分子印迹聚合物负载Fe(III)催化剂的底物识别性能

doi:10.1016/S1872-2067(12)60624-X

催化学报 ›› 2013, Vol. 34 ›› Issue (8): 1589-1598.DOI: 10.1016/S1872-2067(12)60624-X

分子印迹聚合物负载Fe(III)催化剂的底物识别性能

孙文庆^a, 谭蓉^a, 郑卫国^a, 银董红^a,b

a 湖南师范大学精细催化合成研究所, 化学生物学和中药分析教育部重点实验室, 湖南长沙410081;
b 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:2013-01-09 修回日期:2013-05-14 出版日期:2013-08-16 发布日期:2013-07-30
通讯作者: 谭蓉,银董红
基金资助:
国家自然科学基金(21003044, 20973057); 湖南省自然科学基金(10JJ6028); 湖南省教育厅高校科技创新团队.

Molecularly imprinted polymer containing Fe(III) catalysts for specific substrate recognition

Wenqing Sun^a, Rong Tan^a, Weiguo Zheng^a, Donghong Yin^a,b

a Institute of Fine Catalysis and Synthesis, Key Laboratory of Chemical Biology and Traditional Chinese Medicine Research (Ministry of Education), Hunan Normal University, Changsha 410081, Hunan, China;
b Research and Development Center, China Tobacco Hunan Industrial Corporation, Changsha 410014, Hunan, China

Received:2013-01-09 Revised:2013-05-14 Online:2013-08-16 Published:2013-07-30
Supported by:
This work was supported by the National Natural Science Foundation of China (21003044, 20973057), the Natural Science Foundation of Hunan Province (10JJ6028), and the Program for Science and Technology Innovative Research Team in Higher Educational Institutions of Hunan Province.

摘要/Abstract

摘要： 分别以o-, m-和p-硝基苯甲醇与FeCl₃的配合物为模板分子,丙烯酰胺为功能单体,二甲基丙烯酸乙二醇酯为交联剂,采用本体聚合法制备了三种Fe(III)含量相同的分子印迹聚合物(MIP)o-Fe(III)-MIP,m-Fe(III)-MIP和p-Fe(III)-MIP.并采用扫描电镜、N₂吸附-脱附及红外光谱等方法对催化剂结构进行了表征.在以水为溶剂,过氧化氢(30%)为氧化剂的苯甲醇衍生物氧化反应中,该类催化剂表现出优异的催化活性和独特的底物识别性能.当以p-Fe(III)-MIP为催化剂时,p-硝基苯甲醇的转化率达到80%,而在其他两个催化剂上均低于58%.这表明Fe(III)-MIP催化剂结构中具有与底物分子匹配的印迹空腔与识别位点,对底物分子表现出专一识别性,因而提高了催化剂对底物的选择性.

关键词: 分子印迹聚合物, 铁(III)催化剂, 苯甲醇衍生物, 催化氧化, 底物识别

Abstract: A series of molecularly imprinted polymers (MIPs) containing equal amounts of iron(III) were prepared by the polymerization of acrylamide and ethylene dimethacrylate in the presence of the template of o-, m-, or p-nitrobenzyl alcohol (NBA) and a FeCl₃ complex. The samples were characterized by scanning electron microscopy, N₂ adsorption, and Fourier transform infrared spectroscopy. The catalysts exhibited high catalytic activity and unique substrate recognition in the oxidation of benzyl alcohol derivatives in water using 30% H₂O₂ as the oxidant. The conversion of p-NBA was 80% over the p-Fe(III)-MIP catalyst when the template molecule was p-NBA, which had a good fit with the substrate. However, the conversion of p-NBA was less than 58% over o-Fe(III)-MIP or m-Fe(III)-MIP due to the mismatch of the substrate with the cavities of the Fe(III)-MIP. The results indicated that the Fe(III)-MIP samples contained molecular recognizable shapes and sites in their cavities that match the corresponding substrate. The special recognizing cavities of the Fe(III)-MIP catalyst exhibited unique substrate recognition, and therefore the selectivity for the substrate was improved.

