Polymer Multi‐Block and Multi‐Block+ Strategies for the Upcycling of Mixed Polyolefins and Other Plastics

Due to a continued rise in the production and use of plastic products, their end‐of‐life pollution has become a pressing global issue. One of the biggest challenges in plastics recycling is the separation of different polymers. Multi‐block copolymers (MBCPs) represent an efficient strategy for the upcycling of mixed plastics via induced compatibilization, but this approach is limited by difficulties associated with synthesis and structural modification. In this contribution, several synthetic strategies are explored to prepare MBCPs with tunable microstructures, which were then used as compatibilizer additives to upcycle mixtures of polyolefins with other plastics. A multi‐block+ strategy based on a reactive telechelic block copolymer platform was introduced, which enabled block extension during the in situ melt blending of mixed plastics, leading to better compatibilizing properties as well as better 3D printing capability. This strategy was also applicable to more complex ternary plastic blends. The polymer multi‐block strategy enabled by versatile MBCPs synthesis and the multi‐block+ strategy enabled by in situ block extension show exciting opportunities for the upcycling of mixed plastics. A series of multi‐block copolymers with tunable microstructures were prepared and used as compatibilizer additives for upcycling mixtures of polyolefins with other plastics. Furthermore, a multi‐block+ strategy based on a reactive telechelic block copolymer platform was demonstrated to enable block extension during in situ melt blending of mixed plastics, leading to better compatibilizing properties and 3D printing capability.