摘要
Imine-linked covalent organic frameworks(COFs)provide distinctive prospects for promoting photocatalytic H_(2)O_(2) production,yet the intricate involvement of imine-derived linkages chemistry under light irradiation remains incompletely elucidated.Here,imine-linked COF-LZU1 demonstrates a visible light-driven H_(2)O_(2) evolution rate of 387μmol g^(-1)h^(-1),particularly,negligible dependence on the sacrificial agents.By virtue of electron paramagnetic spectroscopy and solid-state nuclear magnetic resonance,we experimentally tracked the structure evolution and identified its autooxidation to Wurster's salt mimics under the photocatalytic conditioning.This finding coincides with the radical anion-O_(2)^(-)-governed reaction pathway and is further rationalized with additional theoretical calculations.This study provides insights into both photophysical/photochemical aspects over the imine-linkage structure.
基金
This work was supported by the National Natural Science Foundation of China(22002013)
the Fundamental Research Funds for the Central Universities(DUT22LAB602)
Liao Ning Revitalization Talents Program(XLYC2008032)
China Postdoctoral Science Foundation(Grant No.2023M740496).
作者简介
Songlin Zhang is a Master student at the School of Chemistry,Dalian University of Technology.Her research primarily focuses on the reaction mechanism of the metal-free polymer photocatalysts.Email:lin9750111@163.com;Corresponding author:Wei Liu,received his BS degree from Northwestern Polytechnical University(2012)and PhD from the University of Science and Technology of China(2017).He is currently an associate professor at the School of Chemistry,Dalian University of Technology,and his research interests focus on X-ray absorption spectroscopy and its application in photoelectrocatalysis for clean energy conversion.E-mail address:liuweikd@dlut.edu.cn。
