光催化
分解水
氮化碳
氧化还原
材料科学
电子转移
光催化分解水
光化学
可见光谱
碳纤维
化学计量学
电子结构
氮化物
太阳能燃料
纳米技术
化学物理
化学
催化作用
光电子学
物理化学
计算化学
复合材料
冶金
复合数
生物化学
图层(电子)
作者
Daming Zhao,Yiqing Wang,Chung‐Li Dong,Fanqi Meng,Yu‐Cheng Huang,Qinghua Zhang,Lin Gu,Lan Liu,Shaohua Shen
标识
DOI:10.1007/s40820-022-00962-x
摘要
Despite of suitable band structures for harvesting solar light and driving water redox reactions, polymeric carbon nitride (PCN) has suffered 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 configuration 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.
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