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분자 분광학 및 동력학 연구단
분자 분광학 및 동력학 연구단
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Two-Dimensional Infrared Spectroscopy and Molecular Dynamics Simulation Studies of Nonaqueous Lithium Ion Battery Electrolytes

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Title
Two-Dimensional Infrared Spectroscopy and Molecular Dynamics Simulation Studies of Nonaqueous Lithium Ion Battery Electrolytes
Author(s)
Joonhyung Lim; Lee, Kyung-Koo; Liang, Chungwen; Kwang-Hee Park; Minjoo Kim; Kyungwon Kwak; Minhaeng Cho
Publication Date
2019-08
Journal
JOURNAL OF PHYSICAL CHEMISTRY B, v.123, no.31, pp.6651 - 6663
Publisher
AMER CHEMICAL SOC
Abstract
Lithium ion battery (LIB) technology is undoubtedly indispensable to modern life. However, despite enormous and extended effort to improve LIB performance, our understanding of the underlying principles and mechanisms of lithium ion transport in nonaqueous LIB electrolytes remained limited until recently. There is a particular lack of knowledge of the microscopic solvation structures and fluctuation dynamics around charge carriers in real electrolytes. Typical electrolytes found in commercially available LIBs consist of lithium salts and mixed carbonate solvents, with the latter playing an essential role in promoting lithium ion transport and forming an electrically stable solid electrolyte interphase. Although a number of linear spectroscopic studies of LIB electrolytes aiming at understanding the complex nature of lithium ion solvation processes have been reported, the notion that each lithium ion is strongly solvated by carbonate molecules to form a long-lasting solvation sheath structure has remained the subject of intense debate. Here, we present the results of FTIR, fs IR pump-probe, two-dimensional IR spectroscopy, and molecular dynamics simulations reported by us and others and discuss the possible interplay of picosecond solvation dynamics and macroscopic ion transport processes within the framework of the fluctuation-dissipation relationship. Further, by measuring the time-dependent fluctuations and spectral diffusions of carbonate carbonyl stretch modes that act as excellent infrared probes for the local electrostatic environment, we show that lithium cations are not only solvated by carbonate molecules but also interact with counteranions at equilibrium depending on solvent composition. Molecular dynamics simulations support the notion that rapid chemical exchanges between carbonate solvent molecules in the first and outer solvation shells are critical for describing mobile lithium ion transport phenomena. We thus anticipate that time-resolved coherent multidimensional vibrational spectroscopy is capable of providing decisive evidence on the ultrafast solvent dynamics of various electrolytes, which is potentially helpful for designing improved and more efficient LIB electrolytes in the future. © 2019 American Chemical Society
URI
https://pr.ibs.re.kr/handle/8788114/6275
ISSN
1520-6106
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Center for Molecular Spectroscopy and Dynamics(분자 분광학 및 동력학 연구단) > Journal Papers (저널논문)
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