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Liebenow, C.

doi:10.1023/a:1018464210084

Cited by 129 publications

(78 citation statements)

References 13 publications

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“…[4][5][6][7][8][9][10][11][12] Particularly, ether solutions of alkylmagnesium halide complexes (Grignard reagents) show an ideal magnesium deposition-dissolution behavior with no overpotential and almost 100% Coulombic efficiency. 4 Moreover, the addition of Lewis acids R y AlCl 3¹y (R = alkyl group, y = 0-3) accept alkyl ligands to form complex anions. Therefore, they stabilize cationic magnesium halide species.…”

Section: Introductionmentioning

confidence: 99%

Solution Structure and Magnesium Deposition Electrochemistry of Mixing Alkylmagnesium Halide with Magnesium Sulfonyl Amide/Glyme Solution

Egashira

Hiratsuka

2016

Electrochemistry

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To elucidate effective species and their quantitative requirements for reversible magnesium deposition, a triglyme solution of ethylmagnesium bromide (EtMgBr) complex was mixed with magnesium bis(trifluoromethanesulfonyl) amide/triglyme solution in various ratios. The mixed electrolyte characteristics have been assessed using electrochemical magnesium deposition tests, titration of methanol, and Raman spectroscopy. The existence of EtMgBr reduces the overpotential of magnesium deposition. The Coulombic efficiency of this process varies linearly with the EtMgBr content, although the active EtMgBr decreases more than expected from the mixing ratio. Raman spectra for the mixed electrolyte suggest a change in the structure of magnesium bromide species and coordination mode of magnesium by mixing of EtMgBr with magnesium sulfonylamide salt.

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Section: Introductionmentioning

confidence: 99%

Solution Structure and Magnesium Deposition Electrochemistry of Mixing Alkylmagnesium Halide with Magnesium Sulfonyl Amide/Glyme Solution

Egashira

Hiratsuka

2016

Electrochemistry

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“…3 Thus, it has generally accepted that reversible Mg deposition and dissolution do not occur in usual organic electrolyte solutions dissolving conventional Mg salts. As the possibility of Mg anode (negative electrode) for rechargeable batteries, Liebenow 4 first reported the reversible deposition and dissolution of Mg in ether solutions of so-called Grignard reagents. It is considered that no compact passivation film covers the Mg surface and hence the reversible deposition and dissolution of Mg occur with low overvoltage in those systems.…”

Section: Introductionmentioning

confidence: 99%

Electrochemical Behavior of Magnesium in Mixed Solutions Consisting of Ionic Liquid and Alkylmagnesiumbromides with Different Alkyl-Chains

2012

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Electrochemical deposition and dissolution of magnesium have been investigated in organic solutions consisting of alkylmagnesiumbromides/tetrahydrofuran (RMgBr/THF) having different alkyl-chains mixed with an ionic liquid. Coulombic efficiency for cathodic deposition and anodic dissolution of magnesium, obtained from voltammetric responses, decreased with the increase in the alkyl-chain length of the magnesium complex. The highest current response was observed in the electrolyte system consisting of CH 3 MgBr/THF with a quaternary ammonium saltbased ionic liquid.

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“…4 However, Grignard reagents are not stable at the high electrochemical potentials required for the positive electrode. 5 Recently, Nakayama et al 6 revealed that, for Al electrolyte systems, certain sulfones (RR´SO 2 ) can be used as a solvent that endures high potentials.…”

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confidence: 99%

Sulfone-Based Electrolyte Solutions for Rechargeable Magnesium Batteries Using 2,5-Dimethoxy-1,4-benzoquinone Positive Electrode

Senoh

Sakaebe

Sano

et al. 2014

J. Electrochem. Soc.

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We examined three sulfone-based electrolyte solutions for use in rechargeable magnesium batteries; i.e., sulfolane (SL), ethyl-i-propyl sulfone (EiPS) and di-n-propyl sulfone (DnPS), in which was dissolved 0.5 mol L −1 magnesium bis(trifluoromethanesulfonyl)amide (Mg(TFSA) 2 ). The specific conductivities of these sulfone-based Mg-electrolyte solutions were 1-2 mS cm −1 at 30 • C. These electrolyte solutions were thermally stable < 250 • C, and electrochemically stable < 2 V vs. Mg reference electrode (Mg wire). In these electrolyte solutions, an organic positive electrode made of 2,5-dimethoxy-1,4-benzoquinone (DMBQ) underwent reversible charge-discharge reactions. The reduction-oxidation current of the metallic Mg negative electrode was observed. A two-electrode cell composed of Mg|Mg(TFSA) 2 /SL|DMBQ endured more than 50 charge-discharge cycles at 30 • Rechargeable magnesium batteries may be an option for replacing the rechargeable lithium batteries because magnesium is much more abundant in the earth's crust and is more widely distributed than lithium. The fact that metallic Mg is less reactive toward ambient water and oxygen than Li may lead to a safer battery. In addition, a volumetric energy density of Mg should be greater than that of metallic Li.To achieve rechargeable magnesium batteries, it is important to consider the combination of the electrolyte and the positive electrode with the Mg negative electrode.1-3 Some solutions of Grignard reagents (RMgX; R = alkyl, X = halogen) are known to function as an electrolyte, in which metallic Mg is electrochemically and reversibly deposited on and dissolved from the negative electrode. 4 However, Grignard reagents are not stable at the high electrochemical potentials required for the positive electrode. 5 Recently, Nakayama et al. 6 revealed that, for Al electrolyte systems, certain sulfones (RR´SO 2 ) can be used as a solvent that endures high potentials. Thus, in the present study, we investigated three sulfones for use as a solvent to dissolve the Mg solute in rechargeable magnesium batteries; viz., sulfolane (SL), ethyl-i-propyl sulfone (EiPS) and di-n-propyl sulfone (DnPS). As the Mg electrolyte, we used magnesium bis(trifluoromethanesulfonyl)amide (Mg(TFSA) 2 ) because it can tolerate a high potential and the large TFSA anion, a soft Lewis base, should facilitate its dissociation from the Mg 2+ cation. In a Mg electrolyte solution, Mg(ClO 4 ) 2 /GBL, in a threeelectrode cell, we previously investigated the potential capability of 2,5-dimethoxy-1,4-benzoquinone (DMBQ), 7 which works as a positive-electrode active material in the lithium system. 8 In Mg(ClO 4 ) 2 /GBL, however, we found that no reversible Mg deposition/dissolution occurred. The objectives of the present study were to determine the fundamental physical properties of these sulfone electrolyte solutions, e.g., the viscosity, conductivity, potential window, etc., and to demonstrate the battery properties of a full-cell, Mg|Mg(TFSA) 2 /sulfone|DMBQ, to shed light on the possibilities and probl...

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Cited by 129 publications

References 13 publications

Solution Structure and Magnesium Deposition Electrochemistry of Mixing Alkylmagnesium Halide with Magnesium Sulfonyl Amide/Glyme Solution

Solution Structure and Magnesium Deposition Electrochemistry of Mixing Alkylmagnesium Halide with Magnesium Sulfonyl Amide/Glyme Solution

Electrochemical Behavior of Magnesium in Mixed Solutions Consisting of Ionic Liquid and Alkylmagnesiumbromides with Different Alkyl-Chains

Sulfone-Based Electrolyte Solutions for Rechargeable Magnesium Batteries Using 2,5-Dimethoxy-1,4-benzoquinone Positive Electrode

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