Multiscale modelling of CO2 reduction to methanol over industrial Cu/ZnO/Al2O3 heterogeneous catalyst: Linking ab initio surface reaction kinetics with reactor fluid dynamics

Abstract

There has been a growing trend to couple different levels of modelling, such as going from first-principle calculations to the meso (e.g. kinetic Monte Carlo-KMC) and macro scale (e.g. computational fluid dynamics-CFD). In the current investigation, we put forward a CFD study of CO 2 hydrogenation to methanol for heterogeneous reacting flows in reactors with complex shape geometries, coupled with first-principle calculations (density functional theory (DFT)). KMC operation simulations were also performed to obtain insight into the uppermost layer conditions during the reaction. With computational fluid dynamics, the focus was placed on the non-uniform catalytic reduction of carbon dioxide to formate, which we treated with a detailed mean-field first-principle microkinetic model, analysed, and corroborated with experiments. The results showed a good consistent agreement with experimental data. The formulated methodological approach paves the way towards full virtual multiscale system descriptions of industrial processing units, encompassing all conventional stages, from catalyst design to the optimisation of mass transfer parameters. Such a bridging is outlined for carbon capture and utilisation.

Improving the Cu/ZnO-Based Catalysts for Carbon Dioxide Hydrogenation to Methanol, and the Use of Methanol As a Renewable Energy Storage Media

“…The atomic configurations, transition states, energetics, energy barriers, and reaction mechanisms derived from first-principles calculations can be used to predict the catalytic activities at an atomic level. The kMC showed how the catalytic surface coverages change with time and conditions on a microscopic scale, and resolve the surface coverage with atomistic detail (Pavlišič et al, 2020). Microkinetic modeling is an important continuum model with even higher accuracy and reliability than DFT and kMC.…”

Ab Initio Multiscale Process Modeling of Ethane, Propane and Butane Dehydrogenation Reactions: A Review

“…While all individual methods matured and are being constantly developed, using them as in a coupled fashion remains challenging. Although for instance DFT and kMC (or MK) are presently often used together in a sort of dual-scale modeling fashion, coupling with additional scale to include for instance macroscopic reactor transport phenomena or evolution of the catalyst surface structure during the reactor operation is still in its infancy [22].…”

“…A schematic representation of the multiscale modeling, with various methods representing different temporal and spatial scales of the modeling phenomena. (Reprinted with permission from[22]. Copyright 2020 Elsevier).…”

Unsteady Stagnation Point Flow of Hybrid Nanofluid Past a Convectively Heated Stretching/Shrinking Sheet with Velocity Slip

“…Nevertheless, in numerous engineering occasions, the slip effect should be comprised, such as flow over lubricated or coated surfaces, rough or striated surfaces [22] and internal rare field gas flow [23]. Examples of industrial applications involving the slip boundary conditions are fluid flow on multiple interfaces, rare field fluid problems, and also the reacting flow in reactors [24,25]. Navier [26] and Maxwell [27] were the primary researchers who pioneered the study of linear slip boundary conditions, while Wang [28] has well reflected a comprehensive theoretical analysis considering the no-slip boundaries concentrating on the stagnation point flow.…”