Thermoplastic poly(ester-ether) elastomers (TPEEs) have
been applied
extensively in automotive components, electrics, medical, and other
fields. However, TPEEs with high thermal resistance and shape recovery
rate are rarely reported, especially the ones derived from renewable
feedstocks. Herein, the renewable 2,5-furandicarboxylic acid (FDCA)
and 1,4-cyclohexanedimethanol were taken to construct the hard segment,
while poly(tetramethylene glycol) (PTMG) was employed as the soft
segment to synthesize poly(ester-ether) elastomers (PCF–PTMG).
Investigation showed that PCF–PTMG had excellent thermal resistance
with T
m up to 254 °C, which was higher
than most of the commercial TPEEs. By adjusting the content of the
PTMG segment from 30 to 80 wt %, the tensile strength of synthesized
TPEEs increased from 31 to 303 MPa and tensile modulus varied in the
range of 17 to 27 MPa. More importantly, PCF–PTMG70, containing
70 wt % of the PTMG segment, showed the elongation at break of 676%
and shape recovery rate as high as 77.4% during the first cyclic test
at 200% strain, which are higher than those of almost all the TPA-based
TPEEs. This work indicates that a bio-based FDCA unit has great potential
to serve as a highly crystallizable hard segment, as well as PTMG
content adjusted the contribution of the soft segments to synthesize
the new poly(ester-ether) elastomers with high thermal resistance.
A range of degradable polyesters have been developed as sustainable alternatives for commercial plastics; however, limitations of composting facilities and uncontrolled degradation in the environment hindered their viability. In this study, biobased itaconic acid was selected as an active site to control the degradation of polyesters. A series of PBXI copolyesters with M w 's ranging from 4.86 to 8.31 × 10 4 g/mol and high intrinsic viscosities of more than 1.15 dL/g were successfully synthesized without any crosslinking by selecting appropriate reaction conditions, including condensation temperature and vacuum, effective inhibitor, and catalyst. The obtained copolyesters were semicrystalline, and their T m 's could be regulated from 42.5 to 179.5 °C. They exhibited outstanding elastic modulus (120−598 MPa) and tensile strength (17.9−51.4 MPa) among degradable polymers. Degradation experiments demonstrated that the incorporation of itaconate segments could facilitate both the hydrolysis and enzymatic degradation of polyesters. The state-of-the-art computation and analysis via molecular dynamics (MD) simulations of PBXI−CALB complexes elucidated the enzymatic degradation mechanism. Experimental results proved that, at room temperature, the degradation could be stimulated and regulated by amines without a catalyst and the M n 's of lactamization products rapidly decreased to less than 5000 g/mol within 24 h. Moreover, the copolymerized structure of copolyesters and solvent factors could influence the aza-Michael addition between amines and itaconate units. This work provides a strategy to synthesize biodegradable copolymers with the potential to undergo controlled and rapid in vivo degradation with outstanding mechanical properties.
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