Zhao Yucheng, Rettner Emma M, Battson Megan E, Hu Zhitao, Miscall Joel, Rorrer Nicholas A, Miyake Garret M
Department of Chemistry, Colorado State University, Fort Collins, CO 80523, USA.
School of Materials Science and Engineering, Colorado State University, Fort Collins, CO 80523, USA.
Angew Chem Int Ed Engl. 2025 Feb 10;64(7):e202415707. doi: 10.1002/anie.202415707. Epub 2024 Nov 5.
Developing plastics that fill the need of polyolefins yet are more easily recyclable is a critical need to address the plastic waste crisis. However, most efforts in this vein have focused on high-density polyethylene (PE), while many different types of PE exist. To create broadly sustainable PE with modular properties, we present the synthesis, characterization, and demonstration of materials applications for chemically recyclable PE-like multiblock polymers prepared from distinct hard and soft blocks using ruthenium-catalyzed dehydrogenative polymerization. By altering the branching pattern within the soft blocks, a series of PE-like multiblock polymers were synthesized with tunable glass transition temperatures (T) while maintaining consistent high melting temperatures (T). A clear U-shape trend between T and mechanical properties was found, showcasing their potential as sustainable materials with tailored properties spanning commercial linear low-density polyethylene (LLDPE) and low-density polyethylene (LDPE). These materials offer adjustable adhesive strength to metal and demonstrate chemical recyclability and selective depolymerization in mixed plastic streams, promoting circularity and separation.
开发出既能满足聚烯烃需求又更易于回收利用的塑料，是应对塑料垃圾危机的一项关键需求。然而，这方面的大多数努力都集中在高密度聚乙烯（PE）上，而PE存在许多不同类型。为了制备具有模块化特性的广泛可持续的PE，我们展示了通过钌催化脱氢聚合由不同的硬段和软段制备的化学可回收类PE多嵌段聚合物的合成、表征及材料应用演示。通过改变软段内的支化模式，合成了一系列具有可调玻璃化转变温度（Tg）且保持一致高熔点温度（Tm）的类PE多嵌段聚合物。发现Tg与机械性能之间呈现明显的U形趋势，展示了它们作为具有定制性能的可持续材料的潜力，其性能涵盖商业线性低密度聚乙烯（LLDPE）和低密度聚乙烯（LDPE）。这些材料对金属具有可调粘合强度，并在混合塑料流中表现出化学可回收性和选择性解聚，促进循环利用和分离。
