|Title||Stabilizing unstable species through single-site isolation: A catalytically active Ta-V trialkyl in a porous organic polymer|
|Publication Type||Journal Article|
|Year of Publication||2013|
|Authors||Tanabe, KK, Siladke, NA, Broderick, EM, Kobayashi, T, Goldston, JF, Weston, MH, Farha, OK, Hupp, JT, Pruski, M, Mader, EA, Johnson, MJA, Nguyen, ST|
|Type of Article||Article|
|Keywords||aromatic framework, catalysis, complexes, gas, high-surface-area, hydrogen storage, inorganic, metathesis, networks, oxides, tantalum|
A catechol-functionalized porous organic polymer (POP) has been successfully metallated with a Ta-V trialkyl and remains thermally and structurally robust. The resulting POP-supported (catecholato)Ta-V 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)Ta-V trialkyl site and its products in reactions with Bronsted 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.
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