Autonomous In-Silico Accelerated Design of Novel Energy Materials

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 electrodes with controlled interfaces for different applications which accelerate the transition to a sustainable future. 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 considers the system's symmetries 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 engineering the interface can positively impact surface properties. I show this concept using two examples. In the first one, I nanostructure materials to increase the Li-storage capacity in C-anodes or to adjust the change in volume during charge/discharge in Si-anodes for Li-ion batteries [4]. In the second example, I apply strain engineering and external stimuli to switch the material’s polarization to decrease the reaction overpotential in oxynitride materials for the oxygen evolution reaction [5, 6].<br/><br/><b>References</b><br/>[1] F. T. Bölle, N. R. Mathiesen, A. J. Nielsen, T. Vegge, J. M. García-Lastra, and I. E. Castelli, <i>Batteries & Supercaps</i> <b>3</b>, 488 (2020).<br/>[2] F. T. Bölle, A. Bhowmik, T. Vegge, J. M. García-Lastra, and I. E. Castelli, <i>Batteries & Supercaps</i> <b>4</b>, 1516 (2021).<br/>[3] B. H. Sjølin, P. B. Jørgensen, A. Fedrigucci, T. Vegge, A. Bhowmik, and I. E. Castelli, <i>Batteries & Supercaps</i> <b>2023</b>, e202300041 (2023).<br/>[4] S. B. Oliva, F. T. Bölle, A. T. Las, X. Xia, and I. E. Castelli, <i>under review</i> (2022).<br/>[5] Z. Lan, D. R. Småbråten, C. Xiao, T. Vegge, U. Aschauer, and I. E. Castelli, <i>ACS Catal</i> <b>11</b>, 12692 (2021).<br/>[6] C. Spezzati, Z. Lan, and I. E. Castelli, <i>Journal of Catalysis </i><b>413</b>, 720 (2022).