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

Citrin, Michael A. and Yang, Heng and Nieh, Simon K. and Berry, Joel and Gao, Wenpei and Pan, Xiaoqing and Srolovitz, David J. and Greer, Julia R. (2020) From ion to atom to dendrite: Formation and nanomechanical behavior of electrodeposited lithium. MRS Bulletin, 45 (11). pp. 891-904. ISSN 0883-7694. doi:10.1557/mrs.2020.148.

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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.

Item Type:Article
Related URLs:
URLURL TypeDescription
Citrin, Michael A.0000-0001-8183-5437
Yang, Heng0000-0001-7431-932X
Gao, Wenpei0000-0002-2776-2676
Pan, Xiaoqing0000-0002-0965-8568
Srolovitz, David J.0000-0001-6038-020X
Greer, Julia R.0000-0002-9675-1508
Additional Information:© The Author(s), 2020, published on behalf of Materials Research Society by Cambridge University Press. Submitted February 6, 2020; Accepted April 10, 2020. Published online by Cambridge University Press: 09 July 2020. The authors would like to acknowledge the generous financial support from the ARPA-E IDEAS Grant No. DE-AR0000884. Part of J.B.'s contribution was performed under the auspices of the US Department of Energy by Lawrence Livermore National Laboratory under Contract No. DE-AC52-07NA27344. We also acknowledge A. Malyutin and S. Mageswaran for their help and discussions on performing TEM, and O. Tertuliano, C. Portela, and J. Zhang for their invaluable help and discussions about the mechanical experiments. The authors acknowledge X. Xia for his help with the SEM electrochemical experiments. J.B. acknowledges useful discussions with A. Fang.
Funding AgencyGrant Number
Advanced Research Projects Agency-Energy (ARPA-E)DE-AR0000884
Department of Energy (DOE)DE-AC52-07NA27344
Issue or Number:11
Record Number:CaltechAUTHORS:20200713-102704003
Persistent URL:
Official Citation:Citrin, M., Yang, H., Nieh, S., Berry, J., Gao, W., Pan, X., . . . Greer, J. (2020). From ion to atom to dendrite: Formation and nanomechanical behavior of electrodeposited lithium. MRS Bulletin, 45(11), 891-904. doi:10.1557/mrs.2020.148
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:104353
Deposited By: Tony Diaz
Deposited On:13 Jul 2020 19:01
Last Modified:16 Nov 2021 18:30

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