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- W2113703192 abstract "Abstract Poly(3‐hydroxybutyrate) (PHB) is produced by numerous bacteria as carbon and energy reserve storage material. Whereas nature only produces PHB in its strictly isotactic ( R ) form, homogeneous catalysis, when starting from racemic ( rac ) β‐butyrolactone (BL) as monomer, can in fact produce a wide variety of tacticities. The variation of the metal center and the surrounding ligand structure enable activity as well as tacticity tuning. However, no homogeneous catalyst exists to date that is easy to modify, highly active, and able to produce PHB with high isotacticities from rac ‐β‐BL. Therefore, in this work, the reaction kinetics of various 2‐methoxyethylamino‐bis(phenolate) lanthanide (Ln=Sm, Tb, Y, Lu) catalysts are examined in detail. The order in monomer and catalyst are determined to elucidate the reaction mechanism and the results are correlated with DFT calculations of the catalytic cycle. Furthermore, the enthalpies and entropies of the rate‐determining steps are determined through temperature‐dependent in situ IR measurements. Experimental and computational results converge in one specific mechanism for the ring‐opening polymerization of BL and even allow us to rationalize the preference for syndiotactic PHB." @default.
- W2113703192 created "2016-06-24" @default.
- W2113703192 creator A5011632856 @default.
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- W2113703192 creator A5056881592 @default.
- W2113703192 creator A5064248499 @default.
- W2113703192 date "2015-08-11" @default.
- W2113703192 modified "2023-10-18" @default.
- W2113703192 title "Mechanistic Investigations of the Stereoselective Rare Earth Metal-Mediated Ring-Opening Polymerization of β-Butyrolactone" @default.
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- W2113703192 doi "https://doi.org/10.1002/chem.201501156" @default.
- W2113703192 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/26263891" @default.
- W2113703192 hasPublicationYear "2015" @default.
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