Large-scale quantum atomistic electrochemistry simulations

ORAL  · Invited

Abstract

We are developing software tools for atomistic electrochemical simulations under operational conditions. These new computational tools are not only capturing the essential chemistry and physics of devices such as batteries but can also give us the parameters needed for bridging atomistic with larger scale simulations. Our developments are within the ONETEP program [1] which is based on a linear-scaling reformulation of density functional theory (DFT) that allows atomistic simulations of orders of magnitude more atoms than conventional approaches, so that we can construct more realistic models. In this talk I will outline our developments so far which include methods for metallic systems, solvent and electrolyte models [2], and a grand-canonical approach which allows simulations at fixed voltage with respect to a computational reference electrode [3-4]. Finally I will present an application of these methods in recent simulations of the process of lithium metal deposition on anodes, which is a common mechanism for battery degradation [5].

*This work was carried out with the funding from the Faraday Institution (https://www.Faraday.ac.uk; EP/S003053/1), grant numbers FIRG003 and FIRG025. The calculations presented in this work were performed on the Iridis5 supercomputer of the University of Southampton, the Michael supercomputer of the Faraday Institution, the Young supercomputer at the UCL and the ARCHER2 UK National Supercomputing Service (https://www.archer2.ac.uk; via EPSRC grant: EP/P022030/1). We acknowledge the United Kingdom Materials and Molecular Modelling Hub for computational resources, partially funded by EPSRC (EP/P020194/1).

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Publication: [1] The ONETEP linear-scaling density functional theory program. J. C. A. Prentice, J. Aarons, J. C. Womack, A. E. A. Allen, L. Andrinopoulos, L. Anton, R. A. Bell, A. Bhandari, G. A. Bramley, R. J. Charlton, R. J. Clements, D. J. Cole, G. Constantinescu, F. Corsetti, S. M.-M. Dubois, K. K. B. Duff, J. M. Escarti´n, A. Greco, Q. Hill, L. P. Lee, E. Linscott, D. D. O'Regan, M. J. S. Phipps, L. E. Ratcliff, A´. R. Serrano, E. W. Tait, G. Teobaldi, V. Vitale, N. Yeung, T. J. Zuehlsdorff, J. Dziedzic, P. D. Haynes, N. D. M. Hine, A. A. Mostofi, M. C. Payne, and C.-K. Skylaris. J. Chem. Phys. 152 (2020) 174111.
[2] Practical Approach to Large-Scale Electronic Structure Calculations in Electrolyte Solutions via Continuum-Embedded Linear-Scaling Density Functional Theory. J. Dziedzic, A. Bhandari, L. Anton, C. Peng, J. C. Womack, M. Famili, D. Kramer, and C.-K. Skylaris. J. Phys. Chem. C. 124 (2020) 7860-7872.
[3] Electronic structure calculations in electrolyte solutions: Methods for neutralization of extended charged interfaces. A. Bhandari, L. Anton, J. Dziedzic, C. Peng, D. Kramer, and C.-K. Skylaris. J. Chem. Phys. 153 (2020) 124101.
[4] Electrochemistry from first-principles in the grand canonical ensemble. A. Bhandari, C. Peng, J. Dziedzic, L. Anton, J. R. Owen, D. Kramer, and C.-K. Skylaris. J. Chem. Phys 155 (2021) 024114.
[5] Mechanism of Li nucleation at graphite anodes and mitigation strategies. C. Peng, A. Bhandari, J. Dziedzic, J. R. Owen, C.-K. Skylaris, and D. Kramer. J. Mater. Chem. A, 2021,9, 16798; Li nucleation on the graphite anode under potential control in Li-ion batteries. A. Bhandari, C. Peng, J. Dziedzic, J.R. Owen, D. Kramer, C.-K. Skylaris, J. Mater. Chem. A, 2022,10, 11426.

Presenters

  • Chris-Kriton Skylaris

    • University of Southampton (UK), The Faraday Institution (UK)
    • University of Southampton

Authors

  • Chris-Kriton Skylaris

    • University of Southampton (UK), The Faraday Institution (UK)
    • University of Southampton