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Electrocatalytically Active Fe-(O-C-2)(4) Single-Atom Sites for Efficient Reduction of Nitrogen to Ammonia
Zhang, Shengbo1,2; Jin, Meng1,2; Shi, Tongfei1; Han, Miaomiao1; Sun, Qiao3; Lin, Yue4; Ding, Zhenhua5; Zheng, Li Rong6; Wang, Guozhong1; Zhang, Yunxia1; Zhang, Haimin1; Zhao, Huijun1,7
2020-05-27
Source PublicationANGEWANDTE CHEMIE-INTERNATIONAL EDITION
ISSN1433-7851
Corresponding AuthorLin, Yue(linyue@ustc.edu.cn) ; Zhang, Haimin(zhanghm@issp.ac.cn) ; Zhao, Huijun(h.zhao@griffith.edu.au)
AbstractSingle-atom catalysts have demonstrated their superiority over other types of catalysts for various reactions. However, the reported nitrogen reduction reaction single-atom electrocatalysts for the nitrogen reduction reaction exclusively utilize metal-nitrogen or metal-carbon coordination configurations as catalytic active sites. Here, we report a Fe single-atom electrocatalyst supported on low-cost, nitrogen-free lignocellulose-derived carbon. The extended X-ray absorption fine structure spectra confirm that Fe atoms are anchored to the support via the Fe-(O-C-2)(4) coordination configuration. Density functional theory calculations identify Fe-(O-C-2)(4) as the active site for the nitrogen reduction reaction. An electrode consisting of the electrocatalyst loaded on carbon cloth can afford a NH3 yield rate and faradaic efficiency of 32.1 mu g h(-1) mg(cat.)(-1) (5350 mu g h(-1) mg(Fe)(-1)) and 29.3 %, respectively. An exceptional NH3 yield rate of 307.7 mu g h(-1) mg(cat.)(-1) (51 283 mu g h(-1) mg(Fe)(-1)) with a near record faradaic efficiency of 51.0 % can be achieved with the electrocatalyst immobilized on a glassy carbon electrode.
Keywordammonia electrocatalysis nitrogen reduction single-atom catalysts
DOI10.1002/anie.202005930
WOS KeywordCATALYSTS ; N-2 ; WATER ; ELECTROSYNTHESIS ; TEMPERATURE ; COMPOSITES ; CONVERSION ; FIXATION ; CARBON ; IRON
Indexed BySCI
Language英语
Funding ProjectNatural Science Foundation of China[51432009] ; Natural Science Foundation of China[11874334] ; Natural Science Foundation of China[51872292] ; Youth Innovation Promotion Association of Chinese Academy of Sciences[2020458] ; CAS/SAFEA International Partnership Program for Creative Research Teams of Chinese Academy of Sciences, China
Funding OrganizationNatural Science Foundation of China ; Youth Innovation Promotion Association of Chinese Academy of Sciences ; CAS/SAFEA International Partnership Program for Creative Research Teams of Chinese Academy of Sciences, China
WOS Research AreaChemistry
WOS SubjectChemistry, Multidisciplinary
WOS IDWOS:000535558200001
PublisherWILEY-V C H VERLAG GMBH
Citation statistics
Cited Times:34[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.hfcas.ac.cn:8080/handle/334002/103226
Collection中国科学院合肥物质科学研究院
Corresponding AuthorLin, Yue; Zhang, Haimin; Zhao, Huijun
Affiliation1.Chinese Acad Sci, Ctr Environm & Energy Nanomat, Anhui Key Lab Nanomat & Nanotechnol,Key Lab Mat P, CAS Ctr Excellence Nanosci,Inst Solid State Phys, Hefei 230031, Anhui, Peoples R China
2.Univ Sci & Technol China, Hefei 230031, Anhui, Peoples R China
3.Soochow Univ, Collaborat Innovat Ctr Radiat Med Jiangsu Higher, Sch Radiol & Interdisciplinary Sci, State Key Lab Radiat Med & Protect, Suzhou 215123, Peoples R China
4.Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Peoples R China
5.Anhui Inst Prod Qual Supervis & Inspect, Hefei 230026, Peoples R China
6.Chinese Acad Sci, Inst High Energy Phys, Beijing Synchrotron Radiat Facil, 19B Yuquan Rd, Beijing 100049, Peoples R China
7.Griffith Univ, Ctr Clean Environm & Energy Energy, Gold Coast Campus, Gold Coast, Qld 4222, Australia
Recommended Citation
GB/T 7714
Zhang, Shengbo,Jin, Meng,Shi, Tongfei,et al. Electrocatalytically Active Fe-(O-C-2)(4) Single-Atom Sites for Efficient Reduction of Nitrogen to Ammonia[J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2020.
APA Zhang, Shengbo.,Jin, Meng.,Shi, Tongfei.,Han, Miaomiao.,Sun, Qiao.,...&Zhao, Huijun.(2020).Electrocatalytically Active Fe-(O-C-2)(4) Single-Atom Sites for Efficient Reduction of Nitrogen to Ammonia.ANGEWANDTE CHEMIE-INTERNATIONAL EDITION.
MLA Zhang, Shengbo,et al."Electrocatalytically Active Fe-(O-C-2)(4) Single-Atom Sites for Efficient Reduction of Nitrogen to Ammonia".ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2020).
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