Electrocatalytic Generation of Singlet Oxygen via ROS-Mediated Redox Chain Reaction for Efficient Disinfection.

Shi, Hao; Wu, Tianming; Duan, Meilin; Yu, Jinping; Liu, Miao; Wen, Xueyun; Wang, Lupeng; Xu, Yuanhong · Nano Lett · 2024

basic_science · Level V

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Abstract

The risk of harmful microorganisms to ecosystems and human health has stimulated exploration of singlet oxygen (<sup>1</sup>O<sub>2</sub>)-based disinfection. It can be potentially generated via an electrocatalytic process, but is limited by the low production yield and unclear intermediate-mediated mechanism. Herein, we designed a two-site catalyst (Fe/Mo-N/C) for the selective <sup>1</sup>O<sub>2</sub> generation. The Mo sites enhance the generation of <sup>1</sup>O<sub>2</sub> precursors (H<sub>2</sub>O<sub>2</sub>), accompanied by the generation of intermediate <sup>•</sup>HO<sub>2</sub>/<sup>•</sup>O<sub>2</sub><sup>-</sup>. The Fe site facilitates activation of H<sub>2</sub>O<sub>2</sub> into <sup>•</sup>OH, which accelerates the <sup>•</sup>HO<sub>2</sub>/<sup>•</sup>O<sub>2</sub><sup>-</sup> into <sup>1</sup>O<sub>2</sub>. A possible mechanism for promoting <sup>1</sup>O<sub>2</sub> production through the ROS-mediated chain reaction is reported. The as-developed electrochemical disinfection system can kill 1 × 10<sup>7</sup> CFU mL<sup>-1</sup> of <i>E. coli</i> within 8 min, leading to cell membrane damage and DNA degradation. It can be effectively applied for the disinfection of medical wastewater. This work provides a general strategy for promoting the production of <sup>1</sup>O<sub>2</sub> through electrocatalysis and for efficient electrochemical disinfection.

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