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Title: Ionic liquid hybrids: Progress toward non-corrosive electrolytes with high-voltage oxidation stability for magnesium-ion based batteries

Journal Article · · Electrochimica Acta
 [1];  [2]; ORCiD logo [2];  [2];  [3];  [3];  [4]
  1. Stony Brook Univ., NY (United States). Dept. of Materials Science and Engineering
  2. Stony Brook Univ., NY (United States). Dept. of Chemistry
  3. Stony Brook Univ., NY (United States). Dept. of Materials Science and Engineering; Stony Brook Univ., NY (United States). Dept. of Chemistry
  4. Stony Brook Univ., NY (United States). Dept. of Materials Science and Engineering; Stony Brook Univ., NY (United States). Dept. of Chemistry; Brookhaven National Lab. (BNL), Upton, NY (United States)

Magnesium – ion batteries have the potential for high energy density but require new types of electrolytes for practical application. Ionic liquid (IL) electrolytes offer the opportunity for increased safety and broader voltage windows relative to traditional electrolytes. We present here a systematic study of both the conductivity and oxidative stability of hybrid electrolytes consisting of eleven ILs mixed with dipropylene glycol dimethylether (DPGDME) or acetonitrile (ACN) cosolvents and magnesium bis(trifluoromethylsulfonyl)imide (Mg(TFSI)2). Our study finds a correlation of higher conductivity of ILs with unsaturated rings and short carbon chain lengths, but by contrast, these ILs also exhibited lower oxidation voltage limits. For the cosolvent additive, although glymes have a demonstrated capability of coordination with Mg2+ ions, a decrease in conductivity compared to acetonitrile hybrid electrolytes was observed. Lastly, when cycled within the appropriate voltage range, the IL-hybrid electrolytes that show the highest conductivity provide the best cathode magnesiation current densities and lowest polarization as demonstrated with a Mg0.15MnO2 and Mg0.07V2O5 cathodes.

Research Organization:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); USDOE Office of Electricity (OE)
Grant/Contract Number:
SC0012704; SC0012673; 1109408; 1275961
OSTI ID:
1341693
Alternate ID(s):
OSTI ID: 1398589
Report Number(s):
BNL-113438-2017-JA
Journal Information:
Electrochimica Acta, Vol. 219, Issue C; ISSN 0013-4686
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 10 works
Citation information provided by
Web of Science

References (55)

