In Silico Screening of Iron-Oxo Catalysts for CH Bond Cleavage

International audienceInspired by oxidation enzymes such as P450 and TauD, several groups have based their research on the iron−oxo moiety in the field of alkanes partial oxidation. Still, the controlled cleavage and oxidation of the aliphatic C−H bond remains a prized goal in chemistry. We present here a computational methodology to predict the comparative reactivity of iron−oxo complexes for this process from linear relations based on the sole electronic structure of the reactant state. The efficient correlation of the C−H activation barrier to a simple but intuitive molecular orbital descriptor enables the design of ligands that permit low barrier C−H abstraction steps and the fast screening of novel potential complexes. The activation of the catalyst by a multidentate effect is also evidenced. We anticipate this study to improve the rational design of hydrocarbon oxidation catalysts