Carbon Nitride Photocatalysts with Integrated Oxidation and Reduction Atomic Active Centers for Improved CO<sub>2</sub>Conversion
Honghui Ou, Shangbo Ning, Peng Zhu, Shenghua Chen, Ali Han, Qing Kang, Zhuofeng Hu, Jinhua Ye, Dingsheng Wang, Yadong Li
Abstract
Abstract Single‐atom active‐site catalysts have attracted significant attention in the field of photocatalytic CO 2 conversion. However, designing active sites for CO 2 reduction and H 2 O oxidation simultaneously on a photocatalyst and combining the corresponding half‐reaction in a photocatalytic system is still difficult. Here, we synthesized a bimetallic single‐atom active‐site photocatalyst with two compatible active centers of Mn and Co on carbon nitride (Mn 1 Co 1 /CN). Our experimental results and density functional theory calculations showed that the active center of Mn promotes H 2 O oxidation by accumulating photogenerated holes. In addition, the active center of Co promotes CO 2 activation by increasing the bond length and bond angle of CO 2 molecules. Benefiting from the synergistic effect of the atomic active centers, the synthesized Mn 1 Co 1 /CN exhibited a CO production rate of 47 μmol g −1 h −1 , which is significantly higher than that of the corresponding single‐metal active‐site photocatalyst.