Ou Honghui, Ning Shangbo, Zhu Peng, Chen Shenghua, Han Ali, Kang Qing, Hu Zhuofeng, Ye Jinhua, Wang Dingsheng, Li Yadong
Department of Chemistry, Tsinghua University, Beijing, 100084, P. R. China.
TJU-NIMS International Collaboration Laboratory, School of Materials Science and Engineering, Tianjin University, Tianjin, 300072, P. R. China.
Angew Chem Int Ed Engl. 2022 Aug 22;61(34):e202206579. doi: 10.1002/anie.202206579. Epub 2022 Jul 8.
Single-atom active-site catalysts have attracted significant attention in the field of photocatalytic CO conversion. However, designing active sites for CO reduction and H 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 Co /CN). Our experimental results and density functional theory calculations showed that the active center of Mn promotes H O oxidation by accumulating photogenerated holes. In addition, the active center of Co promotes CO activation by increasing the bond length and bond angle of CO molecules. Benefiting from the synergistic effect of the atomic active centers, the synthesized Mn Co /CN exhibited a CO production rate of 47 μmol g h , which is significantly higher than that of the corresponding single-metal active-site photocatalyst.
单原子活性位点催化剂在光催化CO转化领域引起了广泛关注。然而，在光催化剂上同时设计用于CO还原和H₂O氧化的活性位点，并在光催化体系中结合相应的半反应仍然具有挑战性。在此，我们合成了一种双金属单原子活性位点光催化剂，在氮化碳上具有两个兼容的Mn和Co活性中心（Mn-Co/CN）。我们的实验结果和密度泛函理论计算表明，Mn活性中心通过积累光生空穴促进H₂O氧化。此外，Co活性中心通过增加CO分子的键长和键角促进CO活化。得益于原子活性中心的协同效应，合成的Mn-Co/CN表现出47 μmol g⁻¹ h⁻¹的CO产率，显著高于相应的单金属活性位点光催化剂。
