含Sn-Mg双金属催化剂的合成及其在合成ε-己内酯反应中的应用  

Synthesis of Sn-Mg Bimetallic Catalysts and Application in Synthesis of ε-Caprolactone

作　　者：张雯艳 郑燕春 王思嘉 郎美东[1] ZHANG Wenyan;ZHENG Yanchun;WANG Sijia;LANG Meidong(School of Materials Science and Engineering,East China University of Science and Technology,Shanghai 200237,China;Quzhou Juhua Polyamide Fibre Limited Company,Quzhou 324000,Zhejiang,China)

机构地区：[1]华东理工大学材料科学与工程学院,上海200237 [2]衢州巨化锦纶有限责任公司,浙江衢州324000

出　　处：《功能高分子学报》2023年第5期492-498,共7页Journal of Functional Polymers

摘　　要：通过简单的合成手段在常温常压下制备出一种含有镁的锡类催化剂,命名为Sn-Mg-M。利用傅里叶红外光谱、X射线衍射、热重分析等表征手段对催化剂结构进行了表征,并且对其在Baeyer-Villiger氧化中的催化效果进行了研究,探究了不同配比的催化剂、氧化剂种类以及反应条件对催化效果的影响。结果表明:当催化剂中n(Sn)∶n(Mg)=4∶1,过氧化氢(H2O2)与环己酮物质的量投料比为4∶1,环己酮浓度为0.33 mmol/mL,催化剂与反应物的质量比为1.57∶1,在65℃的反应条件下反应12 h时,环己酮的转换率可以为73.27%,ε-己内酯产率为24.16%。同时催化剂结构稳定,且能够被循环使用。As an extensively utilized organic synthetic monomer,ε-caprolactone(ε-CL)exhibits notable properties such as biodegradability and biocompatibility.Consequently,the investigation ofε-CL monomer synthesis holds great significance.In this study,a tin catalyst containing magnesium named Sn-Mg-M,was synthesized by a simple method at ambient temperature and atmospheric pressure for the preparation ofɛ-caprolactone monomers.This study focuses on the characterization of catalyst structure using Fourier Infrared Spectroscopy(FT-IR),X-ray Diffraction(XRD),Thermogravimetric analysis(TGA).Furthermore,the catalytic effect of catalyst Sn-Mg-M in Baeyer-Villiger oxidation was investigated to examine the impact of various catalyst ratios,oxidant types,and reaction conditions on the catalytic effect.The experimental results demonstrated that a molar ratio of 4∶1 between Sn and Mg in the catalyst,a feeding molar ratio of 1∶4 between cyclohexanone and hydrogen peroxide(H2O2),a cyclohexanone concentration of 0.33 mmol/mL,and a catalyst-to-reactants mass ratio of 1.57∶1,along with a reaction conducted at 65℃for 12 h,resulted in a cyclohexanone conversion rate of 73.27%and a yield of 24.16% for ε-CL. Additionally, it was confirmed that the catalyst exhibited structural stability and could be recycled.

关 键 词：金属催化剂 Ε-己内酯 BAEYER-VILLIGER氧化 循环使用 结构稳定 

分 类 号：TQ426.8[化学工程]