亚胺
光催化
共价键
吡啶
光化学
化学
共价有机骨架
组合化学
过氧化氢
有机化学
催化作用
作者
Wenwang Wu,Zixuan Li,Shiyin Liu,Di Zhang,Bowen Cai,Yun-Feng Liang,Mingxing Wu,Yaozu Liao,Xiaojia Zhao
标识
DOI:10.1002/anie.202404563
摘要
Bipyridine-based covalent organic frameworks (COFs) have emerged as promising contenders for the photocatalytic generation of hydrogen peroxide (H2O2). However, the presence of imine nitrogen alters the mode of H2O2 generation from an efficient one-step two-electron (2e-) route to a two-step 2e- oxygen reduction pathway. In this work, we introduce 3,3'-bipyridine units into imine-based COF skeletons, creating a pyridyl-imine structure with two adjacent nitrogen atoms between the pyridine ring and imine linkage. This unique bipyridine-like architecture can effectively suppress the two-step 2e- ORR process at the single imine-nitrogen site, facilitating a more efficient one-step 2e- pathway. Consequently, the optimized pyridyl-imine COF (PyIm-COF) exhibits a remarkable H2O2 production rate of up to 5850 μmol h-1 g-1, nearly double that of pristine bipyridine COFs. This work provides valuable insight into the rational design of functionalized COFs for enhanced H2O2 production in photocatalysis.
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