Despite of suitable band structures for harvesting solar light and driving water redox reactions,polymeric carbon nitride(PCN)has suf-fered from poor charge transfer ability and sluggish surface reaction kinetics,which limit its photocatalytic activity for water splitting.Herein,atomically dispersed Zn-coordinated three-dimensional(3D)sponge-like PCN(Zn-PCN)is synthesized through a novel intermediate coordination strategy.Advanced characterizations and theoretical calculations well evidence that Zn single atoms are coordinated and stabilized on PCN in the form of Zn-N6 configura-tion featured with an electron-deficient state.Such an electronic configuration has been demonstrated contributive to promoted electron excitation,accelerated charge separation and transfer as well as reduced water redox barriers.Further benefited from the abundant surface active sites derived from the 3D porous structure,Zn-PCN realizes visible-light photocatalysis for overall water splitting with H2 and O2 simultaneously evolved at a stoichiometric ratio of 2∶1.This work brings new insights into the design of novel single-atom photocatalysts by deepening the understanding of electronic configurations and reactive sites favorable to excellent photocatalysis for water splitting and related solar energy conversion reactions.

Daming Zhao;Yiqing Wang;Chung-Li Dong;Fanqi Meng;Yu-Cheng Huang;Qinghua Zhang;Lin Gu;Lan Liu;Shaohua Shen

International Research Center for Renewable Energy,State Key Laboratory of Multiphase Flow in Power Engineering,Xi'an Jiaotong University,Xi'an 710049,People's Republic of China;State Key Laboratory of Rare Earth Resource Utilization,Changchun Institute of Applied Chemistry,Chinese Academy of Sciences,Changchun 130022,People's Republic of China;Department of Physics,Tamkang University,New Taipei City 25137,Taiwan,People's Republic of China;Beijing National Laboratory for Condensed Matter Physics,Institute of Physics,Chinese Academy of Sciences,Beijing 100190,People's Republic of China

纳微快报（英文）

[1]Daming Zhao;Yiqing Wang;Chung-Li Dong;Fanqi Meng;Yu-Cheng Huang;Qinghua Zhang;Lin Gu;Lan Liu;Shaohua Shen-.Electron-Deficient Zn-N6 Configuration Enabling Polymeric Carbon Nitride for Visible-Light Photocatalytic Overall Water Splitting)[J].纳微快报（英文）,2022(12):602-616

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