DOE OSTI · 3002406
Alloying Interlayers for Anode‐Less Lithium‐Metal Polymer Batteries
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.
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Counihan, Michael J. [Argonne National Laboratory (ANL), Argonne, IL (United States)], Steinle, Dominik [Helmholtz Institute Ulm (HIU) (Germany); Karlsruhe Inst. of Technology (KIT) (Germany)], Sahore, Ritu [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)] (ORCID:0000000223909570), Browning, Katie [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)], Meyer III, Harry M. [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)] (ORCID:0000000349941664), Krude, Annalena [Forschungszentrum Juelich, Münster (Germany)] (ORCID:0009000974944630), Wichmann, Lennart [Forschungszentrum Juelich, Münster (Germany)], Brunklaus, Gunther [Forschungszentrum Juelich, Münster (Germany)], Winter, Martin [Forschungszentrum Juelich, Münster (Germany); Univ. of Münster (Germany)], Westover, Andrew [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)], Bresser, Dominic [Helmholtz Institute Ulm (HIU) (Germany); Karlsruhe Inst. of Technology (KIT) (Germany); Ulm Univ. (UUlm) (Germany)] (ORCID:0000000257381233), Tepavcevic, Sanja [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000301518832). 2025-09-27. Alloying Interlayers for Anode‐Less Lithium‐Metal Polymer Batteries. https://doi.org/10.1002/sstr.202500429
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