Solid-liquid interfaces are critical to battery operations. Using our ab initio molecular dynamics simulations (AIMD) of interfaces at lithium ion battery cathode and anode surfaces as illustrations, we discuss the challenges associated with such modeling efforts. These challenges include the need to deal with side reactions and surface films; the difficulty in controlling voltages, especially for small-polaron-conducting cathode materiacsals; and the lack of a Grand Canonical Ensemble method to control lithium content. We also apply AIMD and MD techniques to study interfaces associated with less conventional batteries and electrolytes, such as water-in-salt in contact with spinel Li(x)Mn(2)O(4), and organic solvent-based redox flow batteries. The unusual acid-base reactions and electric double layer behavior revealed in the simulations provide impetus for future experimental studies.<br/><br/>Sandia National Laboratories is a multi-mission laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000. KL was supported by Nanostructures for Electrical Energy Storage (NEES), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Award Number DESC0001160.

Modeling solid-liquid interfaces in batteries: Degradation/acid-base reactions, electric double layers, and challenges

254th National Meeting (2017)

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