超低密度的单原子钴位点高效去除抗生素
Engineering ultra-low density and fully exposed atomic cobalt sites for antibiotics removal
葛骁 1王杰 1周冬琴 1王小治 1吴宇恩2
作者信息
- 1. College of Environmental Science and Engineering,Yangzhou University,Yangzhou 225000,China
- 2. 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
- 折叠
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.
Abstract
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.
关键词
single atom site catalyst/antibiotics/ultralow-content Co site catalyst/advanced oxidation processes(AOPs)/reactive oxygen speciesKey words
single atom site catalyst/antibiotics/ultralow-content Co site catalyst/advanced oxidation processes(AOPs)/reactive oxygen species引用本文复制引用
基金项目
National Natural Science Foundation of China(41977085)
Qing Lan Project,the 333 Project of Jiangsu Province(BRA202030)
Six Talent Peaks Project in Jiangsu Province(2018-TD-JNHB-012)
Lvyang Jinfeng Fund of Yangzhou(137012724)
Research Foundation of Yangzhou University(137012446)
Doctor of Mass Entrepreneurship and Innovation of Jiangsu Province(337090323)
Innovation Fostering Fund of Yangzhou University()
出版年
2024
NETL
NSTL
万方数据