In situ, operando studies on the size and structure of supported Pt catalysts under supercritical conditions by simultaneous synchrotron-based X-ray techniques
Abstract
To control the size and structure of supported Pt catalysts, the influence of additional metal particles and the effect of supports were elucidated during the cracking reaction of n-dodecane under supercritical reaction conditions. The dynamical changes in nanocatalysts and catalytic activity are studied under realistic reaction conditions by using a combination of simultaneous temperature-programmed heating, in situ Small Angle X-ray Scattering (SAXS) and X-ray Absorption Near Edge Structure (XANES). In situ SAXS results indicate that the stability of the catalysts increases with Sn concentration. In situ XANES analysis reveals that the degree of oxidation and the electronic states of catalysts are dependent on the amount of Sn. Carbonaceous deposits over spent catalysts were characterized by Raman spectroscopy, suggesting that the highest Sn loading inhibits the formation of disordered graphitic lattices, which leads to an increased catalytic activity. SiO2, γ-Al2O3 and Mg(Al)Ox were employed as supports to investigate the support effect on the stability of Pt catalysts. In situ SAXS and XANES findings clearly reflect the improved stability of catalysts on γ-Al2O3 and Mg(Al)Ox supports compared to Pt catalysts on SiO2 and the electronic states of catalysts are strongly influenced by support materials.
- Authors:
-
[1];
[1];
[2];
[2];
[2];
[2];
[1]
- Argonne National Lab. (ANL), Lemont, IL (United States)
- Univ. of Wisconsin, Madison, WI (United States)
- Publication Date:
- Research Org.:
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC); Air Force Research Laboratory (AFRL); US Air Force Office of Scientific Research (AFOSR)
- OSTI Identifier:
- 1559532
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Chemistry Chemical Physics. PCCP
- Additional Journal Information:
- Journal Volume: 21; Journal Issue: 22; Journal ID: ISSN 1463-9076
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Lee, Sungwon, Lee, Sungsik, Gerceker, Duygu, Kumbhalkar, Mrunmayi D., Wiaderek, Kamila M., Ball, Madelyn R., Mavrikakis, Manos, Dumesic, James A., and Winans, Randall E. In situ, operando studies on the size and structure of supported Pt catalysts under supercritical conditions by simultaneous synchrotron-based X-ray techniques. United States: N. p., 2019.
Web. doi:10.1039/C9CP00347A.
Lee, Sungwon, Lee, Sungsik, Gerceker, Duygu, Kumbhalkar, Mrunmayi D., Wiaderek, Kamila M., Ball, Madelyn R., Mavrikakis, Manos, Dumesic, James A., & Winans, Randall E. In situ, operando studies on the size and structure of supported Pt catalysts under supercritical conditions by simultaneous synchrotron-based X-ray techniques. United States. https://doi.org/10.1039/C9CP00347A
Lee, Sungwon, Lee, Sungsik, Gerceker, Duygu, Kumbhalkar, Mrunmayi D., Wiaderek, Kamila M., Ball, Madelyn R., Mavrikakis, Manos, Dumesic, James A., and Winans, Randall E. Wed .
"In situ, operando studies on the size and structure of supported Pt catalysts under supercritical conditions by simultaneous synchrotron-based X-ray techniques". United States. https://doi.org/10.1039/C9CP00347A. https://www.osti.gov/servlets/purl/1559532.
@article{osti_1559532,
title = {In situ, operando studies on the size and structure of supported Pt catalysts under supercritical conditions by simultaneous synchrotron-based X-ray techniques},
author = {Lee, Sungwon and Lee, Sungsik and Gerceker, Duygu and Kumbhalkar, Mrunmayi D. and Wiaderek, Kamila M. and Ball, Madelyn R. and Mavrikakis, Manos and Dumesic, James A. and Winans, Randall E.},
abstractNote = {To control the size and structure of supported Pt catalysts, the influence of additional metal particles and the effect of supports were elucidated during the cracking reaction of n-dodecane under supercritical reaction conditions. The dynamical changes in nanocatalysts and catalytic activity are studied under realistic reaction conditions by using a combination of simultaneous temperature-programmed heating, in situ Small Angle X-ray Scattering (SAXS) and X-ray Absorption Near Edge Structure (XANES). In situ SAXS results indicate that the stability of the catalysts increases with Sn concentration. In situ XANES analysis reveals that the degree of oxidation and the electronic states of catalysts are dependent on the amount of Sn. Carbonaceous deposits over spent catalysts were characterized by Raman spectroscopy, suggesting that the highest Sn loading inhibits the formation of disordered graphitic lattices, which leads to an increased catalytic activity. SiO2, γ-Al2O3 and Mg(Al)Ox were employed as supports to investigate the support effect on the stability of Pt catalysts. In situ SAXS and XANES findings clearly reflect the improved stability of catalysts on γ-Al2O3 and Mg(Al)Ox supports compared to Pt catalysts on SiO2 and the electronic states of catalysts are strongly influenced by support materials.},
doi = {10.1039/C9CP00347A},
journal = {Physical Chemistry Chemical Physics. PCCP},
number = 22,
volume = 21,
place = {United States},
year = {Wed May 15 00:00:00 EDT 2019},
month = {Wed May 15 00:00:00 EDT 2019}
}
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