Carbon Nitride Photocatalysts with Integrated Oxidation and Reduction Atomic Active Centers for Improved CO₂Conversion

Abstract

Single-atom active-site catalysts have attracted significant attention in the field of photocatalytic CO₂ conversion. However, designing active sites for CO₂ reduction and H₂ 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 (Mn₁ Co₁ /CN). Our experimental results and density functional theory calculations showed that the active center of Mn promotes H₂ O oxidation by accumulating photogenerated holes. In addition, the active center of Co promotes CO₂ activation by increasing the bond length and bond angle of CO₂ molecules. Benefiting from the synergistic effect of the atomic active centers, the synthesized Mn₁ Co₁ /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.