Polyethylene-Like Blends Amenable to Abiotic Hydrolytic Degradation

Lade...
Vorschaubild
Dateien
Eck_2-1s91soc9chsy05.pdf
Eck_2-1s91soc9chsy05.pdfGröße: 5.13 MBDownloads: 9
Datum
2023
Herausgeber:innen
Kontakt
ISSN der Zeitschrift
Electronic ISSN
ISBN
Bibliografische Daten
Verlag
Schriftenreihe
Auflagebezeichnung
ArXiv-ID
Internationale Patentnummer
Link zur Lizenz
Angaben zur Forschungsförderung
Projekt
Open Access-Veröffentlichung
Open Access Hybrid
Sammlungen
Core Facility der Universität Konstanz
Gesperrt bis
Titel in einer weiteren Sprache
Forschungsvorhaben
Organisationseinheiten
Zeitschriftenheft
Publikationstyp
Zeitschriftenartikel
Publikationsstatus
Published
Erschienen in
Zusammenfassung

Long-chain aliphatic polyester-18,18 (PE-18,18) exhibits high density polyethylene-like material properties and, as opposed to high density polyethylene (HDPE), can be recycled in a closed loop via depolymerization to monomers under mild conditions. Despite the in-chain ester groups, its high crystallinity and hydrophobicity render PE-18,18 stable toward hydrolysis even under acidic conditions for one year. Hydrolytic degradability, however, can be a desirable material property as it can serve as a universal backstop to plastic accumulation in the environment. We present an approach to render PE-18,18 hydrolytically degradable by melt blending with long-chain aliphatic poly(H-phosphonate)s (PP). The blends can be processed via common injection molding and 3D printing and exhibit HDPE-like tensile properties, namely, high stiffness (E = 750–940 MPa) and ductility (εtb = 330–460%) over a wide range of blend ratios (0.5–20 wt % PP content). Likewise, the orthorhombic solid-state structure and crystallinity (χ ≈ 70%) of the blends are similar to HDPE. Under aqueous conditions in phosphate-buffered media at 25 °C, the blends’ PP component is hydrolyzed completely to the underlying long-chain diol and phosphorous acid within four months, as evidenced by NMR analyses. Concomitant, the PE-18,18 major blend component is partially hydrolyzed, while neat PE-18,18 is inert under identical conditions. The hydrolysis of the blend components proceeded throughout the bulk of the specimens as confirmed by gel permeation chromatography (GPC) measurements. The significant molar mass reduction upon extended immersion in water (Mn(virgin blends) ≈ 50–70 kg mol–1; Mn(hydrolyzed blends) ≈ 7–11 kg mol–1) resulted in embrittlement and fragmentation of the injection molded specimens. This increases the surface area and is anticipated to promote eventual mineralization by abiotic and biotic pathways of these HDPE-like polyesters in the environment.

