介孔材料中甲基三氧化錸和氯化鎳的組裝及對烯烴氧化反應的催化性能.pdf

1、河北工業(yè)大學碩士學位論文介孔材料中甲基三氧化錸和氯化鎳的組裝及對烯烴氧化反應的催化性能姓名：丁春浦申請學位級別：碩士專業(yè)：應用化學指導教師：趙繼全2011-03介孔材料中甲基三氧化錸和氯化鎳的組裝及對烯烴氧化反應的催化性能 ii ASSEMBLY OF METHYLTRIOXORHENIUM AND NICKEL CHLORIDE ON MCM-41 AND THEIR CATALYTIC PERFORMANCES ON THE OXI

2、DATION OF ALKENES ABSTRACT Three di-nitrogen schiff base ligands were synthesized by the condensation of 2-pyridinecarboxaldehyde with aniline and its derivatives and their structures were characterized by FT-IR、1H NMR、

3、13C NMR. The effects of the in situ coordination of methyltrioxorhenium (MTO) with schiff bases on the epoxidation of alkenes with 30% H2O2 as oxidant were studied. The results revealed that the ligand with an electron-w

4、ithdrawing carboxy group has suitable coordination capacity and acidity, therefore, it can largely increase the selectivity of epoxides without concomitancy of the obvious decrease of reaction rate in the epoxidation of

5、olefins catalyzed by MTO. For example, when the molar ratio of the schiff base I to MTO was 2 and the reaction was run at 10 oC for 4 h, the conversion of cyclohexene and the selectivity of the epoxide reached 94.6% a

6、nd 99.0%, respectively. However, the ligands without electron-withdrawing group decreased the catalytic activity of MTO, though they could increase the selectivity of epoxides in some degree. MCM-41 reacted with b

7、is(3-(triethoxysilyl)propyl)amine to give MCM-41-I which was functionalized with amino groups. Then the dinitrogen schiff base ligand was attached to MCM-41-I by employing amidation reaction to give MCM-41-II. The dinit

8、rogen schiff base ligand supported on MCM-41 coordinated with MTO to bring about assembling of MTO on MCM-41, which give the heterogenized catalyst. The catalyst was characterized by means of FT-IR, DR UV-vis, XRD, N2 ad

9、sorption and atomic absorption analysis. The catalytic experimental results showed that the heterogenized catalyst has poor catalytic performance in the epoxidation of alkenes with aqueous 30% H2O2 as oxidant. Nickel ch