Electron Transfer Expressway from Peroxydisulfate to O2 Mediated by Diatomic Sites Accelerating 1O2 Production for Disinfection

作者：Wei Qi, Xiaodan Tang, Yan Huang, Shuanglong Ma, Jingzhen Wang, Boqiang Gao, Jiale Pang, Jinge Du, Pengfei Wang, Sihui Zhan, Bing‐Jie Ni, Shengjun Xu · 发表于：Environmental Science & Technology · 年份：2025 · DOI：10.1021/acs.est.5c01975 · 被引用次数：22 · 研究领域：Advanced oxidation water treatment、Water Treatment and Disinfection、Electrochemical Analysis and Applications

Current studies on high-density single-atom catalysts (SACs) with the coexistence of single atomic and diatomic sites have ignored the underlying contribution of diatomic sites for persulfate-based disinfection technology. Herein, high-density atomic Ni anchored on N -doped carbon (Ni 1 –NC) containing abundant Ni diatomic (Ni 2 –N 6 ) sites, was fabricated, exhibiting superior peroxydisulfate (PDS) activation to generate singlet oxygen ( 1 O 2 ) for disinfection compared with other M 1 –NC, due to the fact that Ni 1 –NC possessed the highest negative crystal orbital Hamilton population value. A dynamic promotion effect toward disinfection, relying on the level of external O 2 was discovered. This promotion effect was achieved through the cooperation of PDS and O 2 which was mediated by Ni 2 –N 6 sites bridging electron transfer from PDS to O 2, thereby suppressing the energy barriers of rate-determining steps. Disinfection with decreased horizontal gene transfer was achieved by disrupting coenzyme Q, inhibiting adenosine triphosphate synthesis, and degrading extracellular polymeric substances via 1 O 2 . A continuous flow system based on a Ni 1 –NC@sponge fixed reaction bed displayed persistent disinfection for 336 h under aeration. This work presents a transboundary integrated PDS disinfection strategy combining physical aeration and chemical oxidation through tailoring diatomic sites in SACs.