Observations of Ethylene-for-CO Ligand Exchanges on a Zeolite-Supported Single-Site Rh Catalyst by X-ray Absorption Spectroscopy

Hoffman, Adam S.; Müller, Oliver; Hong, Jiyun; Canning, Griffin A.; Fang, Chia-Yu; Perez-Aguilar, Jorge E.; Gates, Bruce C.; Bare, Simon R.

doi:10.1021/acs.jpclett.3c00349

Title: Observations of Ethylene-for-CO Ligand Exchanges on a Zeolite-Supported Single-Site Rh Catalyst by X-ray Absorption Spectroscopy

Journal Article · 11 May 2023 · Journal of Physical Chemistry Letters

DOI: https://doi.org/10.1021/acs.jpclett.3c00349 · OSTI ID:1974045

^[1]; Müller, Oliver ^[1]; Hong, Jiyun ^[1]; Canning, Griffin A. ^[2]; Fang, Chia-Yu ^[3]; Perez-Aguilar, Jorge E. ^[4];

^[3];

^[1]

SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
Pennsylvania State Univ., University Park, PA (United States)
Univ. of California, Davis, CA (United States)
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL); Univ. of California, Davis, CA (United States)

Quick-scanning X-ray absorption fine structure (QXAFS) measurements were used to characterize the exchanges of ethylene and CO ligands in a zeolite HY-supported single-site Rh complex at a sampling rate of 1.0 Hz. The two ligands were reversibly exchanged on the rhodium, with quantitative results determined for the C₂H₄-for-CO exchange that are consistent with a first-order process. The apparent rate constant for the exchange decreased with increasing temperature. Fourier-transform infrared spectra characterizing the C₂H₄ sorbed in the zeolite showed that the amount decreased with increasing temperature, consistent with the decrease in the exchange rate with increasing temperature. Here the results, illustrating the dynamics of ligand exchanges on a single-site supported metal catalyst, demonstrate the broad emerging applicability of the QXAFS technique for characterizing the dynamics of reactive intermediates on catalysts.

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); USDOE Office of Science (SC), Office of Workforce Development for Teachers & Scientists (WDTS); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-76SF00515; FG0204ER15513; FG02-04ER15513

OSTI ID:: 1974045

Alternate ID(s):: OSTI ID: 2263479

Journal Information:: Journal of Physical Chemistry Letters, Vol. 14, Issue 19; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
QEXAFS
QXAFS
XAS
kinetics
spectroscopy
rhodium
single-site catalyst
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Title: Observations of Ethylene-for-CO Ligand Exchanges on a Zeolite-Supported Single-Site Rh Catalyst by X-ray Absorption Spectroscopy

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