Autonomous Workflows for an Accelerated Design of Battery Electrodes and Interfaces

The development of automated computational tools is required to accelerate the discovery of new functional materials, to speed up the transition to a sustainable future. Here, I address this topic by designing new battery electrodes for different intercalation battery chemistries. These workflows are implemented in the framework of Density Functional Theory, using MyQueue and the Atomistic Simulation Environment (ASE). In the first part, I describe a fully autonomous workflow, which identifies materials to be used as intercalation electrodes in batteries, based on thermodynamic and kinetic descriptors like adsorption energies and diffusion barriers [1]. A substantial acceleration for the calculations of the kinetic properties has been obtained due to a recent implementation of the Nudged Elastic Bands (NEB) method, which takes into consideration the symmetries of the system to reduce the number of images to calculate. Moreover, we have established a surrogate model to identify the transition states, which can further reduce the computational cost to at least one order of magnitude [2, 3]. We have applied this workflow to discover new cathode materials for Mg batteries as well as solid state electrolytes for Li, Na, and Mg all-solid-state batteries [1, 3]. In the second part of my talk, I discuss how nanostructured materials can positively impact the Li-ion battery solid/electrolyte interface towards a controlled formation of the Solid Electrolyte Interface (SEI) [4, 5] and to adjust the volume expansion in Si-anodes during battery cycling [6].<br/><br/>References<br/>[1] F. T. Bölle, N. R. Mathiesen, A. J. Nielsen, T. Vegge, J. M. García-Lastra, and I. E. Castelli, Batteries & Supercaps 3, 488 (2020).<br/>[2] F. T. Bölle, A. Bhowmik, T. Vegge, J. M. García-Lastra, and I. E. Castelli, Batteries & Supercaps 4, 1516 (2021).<br/>[3] B. H. Sjølin, P. B. Jørgensen, A. Fedrigucci, T. Vegge, A. Bhowmik, and I. E. Castelli, under review, DOI: 10.21203/rs.3.rs-1780345/v1 (2022).<br/>[4] I. E. Castelli, M. Zorko, T. M. Østergaard, P. F. B. D. Martins, P. P. Lopes, B. K. Antonopoulos, F. Maglia, N. M. Markovic, D. Strmcnik, and J. Rossmeisl, Chem. Sci. 11, 3914 (2020).<br/>[5] K. L. Svane, S. Z. Lefmann, M. S. Vilmann, J. Rossmeisl, and I. E. Castelli, ACS Appl. Energy Mater. 4, 35 (2021).<br/>[6] S. B. Oliva, F. T. Bölle, A. T. Las, X. Xia, and Castelli, in preparation (2022).