Water or Anion? Uncovering the Zn2+ Solvation Environment in Mixed Zn(TFSI)2 and LiTFSI Water-in-Salt Electrolytes
- Yong ZhangYong ZhangDepartment of Chemical and Biomolecular Engineering, University of Notre Dame, Notre Dame, Indiana 46556, United StatesJoint Center for Energy Storage Research, Argonne National Laboratory, Lemont, Illinois 60439, United StatesMore by Yong Zhang
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- Gang WanGang WanStanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, California 94025, United StatesJoint Center for Energy Storage Research, Argonne National Laboratory, Lemont, Illinois 60439, United StatesMore by Gang Wan
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- Nicholas H. C. LewisNicholas H. C. LewisDepartment of Chemistry, James Franck Institute, and Institute for Biophysical Dynamics, The University of Chicago, Chicago, Illinois 60637, United StatesJoint Center for Energy Storage Research, Argonne National Laboratory, Lemont, Illinois 60439, United StatesMore by Nicholas H. C. Lewis
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- Julian MarsJulian MarsDepartment of Chemical and Biological Engineering, University of Colorado Boulder, Boulder, Colorado 80303, United StatesJoint Center for Energy Storage Research, Argonne National Laboratory, Lemont, Illinois 60439, United StatesMore by Julian Mars
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- Sharon E. BoneSharon E. BoneStanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, California 94025, United StatesMore by Sharon E. Bone
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- Hans-Georg SteinrückHans-Georg SteinrückDepartment of Chemistry, Paderborn University, Paderborn 33098, GermanyMore by Hans-Georg Steinrück
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- Maria R. LukatskayaMaria R. LukatskayaDepartment of Mechanical and Process Engineering, ETH Zurich, Zurich 8092, SwitzerlandMore by Maria R. Lukatskaya
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- Nicholas J. WeadockNicholas J. WeadockDepartment of Chemical and Biological Engineering, University of Colorado Boulder, Boulder, Colorado 80303, United StatesMore by Nicholas J. Weadock
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- Michal BajdichMichal BajdichSUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, Menlo Park, California 94025, United StatesMore by Michal Bajdich
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- Oleg BorodinOleg BorodinElectrochemistry Branch, Senior and Electron Devices Directorate, Power and Energy Division, U.S. Army Research Laboratory, Adelphi, Maryland 20783, United StatesJoint Center for Energy Storage Research, Argonne National Laboratory, Lemont, Illinois 60439, United StatesMore by Oleg Borodin
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- Andrei Tokmakoff*Andrei Tokmakoff*Email: [email protected]Department of Chemistry, James Franck Institute, and Institute for Biophysical Dynamics, The University of Chicago, Chicago, Illinois 60637, United StatesJoint Center for Energy Storage Research, Argonne National Laboratory, Lemont, Illinois 60439, United StatesMore by Andrei Tokmakoff
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- Michael F. Toney*Michael F. Toney*Email: [email protected]Department of Chemical and Biological Engineering, University of Colorado Boulder, Boulder, Colorado 80303, United StatesJoint Center for Energy Storage Research, Argonne National Laboratory, Lemont, Illinois 60439, United StatesMore by Michael F. Toney
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- Edward J. Maginn*Edward J. Maginn*Email: [email protected]Department of Chemical and Biomolecular Engineering, University of Notre Dame, Notre Dame, Indiana 46556, United StatesJoint Center for Energy Storage Research, Argonne National Laboratory, Lemont, Illinois 60439, United StatesMore by Edward J. Maginn
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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