Site-isolated Pt-SBA15 materials from tris(tert-butoxy)siloxy complexes of Pt(II) and Pt(IV)

Daniel A. Ruddy, Jonggol Jarupatrakorn, Robert M. Rioux, Jeffrey T. Miller, Meredith J. McMurdo, Jennifer L. McBee, Karl A. Tupper, T. Don Tilley

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Abstract

Two novel tris(tert-butoxy)siloxy complexes of Pt(II) and Pt(IV) were prepared in high yields, (cod)Pt[OSi(OtBu)3]2 (1; 87%; cod = 1,5-cyclooctadiene) and Me3Pt(tmeda)[OSi(O tBu)3] (2; 81%; tmeda = N,N,N′,N′- tetramethylethylenediamine). The structures of these compounds were determined by multinuclear NMR spectroscopy and by single-crystal X-ray analysis. The thermolytic chemistry of 1 and 2 in the solid state was studied by thermogravimetric analysis. The thermal decomposition of these complexes resulted in the formation of Pt metal, with the elimination of HOSi(O tBu)3. Precursors 1 and 2 react with the surface Si-OH groups of mesoporous SBA15 silica to generate surface-supported Pt centers. The coordination environments of the supported Pt centers in these new materials, termed Pt(II)SBA15 and Pt(IV)SBA15, were investigated using Fourier-transform infrared spectroscopy, X-ray absorption near-edge spectroscopy, and extended X-ray absorption fine structure analysis. These materials were also characterized using N2 porosimetry, powder X-ray diffraction and transmission electron microscopy. Comparisons with the molecular precursors 1 and 2 revealed many similarities, and the results are indicative of isolated Pt(II) and Pt(IV) centers. In addition, isolated Pt centers proved to be robust in inert atmosphere to 150-200 °C, which is similar to the decomposition temperatures of 1 and 2.

Original languageEnglish (US)
Pages (from-to)6517-6527
Number of pages11
JournalChemistry of Materials
Volume20
Issue number20
DOIs
StatePublished - Oct 28 2008

All Science Journal Classification (ASJC) codes

  • Chemistry(all)
  • Chemical Engineering(all)
  • Materials Chemistry

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    Ruddy, D. A., Jarupatrakorn, J., Rioux, R. M., Miller, J. T., McMurdo, M. J., McBee, J. L., Tupper, K. A., & Don Tilley, T. (2008). Site-isolated Pt-SBA15 materials from tris(tert-butoxy)siloxy complexes of Pt(II) and Pt(IV). Chemistry of Materials, 20(20), 6517-6527. https://doi.org/10.1021/cm801598k