Theoretical Investigation of the Na+ Transport Mechanism and the Performance of Ionic Liquid-Based Electrolytes in Sodium-Ion Batteries

Autor(es)

Lourenco, Tuanan C. ^[1] ; Dias, Luis Gustavo ^[2] ; Da Silva, Juarez L. F. ^[1]

Afiliação do(s) autor(es)

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

^[2] Univ Sao Paulo, Chem Dept, FFCLRP, BR-14040901 Ribeirao Preto, SP - Brazil

• Tipo de documento: Artigo Científico
• Fonte: ACS APPLIED ENERGY MATERIALS; v. 4, n. 5, p. 4444-4458, MAY 24 2021.
• Citações Web of Science: 0

Resumo

Ionic liquids are a promising alternative to common organic electrolytes in sodium-ion batteries that offer a unique combination of physical and chemical properties, leading to the development of high-performance batteries. To improve our atomistic understanding of the Na+ transport mechanism, aggregation effects, and electrolyte performance, we report a theoretical investigation based on the combination of classical molecular dynamics simulations based on the CL\&P force field and density functional theory calculations for 25 different ionic liquids (ILs), which includes anions based or related to the {[}Tf2N](-) anion, while the cations are based on the imidazolium and ammonium-based ones. From our molecular dynamics (MD) simulations and analyses, we found that the Na+ aggregation is a result of multiple Na+-anion interactions in the systems and the consequent improvement of the Na+ transport number due to the hopping diffusion mechanism. Although all studied systems have shown X{[}anion](x)(-y) aggregates, there is a direct correlation between the anion structure and the size of the aggregates, in which flexible anions with a large degree of charge delocalization yield larger aggregates. The electrochemical windows estimated from first-principles calculations exceed 4.0 eV, which indicates the good performance of the systems for electrolyte applications. (AU)

• Processo FAPESP: 18/21401-7 - EMU concedido no processo 2017/11631-2: cluster computacional de alto desempenho - ENIAC
• Beneficiário: Juarez Lopes Ferreira da Silva
• Modalidade de apoio: Auxílio à Pesquisa - Programa Equipamentos Multiusuários
• Processo FAPESP: 17/11631-2 - CINE: desenvolvimento computacional de materiais utilizando simulações atomísticas, meso-escala, multi-física e inteligência artificial para aplicações energéticas
• Beneficiário: Juarez Lopes Ferreira da Silva
• Modalidade de apoio: Auxílio à Pesquisa - Programa Centros de Pesquisa em Engenharia
• Processo FAPESP: 19/23681-0 - De métodos ab initio até o contínuo para a busca de materiais para baterias de sódio-íon
• Beneficiário: Tuanan da Costa Lourenço
• Modalidade de apoio: Bolsas no Brasil - Pós-Doutorado