Abstract
AbstractCovalent organic frameworks (COFs) are highly desirable for achieving high‐efficiency overall photosynthesis of hydrogen peroxide (H2O2) via molecular design. However, precise construction of COFs toward overall photosynthetic H2O2remains a great challenge. Herein, we report the crystallines‐heptazine‐based COFs (HEP‐TAPT‐COF and HEP‐TAPB‐COF) with separated redox centers for efficient H2O2production from O2and pure water. The spatially and orderly separated active sites in HEP‐COFs can efficiently promote charge separation and enhance photocatalytic H2O2production. Compared with HEP‐TAPB‐COF, HEP‐TAPT‐COF exhibits higher H2O2production efficiency for integrating dual O2reduction active centers ofs‐heptazine and triazine moieties. Accordingly, HEP‐TAPT‐COF bearing dual O2reduction centers exhibits a remarkable solar‐to‐chemical energy efficiency of 0.65 % with a high apparent quantum efficiency of 15.35 % at 420 nm, surpassing previously reported COF‐based photocatalysts.
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