Authors
Yuan Jing, Jiabin Chen, Menglong Sun, Kaiheng Zhao, Xiaomin Wang, Lili Chen, Chuang Zhang, Xi Wang, Jiannian Yao
Published in
Angewandte Chemie (International ed. in English). Pages e6447296. Aug 14, 2026. Epub Aug 14, 2026.
Abstract
Solar-driven hydrogen peroxide (H2O2) synthesis offers a sustainable alternative to the energy-intensive anthraquinone process, yet its efficiency is fundamentally constrained by the inability to simultaneously harness photogenerated electrons and holes in a balanced, synergistic manner. Here we report a spatially separated yet electronically coupled dual-active-site photocatalyst, comprising atomic chromium (Cr) and oxygen vacancies (OVs) anchored on ultrathin TiO2 nanosheets (Cr-TiO2-x), that enables the cooperative coupling of two-electron water oxidation (2e- WOR) and oxygen reduction (2e- ORR) in a single photocatalytic framework. In situ x-ray absorption/emission spectroscopy and excited-state density functional theory calculations reveal that Cr single atoms selectively accumulate photogenerated holes to drive 2e- WOR, while OV sites trap electrons to activate O2 for 2e- ORR. This self-sustaining proton-coupled electron transfer (PCET) loop not only suppresses charge recombination but also achieves a record H2O2 production rate of 764.9 µmol g-1 h-1 in pure water without sacrificial agents, with a solar-to-chemical conversion efficiency of 1.23% and an apparent quantum yield of 11.5% at 420 nm. This work establishes a blueprint for the atomic-level design of dual-redox photocatalysts and provides direct spectroscopic evidence of excited-state charge partitioning, opening new avenues for efficient solar-fuel synthesis.
PMID:
42599811
Bibliographic data and abstract were imported from PubMed on 15 Aug 2026.
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