Qi-Bin Han, Hui‐Long Wang, Hao Huang, Wen‐Feng Jiang
Developing round‐the‐clock photocatalysts with sustained high‐efficiency performance remains one of the most challenging frontiers in environmental remediation. Herein, we propose a strategy of construction of highly efficient round‐the‐clock photocatalysts through a mechanism based on photo‐induced electron storage coupled with peroxidase‐like activity. Based on this strategy, a novel S‐scheme WO 3 /COFTB heterojunction was successfully developed by integrating bipyridine‐based covalent organic framework (COFTB) with hexagonal WO 3 for the round‐the‐clock degradation of organic contaminants. Under illumination, the WO 3 /COFTB heterojunction efficiently generates H 2 O 2 in situ from water and air. WO 3 acts as an electron transfer station in COFTBW, enabling efficient ciprofloxacin (CIP) degradation under both light irradiation (99.32%, 60 min) and dark conditions (92.95%, 60 min). The S‐scheme charge transfer mechanism in COFTBW is revealed, where the heterojunction structure facilitates photoinduced carrier separation and transfer, thereby boosting photocatalytic efficiency. In darkness, the stored electrons in WO 3 migrate to COFTB, triggering direct O 2 reduction and subsequent H 2 O 2 activation to generate ROS, which drive pollutant degradation in the absence of light. This study provides a novel design strategy for round‐the‐clock photocatalysts through the synergistic coupling of multiple mechanisms, allowing the construction of an energy‐efficient and robust photocatalytic system capable of effective round‐the‐clock degradation of pollutants.