Authors
Ruixue Sun, Shaoyang Gao, Luqiao Feng, Peixuan Xie, Wenyu Shen, Nikita Rog, Marwan Mohammed, Qi Huang, Giulio Santori, Xianfeng Fan, Bien Tan, Cher Hon Lau
Published in
Angewandte Chemie (International ed. in English). Pages e7792190. Sep 04, 2026. Epub Sep 04, 2026.
Abstract
Photocatalytic hydrogen peroxide (H2O2) synthesis from water and oxygen is a promising alternative to the anthraquinone process, but its efficiency depends on charge separation and reactant transport. Herein, we report a side chain strategy to regulate nanochannel microenvironments of hydrazone-linked covalent organic frameworks (COFs). Four COFs bearing H, OMe, OEt, or OEtOMe groups were prepared using the same benzotrithiophene node and hydrazone-linked framework. The alkoxy side chains tune pore polarity, accessible porosity, electronic properties, and water and oxygen adsorption. Among them, COF-Hz-OEtOMe exhibits the strongest water and oxygen affinity and favorable charge-separation behavior. It achieves an H2O2 production rate of 7240 µmol g-1 h-1 at the optimized catalyst loading in pure water and 22910 µmol g-1 h-1 with benzyl alcohol. A 1 L reactor using tap water and air accumulates 1.42 mM H2O2 after 4 h under natural sunlight. Experiments and theoretical calculations suggest that the conjugated framework promotes charge separation, while the alkoxy-functionalized nanochannels improve reactant adsorption and oxygen activation. Life cycle assessment (LCA) highlights that natural sunlight and larger-scale catalyst synthesis can reduce the calculated climate impact. These results demonstrate that pore-wall side chain engineering provides an effective strategy for regulating charge behavior and reactant transport in porous photocatalysts.
PMID:
42698127
Bibliographic data and abstract were imported from PubMed on 05 Sep 2026.
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