Multiscale modeling of reaction-coupled transport of molecules in zeolite catalysts for alcohol dehydration

Zeolites, characterized by their well-defined crystalline and nanoporous structures, are pivotal in transitioning from fossil fuels to renewable energy sources to produce fuels and chemicals. It is critical to accurately predict reaction rates to surpass traditional trial-and-error methods and foster the development of innovative catalysts for biomass conversion. However, the modeling of zeolite-based catalysts requires the integration of various length and time scales, which are typically addressed independently. Ab initio calculations shed light on reaction mechanisms at the atomic level, while force field (FF) based calculations provide insights into collective behaviors, such as adsorption isotherms and diffusion coefficients. Despite the critical need to merge these scales for precise predictions of catalytic performance, such integrations are seldom seen, especially in the context of dehydration reactions involving bio-based alcohols, which are essential for producing high-value fuel and chemical precursors. This thesis seeks to fill this gap by linking available ab initio simulation data—particularly, reaction mechanisms and associated rate constants for the catalyzed dehydration of isobutanol by proton-exchanged zeolites—with adsorption and diffusion data derived from a multiscale approach. This approach encompasses Monte Carlo simulations, force field molecular dynamics (potentially corroborated by ab initio molecular dynamics), and kinetic Monte Carlo simulations. The ultimate objective is to develop a reactive transport model that can accurately predict effective reaction rates, thus enhancing the design and optimization of zeolite-based catalysts for sustainable chemical processes.

Keywords: Theoretical Chemistry, Molecular modelling, Materials, Diffusion

• Academic and IFPEN supervisor    Dr Carlos NIETO-DRAGHI, IFPEN, carlos.nieto@ifpen.fr, ORCID: 0000-0001-5956-9259
• Academic co supervisor    Dr Benoît Coasne, CNRS, LiPhy, benoit.coasne@univ-grenoble-alpes.fr, ORCID: 0000-0002-3933-9744 
• Doctoral School    ED388, Sorbonne Université
• PhD location    IFPEN, Rueil-Malmaison, France.  
• Duration and start date    3 years, starting from the beginning of November 2025
• Employer    IFPEN
• Academic requirements    University master’s degree in chemical sciences, physical chemistry, materials or condensed-phase chemistry or physics.     
• Language requirements    Fluency in English, and in French or willingness to learn French 
• Other requirements    Molecular Modeling, computer science

To apply, please send your cover letter and CV to the IFPEN supervisor indicated here below.