Development of coarse-grained force field to investigate sodium-ion transport mechanisms in cyanoborate-based ionic liquid

Author(s)

de Souza, Rafael Maglia ^[1] ; Lourenco, Tuanan C. ^[2] ; Amaral de Siqueira, Leonardo Jose ^[3] ; Karttunen, Mikko ^{[4, 5, 6]} ; Da Silva, Juarez L. F. ^[2] ; Dias, Luis Gustavo ^[1]

Affiliation

^[1] Univ Sao Paulo, Dept Quim, FFCLRP, Ave Bandeirantes 3900, BR-14040901 Ribeirao Preto, SP - Brazil

^[2] Univ Sao Paulo, Sao Carlos Inst Chem, POB 780, BR-13560970 Sao Carlos, SP - Brazil

^[3] Univ Fed Sao Paulo, Inst Ciencias Ambientais Quim & Farmaceut, Dept Quim, Rua Sao Nicolau 210, BR-09913030 Diadema, SP - Brazil

^[4] Univ Western Ontario, Dept Chem, London, ON N6A 3K7 - Canada

^[5] Univ Western Ontario, Dept Appl Math, London, ON N6A 3K7 - Canada

^[6] Univ Western Ontario, Ctr Adv Mat & Biomat Res, 1151 Richmond St, Richmond, ON N6A 5B7 - Canada

• Document type: Journal article
• Source: JOURNAL OF MOLECULAR LIQUIDS; v. 338, SEP 15 2021.
• Web of Science Citations: 0

Abstract

Sodium-ion batteries have a great potential for energy storage applications, however, its realization depends strongly on a deep atomistic understanding of the sodium-ion transport mechanisms, which is a key step to optimize its performance. A complete characterization of sodium-ion transport mechanism requires large time-scale calculations, which is a challenge even for classical atomistic force-field molecular dynamics simulations. Thus, in this work, we performed a calibration of a coarse-grained force-field to describe the thermodynamic and transport properties of sodium-ion for the particular case of cyanoborate-based ionic liquid using different molar fractions of sodium tetracyanoborate salt dissolved in 1-ethyl-3-methyl-imidazolium tetracyanoborate. The results from coarse-grained modeling were found to be in fair agreement with atomistic simulations and experimental data, and they captured concentration dependence of {[}Na-x{[}Anion](y)](x-y) aggregate sizes. In particular, two distinct populations of sodium-ions were identified inside the {[}Na-x{[}Anion](y)](x-y) aggregates: 1) a slow one in vehicular diffusion and 2) a fast one in hoping diffusion. Both of them contribute to sodium ion transport and occur preferentially at different sodium-ion concentrations. The present findings were obtained for a cyanoborate-based ionic liquid, however, we expect that our insights can be used to understand similar ionic liquids. (C) 2021 Elsevier B.V. All rights reserved. (AU)

• 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
• FAPESP's process: 17/26102-5 - Computational simulation of the electrolytic medium of secondary alkali and/or alkaline earth metal ion batteries
• Grantee: Rafael Maglia de Souza
• Support Opportunities: Scholarships in Brazil - Doctorate
• 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: 19/23681-0 - From ab initio to continuum methods to the screening of sodium-ion battery materials
• Grantee: Tuanan da Costa Lourenço
• Support Opportunities: Scholarships in Brazil - Post-Doctoral
• FAPESP's process: 18/13867-6 - Computational simulation of the electrolytic medium of secondary alkaline and/or alkaline earth metal ion batteries
• Grantee: Rafael Maglia de Souza
• Support Opportunities: Scholarships abroad - Research Internship - Doctorate
• FAPESP's process: 19/18125-0 - Computational study of materials with application in energy storage
• Grantee: Leonardo José Amaral de Siqueira
• Support Opportunities: Regular Research Grants