Mit der nächsten Generation von Zink‐Bisguanidin‐Polymerisationskatalysatoren zu hochkristallinen, biologisch abbaubaren Polyestern

Hermann, Alina; Hill, Stephen A.; Metz, Angela; Heck, Joshua; Hoffmann, Alexander; Hartmann, Laura; Herres‐Pawlis, Sonja

doi:10.1002/ange.202008473

Cited by 18 publications

(1 citation statement)

References 64 publications

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“…Recently, Herres‐Pawlis et al. presented a Zn guanidine catalyst, drastically outperforming the industry catalyst under such conditions [15] . However, the majority of these examples states biodegradation as the only end of life option for PLA.…”

Section: Introductionmentioning

confidence: 99%

Guanidine Carboxy Zinc Complexes for the Chemical Recycling of Renewable Polyesters

et al. 2022

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Our previously published non‐toxic guanidine carboxy Zn catalysts, suitable for lactide ring opening polymerisation (ROP) under industrially preferred melt conditions, have been tested towards the alcoholysis of renewable polyesters. A structure‐reactivity relationship has been found for the methanolysis of PLA in anhydrous THF, dependent on the substituents introduced at the ligand backbone. Using the unsubstituted “TMGasme” catalyst C2, a polyester conversion of 41 % was reached after 5 h at 60 °C. Introducing an electron density donating ‐NMe2 group at the ligand (C3) caused and increase in catalyst activity, resulting in a PLA conversion of 72 %. Hence, C3 was further tested, stressing the industrial applicability of PLA chemical recycling. Catalyst recycling, process scale up as well as solvent free alcoholysis, with full degradation in the PLA melt after 1 h, were demonstrated, allowing for the implementation of a circular (bio)plastics economy promoted by these catalysts.

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Section: Introductionmentioning

confidence: 99%

Guanidine Carboxy Zinc Complexes for the Chemical Recycling of Renewable Polyesters

et al. 2022

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Nachtaktiv: Eisen‐Guanidin‐Komplex katalysiert ROP auf der schlafenden Seite der ATRP

et al. 2021

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Copolymere sind die Antwort auf die limitierten Eigenschaften von Homopolymeren. Um die gesamte Vielfalt der verfügbaren Monomere nutzen zu können, werden derzeit Katalysatoren untersucht, die in mehr als einem Polymerisationsmechanismus aktiv sind. Eisen‐Guanidin‐Katalysatoren haben sich bei der ROP von Lactid als außerordentlich aktiv erwiesen und zeigen jetzt ihre Vielseitigkeit, indem sie auch die ATRP von Styrol katalysieren. Der vorgestellte Eisenkomplex ist der erste, der Lactid und Styrol gleichzeitig zu einem definierten Blockcopolymer in einem Reaktionsgefäß polymerisiert. Beide Mechanismen arbeiten dabei Hand in Hand, wobei die ROP die überwiegend vorhandene FeII‐Spezies auf der inaktiven Seite des ATRP‐Gleichgewichts nutzt. Diese orthogonale Copolymerisation durch einen nicht‐toxischen Eisenkatalysator ebnet neue Wege zu biokompatiblen Polymerisationsverfahren und erweitert den Anwendungsbereich der ATRP.

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O‐to‐S Substitution Enables Dovetailing Conflicting Cyclizability, Polymerizability, and Recyclability: Dithiolactone vs. Dilactone

Wang

Chen

et al. 2021

Angewandte Chemie

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Developing chemically recyclable polymers represents a greener alternative to landfill and incineration and offers a closed‐loop strategy toward a circular materials economy. However, the synthesis of chemically recyclable polymers is still plagued with certain fundamental limitations, including trade‐offs between the monomer's cyclizability and polymerizability, as well as between polymer's depolymerizability and properties. Here we describe the subtle O‐to‐S substitution, dithiolactone monomers derived from abundant feedstock α‐amino acids can demonstrate appealing chemical properties different from those of dilactone, including accelerated ring closure, augmented kinetics polymerizability, high depolymerizability and selectivity, and thus constitute a unique class of polythioester materials exhibiting controlled molecular weight (up to 100.5 kDa), atactic yet high crystallinity, structurally diversity, and chemical recyclability. These polythioesters well addresses the formidable challenges of developing chemically recyclable polymers by having an unusual set of desired properties, including easy‐to‐make monomer from ubiquitous feedstock, and high polymerizability, crystallinity and precise tunability of physicochemical performance, as well as high depolymerizability and selectivity. Computational studies explain why O‐to‐S modification of polymer backbone enables dovetailing desirable, but conflicting, performance into one polymer structure.

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Mit der nächsten Generation von Zink‐Bisguanidin‐Polymerisationskatalysatoren zu hochkristallinen, biologisch abbaubaren Polyestern

Cited by 18 publications

References 64 publications

Guanidine Carboxy Zinc Complexes for the Chemical Recycling of Renewable Polyesters

Guanidine Carboxy Zinc Complexes for the Chemical Recycling of Renewable Polyesters

Nachtaktiv: Eisen‐Guanidin‐Komplex katalysiert ROP auf der schlafenden Seite der ATRP

O‐to‐S Substitution Enables Dovetailing Conflicting Cyclizability, Polymerizability, and Recyclability: Dithiolactone vs. Dilactone

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