A New Method for Immobilization of NDHPI on SBA-15 Carrier Used as Catalyst for Selective Oxidation of Toluene

A New Method for Immobilization of NDHPI on SBA-15 Carrier Used as Catalyst for Selective Oxidation of Toluene
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SBA-15载体固定NDHPI的新方法用作甲苯选择性氧化催化剂

DOI:
10.1007/s10562-015-1635-z
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发表时间:
2016-02
期刊:
影响因子:
2.8
通讯作者:
Luo He'an
Luo He'an
中科院分区:
化学4区
文献类型:
--
作者:
Zhou Meng;Li Xingxing;Bao Li;Yuan Xia;Luo He'an

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摘要通过将N,N-二羟基均苯四酰亚胺(NDHPI)与预接枝的缩水甘油氧丙基-SBA-15分子筛的缩水甘油氧丙基链偶联,制备了介孔分子筛SBA-15固载NDHPI。为了比较,还采用浸渍法制备了SBA-15固定化N-羟基邻苯二甲酰亚胺(NHPI)。采用傅里叶变换红外光谱、N2吸附-脱附、热重分析、X射线衍射、扫描电镜、透射电镜和X射线光电子能谱等手段对催化剂进行了表征。将该催化剂和N,N-双(水杨醛)乙二胺钴(Cosalen)配合物用于甲苯分子氧氧化反应。NDHPI与SBA-15偶联的固定化催化剂活性更高,可重复使用,在90 °C反应7 h,苯甲醛和苯甲醇的总选择性提高到46.0%,甲苯转化率为14.8%。图示摘要采用新方法制备了介孔分子筛SBA-15固定化N,N-二羟基均苯四酰亚胺(NDHPI),这是通过NDHPI与缩水甘油氧基丙基-SBA-15的预接枝缩水甘油氧基丙基链的偶联来实现的。采用浸渍法制备了SBA-15固定化NHPI。对它们的结构进行了表征,并比较了它们与Cosalen配合物在甲苯分子氧化反应中的催化性能。并讨论了它们的复用性能。
AbstractMesoporous molecular sieve SBA-15 immobilizedN,N-dihydroxypyromellitimide (NDHPI) was prepared by a new method, which was realized through the coupling NDHPI with pre-grafted glycidoxypropyl chains of glycidoxypropyl-SBA-15. SBA-15 immobilizedN-hydroxyphthalimide (NHPI) by impregnation method was also prepared for comparison. The two catalysts were characterized by Fourier transform infrared spectroscopy, N2adsorption–desorption technique, thermogravimetric analyses, X-ray diffraction, scanning electron microscope, transmission electron microscope and X-ray photoelectron spectroscopy. Then the catalysts andN,N-bis(salicylidene) ethylenediiminocobalt (Cosalen) complex were used into oxidation of toluene with molecular oxygen. The more active and reusable catalyst was the immobilized one coupled by NDHPI with glycidoxypropyl-SBA-15, which improved the total selectivity of benzaldehyde and benzyl alcohol to 46.0 % with the conversion of toluene 14.8 % at 90 °C for 7 h.Graphical AbstractMesoporous molecular sieve SBA-15 immobilizedN,N-dihydroxypyromellitimide (NDHPI) was prepared by a new method, which was realized through the coupling NDHPI with pre-grafted glycidoxypropyl chains of glycidoxypropyl-SBA-15. SBA-15 immobilized NHPI by impregnation method was also prepared for comparison. Their structure was characterized and their catalytic performance combined with Cosalen complex in the molecule oxidation of toluene were compared. Their reusability performance was also discussed.
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