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Role of curvature in modulating electronic structure of active sites on hollow carbon spheres for efficient decontamination in catalytic ozonation process

Journal 2025 · IF 21.1 · 发表于 2025 年 1 月 15 日
作者: Lanlan Liang,Peike Cao,Haokun Bai,Xiaojun Du,Shuo Chen,Hongtao Yu,Yanming Liu,Yan Su,Xie Quan
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摘要

The decontamination performance of heterogeneous catalytic ozonation catalysts is limited due to low electron transfer between active sites and O 3 . Herein, we modulated the electronic state of metal sites by coating copper oxides on hollow carbon (CuO x -HNC) with different spherical curvatures. CuO x -HNC with larger curvature exhibited more hydroxyl radical generation and higher degradation performance of sulfamethoxazole, achieving 60 % mineralization efficiency within 90 min. Experimental and theoretical results revealed that high curvature of hollow carbon induced a shift of π-electron density from concave to convex forming electron-rich exterior surface, which strengthened orbital overlap between Cu 3d and O 2p, consequently accelerating the electron transfer from Cu to O 3 . CuO x -HNC exhibited efficient decontamination performance for pharmaceutical wastewater in a continuous-flow reactor with COD reducing from 105 mg L −1 to below 50 mg L −1 . This study offered a valuable strategy to modify the electronic structure of catalysts for efficient wastewater decontamination.

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