Abstract
To systematically investigate the synthesis of poly(butylene succinate)-co-(dilinoleic succinate) (PBS-DLS) copolymers and to enrich the library of polyesters synthesized via a sustainable route, we conducted a two-step polycondensation using fully biobased monomers such as diethyl succinate (DS), 1,4-butanediol (1,4-BD) and dilinoleic diol (DLD) in diphenyl ether, using Candida Antarctica lipase B (CAL-B) as biocatalyst. A series of PBS-DLS copolyesters with a 90-10, 70-30 and 50-50 wt% of hard (PBS) to soft (DLS) segments ratio were compared to their counterparts, which were synthesized using heterogenous titanium dioxide/silicon dioxide (TiO2/SiO2) catalyst. Chemical structure and molecular characteristics of resulting copolymers were assessed using nuclear magnetic spectroscopy (1H- and 13C-NMR) and gel permeation chromatography (GPC), whereas thermal and thermomechanical properties as well as crystallization behavior were investigated by differential scanning microscopy (DSC), dynamic mechanical thermal analysis (DMTA), digital holographic microscopy (DHM) and X-ray diffraction (XRD). The obtained results showed that, depending on the type of catalyst, we can control parameters related to blockiness and crystallinity of copolymers. Materials synthesized using CAL-B catalysts possess more blocky segmental distribution and higher crystallinity in contrast to materials synthesized using heterogenous catalysts, as revealed by DSC, XRD and DHM measurements.
Highlights
Fully biobased poly(butylene succinate)-co-(dilinoleic succinate) (PBS-DLS) copolymers containing poly(butylene succinate) (PBS) as the hard segments and poly(dilinoleic succinate) (DLS) as the soft segments were successfully synthesized via two-step polycondensation in diphenyl ether using
We evidence that enzymatic synthesis is a valuable approach for the synthesis of biobased poly(butylene succinate)-co-(dilinoleic succinate) (PBS-DLS)
Poly(butylene succinate) (PBS)-DLS with a hard to soft segment ratio from 90-10 to 50-50 wt% was synthesized via two-step polycondensation in diphenyl ether using Candida antarctica lipase
Summary
Worldwide polymer production and consumption has relied on petroleum-based materials, whose processing exerts a negative impact on the environment and ecosystems, including CO2 emission, depletion of fossil resources and accumulation of waste Since these undesirable effects led to critical values at the end of the 20th century, the development of biodegradable materials and sustainable chemistry has become the main priority in academia and industry [1]. Biomass feedstocks seem to have enormous potential as an inexhaustible source of carbohydrates, whose processing into biobased monomers or polymers can bring more positive aspects, such as lower energy consumption and greenhouse gas emissions Among those biobased materials that may be taken under consideration, aliphatic polyesters exhibit several desirable properties, and they can be produced from plant-derived monomers, which is associated with a low environmental impact upon disposal.
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