高等学校化学学报 ›› 2019, Vol. 40 ›› Issue (9): 1805-1812.doi: 10.7503/cjcu20190191

• 研究论文:无机化学 • 上一篇    下一篇

基于中心辐射树枝状介孔二氧化硅构筑CPO固定化酶反应器及应用

宋艺超1,胡满成1,2,李淑妮1,2,翟全国1,2,蒋育澄1,2,*()   

  1. 1. 陕西师范大学化学化工学院
    2. 大分子科学陕西省重点实验室, 西安 710062
  • 收稿日期:2019-03-31 出版日期:2019-09-10 发布日期:2019-07-17
  • 通讯作者: 蒋育澄 E-mail:jyc@snnu.edu.cn
  • 基金资助:
    国家自然科学基金(21873061)

Construction of CPO Immobilized Enzyme Reactor Based on Center-radial Dendritic Mesoporous Silica and Its Application

SONG Yichao1,HU Mancheng1,2,LI Shuni1,2,ZHAI Quanguo1,2,JIANG Yucheng1,2,*()   

  1. 1. School of Chemistry & Chemical Engineering;
    2. Key Laboratory of Macromolecular Science of Shaanxi Province, Shaanxi Normal University,Xi’an 710062, China;
  • Received:2019-03-31 Online:2019-09-10 Published:2019-07-17
  • Contact: JIANG Yucheng E-mail:jyc@snnu.edu.cn
  • Supported by:
    ? Supported by the National Natural Science Foundation of China(21873061)

摘要:

首先制备粒径均匀的具有开放的三维中心辐射树枝状结构的介孔二氧化硅(DSP)粒子, 再通过静电相互作用在孔道内负载氯过氧化物酶(CPO)构筑了CPO@DSP固定化酶反应器. 通过改变硅源正硅酸乙酯(TEOS)和模板剂十六烷基三甲基氯化铵(CTAC)的浓度调控孔径大小, 研究了孔径对固定化酶反应器催化活性的影响; 同时基于酶促反应动力学分析探讨了孔道内酶催化反应的限域效应, 并进一步在CPO@DSP表面包覆海藻酸钠(SA)水凝胶薄膜以抑制酶反应器在使用过程中酶分子的泄露, 所得SA-CPO@DSP固定化酶反应器的重复使用性显著提高, 循环使用10次后, 仍能保持90%以上的催化活性. 将SA-CPO@DSP酶反应器用于环境水体中残留抗生素左氧氟沙星的降解, 对100 μg/mL的底物在25 min内降解率可达88%以上; 将该反应器用于苯酚的视觉比色检测, 裸眼可检测到5 μmol/L的苯酚, 表明SA-CPO@DSP酶反应器在环境保护方面具有良好的应用前景.

关键词: 固定化酶反应器, 介孔二氧化硅, 氯过氧化物酶, 环境应用

Abstract:

The mesoporous silica particles(DSP) with open three-dimensional center-radial dendrimers and uniform particle size were first prepared. Then CPO@DSP immobilized enzyme reactor was prepared by electrostatic interaction with chloroperoxidase(CPO) entrapped into the pore channel. The pore size was regulated by changing the concentrations of tetraethyl orthosilicate(TEOS) and the template agent cetyltrimethylammo-nium chloride(CTAC). The effect of pore size on the catalytic activity of immobilized enzyme reactor was studied. At the same time, the limiting effect of pore channel was discussed based on the kinetic analysis of enzymatic reaction. In addition, sodium alginate(SA) hydrogel film coated on the surface of CPO@DSP was used to improve the leakage of enzyme molecules in the enzyme reactor, and the reusability of the obtained SA-CPO@DSP enzyme reactor was significantly improved. After 10 times of reuse, more than 90% of the catalytic activity was still maintained. When SA-CPO@DSP was applied to the degradation of residual antibiotics in environmental water, the degradation rate of 100 μg/mL substrate in 25 min was over 88%. SA-CPO@DSP was also used for visual colorimetric detection of phenol and 5 μmol/L phenol could be detected by naked eyes. It showed the application prospect of SA-CPO@DSP in environmental protection.

Key words: Immobilized enzyme reactor, Mesoporous silica, Chloroperoxidase, Environmental application

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