4.6 Article

Water-gas shift: Characterization and testing of nanoscale YSZ supported Pt catalysts

Journal

APPLIED CATALYSIS A-GENERAL
Volume 497, Issue -, Pages 184-197

Publisher

ELSEVIER SCIENCE BV
DOI: 10.1016/j.apcata.2014.12.055

Keywords

Water-gas-shift; Zirconia; Pt/ZrO2; Yttrium stabilized zirconia (YSZ); Pt/YSZ; Surface defects; Surface mobility

Funding

  1. Commonwealth of Kentucky
  2. Italian Ministry of Education, Universities and Research
  3. US DOE, Division of Materials Science and Chemical Science
  4. U.S. DOE, Office of Fossil Energy, NETL
  5. U.S. DOE, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]
  6. DOE
  7. MRCAT

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Nano-scale Y-doped zirconium oxide materials were prepared with high surface areas (150-200 m(2)/g) and small nano-crystallites (<8 nm). A combination of XANES and EXAFS was used to show that ZrO2 exhibited the tetragonal phase, while the Zr0.5Y0.5O1.75 support displayed the cubic phase. A comparison with undoped zirconia suggests that the Zr0.9Y0.1O1.95 support was tetragonal in structure. A slight increase in d-spacing observed in HR-TEM for the Zr0.9Y0.1O1.95 support relative to undoped ZrO2, along with a shift to lower 2 theta in XRD, provide evidence that Y-doping caused macrostrain. STEM imaging confirmed that the Pt clusters ranged from 0.5 to 2 nm over all three supports. Catalyst reducibility was explored by H-2-TPR, XANES at the Zr K-edge, and TPR-XANES at the Pt L-III edge. A higher concentration of surface defects for the 0.5%Pt/Zr0.9Y0.1O1.95 catalyst relative to 0.5%Pt/ZrO2 was confirmed by DRIFTS of adsorbed CO, while a greater surface mobility of surface formate was suggested based on forward formate decomposition experiments in steam. The Y-doped Pt promoted catalysts displayed higher water-gas-shift activity relative to the 0.5%Pt/ZrO2 catalyst when the Y content was at or below 50%, with the best catalyst being 0.5%Pt/Zr0.9Y0.1O1.95. (C) 2015 Elsevier B.V. All rights reserved.

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