Carbon Nitride Photocatalysts with Integrated Oxidation and Reduction Atomic Active Centers for Improved CO 2 Conversion
Carbon Nitride Photocatalysts with Integrated Oxidation and Reduction Atomic Active Centers for Improved CO 2 Conversion
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具有集成氧化和还原原子活性中心的氮化碳光催化剂可提高 CO 2 转化率
DOI：
10.1002/ange.202206579
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发表时间：
2022
影响因子：
--
通讯作者：
Yadong Li
中科院分区：
文献类型：
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作者：
Honghui Ou;Shangbo Ning;Peng Zhu;Shenghua Chen;Ali Han;Qing Kang;Zhuofeng Hu;Jinhua Ye;Dingsheng Wang;Yadong Li
单原子活性中心催化剂在光催化CO2转化领域引起了极大的关注。然而，在光催化剂上同时设计用于CO2还原和H2O氧化的活性位点并在光催化体系中组合相应的半反应仍然是困难的。在这里，我们合成了一种在氮化碳上具有Mn和Co两个相容活性中心的单原子活性位光催化剂（Mn 1Co 1/CN）。我们的实验结果和密度泛函理论计算表明，Mn的活性中心促进H2O氧化通过积累光生空穴。另外，Co的活性中心通过增加CO2分子的键长和键角来促进CO2的活化.得益于原子活性中心的协同效应，合成的Mn 1Co 1/CN表现出47 μmol g−1h−1的CO生成速率，这显著高于相应的单金属活性中心光催化剂。
Single‐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−1h−1, which is significantly higher than that of the corresponding single‐metal active‐site photocatalyst.