Journal
JOURNAL OF PHYSICAL CHEMISTRY C
Volume 120, Issue 41, Pages 23339-23350Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.6b06804
Keywords
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Funding
- MEXT program Elements Strategy Initiative to Form Core Research Center of the Ministry of Education, Culture, Sports, Science, and Technology (MEXT) of Japan
- JSPS KAKENHI from the Japan Society for the Promotion of Science (JSPS) [15H03874, 15K13815, 16H06368]
- Advanced Low Carbon Technology Research and Development Program (ALCA) of the Japan Science and Technology Agency (JST)
- Grants-in-Aid for Scientific Research [15H03874, 16J11045, 15K13815, 16H06368] Funding Source: KAKEN
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Physicochemical properties and battery performance of [Na-(glyme)][TFSA] complexes (TFSA: bis(trifluoromethanesulfonyl)amide) dissolved in a hydrofluoroether (HFE) were investigated. Glyme (tetraglyme (G4) or pentaglyme (G5)) coordinates to Na+ to form a 1:1 complex [Na(G4 or GS)](+) cation. Raman spectroscopy revealed that the complex structure of [Na(glyme)](+) is maintained in the HFE solution, and free (uncoordinated) glyrnes are not liberated on adding HFE. HFE molecules are scarcely involved in the first solvation shell of Na+ because of their low electron-pair-donating ability. Raman spectra of the [TFSA](-) anion suggests that the attractive interaction between the complex [Na(glyme)](+) cation and [TFSA](-) anion is enhanced on adding HFE. The population of contact ion-pair (CIP) and/or aggregate (AGG) is smaller for the G5 system than for the G4 one, and the [Na(G5)][TFSA]/HFE has higher ionic conductivity. The self-diffusion coefficients of the [Na(glyme)]+ complex and [TFSA](-) were measured by pulsed field gradient (PFG) NMR, and the dissociativity of [Na(glyme)] [TFSA] was assessed. The dissociativity of the G5 system is greater than that of the G4 one, and the dissociativity can be correlated with the attractive interaction between [Na(glyme)](+) and [TFSA](-), as evaluated by ab initio calculations. The dissociativity of the complexes gave significant effects on the battery performance.
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