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Correlation of Enzymatic Depolymerization Rates with the Structure of Polyethylene-Like Long-Chain Aliphatic Polyesters.
Schwab, Simon T; Bühler, Leonie Y; Schleheck, David; Nelson, Taylor F; Mecking, Stefan.
Afiliación
  • Schwab ST; Chair of Chemical Materials Science, Department of Chemistry, University of Konstanz, Universitätsstraße 10, 78457 Konstanz, Germany.
  • Bühler LY; Chair of Chemical Materials Science, Department of Chemistry, University of Konstanz, Universitätsstraße 10, 78457 Konstanz, Germany.
  • Schleheck D; Microbial Ecology and Limnic Microbiology, Department of Biology, University of Konstanz, Universitätsstraße 10, 78457 Konstanz, Germany.
  • Nelson TF; Chair of Chemical Materials Science, Department of Chemistry, University of Konstanz, Universitätsstraße 10, 78457 Konstanz, Germany.
  • Mecking S; Chair of Chemical Materials Science, Department of Chemistry, University of Konstanz, Universitätsstraße 10, 78457 Konstanz, Germany.
ACS Macro Lett ; 13(10): 1245-1250, 2024 Oct 15.
Article en En | MEDLINE | ID: mdl-39259499
ABSTRACT
Long-chain aliphatic polyesters are emerging sustainable materials that exhibit polyethylene-like properties while being amenable to chemical recycling and biodegradation. However, varying polyester chemical structures results in markedly different degradation rates, which cannot be predicted from commonly correlated bulk polyester properties, such as polymer melting temperature. To elucidate these structure-degradability relationships, long-chain polyesters varying in their monomer composition and crystallinity were subjected to enzymatic hydrolysis, the rates of which were quantified via detection of formed monomers. Copolymers with poorly water-soluble, long-chain diol monomers (e.g., 1,18-octadecanediol) demonstrated strongly reduced depolymerization rates compared to copolymers with shorter chain length diol monomers. This was illustrated by, e.g., the 20× faster hydrolysis of PE-4,18, consisting of 1,4-butanediol and 1,18-octadecanedicarboxylic acid monomers, relative to PE-18,4. The insoluble long-chain diol monomer released upon hydrolysis was proposed to remain attached to the bulk polymer surface, decreasing the accessibility of the remaining ester bonds to enzymes for further hydrolysis. Tuning of polyester crystallinity via the introduction of branched monomers led to variable hydrolysis rates, which increased by an order of magnitude when crystallinity decreased from 72% to 45%. The results reported enables the informed design of polyester structures with balanced material properties and amenability to depolymerization.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: ACS Macro Lett Año: 2024 Tipo del documento: Article País de afiliación: Alemania Pais de publicación: Estados Unidos
Texto completo
Añadir a Mi BVS
Imprimir
XML
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: ACS Macro Lett Año: 2024 Tipo del documento: Article País de afiliación: Alemania Pais de publicación: Estados Unidos