Abstract In this work we aimed to achieve a totally sustainable Ring Opening Polymerisation (ROP) process, by harmonising the use of naturally occurring or derivable initiators and the green solvent 2-Methyltetrahydrofuran (2-MeTHF). First, a library of novel monoterpene-alcohols and existing terpenoids was used to provide renewably sourced initiators for a metal-free ROP synthetic step. A number of these initiators are derived from waste materials, further improving their sustainability. Secondly, we selected lactide (LA) as a monomer, because not only is it derived from biomass, but its resultant polymers are biocompatible and biodegradable. Interestingly, these new polymers self-assembled in water producing well defined, biocompatible nanoparticles (NPs) via direct nanoprecipitation without the use of additional stabilisers. We have highlighted a novel and promising (ROP) approach to produce biodegradable, amphiphilic ester-based macromolecules, based on lactide and terpenes (as initiators) in a green solvent, 2-MeTHF thus reducing solvent toxicity in an efficient, simple and sustainable new synthesis. The monoterpenes may provide a highly functionalisable and bio-renewable toolbox for a new generation of ROP initiators.

中文翻译：

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单萜功能化丙交酯低聚物的“绿色”一锅法合成

摘要 在这项工作中，我们旨在通过协调使用天然存在或衍生的引发剂和绿色溶剂 2-甲基四氢呋喃 (2-MeTHF) 来实现完全可持续的开环聚合 (ROP) 过程。首先，使用新型单萜醇和现有萜类化合物库为无金属 ROP 合成步骤提供可再生来源的引发剂。许多这些引发剂来自废料，进一步提高了它们的可持续性。其次，我们选择丙交酯 (LA) 作为单体，因为它不仅来自生物质，而且其所得聚合物具有生物相容性和可生物降解性。有趣的是，这些新聚合物在水中自组装，通过直接纳米沉淀产生定义明确的生物相容性纳米颗粒 (NPs)，无需使用额外的稳定剂。我们强调了一种新颖且有前景的 (ROP) 方法来生产基于丙交酯和萜烯（作为引发剂）在绿色溶剂 2-MeTHF 中的可生物降解、两亲酯类大分子，从而以一种高效、简单和可持续的新方法降低溶剂毒性。合成。单萜可为新一代 ROP 引发剂提供高度功能化和生物可再生的工具箱。