Journal
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
Volume 22, Issue 19, Pages 10412-10425Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c9cp06485k
Keywords
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Funding
- Nanostructures for Electrical Energy Storage (NEES), an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DESC0001160]
- Laboratory Directed Research and Development Program at Sandia National Laboratories
- U.S. Department of Energy National Nuclear Security Administration [DE-NA0003525]
- Advanced Strategic Computing (ASC) Program
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Density Functional Theory (DFT) calculations of electrode material properties in high energy density storage devices like lithium batteries have been standard practice for decades. In contrast, DFT modelling of explicit interfaces in batteries arguably lacks universally adopted methodology and needs further conceptual development. In this paper, we focus on solid-solid interfaces, which are ubiquitous not just in all-solid state batteries; liquid-electrolyte-based batteries often rely on thin, solid passivating films on electrode surfaces to function. We use metal anode calculations to illustrate that explicit interface models are critical for elucidating contact potentials, electric fields at interfaces, and kinetic stability with respect to parasitic reactions. The examples emphasize three key challenges: (1) the dirty nature of most battery electrode surfaces; (2) voltage calibration and control; and (3) the fact that interfacial structures are governed by kinetics, not thermodynamics. To meet these challenges, developing new computational techniques and importing insights from other electrochemical disciplines will be beneficial.
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