SBA-15分子筛负载氮化碳催化二氧化碳与环氧化合物环加成反应  

Cycloaddition of carbon dioxide with epoxide catalyzed by SBA-15 molecular sieves loaded with graphitic carbon nitride

作　　者：柳士鑫 闫洪伟[2] 

机构地区：[1]中国石油集团东北炼化工程有限公司,辽宁沈阳110032 [2]中国石油天然气股份有限公司大庆石化公司,黑龙江大庆163714

出　　处：《工业催化》2015年第6期469-475,共7页Industrial Catalysis

摘　　要：二氧化碳的催化活化是其作为C1资源利用的关键。为了开发高效二氧化碳活化催化剂,将二聚氰胺通过浸渍法负载到介孔分子筛SBA-15孔道中,高温焙烧后,得到SBA-15负载的石墨相氮化碳g-C3N4催化剂。采用透射电镜、X射线衍射、N2吸附和X射线光电子能谱对催化剂进行表征。结果表明,负载g-C3N4后,SBA-15分子筛的介孔结构未发生明显变化,g-C3N4以纳米态分布于SBA-15分子筛的孔道中。将g-C3N4/SBA-15催化剂用于催化二氧化碳与环氧化合物环加成反应制备环状碳酸酯,考察催化剂组成和反应条件对催化性能的影响。结果表明,g-C3N4/SBA-15催化剂有效催化二氧化碳与环氧化合物环加成反应。以g-C3N4/SBA-15为催化剂,在反应温度140℃、反应压力3.5 MPa、反应时间4 h、Zn Br2物质的量分数为1.0%和二聚氰胺负载质量分数为20%条件下,环状碳酸酯产率达91.6%,g-C3N4/SBA-15催化剂制备工艺简单,原料价廉,催化性能优异。The catalytic activation of carbon dioxide is the key for its utilization as C1 resource. In order to develop efficient catalysts for the activation of carbon dioxide, dicyandiamide was loaded on the mesochannels of SBA-15 molecular sieve by impregnation method, and then after calcination, SBA-15 loaded graphitic carbon nitrlde （g-CaN4 ） catalysts were obtained. The catalysts were characterized by transmission electron microscopy, X-ray diffraction, N2 adsorption and X-ray photoelectron spectroscopy. The results showed that the mesoporous structure of SBA-15 molecular sieve had not changed significantly after loading g-C3N4. g-C3N4 nanophases were dispersed in the channels of SBA-15 molecular sieve, g-C3N4/SBA-15 catalyst was employed for the catalytic synthesis of cyclic carbonate from cycloaddition of carbon dioxide with epoxide. The effects of catalyst composition and the reaction conditions on catalytic performance were investigated. The results showed that g-C3N4/SBA-15 catalyst could effectively catalyze the cycloaddition of carbon dioxide with epoxide. Under the condition of reaction temperature 140 ℃, reaction pressure 3.5 MPa, reaction time 4 h,ZnBr2 amount 1.0mol%, dicyandiamide mass fraction 20% and g-C3N4/SBA-15 as the catalyst,cyclic carbonate yield reached 91.6%. g-C3N4/SBA-15 catalyst had the advantages of simple preparation process, cheap raw materials and excellent catalytic performance.

关 键 词：精细化学工程 二氧化碳 环加成 SBA-15分子筛 石墨相氮化碳 

分 类 号：TQ426.94[化学工程] O643.36[理学—物理化学]