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Precise cooperative sulfur placement leads to semi-crystallinity and selective depolymerisability in CS₂/oxetane copolymers

Title data

Fornacon-Wood, Christoph ; Manjunatha, Bhargav Rampura ; Stühler, Merlin R. ; Gallizioli, Cesare ; Müller, Carsten ; Pröhm, Patrick ; Plajer, Alex:
Precise cooperative sulfur placement leads to semi-crystallinity and selective depolymerisability in CS₂/oxetane copolymers.
In: Nature Communications. Vol. 14 (2023) . - 4525.
ISSN 2041-1723
DOI: https://doi.org/10.1038/s41467-023-39951-y

Abstract in another language

CS2 promises easy access to degradable sulfur-rich polymers and insights into how main-group derivatisation affects polymer formation and properties, though its ring-opening copolymerisation is plagued by low linkage selectivity and small-molecule by-products. We demonstrate that a cooperative Cr(III)/K catalyst selectively delivers poly(dithiocarbonates) from CS2 and oxetanes while state-of-the-art strategies produce linkage scrambled polymers and heterocyclic by-products. The formal introduction of sulfur centres into the parent polycarbonates results in a net shift of the polymerisation equilibrium towards, and therefore facilitating, depolymerisation. During copolymerisation however, the catalyst enables near quantitative generation of the metastable polymers in high sequence selectivity by limiting the lifetime of alkoxide intermediates. Furthermore, linkage selectivity is key to obtain semi-crystalline materials that can be moulded into self-standing objects as well as to enable chemoselective depolymerisation into cyclic dithiocarbonates which can themselves serve as monomers in ring-opening polymerisation. Our report demonstrates the potential of cooperative catalysis to produce previously inaccessible main-group rich materials with beneficial chemical and physical properties.

Further data

Item Type: Article in a journal
Refereed: Yes
Institutions of the University: Faculties
Faculties > Faculty of Biology, Chemistry and Earth Sciences
Faculties > Faculty of Biology, Chemistry and Earth Sciences > Department of Chemistry
Faculties > Faculty of Biology, Chemistry and Earth Sciences > Department of Chemistry > Chair Macromolecular Chemistry I
Faculties > Faculty of Biology, Chemistry and Earth Sciences > Department of Chemistry > Junior Professor Polymers for Electrooptical and Sensory Applications > Junior Professor Polymers for Electrooptical and Sensory Applications - Juniorprof. Dr. Alex Johannes Plajer
Faculties > Faculty of Biology, Chemistry and Earth Sciences > Department of Chemistry > Junior Professor Polymers for Electrooptical and Sensory Applications
Result of work at the UBT: No
DDC Subjects: 500 Science > 540 Chemistry
Date Deposited: 19 Mar 2024 10:51
Last Modified: 09 Jul 2024 10:37
URI: https://eref.uni-bayreuth.de/id/eprint/88941