Development of bio-inspired/catalysts for tandem processes. Synthesis of biologically relevant molecules
Head researcher: Mariette M. Pereira
Research Area: Coordination Chemistry and Catalysis
Abstract
There is a growing interest in the application of sequential/tandem one-pot reactions that allow the maximization of structural complexity of “simple” molecules with a minimum of synthetic isolated steps.
Particularly, the development of multicatalytic processes for activation of “small molecules” (O2, CO2, CO and H2) in order to prepare biologically relevant products is of upmost importance.
In biological systems, these molecules are paradigmatic entities, since they may act as reservoirs of chemical energy and crucial synthons for the construction of complex structures.
However, they are thermodynamically stable and their successful utilization as reactants requires overcoming high kinetics barriers, where metal catalysts such as the enzyme’s prosthetic groups play important roles.
Outside biological systems, their activation has been successfully achieved by the use of catalysts based on expensive and toxic transition metals.
Nevertheless, to mimic enzymatic processes, the continuous search for active and selective bio-inspired catalysts using nontoxic and earth-abundant first-row metal complexes is considered a major aspiration for the future of catalysis.
The main goal of this project is the design and synthesis of active, selective and reusable bio-inspired catalysts, based on cheap/less-pollutant metals (Fe, Cu, Co, Zn, Ru) and appropriate P- and N-based ligands, to selectively promote the activation of small molecules via sequential/tandem multicatalytic reactions, aiming at the preparation of added-value products with potential biological activity.
Selected Publications
1. Hydroaminomethylation reaction as powerful tool for preparation of rhodium/phosphine functionalized nanomaterials. Catalytic evaluation in styrene hydroformylation, Fábio M. S. Rodrigues, Mário J. F. Calvete, Carlos J. P. Monteiro, Sónia A. C. Carabineiro, Teresa M. R. Maria, José L. Figueiredo, Mariette M. Pereira, Catalysis Today (2019), in press, DOI: 10.1016/j.cattod.2019.05.045.
2. A novel Pd-catalysed sequential carbonylation/cyclization approach toward bis-N-heterocycles: rationalization by electronic structure calculations, Liliana Damas, Rui M. B. Carrilho, Sandra C. C. Nunes, Alberto A. C. C. Pais, L. Kollar, M. Pineiro, Mariette M. Pereira, Royal Society Open Science 5 (2018) 181140 DOI: 10.1098/rsos.181140.
3. Dual Rh-Ru catalysts for reductive hydroformylations of olefins to alcohols, Fábio M. S. Rodrigues, Peter K. Kucmierczyk, Marta Pineiro, Ralf Jackstell, Robert Franke, Matthias Beller, Mariette M. Pereira, ChemSusChem 11 (2018), 2310-2314 DOI: 10.1002/cssc.201800488.