纳米孔壳聚糖固载四(p-磺酸基苯基)铁卟啉催化氧化乙苯  

Catalytic oxidation of ethylbenzene by iron tetrakis( p-sulphophenyl) porphyrin grafted to nano porous chitosan

作　　者：卫炎勋 黄冠[1] 刘垚[1] 陈祥凤[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5期1284-1291,共8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：为了模拟细胞色素P-450酶催化活性空腔,最大发挥固载金属卟啉的催化活性功能。研究以纳米孔壳聚糖微球(np-CTS)作为载体,通过离子键接枝四(p-磺酸基苯基)铁卟啉(Fe TPPSO3H),制备相关的纳米孔壳聚糖固载金属卟啉仿生催化材料(Fe TPPSO3-H3+N-np-CTS)。采用紫外可见光谱(UV-Vis)、傅里叶红外光谱(FT-IR)、X-射线衍射技术(XRD)、差热分析技术(TG),比表面测试(BET)和扫描电镜技术(SEM)对该催化材料进行形态与结构的表征。研究其催化氧化乙苯性能。实验结果表明:在最佳的温度(140℃),压力(0.8 Mpa)和1 mg的催化剂(Fe TPPSO3H)用量反应条件下,催化剂可再重复使用4次,平均的乙苯转化率为52.72%,选择性为63.85%,醇酮产率为33.67%,催化剂转化数为3.39×106。与相应无孔的壳聚糖固载金属卟啉仿生催化材料及未固载金属卟啉的催化性能相比,其催化氧气氧化乙苯生成主要产物的收率分别提高9.54%和2.40%。这表明纳米孔壳聚糖固载四(p-磺酸基苯基)铁卟啉催化剂材料,具有更好的催化性能。In order to mimic the catalytic activity cavacity of cytochrome P-450 enzyme and display the best catalytic performance of the supported iron tetrakis （p-sulphophenyl）porphyrin（ Fe TPPSO3 H） , nano porous chitosan （np-CTS） was used to graft the metalloporphyrins by ionic bonds, forming an iron tetrakis （p-sulphophenyl）porphyrin grafted to nano porous chitosan （ Fe TPPSO3- H3 ＊N-np- CTS）. The mimicking catalyst material was charactierized by UV-Vis and FT-IR spectra, X-ray dif- fraction（XRD） pattern, Thermoanalyser（TG）, Bmnauer Enmet Teller （BET）surface area analysis and Scaning Electron Microscope （SEM）. The catalytic performance for ethylbenzene oxidation over the Fe TPPSO3-H3＋ N-np-CTS was studied. The experimental results indicate that the only amount of 1 mg Fe TPPSO3 H grafted in np-CTS, the such supported catalyst can be reused for 4 times in the ethylbenzene oxidation, on everage, with 43.27% of ethylbenzene conversion, 27.88% of yields and 64. 31% of selectivity （alcohol and ketone）, and the catalyst turnover number of 3.40 × 106, under the optimal reaction conditions of 140℃ and 0. 8 MPa oxygen pressure. Compared with the yields of main products from the oxidation of ethylbenzene over the correspongding Fe TPPSO3- H3- N-nonp-CTS and Fe TPPSO3H, those from the Fe TPPSO3-H3＋N-np-CTS have elevated 6. 16% and 1.15% , respectively. It shows that the catalyst material has a better catalytic performance.

关 键 词：纳米孔壳聚糖 四(p-磺酸基苯基)铁卟啉 催化氧化乙苯 

分 类 号：O643.3[理学—物理化学]