Make or break: Mg(II)- and Zn(II)-catalen complexes for PLA production and recycling of commodity polyesters,Polymer Chemistry

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Make or break: Mg(II)- and Zn(II)-catalen complexes for PLA production and recycling of commodity polyesters
Polymer Chemistry ( IF 4.1 ) Pub Date : 2021-1-12 , DOI: 10.1039/d0py01519a
Jack Payne _{1,

2,

3,

4} , Paul McKeown _{2,

3,

4,

5} , Oliver Driscoll _{2,

3,

4,

5} , Gabriele Kociok-Köhn _{2,

3,

4,

5} , Emma A. C. Emanuelsson _{2,

3,

4,

6} , Matthew D. Jones _{1,

2,

3,

4,

5}

Affiliation

Recently we reported a series of highly active Al(III)-complexes bearing a catalen ligand support for lactide polymerisation, observing unprecedented activity in the melt. Herein we report diversification of the metal to furnish a series of well-defined dimeric Zn(II)- and Mg(II)-complexes, which were fully characterised by X-ray crystallography and NMR spectroscopy. The production of biocompatible atactic PLA from rac-LA in solution and under industrially preferred solvent-free conditions was demonstrated, typically observing good activity and M_n control with a broad range of dispersities (Đ = 1.08–2.04). Mg(II)-Complexes were shown to facilitate the relatively mild methanolysis of PLA, achieving up to 64% conversion to Me-LA within 8 h at 80 °C in THF. Further kinetic analysis found [Mg(1,3)]₂ to have k_app values of 0.628 ± 0.0536 {4 wt% cat. loading} and 0.265 ± 0.0193 h⁻¹ {8 wt% cat. loading} respectively for the rate of consumption of PLA. Preliminary work extended polymer scope to PET from various sources, demonstrating catalyst versatility.

中文翻译：

成败：Mg（II）-和Zn（II）-catalen复合物用于PLA生产和商品聚酯的回收

最近，我们报道了一系列高活性的Al（III）配合物，这些配合物带有用于催化丙交酯聚合反应的卡塔琳配体，在熔体中观察到前所未有的活性。本文中，我们报告了金属的多样化，以提供一系列定义明确的二聚体Zn（II）和Mg（II）复合物，这些复合物已通过X射线晶体学和NMR光谱进行了全面表征。从生产生物相容无规PLA的外消旋溶液中和工业上优选在无溶剂条件下-LA证实，典型地观察良好的活性和中号_Ñ控制与广泛的分散度的（Đ = 1.08-2.04）。镁（II））-复合物显示出可促进PLA的相对温和的甲醇分解，在80°C的THF中在8小时内可实现高达64％的转化为Me-LA。进一步的动力学分析发现[镁（1,3）] ₂具有ķ_应用0.628±0.0536 {4％（重量）的猫的值。负载}和0.265±0.0193 h ^-1 {8 wt％cat。分别为PLA的消耗率。初步工作将聚合物的来源从各种来源扩展到PET，证明了催化剂的多功能性。

更新日期：2021-01-18

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