二维层状H型丝光沸石的二甲醚羰基化性能  

Carbonylation of Dimethyl Ether over the Two-Dimensional Layered H-Mordenite

作　　者：牛君阳 刘亚华 董红文[1,2] 李新刚 

机构地区：[1]天津大学化工学院天津市应用催化科学与工程重点实验室,天津300072 [2]天津化学化工协同创新中心,天津300072

出　　处：《化学工业与工程》2015年第6期7-12,共6页Chemical Industry and Engineering

基　　金：国家自然科学基金(21476159;U1162103);教育部新世纪优秀人才支持计划(NCET-10-0615);教育部留学归国人员科研启动基金(2011-1568);天津大学绿色合成与转化教育部重点实验室开放基金

摘　　要：采用水热法合成了H型丝光沸石(H-MOR-S),考察了其二甲醚(DME)羰基化合成乙酸甲酯(MA)的活性,并与购买的商业H型丝光沸石(H-MOR-C)的羰基化活性进行比较。结果表明,水热法合成的样品H-MOR-S在180℃具有较高的DME羰基化活性,DME转化率可达到53.0%;但购买的样品H-MOR-C的DME转化率仅为20.5%。通过XRD和BET表征发现:样品H-MOR-S具有更大的比表面积,尤其是微孔比表面积和体积较大,其平均孔径为0.430 nm,接近八元环通道的大小,表明该样品中有更多八元环尺寸的通道,从而具有更多的DME吸附活性位,有助于提高催化剂的DME羰基化性能;通过SEM表征发现:样品H-MOR-S呈椭球状颗粒分布,每个颗粒由光滑二维平面成层状沿分子筛c轴方向整齐有序堆叠起来,提高了分子扩散速度,因而表现出较高的DME羰基化活性。The H-Mordenite( H-MOR) was prepared by a hydrothermal method. The catalytic activity of H-MOR upon carbonylation of dimethyl ether( DME) to methyl acetate( MA) was investigated and it was compared with the commercial H-Mordenite. Our results showed that the synthesized sample( HMOR-S) presented the higher catalytic carbonylation activity: the DME conversion reached 53. 0% after4. 5 h on stream at 180 ℃,while the DME conversion of the commercial sample( H-MOR-C) was only20. 5% under the same reaction conditions. The XRD and BET results demonstrate that the sample HMOR-S has the larger BET surface areas,and especially larger micropore surface areas and volumes. The average pore size of the H-MOR-S sample is close to the size of the eight-membered ring( 8-MR) channels in zeolites. It indicates the increased amount of the 8-MR channels in the H-MOR-S sample further improves the DME carbonylation activity. SEM images clearly show that the H-MOR-S sample is in the form of the ellipsoidal particles assembled of smoothly and orderly two-dimensional sheets. This morphology accelerates the diffusion rate of reactants,as well as products,in the c-axis direction,which thus en-hances the DME carbonylation activities.

关 键 词：水热法 H型丝光沸石 二维层状 二甲醚 羰基化 

分 类 号：O621.251[理学—有机化学]