Laboratory of Catalysis and Catalytic Processes - Research lines - First-principles guided chemical reaction engineering
Research and Publications
First-principles guided chemical reaction engineering
The identification of the dominant reaction mechanism is the center piece in the quest towards an atomic-scale understanding of a catalytic process. In this view, the development of fundamental mathematical models that link insights across all relevant time and space scales is required, spanning from the microscale (making and breaking of chemical bonds, electronic structure) to the macroscale (reactor and reaction engineering). In this respect, methodological approaches that efficiently integrate the various levels of theories into one multiscale analysis are of particular relevance and still represent a great challenge especially for complex processes of real technological interest. Key is to efficiently incorporate electronic structure theory calculations, that explicitly treat the electronic degrees of freedom and the quantum-mechanical nature of the chemical bonds, in the reaction engineering framework.
In this respect, we study in detail the kinetics and the observed behavior of a catalyst material under reacting conditions by means of a multiscale approach. Main activities concern the development of microkinetic models and the fundamental assessment of the interactions between transport and reaction. A broad portfolio of interdisciplinary methodologies is employed, from electronic structure calculations at the nanoscale to computational fluid-dynamics simulations at the macroscale. This has resulted in the development in the new computational framework catalyticFoam (www.catalyticfoam.polimi.it) which can be considered as the enabling tool for the fundamental multiscale analysis of complex catalytic systems. The proposed methodology constitutes a new avenue to transport the ab initio predictive-quality to a new level of system complexity. Such an approach can provide a unique input for the atomic-scale understanding of complex processes, with a profound impact in the rational understanding of the experimental evidence.
So far, the methane partial oxidation and CO2 activation on metal surfaces have been used as show-case. This analysis has substantially contributed to the comprehension of the molecular level mechanisms underlying the macroscopic phenomena. On one hand, these findings have been of primary interest for the interpretation of the complex experimental evidence. On the other hand, they have been of direct use for the design and scale-up of short-contact-time reformers for small scale hydrogen production in the sustainable energy field.
Faculties involved in the project are: Matteo Maestri