Screening of the Role of the Chemical Structure in the Electrochemical Stability Window of Ionic Liquids: DFT Calculations Combined with Data Mining.
J Chem Inf Model
; 62(19): 4702-4712, 2022 Oct 10.
Article
em En
| MEDLINE
| ID: mdl-36122418
Ionic liquids have attracted the attention of researchers as possible electrolytes for electrochemical energy storage devices. However, their properties, such as the electrochemical stability window (ESW), ionic conductivity, and diffusivity, are influenced both by the chemical structures of cations and anions and by their combinations. Most studies in the literature focus on the understanding of common ionic liquids, and little effort has been made to find ways to improve our atomistic understanding of those systems. The goal of this paper is to explore the structural characteristics of cations and anions that form ionic liquids that can expand the HOMO/LUMO gap, a property directly linked to the ESW of the electrolyte. For that, we design a framework for randomly generating new ions by combining their fragments. Within this framework, we generate about 104 cations and 104 anions and fully optimize their structures using density functional theory. Our calculations show that aromatic cations are less stable ionic liquids than aliphatic ones, an expected result if chemical rationale is used. More importantly, we can improve the gap by adding electron-donating and electron-withdrawing functional groups to the cations and anions, respectively. The increase can be about 2 V, depending on the case. This improvement is reflected in a wider ESW.
Texto completo:
1
Coleções:
01-internacional
Base de dados:
MEDLINE
Tipo de estudo:
Diagnostic_studies
/
Screening_studies
Idioma:
En
Revista:
J Chem Inf Model
Assunto da revista:
INFORMATICA MEDICA
/
QUIMICA
Ano de publicação:
2022
Tipo de documento:
Article
País de afiliação:
Brasil