Wada Naoki, Hara Takahiro, Takahashi Kenji
Faculty of Biological Science and Technology, Institute of Science and Engineering, Kanazawa University, Kanazawa, Ishikawa 920-1192, Japan.
Graduate School of Natural Science and Technology, Kanazawa University, Kanazawa, Ishikawa 920-1192, Japan.
J Phys Chem B. 2024 Mar 21;128(11):2755-2761. doi: 10.1021/acs.jpcb.3c07225. Epub 2024 Mar 10.
1-Ethyl-3-methylimidazolium acetate (EmimAc), an excellent solvent for cellulosic biomass, is expected to be utilized in chemical conversion, such as in biomass acetylation with acetic anhydride. The corresponding carboxylic acid, acetic acid (AcH), is quantitatively generated as a byproduct and should be separated from EmimAc for recycling. However, the strong interaction between EmimAc and AcH makes their separation difficult under moderate conditions. This study examined the efficacy of protic solvents in distillation and extraction to weaken this interaction through solvation or hydrogen-bonding interactions. The separation efficiency of AcH from EmimAc via distillation increased as the boiling point of the protic solvent increased. Water addition was more effective than the addition of alcohols with boiling points similar to those of water such as 1-propanol and 2-butanol. Furthermore, the favorable effect of water addition on the extraction of AcH was confirmed using common organic solvents, such as diisopropyl ether, diethyl ether, and ethyl acetate. The partition coefficient (α) of AcH between the aqueous and organic phases increased with an increasing dielectric constant of the organic solvent, whereas the α value of EmimAc decreased. Repeated treatments in both distillation and extraction facilitated the complete separation of AcH from EmimAc.
1-乙基-3-甲基咪唑醋酸盐(EmimAc)是纤维素生物质的优良溶剂,有望用于化学转化,例如与乙酸酐进行生物质乙酰化反应。相应的羧酸,即乙酸(AcH),会作为副产物定量生成,并且应与EmimAc分离以便循环利用。然而,EmimAc与AcH之间的强相互作用使得在适度条件下将它们分离变得困难。本研究考察了质子溶剂在蒸馏和萃取过程中的效果,以通过溶剂化或氢键相互作用来削弱这种相互作用。随着质子溶剂沸点的升高,通过蒸馏从EmimAc中分离AcH的效率提高。加水比添加沸点与水相似的醇(如1-丙醇和2-丁醇)更有效。此外,使用二异丙醚、乙醚和乙酸乙酯等常见有机溶剂证实了加水对萃取AcH的有利影响。AcH在水相和有机相之间的分配系数(α)随着有机溶剂介电常数的增加而增大,而EmimAc的α值则减小。蒸馏和萃取中的重复处理有助于将AcH与EmimAc完全分离。