纳米孔壳聚糖接枝四(对-羧基苯基)锰卟啉催化氧化乙苯  

Catalysis of nan-porous chitosan grafted manganese tetra(p-carboxylphenyl) porphyrin for oxidation of ethylbenzene

作　　者：曾凯[1] 黄冠[1] 原汝迅 王未来[1] 郭勇安[1] 赵树凯[1] 

机构地区：[1]广西大学化学化工学院,广西南宁530004

出　　处：《广西大学学报（自然科学版）》2015年第3期505-513,共9页Journal of Guangxi University（Natural Science Edition）

基　　金：国家自然科学基金资助项目(51363001);广西科技攻关项目(桂科攻12118008-12-3);广西自然科学基项目(2012GXNSFAA053016和2014GXNSFDA118009);广西大学实验建设与实验教学改革项目基金资助(20120322)

摘　　要：为模拟细胞色素P-450酶的催化空腔场所,提高壳聚糖接枝四(对-羧基苯基)锰卟啉(Mn TCPP)的催化活性。采用冷冻干燥法制备纳米孔壳聚糖(np-CTS),并用酰化反应接枝四(对-羧基苯基)锰卟啉获得仿生催化材料―Mn TCPP/np-CTS,同时制备相应的无孔催化材料―Mn TCPP/nonp-CTS。用紫外可见光谱(UV-vis),傅里叶变换红外光谱(FT-IR),X射线(XRD),热重分析(TG)和扫描电镜(SEM)技术对其进行表征,并用于催化空气氧化乙苯研究。催化结果表明:在最佳反应条件下(145℃,0.8 MPa),纳米孔壳聚糖接枝四(对-羧基苯基)锰卟啉比无孔催化材料催化活性提高26%,醇酮收率提高38%。实验结果表明:纳米级空腔有利于充分发挥所固载的锰卟啉催化活性,最大程度地提高固载仿生催化材料的催化效率。To mimic the catalytic cavity site of Cytochrome P-450 enzyme, promoting the activity of chitosan grafted manganese tetra （ p-carboxylphenyl ） porphyrin （ Mn TCPP ） . Nan-porous chitosan （ np-CTS） was prepared by freeze drying method, to which was the Mn TCPP grafted by acylation, forming biomimetic catalytic material, Mn TCPP/ np-CTS. Non-porous chitosan grafted manganese tetra（ p-carboxylphenyl） porphyrin（ Mn TCPP/nonp-CTS） was prepared by a similar procedure. The materials were characterized by UV-Vis and FT-IR spectra, X-ray diffraction（ XRD） pattern, ther-moanalyser（ TG） and transmission electron microscope （ SEM） . The materials were used as a cata-lyst for an oxidation of ethylbenzene. The experimental results show that under an optimum oxidation conditions（145 ℃ and 0. 8 MPa） , the catalytic actvitiy of Mn TCPP/ np-CTS was 26% greater than＆amp;nbsp;that of Mn TCPP/ nonp-CTS, the yields （ keton and alcohol） of ethylbenzene oxidation over the for-mer was 38% greater than that over the latter. This indicates that the nano cavity in CTS benifite to fully displaying the catalytic activity of the CTS-grafted Mn TCPP and elevating the catalytic efficen-cy of the biomimetic catalytic material.

关 键 词：壳聚糖 接枝 四(对-羧基苯基)锰卟啉 氧化 乙苯 

分 类 号：O643.3[理学—物理化学]