多级孔道Ni-TS-1分子筛的原位合成及其脱硫性能  

In Situ Synthesis of Ni-TS-1 Molecular Sieves with Hierarchical Pores and Their Desulfurization Performances

作　　者：王广建[1] 褚衍佩 韩亚飞[1] 冯庆吉 王芳[1] 

机构地区：[1]青岛科技大学化工学院,山东青岛266042

出　　处：《石油化工》2015年第3期302-307,共6页Petrochemical Technology

基　　金：国家自然科学基金资助项目(21276130)

摘　　要：以硝酸镍为镍源、四丙基溴化铵为模板剂,通过一步法合成了多级孔道的Ni-TS-1分子筛,采用XRD、FTIR、UVVis和N2吸附-脱附等方法对Ni-TS-1分子筛进行了表征,并分别以噻吩、苯并噻吩和二苯并噻吩为模型硫化物、双氧水为氧化剂对Ni-TS-1分子筛的催化氧化脱硫性能进行了研究。实验结果表明,金属Ni的引入没有改变TS-1分子筛的骨架结构,其骨架仍为MFI拓扑结构;与传统方法制备的TS-1分子筛相比,Ni-TS-1分子筛在超微孔和介孔范围内有次生孔存在,且具有更大的BET比表面积和平均孔径,在氧化脱除模型硫化物时不受空间位阻的限制,对噻吩、苯并噻吩和二苯并噻吩均具有较好的催化效果;n(Si)∶n(Ni)=40的Ni-TS-1分子筛在重复使用6次后,二苯并噻吩的脱除率仍保持在90%以上。Ni-TS-1 molecular sieves with hierarchical structure were synthesized by a one step method with nickel nitrate as the nickel source and tetraisopropyl bromide as template, and characterized by means of XRD, FTIR, UV-Vis and N2 adsorption-desorption. The catalytic performances of Ni-TS-1 in the oxidative desulfurization of n-octane containing thiophene, benzothiophene or dibenzothiophene with hydrogen peroxide as the oxidant were studied. The results showed that the introduction of nickel did not change the MFI topological structure of TS-1. Compared with the traditional preparation method for TS-1, NiTS-1 had secondary pores with supermicro-mesopore structure, big BET specific surface area and big average pore diameter. Ni-TS-1 was not affected by steric hindrance in the oxidative desulfurization and exhibited good removal performances for thiophene, benzothiophene and dibenzothiophene. After Ni-TS-1 was reused 6 times, the dibenzothiophene removal rate still reached more than 90%.

关 键 词：Ni-TS-1分子筛 催化剂 氧化脱硫 噻吩 

分 类 号：TQ426[化学工程]