H-Cell Evaluation of Electrolyte Solvation Energies in the Presence of Silicon Electrodes

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Poor calendar life of Li-ion batteries with silicon anodes has been identified as an important obstacle that must be addressed for silicon to be fully commercialized in applications such as electric vehicles. The silicon-electrolyte interface likely plays a key role in calendar life performance since silicon’s reactivity and unstable solid electrolyte interphase (SEI) may lead to increased lithium loss and self discharge. New electrolytes that will better stabilize the SEI are a promising direction to improve calendar life. We hypothesize that the solvation energy of lithium ions in the electrolyte is related to observed lifetimes. Here, we use an H-cell, demonstrated previously as a method to quantify relative solvation energies of Li-ions in promising electrolytes to improve silicon calendar life and compare to performance data. We observe that the solvation energy is dependent on the electrode present, giving further credence to the need to optimize the electrolyte specifically for silicon anodes, accounting for both cycle and calendar life.Sandia National Laboratories is a multimission laboratory managed and operated by the National Technology and Engineering Solutions of Sandia, LLC (NTESS), a wholly owned subsidiary of Honeywell International Inc., for the U.S. Department of Energy’s National Nuclear Security Administration (DOE/NNSA) under contract DE-NA0003525. This written work is authored by an employee of NTESS. The employee, not NTESS, owns the right, title and interest in and to the written work and is responsible for its contents. Any subjective views or opinions that might be expressed in the written work do not necessarily represent the views of the U.S. Government. The publisher acknowledges that the U.S. Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this written work or allow others to do so, for U.S. Government purposes. The DOE will provide public access to results of federally sponsored research in accordance with the DOE Public Access Plan. Figure 1