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Research

Sustainable Catalysis with Earth-abundant Metals

One of the most daunting challenges in chemistry is to develop environmentally friendly and efficient catalytic processes that contribute to advancing towards a more sustainable chemical industry. Catalysis plays a pivotal role in addressing the urgent demand of achieving green production of high-value chemicals from abundant and renewable feedstocks.

On the quest of more sustainable organic synthesis, our research group focuses on the discovery and development of earth-abundant metal-catalyzed organic reactions. The exploration of base metals (Mn, Fe, Co, Ni) in catalysis is still in an early stage in comparison to noble metals (for instance, Pd, Rh, Ir). The unique chemical properties of base metals, together with creative ligand design, offers an outstanding opportunity to discover innovative catalytic methodologies.

Our interdisciplinary projects span across the areas of organic chemistry, organometallic chemistry and catalysis. We focus in developing innovative synthetic methods and in performing  mechanistic studies to elucidate catalytic cycles involving mid to late first-row metals. To accomplish these goals, modern spectroscopic and theoretical methods are integrated in our projects. 

Current research lines:

1. Low-valent cobalt catalysis. Despite reductive cobalt-catalyzed methods are gaining momentum as an environmentally benign alternative to the methods described with its heavier congeners Rh and Ir. Monovalent cobalt(I) species are often proposed as the active catalytic species that are formed in situ by either the use of metal reductants (Zn, Mn) or photoredox catalysts under reductive quenching cycles. However, the complete mechanistic picture for many of the developed reactions still remains elusive.   We focus on the development of catalytic methodologies towards bond-forming processes by using well-defined cobalt(I) complexes, while elucidating reactions mechanisms. Gaining mechanistic undestanding is essential to apply a rational design towards the invention or re-design of metal-catalyzed organic reactions.

Key publications: Experimental and Computational Studies on Cobalt(I)-Catalyzed Regioselective Allylic Alkylation Reactions. Angew. Chem. Int. Ed. 2023, 62, e202310129. 

2. Unlocking the synthesis and reactivity of high-valent organoiron complexes. Organometallic iron complexes in formal high oxidation state that contain either metal–carbon s-bonds or metal–carbon multiple bonds (alkylidenes and carbynes) are exceedingly rare due to their inherent thermal unstability. Aiming at fulfilling this gap, in this project we tarted the synthetic, structural and reactivity studies of novel high-valent organometallic iron complexes. Reactivity studies focus on metal complexes that display distinctive electronic and/or coordination environments for the metal center could potentially unveil new chemical transformations.

Key publications: Synthesis of Fe(IV) cyanide complexes using hypervalent iodine(III) reagents as cyano-transfer one-electron oxidants. Angew. Chem. Int. Ed. 2022, 61, e202201699