Electrochemically-driven formation of Intermetallic Cu3ZnLi2 alters Li-transport in nanostructured bimetallic battery anode

Fuente: arXiv
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Autores principales: Woods, Eric V., Chen, Xinren, Zhang, Yuwei, Prabhakar, J. Manoj, Jovivcevic-Klug, Patricia, Jovivcevic-Klug, Matic, Singh, Mahander P., Zhao, Yujun, Zhang, Siyuan, Zaefferer, Stefan, Liu, Jian, Joshi, Yug, Gault, Baptiste
Formato: Preprint
Publicado: 2025
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author Woods, Eric V.
Chen, Xinren
Zhang, Yuwei
Prabhakar, J. Manoj
Jovivcevic-Klug, Patricia
Jovivcevic-Klug, Matic
Singh, Mahander P.
Zhao, Yujun
Zhang, Siyuan
Zaefferer, Stefan
Liu, Jian
Joshi, Yug
Gault, Baptiste
author_facet Woods, Eric V.
Chen, Xinren
Zhang, Yuwei
Prabhakar, J. Manoj
Jovivcevic-Klug, Patricia
Jovivcevic-Klug, Matic
Singh, Mahander P.
Zhao, Yujun
Zhang, Siyuan
Zaefferer, Stefan
Liu, Jian
Joshi, Yug
Gault, Baptiste
contents The role of Li-based batteries in the electrification of society cannot be understated, however their operational lifetime is often limited by the formation of dendrites, i.e. the localised deposition of Li that can cause shorts between the two electrodes leading to the failure of the battery. Nanocrystalline bimetallic current collectors can be used for anode-free Li-metal batteries, with improved Li plating and limited or suppressed formation of dendrites. Here, we demonstrate that the microstructure of an alpha-Brass current collector, Cu 63% Zn 37%, used in an anode-free Li-metal battery evolves during cycling. It initially had a nanocrystalline deformation layer approximately 80 nm in thickness after polishing. After 100 cycles, the initial deformed brass layer was partially converted to a ternary Laves phase Cu3ZnLi2 within a nanocrystalline brass matrix that grew to 200 - 250 nm in thickness. Upon Li stripping, the phase partially decomposes electrochemically, but what remains can sequester Li thus forming "dead Li" thereby contributing to capacity loss. We propose a mechanism for the microstructural evolution including dynamic recrystallization and phase formation. Since this ternary Laves phase emerges during electrochemical cycling alone, binary alloy current collectors must be assessed for metastable ternary phase formation under different cycling conditions to either stabilize and exploit such phases or electrochemically fully strip them.
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id arxiv_https___arxiv_org_abs_2507_21673
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Electrochemically-driven formation of Intermetallic Cu3ZnLi2 alters Li-transport in nanostructured bimetallic battery anode
Woods, Eric V.
Chen, Xinren
Zhang, Yuwei
Prabhakar, J. Manoj
Jovivcevic-Klug, Patricia
Jovivcevic-Klug, Matic
Singh, Mahander P.
Zhao, Yujun
Zhang, Siyuan
Zaefferer, Stefan
Liu, Jian
Joshi, Yug
Gault, Baptiste
Materials Science
The role of Li-based batteries in the electrification of society cannot be understated, however their operational lifetime is often limited by the formation of dendrites, i.e. the localised deposition of Li that can cause shorts between the two electrodes leading to the failure of the battery. Nanocrystalline bimetallic current collectors can be used for anode-free Li-metal batteries, with improved Li plating and limited or suppressed formation of dendrites. Here, we demonstrate that the microstructure of an alpha-Brass current collector, Cu 63% Zn 37%, used in an anode-free Li-metal battery evolves during cycling. It initially had a nanocrystalline deformation layer approximately 80 nm in thickness after polishing. After 100 cycles, the initial deformed brass layer was partially converted to a ternary Laves phase Cu3ZnLi2 within a nanocrystalline brass matrix that grew to 200 - 250 nm in thickness. Upon Li stripping, the phase partially decomposes electrochemically, but what remains can sequester Li thus forming "dead Li" thereby contributing to capacity loss. We propose a mechanism for the microstructural evolution including dynamic recrystallization and phase formation. Since this ternary Laves phase emerges during electrochemical cycling alone, binary alloy current collectors must be assessed for metastable ternary phase formation under different cycling conditions to either stabilize and exploit such phases or electrochemically fully strip them.
title Electrochemically-driven formation of Intermetallic Cu3ZnLi2 alters Li-transport in nanostructured bimetallic battery anode
topic Materials Science
url https://arxiv.org/abs/2507.21673