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A heterogeneous single-atom palladium catalyst surpassing homogeneous systems for Suzuki coupling

DOI: 10.1038/s41565-018-0167-2 DOI Help

Authors: Zupeng Chen (ETH Zürich) , Evgeniya Vorobyeva (ETH Zürich) , Sharon Mitchell (ETH Zürich) , Edvin Fako (Institute of Chemical Research of Catalonia (ICIQ), The Barcelona Institute of Science and Technology) , Manuel A. Ortuño (Institute of Chemical Research of Catalonia (ICIQ), The Barcelona Institute of Science and Technology) , Núria López (Institute of Chemical Research of Catalonia (ICIQ), The Barcelona Institute of Science and Technology) , Sean M. Collins (University of Cambridge) , Paul A. Midgley (University of Cambridge) , Sylvia Richard (Idorsia Pharmaceuticals Ltd) , Gianvito Vilé (Idorsia Pharmaceuticals Ltd) , Javier Pérez-ramírez (ETH Zürich)
Co-authored by industrial partner: Yes

Type: Journal Paper
Journal: Nature Nanotechnology , VOL 107

State: Published (Approved)
Published: June 2018
Diamond Proposal Number(s): 16967

Abstract: Palladium-catalysed cross-coupling reactions, central tools in fine-chemical synthesis, predominantly employ soluble metal complexes despite recognized challenges with product purification and catalyst reusability. Attempts to tether these homogeneous catalysts on insoluble carriers have been thwarted by suboptimal stability, which leads to a progressively worsening performance due to metal leaching or clustering4. The alternative application of supported Pd nanoparticles has faced limitations because of insufficient activity under the mild conditions required to avoid thermal degradation of the substrates or products. Single-atom heterogeneous catalysts lie at the frontier. Here, we show that the Pd atoms anchored on exfoliated graphitic carbon nitride (Pd-ECN) capture the advantages of both worlds, as they comprise a solid catalyst that matches the high chemoselectivity and broad functional group tolerance of state-of-the-art homogeneous catalysts for Suzuki couplings, and also demonstrate a robust stability in flow. The adaptive coordination environment within the macroheterocycles of ECN facilitates each catalytic step. The findings illustrate the exciting opportunities presented by nanostructuring single atoms in solid hosts for catalytic processes that remain difficult to heterogenize.

Journal Keywords: Catalysis; Catalytic mechanisms; Nanoscale materials; Theoretical chemistry

Subject Areas: Chemistry

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