Enhanced Anodic Dissolution of Magnesium in Quaternary-Ammonium-Based Ionic Liquid Containing a Small Amount of Water

Murase, Kuniaki; Sasaki, Izuru; Kitada, Atsushi; Uchimoto, Yoshiharu; Ichii, Takashi; Sugimura, Hiroyuki

doi:10.1149/2.057310jes

Cited by 12 publications

(12 citation statements)

References 40 publications

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“…Although noble Pt working electrodes are widely used to assess the Mg deposition/dissolution behavior of Mg electrolytes, the electrochemical properties of the Mg electrode itself are more relevant to its practical application. 34 In particular, the anodic dissolution of Mg must be facile enough to supply the Mg ions required for magnesiation of the cathode because nearly all of the Mg cathode materials are Mg-deficient in their pristine state. Although the excess electrolyte serves as a reservoir of Mg ions in a flooded cell configuration and the magnesiation of the cathode can be achieved without the supply of Mg ions from the anode, this is not practical for Mg batteries where the electrolyte volume should be minimized.…”

Section: Resultsmentioning

confidence: 99%

Section: Results and Discussionmentioning

confidence: 99%

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Electrolyte Additive Enabling Conditioning-Free Electrolytes for Magnesium Batteries

Kang

Kim

Hwang

et al. 2018

ACS Appl. Mater. Interfaces

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Most electrolytes for rechargeable Mg batteries require time-consuming conditioning or precycling process to achieve a fully reversible Mg deposition/dissolution, which hinders the normal operation of Mg batteries. This study details a simple and effective method for eliminating this conditioning behavior using heptamethyldisilazane (HpMS) as an electrolyte additive. It was found that the HpMS additive greatly increases the current density and Coulombic efficiency of Mg deposition/dissolution from the initial cycles in various sulfone and glyme solutions containing MgCl 2 or Mg(TFSI) 2 . The beneficial effect of HpMS was ascribed to its ability to scavenge trace water in the electrolytes and remove Mg(OH) 2 and Mg(TFSI) 2 -decomposition products from the Mg surface. Considering its applicability for a wide range of Mg electrolytes, the use of HpMS is expected to accelerate the development of practical Mg batteries.

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Section: Resultsmentioning

confidence: 99%

Section: Results and Discussionmentioning

confidence: 99%

Electrolyte Additive Enabling Conditioning-Free Electrolytes for Magnesium Batteries

Kang

Kim

Hwang

et al. 2018

ACS Appl. Mater. Interfaces

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“…Cu sheet (Nilaco, 99.9% purity) and Mg sheet or rod (Nilaco, 99.9% purity) were used as the working electrode (WE) and counter electrode (CE), respectively. Because the potential of Mg was not stable in some Tf 2 N-based ILs, 26 as reference electrodes (RE) we used a Mg rod immersed in ethylmagnesium bromide (EtMgBr) in THF (Kanto Chemical, 0.95 mol dm −3 ), separated from the main electrolyte by porous vycor glass (see Fig. 1).…”

Section: Electrochemical Measurements and Characterization Of Deposits-mentioning

confidence: 99%

Room-Temperature Electrodeposition of Mg Metal from Amide Salts Dissolved in Glyme-Ionic Liquid Mixture

Kitada

Kang

Uchimoto

et al. 2013

J. Electrochem. Soc.

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The electrodeposition of Mg metal from an ionic liquid-glyme mixture was investigated at room temperature. The mixture contains a glyme, a simple amide salt Mg(Tf 2 N) 2 (Tf = SO 2 CF 3), and a quaternary-ammonium Tf 2 N ionic liquid. Using the mixture bath, substantial cathodic electrodeposition of Mg at a large current density (∼10 mA cm −2) was observed, suggesting a change in coordination geometry around Mg 2+ cation together with improved conductivity. By mixing diglyme, the conductivity increased by an order of magnitude (2.5-2.6 mS cm −1) compared to the glyme-free ionic liquid (0.35 mS cm −1) and the viscosity became as low as that of pure glyme. Additionally, potentiostatic electrolysis resulted in a non-dendritic thin film of elemental Mg with metallic luster.

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“…Ionic liquids have recently been explored as electrolytes for Mg battery systems, but so far with only limited success. − We report here for the first time reversible Mg electrodeposition/dissolution from a purely ionic liquid mediumdesigned to specifically enhance the Mg deposition/dissolution process. These results were achieved by synthesizing task specific ILs to meet the specific coordination conditions required for Mg deposition/dissolution from a Mg(BH 4 ) 2 source.…”

Section: Introductionmentioning

confidence: 97%

Designer Ionic Liquids for Reversible Electrochemical Deposition/Dissolution of Magnesium

2016

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Chelating ionic liquids (ILs), in which polyether chains are pendent from the organic pyrrolidinium cation of the ILs (PEGylated ILs), were prepared that facilitate reversible electrochemical deposition/dissolution of Mg from a Mg(BH4)2 source. Mg electrodeposition processes in two specific PEGylated-ILs were compared against that in the widely studied N-butyl-N-methylpyrrolidinium bis(trifluoromethylsulfonyl)imide ionic liquid (BMPyrTFSI). The two chelating IL systems (one with a pendent polyether chain with three ether oxygens, MPEG3PyrTFSI, and the other with a seven-ether chain, MPEG7PyrTFSI) showed substantial improvement over BMPyrTFSI for Mg electrodeposition/dissolution. The best overall electrochemical performance was in MPEG7PyrTFSI. X-ray diffraction (XRD), scanning electron microscopy (SEM), and energy dispersive X-ray spectroscopy (EDS) were used to characterize galvanostatically deposited Mg, revealing production of pure, dendrite-free Mg deposits. Reversible Mg electrodeposition was achieved with high Coulombic efficiency (CE) of 90% and high current density (ca. 2 mA/cm(2) for the stripping peak). Raman spectroscopy was used to characterize Mg(2+) speciation in the PEGylated ILs and BMPyrTFSI containing Mg(BH4)2 by study of Raman modes of the coordinated and free states of borohydride, TFSI(-), and polyether COC groups. Quantitative analysis revealed that the polyether chains can displace both TFSI(-) and BH4(-) from the coordination sphere of Mg(2+). Comparison of the different IL electrolytes suggested that these displacement reactions may play a role in enabling Mg deposition/dissolution with high CE and current density in these PEGylated IL media. These results represent the first demonstration of reversible electrochemical deposition/dissolution of Mg in an ionic liquid specifically designed with this task in mind.

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Enhanced Anodic Dissolution of Magnesium in Quaternary-Ammonium-Based Ionic Liquid Containing a Small Amount of Water

Cited by 12 publications

References 40 publications

Electrolyte Additive Enabling Conditioning-Free Electrolytes for Magnesium Batteries

Electrolyte Additive Enabling Conditioning-Free Electrolytes for Magnesium Batteries

Room-Temperature Electrodeposition of Mg Metal from Amide Salts Dissolved in Glyme-Ionic Liquid Mixture

Designer Ionic Liquids for Reversible Electrochemical Deposition/Dissolution of Magnesium

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