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Title: Highly Active Electrolytes for Rechargeable Mg Batteries Based on [Mg2(μ-Cl)2]2+ Cation Complex in Dimethoxyethane

Abstract

Highly active electrolytes based on a novel [Mg2(μ-Cl)2]2+ cation complex for reversible Mg deposition were developed and analyzed in this work. These electrolytes were formulated in dimethoxyethane through dehalodimerization of non-nucleophilic MgCl2 by reacting with either Mg salts (such as Mg(TFSI)2, TFSI= bis(trifluoromethane)sulfonylimide) or Lewis acid salts (such as AlEtCl2 or AlCl3). The cation complex was identified for the first time as [Mg2(μ-Cl)2(DME)4]2+ (DME=dimethoxyethane) and its molecular structure was characterized by single crystal X-ray diffraction, Raman spectroscopy and NMR. The electrolyte synthesis process was studied and rational approaches for formulating highly active electrolytes were proposed. Through control of the anions, electrolytes with efficiency close to 100%, wide electrochemical window (up to 3.5V) and high ionic conductivity (> 6 mS/cm) were obtained. The electrolyte synthesis and understandings developed in this work could bring significant opportunities for rational formulation of electrolytes with the general formula [Mg2(μ-Cl)2(DME)4][anion]x for practical Mg batteries.

Authors:
; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1182866
Report Number(s):
PNNL-SA-106553
48681; TE1400000
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Physical Chemistry Chemical Physics. PCCP, 17(20):13307-13314
Country of Publication:
United States
Language:
English
Subject:
Mg Battery, Electrolytes, DME, Mg dimer complex; Environmental Molecular Sciences Laboratory

Citation Formats

Cheng, Yingwen, Stolley, Ryan M., Han, Kee Sung, Shao, Yuyan, Arey, Bruce W., Washton, Nancy M., Mueller, Karl T., Helm, Monte L., Sprenkle, Vincent L., Liu, Jun, and Li, Guosheng. Highly Active Electrolytes for Rechargeable Mg Batteries Based on [Mg2(μ-Cl)2]2+ Cation Complex in Dimethoxyethane. United States: N. p., 2015. Web. doi:10.1039/C5CP00859J.
Cheng, Yingwen, Stolley, Ryan M., Han, Kee Sung, Shao, Yuyan, Arey, Bruce W., Washton, Nancy M., Mueller, Karl T., Helm, Monte L., Sprenkle, Vincent L., Liu, Jun, & Li, Guosheng. Highly Active Electrolytes for Rechargeable Mg Batteries Based on [Mg2(μ-Cl)2]2+ Cation Complex in Dimethoxyethane. United States. doi:10.1039/C5CP00859J.
Cheng, Yingwen, Stolley, Ryan M., Han, Kee Sung, Shao, Yuyan, Arey, Bruce W., Washton, Nancy M., Mueller, Karl T., Helm, Monte L., Sprenkle, Vincent L., Liu, Jun, and Li, Guosheng. Thu . "Highly Active Electrolytes for Rechargeable Mg Batteries Based on [Mg2(μ-Cl)2]2+ Cation Complex in Dimethoxyethane". United States. doi:10.1039/C5CP00859J.
@article{osti_1182866,
title = {Highly Active Electrolytes for Rechargeable Mg Batteries Based on [Mg2(μ-Cl)2]2+ Cation Complex in Dimethoxyethane},
author = {Cheng, Yingwen and Stolley, Ryan M. and Han, Kee Sung and Shao, Yuyan and Arey, Bruce W. and Washton, Nancy M. and Mueller, Karl T. and Helm, Monte L. and Sprenkle, Vincent L. and Liu, Jun and Li, Guosheng},
abstractNote = {Highly active electrolytes based on a novel [Mg2(μ-Cl)2]2+ cation complex for reversible Mg deposition were developed and analyzed in this work. These electrolytes were formulated in dimethoxyethane through dehalodimerization of non-nucleophilic MgCl2 by reacting with either Mg salts (such as Mg(TFSI)2, TFSI= bis(trifluoromethane)sulfonylimide) or Lewis acid salts (such as AlEtCl2 or AlCl3). The cation complex was identified for the first time as [Mg2(μ-Cl)2(DME)4]2+ (DME=dimethoxyethane) and its molecular structure was characterized by single crystal X-ray diffraction, Raman spectroscopy and NMR. The electrolyte synthesis process was studied and rational approaches for formulating highly active electrolytes were proposed. Through control of the anions, electrolytes with efficiency close to 100%, wide electrochemical window (up to 3.5V) and high ionic conductivity (> 6 mS/cm) were obtained. The electrolyte synthesis and understandings developed in this work could bring significant opportunities for rational formulation of electrolytes with the general formula [Mg2(μ-Cl)2(DME)4][anion]x for practical Mg batteries.},
doi = {10.1039/C5CP00859J},
journal = {Physical Chemistry Chemical Physics. PCCP, 17(20):13307-13314},
number = ,
volume = ,
place = {United States},
year = {Thu Jan 01 00:00:00 EST 2015},
month = {Thu Jan 01 00:00:00 EST 2015}
}