催化学报

催化学报 ›› 2011, Vol. 32 ›› Issue (9): 1508-1512.DOI: 10.3724/SP.J.1088.2011.10514

• 研究论文 • 上一篇    下一篇

分子印迹聚合物负载纳米金催化剂的制备及其底物识别性能

祝贞科 1, 谭蓉 1,a, 孙文庆 1, 银董红 1,2,b   

  1. 1湖南师范大学精细催化合成研究所, 湖南长沙 410081; 2湖南中烟工业有限责任公司技术研发中心, 湖南长沙 410014
  • 收稿日期:2011-05-14 修回日期:2011-06-17 出版日期:2011-09-09 发布日期:2015-01-24

Preparation of Molecularly Imprinted Polymer-Supported Gold Nanoparticles and Their Ability for Specific Substrate Recognition

ZHU Zhenke1, TAN Rong1,a, SUN Wenqing1, YIN Donghong1,2,b   

  1. 1Institute of Fine Catalysis and Synthesis, Hunan Normal University, Changsha 410081, Hunan, China; 2R&D Center, China Tobacco Hunan Industrial Corporation, Changsha 410014, Hunan, China
  • Received:2011-05-14 Revised:2011-06-17 Online:2011-09-09 Published:2015-01-24

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摘要： 以 4-硝基苯甲醇与氯金酸的络合物为模板, 利用聚合物空腔内胺基捕获 NaBH4 还原的纳米粒子, 设计和制备了一种具有底物识别性能的分子印迹聚合物负载纳米 Au 催化剂 (Au/MIP). 运用红外光谱、紫外-可见光谱和扫描电镜等方法对催化剂进行了表征. 同时以水为溶剂, 过氧化氢为氧化剂, 考察了催化剂在取代苯甲醇氧化反应中的催化性能. 结果表明, 以 Au/MIP 为催化剂时, 4-硝基苯甲醇转化率为 75.6%, 而以非印迹聚合物负载的纳米 Au (Au/NIP) 为催化剂时, 4-硝基苯甲醇转化率仅为 41.5%. 以其它取代苯甲醇为底物时, Au/MIP 与 Au/NIP 的催化活性差别不大. 这说明 Au/MIP 催化剂活性与反应底物结构有关, 脱除模板剂后它具有与 4-硝基苯甲醇相匹配的空腔结构和识别位点, 对反应底物表现出专一的识别性, 因而提高了催化剂活性.

关键词: 分子印迹聚合物, 金纳米粒子, 取代苯甲醇, 催化氧化, 底物识别性

Abstract: A molecularly imprinted polymer-supported gold nanoparticle (Au/MIP) catalyst, which has the characteristics of specific substrate recognition, was prepared by the template complex of 4-nitrobenzyl alcohol (4-NBA) and hydrogen tetrachloroaurate(III), where Au nanaoparticles were formed by the reduction with NaBH4 solution and captured by amino groups (-NH2) in the cavities of the MIP. The obtained samples were characterized with FT-IR spectroscopy, UV-Vis spectroscopy, and scanning electron microscopy. The catalytic activity and substrate recognition of the Au/MIP were investigated by the oxidation of substituted benzyl alcohol using H2O2 as the oxidant in water. It was found that the conversion of 4-NBA was up to 75.6% over Au/MIP when using the template molecule of 4-NBA as the substrate. However, the conversion of 4-NBA was only 41.5% over non-imprinted polymer-supported gold nanoparticle (Au/NIP) because no template molecule of 4-NBA was used in the preparation of catalyst. Furthermore, no significant difference of the catalytic activity between the catalysts Au/MIP and Au/NIP was observed when other substituted benzyl alcohols were used as the substrate. These results indicated that the catalytic activity of Au/MIP was related to the structure of substrates. The Au/MIP after removal of the template had molecular recognition shape and sites in the cavities matching to the substrate of 4-NBA molecule. The special recognizable cave of the Au/MIP exhibited unique substrate recognition and therefore improved the catalytic activity.

Key words: molecular imprinted polymer, gold nanoparticle, substituted benzyl alcohol, catalytic oxidation, substrate recognition