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机构地区:[1]东北石油大学化学化工学院 石油与天然气化工省重点实验室,黑龙江大庆163318
出 处:《物理化学学报》2010年第9期2461-2467,共7页Acta Physico-Chimica Sinica
基 金:黑龙江省科技厅(2009G0947-00)资助项目~~
摘 要:采用溶胶-凝胶法制备了TiO2-Al2O3复合载体,采用浸渍法制备了Ni2P/TiO2-Al2O3催化剂,并用X射线衍射(XRD)、N2吸附比表面积(BET)测定、热重-差热分析(TG-DTA)、X射线光电子能谱(XPS)等技术对催化剂的结构和性质进行了表征.催化剂加氢脱硫(HDS)和脱氮(HDN)活性评价在实验室固定床连续反应装置上,以噻吩和吡啶为模型反应物进行.考察了不同载体、Ni2P负载量、标称Ni/P摩尔比、催化剂焙烧温度对Ni2P/TiO2-Al2O3催化剂上同时进行的噻吩加氢脱硫和吡啶加氢脱氮性能的影响.结果表明,TiO2含量为80%(w)的TiO2-Al2O3复合氧化物为载体,Ni2P负载量为30.0%(w),标称Ni/P摩尔比为1/2,催化剂焙烧温度为500℃时,Ni2P/TiO2-Al2O3催化剂加氢脱硫脱氮活性最高.在360℃,3.0MPa,氢油比800(V/V),液时体积空速1.5h-1的条件下,噻吩HDS和吡啶HDN转化率分别为61.32%和64.43%.We prepared a TiO2-Al2O3 complex support by the sol-gel method.A nickel phosphide catalyst,Ni2P/ TiO2-Al2O3,was prepared by the impregnation method.The catalysts were characterized by X-ray diffraction(XRD),N2-adsorption specific surface area measurements(BET),thermogravimetry-differential thermal analysis(TG-DTA),and X-ray photoelectron spectroscopy(XPS).The catalysts were evaluated using a lab-scale continuous flow fixed-bed reactor for simultaneously hydrodesulfurization(HDS) and hydrodenitrogenation(HDN) of thiophene and pyridine.The effects of different supports,Ni2P loading,Ni/P molar ratio,and calcination temperature on catalyst activity for the HDS and HDN were studied.The catalytic activity of the Ni2P/TiO2-Al2O3 catalyst with a TiO2 mass fraction of 80%,a Ni2P loading of 30.0%(w),a Ni/P molar ratio of 1/2 as well as a calcination temperature of 500℃ was found to be optimal.At a reaction temperature of 360℃,a pressure of 3.0 MPa,a hydrogen/oil ratio of 800(V/V),and a liquid hourly space velocity of 1.5 h-1,the conversion of thiophene HDS and pyridine HDN were 61.32% and 64.43%,respectively.
关 键 词:磷化二镍 二氧化钛 三氧化二铝 加氢脱硫 加氢脱氮
分 类 号:TE624.9[石油与天然气工程—油气加工工程]
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