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      Enhanced Electrochemical Stability of Molten Li Salt Hydrate Electrolytes by the Addition of Divalent Cations


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          Water can be an attractive solvent for Li-ion battery electrolytes owing to numerous advantages such as high polarity, nonflammability, environmental benignity, and abundance, provided that its narrow electrochemical potential window can be enhanced to a similar level to that of typical nonaqueous electrolytes. In recent years, significant improvements in the electrochemical stability of aqueous electrolytes have been achieved with molten salt hydrate electrolytes containing extremely high concentrations of Li salt. In this study, we investigated the effect of divalent salt additives (magnesium and calcium bis(trifluoromethanesulfonyl)amides) in a molten salt hydrate electrolyte (21 mol kg –1 lithium bis(trifluoromethanesulfonyl)amide) on the electrochemical stability and aqueous lithium secondary battery performance. We found that the electrochemical stability was further enhanced by the addition of the divalent salt. In particular, the reductive stability was increased by more than 1 V on the Al electrode in the presence of either of the divalent cations. Surface characterization with X-ray photoelectron spectroscopy suggests that a passivation layer formed on the Al electrode consists of inorganic salts (most notably fluorides) of the divalent cations and the less-soluble solid electrolyte interphase mitigated the reductive decomposition of water effectively. The enhanced electrochemical stability in the presence of the divalent salts resulted in a more-stable charge–discharge cycling of LiCoO 2 and Li 4Ti 5O 12 electrodes.

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          Most cited references 56

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          Electrolytes and interphases in Li-ion batteries and beyond.

           Kang Xu (2014)
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            "Water-in-salt" electrolyte enables high-voltage aqueous lithium-ion chemistries.

            Lithium-ion batteries raise safety, environmental, and cost concerns, which mostly arise from their nonaqueous electrolytes. The use of aqueous alternatives is limited by their narrow electrochemical stability window (1.23 volts), which sets an intrinsic limit on the practical voltage and energy output. We report a highly concentrated aqueous electrolyte whose window was expanded to ~3.0 volts with the formation of an electrode-electrolyte interphase. A full lithium-ion battery of 2.3 volts using such an aqueous electrolyte was demonstrated to cycle up to 1000 times, with nearly 100% coulombic efficiency at both low (0.15 coulomb) and high (4.5 coulombs) discharge and charge rates.
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              Rechargeable lithium batteries with aqueous electrolytes.

               Jason Dahn,  J Dahn,  W. Li (1994)
              Rechargeable lithium-ion batteries that use an aqueous electrolyte have been developed. Cells with LiMn(2)O(4) and VO(2)(B) as electrodes and 5 M LiNO(3) in water as the electrolyte provide a fundamentally safe and cost-effective technology that can compete with nickelcadmium and lead-acid batteries on the basis of stored energy per unit of weight.

                Author and article information

                J Phys Chem C Nanomater Interfaces
                J Phys Chem C Nanomater Interfaces
                The Journal of Physical Chemistry. C, Nanomaterials and Interfaces
                American Chemical Society
                16 August 2018
                06 September 2018
                16 August 2019
                : 122
                : 35
                : 20167-20175
                []Department of Chemistry and Biotechnology, Yokohama National University , 79-5 Tokiwadai, Hodogaya-ku, Yokohama 240-8501, Japan
                []Graduate School of Science and Technology, Niigata University , 8050 Ikarashi, 2-no-cho, Nishi-ku, Niigata City 950-2181, Japan
                [§ ]Unit of Elements Strategy Initiative for Catalysts & Batteries (ESICB), Kyoto University , Kyoto 615-8510, Japan
                Author notes
                [* ]E-mail: ueno-kazuhide-rc@ 123456ynu.ac.jp . Tel/Fax: +81-45-339-3951.
                Copyright © 2018 American Chemical Society

                This is an open access article published under an ACS AuthorChoice License, which permits copying and redistribution of the article or any adaptations for non-commercial purposes.

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