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Solvent Effects on Metal‐free Covalent Organic Frameworks in Oxygen Reduction Reaction.

Authors :
Yang, Xiubei
Fu, Yubin
Liu, Minghao
Zheng, Shuang
Li, Xuewen
Xu, Qing
Zeng, Gaofeng
Source :
Angewandte Chemie International Edition. Apr2024, Vol. 63 Issue 16, p1-7. 7p.
Publication Year :
2024

Abstract

Binding water molecules to polar sites in covalent organic frameworks (COFs) is inevitable, but the corresponding solvent effects in electrocatalytic process have been largely overlooked. Herein, we investigate the solvent effects on COFs for catalyzing the oxygen reduction reaction (ORR). Our designed COFs incorporated different kinds of nitrogen atoms (imine N, pyridine N, and phenazine N), enabling tunable interactions with water molecules. These interactions play a crucial role in modulating electronic states and altering the catalytic centers within the COFs. Among the synthesized COFs, the one with pyridine N atoms exhibits the highest activity, with characterized by a half‐wave potential of 0.78 V and a mass activity of 0.32 A mg−1, which surpass those from other metal‐free COFs. Theoretical calculations further reveal that the enhanced activity can be attributed to the stronger binding ability of *OOH intermediates to the carbon atoms adjacent to the pyridine N sites. This work sheds light on the significance of considering solvent effects on COFs in electrocatalytic systems, providing valuable insights into their design and optimization for improved performance. [ABSTRACT FROM AUTHOR]

Details

Language :
English
ISSN :
14337851
Volume :
63
Issue :
16
Database :
Academic Search Index
Journal :
Angewandte Chemie International Edition
Publication Type :
Academic Journal
Accession number :
176535590
Full Text :
https://doi.org/10.1002/anie.202319247