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

引用本文: 王佳瑶, 潘桂旭, 王宁, 王诗涵, 朱耀麟, 李云锋. 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[J]. 物理化学学报, 2025, 41(12): 100168. doi: 10.1016/j.actphy.2025.100168 shu

Citation: Jiayao Wang, Guixu Pan, Ning Wang, Shihan Wang, Yaolin Zhu, Yunfeng Li. Preparation of donor-π-acceptor type graphitic carbon nitride photocatalytic systems via molecular level regulation for high-efficient H₂O₂ production[J]. Acta Physico-Chimica Sinica, 2025, 41(12): 100168. doi: 10.1016/j.actphy.2025.100168 shu

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.
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

通讯作者: 王宁, ninaw2018@163.com; 朱耀麟, 20070802@xpu.edu.cn; 李云锋, liyf377@nenu.edu.cn

基金项目:
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
^†These authors contributed equally to this work.

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:

English

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

Jiayao Wang ^{1, †,} ,
Guixu Pan ^{1, †,} ,
Ning Wang ^{1,
,} ,
Shihan Wang ^1, ,
Yaolin Zhu ^{2,
,} ,
Yunfeng Li ^{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

Corresponding author: E-mail: ninaw2018@163.com (N.W.); E-mail: 20070802@xpu.edu.cn (Y.Z.); E-mail: liyf377@nenu.edu.cn (Y.L.)

Received Date: 19 July 2025
Accepted Date: 18 August 2025
Revised Date: 17 August 2025
Available Online: 15 December 2025
Fund Project:
the National Natural Science Foundation of China

the National Natural Science Foundation of China

the Shaanxi Provincial Key Research and Development Program

the Shaanxi Provincial Key Research and Development Program

the Shaanxi Provincial Department of Education Youth Innovation Team Research Plan Project

Scientific Research Program Funded by Shaanxi Provincial Education Department

the Xi'an Science and Technology Planning Project

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).

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沈阳化工大学材料科学与工程学院沈阳 110142

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

通讯作者: 王宁, ninaw2018@163.com; 朱耀麟, 20070802@xpu.edu.cn; 李云锋, liyf377@nenu.edu.cn

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

Corresponding author: E-mail: ninaw2018@163.com (N.W.); E-mail: 20070802@xpu.edu.cn (Y.Z.); E-mail: liyf377@nenu.edu.cn (Y.L.)

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