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DOI10.1039/c8ee02703j
Probing microstructure and electrolyte concentration dependent cell chemistry: Via operando small angle neutron scattering
Jafta C.J.; Sun X.-G.; Veith G.M.; Jensen G.V.; Mahurin S.M.; Paranthaman M.P.; Dai S.; Bridges C.A.
发表日期2019
ISSN17545692
起始页码1866
结束页码1877
卷号12期号:6
英文摘要The key to understanding the cycling mechanism of lithium-ion battery electrodes is to develop methods to monitor the dynamic cell chemistry, but the complexity of the problem has continued to pose an obstacle. Here we describe the use of operando small-angle neutron scattering (SANS) to show directly how the use of concentrated LiTFSI electrolyte in Li/ordered mesoporous carbon (OMC) half-cells influences the mechanism of solid electrolyte interphase (SEI) formation, lithium intercalation, and carbon framework expansion. We find that a complex interplay between the viscosity, lithium solvation shell and electrode microstructure in the concentrated 4 M electrolyte changes the dynamics of SEI formation and pore filling at a given applied potential. Both the filling of micropores and co-intercalation are found to drive the expansion of the carbon framework. Lithium-rich reduction products form at much higher potentials in the micropores of the 4 M electrolyte system, while on mesopore surfaces the lithium-rich salts form quickly before giving way to carbonaceous products. This study reveals operando SANS as a unique method for providing microstructure dependent information on the dynamics of electrochemical processes. © 2019 The Royal Society of Chemistry.
英文关键词Carbon; Electrodes; Intercalation; Lithium-ion batteries; Microporosity; Microstructure; Solid electrolytes; Carbonaceous products; Electrochemical process; Electrode microstructures; Electrolyte concentration; Electrolyte systems; Lithium Intercalation; Reduction products; Solid electrolyte interphase; Neutron scattering; concentration (composition); electrochemistry; electrode; electrolyte; energy storage; lithium; microstructure; neutron scattering
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/189892
作者单位Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831, United States; Center for Neutron Research, National Institute of Standards and Technology, Gaithersburg, MD 20899, United States
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Jafta C.J.,Sun X.-G.,Veith G.M.,et al. Probing microstructure and electrolyte concentration dependent cell chemistry: Via operando small angle neutron scattering[J],2019,12(6).
APA Jafta C.J..,Sun X.-G..,Veith G.M..,Jensen G.V..,Mahurin S.M..,...&Bridges C.A..(2019).Probing microstructure and electrolyte concentration dependent cell chemistry: Via operando small angle neutron scattering.Energy & Environmental Science,12(6).
MLA Jafta C.J.,et al."Probing microstructure and electrolyte concentration dependent cell chemistry: Via operando small angle neutron scattering".Energy & Environmental Science 12.6(2019).
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