Key words: Molecularly imprinted polymer, Iron(III) catalyst, Benzyl alcohol derivative, Catalytic oxidation, Substrate recognition

孙文庆, 谭蓉, 郑卫国, 银董红. 分子印迹聚合物负载Fe(III)催化剂的底物识别性能[J]. 催化学报, 2013, 34(8): 1589-1598.

Wenqing Sun, Rong Tan, Weiguo Zheng, Donghong Yin. Molecularly imprinted polymer containing Fe(III) catalysts for specific substrate recognition[J]. Chinese Journal of Catalysis, 2013, 34(8): 1589-1598.

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参考文献

[1] Petcu M, Karlsson J P, Whitcombe M J, Nicholls I A. J Mol Recognit, 2009, 22: 18

[2] Haupt K, Dzgoev A, Mosbach K. Anal Chem, 1998, 70: 628

[3] Andersson L, Sellergren B, Mosbach K. Tetrahedron Lett, 1984, 25: 5211

[4] Matsui J, Nicholls I A, Takeuchi T, Mosbach K, Karube I. Anal Chim Acta, 1996, 335: 71

[5] Brunkan N M, Gagné M R. J Am Chem Soc, 2000, 122: 6217

[6] Li Y Z, Fan Y N, Yang H P, Xu B L, Feng L Y, Yang M F, Chen Y. Chem Phys Lett, 2003, 372: 160

[7] Tang Z C, Li Q Y, Lu G X. Carbon, 2007, 45: 41

[8] Li S J, Gong S Q. Adv Funct Mater, 2009, 19: 2601

[9] Guo J J, Cai J B, Su Q D. J Rare Earths, 2009, 27: 22

[10] Liu H X, Yue H, Li S J, Li W K. J Inorg Organomet Polym Mater, 2009, 19: 335

[11] Tada M, Iwasawa Y. J Mol Catal A, 2003, 199: 115

[12] Hashmi A S K. Chem Rev, 2007, 107: 3180

[13] Yadav G D, Mistry C K. J Mol Catal A, 2001, 172: 135

[14] Liu C, Tan R, Yu N Y, Yin D H. Microporous Mesoporous Mater, 2010, 131: 162

[15] Liu C B, Ye X K, Wu Y. Chin J Catal (刘诗标, 叶兴凯, 吴越. 催化学报), 1997, 18: 140

[16] Lan W, Zhong S, Fu Z H. Ind Catal (China) (兰婉, 衷晟, 伏再辉. 工业催化),2008, 116: 52

[17] Li S J, Tong K J, Zhang D N, Huang X. J Inorg Organomet Polym Mater, 2008, 18: 264

[18] Liu C, Tan R, Sun W Q, Yin D H. Chin J Catal (刘成, 谭蓉, 孙文庆, 银董红. 催化学报), 2012, 33: 1032

[19] Peng L, Yu N Y, Tang Q L, Qiu H Y, Yin D L, Yin D H. Acta Phys-Chim Sin, 2007, 23: 1572

[20] Li S J, Liao C, Li W K, Chen Y F, Hao X. Macromol Biosci, 2007, 7: 1112

[21] Zhang D N, Li S G, Li W K, Chen Y F. Catal Lett, 2007, 115: 169

[22] Hoshino Y, Koide H, Urakami T, Kanazawa H, Kodama T, Oku N, Shea K J. J Am Chem Soc, 2010, 132: 6644

[23] Zhu Z K, Tan R, Sun W Q, Yin D H. Chin J Catal (祝贞科, 谭蓉, 孙文庆, 银董红. 催化学报), 2011, 32: 1508

分子印迹聚合物负载Fe(III)催化剂的底物识别性能

Molecularly imprinted polymer containing Fe(III) catalysts for specific substrate recognition

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