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

被引:17
|
作者
Martinelli, Michela [1 ,2 ]
Jacobs, Gary [1 ]
Graham, Uschi M. [1 ]
Shafer, Wilson D. [1 ]
Cronauer, Donald C. [3 ]
Kropf, A. Jeremy [3 ]
Marshall, Christopher L. [3 ]
Khalid, Syed [4 ]
Visconti, Carlo G. [2 ]
Lietti, Luca [2 ]
Davis, Burtron H. [1 ]
机构
[1] Univ Kentucky, Ctr Appl Energy Res, Lexington, KY 40511 USA
[2] Politecn Milan, Dipartimento Energia, I-20133 Milan, Italy
[3] Argonne Natl Lab, Argonne, IL 60439 USA
[4] Brookhaven Natl Lab, Natl Synchrotron Light Source, Upton, NY 11973 USA
关键词
Water-gas-shift; Zirconia; Pt/ZrO2; Yttrium stabilized zirconia (YSZ); Pt/YSZ; Surface defects; Surface mobility; X-RAY-ABSORPTION; FUEL-CELL APPLICATIONS; IN-SITU DRIFTS; LOW-TEMPERATURE; STABILIZED ZIRCONIA; REACTION-MECHANISM; PROCESSING CATALYSTS; COMPUTER-SIMULATION; PT/CERIA CATALYSTS; PLATINUM CATALYSTS;
D O I
10.1016/j.apcata.2014.12.055
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
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.
引用
收藏
页码:184 / 197
页数:14
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