Partially Biobased Block Copolymers Derived from Phenol and Butanol for High-Performance Elastomers and Pressure-Sensitive Adhesives

Upcycling renewable resources into value-added products has shown substantial promise for producing sustainable polymers and reducing environmental pollution. To achieve this, careful and cost-effective selections of monomers derived from bioresources are critical. We herein report ABA-type triblock copolymers that partly contain phenyl acrylate and n-butyl acrylate, which could be derived from natural resources, such as lignin (for phenol) and microorganisms (for n-butanol). A hard block ("A" block) is first formed using phenyl acrylate and styrene with a bifunctional reversible addition–fragmentation chain-transfer agent, followed by the incorporation of n-butyl acrylate to form a soft block ("B" block) in the middle. The biomass contents are calculated to range from 32 to 53%. By simply altering the feeding ratios of these monomers, we have developed materials that exhibit excellent properties, ranging from elastomers to pressure-sensitive adhesives (PSAs). For example, one of the synthesized polymers indicates a Young's modulus of 106 MPa and a toughness of 15 MJ/m3, outperforming those obtained from commercial petrochemical-based elastomers. Additionally, some of the copolymers exhibited PSA properties that surpass those of commercial packaging tapes and glue sticks on a certain substrate. The Dahlquist criteria and viscoelastic window indicate great promise for these biobased polymers as PSAs.