Understanding and advancing the reactivity of biomimetic models for mononuclear non-heme iron enzymes

• Applicant: Professor Dr. Christian Limberg
• Subject Area: Inorganic Molecular Chemistry - Synthesis and Characterisation
• Term: since 2022
• Project identifier: Deutsche Forschungsgemeinschaft (DFG) - Project number 445916766

In recent years we have been able to develop rather realistic trispyrazolyl borate-based structural and functional models for representatives of O2-activating non-heme iron enzymes, like the Cysteine Dioxygenase (CDO), the 2-Aminoethanethiol Dioxygenase (ADO) and the 1-Aminocyclopropane-1-carboxylic acid Oxidase (ACCO). However, due to the complexity of their multi-step conversions mechanistic information until now could only be accessed indirectly, and the trapping and experimental identification of intermediates has so far remained challenging. The main goal of this project is to contribute to the understanding of the complicated mechanisms, by which such mononuclear non-heme iron enzymes convert their amino acid substrates and the cysteine-related aminoethanethiol, respectively, with the aid of faithful model compounds constructed with carefully selected and designed ligand systems. Particular emphasis will lie on the identification of transient species to reveal the reaction principles inherent to such enzymes as a basis for the development of synthetic O2-activating iron catalysts, and cooperations within the FOR team will be key.

• DFG Programme: Research Units
• Subproject of: FOR 5215: Bioinspired Oxidation Catalysis with Iron Complexes