Customized Design of Covalent Organic Framework with Asymmetric Dual-Function Hybrid Linkages for Promoting H<sub>2</sub>O<sub>2</sub> Photosynthesis in Air and Water.

Jia, Yuanzhe; Liu, Yuxuan; Guo, Liecheng; Huang, Zhe Cheng; Luo, Feng · Nano Lett · 2025

basic_science · Level V

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Abstract

Efficient sacrificial-agent-free photosynthesis of H<sub>2</sub>O<sub>2</sub> from air and water represents the greenest, lowest-cost, most real-time avenue for H<sub>2</sub>O<sub>2</sub> production but remains a challenging issue. Here, we show a general and effective approach through a structural design on covalent organic frameworks (COFs) with asymmetric dual-function hybrid linkages for boosting the H<sub>2</sub>O<sub>2</sub> photosynthesis of the COFs. Through such design we can equip a COF with not only a catalytic active center but also a special function for isolating the D-A motif, which consequently endows the COF (CI-COF) built on asymmetric dual-function hybrid linkages with a significantly enhanced efficiency in the generation, transmission, and separation of photogenerated carriers, relative to the COF (II-COF and CC-COF) built on symmetric single-function single linkages. Correspondingly, the performance of H<sub>2</sub>O<sub>2</sub> photosynthesis is enhanced by three or five times. Accompanied is the largely promoted O<sub>2</sub> utilization and conversion efficiency from 36.6% to 99.9%. A rare dual-channel H<sub>2</sub>O<sub>2</sub> photosynthesis is suggested for the CI-COF.