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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

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

  • 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

  • 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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