Stabilizing unstable species through single-site isolation

A catalytically active TaV trialkyl in a porous organic polymer

Kristine K. Tanabe, Nathan A. Siladke, Erin M. Broderick, Takeshi Kobayashi, Jennifer F. Goldston, Mitchell H. Weston, Omar K. Farha, Joseph T Hupp, Marek Pruski, Elizabeth A. Mader, Marc J A Johnson, Sonbinh T. Nguyen

Research output: Contribution to journalArticle

34 Citations (Scopus)

Abstract

A catechol-functionalized porous organic polymer (POP) has been successfully metallated with a TaV trialkyl and remains thermally and structurally robust. The resulting POP-supported (catecholato)TaV trialkyl sites remain accessible to small molecules and can undergo reactions to yield stable, monomeric complexes that are quite different from those observed with the homogeneous analogues. Using a combination of reactivity studies, high-resolution solid-state NMR spectroscopy, and X-ray absorption spectroscopy (XAS), we are able to precisely determine the functionality and coordination environment of the active (catecholato)TaV trialkyl site and its products in reactions with Brønsted acids. Additionally, the Ta-metallated POP was found to have enhanced catalytic activity in the hydrogenation of cyclohexene and toluene relative to a homogeneous analogue.

Original languageEnglish
Pages (from-to)2483-2489
Number of pages7
JournalChemical Science
Volume4
Issue number6
DOIs
Publication statusPublished - Jun 2013

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Organic polymers
X ray absorption spectroscopy
Toluene
Nuclear magnetic resonance spectroscopy
Hydrogenation
Catalyst activity
Molecules
Acids

ASJC Scopus subject areas

  • Chemistry(all)

Cite this

Tanabe, K. K., Siladke, N. A., Broderick, E. M., Kobayashi, T., Goldston, J. F., Weston, M. H., ... Nguyen, S. T. (2013). Stabilizing unstable species through single-site isolation: A catalytically active TaV trialkyl in a porous organic polymer. Chemical Science, 4(6), 2483-2489. https://doi.org/10.1039/c3sc22268c

Stabilizing unstable species through single-site isolation : A catalytically active TaV trialkyl in a porous organic polymer. / Tanabe, Kristine K.; Siladke, Nathan A.; Broderick, Erin M.; Kobayashi, Takeshi; Goldston, Jennifer F.; Weston, Mitchell H.; Farha, Omar K.; Hupp, Joseph T; Pruski, Marek; Mader, Elizabeth A.; Johnson, Marc J A; Nguyen, Sonbinh T.

In: Chemical Science, Vol. 4, No. 6, 06.2013, p. 2483-2489.

Research output: Contribution to journalArticle

Tanabe, KK, Siladke, NA, Broderick, EM, Kobayashi, T, Goldston, JF, Weston, MH, Farha, OK, Hupp, JT, Pruski, M, Mader, EA, Johnson, MJA & Nguyen, ST 2013, 'Stabilizing unstable species through single-site isolation: A catalytically active TaV trialkyl in a porous organic polymer', Chemical Science, vol. 4, no. 6, pp. 2483-2489. https://doi.org/10.1039/c3sc22268c
Tanabe, Kristine K. ; Siladke, Nathan A. ; Broderick, Erin M. ; Kobayashi, Takeshi ; Goldston, Jennifer F. ; Weston, Mitchell H. ; Farha, Omar K. ; Hupp, Joseph T ; Pruski, Marek ; Mader, Elizabeth A. ; Johnson, Marc J A ; Nguyen, Sonbinh T. / Stabilizing unstable species through single-site isolation : A catalytically active TaV trialkyl in a porous organic polymer. In: Chemical Science. 2013 ; Vol. 4, No. 6. pp. 2483-2489.
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