POS9-0590
Fiber-Grade Polyurethane Elastomers with Green-Solvent Reprocessability and Mechanical Robustness through Dynamic Covalent Topology Engineering
Topic
S9. Polymer Technology for Sustainability
When and Where
Sep 30, 2026
08:30 - 09:30
Room 301 (Grand Ballroom)
Session Chairs
Heesuk KIM
Jinhye BAE
Presenter(s)
MinJeong Kim (BK21 FOUR Department of Materials Science and Engineering, Korea University, Seoul, 02841, Republic of Korea)
Co-Author(s)
Abstract
Achieving processability in low-boiling green-solvents without sacrificing mechanical robustness remains a major challenge in fiber-grade polyurethane elastomers. Conventional elastomeric fibers rely on cohesive hard segments and permanent crosslinks for durability and elastic recovery, yet these features limit solvent accessibility and recyclability. Although dynamic covalent networks offer a promising route toward reprocessable elastomers, enhanced network mobility often compromises mechanical performance.
Herein, dynamic polyurethane elastomers were developed through dynamic covalent topology engineering using reversible disulfide exchange chemistry. Bis(4-hydroxyphenyl) disulfide was incorporated as a dynamic chain extender, while aromatic 4,4′-methylenebis(phenyl isocyanate), cycloaliphatic isophorone diisocyanate, and controlled branching structures were combined to regulate network topology, segmental packing, and chain mobility.
Systematic variation of network topology revealed the molecular determinants governing the trade-off between solvent accessibility and mechanical robustness. An optimized hybrid network achieved complete dissolution in tetrahydrofuran and diethyl carbonate below 70 °C while maintaining a tensile strength of 37.3 MPa and an elongation at break exceeding 620%. Furthermore, the elastomer was successfully wet-spun into continuous fibers, producing monofilaments with a tenacity of 0.53 g d-1.
These findings reveal that solvent accessibility in crosslinked polyurethane networks can emerge from topology-controlled molecular rearrangement rather than simple network dilution. By coupling dynamic covalent exchange with controlled hard-segment packing, the optimized elastomer achieves green-solvent processability without sacrificing fiber-grade mechanical performance. This work establishes a practical molecular design framework for recyclable spandex and sustainable fiber manufacturing through dynamic covalent topology engineering.
Herein, dynamic polyurethane elastomers were developed through dynamic covalent topology engineering using reversible disulfide exchange chemistry. Bis(4-hydroxyphenyl) disulfide was incorporated as a dynamic chain extender, while aromatic 4,4′-methylenebis(phenyl isocyanate), cycloaliphatic isophorone diisocyanate, and controlled branching structures were combined to regulate network topology, segmental packing, and chain mobility.
Systematic variation of network topology revealed the molecular determinants governing the trade-off between solvent accessibility and mechanical robustness. An optimized hybrid network achieved complete dissolution in tetrahydrofuran and diethyl carbonate below 70 °C while maintaining a tensile strength of 37.3 MPa and an elongation at break exceeding 620%. Furthermore, the elastomer was successfully wet-spun into continuous fibers, producing monofilaments with a tenacity of 0.53 g d-1.
These findings reveal that solvent accessibility in crosslinked polyurethane networks can emerge from topology-controlled molecular rearrangement rather than simple network dilution. By coupling dynamic covalent exchange with controlled hard-segment packing, the optimized elastomer achieves green-solvent processability without sacrificing fiber-grade mechanical performance. This work establishes a practical molecular design framework for recyclable spandex and sustainable fiber manufacturing through dynamic covalent topology engineering.