Cathode materials for magnesium and magnesium-ion based batteries journal March 2015
Lithium and sodium battery cathode materials: computational insights into voltage, diffusion and nanostructural properties journal January 2014
Life-cycle analysis of flow-assisted nickel zinc-, manganese dioxide-, and valve-regulated lead-acid batteries designed for demand-charge reduction journal March 2015
Rechargeable magnesium battery: Current status and key challenges for the future journal October 2014
Thermodynamic analysis on energy densities of batteries journal January 2011
Addressing the terawatt challenge: scalability in the supply of chemical elements for renewable energy journal January 2012
Paving the Way towards Highly Stable and Practical Electrolytes for Rechargeable Magnesium Batteries journal October 2014
Prototype systems for rechargeable magnesium batteries journal October 2000
Electrolyte Solutions with a Wide Electrochemical Window for Rechargeable Magnesium Batteries journal January 2008
Battery electrolytes based on saturated ring ionic liquids: Physical and electrochemical properties journal October 2013
Battery Electrolytes Based on Unsaturated Ring Ionic Liquids: Conductivity and Electrochemical Stability journal January 2013
Improved electrolytes for Li-ion batteries: Mixtures of ionic liquid and organic electrolyte with enhanced safety and electrochemical performance journal February 2010
Studies on the Electrodeposition of Magnesium in Ionic Liquids journal January 2008
Mixed electrolyte consisting of ethylmagnesiumbromide with ionic liquid for rechargeable magnesium electrode journal April 2010
Binary ionic liquid electrolytes containing organo-magnesium complex for rechargeable magnesium batteries journal April 2012
Optimization of cation structure of imidazolium-based ionic liquids as ionic solvents for rechargeable magnesium batteries journal November 2010
Room Temperature Magnesium Electrodeposition from Glyme-Coordinated Ammonium Amide Electrolytes journal January 2015
Room-Temperature Electrodeposition of Mg Metal from Amide Salts Dissolved in Glyme-Ionic Liquid Mixture journal December 2013
Electrochemistry of Magnesium Electrolytes in Ionic Liquids for Secondary Batteries journal October 2014
Electrochemical Magnesium Deposition and Dissolution with High Efficiency in Ionic Liquid journal January 2005
Electrodeposition of magnesium film from BMIMBF4 ionic liquid journal September 2006
Reversible deposition and dissolution of magnesium from BMIMBF4 ionic liquid journal November 2005
Complex Nature of Ionic Coordination in Magnesium Ionic Liquid-Based Electrolytes: Solvates with Mobile Mg 2+ Cations journal May 2014
Mechanisms of Magnesium Ion Transport in Pyrrolidinium Bis(trifluoromethanesulfonyl)imide-Based Ionic Liquid Electrolytes journal November 2014
Progress in nonaqueous magnesium electrochemistry journal December 2007
Determination of Mg 2+ Speciation in a TFSI -Based Ionic Liquid With and Without Chelating Ethers Using Raman Spectroscopy journal June 2015
Designer Ionic Liquids for Reversible Electrochemical Deposition/Dissolution of Magnesium journal January 2016
Electrodeposited Bi, Sb and Bi1-xSbx alloys as anodes for Mg-ion batteries journal March 2012
Composite Anodes for Secondary Magnesium Ion Batteries Prepared via Electrodeposition of Nanostructured Bismuth on Carbon Nanotube Substrates journal October 2014
Communication—Sol-Gel Synthesized Magnesium Vanadium Oxide, Mg x V 2 O 5 · nH 2 O: The Role of Structural Mg 2+ on Battery Performance journal January 2016
Sol Gel Based Synthesis and Electrochemistry of Magnesium Vanadium Oxide: A Promising Cathode Material for Secondary Magnesium Ion Batteries journal January 2014
Ionic Liquid Hybrid Electrolytes for Lithium-Ion Batteries: A Key Role of the Separator–Electrolyte Interface in Battery Electrochemistry journal May 2015
Theoretical Analysis on De-Solvation of Lithium, Sodium, and Magnesium Cations to Organic Electrolyte Solvents journal January 2013
Magnesium(II) Bis(trifluoromethane sulfonyl) Imide-Based Electrolytes with Wide Electrochemical Windows for Rechargeable Magnesium Batteries journal March 2014
Solvation of Magnesium Ion in Triglyme-Based Electrolyte Solutions journal August 2015
Inhibition of Electrolyte Oxidation in Lithium Ion Batteries with Electrolyte Additives journal January 2009
Recent progress in high-voltage lithium ion batteries journal September 2013
Synthesis and Properties of Acyclic Ammonium-based Ionic Liquids with Allyl Substituents as Electrolytes journal May 2009
Anodic Stability of Several Anions Examined by Ab Initio Molecular Orbital and Density Functional Theories journal January 2002
Lithium insertion in graphite from ternary ionic liquid-lithium salt electrolytesI. Electrochemical characterization of the electrolytes journal July 2009
Effect of the alkyl group on the synthesis and the electrochemical properties of N-alkyl-N-methyl-pyrrolidinium bis(trifluoromethanesulfonyl)imide ionic liquids journal January 2009
The Influence of Cation Structure on the Chemical–Physical Properties of Protic Ionic Liquids journal April 2016
Electrochemical Stability Window of Imidazolium-Based Ionic Liquids as Electrolytes for Lithium Batteries journal June 2016
Ionic liquids as electrolytes journal August 2006
Operating mechanisms of electrolytes in magnesium ion batteries: chemical equilibrium, magnesium deposition, and electrolyte oxidation journal January 2014
Coordination Chemistry in magnesium battery electrolytes: how ligands affect their performance journal November 2013
The High Performance of Crystal Water Containing Manganese Birnessite Cathodes for Magnesium Batteries journal May 2015
Activation of a MnO 2 cathode by water-stimulated Mg 2+ insertion for a magnesium ion battery journal January 2015
M x Mn 8 O 16 (M = Ag or K) as promising cathode materials for secondary Mg based batteries: the role of the cation M journal January 2016
Investigation of the Mechanism of Mg Insertion in Birnessite in Nonaqueous and Aqueous Rechargeable Mg-Ion Batteries journal January 2016
On the Way to Rechargeable Mg Batteries: The Challenge of New Cathode Materials journal February 2010
Electrochemical Insertion of Magnesium in Metal Oxides and Sulfides from Aprotic Electrolytes journal January 1993
Magnesium insertion electrodes for rechargeable nonaqueous batteries — a competitive alternative to lithium? journal September 1999
Highly Reversible Mg Insertion in Nanostructured Bi for Mg Ion Batteries journal December 2013
Evaluation of Mg[N(SO 2 CF 3 ) 2 ] 2 /Acetonitrile Electrolyte for Use in Mg-Ion Cells journal January 2012

Cited By (1)

Mg Cathode Materials and Electrolytes for Rechargeable Mg Batteries: A Review journal January 2019