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机构地区:[1]中国石油大学重质油国家重点实验室CNPC催化重点实验室,山东青岛266580
出 处:《石油炼制与化工》2013年第9期19-24,共6页Petroleum Processing and Petrochemicals
基 金:国家重点基础研究发展计划"973"项目(2010CB226905);教育部自主创新科研计划新项目(14CX06032A);中国石油大学(华东)研究生创新工程项目(JD1112-11)
摘 要:采用水热反应法合成了一系列不同Ni、Mo比例的多孔Ni-Mo复合金属氧化物,用XRD,BET,SEM分析手段对其结构、孔性质等进行表征,并将Ni-Mo复合金属氧化物制备成Ni-Mo非负载型加氢催化剂,在连续流动高压微反装置上考察了其加氢脱硫、加氢脱氮和芳烃加氢饱和反应活性。结果表明,Ni-Mo复合金属氧化物具有钼酸镍铵晶相,而硫化态非负载型催化剂则具有MoS2和Ni3S2晶相,并且随着镍含量的增加,合成的Ni-Mo复合金属氧化物的比表面积和孔体积呈增加的趋势,而孔径则表现出双介孔的特征;当Ni、Mo摩尔比为1∶1时,制备的非负载型催化剂具有较高的催化反应性能,加氢脱硫率达到100%,加氢脱氮率和加氢饱和率分别达到62.3%和27.3%。The composite metal oxides with different Ni-Mo atomic ratio were synthesized by hydrothermal reaction and characterized by XRD,BET and SEM.The unsupported catalysts were prepared from the composite metal oxides and their activities of HDS,HDN and HYD were evaluated in a continuous flow high-pressure micro reactor.The results show that the composite metal oxides are mainly composed of ammonium nickel molybdate,while the phase of Ni3S2 and MoS2 are detected in the unsupported sulfided catalysts.N2 adsorption-desorption characterization indicate that the composite oxides exhibits the bimodal mesoporous structures,and the specific surface area and pore volume increase with increasing amount of basic nickel carbonate tetrahydrate.Catalytic results manifest that the unsupported Ni-Mo catalyst with the Ni-Mo ratio of 1∶1 has better hydrogenation activity: HDS rate of DBT is 100%,while HDN rate of quinoline and HYD of naphthalene reach 62.3% and 27.3%,respectively.
关 键 词:水热反应 超低硫柴油 加氢脱硫 非负载型催化剂 Ni-Mo复合金属氧化物
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