Light-Induced Variation of Lithium Coordination Environment in g-C<sub>3</sub>N<sub>4</sub> Nanosheet for Highly Efficient Oxygen Reduction Reactions
Chunqiang Zhuang, Yuan Chang, Weiming Li, Shijie Li, Peng Xu, Hang Zhang, Yihong Zhang, Can Zhang, Junfeng Gao, Ge Chen, Tianyang Zhang, Zhenhui Kang, Xiaodong Han
Abstract
The structure and electronic state of the active center in a single-atom catalyst undergo noticeable changes during a dynamic catalytic process. The metal atom active center is not well demonstrated in a dynamic manner. This study demonstrated that Li metal atoms, serving as active centers, can migrate on a C 3 N 4 monolayer or between C 3 N 4 monolayers when exposed to light irradiation. This migration alters the local coordination environment of Li in the C 3 N 4 nanosheets, leading to a significant enhancement in photocatalytic activity. The photocatalytic H 2 O 2 process could be maintained for 35 h with a 920 mmol/g record-high yield, corresponding to a 0.4% H 2 O 2 concentration, which is far greater than the value (0.1%) of practical application for wastewater treatment. Density functional theory calculations indicated that dynamic Li-coordinated structures contributed to the superhigh photocatalytic activity.