High‐Energy‐Resolution X‐ray Absorption Spectroscopy for Identification of Reactive Surface Species on Supported Single‐Site Iridium Catalysts
Abstract
Abstract We report high‐energy‐resolution X‐ray absorption spectroscopy detection of ethylene and CO ligands adsorbed on catalytically active iridium centers isolated on zeolite HY and on MgO supports. The data are supported by density functional theory and FEFF X‐ray absorption near‐edge modelling, together with infrared (IR) spectra. The results demonstrate that high‐energy‐resolution X‐ray absorption spectra near the iridium L III (2p 3/2 ) edge provide clearly ascribable, distinctive signatures of the ethylene and CO ligands and illustrate effects of supports and other ligands. This X‐ray absorption technique is markedly more sensitive than conventional IR spectroscopy for characterizing surface intermediates, and it is applicable to samples having low metal loadings and in reactive atmospheres and is expected to have an increasing role in catalysis research by facilitating the determination of mechanisms of solid‐catalyzed reactions through identification of reaction intermediates in working catalysts.
- Authors:
-
[4]
- Department of Chemical Engineering University of California, Davis Davis CA 95616 USA, Present address: Stanford Synchrotron Radiation Lightsource SLAC National Accelerator Laboratory Menlo Park CA 94025 USA
- Stanford Synchrotron Radiation Lightsource SLAC National Accelerator Laboratory Menlo Park CA 94025 USA
- Department of Chemistry The University of Alabama Tuscaloosa AL 35487 USA
- Department of Chemical Engineering University of California, Davis Davis CA 95616 USA
- Department of Chemical Engineering University of California, Davis Davis CA 95616 USA, Department of Materials Science and Engineering University of California, Davis Davis CA 95616 USA
- Department of Chemical Engineering Stanford University Stanford CA 94305 USA, SUNCAT Center for Interface Science and Catalysis SLAC National Accelerator Laboratory Menlo Park CA 94025 USA
- Publication Date:
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1401811
- Grant/Contract Number:
- AC02-76SF00515
- Resource Type:
- Publisher's Accepted Manuscript
- Journal Name:
- Chemistry - A European Journal
- Additional Journal Information:
- Journal Name: Chemistry - A European Journal Journal Volume: 23 Journal Issue: 59; Journal ID: ISSN 0947-6539
- Publisher:
- Wiley Blackwell (John Wiley & Sons)
- Country of Publication:
- Germany
- Language:
- English
Citation Formats
Hoffman, Adam S., Sokaras, Dimosthenis, Zhang, Shengjie, Debefve, Louise M., Fang, Chia‐Yu, Gallo, Alessandro, Kroll, Thomas, Dixon, David A., Bare, Simon R., and Gates, Bruce C. High‐Energy‐Resolution X‐ray Absorption Spectroscopy for Identification of Reactive Surface Species on Supported Single‐Site Iridium Catalysts. Germany: N. p., 2017.
Web. doi:10.1002/chem.201701459.
Hoffman, Adam S., Sokaras, Dimosthenis, Zhang, Shengjie, Debefve, Louise M., Fang, Chia‐Yu, Gallo, Alessandro, Kroll, Thomas, Dixon, David A., Bare, Simon R., & Gates, Bruce C. High‐Energy‐Resolution X‐ray Absorption Spectroscopy for Identification of Reactive Surface Species on Supported Single‐Site Iridium Catalysts. Germany. https://doi.org/10.1002/chem.201701459
Hoffman, Adam S., Sokaras, Dimosthenis, Zhang, Shengjie, Debefve, Louise M., Fang, Chia‐Yu, Gallo, Alessandro, Kroll, Thomas, Dixon, David A., Bare, Simon R., and Gates, Bruce C. Thu .
"High‐Energy‐Resolution X‐ray Absorption Spectroscopy for Identification of Reactive Surface Species on Supported Single‐Site Iridium Catalysts". Germany. https://doi.org/10.1002/chem.201701459.
@article{osti_1401811,
title = {High‐Energy‐Resolution X‐ray Absorption Spectroscopy for Identification of Reactive Surface Species on Supported Single‐Site Iridium Catalysts},
author = {Hoffman, Adam S. and Sokaras, Dimosthenis and Zhang, Shengjie and Debefve, Louise M. and Fang, Chia‐Yu and Gallo, Alessandro and Kroll, Thomas and Dixon, David A. and Bare, Simon R. and Gates, Bruce C.},
abstractNote = {Abstract We report high‐energy‐resolution X‐ray absorption spectroscopy detection of ethylene and CO ligands adsorbed on catalytically active iridium centers isolated on zeolite HY and on MgO supports. The data are supported by density functional theory and FEFF X‐ray absorption near‐edge modelling, together with infrared (IR) spectra. The results demonstrate that high‐energy‐resolution X‐ray absorption spectra near the iridium L III (2p 3/2 ) edge provide clearly ascribable, distinctive signatures of the ethylene and CO ligands and illustrate effects of supports and other ligands. This X‐ray absorption technique is markedly more sensitive than conventional IR spectroscopy for characterizing surface intermediates, and it is applicable to samples having low metal loadings and in reactive atmospheres and is expected to have an increasing role in catalysis research by facilitating the determination of mechanisms of solid‐catalyzed reactions through identification of reaction intermediates in working catalysts.},
doi = {10.1002/chem.201701459},
journal = {Chemistry - A European Journal},
number = 59,
volume = 23,
place = {Germany},
year = {Thu Jul 27 00:00:00 EDT 2017},
month = {Thu Jul 27 00:00:00 EDT 2017}
}
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