Cu-optimized long-range interaction between Co nanoparticles and Co single atoms:Improved Fenton-like reaction activity

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外文摘要：The interplay between multi-atom assembly configurations and single atoms(SAs)has been gaining attention in research.However,the effect of long-term range interactions between SAs and multi-atom assemblies on the orbital filling characteristics has yet to be investigated.In this context,we introduced copper(Cu)doping to strengthen the interaction between cobalt(Co)nanoparticles(NPs)and Co SAs by promoting the spontaneous formation of Co-Cu alloy NPs that tends toward aggregation owing to its neg-ative cohesive energy(-0.06454),instead of forming Cu SAs.The incorporation of Cu within the Co-Cu alloy NPs,compared to the pure Co NPs,significantly expedites the kinetics of peroxymonosulfate(PMS)oxidation processes on Co SAs.Unlike Co NPs,Co-Cu NPs facilitate electron rearrangement in the d orbi-tals(especially dz2 and dxz)near the Fermi level in Co SAs,thereby optimizing the dz2-O(PMS)and dxz-O(SO5)orbital interaction.Eventually,the Co-Cu alloy NPs embedded in nitrogen-doped carbon(CC@CNC)catalysts rapidly eliminated 80.67％of 20 mg L-1 carbamazepine(CBZ)within 5 min.This performance significantly surpasses that of catalysts consisting solely of Co NPs in a similar matrix(C@CNC),which achieved a 58.99％reduction in 5 min.The quasi in situ characterization suggested that PMS acts as an electron donor and will transfer electrons to Co SAs,generating 1O2 for contaminant abatement.This study offers valuable insights into the mechanisms by which composite active sites formed through multi-atom assembly interact at the atomic orbital level to achieve high-efficiency PMS-based advanced oxidation processes at the atomic orbital level.

外文关键词：

Spontaneous alloyingCo-Cu alloy NPsCo SAsSynergismOrbital electron filling

作者：

Fan Mo、Zelin Hou、Qixing Zhou、Xixi Chen、Weitao Liu、Wendan Xue、Qi Wang、Jianling Wang、Tong Zheng、Zongxin Tao

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作者单位：

Key Laboratory of Pollution Processes and Environmental Criteria(Ministry of Education)/Tianjin Key Laboratory of Environmental Remediation and Pollution Control,Carbon Neutrality Interdisciplinary Science Center,College of Environmental Science and Engineering,Nankai University,Tianjin 300350,China

National Engineering Research Center of Pesticide,Nankai University,Tianjin 300350,China

基金：

Ministry of Science and Technology of People's Republic of China as a Key Technology Research and Development Program ProjecMinistry of Science and Technology of People's Republic of China as a Key Technology Research and Development Program ProjecMinistry of Education of People's Republic of China as a Discipline Innovation and Intelligence Introduction ProjectNational Natural Science Foundation of China as a Shandong Joint Fund ProjectTianjin Science and Technology Bureau as a Key Science and Technology Supporting ProjectApplied Chemistry and Engineering Institute(Nankai University)

项目编号：

2023YFC37090012019YFC1804104B17025U190622219YFZCSF00920JEM-ARM200F

出版年：

2024

DOI：

10.1016/j.scib.2024.05.002

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(16)