食品科学

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硼钨杂多酸盐催化合成柠檬烯-1,2-环氧化物的工艺优化

李胜芮,潘思轶*,王可兴   

  1. 华中农业大学食品科学技术学院,环境食品学教育部重点实验室,湖北 武汉 430070
  • 出版日期:2016-05-25 发布日期:2016-05-18

Optimization of Preparation Process of Heteropolytungstoborate Catalyst Used for the Synthesis of Limonene-1,2-epoxide

LI Shengrui, PAN Siyi*, WANG Kexing   

  1. Key Laboratory of Environment Correlative Dietology, Ministry of Education, College of Food Science and Technology,Huazhong Agricultural University, Wuhan 430070, China
  • Online:2016-05-25 Published:2016-05-18

摘要:

为提高柠檬烯-1,2-环氧化物收率,采用正交试验法,优选硼钨杂多酸盐的最佳制备工艺。通过单因素试验研究了催化剂制备工艺中稀硫酸-钨酸钠物质的量比、钨酸钠-硼酸物质的量比、十六烷基三甲基氯化铵(cetyltrimethyl ammonium chloride,CTMA)-钨酸钠物质的量比、合成温度及合成时间对柠檬烯-1,2-环氧化物收率的影响,利用正交试验法优化最佳制备工艺条件。结果:当稀硫酸-钨酸钠物质的量比1.5∶1、钨酸钠-硼酸物质的量比3∶1、CTMA-钨酸钠物质的量比1∶3、合成温度80 ℃、合成时间1 h时,柠檬烯-1,2-环氧化物的收率可达到4.351 6%。对最优条件下制备的催化剂进行表征分析,表明硼酸、季铵盐均已成功接枝到活性中心上,并且硼钨杂多酸盐催化剂保持Keggin结构的基本骨架,是一种微孔的晶体结构,分子式为C19H44W3BNO18。

关键词: 硼钨杂多酸盐, 柠檬烯, 柠檬烯-1, 2-环氧化物, 催化氧化

Abstract:

The preparation of heteropolytungstoborate, a green and highly active catalyst for the synthesis of limonene-
1,2-epoxide, by chemical reaction was optimized in order to obtain increased yield of limonene-1,2-epoxide. The effects
of molar ratio of dilute sulphuric acid to sodium tungstate, molar ratio of sodium tungstate to boric acid, molar ratio of
cetyl trimethyl ammonium chloride (CTMA) to sodium tungstate, reaction temperature and time on the yield of limonene-
1,2-epoxide were investigated by one-factor-at-a-time method. Further, all process parameters except reaction time were
optimized using an orthogonal array design. Results showed that when the synthesis of limonene-1,2-epoxide was carried out
using the heteropolytungstoborate catalyst obtained after 1 h reaction at 80 ℃ with a molar ratio of dilute sulphuric acid to
sodium tungstate, sodium tungstate to boric acid, and CTMA to sodium tungstate of 1.5:1, 3:1, and 1:3 respectively, the yield
of product was as high as 4.351 6%. These results suggested that the optimized process produced a catalyst that allowed a
remarkable increase in product yield in the synthesis of limonene-1,2-epoxide.

Key words: heteropolytungstoborate, limonene, limonene-1,2-epoxide, catalytic oxidation

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