Synthesis of Na-Stabilized Nonporous t-ZrO2 Supports and Pt/t-ZrO2 Catalysts and Application to Water-Gas-Shift Reaction

被引:66
作者
Xie, Hong [1 ]
Lu, Junling [2 ]
Shekhar, Mayank [3 ]
Elam, Jeffery W. [2 ]
Delgass, W. Nicholas [3 ]
Ribeiro, Fabio H. [3 ]
Weitz, Eric [1 ]
Poeppelmeier, Kenneth R. [1 ]
机构
[1] Northwestern Univ, Dept Chem, Ctr Catalysis & Surface Sci, Evanston, IL 60208 USA
[2] Argonne Natl Lab, Div Energy Syst, Argonne, IL 60439 USA
[3] Purdue Univ, Sch Chem Engn, W Lafayette, IN 47907 USA
来源
ACS CATALYSIS | 2013年 / 3卷 / 01期
关键词
tetragonal ZrO2; hydrothermal synthesis; Na; Pt/ZrO2; water-gas-shift reaction; ATOMIC LAYER DEPOSITION; HYDROTHERMAL CONDITIONS; TETRAGONAL PHASE; BUTANE ISOMERIZATION; ZIRCONIA POLYMORPHS; ZRO2; CRYSTALLIZATION; NANOPARTICLES; TEMPERATURE; METHANE;
D O I
10.1021/cs300596q
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
t-ZrO2, synthesized under hydrothermal treatment conditions at 150 degrees C for 20 h using NaOH as the mineralizer, was phase stable up to 600 degrees C in air. The t-ZrO2 calcined at 600 degrees C (denoted as Z600) were nonporous spherical nanocrystallites with an average size of similar to 12 nm and a surface area of similar to 55 m(2)/g, which exhibited hydrothermal stability in a wide range of pH environments from acidic to basic conditions at 200 degrees C for 20 h. Monodispersed platinum nanoparticles similar to 1.5 +/- 0.3 nm were obtained on the Z600 supported Pt/t-ZrO2 catalyst by the Pt atomic layer deposition (AID) method. Na ions were found to play a crucial role in the formation of the stable t-ZrO2 by incorporating into the internal crystal structure of ZrO2 during the hydrothermal synthesis. The rate of water-gas-shift (WGS) reaction per mole of surface Pt on the Pt/Z600 catalyst was about five times higher compared to the catalysts prepared on commercial nonporous ZrO2. The incorporation of Na into the t-ZrO2 structure had a synergistic effect: stabilizing ZrO2 in the tetragonal phase and promoting the WGS reaction.
引用
收藏
页码:61 / 73
页数:13
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