Abstract
To meet the ever-growing need for high capacity, fast-charge batteries, lithium anodes have been considered a direct upgrade to previous commercial anode materials thanks to their high gravimetric density and low coulombic efficiency. However, their implementation into crucial applications such as electric vehicles has been hindered by safety issues during and at the end of their operational lifetime. Over hundreds of cycles, nonhomogeneous plating and stripping of lithium on the anode surface encourages the growth of dendrites, which eventually lead to capacity loss, cell failure, and fire. The application of stack pressure has been found to mitigate dendrite growth to an extent; however, the impacts of long-term pressure application on lithium deposition, and subsequent lithium plastic deformation and creep, are not well understood. In this work, we present a novel method for accurately modeling the interplay between mechanical deformation and electrochemical deposition. We develop a 3D, finite-element, transient model of lithium plating and stripping at the mesoscale. A stack pressure is applied to a lithium anode in contact with a polymer separator, and the electrochemical response to an applied current density is evaluated. The lithium protrusion is then reshaped to model incremental plating or stripping, thus simulating the cumulative interfacial movement over a full charge-discharge cycle. Mechanical complexities of the materials, such as lithium plastic deformation and separator porosity, are accounted for. The interfacial response is studied with respect to applied stack pressure and assumed lithium yield strength. Through this work, the impacts of stack pressure on dendrite growth at the microscale are explored. The lithium yield strength assumption is found to be crucial for accurately predicting deposition behavior.Supported by the Laboratory Directed Research and Development program at Sandia National Laboratories, a multimission laboratory managed and operated by National Technology and Engineering Solutions of Sandia, LLC., a wholly owned subsidiary of Honeywell International, Inc., for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-NA-0003525.
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