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(k per-site,2.4726×10^(5) 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.
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 utilization and reduce the risk of metal leaching during the elimination of antibiotics.As expected,the catalysts with limited Co sites accompanied by abundant defects and numerous open-framework pores distributed from macropores to mesopores and to micropores,achieve the rapid tetracycline degradation(0.07133 min^(−1))and an excellent normalized rate constant(kper-site,2.4726×10^(5) min^(−1) M^(−1)).Both the experimental 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 utilization for PDS activation.This study may provide valuable insights into the design of high performance and environmentally safe SSCs for water restoration.
作者
葛骁
王杰
周冬琴
王小治
吴宇恩
Xiao Ge;Jie Wang;Dongqin Zhou;Xiaozhi Wang;Yuen Wu(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)
基金
supported by the National Natural Science Foundation of China(41977085)
the Qing Lan Project,the 333 Project of Jiangsu Province(BRA202030)
the Six Talent Peaks Project in Jiangsu Province(2018-TD-JNHB-012)
the Lvyang Jinfeng Fund of Yangzhou(137012724)
the Research Foundation of Yangzhou University(137012446)
Doctor of Mass Entrepreneurship and Innovation of Jiangsu Province(337090323)
the Innovation Fostering Fund of Yangzhou University.
