Active and Regioselective Ru Single-Site Heterogeneous Catalystsfor Alpha-Olefin Hydroformylation

Abstract

[EN] A heterogeneous ruthenium catalyst consisting ofisolated single atoms and disordered clusters stabilized in a N-doped carbon matrix has been synthesized with very good activityand remarkable regioselectivity in the hydroformylation of 1-hexene. The role of the nitrogen heteroatoms has been probedessential to increase the catalyst stability and activity, enabling thestabilization of Ru(II)-N sites according to X-ray photoelectronspectroscopy (XPS) and XANES. Intrinsic size-dependent activityof Ru species of different atomicity has been extracted, correlatingthe observed reaction rate and the particle size distributiondetermined by means of aberration-corrected high-angle annulardark-field scanning transmission electron microscopy, permittingthe identification of single-atom sites as the most active ones. This catalyst appears as a promising alternative with respect to itsheterogeneous counterparts, paving the way for designing improved Ru heterogeneous catalysts.