Litcius/Paper detail

Adaptive Catalysts for the Selective Hydrogenation of Bicyclic Heteroaromatics using Ruthenium Nanoparticles on a CO<sub>2</sub>‐Responsive Support

Yuyan Zhang, Sami El Sayed, Liqun Kang, Matthew Sanger, Thomas Wiegand, Philip G. Jessop, Serena DeBeer, Alexis Bordet, Walter Leitner

2023Angewandte Chemie International Edition12 citationsDOIOpen Access PDF

Abstract

Abstract Ruthenium nanoparticles (NPs) immobilized on an amine‐functionalized polymer‐grafted silica support act as adaptive catalysts for the hydrogenation of bicyclic heteroaromatics. Whereas full hydrogenation of benzofuran and quinoline derivatives is achieved under pure H 2 , introducing CO 2 into the H 2 gas phase leads to an effective shutdown of the arene hydrogenation while preserving the activity for the hydrogenation of the heteroaromatic part. The selectivity switch originates from the generation of ammonium formate species on the surface of the materials by catalytic hydrogenation of CO 2 . The CO 2 hydrogenation is fully reversible, resulting in a robust and rapid switch between the two states of the catalyst adapting its performance in response to the feed gas composition. A variety of benzofuran and quinoline derivatives were hydrogenated to fully or partially saturated products in high selectivity and yields simply by altering the composition of the feed gas from H 2 to H 2 /CO 2 . The adaptive catalytic system thus provides controlled access to valuable products using a single catalyst rather than two specific and distinct catalysts with static reactivity.

Topics & Concepts

RutheniumCatalysisBicyclic moleculeNanoparticleCombinatorial chemistryChemistryNoyori asymmetric hydrogenationSelectivityOrganic chemistryNanotechnologyMaterials scienceAsymmetric Hydrogenation and CatalysisCatalysis for Biomass ConversionCarbon dioxide utilization in catalysis