Chemical/electrochemical reactions at solid-solid interfaces are ubiquitous in lithium ion and other high energy batteries. Both solid- and liquid-electrolyte battery electrode surfaces can feature "solid electrolyte interphase" films which come from chemical and/or electrochemical reactions between electrode and electrolytes. The formation and evolution of these films are generally kinetically controlled, and the atomic lengthscale interfacial structure and electric fields present govern lithium transport and degradation. Since buried solid-solid interfaces are challenging to probe, electronic structure calculations are useful guides. In this presentation, we predict the reaction rates at the interfaces of electrode materials and lithium carbonate (from liquid electrolytes) and LiPON (a solid electrolyte), and make corroborative comparison with measurements. Particular attention will be paid to the potential dependence. We will further discuss the calculation of voltages and overpotentials, which has been a source of confusion in electronic structure simulation of interfaces.

Simulating electrochemical evolutions of interfaces/interphases in batteries, and modeling their potential dependences

256th National Meeting (2018)

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