Pyridine‐Based Covalent Organic Frameworks with Pyridyl‐Imine Structures for Boosting Photocatalytic H 2 O 2 Production via One‐Step 2e − Oxygen Reduction

Abstract Bipyridine‐based covalent organic frameworks (COFs) have emerged as promising contenders for the photocatalytic generation of hydrogen peroxide (H 2 O 2 ). However, the presence of imine nitrogen alters the mode of H 2 O 2 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.…

• NN
  National Natural Science Foundation of China

  Award: 22105060
• NS
  Natural Science Foundation of Hebei Province

  Awards: E2023205001, 22567604H
• SK
  State Key Laboratory for Modification of Chemical Fibers and Polymer Materials

  Award: KF2316