Engineering the S-scheme heterojunction modulating the charge density of the central carbon atom of half-metallic carbon nitride for boosting CO2 photoreduction

作者：Chentao Zhu, Kang Zhong, Bingbing Zhu, Shuting Li, Huaming Li, Jinman Yang, Hui Xu · 发表于：Applied Catalysis B: Environmental · 年份：2025 · DOI：10.1016/j.apcatb.2025.125200 · 被引用次数：34 · 研究领域：Electronic and Structural Properties of Oxides、Advanced Photocatalysis Techniques、Gas Sensing Nanomaterials and Sensors

The construction of S-scheme heterojunction can effectively retain higher oxidation and reduction potentials within a compound semiconductor system, exhibiting significant potential in photogenerated carrier separation. Herein, Bi 2 MoO 6 (BMO) nanosheets were grown in - situ on bulk hm-C 4 N 3 (hm-CN) by a one-step hydrothermal method , creating an extremely tight S-scheme heterojunction interface. This interface accelerates the photogenerated electron migration from BMO to hm-CN and inhibits photogenerated electron-hole complexation. DFT calculations confirm that S-scheme heterojunction exhibits the mechanism of charge density modulation for hm-CN, with more electrons enrich on the central C atom. Meanwhile, the energy barrier for photocatalytic CO 2 reduction is reduced from 0.82 eV to 0.59 eV. Consequently, the optimized BMO/CN-150 photocatalyst exhibits the highest performance enhancement in CO 2 photoreduction to CO and CH 4 , which is 14.5 times (CO) and 16.1 times (CH 4 ) of the hm-CN monomer and maintains exception stability over 24 h. This study provides an effective strategy to utilize the charge transfer interaction between heterojunctions to precisely modulate the charge density of a certain component and thus design efficient artificial photosynthesis catalysts.