Accurate prediction of ionic liquid density-of-states from low-cost calculations
Fogarty, R. M., Matthews, R. P., Hunt, P. A. and Lovelock, K. R. J.
It is advisable to refer to the publisher's version if you intend to cite from this work. See Guidance on citing. To link to this item DOI: 10.1039/D5CP00214A Abstract/SummaryThe electronic structure of ionic liquids (ILs) is a key factor in their chemical reactivity. Experimental techniques provide insight into IL electronic structure (e.g. X-ray photoelectron spectroscopy, XPS), but are impractical for screening large numbers of potential ILs. Computational screening offers an alternative approach, but current ab initio calculation methods (ion-pairs or large calculations with periodic boundaries) are not suitable for screening. We establish that a simple and computationally low-cost method, lone-ions evaluated at the B3LYP-D3(BJ)/6-311+G(d,p) level employing a generalised solvation model SMD (Solvation Model based on Density), captures IL liquid-phase density-of-states (DoS) with good accuracy by validating against XPS data for a wide range of ILs. The additivity of the results from individual lone-ion calculations provides a significant advantage, enabling predictions of the DoS for a large number of ILs and delivering a significant step towards the computational screening of ILs for many applications.
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