DOE OSTI · 2497380
Control of Two Solid Electrolyte Interphases at the Negative Electrode of an Anode‐Free All Solid‐State Battery based on Argyrodite Electrolyte
Abstract
Abstract Anode‐free all solid‐state batteries (AF‐ASSBs) employ “empty” current collector with three active interfaces that determine electrochemical stability; lithium metal – Solid electrolyte (SE) interphase (SEI‐1), lithium – current collector interface, and collector – SE interphase (SEI‐2). Argyrodite Li 6 PS 5 Cl (LPSCl) solid electrolyte (SE) displays SEI‐2 containing copper sulfides, formed even at open circuit. Bilayer of 140 nm magnesium/30 nm tungsten (Mg/W‐Cu) controls the three interfaces and allows for state‐of‐the‐art electrochemical performance in half‐cells and fullcells. AF‐ASSB with NMC811 cathode achieves 150 cycles with Coulombic efficiency (CE) above 99.8%. With high mass‐loading cathode (8.6 mAh cm −2 ), AF‐ASSB retains 86.5% capacity after 45 cycles at 0.2C. During electrodeposition of Li, gradient Li‐Mg solid solution is formed, which reverses upon electrodissolution. This promotes conformal wetting/dewetting by Li and stabilizes SEI‐1 by lowering thermodynamic driving force for SE reduction. Inert refractory W underlayer is required to prevent ongoing formation of SEI‐2 that also drives electrochemical degradation. Inert Mo and Nb layers likewise protect Cu from corroding, while Li‐alloying layers (Mg, Sn) are less effective due to ongoing volume changes and associated pulverization. Mechanistic explanation for observed Li segregation within alloying Li x Mg layer is provided through mesoscale modelling, considering opposing roles of diffusivity differences and interfacial stresses.
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Wang, Yixian [Materials Science and Engineering Program Walker Department of Mechanical Engineering and Texas Materials Institute The University of Texas at Austin Austin TX 78712 USA] (ORCID:0000000161078352), Raj, Vikalp [Materials Science and Engineering Program Walker Department of Mechanical Engineering and Texas Materials Institute The University of Texas at Austin Austin TX 78712 USA], Naik, Kaustubh G. [School of Mechanical Engineering Purdue University West Lafayette IN 47907 USA], Vishnugopi, Bairav S. [School of Mechanical Engineering Purdue University West Lafayette IN 47907 USA], Cho, Jaeyoung [Department of Chemistry The University of Texas at Austin Austin TX 78712 USA], Nguyen, Mai [Department of Chemistry The University of Texas at Austin Austin TX 78712 USA], Recker, Elizabeth A. [Department of Chemistry The University of Texas at Austin Austin TX 78712 USA, McKetta Department of Chemical Engineering The University of Texas at Austin Austin TX 78712 USA], Su, Yufeng [Materials Science and Engineering Program Walker Department of Mechanical Engineering and Texas Materials Institute The University of Texas at Austin Austin TX 78712 USA], Celio, Hugo [Materials Science and Engineering Program Walker Department of Mechanical Engineering and Texas Materials Institute The University of Texas at Austin Austin TX 78712 USA], Dolocan, Andrei [Materials Science and Engineering Program Walker Department of Mechanical Engineering and Texas Materials Institute The University of Texas at Austin Austin TX 78712 USA], Page, Zachariah A. [Department of Chemistry The University of Texas at Austin Austin TX 78712 USA] (ORCID:0000000210135422), Watt, John [Center for Integrated Nanotechnologies Los Alamos National Laboratory Los Alamos NM 87545 USA], Henkelman, Graeme [Department of Chemistry The University of Texas at Austin Austin TX 78712 USA], Tu, Qingsong Howard [Department of Mechanical Engineering Rochester Institute of Technology Rochester NY 14623 USA], Mukherjee, Partha P. [School of Mechanical Engineering Purdue University West Lafayette IN 47907 USA], Mitlin, David [Materials Science and Engineering Program Walker Department of Mechanical Engineering and Texas Materials Institute The University of Texas at Austin Austin TX 78712 USA] (ORCID:0000000275563575). 2025-01-06. Control of Two Solid Electrolyte Interphases at the Negative Electrode of an Anode‐Free All Solid‐State Battery based on Argyrodite Electrolyte. https://doi.org/10.1002/adma.202410948
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