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Synthesis of highly selective and stable mesoporous Ni–Ce/SAPO-34 nanocatalyst for methanol-to-olefin reaction: Role of polar aprotic N,N-dimethylformamide solvent
Particuology ( IF 4.1 ) Pub Date : 2018-02-21 , DOI: 10.1016/j.partic.2017.11.004
Hossein Akhoundzadeh , Majid Taghizadeh , Hassan Sharifi Pajaie

A series of mesoporous nanocrystalline silicoaluminophosphate (SAPO) zeolites (SAPO-34) were synthesized via an ultrasonic and microwave-assisted hydrothermal method in the presence of [3-(trimethoxysilyl)propyl]octadecyldimethylammonium chloride and cetyltrimethylammonium bromide surfactants as soft templates. Nickel and cerium were then doped on SAPO-34 using incorporation and impregnation methods, and all the catalysts were applied to the methanol-to-olefin (MTO) reaction. The catalysts were characterized using X-ray diffraction, field-emission scanning electron microcopy, inductively coupled plasma–atomic emission spectroscopy, transmission electron microscopy, Fourier-transform infrared spectroscopy, Brunauer–Emmett–Teller analysis, NH3 temperature-programmed desorption analysis, and thermogravimetric analysis. For the impregnation method, the effect of using protic or aprotic solvents as impregnation media on the physico-chemical properties of the metal-based SAPO-34 was investigated. Water and N,N-dimethylformamide (DMF) were employed as the protic and aprotic solvents, respectively. The catalyst prepared using the aprotic DMF solvent exhibited higher dispersion and lower aggregation of metal species compared with that prepared using the protic water solvent. Furthermore, the sample synthesized using the incorporation method exhibited good catalytic performance; however, the Ni–Ce/SAPO-34 sample prepared using the impregnation method and aprotic DMF solvent exhibited superior catalytic performance in the MTO reaction.



中文翻译:

用于甲醇-烯烃反应的高选择性且稳定的介孔Ni-Ce / SAPO-34纳米催化剂的合成:极性非质子传递NN-二甲基甲酰胺溶剂的作用

在[3-(三甲氧基甲硅烷基)丙基]十八烷基二甲基氯化铵和十六烷基三甲基溴化铵表面活性剂作为软模板存在下,通过超声和​​微波辅助水热法合成了一系列介孔纳米晶体硅铝磷酸盐(SAPO-34)沸石。然后使用掺入和浸渍方法将镍和铈掺杂在SAPO-34上,并将所有催化剂应用于甲醇制烯烃(MTO)反应。使用X射线衍射,场发射扫描电子显微镜,电感耦合等离子体-原子发射光谱,透射电子显微镜,傅里叶变换红外光谱,Brunauer-Emmett-Teller分析,NH 3表征催化剂。程序升温解吸分析和热重分析。对于浸渍方法,研究了使用质子或非质子溶剂作为浸渍介质对基于金属的SAPO-34的物理化学性质的影响。水和Ññ-二甲基甲酰胺(DMF)分别用作质子和非质子溶剂。与使用质子性水溶剂制备的催化剂相比,使用非质子性DMF溶剂制备的催化剂表现出更高的分散度和更低的金属种类聚集。此外,采用掺入法合成的样品具有良好的催化性能。但是,使用浸渍法和非质子传递性DMF溶剂制备的Ni-Ce / SAPO-34样品在MTO反应中表现出优异的催化性能。

更新日期:2018-02-21
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