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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

Journal Article · · Physical Chemistry Chemical Physics. PCCP
DOI:https://doi.org/10.1039/C9CP00347A· OSTI ID:1559532

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.

Research Organization:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC); Air Force Research Laboratory (AFRL); US Air Force Office of Scientific Research (AFOSR)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1559532
Journal Information:
Physical Chemistry Chemical Physics. PCCP, Vol. 21, Issue 22; ISSN 1463-9076
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 6 works
Citation information provided by
Web of Science

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