19章。催化开环聚合过程中非共价相互作用的影响

Marta E. G. Mosquera, M. Palenzuela, María Fernández-Millán
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摘要

近年来,人们对开环聚合(ROP)过程中的非共价相互作用越来越感兴趣。虽然这些相互作用的存在已经在几个ROP机制中被提出,但非共价相互作用的作用已经被强调并用于催化剂设计的领域是所谓的氢键催化剂。酸性和碱性/亲核物质都可以通过氢键机制促进环单体的ROP,理论研究和实验证据均支持这一结论。在这些催化体系中,氢键供体(HBD)和氢键受体(HBA)的结合导致双功能催化体系,其中HBD通过氢键相互作用激活单体,HBA通过氢键相互作用激活起始/传播醇。在大多数情况下,聚合发生在温和的条件下,具有活性。实现了对聚合的很好的控制,并获得了分子量可预测的窄分散聚合物,尽管分子量低到中等。这种类型的催化剂在共聚过程中也很有效。除了氢键外,其他非共价相互作用几乎没有被探索过。这是一个令人兴奋的领域,只是在其起步阶段,探索其他非共价相互作用的影响和寻找更活跃的系统,同时保持良好的聚合控制仍然是开放的挑战。
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CHAPTER 19. Influence of Noncovalent Interactions in Catalytic Ring-opening Polymerization Processes
Interest in noncovalent interactions in ring-opening polymerization (ROP) processes has burgeoned in recent years. Although the presence of these interactions has been proposed in several ROP mechanisms, the field where the role of noncovalent interactions has been emphasized and used for the design of catalysts is the so-called H-bonding catalysts. Both acidic and basic/nucleophilic species can promote the ROP of cyclic monomers via an H-bonding mechanism, as supported by theoretical studies and experimental evidence. In these catalytic systems, the combination of an H-bonding donor (HBD) and an H-bonding acceptor (HBA) leads to a bifunctional catalytic system in which the HBD activates the monomer and the HBA the initiating/propagating alcohol by H-bonding interactions. In most cases, the polymerization takes place under mild conditions with a living character. Very good control of the polymerization is achieved and narrowly dispersed polymers of predictable molecular weights are obtained, although the molecular weights are low to moderate. This type of catalyst is also effective in copolymerization processes. Apart from H-bonding, other noncovalent interactions have hardly been explored for ROP. This is an exciting area that is only in its infancy, and the exploration of the influence of other noncovalent interactions and the search for more active systems while maintaining good polymerization control are still open challenges.
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