The unsustainable exploitation of fossil feedstocks for energy and chemical production has led, in the past few years, to the modern energy and environmental crisis, thus stimulating increased awareness in the definition of more sustainable alternatives. Among the transformations of biomass-derived levulinic acid, recognized as one of the top 10 platform molecules, the production of 5-methylpyrrolidinones is of great importance in diverse industrial fields. In this work, we defined a waste-minimized protocol for the production of N-aryl 5-methylpyrrolidinones, aiming both at the synergistic employment of a benign H-source and reaction media and at the optimization of the workup and purification step. The choice of formic acid as the hydrogen carrier and water as the solvent was beneficial for the replacement of gaseous hydrogen typically used in the synthesis of N-aryl 5-methylpyrrolidinones. Moreover, the safety and economic advantages of formic acid as a benign LOHC for this transformation were further confirmed by a comparison, with other H-sources, of the Ecoscale penalty points. The optimized extraction workup protocol allowed an E-factor reduction of 63% compared to a simple filtration for purification method. To further evidence the environmental improvement, Ecoscale was exploited, highlighting the benefits of our process in comparison to available literature protocols.

中文翻译：

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利用甲酸作为 LOHC 的乙酰丙酸平台分子的环保还原胺化，用于合成 5-甲基-N-芳基-吡咯烷酮


在过去几年中，用于能源和化工生产的化石原料的不可持续开采导致了现代能源和环境危机，从而激发了人们对定义更可持续替代品的认识提高。在生物质衍生的乙酰丙酸（公认的 10 大平台分子之一）的转化中，5-甲基吡咯烷酮的生产在不同的工业领域中具有重要意义。在这项工作中，我们定义了一种用于生产 N-芳基 5-甲基吡咯烷酮的废物最小化方案，旨在协同使用良性 H 源和反应介质以及优化后处理和纯化步骤。选择甲酸作为氢载体，选择水作为溶剂，有利于替代通常用于合成 N-芳基 5-甲基吡咯烷酮的气态氢。此外，通过与其他 H 源的 Ecoscale 惩罚点的比较，进一步证实了甲酸作为这种转化的良性 LOHC 的安全性和经济优势。与简单的纯化过滤方法相比，优化的提取后处理方案可将 E 因子降低 63%。为了进一步证明环境改善，我们利用了 Ecoscale，与现有文献方案相比，突出了我们工艺的优势。