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From ion to atom to dendrite: Formation and nanomechanical behavior of electrodeposited lithium

Published online by Cambridge University Press:  09 July 2020

Michael A. Citrin ,
Heng Yang ,
Simon K. Nieh ,
Joel Berry ,
Wenpei Gao ,
Xiaoqing Pan ,
David J. Srolovitz  and
Julia R. Greer
Michael A. Citrin
Affiliation:
Division of Engineering and Applied Science, California Institute of Science and Technology, USA
Heng Yang
Affiliation:
Division of Engineering and Applied Science, California Institute of Science and Technology, USA
Simon K. Nieh
Affiliation:
Front Edge Technology, Baldwin Park, USA
Joel Berry
Affiliation:
Department of Materials Science and Engineering, University of Pennsylvania; Materials Science Division, Lawrence Livermore National Laboratory, Livermore, USA
Wenpei Gao
Affiliation:
Department of Chemical Engineering and Materials Science, University of California, Irvine, USA
Xiaoqing Pan
Affiliation:
Department of Chemical Engineering and Materials Science, University of California, Irvine; Department of Physics and Astronomy, University of California, Irvine, USA
David J. Srolovitz
Affiliation:
Department of Materials Science and Engineering, City University of Hong Kong, Hong Kong SAR
Julia R. Greer*
Affiliation:
Division of Engineering and Applied Science, California Institute of Science and Technology; jrgreer@caltech.edu
*
*Corresponding author.
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Abstract

Development of high energy density solid-state batteries with Li metal anodes has been limited by uncontrollable growth of Li dendrites in liquid and solid electrolytes (SEs). This, in part, may be caused by a dearth of information about mechanical properties of Li, especially at the nano- and microlength scales and microstructures relevant to Li batteries. We investigate Li electrodeposited in a commercial LiCoO2/LiPON/Cu solid-state thin-film cell, grown in situ in a scanning electron microscope equipped with nanomechanical capabilities. Experiments demonstrate that Li was preferentially deposited at the LiPON/Cu interface along the valleys that mimic the domain boundaries of underlying LiCoO2 (cathode). Cryogenic electron microscopy analysis of electrodeposited Li revealed a single-crystalline microstructure, and in situ nanocompression experiments on nano-pillars with 360–759 nm diameters revealed their average Young's modulus to be 6.76 ± 2.88 GPa with an average yield stress of 16.0 ± 6.82 MPa, ~24x higher than what has been reported for bulk polycrystalline Li. We discuss mechanical deformation mechanisms, stiffness, and strength of nano-sized electrodeposited Li in the framework of its microstructure and dislocation-governed nanoscale plasticity of crystals, and place it in the parameter space of existing knowledge on small-scale Li mechanics. The enhanced strength of Li at small scales may explain why it can penetrate and fracture through much stiffer and harder SEs than theoretically predicted.

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MRS Bulletin , Volume 45 , Issue 11: Processing Metallic Materials Far from Equilibrium , November 2020 , pp. 891 - 904
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Copyright © The Author(s), 2020, published on behalf of Materials Research Society by Cambridge University Press

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