2022
DOI: 10.1039/d1cc05127j
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N-Oxides amplify catalyst reactivity and isoselectivity in the ring-opening polymerization of rac-β-butyrolactone

Abstract: N-oxides can amplify the performance of a lanthanum aminobisphenolate catalyst in the ring-opening polymerization (ROP) of rac-β-butyrolactone (rac-BBL) to unprecedented levels (TOF / Pm ; At RT: 1,900 h-1 /...

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Cited by 13 publications
(8 citation statements)
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“…Changing either the temperature or ionic radii of the initiators did not lead to any improvement, which is different from those observed in rac -lactide polymerization. , The polymerizations initiated by complexes 1 , 2 , 5 , and 6 gave polymers of narrower Đ (1.30–1.40), indicating that these lanthanide complexes have good control on mass distributions of polymers. These results are comparable with those reported initiated by lanthanide complexes . The M n values determined are larger than the theoretical ones ( M c ) suggesting that the average number of propagating chains per dinuclear complex may be between 1 and 2.…”
Section: Resultssupporting
confidence: 88%
“…Changing either the temperature or ionic radii of the initiators did not lead to any improvement, which is different from those observed in rac -lactide polymerization. , The polymerizations initiated by complexes 1 , 2 , 5 , and 6 gave polymers of narrower Đ (1.30–1.40), indicating that these lanthanide complexes have good control on mass distributions of polymers. These results are comparable with those reported initiated by lanthanide complexes . The M n values determined are larger than the theoretical ones ( M c ) suggesting that the average number of propagating chains per dinuclear complex may be between 1 and 2.…”
Section: Resultssupporting
confidence: 88%
“…The development of volcano plots provides a straightforward method to map catalyst structural attributes with their performance and can provide rational approaches for further catalyst design. The observation of volcano plots and Sabatier relationships have been limited in homogeneous catalysis, but the utility of such relationships in heterogeneous (electro)­catalysis suggests a rich opportunity for both experimental and in silico catalyst optimization. This should also include the optimization of catalysts capable of accessing different copolymer architectures, where the selection of catalysts with appropriate relative rates of monomer homopolymerization might generate block, gradient, or random copolymers .…”
Section: Discussionmentioning
confidence: 99%
“…In contrast to that, examples of discrete, isoselective initiators in the ROP of β-BL remain very scarce. Chromium salen catalysts yielding isotactic-enriched PHB with P m up to 0.67 were reported by our group in 2008. A heterogenous neodymium-based catalyst achieved high stereocontrol ( P m = 0.85) as well as lanthanum bis(phenolate) systems resembling those of Carpentier and co-workers in combination with neutral donor ligands ( P m up to 0.82). , Very interestingly, Luo and co-workers showed recently that rare-earth metal salan-type catalysts are capable of either producing syndiotactic- or isotactic-enriched PHB ( P r = 0.78, P m = 0.77) depending on the ligand substitution …”
Section: Introductionmentioning
confidence: 97%
“…34−36 A heterogenous neodymium-based catalyst achieved high stereocontrol (P m = 0.85) 37 as well as lanthanum bis(phenolate) systems resembling those of Carpentier and co-workers 22 in combination with neutral donor ligands (P m up to 0.82). 38,39 Very interestingly, Luo and co-workers showed recently that rareearth metal salan-type catalysts are capable of either producing syndiotactic-or isotactic-enriched PHB (P r = 0.78, P m = 0.77) depending on the ligand substitution. 40 It was in this context that we became interested in understanding the factors influencing activity as well as stereocontrol in catalyst design for ROP of β-BL.…”
Section: ■ Introductionmentioning
confidence: 99%