TYC Symposium: Georg Kresse – Vienna, Volker Blum – Duke & Chris Skylaris – Soton

XLG1 LT, Christopher Ingold Building, followed by a drinks reception in the Nyholm Room

TYC Symposium: Georg Kresse – Vienna, Volker Blum – Duke & Chris Skylaris – Soton Click To Tweet

Large-scale quantum atomistic and multiscale simulations of batteries – Chris-Kriton Skylaris, University of Southampton
We are developing new software tools with unique capabilities for large-scale atomistic electrochemical simulations under operational conditions. The aim is to not only capture all the essential chemistry and physics of devices such as batteries, but also to provide 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 several orders of magnitude more atoms than conventional DFT approaches, so that we can study more complex 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]. Also, I will describe our ongoing development of new DFTB approaches within the linear-scaling framework of ONETEP which will enable simulations at longer timescales to allow study of problems such as the chemistry taking place during SEI formation. Finally, I will summarise recent applications of these tools to the process of lithium metal deposition on anodes and its competition with Li dendrite formation [5], one of the major mechanisms of battery degradation.

References

[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. Escartín, A. Greco, Q. Hill, L. P. Lee, E. Linscott, D. D. O’Regan, M. J. S. Phipps, L. E. Ratcliff, Á. 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.

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