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题名

Atomically-precise dopant-controlled single cluster catalysis for electrochemical nitrogen reduction

作者
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
DOI
发表期刊
ISSN
2041-1723
EISSN
2041-1723
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.

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英语
重要成果
NI论文
学校署名
通讯
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]
WOS研究方向
Science & Technology - Other Topics
WOS类目
Multidisciplinary Sciences
WOS记录号
WOS:000569891500016
出版者
Scopus记录号
2-s2.0-85090046271
来源库
Scopus
引用统计
被引频次[WOS]:117
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).
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).
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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