题名 | Atomically-precise dopant-controlled single cluster catalysis for electrochemical nitrogen reduction |
作者 | Yao,Chuanhao1,2; Guo,Na3; Xi,Shibo4; Xu,Cong Qiao5 ![]() ![]() ![]() ![]() ![]() ![]() ![]() ![]() ![]() ![]() ![]() ![]() |
通讯作者 | Li,Jun; Zhang,Chun; Du,Yonghua; Lu,Jiong; Li,Jun; Zhang,Chun; Du,Yonghua; Lu,Jiong |
共同第一作者 | Yao,Chuanhao; Guo,Na; Xi,Shibo; Xu,Cong Qiao; Yao,Chuanhao; Guo,Na; Xi,Shibo; Xu,Cong Qiao |
发表日期 | 2020-12-01
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DOI | |
发表期刊 | |
ISSN | 2041-1723
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EISSN | 2041-1723
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卷号 | 11期号:1 |
摘要 | The ability to precisely engineer the doping of sub-nanometer bimetallic clusters offers exciting opportunities for tailoring their catalytic performance with atomic accuracy. However, the fabrication of singly dispersed bimetallic cluster catalysts with atomic-level control of dopants has been a long-standing challenge. Herein, we report a strategy for the controllable synthesis of a precisely doped single cluster catalyst consisting of partially ligand-enveloped AuPt clusters supported on defective graphene. This creates a bimetal single cluster catalyst (AuPt/G) with exceptional activity for electrochemical nitrogen (N) reduction. Our mechanistic study reveals that each N molecule is activated in the confined region between cluster and graphene. The heteroatom dopant plays an indispensable role in the activation of N via an enhanced back donation of electrons to the N LUMO. Moreover, besides the heteroatom Pt, the catalytic performance of single cluster catalyst can be further tuned by using Pd in place of Pt as the dopant. |
相关链接 | [Scopus记录] |
收录类别 | |
语种 | 英语
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重要成果 | NI论文
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学校署名 | 通讯
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资助项目 | MOE[MOE2017-T2-1-056][R-143000-B47-114]
; NUS Flagship Green Energy Program[R-143-000-A55-646]
; Natural Science Foundation of China[21601193][21703143]
; Fundamental Research Funds for the Central Universities[31020190QD013]
; NUS[R-143-000-A63-114][R-144-000-410-114]
; National Natural Science Foundation of China[21590792][91645203][21521091]
; U.S. DOE[DE-AC02-06CH11357]
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WOS研究方向 | Science & Technology - Other Topics
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WOS类目 | Multidisciplinary Sciences
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WOS记录号 | WOS:000569891500016
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出版者 | |
Scopus记录号 | 2-s2.0-85090046271
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来源库 | Scopus
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引用统计 |
被引频次[WOS]:117
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成果类型 | 期刊论文 |
条目标识符 | http://sustech.caswiz.com/handle/2SGJ60CL/153666 |
专题 | 理学院_化学系 工学院_材料科学与工程系 |
作者单位 | 1.Department of Chemistry,National University of Singapore,Singapore,3 Science Drive 3,117543,Singapore 2.Frontiers Science Center for Flexible Electronics (FSCFE),Shaanxi Institute of Flexible Electronics (SIFE) & Shaanxi Institute of Biomedical Materials and Engineering (SIBME),Northwestern Polytechnical University (NPU),Xi’an,127 West Youyi Road,710072,China 3.Department of Physics,National University of Singapore,Singapore,2 Science Drive 3,117542,Singapore 4.Institute of Chemical and Engineering Sciences,Jurong Island,1 Pesek Road,627833,Singapore 5.Department of Chemistry,Southern University of Science and Technology,Shenzhen,518055,China 6.Centre for Advanced 2D Materials and Graphene Research Centre,National University of Singapore,Singapore,117546,Singapore 7.NUS Graduate School for Integrative Sciences and Engineering,National University of Singapore,Singapore,28 Medical Drive,117456,Singapore 8.Department of Materials Science & Engineering,National University of Singapore,Singapore,9 Engineering Drive 1,117575,Singapore 9.School of Chemical and Biomedical Engineering,Nanyang Technological University,Singapore,Singapore 10.SZU-NUS Collaborative Centre and International Collaborative Laboratory of 2D Materials for Optoelectronic Science & Technology,College of Optoelectronic Engineering,Shenzhen University,Shenzhen,518060,China 11.Advanced Photon Source,Argonne National Laboratory,Argonne,9700 South Cass Avenue,60439,United States 12.Department of Chemistry and Key Laboratory of Organic Optoelectronics & Molecular Engineering of Ministry of Education,Tsinghua University,Beijing,100084,China 13.National Synchrotron Light Source II,Brookhaven National Laboratory,Upton,11973,United States 14.Department of Chemistry,National University of Singapore,Singapore,3 Science Drive 3,117543,Singapore 15.Frontiers Science Center for Flexible Electronics (FSCFE),Shaanxi Institute of Flexible Electronics (SIFE) & Shaanxi Institute of Biomedical Materials and Engineering (SIBME),Northwestern Polytechnical University (NPU),Xi’an,127 West Youyi Road,710072,China 16.Department of Physics,National University of Singapore,Singapore,2 Science Drive 3,117542,Singapore 17.Institute of Chemical and Engineering Sciences,Jurong Island,1 Pesek Road,627833,Singapore 18.Department of Chemistry,Southern University of Science and Technology,Shenzhen,518055,China 19.Centre for Advanced 2D Materials and Graphene Research Centre,National University of Singapore,Singapore,117546,Singapore 20.NUS Graduate School for Integrative Sciences and Engineering,National University of Singapore,Singapore,28 Medical Drive,117456,Singapore 21.Department of Materials Science & Engineering,National University of Singapore,Singapore,9 Engineering Drive 1,117575,Singapore 22.School of Chemical and Biomedical Engineering,Nanyang Technological University,Singapore,Singapore 23.SZU-NUS Collaborative Centre and International Collaborative Laboratory of 2D Materials for Optoelectronic Science & Technology,College of Optoelectronic Engineering,Shenzhen University,Shenzhen,518060,China 24.Advanced Photon Source,Argonne National Laboratory,Argonne,9700 South Cass Avenue,60439,United States 25.Department of Chemistry and Key Laboratory of Organic Optoelectronics & Molecular Engineering of Ministry of Education,Tsinghua University,Beijing,100084,China 26.National Synchrotron Light Source II,Brookhaven National Laboratory,Upton,11973,United States |
通讯作者单位 | 化学系 |
推荐引用方式 GB/T 7714 |
Yao,Chuanhao,Guo,Na,Xi,Shibo,et al. Atomically-precise dopant-controlled single cluster catalysis for electrochemical nitrogen reduction[J]. Nature Communications,2020,11(1).
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APA |
Yao,Chuanhao.,Guo,Na.,Xi,Shibo.,Xu,Cong Qiao.,Liu,Wei.,...&Lu,Jiong.(2020).Atomically-precise dopant-controlled single cluster catalysis for electrochemical nitrogen reduction.Nature Communications,11(1).
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MLA |
Yao,Chuanhao,et al."Atomically-precise dopant-controlled single cluster catalysis for electrochemical nitrogen reduction".Nature Communications 11.1(2020).
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