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

Angewandte Chemie - Tập 134 Số 34 - 2022
Honghui Ou1, Shangbo Ning2,3, Peng Zhu1, Shenghua Chen1, Aijuan Han1, Qing Kang2, Zhuofeng Hu4, Jinhua Ye5,3, Dingsheng Wang1, Yadong Li1
1Department of Chemistry, Tsinghua University, Beijing 100084, P.R. China
2Department Institute of Surface Analysis and Chemical Biology University of Jinan Jinan Shandong 250022 P. R. China
3TJU-NIMS International Collaboration Laboratory School of Materials Science and Engineering Tianjin University Tianjin 300072 P. R. China
4Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology School of Environmental Science and Engineering Sun Yat-sen University Guangzhou 510006 P. R. China
5International Center for Materials Nanoarchitectonics (WPI-MANA) National Institute for Materials Science (NIMS) Tsukuba 305-0047 Japan

Tóm tắt

AbstractSingle‐atom active‐site catalysts have attracted significant attention in the field of photocatalytic CO2conversion. However, designing active sites for CO2reduction and H2O 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 (Mn1Co1/CN). Our experimental results and density functional theory calculations showed that the active center of Mn promotes H2O oxidation by accumulating photogenerated holes. In addition, the active center of Co promotes CO2activation by increasing the bond length and bond angle of CO2molecules. Benefiting from the synergistic effect of the atomic active centers, the synthesized Mn1Co1/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.

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Angewandte Chemie

Tập 134 Số 34

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