Fundamentals of energy storage from first principles simulations: Challenges and opportunities

Abstract

Efficient electrochemical energy storage and conversion require high performance electrodes, electrolyte or catalyst materials. In this contribution we discuss the simulation-based effort made by Institute of Energy and Climate Research at Forschungszentrum Jülich (IEK-13) and partner institutions aimed at improvement of computational methodologies and providing molecular level understanding of energy materials. We focus on discussing correct computation of electronic structure, oxidation states and related redox reactions, phase transformation in doped oxides and challenges in computation of surface chemical reactions on oxides and metal surfaces in presence of electrolyte. Particularly, in the scope of this contribution we present new simulated data on Ni/Co and Am/U-bearing oxides, and Pb, Au and Ag metal surface materials. The computed results are combined with the available experimental data for thoughtful analysis of the computational methods performance.

Stay Hydrated! Impact of Solvation Phenomena on the CO2 Reduction Reaction at Pb(100) and Ag(100) surfaces

“…HCOO* is stabilized by 0.74 eV, whereas COOH* is stabilized by only 0.22 eV in the explicit solvation environment. Overall, these results agree with our previous findings [44] . In addition to these findings, we explain the greater stabilization of HCOO* compared to COOH* with the fact that explicit water molecules have a significant impact on the orientation of HCOO* relative to the surface, as illustrated in Figure 1.…”

“…Overall, these results agree with our previous findings. [44] In addition to these findings, we explain the greater stabilization of HCOO* compared to COOH* with the fact that explicit water molecules have a significant impact on the orientation of HCOO* relative to the surface, as illustrated in Figure 1. HCOO* changes from perpendicular orientation towards the surface for vacuum and implicit solvation cases to parallel orientation for the explicit solvation case.…”

“…Similar calculations were performed in our previous study, [44] where VASP [45–47] and VASPsol [48,49] software packages were used to perform DFT calculations in vacuum and in solvation. As observed in the previous study, [44] applying implicit solvation stabilizes reaction energies of HCOO* and COOH* by around 0.2 eV relative to the vacuum case. The difference between these reaction energies remains the same as in the vacuum case.…”

“…In the Theoretical Section a more detailed explanation of the initial configuration of water molecules considered in the explicit solvation case is provided. Similar calculations were performed in our previous study, [44] where VASP [45][46][47] and VASPsol [48,49] software packages were used to perform DFT calculations in vacuum and in solvation. As observed in the previous study, [44] applying implicit solvation stabilizes reaction energies of HCOO* and COOH* by around 0.2 eV relative to the vacuum case.…”

Basic guidelines of first-principles calculations for suitable selection of electrochemical Li storage materials: a review

“…19 Kowalski et al discussed correct computation of electronic structures, oxidation states and related redox reactions, phase transformation in doped oxides and challenges in the computation of surface chemical reactions on oxides and metal surfaces in the presence of electrolyte. 21 DFT has significant potential to aid understanding of advanced LIB technology by enabling material discovery, understanding electrochemical reactions, optimizing electrolytes, studying interfaces, analyzing stress and strain, exploring new materials, elucidating energy storage mechanisms, reducing costs, and accelerating research and development.…”