Alloying Interlayers for Anode‐Less Lithium‐Metal Polymer Batteries

Anode‐less lithium‐metal batteries potentially offer further increased energy densities. However, the Coulombic efficiency (CE) of lithium plating and stripping, as a classical measure of Li inventory reversibility, is commonly still insufficient for achieving long‐lasting rechargeable batteries. Herein, the potential benefits of employing thin (20 nm) metal interlayers of Ag, Pt, and Au on Cu to alloy with Li in Cu||Li half‐cells and induce homogeneous Li plating with poly(ethylene oxide)‐based electrolytes are investigated. Interestingly, not all alloying interlayers enable a higher CE compared to neat Cu foil with 84%—specifically Ag@Cu with only 81 %, while the best performing one, Au@Cu, provides a substantially increased CE of 91%. While generally the formation of “dead lithium” is found to be the major source of CE, this appears to be less pronounced in the case of Au@Cu, indeed. Further improvement can be achieved by carefully adjusting the cell voltage to a region in which the continuous de‐/alloying is suppressed, yielding a further enhanced CE of 94%, thus highlighting the need for a comprehensive approach to design suitable electrode chemistries and designs beyond a “simple” material improvement.

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Publication Details

Journal
Small Structures
Published
2025-09-27
DOI
https://doi.org/10.1002/sstr.202500429
Citations
1
Primary Topic
Advanced Battery Materials and Technologies
Type
article
Field-Weighted Citation Impact
0.73

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article

Alloying Interlayers for Anode‐Less Lithium‐Metal Polymer Batteries

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Alloying Interlayers for Anode‐Less Lithium‐Metal Polymer Batteries

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article en
1 citations

Abstract

Anode‐less lithium‐metal batteries potentially offer further increased energy densities. However, the Coulombic efficiency (CE) of lithium plating and stripping, as a classical measure of Li inventory reversibility, is commonly still insufficient for achieving long‐lasting rechargeable batteries. Herein, the potential benefits of employing thin (20 nm) metal interlayers of Ag, Pt, and Au on Cu to alloy with Li in Cu||Li half‐cells and induce homogeneous Li plating with poly(ethylene oxide)‐based electrolytes are investigated. Interestingly, not all alloying interlayers enable a higher CE compared to neat Cu foil with 84%—specifically Ag@Cu with only 81 %, while the best performing one, Au@Cu, provides a substantially increased CE of 91%. While generally the formation of “dead lithium” is found to be the major source of CE, this appears to be less pronounced in the case of Au@Cu, indeed. Further improvement can be achieved by carefully adjusting the cell voltage to a region in which the continuous de‐/alloying is suppressed, yielding a further enhanced CE of 94%, thus highlighting the need for a comprehensive approach to design suitable electrode chemistries and designs beyond a “simple” material improvement.

Small StructuresVol. 6(12)
Karlsruhe Institute of Technology (DE), Argonne National Laboratory (US), Oak Ridge National Laboratory (US), Universität Ulm (DE), University of Münster (DE), Helmholtz-Institute Ulm (DE), Helmholtz-Institute Münster (DE), Technische Hochschule Ulm (DE)
U.S. Department of Energy, Bundesministerium für Bildung und Forschung, Office of Science, Office of Energy Efficiency and Renewable Energy, Division of Materials Research, Argonne National Laboratory, Oak Ridge National Laboratory
Openalex Percentile: Top 23%
Advanced Battery Materials and Technologies
0.73
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