4.8 Article

Effect of organic capping layers over monodisperse platinum nanoparticles upon activity for ethylene hydrogenation and carbon monoxide oxidation

Journal

JOURNAL OF CATALYSIS
Volume 265, Issue 2, Pages 209-215

Publisher

ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2009.05.001

Keywords

Nanoparticle; Capping agent; Ethylene hydrogenation; CO oxidation; Platinum

Funding

  1. Director, Office of Science
  2. Office of Basic Energy Sciences
  3. Division of Chemical Sciences
  4. Geological and Biosciences and Division of Materials Sciences and Engineering
  5. US Department of Energy [DE-AC02-05CH11231]
  6. Chevron's Richmond Technological Center

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The influence of oleylamine (OA), trimethyl tetradecyl ammonium bromide (TTAB), and polyvinlypyrrolidone (PVP) capping agents upon the catalytic properties of Pt/silica catalysts was evaluated. Pt nanoparticles that were 1.5 nm in size were synthesized by the same procedure (ethylene glycol reduction under basic conditions) with the various capping agents added afterward for stabilization. Before examining catalytic properties for ethylene hydrogenation and CO oxidation, the Pt NPs were deposited onto mesoporous silica (SBA-15) supports and characterized by transmission electron microscopy (TEM), H-2 chemisorption, and elemental analysis (ICP-MS). PVP- and TTAB-capped Pt yielded mass-normalized reaction rates that decreased with increasing pretreatment temperature, and this trend was attributed to the partial coverage of the Pt surface with decomposition products from the organic capping agent. Once normalized to the Pt surface area, similar intrinsic activities were obtained regardless of the pretreatment temperature, which indicated no influence on the nature of the active sites. Consequently, a chemical probe technique using intrinsic activity for ethylene hydrogenation was demonstrated as an acceptable method for estimating the metallic surface areas of Pt. Amine (OA) capping exhibited a detrimental influence on the catalytic properties as severe deactivation and low activity were observed for ethylene hydrogenation and CO oxidation, respectively. These results were consistent with amine groups being strong poisons for Pt surfaces, and revealed the need to consider the effects of capping agents on the catalytic properties. Published by Elsevier Inc.

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