Charging modulation of the pyridine nitrogen of covalent organic frameworks for promoting oxygen reduction reaction

咪唑 离子键合 共价键 催化作用 吡啶 化学 金属 无机化学 光化学 离子 有机化学
作者
Xiubei Yang,Qizheng An,Xuewen Li,Yubin Fu,Shuai Yang,Minghao Liu,Qing Xu,Gaofeng Zeng
出处
期刊:Nature Communications [Nature Portfolio]
卷期号:15 (1) 被引量:43
标识
DOI:10.1038/s41467-024-46291-y
摘要

Abstract Covalent organic frameworks (COFs) are ideal templates for constructing metal-free catalysts for the oxygen reduction reaction due to their highly tuneable skeletons and controllable porous channels. However, the development of highly active sites within COFs remains challenging due to their limited electron-transfer capabilities and weak binding affinities for reaction intermediates. Herein, we constructed highly active catalytic centres by modulating the electronic states of the pyridine nitrogen atoms incorporated into the frameworks of COFs. By incorporating different pyridine units (such as pyridine, ionic pyridine, and ionic imidazole units), we tuned various properties including dipole moments, reductive ability, hydrophilicity, and binding affinities towards reaction intermediates. Notably, the ionic imidazole COF ( im -PY-BPY-COF) exhibited greater activity than the neutral COF (PY-BPY-COF) and ionic pyridine COF ( ion -PY-BPY-COF). Specifically, im -PY-BPY-COF demonstrated a half-wave potential of 0.80 V in 0.1 M KOH, outperforming other metal-free COFs. Theoretical calculations and in situ synchrotron radiation Fourier transform infrared spectroscopy confirmed that the carbon atoms in the ionic imidazole rings improved the activity by facilitating binding of the intermediate OOH* and promoting the desorption of OH*. This study provides new insights into the design of highly active metal-like COF catalysts.
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