TY - JOUR
T1 - Rethinking how external pressure can suppress dendrites in lithium metal batteries
AU - Zhang, Xin
AU - Wang, Q. Jane
AU - Harrison, Katharine L.
AU - Jungjohann, Katherine
AU - Boyce, Brad L.
AU - Roberts, Scott A.
AU - Attia, Peter M.
AU - Harris, Stephen J.
N1 - Funding Information:
The authors acknowledge Prof. Y.T. Cheng of University of Kentucky, Prof. Brian Sheldon of Brown University, and Prof. Craig Arnold of Princeton University for valuable discussions. S.J.H. was supported by the Assistant Secretary for Energy Efficiency, Vehicle Technologies Office of the US Department of Energy under the Advanced Battery Materials Research Program. K.L.H, K.L.J., and B.L.B were supported by the Laboratory Directed Research and Development program at Sandia National Laboratories, a multi-mission 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-NA0003525.
Funding Information:
The authors acknowledge Prof. Y.T. Cheng of University of Kentucky, Prof. Brian Sheldon of Brown University, and Prof. Craig Arnold of Princeton University for valuable discussions. S.J.H. was supported by the Assistant Secretary for Energy Efficiency, Vehicle Technologies Office of the US Department of Energy under the Advanced Battery Materials Research Program. K.L.H, K.L.J., and B.L.B were supported by the Laboratory Directed Research and Development program at Sandia National Laboratories, a multi-mission 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-NA0003525.
Publisher Copyright:
© The Author(s) 2019. Published by ECS.
PY - 2019
Y1 - 2019
N2 - We offer an explanation for how dendrite growth can be inhibited when Li metal pouch cells are subjected to external loads, even for cells using soft, thin separators. We develop a contact mechanics model for tracking Li surface and sub-surface stresses where electrodes have realistically (micron-scale) rough surfaces. Existing models examine a single, micron-scale Li metal protrusion under a fixed local current density that presses more or less conformally against a separator or stiff electrolyte. At the larger, sub-mm scales studied here, contact between the Li metal and the separator is heterogeneous and far from conformal for surfaces with realistic roughness: the load is carried at just the tallest asperities, where stresses reach tens of MPa, while most of the Li surface feels no force at all. Yet, dendrite growth is suppressed over the entire Li surface. To explain this dendrite suppression, our electrochemical/mechanics model suggests that Li avoids plating at the tips of growing Li dendrites if there is sufficient local stress; that local contact stresses there may be high enough to close separator pores so that incremental Li+ ions plate elsewhere; and that creep ensures that Li protrusions are gradually flattened. These mechanisms cannot be captured by single-dendrite-scale analyses.
AB - We offer an explanation for how dendrite growth can be inhibited when Li metal pouch cells are subjected to external loads, even for cells using soft, thin separators. We develop a contact mechanics model for tracking Li surface and sub-surface stresses where electrodes have realistically (micron-scale) rough surfaces. Existing models examine a single, micron-scale Li metal protrusion under a fixed local current density that presses more or less conformally against a separator or stiff electrolyte. At the larger, sub-mm scales studied here, contact between the Li metal and the separator is heterogeneous and far from conformal for surfaces with realistic roughness: the load is carried at just the tallest asperities, where stresses reach tens of MPa, while most of the Li surface feels no force at all. Yet, dendrite growth is suppressed over the entire Li surface. To explain this dendrite suppression, our electrochemical/mechanics model suggests that Li avoids plating at the tips of growing Li dendrites if there is sufficient local stress; that local contact stresses there may be high enough to close separator pores so that incremental Li+ ions plate elsewhere; and that creep ensures that Li protrusions are gradually flattened. These mechanisms cannot be captured by single-dendrite-scale analyses.
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U2 - 10.1149/2.0701914jes
DO - 10.1149/2.0701914jes
M3 - Article
AN - SCOPUS:85076099347
SN - 0013-4651
VL - 166
SP - A3639-A3652
JO - Journal of the Electrochemical Society
JF - Journal of the Electrochemical Society
IS - 15
ER -