journal article·2017-10-24

Liquid Structure with Nano-Heterogeneity Promotes Cationic Transport in Concentrated Electrolytes

Oleg Borodin, Liumin Suo, Mallory Gobet, Xiaoming Ren, Fei Wang, Antonio Faraone, Jing Peng, Marco Olguin, Marshall Schroeder, Michael S. Ding, Eric Gobrogge, Arthur von Wald Cresce, Stephen Munoz, Joseph A. Dura, Steve Greenbaum, Chunsheng Wang, Kang Xu

ACS Nano· Volume 11· Issue 10
Publisher page

Abstract

Using molecular dynamics simulations, small-angle neutron scattering, and a variety of spectroscopic techniques, we evaluated the ion solvation and transport behaviors in aqueous electrolytes containing bis(trifluoromethanesulfonyl)imide. We discovered that, at high salt concentrations (from 10 to 21 mol/kg), a disproportion of cation solvation occurs, leading to a liquid structure of heterogeneous domains with a characteristic length scale of 1 to 2 nm. This unusual nano-heterogeneity effectively decouples cations from the Coulombic traps of anions and provides a 3D percolating lithium-water network, via which 40% of the lithium cations are liberated for fast ion transport even in concentration ranges traditionally considered too viscous. Due to such percolation networks, superconcentrated aqueous electrolytes are characterized by a high lithium-transference number (0.73), which is key to supporting an assortment of battery chemistries at high rate. The in-depth understanding of this transport mechanism establishes guiding principles to the tailored design of future superconcentrated electrolyte systems.
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Research context

OpenAlex topics: Advanced Battery Materials and Technologies · Advancements in Battery Materials · Advanced battery technologies research

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Electrochemistry Branch, Sensor and Electron Devices Directorate, U.S. Army Research Laboratory, Adelphi, Maryland 20783, United States

Key Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, School of Physical Sciences, University of Chinese Academy of Sciences, Beijing 100190, China

Department of Chemical and Biomolecular Engineering, University of Maryland, College Park, Maryland 20742, United States

Department of Physics and Astronomy, Hunter College, City University of New York, New York, New York 10065, United States

NIST Center for Neutron Research, National Institute of Standards and Technology, Gaithersburg, Maryland 20899-6100, United States

Funding

National Institute of Standards and Technology · University of Maryland · Advanced Research Projects Agency · Oak Ridge Associated Universities · Army Research Laboratory

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