Advancing Computational Approaches for Study and Design in Catalysis

Abstract

Our group deals with the development of computational methods and their application to complex systems and processes. Emphasis is laid on accurate approaches derived from quantum mechanics, which we have used to investigate challenging questions in an interdisciplinary field encompassing chemistry, biology, physics, and materials science. In this review, we describe our recent activities for advancing computational approaches in catalysis. Moreover, our work for the study and design of catalysts for solar light-driven water splitting is summarized. The latter is a promising approach to face the world's increasing demand for sustainable energy storage and conversion. Emphasis is put on forefront methods for highly accurate electronic structure, sophisticated inclusion of environmental and dynamic effects and the derivation of structure-activity relationships for informed in silico design. This paves the way for the development of more efficient catalysts in close collaboration with experimental groups.

Recent progress in computational exploration and design of functional materials

“…Aside from that, the energetics of proton coupled electron transfer frequently occurring in water oxidation catalysis has been elucidated using a thermodynamic integration-based AIMD protocol [48], which can also be applied to prediction of properties such as redox potentials [49]. Since DFT has difficulties to describe the involved electronic structure of (strongly coupled) transition metals in an highly accurate way as required for, e.g., spin state energetics important for water oxidation catalysis, multiconfigurational wavefunction-based approaches have been explored for the description of WOCs as well [50]. Standard approaches such as complete active space self consistent field (CASSCF) methods are, however, limited to rather small systems.…”

Zooming in on the O–O Bond Formation—An Ab Initio Molecular Dynamics Study Applying Enhanced Sampling Techniques

“…2 For a general overview of computational studies focusing on the water oxidation mechanism we refer the interested reader to Refs. [7][8][9][10][11][12] In the previous study, catalytic intermediates as well as the corresponding transition states (TSs) were simulated by means of density functional theory (DFT) calculations, whereby the energetic contributions of the solute-solvent interaction were approximated by the conductor-like-screening-model (COSMO). 13,14 Within said method directed solutesolvent interactions such as hydrogen bonding are not explicitly accounted for.…”

“…The in-depth study of those catalysts allowed for the in silico design of novel WOCs by proposing modifications of the dangling base to lower the activation barrier of the WNA while keeping the overall thermodynamics about the same . For a general overview of computational studies focusing on the water oxidation mechanism, we refer the interested reader to refs. − …”