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
刊名ACS SUSTAINABLE CHEMISTRY & ENGINEERING
2018-11-05
卷号6期号:11页码:14033-14041
关键词Metal-organic frameworks Oxygen reduction reaction Electron transfer Co core/Ag mantle structure Tuning electronic structure
ISSN号2168-0485
DOI10.1021/acssuschemeng.8b02573
通讯作者Chen, Qianwang(cqw@ustc.edu.cn)
英文摘要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.
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]
WOS关键词HYDROGEN EVOLUTION REACTION ; REACTION CATALYST ; ALLOY CATALYSTS ; NANOPARTICLES ; STRAIN ; COBALT ; PD ; NANOCRYSTALS ; SPECTROSCOPY ; ENERGY
WOS研究方向Chemistry ; Science & Technology - Other Topics ; Engineering
语种英语
出版者AMER CHEMICAL SOC
WOS记录号WOS:000449577200048
资助机构National Natural Science Foundation (NSFC) ; National Natural Science Foundation (NSFC) ; National Natural Science Foundation (NSFC) ; National Natural Science Foundation (NSFC) ; National Natural Science Foundation (NSFC) ; National Natural Science Foundation (NSFC) ; National Natural Science Foundation (NSFC) ; National Natural Science Foundation (NSFC) ; National Natural Science Foundation (NSFC) ; National Natural Science Foundation (NSFC) ; National Natural Science Foundation (NSFC) ; National Natural Science Foundation (NSFC) ; 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 ; Fundamental Research Funds for the Central Universities ; 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内容类型期刊论文
源URL[http://ir.hfcas.ac.cn:8080/handle/334002/34241]  
专题合肥物质科学研究院_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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