Lars FABER PhD defense

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Organometallics: Materials & Catalysis (OMC) team Abstract Sustainable catalytic processes are essential to meet the growing demand for resource-efficient and environmentally benign chemical production. Although homogeneous catalysis offers outstanding activity and selectivity, its industrial application remains limited by challenges in catalyst recovery and reuse. This thesis addresses these limitations through the development of catalytic methodologies, catalyst recovery strategies, and earth-abundant catalysts, with a particular focus on integrating organic solvent nanofiltration (OSN) into homogeneous catalytic processes. The first part of this work investigates the valorisation of biomass-derived terpenoids through ring-closing olefin metathesis to access value-added cyclic compounds. The introduction of OSN subsequently allowed the shift in equilibrium towards the macrocyclisation of olefinic esters to give macrocyclic lactones in the second part of this work. The applicability of nanofiltration is further demonstrated in form of the reuse of an iridium catalyst for transfer hydrogenation toward valerolactone, enabling efficient catalyst recovery and reuse over multiple catalytic cycles. The final chapters focus on the development of manganese-based transfer hydrogenation catalysts as sustainable alternatives to noble metals. Catalyst design evolved from base-mediated systems to base-free catalytic protocols, providing insight into ligand design and structure–activity relationships while advancing more practical and environmentally benign transfer hydrogenation methodologies. Overall, this thesis demonstrates complementary approaches to improving the sustainability of homogeneous catalysis through renewable feedstock valorisation, membrane-assisted process intensification, catalyst reuse, and the development of catalysts based on earth-abundant metals. Jury Dr. Estelle Métay, CNRS Research Director, ICBMS, Lyon / Reviewer Prof. Jean-François Soulé, Chimie Paritech-PSL, Paris / Reviewer Dr. Evgueni Kirillov, Associate Professor, University of Rennes, ISCR / Examinator Dr. Andreas Vorholt, Deputy-professor, MPI, RWTH Aachen, Germany / Examinator Prof. Murielle Rabiller-Baudry, University of Rennes, ISCR / Examinator Invited Dr. Christian Bruneau, University of Rennes PhD director Dr. Cédric Fischmeister, CNRS research engineer HDR, University of Rennes, ISCR Contact Cédric Fischmeister_,_ cedric.fischmeister@univ-rennes.fr