Interfacial Structures in Ionic Liquid-Based Ternary Electrolytes for Lithium-Metal Batteries: A Molecular Dynamics Study

Author(s)

Lourenco, Tuanan C. ^[1] ; Ebadi, Mahsa ^[2] ; Brandell, Daniel ^[2] ; Da Silva, Juarez L. F. ^[1] ; Costa, Luciano T. ^[3]

Affiliation

^[1] Univ Sao Paulo, Sao Carlos Inst Chem, BR-13560970 Sao Carlos, SP - Brazil

^[2] Uppsala Univ, Dept Chem, Angstrom Lab, S-75121 Uppsala - Sweden

^[3] Fed Fluminense Univ, Inst Chem, Outeiro Sao Joao Batista, BR-24020141 Niteroi, RJ - Brazil

• Document type: Journal article
• Source: Journal of Physical Chemistry B; v. 124, n. 43, p. 9648-9657, OCT 29 2020.
• Web of Science Citations: 0

Abstract

Lithium-metal batteries are promising candidates to fulfill the future performance requirements for energy storage applications. However, the tendency to form metallic dendrites and the undesirable side reactions between the electrolyte and the Li electrode lead to poor performance and safety issues in these batteries. Therefore, understanding the interfacial properties and the Li-metal surface/electrolyte interactions is crucial to resolve the remaining obstacles and make these devices feasible. Here, we report a computational study on the interface effects in ternary polymer electrolytes composed by poly(ethylene oxide) (PEO), lithium salts, and different ionic liquids (ILs) confined between two Li-metal slabs. Atomistic simulations are used to characterize the local environment of the Li+ ions and the transport properties in the bulk and at the interface regions. Aggregation of ions at the metal surface is seen in all investigated systems; the structure and composition are directly correlated to the IL components. The strong interactions between the electrolyte species and the Li-metal atoms result in the structuring of the electrolyte at the interface region, in which comparatively small and flat ions result in a well-defined region with extensive Li+ populations and high self-diffusion coefficients. In contrast, large ions such as {[}P222mom](+) increase the PEO density in the bulk due to large steric effects at the interface. Therefore, the choice of specific ILs in ternary polymer electrolytes can tune the structure-dynamic properties at the Li-metal surface/electrolyte interface, controlling the SEI formation at the electrode surface, and thereby improve battery performance. (AU)

• FAPESP's process: 17/11631-2 - CINE: computational materials design based on atomistic simulations, meso-scale, multi-physics, and artificial intelligence for energy applications
• Grantee: Juarez Lopes Ferreira da Silva
• Support Opportunities: Research Grants - Research Centers in Engineering Program
• FAPESP's process: 18/21401-7 - Multi-User Equipment approved in grant 2017/11631-2: cluster computational de alto desempenho - ENIAC
• Grantee: Juarez Lopes Ferreira da Silva
• Support Opportunities: Multi-user Equipment Program