TY - JOUR
T1 - Stability of Solid Electrolyte Interphase Components on Lithium Metal and Reactive Anode Material Surfaces
AU - Leung, Kevin
AU - Soto, Fernando
AU - Hankins, Kie
AU - Balbuena, Perla B.
AU - Harrison, Katharine L.
N1 - Funding Information:
We thank Oleg Borodin, Byron Konstantinos Antonopoulos, Wentao Song, and Janice Reutt-Robey for discussions and input. Sandia National Laboratories is a multiprogram 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. This work was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231, Subcontract No. 7060634 under the Advanced Batteries Materials Research (BMR) Program.
Publisher Copyright:
© 2016 American Chemical Society.
PY - 2016/3/31
Y1 - 2016/3/31
N2 - Lithium ion batteries (LIB) can feature reactive anodes that operate at low potentials, such as lithium metal or silicon, passivated by solid electrolyte interphase (SEI) films. SEI is known to evolve over time as cycling proceeds. In this modeling work, we focus on the stability of two main SEI components, lithium carbonate (Li2CO3) and lithium ethylene dicarbonate (LEDC). Both components are electrochemically stable but thermodynamically unstable near the equilibrium Li+/Li(s) potential. Interfacial reactions represent one way to trigger the intrinsic thermodynamic instability. Both Li2CO3 and LEDC are predicted to exhibit exothermic reactions on lithium metal surfaces, and the barriers are sufficiently low to permit reactions on battery operation time scales. LEDC also readily decomposes on high Li-content LixSi surfaces. Our studies suggest that the innermost SEI layer on lithium metal surfaces should be a thin layer of Li2O, the only thermodynamically and kinetically stable component (in the absence of a fluoride source). This work should also be relevant to inadvertent lithium plating during battery cycling and SEI evolution on LixSi surfaces. (Chemical Equation Presented).
AB - Lithium ion batteries (LIB) can feature reactive anodes that operate at low potentials, such as lithium metal or silicon, passivated by solid electrolyte interphase (SEI) films. SEI is known to evolve over time as cycling proceeds. In this modeling work, we focus on the stability of two main SEI components, lithium carbonate (Li2CO3) and lithium ethylene dicarbonate (LEDC). Both components are electrochemically stable but thermodynamically unstable near the equilibrium Li+/Li(s) potential. Interfacial reactions represent one way to trigger the intrinsic thermodynamic instability. Both Li2CO3 and LEDC are predicted to exhibit exothermic reactions on lithium metal surfaces, and the barriers are sufficiently low to permit reactions on battery operation time scales. LEDC also readily decomposes on high Li-content LixSi surfaces. Our studies suggest that the innermost SEI layer on lithium metal surfaces should be a thin layer of Li2O, the only thermodynamically and kinetically stable component (in the absence of a fluoride source). This work should also be relevant to inadvertent lithium plating during battery cycling and SEI evolution on LixSi surfaces. (Chemical Equation Presented).
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U2 - 10.1021/acs.jpcc.5b11719
DO - 10.1021/acs.jpcc.5b11719
M3 - Article
AN - SCOPUS:84963535701
SN - 1932-7447
VL - 120
SP - 6302
EP - 6313
JO - Journal of Physical Chemistry C
JF - Journal of Physical Chemistry C
IS - 12
ER -
