Pd/Al2O3-Novozyme 435动态动力学拆分1,1,1-三氟异丙胺

doi:10.16085/j.issn.1000-6613.2017.01.041

化工进展 ›› 2017, Vol. 36 ›› Issue (01): 324-328.DOI: 10.16085/j.issn.1000-6613.2017.01.041

Pd/Al₂O₃-Novozyme 435动态动力学拆分1,1,1-三氟异丙胺

蒋成君^1,2, 徐国明³, 袁慎峰¹

1 浙江大学化学工程与生物工程学院, 浙江杭州 310027;
2 浙江科技学院生物与化学工程学院, 浙江杭州 310023;
3 捷马化工股份有限公司, 浙江龙游 324400

收稿日期:2016-05-20 修回日期:2016-09-08 出版日期:2017-01-05 发布日期:2017-01-05
通讯作者: 蒋成君(1981-),男,博士,高级工程师。E-mail:jcj312@163.com。
作者简介:蒋成君(1981-),男,博士,高级工程师。E-mail:jcj312@163.com。
基金资助:
中国博士后科学基金（2014M551745）及浙江省自然科学基金（LY15B060008）项目。

Research on the dynamic kinetic resolution of 1,1,1-trifluoroisopropylamine by Pd/Al₂O₃ and Novozyme 435

JIANG Chengjun^1,2, XU Guoming³, YUAN Shenfeng¹

1 College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, Zhejiang, China;
2 School of Biological and Chemical Engineering, Zhejiang University of Science & Technology, Hangzhou 310023, Zhejiang, China;
3 JingMa Chemicals Co., Ltd., Longyou 324400, Zhejiang, China

Received:2016-05-20 Revised:2016-09-08 Online:2017-01-05 Published:2017-01-05

摘要/Abstract

摘要： 应用响应面优化的方法研究Pd/Al₂O₃和Novozyme 435动态动力学拆分1，1，1-三氟异丙胺（TFPA）的协同作用。根据Box-Behnken实验设计原理，对实验进行设计与分析，以转化率和ee值为响应量建立回归模型，分析各因素的显著性与交互作用。结果表明：反应条件对ee值的影响较小，以转化率为响应量时，Pd/Al₂O₃和Novozyme 435交互作用显著，两种催化剂有相互抑制作用。最佳工艺条件为：Pd/Al₂O₃催化剂用量5g/L、反应温度50℃、Novozyme 435的用量10g/L、TFPA的浓度0.5mol/L，预测转化率可以达到98.56%，与实验相符。产物N-[（1R）-2，2，2-三氟-1-甲基乙基]-乙酰胺的ee值可达到96.69%。

关键词: 酶, 催化, 化学反应, 选择性

Abstract: Response Surface Methodology (RSM) was successfully applied to study the synergistic effect of Pd/Al₂O₃ and Novozyme 435 on the dynamic kinetic resolution of 1,1,1-trifluoroisopropylamine(TFPA). The variables taken into consideration were reaction temperature,substrate concentration,the Pd/Al₂O₃ amount,and the Novozyme 435 amount. Experiments were designed and analyzed based on Box-Behnken principle. A statistical model was used to evaluate the influence of the variables on the conversion and enantiomeric excess(ee). It was found that the interaction between the Novozyme 435 and Pd/Al₂O₃ was a significant parameter that affected TFPA conversion. The optimum conditions for RSM were:reaction temperature of 50℃,TFPA concentration of 0.5mol/L,10g/L of Novozyme 435,and 5g/L of Pd/Al₂O₃. The actual experimental conversion rate under optimum conditions was similarly as the maximum predicted value of 98.56%. The product N-[(1R)-2,2,2-trifluoro-1-methylethyl]-acetamide was obtained with enantiomeric excesses of 96.69%.

Key words: enzyme, catalysis, chemical reaction, selectivity

中图分类号:

TQ463

蒋成君, 徐国明, 袁慎峰. Pd/Al₂O₃-Novozyme 435动态动力学拆分1,1,1-三氟异丙胺[J]. 化工进展, 2017, 36(01): 324-328.

JIANG Chengjun, XU Guoming, YUAN Shenfeng. Research on the dynamic kinetic resolution of 1,1,1-trifluoroisopropylamine by Pd/Al₂O₃ and Novozyme 435[J]. Chemical Industry and Engineering Progree, 2017, 36(01): 324-328.

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Pd/Al₂O₃-Novozyme 435动态动力学拆分1,1,1-三氟异丙胺

Research on the dynamic kinetic resolution of 1,1,1-trifluoroisopropylamine by Pd/Al₂O₃ and Novozyme 435

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