Research Unit of Sustainable Chemistry, University of Oulu, P.O. Box 4300, FI-90014 Oulu, Finland.
Fibre and Particle Engineering Research Unit, University of Oulu, P.O. Box 4300, FI-90014 Oulu, Finland.
Biomacromolecules. 2022 Apr 11;23(4):1803-1811. doi: 10.1021/acs.biomac.2c00097. Epub 2022 Mar 23.
With the goal of achieving high barrier with bio-based materials, for example, for packaging applications, a series of novel furfural-based polyesters bearing sulfide-bridged difuran dicarboxylic acid units with high oxygen barrier properties were synthesized and characterized. For the novel poly(alkylene sulfanediyldifuranoate)s, a 11.2-1.9× higher barrier improvement factor compared to amorphous poly(ethylene terephthalate) was observed which places the novel polyesters in the top class among previously reported 2,5-furandicarboxylic acid (FDCA) and 2,2'-bifuran-based polyesters. Titanium-catalyzed polycondensation reactions between the novel synthesized monomer, dimethyl 5,5'-sulfanediyldi(furan-2-carboxylate), and four different diols, ethylene glycol, 1,3-propanediol, 1,4-butanediol, and 1,5-pentanediol, afforded difuran polyesters with high intrinsic viscosities (0.76-0.90 dL/g). These polyesters had good thermal stability, decomposing at 342-363 and 328-570 °C under nitrogen and air, respectively, which allowed processing them into free-standing films via melt-pressing. In tensile testing of the film specimens, tensile moduli in the range of 0.4-2.6 GPa were recorded, with higher values observed for the polyesters with shorter diol units. Interestingly, besides the low oxygen permeability, the renewable sulfide-bridged furan monomer also endowed the polyesters with slight UV shielding effect, with cutoff wavelengths of ca. 350 nm, in contrast to FDCA-based polyesters, which lack significant UV light absorption at over 300 nm.
为了实现生物基材料的高阻隔性,例如在包装应用中,我们合成并表征了一系列具有高氧阻隔性能的新型呋喃基聚酯,其结构中含有硫桥键连接的二呋喃二甲酸单元。对于新型聚(亚烷基亚磺酰基二呋喃二甲酸酯),与无定形聚对苯二甲酸乙二醇酯相比,其阻隔性能提高了 11.2-1.9 倍,这使得新型聚酯在之前报道的 2,5-呋喃二甲酸(FDCA)和 2,2'-双呋喃基聚酯中处于顶级水平。通过新型合成单体二甲酯 5,5'-亚磺酰基二(呋喃-2-羧酸)与四种不同二醇(乙二醇、1,3-丙二醇、1,4-丁二醇和 1,5-戊二醇)之间的钛催化缩聚反应,得到了具有高特性粘度(0.76-0.90 dL/g)的二呋喃聚酯。这些聚酯具有良好的热稳定性,在氮气和空气中分别在 342-363°C 和 328-570°C 下分解,这允许它们通过熔融压制加工成独立的薄膜。在薄膜样品的拉伸测试中,记录到拉伸模量在 0.4-2.6 GPa 范围内,具有较短二醇单元的聚酯表现出更高的值。有趣的是,除了低氧气透过率外,可再生的硫桥键合呋喃单体还赋予了聚酯轻微的紫外线屏蔽效果,截止波长约为 350nm,与 FDCA 基聚酯形成对比,后者在 300nm 以上没有明显的紫外线吸收。