期刊
APPLIED CATALYSIS A-GENERAL
卷 497, 期 -, 页码 184-197出版社
ELSEVIER SCIENCE BV
DOI: 10.1016/j.apcata.2014.12.055
关键词
Water-gas-shift; Zirconia; Pt/ZrO2; Yttrium stabilized zirconia (YSZ); Pt/YSZ; Surface defects; Surface mobility
资金
- Commonwealth of Kentucky
- Italian Ministry of Education, Universities and Research
- US DOE, Division of Materials Science and Chemical Science
- U.S. DOE, Office of Fossil Energy, NETL
- U.S. DOE, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]
- DOE
- MRCAT
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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