Dr. Alexis Bordet - Multifunctional Catalytic Systems

Molecular modifiers commonly used in our group include small organic molecules, ionic liquids, and polymers. Metal nanoparticles (e.g. Mn, Fe, Co, Ni, Ru, Rh, Pt and bimetallic) are synthesized directly in the MMS from organometallic precursors under mild conditions. This organometallic approach provides a fine control over the nanoparticles size, dispersion, and in the case of bimetallic nanoparticles, composition. In addition, this insures a close contact between the metal NPs and the molecular modifiers, leading to high NPs stability and strong synergistic effects.

Relevant recent publications:

• Accounts: Bordet, A., Leitner, W. Metal Nanoparticles Immobilized on Molecularly Modified Surfaces: Versatile Catalytic Systems for Controlled Hydrogenation and Hydrogenolysis. Acc. Chem. Res. 2021, 54, 2144-2157 https://doi.org/10.1021/acs.accounts.1c00013
• N. Antil et al. Ruthenium Nanoparticles on Water-Stable Supported Ionic Liquid Phases as Catalytic Systems for Aqueous Phase CO₂ Hydrogenation. ACS Catal. 2025, 15, 14601-14610. https://doi.org/10.1021/acscatal.5c03605
• M. Durai et al. One-Pot Synthesis of E-Chalcones Using a Multifunctional Catalyst Comprised of Ruthenium Nanoparticles and Palladium N-Heterocyclic Carbene Complexes Immobilized on Silica. Chem. Sci. 2025, 16, 5776-5785. https://doi.org/10.1039/D4SC07773C
• J. Zenner et al. Bimetallic Mn_xRu_100-x Nanoparticles on Supported Ionic Liquid Phases (Mn_xRu_100-x@SILP) as Tunable Hydrogenation Catalysts. ACS Catal. 2025, 15, 3227-3235. https://doi.org/10.1021/acscatal.4c05494
• W. Fang et al. Molecularly Modified Aluminum Phosphates as Support Materials for Ru Nanoparticles in Selective Hydrogenation. J. Catal. 2025, 442, 115911. https://doi.org/10.1016/j.jcat.2024.115911
• Levin et al. Decarboxylation and Tandem Reduction/Decarboxylation Pathways to Substituted Phenols from Aromatic Carboxylic Acids using Bimetallic Nanoparticles on Supported Ionic Liquid Phases as Multifunctional Catalysts. J. Am. Chem. Soc. 2023, 145, 22845-22854. https://doi.org/10.1021/jacs.3c09290

From Optimized to Adaptive Catalytic Systems

While the developed NPs@MMS catalysts present outstanding properties regarding their dedicated tasks, their performance is typically optimized to remain static (Figure 2a). However, flexibility and adaptivity are becoming increasingly important to cope with the dynamics of alternative energy resources, quality variations of chemical feedstocks, and to enable customized and decentralized production. 

In this context, we work on the design of adaptive catalytic systems (Figure 2b), that we recently defined as “capable of adjusting or being adjusted into different states of their performance in response to dynamic changes in the reactive environment”, and that provide opportunities to adjust product selectivity (i.e. adaptivity in product formation) and/or catalytic activity (i.e. adaptivity to intermittent electricity supply). The switch of the catalyst state must be reversible, rapid, and robust manner (R³ rule), and can be initiated through the application of various types of external stimuli (e.g. electrons, photons, magnetic fields, reversible chemical reactions, etc.).

Relevant recent publications:

• Scientific perspective: A. Bordet et al. Magnetically-Induced Catalysis: Definition, Advances and Potential. Angew. Chem. Int. Ed. 2025, e202424151. https://doi.org/10.1002/anie.202424151
• S. Ahmedi et al. Magnetically Induced Iron-Catalyzed Hydrodeoxygenation of Benzylic Esters and Polyesters. J. Am. Chem. Soc. 2025, 147, 34758-34766. https://doi.org/10.1021/jacs.5c10464
• S.-H. Lin et al. Low-Pressure Amide Hydrogenation Enabled by Magnetocatalysis. Nat. Commun. 2025, 16, 3464. https://doi.org/10.1038/s41467-025-58713-6
• S.-H. Lin et al. Copper-Decorated Iron Carbide Nanoparticles Heated by Magnetic Induction as Adaptive Multifunctional Catalysts for the Selective Hydrodeoxygenation of Aldehydes. Adv. Energy Mater. 2022, 2201783. https://doi.org/10.1002/aenm.202201783
• H. Kreissl et al. Commercial Cu₂Cr₂O₅ Decorated with Iron Carbide Nanoparticles as Multifunctional Catalyst for Magnetically Induced Continuous Flow Hydrogenation of Aromatic Ketones. Angew. Chem. Int. Ed. 2021, 60, 26639-26646. https://doi.org/10.1002/anie.202107916

Adaptivity through the use of molecular triggers (e.g. CO₂, CO, etc.) 

In this research line, we explore the use of small molecule as triggers to control the selectivity of catalytic systems in an adaptive manner. This is achieved by introducing specific functionalities in our molecular modifiers that take part in reversible chemical reactions used to modify metal active sites and impact on intermediates and transition states of the catalytic cycle, thereby opening or closing certain pathways. As a prominent recent example, we have shown that CO₂ can be a very effective trigger, using the CO₂ + H₂  HCOOH equilibrium to switch the selectivity in hydrogenation of appropriately-designed NPs@MMS catalysts in a fully reversible, rapid, and robust manner (Figure 4). Current work focuses on simplifying and expanding the application of this concept, and exploring other potential molecular triggers such as CO and NH₃.