Atomically dispersed zeolite-supported rhodium complex: Selective and stable catalyst for acetylene semi-hydrogenation

Document Type

Article

Publication Date

1-2024

Abstract

Highlights

  • Rhodium has heretofore been known to be unselective for acetylene semi-hydrogenation.

  • Electronic properties of rhodium are tuned by choice of support and metal nuclearity.

  • Selectivity is maximized when Rh is atomically dispersed on a weak electron donor.

  • Zeolite-supported Rh complex with C2H2 ligands offers a stable C2H4 selectivity > 90 %.

  • Results demonstrate unprecedented catalytic properties of Rh for semi-hydrogenation.

Abstract

Supported rhodium catalysts are known to be unselective for semi-hydrogenation reactions. Here, by tuning the electronic structure of supported mononuclear rhodium sites determined by the metal nuclearity and the electron-donor properties of the support, we report that atomically dispersed HY zeolite-supported rhodium with reactive acetylene ligands affords a stable ethylene selectivity > 90 % for acetylene semi-hydrogenation at 373 K and atmospheric pressure, even when ethylene is present in a large excess over acetylene. Infrared and X-ray absorption spectra and measurements of rates of the catalytic reaction complemented with calculations at the level of density functional theory show how the catalyst performance depends on the electronic structure of the rhodium, influenced by the support as a ligand that is a weak electron donor.

Publication Title

Journal of Catalysis

DOI

10.1016/j.jcat.2023.115196

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