Mono- and dimeric zinc(II) complexes for PLA production and degradation into methyl lactate – a chemical recycling method,Polymer Chemistry

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Mono- and dimeric zinc(II) complexes for PLA production and degradation into methyl lactate – a chemical recycling method
Polymer Chemistry ( IF 4.1 ) Pub Date : 2020/02/27 , DOI: 10.1039/d0py00192a
Jack Payne _{1,

2,

3,

4} , Paul McKeown _{1,

2,

3,

4} , Mary F. Mahon _{2,

3,

4,

5} , Emma A. C. Emanuelsson _{1,

2,

3,

4,

6} , Matthew D. Jones _{1,

2,

3,

4,

5}

Affiliation

A series of well-defined mono- and dimeric Zn(II)-complexes were prepared and fully characterised by X-ray crystallography and NMR spectroscopy. Their application to the ROP of rac-LA to produce biocompatible atactic PLA was demonstrated in both solution and under industrially preferred melt conditions at 180 °C with a [rac-LA] : [Init] : [BnOH] of 3000 : 1 : 10. Exceptional activity was observed in all instances, albeit with generally poor molecular weight control (M_n) and broad dispersities (Đ), with dimers outperforming their monomeric counterparts. The propensity of all Zn(II)-complexes to facilitate PLA degradation into methyl lactate (Me-LA) under mild conditions is also demonstrated. Zn(2–3)₂ were identified as the outstanding candidates, achieving full conversion to Me-LA within 8 h at 80 °C in THF. Further degradation kinetic analysis revealed Zn(2–3)₂ to have k_app values of 0.63 ± 0.051 and 0.44 ± 0.029 h⁻¹ for the rate of consumption of PLA respectively.

中文翻译：

用于PLA生产和降解为乳酸甲酯的单和二聚锌（II）配合物-化学回收方法

制备了一系列定义明确的单和二聚Zn（II）配合物，并通过X射线晶体学和NMR光谱进行了全面表征。在溶液和工业上优选的熔融条件下，在180°C的[ rac -LA]：[Init]：[BnOH]为3000：1：10的溶液和工业首选熔融条件下，证明了它们在rac -LA的ROP中生产生物相容的无规立构PLA的应用。。在所有情况下，观察到异常的活性，尽管一般较差分子量控制（中号_ñ）和广泛的分散度（Đ）中，用二聚物优于它们的单体对应。所有Zn（II还显示了在温和条件下促进PLA降解为乳酸甲酯（Me-LA）的复合物。Zn（2-3）₂被确定为出色的候选物，在THF中于80°C在8 h内完全转化为Me-LA。进一步降解动力学分析揭示的Zn（2-3）₂为具有ķ_应用的0.63±0.051和0.44±0.029ħ值^-1分别为PLA的消耗速率。

更新日期：2020-03-31

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