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

Research output: Contribution to journalArticle

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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

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X ray absorption
X ray analysis
Silicon Dioxide
X ray powder diffraction
Nuclear magnetic resonance spectroscopy
Fourier transform infrared spectroscopy
Thermogravimetric analysis
Pyrolysis
Metals
Silica
Single crystals
Spectroscopy
Transmission electron microscopy
Decomposition
Temperature
tert-butoxy
N,N,N',N'-tetramethylethylenediamine
1,5-cyclooctadiene

All Science Journal Classification (ASJC) codes

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

Cite this

Ruddy, D. A., Jarupatrakorn, J., Rioux, R. M., Miller, J. T., McMurdo, M. J., McBee, J. L., ... 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
Ruddy, Daniel A. ; Jarupatrakorn, Jonggol ; Rioux, Robert M. ; Miller, Jeffrey T. ; McMurdo, Meredith J. ; McBee, Jennifer L. ; Tupper, Karl A. ; Don Tilley, T. / Site-isolated Pt-SBA15 materials from tris(tert-butoxy)siloxy complexes of Pt(II) and Pt(IV). In: Chemistry of Materials. 2008 ; Vol. 20, No. 20. pp. 6517-6527.
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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.",
author = "Ruddy, {Daniel A.} and Jonggol Jarupatrakorn and Rioux, {Robert M.} and Miller, {Jeffrey T.} and McMurdo, {Meredith J.} and McBee, {Jennifer L.} and Tupper, {Karl A.} and {Don Tilley}, T.",
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Ruddy, DA, Jarupatrakorn, J, Rioux, RM, Miller, JT, McMurdo, MJ, McBee, JL, Tupper, KA & Don Tilley, T 2008, 'Site-isolated Pt-SBA15 materials from tris(tert-butoxy)siloxy complexes of Pt(II) and Pt(IV)', Chemistry of Materials, vol. 20, no. 20, pp. 6517-6527. https://doi.org/10.1021/cm801598k

Site-isolated Pt-SBA15 materials from tris(tert-butoxy)siloxy complexes of Pt(II) and Pt(IV). / Ruddy, Daniel A.; Jarupatrakorn, Jonggol; Rioux, Robert M.; Miller, Jeffrey T.; McMurdo, Meredith J.; McBee, Jennifer L.; Tupper, Karl A.; Don Tilley, T.

In: Chemistry of Materials, Vol. 20, No. 20, 28.10.2008, p. 6517-6527.

Research output: Contribution to journalArticle

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T1 - Site-isolated Pt-SBA15 materials from tris(tert-butoxy)siloxy complexes of Pt(II) and Pt(IV)

AU - Ruddy, Daniel A.

AU - Jarupatrakorn, Jonggol

AU - Rioux, Robert M.

AU - Miller, Jeffrey T.

AU - McMurdo, Meredith J.

AU - McBee, Jennifer L.

AU - Tupper, Karl A.

AU - Don Tilley, T.

PY - 2008/10/28

Y1 - 2008/10/28

N2 - 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.

AB - 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.

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