Department of Fibre and Polymer Technology, School of Engineering Sciences in Chemistry, Biotechnology and Health, KTH Royal Institute of Technology, Teknikringen, 56-58, 100-44, Stockholm, Sweden.
Angew Chem Int Ed Engl. 2021 Jul 5;60(28):15482-15489. doi: 10.1002/anie.202103143. Epub 2021 Jun 9.
The clever one-pot combination of two macromolecular concepts, ring-opening polymerization (ROP) and step-growth polymerization (SGP), is demonstrated to be a simple, yet powerful tool to design a library of sequence-controlled polymers with diverse and spatially regulated degradability functions. ROP and SGP occur sequentially at room temperature when the organocatalytic conditions are switched from basic to acidic, and each allows the encoding of specific degradable bonds. ROP controls the sequence length and position of the degradability functions, while SGP between the complementary vinyl ether and hydroxyl chain-ends enables the formation of acetal bonds and high-molar-mass copolymers. The result is the rational combination of cleavable bonds prone to either bulk or surface erosion within the same macromolecule. The strategy is versatile and offers higher chemical diversity and level of control over the primary structure than current aliphatic polyesters or polycarbonates, while being simple, effective, and atom-economical and having potential for scalability.
本文巧妙地结合了两种高分子概念，开环聚合（ROP）和逐步聚合（SGP），为设计具有多种空间调控降解功能的序列可控聚合物库提供了一种简单而强大的工具。当有机催化条件从碱性切换到酸性时，ROP 和 SGP 在室温下顺序发生，并且每种聚合都允许编码特定的可降解键。ROP 控制序列长度和降解功能的位置，而互补的乙烯基醚和羟基链末端之间的 SGP 则可以形成缩醛键和高分子量共聚物。其结果是在同一大分子内合理地组合了易于发生整体或表面侵蚀的可裂解键。该策略具有多功能性，在一级结构的控制上比现有脂肪族聚酯或聚碳酸酯具有更高的化学多样性和水平，同时简单、有效、原子经济性，并且具有可扩展性的潜力。
