Journal
JOURNAL OF PHYSICAL CHEMISTRY C
Volume 124, Issue 52, Pages 28510-28519Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.0c08268
Keywords
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Funding
- Japan Science and Technology Agency (JST), Advanced Low Carbon Technology Research and Development Program (ALCA)
- Specially Promoted Research for Innovative Next Generation Batteries (SPRING) Project [JPMJAL1301]
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To clarify the effects of anion species and solvents on the Coulombic efficiency and polarization of magnesium deposition/dissolution reactions, the anode/electrolyte interfacial behavior of magnesium tetrakis(hexafluoroisopropyloxy) borate (Mg[B(HFIP)(4)](2)) and magnesium bis(trifluoromethanesulfony)amide (Mg(TFSA) 2 ) was investigated and compared in triglyme and 2-methlytetrahydrofuran (2-MeTHF). When using triglyme, which has strong interaction with magnesium ions, decomposition of [B(HFIP)(4)](-) in Mg[B(HFIP)(4)](2)/triglyme was hard to occur because of the high reduction stability of the uncoordinated [B(HFIP)(4)](-) anion, resulting in significantly higher Coulombic efficiency and smaller polarization than Mg(TFSA)(2)/triglyme. When 2-MeTHF was used as the solvent, magnesium deposition/dissolution reactions occurred in the Mg[B(HFIP)(4)](2)/2-MeTHF electrolyte but not in the Mg[TFSA](2)/2-MeTHF electrolyte. This is because the coordinated [B(HFIP)(4)](-) anion in Mg[B(HFIP)(4)](2) /2-MeTHF is stable at the magnesium deposition potential. However, the reductive stability of the coordinated [B(HFIP)(4)](-) anion is inferior to that of the uncoordinated [B(HFIP)(4)](-) anion, resulting in the Mg[B(HFIP)(4)](2)/2-MeTHF Coulombic efficiency being lower than that of Mg[B(HFIP)(4)](2)/triglyme. Our results indicate that solvents that could not be used with Mg(TFSA) 2 are suitable in weakly coordinating anion electrolytes, such as Mg[B(HFIP)(4)](2). Controlling the interaction between magnesium ions and anions by selecting suitable anions and solvents is essential for designing new electrolytes for magnesium rechargeable batteries.
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