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• W2014528360 abstract "The mechanisms of chain epimerization during propylene polymerization with methylaluminoxane-activated rac-(EBTHI)ZrCl(2) and rac-(EBI)ZrCl(2) catalysts (EBTHI = ethylenebis(eta(5)-tetrahydroindenyl); EBI = ethylenebis(eta(5)-indenyl)) have been studied using specifically isotopically labeled propylene: CH(2)=CD(13)CH(3). These isospecific catalysts provide predominantly the expected [mmmm] pentads with [minus signCH(2)CD(13)CH(3)(-)] repeating units ((13)C NMR). Under relatively low propylene concentrations at 50 and 75 degreesC, where stereoerrors attributable to chain epimerization are prevalent, (13)C NMR spectra reveal (13)C-labeled methylene groups along the polymer main chain, together with [CD(13)CH(3)] units in [mmmr], [mmrr], and [mrrm] pentads and [CH(13)CH(3)] units in [mmmmmm] and [mmmmmr] heptads, as well as [mrrm] pentads. The isotopomeric regiomisplacements and stereoerrors are consistent with a mechanism involving beta-D elimination, olefin rotation and enantiofacial interconversions, and insertion to a tertiary alkyl intermediate [Zr-C(CH(2)D)((13)CH(3))P] (P = polymer chain), followed by the reverse steps to yield two stereoisomers of [Zr-CHDCH((13)CH(3))P] and [Zr-(13)CH(2)CH(CH(2)D)P], as well as unrearranged [Zr-CH(2)CD((13)CH(3))P]. The absence of observable [-CH(2)CH(13)CH(2)D-] in the [mrrm] pentad region of the (13)C NMR spectra provides evidence that an allyl/dihydrogen complex does not mediate chain epimerization." @default.
• W2014528360 created "2016-06-24" @default.
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• W2014528360 date "2002-02-20" @default.
• W2014528360 modified "2023-10-14" @default.
• W2014528360 title "Chain Epimerization during Propylene Polymerization with Metallocene Catalysts: Mechanistic Studies Using a Doubly Labeled Propylene" @default.
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• W2014528360 doi "https://doi.org/10.1021/ja0123296" @default.
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