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Turning Carbon Atoms into Highly Active Oxygen Reduction Reaction Electrocatalytic Sites in Nitrogen-Doped Graphene-Coated Co@Ag
Li, Mengsi1,2; Wang, Changlai1,2; Yang, Yang1,2; Jiang, Peng1,2; Lin, Zhiyu1,2; Xia, Guoliang1,2; Yang, Kang1,2; Xu, Pengping1,2; Chen, Qianwang1,2,3
2018-11-05
发表期刊ACS SUSTAINABLE CHEMISTRY & ENGINEERING
ISSN2168-0485
卷号6期号:11页码:14033-14041
通讯作者Chen, Qianwang(cqw@ustc.edu.cn)
摘要In recent years, 3d transition metals or alloys encapsulated by graphene layers (M@NG) have been emerging as prospective electrocatalysts especially for hydrogen evolution reactions (HERs) and oxygen evolution reactions (OERs). However, this strategy is limited in preparation of high-performance oxygen reduction reaction (ORR) catalysts. Herein we prepared Co@Ag bimetallic nanoparticles embedded in nitrogen rich graphene layers via pyrolysis metal organic frameworks (MOFs). The catalyst displays extraordinarily high ORR performance with a high onset potential of 0.989 V and a half-wave potential of 0.872 V in 0.1 M KOH. Moreover, it shows a superb long-term stability performance after 5000 cycles on account of the carbon layers that protect the material from corrosion as well as high methyl alcohol tolerance under methanol environments. Density functional theory calculations suggest that carbon atoms, which are adjacent to nitrogen dopants in Co@Ag@NC, are active sites for ORR Especially, Ag "mantle" in Co@Ag@NC contributes a great deal to tuning of electronic structure of carbon active sites, thereby promoting the activity of carbon atoms and enhancing ORR kinetics. This unique Co core/Ag mantle structure can boost the overall ORR activity of M@NG while keeping cost-effectiveness due to the very low requirement of Ag content, providing a new insight into design of other efficient electrocatalysts.
关键词Metal-organic frameworks Oxygen reduction reaction Electron transfer Co core/Ag mantle structure Tuning electronic structure
资助者National Natural Science Foundation (NSFC) ; National Natural Science Foundation (NSFC) ; National Natural Science Foundation (NSFC) ; National Natural Science Foundation (NSFC) ; Fundamental Research Funds for the Central Universities ; Fundamental Research Funds for the Central Universities ; Fundamental Research Funds for the Central Universities ; Fundamental Research Funds for the Central Universities ; CAS/SAFEA International Partnership Program for Creative Research Teams ; CAS/SAFEA International Partnership Program for Creative Research Teams ; CAS/SAFEA International Partnership Program for Creative Research Teams ; CAS/SAFEA International Partnership Program for Creative Research Teams ; Hefei Science Center CAS ; Hefei Science Center CAS ; Hefei Science Center CAS ; Hefei Science Center CAS ; National Natural Science Foundation (NSFC) ; National Natural Science Foundation (NSFC) ; National Natural Science Foundation (NSFC) ; National Natural Science Foundation (NSFC) ; Fundamental Research Funds for the Central Universities ; Fundamental Research Funds for the Central Universities ; Fundamental Research Funds for the Central Universities ; Fundamental Research Funds for the Central Universities ; CAS/SAFEA International Partnership Program for Creative Research Teams ; CAS/SAFEA International Partnership Program for Creative Research Teams ; CAS/SAFEA International Partnership Program for Creative Research Teams ; CAS/SAFEA International Partnership Program for Creative Research Teams ; Hefei Science Center CAS ; Hefei Science Center CAS ; Hefei Science Center CAS ; Hefei Science Center CAS ; National Natural Science Foundation (NSFC) ; National Natural Science Foundation (NSFC) ; National Natural Science Foundation (NSFC) ; National Natural Science Foundation (NSFC) ; Fundamental Research Funds for the Central Universities ; Fundamental Research Funds for the Central Universities ; Fundamental Research Funds for the Central Universities ; Fundamental Research Funds for the Central Universities ; CAS/SAFEA International Partnership Program for Creative Research Teams ; CAS/SAFEA International Partnership Program for Creative Research Teams ; CAS/SAFEA International Partnership Program for Creative Research Teams ; CAS/SAFEA International Partnership Program for Creative Research Teams ; Hefei Science Center CAS ; Hefei Science Center CAS ; Hefei Science Center CAS ; Hefei Science Center CAS ; National Natural Science Foundation (NSFC) ; National Natural Science Foundation (NSFC) ; National Natural Science Foundation (NSFC) ; National Natural Science Foundation (NSFC) ; Fundamental Research Funds for the Central Universities ; Fundamental Research Funds for the Central Universities ; Fundamental Research Funds for the Central Universities ; Fundamental Research Funds for the Central Universities ; CAS/SAFEA International Partnership Program for Creative Research Teams ; CAS/SAFEA International Partnership Program for Creative Research Teams ; CAS/SAFEA International Partnership Program for Creative Research Teams ; CAS/SAFEA International Partnership Program for Creative Research Teams ; Hefei Science Center CAS ; Hefei Science Center CAS ; Hefei Science Center CAS ; Hefei Science Center CAS
DOI10.1021/acssuschemeng.8b02573
