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Experimental verification of increased electronic excitation energy of water in hydrate-melt water by attenuated total reflection-far-ultraviolet spectroscopy
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- Nami Ueno
- Department of Chemistry, School of Science and Engineering, Kindai University 1 , Kowakae, Higashi-Osaka, Osaka 577-8502, Japan
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- Masato Takegoshi
- Department of Chemistry, School of Science and Engineering, Kindai University 1 , Kowakae, Higashi-Osaka, Osaka 577-8502, Japan
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- Anna Zaitceva
- Faculty of Fundamental Physical-Chemical Engineering, M. V. Lomonosov Moscow State University 2 , GSP-1, 1 Leninskiye Gory, Moscow 11999, Russia
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- Yukihiro Ozaki
- School of Biological and Environmental Sciences, Kwansei Gakuin University 3 , Sanda, Hyogo 669-1337, Japan
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- Yusuke Morisawa
- Department of Chemistry, School of Science and Engineering, Kindai University 1 , Kowakae, Higashi-Osaka, Osaka 577-8502, Japan
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Description
<jats:p>The demand for Li secondary batteries is increasing, with the need for batteries with a higher level of performance and improved safety features. The use of a highly concentrated aqueous electrolyte solution is an effective way to increase the safety of batteries because it is possible to use “water-in-salt” (WIS) and “hydrate-melt” (HM) electrolytes for practical applications. These electrolytes exhibit a potential window of >3.0 V, which is attributed to the difference between the HOMO and the LUMO energies of the n orbital of the pure water molecules and that of the water molecules in the hydration shells of a metal ion, according to theoretical predictions. Thus, in the present study, the attenuated total reflectance (ATR)-far-ultraviolet (FUV) spectra of water and super-concentrated aqueous solutions, such as WIS and HM using a Li salt, were experimentally investigated. The effects of anions, cations, and deuteriums on the ATR-FUV spectra were examined. The ATR-FUV method is an excellent means of studying highly concentrated aqueous salt solutions. The results suggest that the transition energy of water molecules in an ultrahighly concentrated aqueous electrolyte containing HM and WIS increased by nearly 0.4 eV (corresponding to an energy shift of over 10 nm) compared to an aqueous electrolyte with a typical water concentration. It was also revealed that the transition energy of water changes depending on the environment of the non-bonding electron, which is directly connected with or affected by hydrogen bonding with other water molecules or directly connected with Li+.</jats:p>
Journal
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- The Journal of Chemical Physics
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The Journal of Chemical Physics 156 (7), 07405-, 2022-02-16
AIP Publishing