Direct synthesis of low-Coordinate pd catalysts supported on SiO2 via surface organometallic chemistry

Shengsi Liu, J. Miles Tan, Ahmet Gulec, Neil M. Schweitzer, Massimiliano Delferro, Laurence D. Marks, Peter C. Stair, Tobin J. Marks

Research output: Contribution to journalArticlepeer-review

8 Citations (Scopus)

Abstract

Highly dispersed low-coordinate Pd sites on SiO2 are fabricated by grafting the PdII PCP-pincer complex (tBuPCP)Pd−OH (tBuPCP = 2,6-C6H3(CH2PtBu2)2) on SiO2, followed by calcination with ozone (100 °C) and reduction with H2 (300 °C). The chemisorption process and structure of this organometallic complex on SiO2 is established by solution-phase1H and31P NMR and solid-state31P CPMAS NMR spectroscopy, XPS, DRIFTS, and AC-HAADF-STEM. The CO adsorption properties of the Pd centers reveal a surprisingly high fraction of adsorption sites where CO is bound in a linear fashion, indicative of low-coordinate Pd. Furthermore, enhanced selectivity of these catalyst centers in aerobic alcohol oxidation versus a control catalyst argues that these low-coordinate sites are the catalytically active sites.

Original languageEnglish
JournalACS Catalysis
Volume6
Issue number12
DOIs
Publication statusPublished - Dec 2 2016

Keywords

  • Benzyl alcohol oxidation
  • DRIFTS
  • Heterogeneous catalysis
  • Palladium nanoparticles
  • Solution-phase grafting
  • Surface organometallic chemistry

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)

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