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

Zhao, Yuxin; Bozkurt, Özge D.; Kurtoğlu-Öztulum, Samira F.; Yordanli, Melisa Su; Hoffman, Adam S.; Hong, Jiyun; Perez-Aguilar, Jorge E.; Saltuk, Aylin; Akgül, Deniz; Demircan, Oktay; Ateşin, Tülay A.; Aviyente, Viktorya; Gates, Bruce C.; Bare, Simon R.; Uzun, Alper

doi:10.1016/j.jcat.2023.115196

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

Journal Article · Sat Nov 04 00:00:00 EDT 2023 · Journal of Catalysis

DOI:https://doi.org/10.1016/j.jcat.2023.115196· OSTI ID:2328668

Zhao, Yuxin ^[1]; ^[2]; Kurtoğlu-Öztulum, Samira F. ^[2]; Yordanli, Melisa Su ^[3]; ^[4]; ^[4]; Perez-Aguilar, Jorge E. ^[4]; Saltuk, Aylin ^[3]; ^[3]; ^[3]; ^[5]; ^[3]; ^[6]; ^[4]; ^[2]

Koç Univ., Istanbul (Turkey); SLAC
Koç Univ., Istanbul (Turkey)
Bogazici Univ., Istanbul (Turkey)
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
University of Texas Rio Grande Valley, Edinburg, TX (United States)
Univ. of California, Davis, CA (United States)

In this study, 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.

View Accepted Manuscript (DOE)

Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Univ. of California, Davis, CA (United States)

Sponsoring Organization:: National Center for High Performance Computing of Turkey (UHEM); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: AC02-76SF00515; FG02-04ER15513

OSTI ID:: 2328668

Alternate ID(s):: OSTI ID: 2222514

Journal Information:: Journal of Catalysis, Journal Name: Journal of Catalysis Vol. 429; ISSN 0021-9517

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Electronic structure effect
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density functional theory

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References (55)

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