Description of the thesis topic

The aim of this PhD thesis is the atomistic modeling of the mechanism of the electro-conversion of isopropanol to acetone and, subsequently, to propose alternative catalysts (other than Pt-Ru) with improved stability. The computations will primarily be conducted using grand-canonical DFT, treating the electrochemical potential explicitly and the solvent implicitly. A part of the mechanistic study, related to the adsorption/desorption of reactants and products, will be carried using explicit water molecules relying on molecular dynamics (thermodynamic integration and/or metadynamics).

The screening for improved catalysts compared to the state-of-the-art (Pt-Ru) will start by exploiting foundational machine-learning potentials such as MACE, SevenNet, or Orb-V3. The predictions will then be progressively refined and verified by DFT and, ultimately, tested experimentally by project collaborators.

Work Context

This thesis will take place within the framework of a European project (IsoPROPEL) in close collaboration with Forschungszentrum Jülich (Germany) for cell design and catalytic testing and ITQ Valencia (Spain) for the synthesis of catalysts. The overall goal of IsoPROPEL is to develop fuel cells that utilize the isopropanol/acetone couple for boats navigating European waterways (canals and rivers).

The recruited candidate will be affiliated as a PhD student at ENS Lyon and registered with the graduate school of Chemistry.

The theoretical chemistry and molecular thermodynamics group of the "Laboratoire de Chimie" is well-known in the field of computational heterogeneous catalysis and electrocatalysis. The following review reflects the spirit of their work in electrocatalysis: doi 10.1002/wcms.1499. The group is highly international and offers a stimulating environment featuring a wide range of research activities, including QM/MM simulations, ionic liquid simulations, and excited-state characterization.

Constraints and risks

Proficiency in English is required.