Meier-Merziger Moritz, Imschweiler Jan, Hartmann Frank, Niebuur Bart-Jan, Kraus Tobias, Gallei Markus, Frey Holger
Johannes Gutenberg University, Mainz, Chemistry Department, Duesbergweg 10-14, 55128, Mainz, Germany.
Saarland University, Chair in Polymer Chemistry, Campus C4 2, 66123, Saarbrücken, Germany.
Angew Chem Int Ed Engl. 2023 Oct 16;62(42):e202310519. doi: 10.1002/anie.202310519. Epub 2023 Sep 11.
Current environmental challenges and the shrinking fossil-fuel feedstock are important criteria for the next generation of polymer materials. In this context, we present a fully bio-based material, which shows promise as a thermoplastic elastomer (TPE). Due to the use of β-farnesene and L-lactide as monomers, bio-based feedstocks, namely sugar cane and corn, can be used. A bifunctional initiator for the carbanionic polymerization was employed, to permit an efficient synthesis of ABA-type block structures. In addition, the "green" solvent MTBE (methyl tert-butyl ether) was used for the anionic polymerisation, enabling excellent solubility of the bifunctional anionic initiator. This afforded low dispersity (Đ=1.07 to 1.10) and telechelic polyfarnesene macroinitiators. These were employed for lactide polymerization to obtain H-shaped triblock copolymers. TEM and SAXS revealed clearly phase-separated morphologies, and tensile tests demonstrated elastic mechanical properties. The materials featured two glass transition temperatures, at - 66 °C and 51 °C as well as gyroid or cylindrical morphologies, resulting in soft elastic materials at room temperature.
当前的环境挑战和不断减少的化石燃料原料是下一代聚合物材料的重要标准。在此背景下，我们展示了一种全生物基材料，它有望成为一种热塑性弹性体（TPE）。由于使用了β-法尼烯和L-丙交酯作为单体，可使用生物基原料，即甘蔗和玉米。采用了用于阴离子聚合的双官能引发剂，以实现ABA型嵌段结构的高效合成。此外，“绿色”溶剂MTBE（甲基叔丁基醚）用于阴离子聚合，使双官能阴离子引发剂具有出色的溶解性。这得到了低分散度（Đ=1.07至1.10）的遥爪聚法尼烯大分子引发剂。这些被用于丙交酯聚合以获得H形三嵌段共聚物。TEM和SAXS清楚地揭示了相分离形态，拉伸试验证明了其弹性力学性能。这些材料具有两个玻璃化转变温度，分别为-66°C和51°C，以及螺旋状或圆柱状形态，从而在室温下形成柔软的弹性材料。
