Low-temperature hydroformylation of ethylene by phosphorous stabilized Rh sites in a one-pot synthesized Rh-(O)-P-MFI zeolite

Minjie Zhao, Chengeng Li, Daviel Gómez, Francisco Gonell, Vlad Martin Diaconescu, Laura Simonelli, Miguel Lopez Haro, Jose Juan Calvino, Debora Motta Meira, Patricia Concepción () and Avelino Corma ()
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Minjie Zhao: Universitat Politècnica de València-Consejo Superior de Investigaciones Científicas (UPV-CSIC)
Chengeng Li: Universitat Politècnica de València-Consejo Superior de Investigaciones Científicas (UPV-CSIC)
Daviel Gómez: Universitat Politècnica de València-Consejo Superior de Investigaciones Científicas (UPV-CSIC)
Francisco Gonell: Universitat Politècnica de València-Consejo Superior de Investigaciones Científicas (UPV-CSIC)
Vlad Martin Diaconescu: CELLS - ALBA Synchrotron Radiation Facility
Laura Simonelli: CELLS - ALBA Synchrotron Radiation Facility
Miguel Lopez Haro: Universidad de Cádiz
Jose Juan Calvino: Universidad de Cádiz
Debora Motta Meira: Argonne National Laboratory
Patricia Concepción: Universitat Politècnica de València-Consejo Superior de Investigaciones Científicas (UPV-CSIC)
Avelino Corma: Universitat Politècnica de València-Consejo Superior de Investigaciones Científicas (UPV-CSIC)

Nature Communications, 2023, vol. 14, issue 1, 1-13

Abstract: Abstract Zeolites containing Rh single sites stabilized by phosphorous were prepared through a one-pot synthesis method and are shown to have superior activity and selectivity for ethylene hydroformylation at low temperature (50 °C). Catalytic activity is ascribed to confined Rh2O3 clusters in the zeolite which evolve under reaction conditions into single Rh3+ sites. These Rh3+ sites are effectively stabilized in a Rh-(O)-P structure by using tetraethylphosphonium hydroxide as a template, which generates in situ phosphate species after H2 activation. In contrast to Rh2O3, confined Rh0 clusters appear less active in propanal production and ultimately transform into Rh(I)(CO)2 under similar reaction conditions. As a result, we show that it is possible to reduce the temperature of ethylene hydroformylation with a solid catalyst down to 50 °C, with good activity and high selectivity, by controlling the electronic and morphological properties of Rh species and the reaction conditions.

Date: 2023
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DOI: 10.1038/s41467-023-42938-4

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