Achievements and Expectations in the Field of Computational Heterogeneous Catalysis in an Innovation Context

Abstract

Heterogeneous catalysis is linked to industrial considerations from its origins, so is computational heterogeneous catalysis. The impact of first principles calculations on discoveries made for industrially relevant systems is growing year after year. In an innovation context, key questions are related to active site structure understanding, chemical reactivity investigations, multi-scale modeling, and prediction of new active phases with optimal catalytic performance. The present short review discusses and illustrates these various stages of the catalyst understanding and performance prediction where computational catalysis has a crucial role to play. Selected achievements in the field are reviewed, with a focus on the simulation of complex metallic and zeolite catalysts of industrial relevance. Future directions are suggested, on the basis of the need for ever more exhaustive and accurate models of catalytic sites and catalytic reactions representative of industrial systems, and for speed up in catalyst understanding and discovery.

Kinetic Monte Carlo simulations for heterogeneous catalysis: Fundamentals, current status, and challenges

“…The accurate computational modeling of heterogeneous catalysis is certainly a challenging and vital endeavor. 4,6,8,10,[35][36][37][38][39][40][41][42] The acceleration of chemical reactions by the catalyst and its ability to direct the paths to yield particular products arise as a consequence of a highly complex interplay between a large number of elementary events (i.e., adsorption, desorption, diffusion, and reaction events) occurring at the active sites of the catalytic surface. A significant challenge in modelling such events is to find efficient ways to treat the time-scale disparity arising from the fact that such elementary events are commonly thermally activated and are thus rare on the typical femtosecond scale of smallest atomistic vibrations.…”

Prospects and challenges for autonomous catalyst discovery viewed from an experimental perspective

“…63 Computational chemistry is mainly employed to support these assumptions energetically. 64,65 This strategy is in conflict with catalyst dynamics and the metastable nature of active sites. Although it is generally accepted that the product of catalyst synthesis is a catalyst precursor and that the generally unknown structure of the active phase is only formed in contact with the reacting molecules under working conditions, this insight is nevertheless hardly taken into account in the paradigm of current catalysis research.…”

Gas Adsorption in Zeolite and Thin Zeolite Layers: Molecular Simulation, Experiment, and Adsorption Potential Theory

“…The impact of this external surface is already documented with striking examples in adsorption uptakes measurements , as well as in separation/chromatography, where it plays a key role in the balance between intraparticle diffusion and hydraulic transport , (see also ref for a discussion on the adsorption of xylene isomers at the external surface of zeolites). In catalysis, the effect of the external surface remains to be fully established, but many papers report pore mouth catalysis mechanisms. , In this context, the geometry and defects at the external surface were shown to affect both the catalysis of reacting molecules (e.g., refs and ) and the adsorption/dynamics of fluids (e.g., refs and ) in nanoporous solids.…”