催化作用
过氧化物
离解(化学)
钴
吸附
介孔二氧化硅
浸出(土壤学)
介孔材料
化学
化学工程
污染物
密度泛函理论
材料科学
光化学
纳米技术
无机化学
物理化学
有机化学
计算化学
土壤科学
土壤水分
工程类
环境科学
作者
Xiaowen Xie,Mingshan Zhu,Fei Xiao,Yongjie Xiang,Huanran Zhong,Zhimin Ao,Haibao Huang
出处
期刊:JACS Au
[American Chemical Society]
日期:2023-04-27
卷期号:3 (5): 1496-1506
被引量:1
标识
DOI:10.1021/jacsau.3c00147
摘要
The construction of highly active catalysts presents great prospects, while it is a challenge for peroxide activation in advanced oxidation processes (AOPs). Herein, we facilely developed ultrafine Co clusters confined in mesoporous silica nanospheres containing N-doped carbon (NC) dots (termed as Co/NC@mSiO2) via a double-confinement strategy. Compared with the unconfined counterpart, Co/NC@mSiO2 exhibited unprecedented catalytic activity and durability for removal of various organic pollutants even in extremely acidic and alkaline environments (pH from 2 to 11) with very low Co ion leaching. Experiments and density functional theory (DFT) calculations proved that Co/NC@mSiO2 possessed strong peroxymonosulphate (PMS) adsorption and charge transfer capability, enabling the efficient O-O bond dissociation of PMS to HO• and SO4•- radicals. The strong interaction between Co clusters and mSiO2 containing NC dots contributed to excellent pollutant degradation performances by optimizing the electronic structures of Co clusters. This work represents a fundamental breakthrough in the design and understanding of the double-confined catalysts for peroxide activation.
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