Simple Zn(ii) complexes for the production and degradation of polyesters.
Simple Zn(ii) complexes for the production and degradation of polyesters.
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DOI：
10.1039/d1ra09087a
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发表时间：
2022-01-05
期刊：
影响因子：
3.9
通讯作者：
Jones MD
中科院分区：
文献类型：
--
作者：
Stewart J;Fuchs M;Payne J;Driscoll O;Kociok-Köhn G;Ward BD;Herres-Pawlis S;Jones MD
已制备出九种基于硫醚附加亚氨基酚盐 (ONS) 配体的新型配合物，并通过 NMR 光谱在溶液中进行了充分表征。还获得了七种配合物的固态结构。在溶液中，所有配合物都是单体的。该配合物对于纯化的外消旋丙交酯的聚合具有高度活性（[M] : [Zn] : [BnOH] = 10 000 : 1 : 30，180°C），TOF值高达250 000 h−1。通过原位拉曼光谱探讨了聚合动力学。使用工业级消旋丙交酯并增加引发剂负载，反应速率显着降低。为了实现循环经济，开发催化剂以促进商品和新兴聚合物材料的化学回收至关重要。在这方面，已经评估了复合物分解聚乳酸和聚对苯二甲酸乙二醇酯的能力。聚合反应和降解反应的结果都根据配体官能度进行了讨论。已制备出九种基于硫醚附加亚氨基酚盐 (ONS) 配体的新型配合物，并通过 NMR 光谱在溶液中进行了充分表征。
Nine new complexes based on thioether appended iminophenolate (ONS) ligands have been prepared and fully characterized in solution by NMR spectroscopy. Solid-state structures were also obtained for seven complexes. In solution, all complexes were monomeric. The complexes were highly active for the polymerization of purified rac-lactide ([M] : [Zn] : [BnOH] = 10 000 : 1 : 30 at 180 °C) reaching TOF values up to 250 000 h−1. The kinetics of the polymerization have been probed by in situ Raman spectroscopy. The rate of reaction was dramatically reduced using technical grade rac-lactide with increased initiator loading. To move towards a circular economy, it is vital that catalysts are developed to facilitate chemical recycling of commodity and emerging polymeric materials. In this vein, the complexes have been assessed for their ability to break down poly(lactic acid) and poly(ethylene terephthalate). The results from both the polymerization and degradation reactions are discussed in terms of ligand functionality. Nine new complexes based on thioether appended iminophenolate (ONS) ligands have been prepared and fully characterized in solution by NMR spectroscopy.
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