Light-Induced Variation of Lithium Coordination Environment in g-C<sub>3</sub>N<sub>4</sub> Nanosheet for Highly Efficient Oxygen Reduction Reactions.

Zhuang, Chunqiang; Chang, Yuan; Li, Weiming; Li, Shijie; Xu, Peng; Zhang, Hang; Zhang, Yihong; Zhang, Can et al. · ACS Nano · 2024

basic_science · Level V

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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<sub>3</sub>N<sub>4</sub> monolayer or between C<sub>3</sub>N<sub>4</sub> monolayers when exposed to light irradiation. This migration alters the local coordination environment of Li in the C<sub>3</sub>N<sub>4</sub> nanosheets, leading to a significant enhancement in photocatalytic activity. The photocatalytic H<sub>2</sub>O<sub>2</sub> process could be maintained for 35 h with a 920 mmol/g record-high yield, corresponding to a 0.4% H<sub>2</sub>O<sub>2</sub> 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.