CBET-EPSRC: Bespoke Porous Catalyst Design via Integrated Stochastic Modelling of Reaction and Transport in Synergy with Experiments

Heterogeneous catalysts encompass porous solid materials that accelerate chemical reactions and are employed in more than 70% of all chemical manufacturing processes. In these materials, the active sites (single atoms or nanoparticles) lie within the porous network of a support, which may be crystalline, e.g. a zeolite, or amorphous, e.g. an activated carbon. Thus, engagement with the catalytic functionality of such porous catalysts involves the transport of gas/liquid reactants around solid pellets (global transfer), transfer through the pore openings and diffusion along the porous networks (local transfer), adsorption and catalytic conversion on active sites, and finally desorption and transport back to the bulk.

Due to the multiscale nature and the complex interplay of these phenomena, a fundamental understanding of structure-performance relationships remains elusive. From an industrial context, what is lacking but essential is an accurate and fully integrated-multiscale kinetic modelling framework that would account for the relevant reactive and transport phenomena within the spatial resolution of the catalyst's porous network structure. Such a framework will guide the development of superior porous catalysts for given applications, and the identification of optimal conditions for reducing the environmental impact of industrial operations.

The proposed international collaborative project will address this challenge, underpinned by experimental investigation and close collaboration with industry (Johnson Matthey). The pertinent aims, methods and outcomes are:

1) To bridge the gap between local pore-scale phenomena (electronic/molecular) and global/bulk phenomena (performance) in porous catalysts. The kinetic Monte Carlo (kMC) method will be the backbone of the envisioned integrated framework, which will link reactive kMC [MS and co-workers, Zacros graph-theoretical kMC framework; J. Chem. Phys., 139: 224706 (2013); Comp. Phys. Comm., 270: 108148 (2022)] and...