在氮化碳上引入双功能位点：调控载流子迁移与O2活化以促进光催化合成H2O2

引用本文: 薛媛, 张艳军, 杜军, 徐祖顺, 廖光福, 李庆. 在氮化碳上引入双功能位点：调控载流子迁移与O₂活化以促进光催化合成H₂O₂[J]. 物理化学学报, 2026, 42(9): 100311. doi: 10.1016/j.actphy.2026.100311 shu

Citation: Yuan Xue, Yanjun Zhang, Jun Du, Zushun Xu, Guangfu Liao, Qing Li. Introducing dual-functional site on carbon nitride: steering carrier migration and O₂ activation for boosted H₂O₂ photosynthesis[J]. Acta Physico-Chimica Sinica, 2026, 42(9): 100311. doi: 10.1016/j.actphy.2026.100311 shu

在氮化碳上引入双功能位点：调控载流子迁移与O₂活化以促进光催化合成H₂O₂

薛媛 ^1, ,
张艳军 ^2, ,
杜军 ^3, ,
徐祖顺 ^1, ,
廖光福 ^{4,
,} ,
李庆 ^{1,
,}

1.
湖北大学材料科学与工程学院, 教育部功能材料绿色制备与应用重点实验室, 湖北省高分子材料重点实验室, 湖北武汉 430062
2.
北部湾大学石油与化工学院, 广西绿色化工新材料与安全技术重点实验室, 广西化工新材料与安全技术工程研究中心, 广西钦州 535000
3.
广西民族大学材料与环境学院, 广西南宁 530105
4.
福建农林大学材料工程学院, 福建福州 350002

通讯作者: Email: liaogf@fafu.edu.cn (廖光福); liqing@hubu.edu.cn (李庆)

摘要: 通过在氮化碳结构中实施精确的分子层面调控策略，可有效实现光生电子的定向传输，从而提升光催化转化效率。本文设计了一种以吡啶环作为电子陷阱的氮化碳体系。该体系在氮化碳结构边缘引入特定吸附位点(–C=O、–OH/–NH₂)，有效促进了O₂分子的活化。在可见光照射及牺牲剂存在条件下，最优样品在催化剂用量为1 mg mL^-1时实现了2798 μmol g^-1 h^-1的光催化H₂O₂产率，表观量子产率在400 nm波长下达到14.5%，优于目前已报道的大多数氮化碳基光催化剂。飞秒瞬态吸收光谱(fs-TA)揭示了电子陷阱诱导的电荷转移现象，该过程加速了电子向表面活性位点的迁移。实验表征与密度泛函理论(DFT)计算表明，氮化碳的边缘功能化改变了其电子结构，引发电荷重新分布，降低了O₂吸附与活化的能垒，并证实了依赖于吡啶环的快速电子离域通道。该工作为利用生物相容性共轭氮杂环化合物修饰氮化碳材料开发高效光催化体系提供了新思路。

关键词:

English

Introducing dual-functional site on carbon nitride: steering carrier migration and O₂ activation for boosted H₂O₂ photosynthesis

Yuan Xue ^1, ,
Yanjun Zhang ^2, ,
Jun Du ^3, ,
Zushun Xu ^1, ,
Guangfu Liao ^{4,
,} ,
Qing Li ^{1,
,}

1.
Ministry of Education Key Laboratory for the Green Preparation and Application of Functional Materials, Hubei Key Laboratory of Polymer Materials, School of Materials Science and Engineering, Hubei University, Wuhan 430062, Hubei Province, China
2.
Guangxi Key Laboratory of Green Chemical Materials and Safety Technology, Guangxi Engineering Research Center for New Chemical Materials and Safety Technology, College of Petroleum and Chemical Engineering, Beibu Gulf University, Qinzhou 535000, Guangxi Zhuang Autonomous Region, China
3.
School of Materials and Environment, Guangxi Minzu University, Nanning 530105, Guangxi Zhuang Autonomous Region, China
4.
College of Materials Engineering, Fujian Agriculture and Forestry University, Fuzhou 350002, Fujian Province, China

Corresponding author: Email: liaogf@fafu.edu.cn (Guangfu Liao); liqing@hubu.edu.cn (Qing Li)

Received Date: 25 March 2026
Accepted Date: 23 April 2026
Revised Date: 22 April 2026
Available Online: 15 September 2026

Abstract: Precise molecular-level control strategies implemented within carbon nitride structures can effectively achieve directional transfer of photogenerated electrons, enhancing photocatalytic conversion efficiency. Herein, a carbon nitride system featuring pyridine rings as electron traps is designed. It introduces specific adsorption sites (–C=O, –OH/–NH₂) at the structure edges of the carbon nitride, which effectively promotes the activation of O₂ molecules. Under visible light irradiation with sacrificial agents, the optimal sample achieves a photocatalytic H₂O₂ production rate of 2798 μmol g^-1 h^-1 at a catalyst dosage of 1 mg mL^-1. The apparent quantum yield for H₂O₂ evolution reaches 14.5% at 400 nm, outperforming most of the previously reported carbon nitride-based photocatalysts. Femtosecond transient absorption spectroscopy (fs-TA) reveals electron trap induced charge transfer that accelerates electron migration to surface active sites. Experimental characterization and density functional theory (DFT) calculations reveal that the edge functionalization of carbon nitride changes its electronic structure, leading to charge redistribution, reducing the energy barrier for O₂ adsorption and activation, and confirming a rapid electron delocalization channel dependent on the pyridine ring. This work provides new insights into modifying carbon nitride materials with biocompatible conjugated N-heterocyclic compounds for developing high-efficiency photocatalytic systems.

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沈阳化工大学材料科学与工程学院沈阳 110142

在氮化碳上引入双功能位点：调控载流子迁移与O₂活化以促进光催化合成H₂O₂

通讯作者: Email: liaogf@fafu.edu.cn (廖光福); liqing@hubu.edu.cn (李庆)

English

Introducing dual-functional site on carbon nitride: steering carrier migration and O₂ activation for boosted H₂O₂ photosynthesis

Corresponding author: Email: liaogf@fafu.edu.cn (Guangfu Liao); liqing@hubu.edu.cn (Qing Li)

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