超低密度的单原子钴位点高效去除抗生素

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中文摘要：单原子位点催化剂(SSCs)由于能够产生丰富的活性物质来清除类芬顿体系中的污染物,而显示出广阔的潜力.然而,在高级氧化工艺中,实现金属原子100％的利用率和减少金属浸出以满足环境安全标准是困难的.在此基础上,利用强极化力获得了 Co原子含量极低(～0.17％)的催化剂,提高了金属原子利用率,降低了抗生素消除过程中金属浸出的风险.正如预期,该催化剂具有有限的Co位点,伴随着丰富的缺陷和大量从大孔到中孔再到微孔分布的骨架,实现了快速的四环素降解(0.07133 min-1)和优异的归一化速率常数(kper-site,2.4726 × 105 min-1 M-1).实验和理论结果均表明,充分暴露具有丰富C-N缺陷的Co位点,可以提高Co活性位点的电子密度,降低过硫酸盐(PDS)的吸附能,从而优化Co原子对PDS活化的利用.该研究为设计高性能、环境友好的水修复用SSCs提供了有价值的见解.

外文标题：Engineering ultra-low density and fully exposed atomic cobalt sites for antibiotics removal

外文摘要：Single atom site catalysts(SSCs)have exhibited broad potential due to their ability to produce abundant active species for the eradication of contaminants in Fenton-like system.However,it is difficult to realize 100％metal atom utilization and reduce metal leaching to meet environmental safety standards in advanced oxidation processes.Herein,the catalysts with ultralow atomic Co site contents(～0.17％)are obtained by strong polar force to increase metal atom utili-zation and reduce the risk of metal leaching during the elim-ination of antibiotics.As expected,the catalysts with limited Co sites accompanied by abundant defects and numerous open-framework pores distributed from macropores to me-sopores and to micropores,achieve the rapid tetracycline de-gradation(0.07133 min-1)and an excellent normalized rate constant(kper-site,2.4726 × 105 min-1 M-1).Both the experi-mental and theoretical results perform that fully exposed Co sites with abundant C-N defects can increase the electronic density of Co active sites and decrease the peroxydisulfate(PDS)adsorption energy,thereby optimizing Co atom utili-zation for PDS activation.This study may provide valuable insights into the design of high performance and en-vironmentally safe SSCs for water restoration.

外文关键词：

single atom site catalystantibioticsultralow-content Co site catalystadvanced oxidation processes(AOPs)reactive oxygen species

作者：

葛骁、王杰、周冬琴、王小治、吴宇恩

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作者单位：

College of Environmental Science and Engineering,Yangzhou University,Yangzhou 225000,China

Department of Chemistry,Hefei National Laboratory for Physical Sciences at the Microscale,iChEM(Collaborative Innovation Center of Chemistry for Energy Materials),University of Science and Technology of China,Hefei 230026,China

关键词：

single atom site catalyst antibiotics ultralow-content Co site catalyst advanced oxidation processes(AOPs) reactive oxygen species

基金：

National Natural Science Foundation of ChinaQing Lan Project,the 333 Project of Jiangsu ProvinceSix Talent Peaks Project in Jiangsu ProvinceLvyang Jinfeng Fund of YangzhouResearch Foundation of Yangzhou UniversityDoctor of Mass Entrepreneurship and Innovation of Jiangsu ProvinceInnovation Fostering Fund of Yangzhou University

项目编号：

41977085BRA2020302018-TD-JNHB-012137012724137012446337090323

出版年：

2024

DOI：

10.1007/s40843-024-2979-6

中国科学:材料科学(英文)

CSTPCD

ISSN：

年,卷(期)：2024.67(7)