Sustainable Thermoplastic Elastomers from Commercial Cyclic Esters: One-Pot Synthesis of Poly(l‑lactide)‑b‑(δ-hexalactone-stat-ε-caprolactone)‑b‑(l‑lactide) and Its Chemical Recycling to the Monomers
Giuseppe Gravina, Joseph N. A. Tagoe, Rocco Di Girolamo, Maria Gentile, Luciano Di Maio, Claudio Pellecchia
TL;DR
Scientists created a new type of recyclable thermoplastic elastomer using a one-pot synthesis method and achieved high monomer recovery through chemical recycling.
Contribution
A one-pot synthesis method for ABA triblock copolymers with precise control and full chemical recyclability under mild conditions.
Findings
ABA triblock copolymers were synthesized using an Fe(II)-based catalyst in a single reactor.
The material properties ranged from soft elastomers to toughened PLA depending on block composition.
Chemical recycling recovered >90% of the original monomers under mild thermal conditions.
Abstract
We report the one-pot synthesis of ABA triblock copolymers composed of poly(l-lactide) (PLA) as hard segments and δ-hexalactone/ε-caprolactone (HL/CL) copolymers as soft midblock. Use of an environmentally benign and highly active and living Fe(II)-based catalyst enabled precise molecular design and control over copolymer architecture, providing low-T g, amorphous statistical HL/CL dihydroxy-terminated copolymers, which could be chain extended with l-lactide in the same reactor, resulting in poly(l-lactide)-b-(δ-hexalactone-stat-ε-caprolactone)-b-(l-lactide) triblock copolymers. The one-pot synthetic route enabled control of block composition and length, resulting in material property profiles ranging from silicone-like soft elastomers to SBS-like rubbers, and to toughened PLA. Finally, efficient chemical recycling to the pristine monomers with >90% recovery was achieved by catalytic…
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Taxonomy
Topicsbiodegradable polymer synthesis and properties · Polymer Nanocomposites and Properties · Carbon dioxide utilization in catalysis