TY - JOUR
T1 - Theoretical analysis of electrode-dependent interfacial structures on hydrate-melt electrolytes
AU - Takenaka, Norio
AU - Inagaki, Taichi
AU - Shimada, Tatau
AU - Yamada, Yuki
AU - Nagaoka, Masataka
AU - Yamada, Atsuo
N1 - Funding Information:
This work was supported by JSPS KAKENHI Specially Promoted Research (Grant No. 15H05701) and Grant-in-Aid for JSPS Research Fellow (Grant No. JP18J14097), as well as the MEXT programs “Elements Strategy Initiative for Catalysts and Batteries (ESICB)” and “Priority Issue on Post-K computer” (Development of new fundamental technologies for high-efficiency energy creation, conversion/storage and use).
Publisher Copyright:
© 2020 Author(s).
PY - 2020/3/31
Y1 - 2020/3/31
N2 - Aqueous electrolytes have the potential to overcome some of the safety issues associated with current Li-ion batteries intended for large-scale applications such as stationary use. We recently discovered a lithium-salt dihydrate melt, viz., Li(TFSI)0.7(BETI)0.3·2H2O, which can provide a wide potential window of over 3 V; however, its reductive stability strongly depends on the electrode material. To understand the underlying mechanism, the interfacial structures on several electrodes (C, Al, and Pt) were investigated by conducting molecular dynamics simulation under the constraint of the electrode potential. The results showed that the high adsorption force on the surface of the metal electrodes is responsible for the increased water density, thus degrading the reductive stability of the electrolyte. Notably, the anion orientation on Pt at a low potential is unfavorable for the formation of a stable anion-derived solid electrolyte interphase, thus promoting hydrogen evolution. Hence, the interfacial structures that depend on the material and potential of the electrode mainly determine the reductive stability of hydrate-melt electrolytes.
AB - Aqueous electrolytes have the potential to overcome some of the safety issues associated with current Li-ion batteries intended for large-scale applications such as stationary use. We recently discovered a lithium-salt dihydrate melt, viz., Li(TFSI)0.7(BETI)0.3·2H2O, which can provide a wide potential window of over 3 V; however, its reductive stability strongly depends on the electrode material. To understand the underlying mechanism, the interfacial structures on several electrodes (C, Al, and Pt) were investigated by conducting molecular dynamics simulation under the constraint of the electrode potential. The results showed that the high adsorption force on the surface of the metal electrodes is responsible for the increased water density, thus degrading the reductive stability of the electrolyte. Notably, the anion orientation on Pt at a low potential is unfavorable for the formation of a stable anion-derived solid electrolyte interphase, thus promoting hydrogen evolution. Hence, the interfacial structures that depend on the material and potential of the electrode mainly determine the reductive stability of hydrate-melt electrolytes.
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U2 - 10.1063/5.0003196
DO - 10.1063/5.0003196
M3 - Article
AN - SCOPUS:85082616533
SN - 0021-9606
VL - 152
JO - Journal of Chemical Physics
JF - Journal of Chemical Physics
IS - 12
M1 - 124706
ER -