Electronic‐State Programming of Ultrasmall CeO 2 Switches H 2 O 2 Activation From Radical to Bio‐
Bo Yuan, Xinyu Wu, Yin‐Song Liao, Chao Zhao, Zhanping Xiao, Wanqing Dai, Jyh‐Pin Chou, Wenchao Peng, Jian Lin Chen, Pi‐Tai Chou, Yung‐Kang PengABSTRACT
Antibiotic resistance, driven by antibiotic‐resistant bacteria (ARB) and genes (ARGs) in aquatic systems, is an escalating threat. Conventional advanced oxidation processes (AOPs) based on OH radicals are limited by rapid radical scavenging. 1 O 2 is a promising alternative, but current H 2 O 2 ‐to‐ 1 O 2 routes rely on HO 2 radical chain‐termination reactions and suffer from short radical lifetimes and equilibrium with 3 O 2 , leading to poor conversion efficiency. Inspired by bromoperoxidases (BPOs), we report a facile, scalable synthesis of carbon framework‐supported ultrasmall CeO 2 nanoparticles (NPs). This material features electron‐lean Ce sites that activate H 2 O 2 exclusively via a nonradical pathway, enabling selective HOBr production and outperforming BPOs in subsequent conversion to 1 O 2 . A counterpart with electron‐rich Ce sites that activate H 2 O 2 only via the conventional radical pathway was further prepared for comparison. Degradation of various contaminants (dyes, antibiotics, and ARB/ARG) reveals that the nonradical pathway far outperforms the radical pathway in both H 2 O 2 utilization and removal efficiency. The optimized sample exhibits high ARB/ARG removal efficiency in a continuous‐flow reactor for 10 h. This work demonstrates a bio‐inspired route for nonradical H 2 O 2 ‐to‐ 1 O 2 conversion and a scalable method for preparing catalysts with optimized electronic states and enhanced performance, guiding their design to combat antibiotic resistance.