Unraveling the High-Activity Origin of Single-Atom Iron Catalysts for Organic Pollutant Oxidation via Peroxymonosulfate Activation
文献类型:期刊论文
作者 | Gao, Yaowen; Zhu, Yue; Li, Tong; Chen, Zhenhuan; Jiang, Qike; Zhao, Zhiyu; Liang, Xiaoying; Hu, Chun |
刊名 | ENVIRONMENTAL SCIENCE & TECHNOLOGY
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出版日期 | 2021-06-15 |
卷号 | 55期号:12页码:8318-8328 |
关键词 | single-atom catalysts organic pollutant oxidation electronic polarization PMS reduction and oxidation electron migration |
ISSN号 | 0013-936X |
英文摘要 | Single-atom catalysts (SACs) have emerged as efficient materials in the elimination of aqueous organic contaminants; however, the origin of high activity of SACs still remains elusive. Herein, we identify an 8.1-fold catalytic specific activity (reaction rate constant normalized to catalyst's specific surface area and dosage) enhancement that can be fulfilled with a single-atom iron catalyst (SA-Fe-NC) prepared via a cascade anchoring method compared to the iron nanoparticle-loaded catalyst, resulting in one of the most active currently known catalysts in peroxymonosulfate (PMS) conversion for organic pollutant oxidation. Experimental data and theoretical results unraveled that the high-activity origin of the SA-Fe-NC stems from the Fe-pyridinic N-4 moiety, which dramatically increases active sites by not only creating the electronrich Fe single atom as the catalytic site but also producing electron- poor carbon atoms neighboring pyridinic N as binding sites for PMS activation including synchronous PMS reduction and oxidation together with dissolved oxygen reduction. Moreover, the SA-Fe-NC exhibits excellent stability and applicability to realistic industrial wastewater remediation. This work offers a novel yet reasonable interpretation for why a small amount of iron in the SA-Fe-NC can deliver extremely superior specific activity in PMS activation and develops a promising catalytic oxidation system toward actual environmental cleanup. |
WOS研究方向 | Engineering, Environmental ; Environmental Sciences |
源URL | [http://ir.rcees.ac.cn/handle/311016/46275] ![]() |
专题 | 生态环境研究中心_中国科学院饮用水科学与技术重点实验室 |
作者单位 | 1.Chinese Acad Sci, Res Ctr Ecoenvironm Sci, Key Lab Drinking Water Sci & Technol, Beijing 100085, Peoples R China 2.Guangzhou Univ, Inst Environm Res Greater Bay, Key Lab Water Qual & Conservat Pearl River Delta, Minist Educ, Guangzhou 510006, Peoples R China 3.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China |
推荐引用方式 GB/T 7714 | Gao, Yaowen,Zhu, Yue,Li, Tong,et al. Unraveling the High-Activity Origin of Single-Atom Iron Catalysts for Organic Pollutant Oxidation via Peroxymonosulfate Activation[J]. ENVIRONMENTAL SCIENCE & TECHNOLOGY,2021,55(12):8318-8328. |
APA | Gao, Yaowen.,Zhu, Yue.,Li, Tong.,Chen, Zhenhuan.,Jiang, Qike.,...&Hu, Chun.(2021).Unraveling the High-Activity Origin of Single-Atom Iron Catalysts for Organic Pollutant Oxidation via Peroxymonosulfate Activation.ENVIRONMENTAL SCIENCE & TECHNOLOGY,55(12),8318-8328. |
MLA | Gao, Yaowen,et al."Unraveling the High-Activity Origin of Single-Atom Iron Catalysts for Organic Pollutant Oxidation via Peroxymonosulfate Activation".ENVIRONMENTAL SCIENCE & TECHNOLOGY 55.12(2021):8318-8328. |
入库方式: OAI收割
来源:生态环境研究中心
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