关键词[WOS]HYDROGEN EVOLUTION REACTION ; REACTION CATALYST ; ALLOY CATALYSTS ; NANOPARTICLES ; STRAIN ; COBALT ; PD ; NANOCRYSTALS ; SPECTROSCOPY ; ENERGY
收录类别SCI
语种英语
资助项目National Natural Science Foundation (NSFC)[21271163] ; National Natural Science Foundation (NSFC)[U1232211] ; National Natural Science Foundation (NSFC)[21571168] ; Fundamental Research Funds for the Central Universities[WK2060140021] ; CAS/SAFEA International Partnership Program for Creative Research Teams ; Hefei Science Center CAS[2016HSC-IU011]
资助者National Natural Science Foundation (NSFC) ; National Natural Science Foundation (NSFC) ; National Natural Science Foundation (NSFC) ; National Natural Science Foundation (NSFC) ; Fundamental Research Funds for the Central Universities ; Fundamental Research Funds for the Central Universities ; Fundamental Research Funds for the Central Universities ; Fundamental Research Funds for the Central Universities ; CAS/SAFEA International Partnership Program for Creative Research Teams ; CAS/SAFEA International Partnership Program for Creative Research Teams ; CAS/SAFEA International Partnership Program for Creative Research Teams ; CAS/SAFEA International Partnership Program for Creative Research Teams ; Hefei Science Center CAS ; Hefei Science Center CAS ; Hefei Science Center CAS ; Hefei Science Center CAS ; National Natural Science Foundation (NSFC) ; National Natural Science Foundation (NSFC) ; National Natural Science Foundation (NSFC) ; National Natural Science Foundation (NSFC) ; Fundamental Research Funds for the Central Universities ; Fundamental Research Funds for the Central Universities ; Fundamental Research Funds for the Central Universities ; Fundamental Research Funds for the Central Universities ; CAS/SAFEA International Partnership Program for Creative Research Teams ; CAS/SAFEA International Partnership Program for Creative Research Teams ; CAS/SAFEA International Partnership Program for Creative Research Teams ; CAS/SAFEA International Partnership Program for Creative Research Teams ; Hefei Science Center CAS ; Hefei Science Center CAS ; Hefei Science Center CAS ; Hefei Science Center CAS ; National Natural Science Foundation (NSFC) ; National Natural Science Foundation (NSFC) ; National Natural Science Foundation (NSFC) ; National Natural Science Foundation (NSFC) ; Fundamental Research Funds for the Central Universities ; Fundamental Research Funds for the Central Universities ; Fundamental Research Funds for the Central Universities ; Fundamental Research Funds for the Central Universities ; CAS/SAFEA International Partnership Program for Creative Research Teams ; CAS/SAFEA International Partnership Program for Creative Research Teams ; CAS/SAFEA International Partnership Program for Creative Research Teams ; CAS/SAFEA International Partnership Program for Creative Research Teams ; Hefei Science Center CAS ; Hefei Science Center CAS ; Hefei Science Center CAS ; Hefei Science Center CAS ; National Natural Science Foundation (NSFC) ; National Natural Science Foundation (NSFC) ; National Natural Science Foundation (NSFC) ; National Natural Science Foundation (NSFC) ; Fundamental Research Funds for the Central Universities ; Fundamental Research Funds for the Central Universities ; Fundamental Research Funds for the Central Universities ; Fundamental Research Funds for the Central Universities ; CAS/SAFEA International Partnership Program for Creative Research Teams ; CAS/SAFEA International Partnership Program for Creative Research Teams ; CAS/SAFEA International Partnership Program for Creative Research Teams ; CAS/SAFEA International Partnership Program for Creative Research Teams ; Hefei Science Center CAS ; Hefei Science Center CAS ; Hefei Science Center CAS ; Hefei Science Center CAS
WOS研究方向Chemistry ; Science & Technology - Other Topics ; Engineering
WOS类目Chemistry, Multidisciplinary ; GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY ; Engineering, Chemical
WOS记录号WOS:000449577200048
出版者AMER CHEMICAL SOC
引用统计
文献类型期刊论文
条目标识符http://ir.hfcas.ac.cn:8080/handle/334002/34242
专题中科院强磁场科学中心
通讯作者Chen, Qianwang
作者单位1.Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, Dept Mat Sci & Engn, 96 JinZhai Rd, Hefei 230026, Anhui, Peoples R China
2.Univ Sci & Technol China, Collaborat Innovat Ctr Suzhou Nanosci & Technol, 96 JinZhai Rd, Hefei 230026, Anhui, Peoples R China
3.Chinese Acad Sci, Hefei Inst Phys Sci, High Magnet Field Lab, Hefei 230031, Anhui, Peoples R China
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Li, Mengsi,Wang, Changlai,Yang, Yang,et al. Turning Carbon Atoms into Highly Active Oxygen Reduction Reaction Electrocatalytic Sites in Nitrogen-Doped Graphene-Coated Co@Ag[J]. ACS SUSTAINABLE CHEMISTRY & ENGINEERING,2018,6(11):14033-14041.
APA Li, Mengsi.,Wang, Changlai.,Yang, Yang.,Jiang, Peng.,Lin, Zhiyu.,...&Chen, Qianwang.(2018).Turning Carbon Atoms into Highly Active Oxygen Reduction Reaction Electrocatalytic Sites in Nitrogen-Doped Graphene-Coated Co@Ag.ACS SUSTAINABLE CHEMISTRY & ENGINEERING,6(11),14033-14041.
MLA Li, Mengsi,et al."Turning Carbon Atoms into Highly Active Oxygen Reduction Reaction Electrocatalytic Sites in Nitrogen-Doped Graphene-Coated Co@Ag".ACS SUSTAINABLE CHEMISTRY & ENGINEERING 6.11(2018):14033-14041.
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