C3N4, D-π-A structure, Supramolecular self-assembly, H2O2 production.