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Title: Morphology and CO Oxidation Activity of Pd Nanoparticles on SrTiO 3 Nanopolyhedra

Abstract

Single crystal SrTiO 3 nanocuboids having primarily TiO 2-(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 TiO 2-(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, demonstrated 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 (~ 3 nm) have lower catalytic activity due to highmore » CO coverage on nanoparticle facets. Smaller nanoparticles (~ 2 nm) have more edge and corner sites and present 2-3 times higher TOF at 80 and 100 degrees C.« less

Authors:
 [1]; ORCiD logo [1];  [1]; ORCiD logo [1];  [1];  [2]; ORCiD logo [1];  [3]; ORCiD logo [3];  [1]; ORCiD logo [1]
  1. Northwestern Univ., Evanston, IL (United States)
  2. Argonne National Lab. (ANL), Lemont, IL (United States)
  3. Northwestern Univ., Evanston, IL (United States); Argonne National Lab. (ANL), Lemont, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1508635
Grant/Contract Number:  
[AC02-06CH11357]
Resource Type:
Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
[ Journal Volume: 8; Journal Issue: 6]; Journal ID: ISSN 2155-5435
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; CO oxidation; X-ray absorption near edge structure; X-ray small angle scattering; atomic layer deposition; diffuse reflectance infrared Fourier transform spectroscopy; heterogeneous catalysts; palladium; strontium titanate

Citation Formats

Chen, Bor-Rong, Crosby, Lawrence A., George, Cassandra, Kennedy, Robert M., Schweitzer, Neil M., Wen, Jianguo, Van Duyne, Richard P., Stair, Peter C., Poeppelmeier, Kenneth R., Marks, Laurence D., and Bedzyk, Michael J. Morphology and CO Oxidation Activity of Pd Nanoparticles on SrTiO 3 Nanopolyhedra. United States: N. p., 2018. Web. doi:10.1021/acscatal.7b04173.
Chen, Bor-Rong, Crosby, Lawrence A., George, Cassandra, Kennedy, Robert M., Schweitzer, Neil M., Wen, Jianguo, Van Duyne, Richard P., Stair, Peter C., Poeppelmeier, Kenneth R., Marks, Laurence D., & Bedzyk, Michael J. Morphology and CO Oxidation Activity of Pd Nanoparticles on SrTiO 3 Nanopolyhedra. United States. doi:10.1021/acscatal.7b04173.
Chen, Bor-Rong, Crosby, Lawrence A., George, Cassandra, Kennedy, Robert M., Schweitzer, Neil M., Wen, Jianguo, Van Duyne, Richard P., Stair, Peter C., Poeppelmeier, Kenneth R., Marks, Laurence D., and Bedzyk, Michael J. Mon . "Morphology and CO Oxidation Activity of Pd Nanoparticles on SrTiO 3 Nanopolyhedra". United States. doi:10.1021/acscatal.7b04173. https://www.osti.gov/servlets/purl/1508635.
@article{osti_1508635,
title = {Morphology and CO Oxidation Activity of Pd Nanoparticles on SrTiO 3 Nanopolyhedra},
author = {Chen, Bor-Rong and Crosby, Lawrence A. and George, Cassandra and Kennedy, Robert M. and Schweitzer, Neil M. and Wen, Jianguo and Van Duyne, Richard P. and Stair, Peter C. and Poeppelmeier, Kenneth R. and Marks, Laurence D. and Bedzyk, Michael J.},
abstractNote = {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, demonstrated 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 (~ 3 nm) have lower catalytic activity due to high CO coverage on nanoparticle facets. Smaller nanoparticles (~ 2 nm) have more edge and corner sites and present 2-3 times higher TOF at 80 and 100 degrees C.},
doi = {10.1021/acscatal.7b04173},
journal = {ACS Catalysis},
number = [6],
volume = [8],
place = {United States},
year = {2018},
month = {4}
}

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