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OX-1 metal-organic framework nanosheets as robust hosts for highly active catalytic palladium species

DOI: 10.1021/acssuschemeng.8b05843 DOI Help

Authors: Kirill Titov (University of Oxford) , Dmitry Eremin (Zelinsky Institute of Organic Chemistry, Russian Academy of Sciences) , Alexey S. Kashin (Zelinsky Institute of Organic Chemistry, Russian Academy of Sciences) , Roberto Boada Romero (Diamond Light Source) , Barbara Souza (University of Oxford) , Chris S. Kelley (Diamond Light Source) , Mark D. Frogley (Diamond Light Source) , Gianfelice Cinque (Diamond Light Source) , Diego Gianolio (Diamond Light Source) , Giannantonio Cibin (Diamond Light Source) , Svemir Rudic (ISIS Facility) , Valentine P Ananikov (Zelinsky Institute of Organic Chemistry, Russian Academy of Sciences) , Jin-chong Tan (University of Oxford)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Acs Sustainable Chemistry & Engineering

State: Published (Approved)
Published: February 2019
Diamond Proposal Number(s): 14902 , 17146

Abstract: A catalytic system based on OX-1 metal-organic framework nanosheets is reported, incorporating catalytically active palladium (Pd) species. The Pd@OX-1 guest@host system is rapidly synthesised via a facile single-pot supramolecular assembly method, with the possibility of controlling the Pd loading. The structures of the re-sulting framework and of the active Pd species before and after catalytic reactions are studied in detail using a wide variety of techniques including synchrotron radiation infrared spectroscopy, inelastic neutron scattering and X-ray absorption spectroscopy. Crystals of the resulting Pd@OX-1 composite material contain predomi-nantly atomic and small cluster Pd species, which selectively reside on benzene rings of the benzenedicarbox-ylate (BDC) linkers. The composites are shown to efficiently catalyse the Suzuki coupling and Heck arylation reactions under a variety of conditions. Pd@OX-1 further shows potential to be recycled for at least five cycles of each reaction as well as an ability to recapture active Pd species during both catalytic reactions.

Journal Keywords: nanosheets; metal-organic framework; palladium; catalysis; inelastic scattering

Subject Areas: Materials, Chemistry


Instruments: B18-Core EXAFS , B22-Multimode InfraRed imaging And Microspectroscopy

Other Facilities: ISIS