Pyridine Heterocycle Driven Microenvironment Regulation of β‐Ketoenamine COFs for Enhanced Photocatalytic H ₂ O ₂ Production

Abstract Pyridine heterocyclic covalent organic frameworks (COFs) have attracted widespread attention in the field of photo‐driven hydrogen peroxide (H 2 O 2 ) synthesis due to their unique optoelectronic properties and excellent electron affinity. In this study, the microenvironment change of COFs is achieved through the system regulation of pyridine content in its skeleton. Among these COFs, the bipyridine‐structured TpDaBp exhibits the best visible‐light‐driven H 2 O 2 evolution rate of 8156 µmol g −1 h −1 and reveals significant potential for photocatalytic uranium extraction, attributed to its enhanced π–π interactions, improved optoelectronic performance, and enlarged specific surface area. This work not only provided a new strategy for further designing novel pyridine N‐heterocyclic‐based COFs but also shows its novel advantages of application.