A Key concept in Magnesium Secondary Battery Electrolytes.
A critical roadblock toward practical Mg-based energy storage technologies is the lack of reversible electrolytes that are safe and electrochemically stable. Here, we report on high-performance electrolytes based on 1-ethyl-3-methylimidazolium chloride (EMImCl) doped with AlCl3 and highly amorphous δ-MgCl2 . The phase diagram of the electrolytes reveals the presence of four thermal transitions that strongly depend on salt content. High-level density functional theory (DFT)-based electronic structure calculations substantiate the structural and vibrational assignment of the coordination complexes. A 3D chloride-concatenated dynamic network model accounts for the outstanding redox behaviour and the electric and magnetic properties, providing insight into the conduction mechanism of the electrolytes. Mg anode cells assembled using the electrolytes were cyclically discharged at a high rate (35 mA g(-1) ), exhibiting an initial capacity of 80 mA h g(-1) and a steady-state voltage of 2.3 V.
Department of Chemical Sciences, University of Padua, Via Marzolo 1, 35131 Padua (Italy).|Department of Industrial Engineering, Section of Chemistry for Technology, University of Padua, Via Gradenigo 6/a, 35131 Padua (Italy).
Federico
F
Bertasi
Energy Nanotechnology and Materials Chemistry Lab, Medgar Evers College and Graduate Center of the City University of New York, 1638 Bedford Avenue, Brooklyn, NY 11225 (USA).
Chaminda
C
Hettige
Department of Chemical and Biomolecular Engineering, University of Tennessee, 419 Dougherty Engineering Bldg. Knoxville, TN 37996-2200 (USA).
Fatemeh
F
Sepehr
Department of Physics, Hunter College and Graduate Center of the City University of New York, 695 Park Avenue, New York, NY 10021 (USA).
Xavier
X
Bogle
Department of Chemical Sciences, University of Padua, Via Marzolo 1, 35131 Padua (Italy).|Department of Industrial Engineering, Section of Chemistry for Technology, University of Padua, Via Gradenigo 6/a, 35131 Padua (Italy).
Gioele
G
Pagot
Department of Industrial Engineering, Section of Chemistry for Technology, University of Padua, Via Gradenigo 6/a, 35131 Padua (Italy).|Veneto Nanotech S.C.p.a., Via San Crispino 106, I-35129 Padua (Italy).
Keti
K
Vezzù
Department of Chemical Sciences, University of Padua, Via Marzolo 1, 35131 Padua (Italy).|Department of Industrial Engineering, Section of Chemistry for Technology, University of Padua, Via Gradenigo 6/a, 35131 Padua (Italy).
Enrico
E
Negro
Department of Chemical and Biomolecular Engineering, University of Tennessee, 419 Dougherty Engineering Bldg. Knoxville, TN 37996-2200 (USA).
Stephen J
SJ
Paddison
Department of Physics, Hunter College and Graduate Center of the City University of New York, 695 Park Avenue, New York, NY 10021 (USA).
Steve G
SG
Greenbaum
Energy Nanotechnology and Materials Chemistry Lab, Medgar Evers College and Graduate Center of the City University of New York, 1638 Bedford Avenue, Brooklyn, NY 11225 (USA).
Michele
M
Vittadello
Department of Chemical Sciences, University of Padua, Via Marzolo 1, 35131 Padua (Italy). vito.dinoto@unipd.it.|Department of Industrial Engineering, Section of Chemistry for Technology, University of Padua, Via Gradenigo 6/a, 35131 Padua (Italy). vito.dinoto@unipd.it.
Vito
V
Di Noto
batteries; conduction mechanism; electrolytes; ionic liquids; magnesium