Designing Heterocyclic Covalent Organic Frameworks with Tunable Electronic Structures for Efficient Electrosynthesis of Hydrogen Peroxide
Zhongjie Yang, Lulu Zuo, Bifu Luo, Caoyu Yang, Shi‐Qiang Wang, Li Tian Chew, Jun Zhu, Xiaofei Zhang
Abstract
Abstract The electrocatalytic production of hydrogen peroxide (H 2 O 2 ) through the two‐electron oxygen reduction reaction (2e − ORR) has garnered significant research attention in recent years due to its numerous appealing advantages, such as being eco‐friendly and exhibiting high energy conversion efficiency. Metal‐free carbon materials with specific catalytic sites have been recognized as potential electrocatalysts for 2e − ORR; however, the design of highly efficient catalysts with well‐defined structures and long‐term stability for large‐scale H 2 O 2 production remains unsatisfactory. In this study, three covalent organic frameworks (COFs) – imine‐linked LZU‐1, oxazole‐linked LZU‐190, and thiazole‐linked LZU‐190(S), are successfully synthesized to explore their catalytic activity in electrocatalytic H 2 O 2 production. Among these, the carbon sites LZU‐190(S) are predominantly activated by the introduced adjacent heteroatoms via electronic effects, resulting in much higher H 2 O 2 selectivity compared to the oxazole and imine linkages. This work provides new insights into developing COFs‐based electrocatalysts for efficient H 2 O 2 generation.