Authors
Lixu Wu, Zhiming Wang, Chao Miao, Yanguang Yang, Nan Hu, Haiyu Wang, Yan Li, Yongxin Zhou, Guohua Zhao
Published in
Advanced materials (Deerfield Beach, Fla.). Pages e75366. Oct 12, 2026. Epub Oct 12, 2026.
Abstract
The two-electron oxygen reduction reaction (2e- ORR) for H2O2 production and the subsequent in situ activation to ·OH are constrained by linear scaling relationships, making it difficult for a single active site to simultaneously optimize O2 activation and H2O2 conversion. This work overcomes the trade-off by spatially decoupling the cascade reaction onto single-atom and cluster-hybrid sites and employing photoelectrocatalysis (PEC). Through a ligand-exchange and pyrolysis route derived from a metal-organic framework precursor, Bi single atoms and clusters are co-anchored on B-doped TiO2. The hybrid interface thermodynamically optimizes the intermediate adsorption energies to ensure cascade selectivity, whereas PEC kinetically accelerates the H2O2-to-·OH conversion by supplying photogenerated electrons. Density functional theory and free-energy diagrams indicate that H2O2 forms at the single atoms and dissociates into ·OH at the clusters, with the relationship between the p-band center and ·OH yield following the Sabatier principle. The catalyst delivers a ·OH production rate of 250 µM h-1 at neutral pH and remains active over a broad pH range (3-9). Moreover, it enables broad-spectrum removal of recalcitrant organic pollutants and retains stable performance over 50 h of operation in a flow-cell reactor. This work offers guidance for designing cascade catalysts at single-atom and cluster-hybrid interfaces.
PMID:
42860908
Bibliographic data and abstract were imported from PubMed on 12 Oct 2026.
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