Electrochemical Windows of Room-Temperature Ionic Liquids from Molecular Dynamics and Density Functional Theory Calculations
By Shyue Ping Ong, O. Andreussi, Yabi Wu, Nicola Marzari, Gerbrand Ceder. 2011
370 citations recorded by the source corpus.
We investigated the cathodic and anodic limits of six room-temperature ionic liquids (ILs) formed from a combination of two common cations, 1-butyl-3-methylimidazolium (BMIM) and N,N-propylmethylpyrrolidinium (P13), and three common anions, PF6, BF4, and bis(trifluoromethylsulfonyl)imide (TFSI), using an approach that combines molecular dynamics (MD) simulations and density functional theory (DFT) calculations. All interion interactions were taken into account by explicitly modeling the entire liquid structure using classical MD, followed by DFT computations of the highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) energies. The relative cathodic and anodic limits of BMIM PF6, BMIM BF4, BMIM TFSI, and P13 TFSI obtained from our approach are in fairly good agreement with existing experimental data. From our DFT calculations, we also obtained the cation- and anion-projected density of states (DOS), which provide information on the likely species contributing to reductiv...
Subfields: Catalysis, Electrochemistry, Renewable Energy, Sustainability and the Environment
View Paper: https://www.semanticscholar.org/paper/fb81b461663a1f561456477b8d81423844b8a44f
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Citations in the corpus
- First Principles Study of the Li10GeP2S12 Lithium Super Ionic Conductor Material (2012, methodology): “Using the methodology outlined in Ong et al.,11 we plotted the lithium grand potential phase diagrams of the Li-Ge-P-S system at various lithium chemical potentials (µLi) of interest in Figure 1.”
- Computation-Accelerated Design of Materials and Interfaces for All-Solid-State Lithium-Ion Batteries (2018, background): “Computational studies have shown that that the gap between HOMO and LUMO is an upper bound of the electrochemical window.(66,67) The GPPD approach is also applied to study the thermal stability of electrode materials, such as oxygen evolution at high temperatures.”
- Computational understanding of Li-ion batteries (2016, methodology): “The most accurate electronic structure method for the prediction of the electrolyte potentials was found to be Møller–Plesset perturbation theory (MP2) with errors in the range of 0.1–0.5 V, whereas DFT (GGA and hybrid functionals) resulted in errors of up to 1.5 V.123 The validity of approximating ”