Zusammenfassung in einer weiteren Sprache
Fachgebiet (DDC)
540 Chemie
Schlagwörter
Polyethylene-like, degradable, biobased, long-chain polyester, polymer blend, 3D printing
Konferenz
Rezension
undefined / . - undefined, undefined
Zitieren
ISO 690ECK, Marcel, Lea BERNABEU, Stefan MECKING, 2023. Polyethylene-Like Blends Amenable to Abiotic Hydrolytic Degradation. In: ACS Sustainable Chemistry & Engineering. ACS Publications. 2023, 11(12), pp. 4523-4530. eISSN 2168-0485. Available under: doi: 10.1021/acssuschemeng.2c07537
BibTex
@article{Eck2023Polye-66437,
  year={2023},
  doi={10.1021/acssuschemeng.2c07537},
  title={Polyethylene-Like Blends Amenable to Abiotic Hydrolytic Degradation},
  number={12},
  volume={11},
  journal={ACS Sustainable Chemistry & Engineering},
  pages={4523--4530},
  author={Eck, Marcel and Bernabeu, Lea and Mecking, Stefan}
}
RDF
<rdf:RDF
    xmlns:dcterms="http://purl.org/dc/terms/"
    xmlns:dc="http://purl.org/dc/elements/1.1/"
    xmlns:rdf="http://www.w3.org/1999/02/22-rdf-syntax-ns#"
    xmlns:bibo="http://purl.org/ontology/bibo/"
    xmlns:dspace="http://digital-repositories.org/ontologies/dspace/0.1.0#"
    xmlns:foaf="http://xmlns.com/foaf/0.1/"
    xmlns:void="http://rdfs.org/ns/void#"
    xmlns:xsd="http://www.w3.org/2001/XMLSchema#" > 
  <rdf:Description rdf:about="https://kops.uni-konstanz.de/server/rdf/resource/123456789/66437">
    <void:sparqlEndpoint rdf:resource="http://localhost/fuseki/dspace/sparql"/>
    <dc:contributor>Mecking, Stefan</dc:contributor>
    <dc:language>eng</dc:language>
    <foaf:homepage rdf:resource="http://localhost:8080/"/>
    <dc:contributor>Bernabeu, Lea</dc:contributor>
    <dcterms:hasPart rdf:resource="https://kops.uni-konstanz.de/bitstream/123456789/66437/1/Eck_2-1s91soc9chsy05.pdf"/>
    <dc:rights>Attribution 4.0 International</dc:rights>
    <dcterms:available rdf:datatype="http://www.w3.org/2001/XMLSchema#dateTime">2023-03-17T09:55:00Z</dcterms:available>
    <dc:contributor>Eck, Marcel</dc:contributor>
    <dc:creator>Eck, Marcel</dc:creator>
    <bibo:uri rdf:resource="https://kops.uni-konstanz.de/handle/123456789/66437"/>
    <dcterms:abstract>Long-chain aliphatic polyester-18,18 (PE-18,18) exhibits high density polyethylene-like material properties and, as opposed to high density polyethylene (HDPE), can be recycled in a closed loop via depolymerization to monomers under mild conditions. Despite the in-chain ester groups, its high crystallinity and hydrophobicity render PE-18,18 stable toward hydrolysis even under acidic conditions for one year. Hydrolytic degradability, however, can be a desirable material property as it can serve as a universal backstop to plastic accumulation in the environment. We present an approach to render PE-18,18 hydrolytically degradable by melt blending with long-chain aliphatic poly(H-phosphonate)s (PP). The blends can be processed via common injection molding and 3D printing and exhibit HDPE-like tensile properties, namely, high stiffness (E = 750–940 MPa) and ductility (ε&lt;sub&gt;tb&lt;/sub&gt; = 330–460%) over a wide range of blend ratios (0.5–20 wt % PP content). Likewise, the orthorhombic solid-state structure and crystallinity (χ ≈ 70%) of the blends are similar to HDPE. Under aqueous conditions in phosphate-buffered media at 25 °C, the blends’ PP component is hydrolyzed completely to the underlying long-chain diol and phosphorous acid within four months, as evidenced by NMR analyses. Concomitant, the PE-18,18 major blend component is partially hydrolyzed, while neat PE-18,18 is inert under identical conditions. The hydrolysis of the blend components proceeded throughout the bulk of the specimens as confirmed by gel permeation chromatography (GPC) measurements. The significant molar mass reduction upon extended immersion in water (M&lt;sub&gt;n&lt;/sub&gt;(virgin blends) ≈ 50–70 kg mol&lt;sup&gt;–1&lt;/sup&gt;; M&lt;sub&gt;n&lt;/sub&gt;(hydrolyzed blends) ≈ 7–11 kg mol&lt;sup&gt;–1&lt;/sup&gt;) resulted in embrittlement and fragmentation of the injection molded specimens. This increases the surface area and is anticipated to promote eventual mineralization by abiotic and biotic pathways of these HDPE-like polyesters in the environment.</dcterms:abstract>
    <dspace:hasBitstream rdf:resource="https://kops.uni-konstanz.de/bitstream/123456789/66437/1/Eck_2-1s91soc9chsy05.pdf"/>
    <dcterms:isPartOf rdf:resource="https://kops.uni-konstanz.de/server/rdf/resource/123456789/29"/>
    <dc:creator>Bernabeu, Lea</dc:creator>
    <dcterms:title>Polyethylene-Like Blends Amenable to Abiotic Hydrolytic Degradation</dcterms:title>
    <dc:date rdf:datatype="http://www.w3.org/2001/XMLSchema#dateTime">2023-03-17T09:55:00Z</dc:date>
    <dcterms:rights rdf:resource="http://creativecommons.org/licenses/by/4.0/"/>
    <dcterms:issued>2023</dcterms:issued>
    <dspace:isPartOfCollection rdf:resource="https://kops.uni-konstanz.de/server/rdf/resource/123456789/29"/>
    <dc:creator>Mecking, Stefan</dc:creator>
  </rdf:Description>
</rdf:RDF>
Interner Vermerk
xmlui.Submission.submit.DescribeStep.inputForms.label.kops_note_fromSubmitter
Kontakt
URL der Originalveröffentl.
Prüfdatum der URL
Prüfungsdatum der Dissertation
Finanzierungsart
Kommentar zur Publikation
Allianzlizenz
Corresponding Authors der Uni Konstanz vorhanden
Internationale Co-Autor:innen
Universitätsbibliographie
Ja
Begutachtet
Ja
Diese Publikation teilen