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Title: 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. SiO 2, γ-Al 2O 3 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-Al 2O 3 and Mg(Al)Ox supports compared to Pt catalysts on SiO 2 and the electronic states of catalysts are strongly influenced by support materials.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2];  [2];  [1]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [1]
  1. Argonne National Lab. (ANL), Lemont, IL (United States)
  2. 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 (Print)
Additional Journal Information:
Journal Name: Physical Chemistry Chemical Physics. PCCP (Print); 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. doi: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. doi:10.1039/C9CP00347A.
@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 (Print)},
number = 22,
volume = 21,
place = {United States},
year = {2019},
month = {5}
}

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