Challenges in Lithium Metal Anodes for Solid-State Batteries

Hatzell, Kelsey B.; Chen, Xi Chelsea; Cobb, Corie L.; Dasgupta, Neil P.; Dixit, Marm B.; Marbella, Lauren E.; McDowell, Matthew T.; Mukherjee, Partha P.; Verma, Ankit; Viswanathan, Venkatasubramanian; Westover, Andrew S.; Zeier, Wolfgang G.

doi:10.1021/acsenergylett.9b02668

Challenges in Lithium Metal Anodes for Solid-State Batteries

Journal Article · Mon Feb 17 23:00:00 EST 2020 · ACS Energy Letters

DOI:https://doi.org/10.1021/acsenergylett.9b02668· OSTI ID:1606705

^[1]; ^[2]; Cobb, Corie L. ^[3]; ^[4]; Dixit, Marm B. ^[1]; ^[5]; ^[6]; Mukherjee, Partha P. ^[7]; Verma, Ankit ^[7]; ^[8]; ^[2]; ^[9]

Vanderbilt Univ., Nashville, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Univ. of Washington, Seattle, WA (United States)
Univ. of Michigan, Ann Arbor, MI (United States)
Columbia Univ., New York, NY (United States)
G. W. Woodruff School of Mechanical Engineering, Atlanta, GA (United States); School of Materials Science and Engineering, Atlanta, GA (United States)
Purdue Univ., West Lafayette, IN (United States)
Carnegie Mellon Univ., Pittsburgh, PA (United States)
Justus-Liebig-Univ. Giessen (Germany)

In this Perspective, we highlight recent progress and challenges related to the integration of lithium metal anodes in solid-state batteries. While prior reports have suggested that solid electrolytes may be impermeable to lithium metal, this hypothesis has been disproven under a variety of electrolyte compositions and cycling conditions. Herein, we describe the mechanistic origins and importance of lithium filament growth and interphase formation in inorganic and organic solid electrolytes. Multimodal techniques that combine real and reciprocal space imaging and modeling will be necessary to fully understand nonequilibrium dynamics at these buried interfaces. Currently, most studies on lithium electrode kinetics at solid electrolyte interfaces are completed in symmetric Li–Li configurations. To fully understand the challenges and opportunities afforded by Li-metal anodes, full-cell experiments are necessary. Lastly, the impacts of operating conditions on solid-state batteries are largely unknown with respect to pressure, geometry, and break-in protocols. Given the rapid growth of this community and the diverse portfolio of solid electrolytes, we highlight the need for detailed reporting of experimental conditions and standardization of protocols across the community.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Advanced Research Projects Agency - Energy (ARPA-E); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); National Science Foundation

Grant/Contract Number:: AC05-00OR22725; AR0000774; AR0000775

OSTI ID:: 1606705

Journal Information:: ACS Energy Letters, Journal Name: ACS Energy Letters Journal Issue: 3 Vol. 5; ISSN 2380-8195

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Mechanical Stress Induced Current Focusing and Fracture in Grain Boundaries Barai, Pallab; Higa, Kenneth; Ngo, Anh T. Journal of The Electrochemical Society, Vol. 166, Issue 10 https://doi.org/10.1149/2.0321910jes	journal	January 2019
Lithium Dendrite Growth in Glassy and Rubbery Nanostructured Block Copolymer Electrolytes Schauser, Nicole S.; Harry, Katherine J.; Parkinson, Dilworth Y. Journal of The Electrochemical Society, Vol. 162, Issue 3 https://doi.org/10.1149/2.0511503jes	journal	December 2014
Impact of External Pressure and Electrolyte Transport Properties on Lithium Dendrite Growth Barai, Pallab; Higa, Kenneth; Srinivasan, Venkat Journal of The Electrochemical Society, Vol. 165, Issue 11 https://doi.org/10.1149/2.0651811jes	journal	January 2018
Evaluating the Effects of Temperature and Pressure on Li/PEO-LiTFSI Interfacial Stability and Kinetics Gupta, A.; Kazyak, E.; Craig, N. Journal of The Electrochemical Society, Vol. 165, Issue 11 https://doi.org/10.1149/2.0901811jes	journal	January 2018
Mesoscale Analysis of the Electrolyte-Electrode Interface in All-Solid-State Li-Ion Batteries Hao, Feng; Mukherjee, Partha P. Journal of The Electrochemical Society, Vol. 165, Issue 9 https://doi.org/10.1149/2.1251809jes	journal	January 2018
Lithium Metal Penetration Induced by Electrodeposition through Solid Electrolytes: Example in Single-Crystal Li ₆ La ₃ ZrTaO ₁₂ Garnet Swamy, Tushar; Park, Richard; Sheldon, Brian W. Journal of The Electrochemical Society, Vol. 165, Issue 16 https://doi.org/10.1149/2.1391814jes	journal	January 2018
Nanoindentation of high-purity vapor deposited lithium films: A mechanistic rationalization of diffusion-mediated flow Herbert, Erik G.; Hackney, Stephen A.; Thole, Violet Journal of Materials Research, Vol. 33, Issue 10 https://doi.org/10.1557/jmr.2018.84	journal	May 2018
Nanoindentation of high-purity vapor deposited lithium films: A mechanistic rationalization of the transition from diffusion to dislocation-mediated flow Herbert, Erik G.; Hackney, Stephen A.; Thole, Violet Journal of Materials Research, Vol. 33, Issue 10 https://doi.org/10.1557/jmr.2018.85	journal	May 2018

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