Support work-function dependent Fenton-like catalytic activity of Co single atoms for selective cobalt(Ⅳ)=O generation

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外文标题：Support work-function dependent Fenton-like catalytic activity of Co single atoms for selective cobalt(Ⅳ)=O generation

外文摘要：In Fenton-like reactions,high-valent cobalt-oxo(CoⅣ=O)has attracted increasing interests due to high redox potential,long lifetime,and anti-interference properties,but its generation is hindered by the elec-tron repulsion between the electron rich oxo-and cobalt centers.Here,we demonstrate CoⅣ-O genera-tion from peroxymonosulfate(PMS)activation over cobalt single-atom catalysts(Co-SACs)using in-situ Co K-edge X-ray absorption spectra,and discern that CoⅣ-O generation is dependent on the support work-function(WF)due to the strong electronic metal-support interaction(EMSI).Supports with a high WF value like anatase-TiO2 facilitate the binding of PMS-terminal oxo-ligand to Co sites by extracting Co-d electrons,thus decreasing the generation barrier for the critical intermediate(Co-OOSO2-).The Co atoms anchored on anatase-TiO2(Co-TiO2)exhibited enhanced CoⅣ=O generation and superior activity for sulfamethoxazole(SMX)degradation during PMS activation.The normalized steady-state concentra-tion of CoⅣ=O in Co-TiO2/PMS system was three orders of magnitude higher than that of free radicals,and 1.3-to 11-fold higher than that generated in other Co-SACs/PMS systems.Co-TiO2/PMS sustained effi-cient removal of SMX with minimal Co2*leaching under continuous flow operation,suggesting its attrac-tive water purification potential.Overall,these results underscore the significance of support selection for enhanced generation of high-valent metal-oxo species and efficient PMS activation in supported metal SACs.

外文关键词：

Peroxymonosulfate activationElectronic metal-support interactionSingle-atom catalystsHigh-valent cobalt-oxoWork-function

作者：

Xue Li、Xiangcheng Zhang、Junyu Lang、Baoxue Zhou、Pedro J.J.Alvarez、Lizhi Zhang、Mingce Long

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作者单位：

School of Environmental Science and Engineering,Shanghai Jiao Tong University,Shanghai 200240,China

School of Physical Science and Technology,ShanghaiTech University,Shanghai 201210,China

Department of Civil and Environmental Engineering,Rice University,Houston,TX 77005,USA

关键词：

Peroxymonosulfate activation Electronic metal-support interaction Single-atom catalysts High-valent cobalt-oxo Work-function

出版年：

2024

DOI：

10.1016/j.scib.2024.09.046

科学通报(英文版)

中国科学院

科学通报(英文版)

CSTPCD

ISSN：1001-6538

年,卷(期)：2024.69(24)