Theoretical Perspective on Operando Spectroscopy of Fluxional Nanocatalysts
Abstract
Improvements in operando spectroscopy have enabled the catalysis community to investigate the dynamic nature of catalysts under operating conditions with increasing detail. Still, the highly dynamic nature of some catalysts, such as fluxional supported subnano clusters, presents a formidable challenge even for the most state-of-the-art techniques. Here, the reason is that such fluxional catalytic interfaces contain a variety of thermally accessible states. Operando spectroscopies used in catalysis generally fall into two categories: ensemble-based techniques, which provide spectra containing the signals of the entire ensemble of states of the catalyst and are not necessarily dominated by the most active species, and localized techniques, which provide atomistic-level information about the dynamics of active sites in a very small area, which might not include the most active species. Combining many different kinds of techniques can provide detailed insight; however, we propose that effective utilization of specific computational techniques and approaches within the fluxionality paradigm can fill the gap and enable atomistic characterization of the most relevant catalytic sites.
- Authors:
-
[1];
[2]
- Univ. of California, Los Angeles, CA (United States)
- Univ. of California, Los Angeles, CA (United States); California NanoSystems Inst., Los Angeles, CA (United States)
- Publication Date:
- Research Org.:
- Univ. of California, Los Angeles, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; US Air Force Office of Scientific Research (AFOSR)
- OSTI Identifier:
- 1968775
- Grant/Contract Number:
- SC0019152; AFOSR FA9550-19-1-0261
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry Letters
- Additional Journal Information:
- Journal Volume: 13; Journal Issue: 19; Journal ID: ISSN 1948-7185
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Catalysts; Cluster chemistry; Metal clusters; Molecular structure; X-ray absorption near edge spectroscopy
Citation Formats
Poths, Patricia, and Alexandrova, Anastassia N. Theoretical Perspective on Operando Spectroscopy of Fluxional Nanocatalysts. United States: N. p., 2022.
Web. doi:10.1021/acs.jpclett.2c00628.
Poths, Patricia, & Alexandrova, Anastassia N. Theoretical Perspective on Operando Spectroscopy of Fluxional Nanocatalysts. United States. https://doi.org/10.1021/acs.jpclett.2c00628
Poths, Patricia, and Alexandrova, Anastassia N. Tue .
"Theoretical Perspective on Operando Spectroscopy of Fluxional Nanocatalysts". United States. https://doi.org/10.1021/acs.jpclett.2c00628. https://www.osti.gov/servlets/purl/1968775.
@article{osti_1968775,
title = {Theoretical Perspective on Operando Spectroscopy of Fluxional Nanocatalysts},
author = {Poths, Patricia and Alexandrova, Anastassia N.},
abstractNote = {Improvements in operando spectroscopy have enabled the catalysis community to investigate the dynamic nature of catalysts under operating conditions with increasing detail. Still, the highly dynamic nature of some catalysts, such as fluxional supported subnano clusters, presents a formidable challenge even for the most state-of-the-art techniques. Here, the reason is that such fluxional catalytic interfaces contain a variety of thermally accessible states. Operando spectroscopies used in catalysis generally fall into two categories: ensemble-based techniques, which provide spectra containing the signals of the entire ensemble of states of the catalyst and are not necessarily dominated by the most active species, and localized techniques, which provide atomistic-level information about the dynamics of active sites in a very small area, which might not include the most active species. Combining many different kinds of techniques can provide detailed insight; however, we propose that effective utilization of specific computational techniques and approaches within the fluxionality paradigm can fill the gap and enable atomistic characterization of the most relevant catalytic sites.},
doi = {10.1021/acs.jpclett.2c00628},
journal = {Journal of Physical Chemistry Letters},
number = 19,
volume = 13,
place = {United States},
year = {Tue May 10 00:00:00 EDT 2022},
month = {Tue May 10 00:00:00 EDT 2022}
}
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