Liang Jiayu, Tian Fengyu, Li Yaohao, Wang Yifan, Yan Xuemin, Zhang Honglei
College of Chemistry and Environment Engineering, Yangtze University, Jingzhou 434023, Hubei, China.
College of Chemistry and Environment Engineering, Yangtze University, Jingzhou 434023, Hubei, China; Key Laboratory of Low Carbon Catalysis and Carbon Dioxide Utilization, Wuhan 430100, Hubei, China.
Environ Res. 2025 Jul 8;285(Pt 1):122324. doi: 10.1016/j.envres.2025.122324.
Solar-driven CO conversion into valuable chemicals offers an intriguing solution to ameliorate the global warming and energy crisis. Although graphitic carbon nitride (g-CN) demonstrates photocatalytic activity for CO reduction, the practical application is hindered by sluggish reaction dynamics and rapid photogenerated charge recombination. Herein, we report Cu single atoms anchored on phosphorus-doped g-CN nanosheets (Cu/PCN), fabricated through an in-situ icing assisted photodeposition method. Experimental results demonstrate that the phosphorus doping effectively enhances the reduction potential of photogenerated electrons and the engineering of Cu atoms can significantly accelerate the photogenerated charge separation. Further DFT calculations reveal that introducing Cu single atoms in the phosphorus-doped g-CN effectively lower the energy barrier for the critical COOH∗ intermediates, thus promoting the CO evolution. As a result, the optimized Cu/PCN photocatalyst exhibits outstanding performance in visible-light-driven CO photoreduction, achieving a remarkable CO generation rate of 6.01 μmol g h. This work provides an atomic-level metal-nonmetal synergistic modulation strategy for promoting CO generation form CO photoreduction kinetically.
