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Title: MetILs3: A Strategy for High Density Energy Storage Using Redox-Active Ionic Liquids

Journal Article · · Advanced Sustainable Systems

A systematic approach is presented for increasing the concentration of redox‐active species in electrolytes for nonaqueous redox flow batteries (RFBs). Starting with an ionic liquid consisting of a metal coordination cation (MetIL), ferrocene‐containing ligands and iodide anions are substituted incrementally into the structure. While chemical structures can be drawn for molecules with 10 m redox‐active electrons (RAE), practical limitations such as melting point and phase stability constrain the structures to 4.2 m RAE, a 2.3× improvement over the original MetIL. Dubbed “MetILs 3 ,” these ionic liquids possess redox activity in the cation core, ligands, and anions. Throughout all compositions, infrared spectroscopy shows the ethanolamine‐based ligands primarily coordinate to the Fe 2+ core via hydroxyl groups. Calorimetry conveys a profound change in thermophysical properties, not only in melting temperature but also in suppression of a cold crystallization only observed in the original MetIL. Square wave voltammetry reveals redox processes characteristic of each molecular location. Testing a laboratory‐scale RFB demonstrates Coulombic efficiencies >95% and increased voltage efficiencies due to more facile redox kinetics, effectively increasing capacity 4×. Application of this strategy to other chemistries, optimizing melting point and conductivity, can yield >10 m RAE, making nonaqueous RFB a viable technology for grid scale storage.

Research Organization:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Organization:
USDOE National Nuclear Security Administration (NNSA); USDOE Office of Electricity (OE)
Grant/Contract Number:
AC04-94AL85000; NA0003525
OSTI ID:
1398783
Alternate ID(s):
OSTI ID: 1378388
Report Number(s):
SAND-2017-10038J; 657059
Journal Information:
Advanced Sustainable Systems, Vol. 1, Issue 9; ISSN 2366-7486
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 10 works
Citation information provided by
Web of Science

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Cited By (3)

Effects of chain length on the size, stability, and electronic structure of redox-active organic–inorganic hybrid polyoxometalate micelles journal January 2019
Synthesis, Crystal Structures, and Thermal Properties of Protic Metal-Containing Ionic Liquids, Diethanolammonium Halometallates: (HOCH2CH2)2NH2FeCl4 and ((HOCH2CH2)2NH2)2CoCl4 journal April 2020
Crossover in Membranes for Aqueous Soluble Organic Redox Flow Batteries journal January 2019