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DOI	10.1073/pnas.2105628118
	Atomically dispersed Fe atoms anchored on S and N-codoped carbon for efficient electrochemical denitrification
	Li J.; Li M.; An N.; Zhang S.; Song Q.; Yang Y.; Liu X.
发表日期	2021
ISSN	0027-8424
卷号	118 期号:33
英文摘要	Nitrate, a widespread contaminant in natural water, is a threat to ecological safety and human health. Although direct nitrate removal by electrochemical methods is efficient, the development of low-cost electrocatalysts with high reactivity remains challenging. Herein, bi-functional single-atom catalysts (SACs) were prepared with Cu or Fe active centers on an N-doped or S, N-codoped carbon basal plane for N2 or NH4+ production. The maximum nitrate removal capacity was 7,822 mg N · g−1 Fe, which was the highest among previous studies. A high ammonia Faradic efficiency (78.4%) was achieved at a low potential (−0.57 versus reversible hydrogen electrode), and the nitrogen selectivity was 100% on S-modified Fe SACs. Theoretical and experimental investigations of the S-doping charge-transfer effect revealed that strong metal-support interactions were beneficial for anchoring single atoms and enhancing cyclability. S-doping altered the coordination environment of single-atom centers and created numerous defects with higher conductivity, which played a key role in improving the catalyst activity. Moreover, interactions between defects and single-atom sites improved the catalytic performance. Thus, these findings offer an avenue for high active SAC design. © 2021 National Academy of Sciences. All rights reserved.
英文关键词	Catalyst; Electrochemistry; Nitrates; Single atom
语种	英语
scopus关键词	ammonia; carbon; iron; nitrate; nitrogen; sulfur; Article; catalysis; catalyst; denitrification; density functional theory; electric conductivity; electrochemical denitrification; electrochemistry; electron spin resonance; energy dispersive X ray spectroscopy; extended X ray absorption fine structure spectroscopy; nitrate electroreduction; single atom catalyst; structure activity relation; transmission electron microscopy; X ray absorption near edge structure spectroscopy; X ray absorption spectroscopy
来源期刊	Proceedings of the National Academy of Sciences of the United States of America
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/238431
作者单位	School of Environment, Tsinghua University, Beijing, 100084, China
推荐引用方式 GB/T 7714	Li J.,Li M.,An N.,et al. Atomically dispersed Fe atoms anchored on S and N-codoped carbon for efficient electrochemical denitrification[J],2021,118(33).
APA	Li J..,Li M..,An N..,Zhang S..,Song Q..,...&Liu X..(2021).Atomically dispersed Fe atoms anchored on S and N-codoped carbon for efficient electrochemical denitrification.Proceedings of the National Academy of Sciences of the United States of America,118(33).
MLA	Li J.,et al."Atomically dispersed Fe atoms anchored on S and N-codoped carbon for efficient electrochemical denitrification".Proceedings of the National Academy of Sciences of the United States of America 118.33(2021).