In situ, operando studies on the size and structure of supported Pt catalysts under supercritical conditions by simultaneous synchrotron-based X-ray techniques. Issue 22 (22nd May 2019)

• Record Type: Journal Article
• Authors: Lee, Sungwon; Lee, Sungsik; Gerceker, Duygu; Kumbhalkar, Mrunmayi D.; Wiaderek, Kamila M.; Ball, Madelyn R.; Mavrikakis, Manos; Dumesic, James A.; Winans, Randall E.
• Is Part Of: Physical chemistry chemical physics. Volume 21:Issue 22(2019)
• Page Start: 11740
• Page End: 11747
• Publication Date: 2019-05-22
• Subjects: Chemistry, Physical and theoretical -- Periodicals; 541.3
• DOI: 10.1039/c9cp00347a
• Languages: English
• ISSNs: 1463-9076

Abstract

Abstract : Investigation of the size and structure of supported Pt catalysts under supercritical conditions leads to a fundamentally new level of understanding of nanoscale materials under extreme conditions. 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, indicating that the highest Sn loading inhibits the formation of disordered graphitic lattices, which leads to an increased catalytic activity. SiO2, γ-Al2 O3 and Mg(Al)O x were employed as supports to investigate the support effect on the stability of Pt catalysts. In situ SAXS and XANES results clearly show the improved stability of catalysts on γ-Al2 O3 and Mg(Al)Ox supports compared to Pt catalysts on SiO2 and the electronic states of catalysts are strongly influenced by support materials.