Phenoxy-imine based Mononuclear Zn(II) Compounds: Applications as Polymerization Catalysts

D. Chakraborty, S. Singha Roy, Saumendra N. Sarkar
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Abstract

The production of aliphatic polyesters (via ROP of cyclic esters) and aliphatic polycarbonates (via ROCOP of CO2/epoxide) is an important synthetic pathway for the production of biodegradable and biocompatible polymers. The study focuses on the catalytic activity and selectivity of phenoxy-imine based zinc compounds for the ROP of cyclic esters (rac-LA and -CL) and ROCOP of carbon dioxide and CHO/PO. The monoligated and bisligated zinc compounds have the same coordination number (four) but differed from each other in the binding mode of the ligand to the metal center (tridentate for monoligated and bidentate for bisligated compounds) and thus the compounds adopt different symmetry. For the ROP of rac-LA, the monoligated zinc compounds gave isotactic-enriched PLA while the bisligated zinc compounds gave heterotactic-enriched PLA. For the ROCOP of epoxide/CO2, isotactic-enriched polycarbonates were obtained with a notable difference in catalytic activity with the variation of the number of ligands attached to the zinc center. In addition, a correlation is established between the percentage of carbonate linkage in the polycarbonate chain and the substituent attached to the phenolate core.
基于苯氧亚胺的单核Zn(II)化合物:作为聚合催化剂的应用
脂肪族聚酯(通过环酯的ROP)和脂肪族聚碳酸酯(通过CO2/环氧化物的ROCOP)的生产是生产生物可降解和生物相容性聚合物的重要合成途径。研究了苯氧亚胺基锌化合物对环酯(rac-LA和 -CL)的ROCOP以及二氧化碳和CHO/PO的ROCOP的催化活性和选择性。单寡锌化合物和双偶锌化合物具有相同的配位数(4),但配体与金属中心的结合方式不同(单寡锌化合物为三齿状,双齿锌化合物为双齿状),因此化合物具有不同的对称性。对于rac-LA的ROP,单聚锌化合物得到等规富集PLA,而偶合锌化合物得到异规富集PLA。对于环氧化物/CO2的ROCOP,得到了等规富集的聚碳酸酯,其催化活性随着锌中心配体数量的变化而显著不同。此外,还建立了聚碳酸酯链中碳酸盐键的百分比与附着在酚酸核上的取代基之间的相关性。
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