Menuel Stéphane, Saitzek Sébastien, Monflier Eric, Hapiot Frédéric
Univ. Artois, CNRS, Centrale Lille, Univ. Lille, UMR 8181, Unité de Catalyse et Chimie du Solide, F-62300 Lens, France.
Beilstein J Org Chem. 2020 Oct 22;16:2598-2606. doi: 10.3762/bjoc.16.211. eCollection 2020.
The mechanically assisted synthesis of organic compounds has recently focused considerable attention as it may be unique in features to selectively direct the reaction pathway. In the continuation of our work on the synthesis of modified cyclodextrins (CDs) via mechanochemical activation, we sought to discriminate the contribution of supramolecular effects and grinding during the course of a reaction in the solid state. As such, we recently investigated the influence of the particle size of β-CD in the synthesis of β-CD mesitylene sulfonate (β-CDMts) in the solid state using a vibrating ball-mill. We were particularly interested in the role of the particle size on the kinetics of the reaction. In this study, we show that grinding β-CD reduces the particles size over time down to a limit of 167 nm. The granulometric composition remains rather invariant for grinding times over 1 h. Each type of β-CD particles reacted with mesitylenesulfonyl chloride (MtsCl) to produce β-CDMts. Contrary to what could be intuitively anticipated, smaller particles did not lead to the highest conversions. The impact of grinding on the conversion was limited. Interestingly, the proportion of β-CDMts mono-substituted on the primary face significantly increased over time when the reaction was carried out in the presence of KOH as a base. The data series were confronted with kinetics models to get insight in the way the reactions proceeded. The diversity of possible models suggests that multiple mechanochemical processes can account for the formation of β-CDMts in the solid state. Throughout the study, we found that the reactivity depended more upon diffusion phenomena in the crystalline parts of the material than on the increase in the surface area of the CD particles resulting from grinding.
机械辅助有机化合物合成最近备受关注,因为它在选择性引导反应路径方面可能具有独特的特性。在我们通过机械化学活化合成改性环糊精(CDs)的工作延续中,我们试图区分超分子效应和固态反应过程中研磨的作用。因此,我们最近使用振动球磨机研究了β-环糊精粒径对固态合成β-环糊精均三甲苯磺酸盐(β-CDMts)的影响。我们特别关注粒径对反应动力学的作用。在这项研究中,我们表明研磨β-环糊精会使粒径随时间减小至167nm的极限。对于超过1小时的研磨时间,粒度组成保持相当不变。每种类型的β-环糊精颗粒都与均三甲苯磺酰氯(MtsCl)反应生成β-CDMts。与直观预期相反,较小的颗粒并没有导致最高转化率。研磨对转化率的影响有限。有趣的是,当反应在作为碱的KOH存在下进行时,主面上单取代的β-CDMts的比例随时间显著增加。将数据系列与动力学模型进行对比,以深入了解反应进行的方式。可能模型的多样性表明,多种机械化学过程可以解释固态β-CDMts的形成。在整个研究过程中,我们发现反应性更多地取决于材料结晶部分中的扩散现象,而不是研磨导致的CD颗粒表面积的增加。