Modelling proton transfer in [HEIM][TFSI] ionic liquid

Protic ionic liquids, PILs, are promising materials for energy storage applications, in part due to their ability to decouple proton transport from ion diffusion. In this work, we model the proton transfer mechanism in 1-ethylimidazolium bis(trifluoromethanesulfonyl)imide ([HEIM][TFSI]) IL by means...

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Detalles Bibliográficos
Autores: Otero Lema, Martín, Goloviznina, Kateryna, Varela Cabo, Luis Miguel, Salanne, Mathieu, Montes-Campos, Hadrián, Serva, Alessandra
Tipo de recurso: artículo
Fecha de publicación:2025
País:España
Institución:Universidad de Santiago de Compostela (USC)
Repositorio:Minerva. Repositorio Institucional de la Universidad de Santiago de Compostela
Idioma:inglés
OAI Identifier:oai:minerva.usc.gal:10347/43334
Acceso en línea:https://hdl.handle.net/10347/43334
Access Level:acceso abierto
Palabra clave:Proton transfer
Protic ionic liquids
Molecular dynamics
Neural network force field
Polarizable force field
Descripción
Sumario:Protic ionic liquids, PILs, are promising materials for energy storage applications, in part due to their ability to decouple proton transport from ion diffusion. In this work, we model the proton transfer mechanism in 1-ethylimidazolium bis(trifluoromethanesulfonyl)imide ([HEIM][TFSI]) IL by means of Neural Network Force Field simulations. The latter are combined with classical polarizable molecular dynamics simulations to explore the structure and dynamics of the fully ionized system and Density Functional Theory calculations to estimate the energy barriers for the different proton transfer reactions. Our results show that proton transfer is indeed possible when doping the ionic liquid with an excess of deprotonated cations, but not with an excess of protonated anions. We highlight the importance of the formation of dimers between donor and acceptor species for the reaction to occur, and we identify the main driving factor for the reaction to be the energy cost for reaching a suitable coordination environment and form such dimers, which is higher than that for the transfer reaction.