DataVXACS Energy LettersPaper
journal article·2021-10-08Open access

Water or Anion? Uncovering the Zn2+ Solvation Environment in Mixed Zn(TFSI)2 and LiTFSI Water-in-Salt Electrolytes

Yong Zhang, Gang Wan, Nicholas H. C. Lewis, Julian Mars, Sharon E. Bone, Hans-Georg Steinrück, Maria R. Lukatskaya, Nicholas J. Weadock, Michal Bajdich, Oleg Borodin, Andrei Tokmakoff, Michael F. Toney, Edward J. Maginn

ACS Energy Letters· Volume 6· Issue 10
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Source abstract

Abstract

Applications of aqueous zinc batteries for grid-scale energy storage are limited by their poor reversibility and the competing water splitting reaction. The recent invention of a water-in-salt (WIS) electrolyte concept provides a new route enabling a stable and highly reversible aqueous zinc battery chemistry. In the present work, a mixed zinc bis(trifluoromethane sulfonyl)imide (Zn(TFSI)2) and LiTFSI WIS electrolyte was studied using X-ray total scattering, X-ray absorption, and Fourier transform infrared spectroscopy in conjunction with classical molecular dynamics simulations. It was found that, in the highly concentrated WIS electrolyte consisting of 1 m Zn(TFSI)2 and 20 m LiTFSI, Zn2+ cations are mainly solvated by six waters in their first solvation shell, while the TFSI– anions are completely excluded. This ion solvation picture is fundamentally different from the previous understandings. The results suggest that additional studies are needed to fully understand the unusual stability and reversibility of zinc-WIS electrolyte-based batteries.
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Research context

Energy storage

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

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

Affiliations

Department of Chemical and Biomolecular Engineering, University of Notre Dame, Notre Dame, Indiana 46556, United States

Joint Center for Energy Storage Research, Argonne National Laboratory, Lemont, Illinois 60439, United States

Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, California 94025, United States

Department of Chemistry, James Franck Institute, and Institute for Biophysical Dynamics, The University of Chicago, Chicago, Illinois 60637, United States

Department of Chemical and Biological Engineering, University of Colorado Boulder, Boulder, Colorado 80303, United States

Department of Chemistry, Paderborn University, Paderborn 33098, Germany

Department of Mechanical and Process Engineering, ETH Zurich, Zurich 8092, Switzerland

SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, Menlo Park, California 94025, United States

Electrochemistry Branch, Senior and Electron Devices Directorate, Power and Energy Division, U.S. Army Research Laboratory, Adelphi, Maryland 20783, United States

Funding

Office of Science

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