Abstract
Thin intermetallic Li2Te–LiTe3 bilayer (0.75 µm) derived from 2D tellurene stabilizes the solid electrolyte interphase (SEI) of lithium metal and argyrodite (LPSCl, Li6PS5Cl) solid-state electrolyte (SSE). Tellurene is loaded onto a standard battery separator and reacted with lithium through single-pass mechanical rolling, or transferred directly to SSE surface by pressing. State-of-the-art electrochemical performance is achieved, e.g., symmetric cell stable for 300 cycles (1800 h) at 1 mA cm−2 and 3 mAh cm−2 (25% DOD, 60 µm foil). Cryo-stage focused ion beam (Cryo-FIB) sectioning and Raman mapping demonstrate that the Li2Te–LiTe3 bilayer impedes SSE decomposition. The unmodified Li–LPSCl interphase is electrochemically unstable with a geometrically heterogeneous reduction decomposition reaction front that extends deep into the SSE. Decomposition drives voiding in Li metal due to its high flux to the reaction front, as well as voiding in the SSE due to the associated volume changes. Analysis of cycled SSE found no evidence for pristine (unreacted) lithium metal filaments/dendrites, implying failure driven by decomposition phases with sufficient electrical conductivity that span electrolyte thickness. DFT calculations clarify thermodynamic stability, interfacial adhesion, and electronic transport properties of interphases, while mesoscale modeling examines interrelations between reaction front heterogeneity (SEI heterogeneity), current distribution, and localized chemo-mechanical stresses.
| Original language | English |
|---|---|
| Article number | 2301338 |
| Journal | Advanced Energy Materials |
| Volume | 13 |
| Issue number | 46 |
| DOIs | |
| State | Published - Dec 8 2023 |
Funding
This work was supported by the Mechano‐Chemical Understanding of Solid Ion Conductors, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Science, contract DE‐SC0023438. This work was performed, in part, at the Center for Integrated Nanotechnologies, an Office of Science User Facility operated by the U.S. Department of Energy (DOE) Office of Science. Los Alamos National Laboratory, an affirmative action‐equal opportunity employer, is managed by Triad National Security, LLC for the U.S. Department of Energy's NNSA, under contract 89233218CNA000001. G. Y. would like to acknowledge the sponsorship by the Office of Energy Efficiency and Renewable Energy (EERE), specifically the Vehicle Technologies Office (VTO), through the Advanced Battery Materials Research (BMR) Program. The authors are grateful to Prof. Yue Qi for numerous highly insightful discussions. This work was supported by the Mechano-Chemical Understanding of Solid Ion Conductors, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Science, contract DE-SC0023438. This work was performed, in part, at the Center for Integrated Nanotechnologies, an Office of Science User Facility operated by the U.S. Department of Energy (DOE) Office of Science. Los Alamos National Laboratory, an affirmative action-equal opportunity employer, is managed by Triad National Security, LLC for the U.S. Department of Energy's NNSA, under contract 89233218CNA000001. G. Y. would like to acknowledge the sponsorship by the Office of Energy Efficiency and Renewable Energy (EERE), specifically the Vehicle Technologies Office (VTO), through the Advanced Battery Materials Research (BMR) Program. The authors are grateful to Prof. Yue Qi for numerous highly insightful discussions.
Keywords
- Li metal
- argyrodite
- solid electrolyte interphase
- solid–state batteries
- tellurene
