1. Co–N2 Bond Precisely Connects the Conduction Band and Valence Band of g‐C3N4/CoCo‐LDH to Enhance Photocatalytic CO2 Activity by High‐Efficiency S‐Scheme
- Author
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Yi-lei Li, Qing Zhao, Xu-jia Liu, Ying Liu, Ying-juan Hao, Xiao-jing Wang, Xin-ying Liu, Diane Hildebrandt, Feng-yu Li, and Fa-tang Li
- Subjects
carbon products ,CoN2 bond ,photocatalytic CO2 reduction ,S-scheme heterojunctions ,water oxidation half-reaction ,Physics ,QC1-999 ,Chemistry ,QD1-999 - Abstract
Precise regulation of photogenic electron transfer path plays an important role in improving photocatalytic carbon dioxide reduction efficiency and product selectivity. Herein, under the guidance of density functional theory calculation, the interface chemical bond (CoN2 bond) at the atomic level is designed, and g‐C3N4/CoCo‐layered double hydroxide (LDH) heterostructure is manufactured. CoCo‐LDH with water oxidation ability and g‐C3N4 were combined to construct S‐scheme heterojunction with redox ability. The valence band and conduction band of g‐C3N4 and CoCo‐LDH are precisely connected by the interfacial CoN2 bond, which realizes the high‐speed transfer of electron transport. Despite the absence of cocatalyst, the heterojunction exhibits high water oxidation and carbon reduction capacity due to the precise regulation of CoN2 bonds. Theoretical calculations and experimental results show that the addition of CoCo‐LDH: reduces the oxidation overpotential of water to provide more H protons; regulates the delocalization charge of g‐C3N4; and reduces the energy barrier of the CO2 intermediate (*COOH) in the reduction half‐reaction. The results show that the selectivity of carbon‐based substances in the products was 100%, and the optimal CO yield was 71.39 μmol g−1 h−1, which is among the highest values of g‐C3N4‐based photocatalysts.
- Published
- 2023
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