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Green process for green materials: viable low-temperature lipase-catalysed synthesis of renewable telechelics in supercritical CO2

机译:绿色材料的绿色工艺:在超临界CO2中可行的低温脂肪酶催化的可再生远螯螯合物的合成

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摘要

We present a novel near ambient temperature approach to telechelic renewable polyesters by exploiting the unique properties of supercritical CO2 (scCO2). Bio-based commercially available monomers have been polymerised and functional telechelic materials with targeted molecular weight were prepared by end-capping the chains with molecules containing reactive moieties in a one-pot reaction. The use of scCO2 as a reaction medium facilitates the effective use of Candida Antarctica Lipase B (CaLB) as a catalyst at a temperature as low as 35 °C, hence avoiding side reactions, maintaining the end-capper functionality and preserving the enzyme activity.udThe functionalised polymer products have been characterised by 1H-NMR, MALDI-TOF, GPC and DSC in order to carefully assess their structural and thermal properties.udWe demonstrate that telechelic materials can be produced enzymatically at mild temperatures, in a solvent-free system and using renewably sourced monomers without pre-modification, by exploiting the unique properties of scCO2. The macromolecules we prepare are ideal green precursors that can be further reacted to prepare useful bio-derived films and coatings.
机译:通过利用超临界CO2(scCO2)的独特性能,我们提出了一种新的近环境温度方法,用于远螯可再生聚酯。已经聚合了生物基市售单体,并通过在一个反应​​罐中用含有反应性部分的分子对链进行了封端,从而制备了具有目标分子量的功能远螯材料。使用scCO2作为反应介质有助于在低至35°C的温度下有效地使用南极假丝酵母脂肪酶B(CaLB)作为催化剂,从而避免了副反应,保持了封端剂的功能性并保留了酶的活性。 ud功能化的聚合物产品已通过1H-NMR,MALDI-TOF,GPC和DSC进行了表征,以便仔细评估其结构和热性能。 ud我们证明了远螯材料可以在温和的温度下以酶法生产,无溶剂。通过利用scCO2的独特性能,可在不进行预修饰的情况下使用可再生来源的单体。我们制备的大分子是理想的绿色前体,可以进一步反应以制备有用的生物衍生膜和涂层。

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