Carbon‐Rich Carbon Nitride with Synergistic Gd‐N <sub>4</sub> Sites and Z‐Scheme Heterojunction for Non‐sacrificial Hydrogen Peroxide Photosynthesis
Yuxin Yao, Teng Liang, Zhijun Li, Zhijun Li, Zhongyuan Wang, Pengze Wang, Tianwei Dou, Ziyu Chen, Zhuo Li, Zhuo Li, Ji Bian, Liqiang Jing
Abstract
Abstract Carbon nitride (CN), a highly promising photocatalyst for hydrogen peroxide (H 2 O 2 ) production, still suffers from rapid electron‐hole recombination and sluggish kinetics in both the O 2 reduction reaction (ORR) and water oxidation reaction (WOR). Here, a molecular engineering strategy enables the controlled synthesis of carbon and Gd‐N 4 single‐atoms co‐incorporated CN nanotubes. Subsequently, a Z‐scheme heterojunction is constructed via electrostatic self‐assembly with Bi 2 WO 6 nanosheets (BWO). The optimized composite exhibits exceptional performance in visible‐light‐driven H 2 O 2 synthesis (749.5 µmol g −1 h −1 ) in pure water, achieving a 37‐fold enhancement compared to pristine CN. Moreover, the apparent quantum yield (AQY) reaches an impressive 11.13% at 420 nm. The enhanced activity is primarily attributed to the synergistic effects of C/Gd co‐incorporation and the Z‐scheme heterojunction, which collectively promote the separation of photogenerated charges in CN. Particularly, the unsaturated coordination Gd‐N 4 sites effectively facilitate O 2 adsorption and the 2e − ORR pathway, enabling efficient H 2 O 2 production. Meanwhile, BWO enhances the WOR, thus improving the matching efficiency of redox reactions in the system. This study establishes a facile molecular engineering strategy for single‐atoms anchoring with tailored coordination environments, while highlighting the critical role of redox dual‐regulation in achieving efficient H 2 O 2 photosynthesis.