Electrical resistance of the current collector controls lithium morphology

Solomon T. Oyakhire, Wenbo Zhang, Andrew Shin, Rong Xu, David T. Boyle, Zhiao Yu, Yusheng Ye, Yufei Yang, James A. Raiford, William Huang, Joel R. Schneider, Yi Cui () and Stacey F. Bent ()
Additional contact information
Solomon T. Oyakhire: Stanford University
Wenbo Zhang: Stanford University
Andrew Shin: Stanford University
Rong Xu: Stanford University
David T. Boyle: Stanford University
Zhiao Yu: Stanford University
Yusheng Ye: Stanford University
Yufei Yang: Stanford University
James A. Raiford: Stanford University
William Huang: Stanford University
Joel R. Schneider: Stanford University
Yi Cui: Stanford University
Stacey F. Bent: Stanford University

Nature Communications, 2022, vol. 13, issue 1, 1-12

Abstract: Abstract The electrodeposition of low surface area lithium is critical to successful adoption of lithium metal batteries. Here, we discover the dependence of lithium metal morphology on electrical resistance of substrates, enabling us to design an alternative strategy for controlling lithium morphology and improving electrochemical performance. By modifying the current collector with atomic layer deposited conductive (ZnO, SnO2) and resistive (Al2O3) nanofilms, we show that conductive films promote the formation of high surface area lithium deposits, whereas highly resistive films promote the formation of lithium clusters of low surface area. We reveal an electrodeposition mechanism in which radial diffusion of electroactive species is promoted on resistive substrates, resulting in lateral growth of large (150 µm in diameter) planar lithium deposits. Using resistive substrates, similar lithium morphologies are formed in three distinct classes of electrolytes, resulting in up to ten-fold improvement in battery performance. Ultimately, we report anode-free pouch cells using the Al2O3-modified copper that maintain 60 % of their initial discharge capacity after 100 cycles, displaying the benefits of resistive substrates for controlling lithium electrodeposition.

Date: 2022
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DOI: 10.1038/s41467-022-31507-w

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