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DOI	10.1039/c7ee03245e
	Isolated Ni single atoms in graphene nanosheets for high-performance CO2 reduction
	Jiang K.; Siahrostami S.; Zheng T.; Hu Y.; Hwang S.; Stavitski E.; Peng Y.; Dynes J.; Gangisetty M.; Su D.; Attenkofer K.; Wang H.
发表日期	2018
ISSN	17545692
起始页码	893
结束页码	903
卷号	11 期号:4
英文摘要	Single-atom catalysts have emerged as an exciting paradigm with intriguing properties different from their nanocrystal counterparts. Here we report Ni single atoms dispersed into graphene nanosheets, without Ni nanoparticles involved, as active sites for the electrocatalytic CO2 reduction reaction (CO2RR) to CO. While Ni metal catalyzes the hydrogen evolution reaction (HER) exclusively under CO2RR conditions, Ni single atomic sites present a high CO selectivity of 95% under an overpotential of 550 mV in water, and an excellent stability over 20 hours' continuous electrolysis. The current density can be scaled up to more than 50 mA cm-2 with a CO evolution turnover frequency of 2.1 × 105 h-1 while maintaining 97% CO selectivity using an anion membrane electrode assembly. Different Ni sites in graphene vacancies, with or without neighboring N coordination, were identified by in situ X-ray absorption spectroscopy and density functional theory calculations. Theoretical analysis of Ni and Co sites suggests completely different reaction pathways towards the CO2RR or HER, in agreement with experimental observations. © 2018 The Royal Society of Chemistry.
英文关键词	Atoms; Carbon dioxide; Density functional theory; Graphene; Nanosheets; X ray absorption spectroscopy; Electrocatalytic; Graphene nanosheets; Hydrogen evolution reactions; In-situ X-ray absorption spectroscopy; Membrane electrode assemblies; Ni Nanoparticles; Reaction pathways; Turnover frequency; Nickel; carbon; carbon dioxide; carbon monoxide; catalysis; catalyst; chemical reaction; electrochemical method; electrode; electrokinesis; experimental study; hydrogen; nanoparticle; performance assessment; reduction; turnover
语种	英语
来源期刊	Energy & Environmental Science
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/190280
作者单位	Rowland Institute, Harvard University, Cambridge, MA 02142, United States; SUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering, Stanford University, Stanford, CA 94305, United States; Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, 230026, China; Canadian Light Source Inc., University of Saskatchewan, 44 Innovation Boulevard, Saskatoon, SK S7N 2V3, Canada; Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, NY 11973, United States; National Synchrotron Light Source II, Brookhaven National Laboratory, Upton, NY 11973, United States; Department of Chemistry, University of Science and Technology of China, Hefei, 230026, China
推荐引用方式 GB/T 7714	Jiang K.,Siahrostami S.,Zheng T.,et al. Isolated Ni single atoms in graphene nanosheets for high-performance CO2 reduction[J],2018,11(4).
APA	Jiang K..,Siahrostami S..,Zheng T..,Hu Y..,Hwang S..,...&Wang H..(2018).Isolated Ni single atoms in graphene nanosheets for high-performance CO2 reduction.Energy & Environmental Science,11(4).
MLA	Jiang K.,et al."Isolated Ni single atoms in graphene nanosheets for high-performance CO2 reduction".Energy & Environmental Science 11.4(2018).