Morphology and CO Oxidation Activity of Pd Nanoparticles on SrTiO3 Nanopolyhedra

被引:42
作者
Chen, Bor-Rong [1 ]
Crosby, Lawrence A. [1 ]
George, Cassandra [2 ]
Kennedy, Robert M. [2 ]
Schweitzer, Neil M. [3 ]
Wen, Jianguo [4 ]
Van Duyne, Richard P. [2 ]
Stair, Peter C. [2 ,5 ]
Poeppelmeier, Kenneth R. [1 ,2 ,5 ]
Marks, Laurence D. [1 ]
Bedzyk, Michael J. [1 ,6 ]
机构
[1] Northwestern Univ, Dept Mat Sci & Engn, Evanston, IL 60208 USA
[2] Northwestern Univ, Dept Chem, Evanston, IL 60208 USA
[3] Northwestern Univ, Dept Chem & Biol Engn, Evanston, IL 60208 USA
[4] Argonne Natl Lab, Ctr Nanoscale Mat, Lemont, IL 60439 USA
[5] Argonne Natl Lab, Chem Sci Engn Div, Lemont, IL 60439 USA
[6] Northwestern Univ, Dept Phys & Astron, Evanston, IL 60208 USA
基金
美国国家科学基金会;
关键词
heterogeneous catalysts; palladium; CO oxidation; strontium titanate; atomic layer deposition; X-ray small angle scattering; X-ray absorption near edge structure; diffuse reflectance infrared Fourier transform spectroscopy; MULTIPLY-TWINNED PARTICLES; ATOMIC LAYER DEPOSITION; PLATINUM NANOPARTICLES; CATALYTIC-OXIDATION; SURFACE SCIENCE; HETEROGENEOUS CATALYSTS; ELEMENTARY STEPS; CARBON-MONOXIDE; THIN-FILMS; SHAPE;
D O I
10.1021/acscatal.7b04173
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
Single crystal SrTiO3 nanocuboids having primarily TiO2-(001) surfaces and nanododecahedra having primarily (110) surfaces were created by two separate hydrothermal synthesis processes. Pd nanoparticles grown on the two sets of STO nanopolyhedra by atomic layer deposition show different morphologies and CO oxidation performance. Transmission electron microscopy and small-angle X-ray scattering show that 2-3 nm Pd nanoparticles with 3-5 nm interparticle distances decorate the STO surfaces. When the number of ALD cycles increases, the growth of the Pd nanoparticles is more significant in size on TiO2-(001)-STO surfaces, while that on (110)-STO surfaces is more predominant in number. High resolution electron microscopy images show that single crystal and multiply twinned Pd nanoparticles coexist on both types of the STO nanopolyhedra and exhibit different degrees of adhesion. The CO oxidation reaction, which was employed to determine the dependence of catalytic activity, showed that the Pd catalytic performance was dominated by the coverage of CO, which is more directly related to Pd nanoparticle size than to shape. CO turnover frequency analysis and diffuse reflectance infrared Fourier transform spectroscopy show that regardless of the shape or degrees of wetting, larger Pd nanoparticles (similar to 3 nm) have lower catalytic activity due to high CO coverage on nanoparticle facets. Smaller nanoparticles (similar to 2 nm) have more edge and corner sites and exhibit 2-3 times higher TOF at 80 and 100 degrees C.
引用
收藏
页码:4751 / 4760
页数:19
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