Gas reactions under intrapore condensation regime within tailored metal–organic framework catalysts

Iker Agirrezabal-Telleria (), Ignacio Luz, Manuel A. Ortuño (), Mikel Oregui-Bengoechea, Iñaki Gandarias, Núria López, Marty A. Lail and Mustapha Soukri ()
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Iker Agirrezabal-Telleria: Engineering School of the University of the Basque Country (UPV/EHU)
Ignacio Luz: RTI International
Manuel A. Ortuño: Institute of Chemical Research of Catalonia (ICIQ), The Barcelona Institute of Science and Technology (BIST)
Mikel Oregui-Bengoechea: Engineering School of the University of the Basque Country (UPV/EHU)
Iñaki Gandarias: Engineering School of the University of the Basque Country (UPV/EHU)
Núria López: Institute of Chemical Research of Catalonia (ICIQ), The Barcelona Institute of Science and Technology (BIST)
Marty A. Lail: RTI International
Mustapha Soukri: RTI International

Nature Communications, 2019, vol. 10, issue 1, 1-8

Abstract: Abstract Production of 1-butene, a major monomer in polymer industry, is dominated by homogeneous protocols via ethylene dimerization. Homogeneous catalysts can achieve high selectivity but require large amounts of activators and solvents, and exhibit poor recyclability; in turn, heterogeneous systems are robust but lack selectivity. Here we show how the precise engineering of metal–organic frameworks (MOFs) holds promise for a sustainable process. The key to the (Ru)HKUST-1 MOF activity is the intrapore reactant condensation that enhances ethylene dimerization with high selectivity (> 99% 1-butene) and high stability (> 120 h) in the absence of activators and solvents. According to spectroscopy, kinetics, and modeling, the engineering of defective nodes via controlled thermal approaches rules the activity, while intrapore ethylene condensation accounts for selectivity and stability. The combination of well-defined actives sites with the concentration effect arising from condensation regimes paves the way toward the development of robust MOF catalysts for diverse gas-phase reactions.

Date: 2019
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DOI: 10.1038/s41467-019-10013-6

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