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作 者:魏妮[1] 季生福[1] 关月明[1] 刘辉[1] 李成岳[1]
机构地区:[1]北京化工大学化工资源有效利用国家重点实验室,北京100029
出 处:《石油学报(石油加工)》2011年第6期852-858,共7页Acta Petrolei Sinica(Petroleum Processing Section)
基 金:国家重点基础研究发展计划"973"项目(2006BC202503)资助
摘 要:以硝酸镍为镍源,磷酸氢二铵为磷源,介孔分子筛SBA-15为载体,采用共浸渍法制备Ni2P/SBA-15前驱体,再将一定量的偏钨酸铵水溶液引入,采用程序升温还原制备了一系列W-Ni2P/SBA-15催化剂。采用XRD、N2吸附-脱附、NH3-TPD和XPS表征了催化剂的结构,并评价了催化剂的二苯并噻吩加氢脱硫活性。结果表明,W-Ni2P/SBA-15催化剂中均只存在Ni2P物相;催化剂的比表面积和孔体积随着W含量的增加先增大后减小;强酸量和总酸量都随W含量的增加有明显增加;W的加入使得催化剂表面的Niδ+含量有所降低,而Pδ-含量有所增加;在大于360℃时,催化剂对二苯并噻吩具有很好的深度加氢脱硫活性,并且以直接脱硫生成联苯的脱硫机理为主。Ni2P/SBA-15 precursors were prepared by co-impregnation method with nickel nitrate as nickel source,ammonium hydrogen phosphate as phosphorus and mesopore molecular sieve SBA-15 as support.Then the W was introduced into the precursors and the W-Ni2P/SBA-15 precursors were converted into corresponding W-Ni2P/SBA-15 catalysts after temperature-programmed reduction in flowing H2.The structure of W-Ni2P/SBA-15 was characterized by XRD,N2 adsorption-desorption isotherms,NH3-TPD,and XPS.The catalytic activity of W-Ni2P/SBA-15 for the hydrodesulfurization of dibenzothiophene was evaluated.The result showed that only Ni2P phase was formed in the W-Ni2P/SBA-15.The specific surface area and the pore volume of W-Ni2P/SBA-15 increased then decreased when W content increased.Both the stronger acid sites and the total acid amount of W-Ni2P/SBA-15 obviously increased with the increase of W content,and so did the Niδ+ and the Pδ-content of the catalyst surface.W-Ni2P/SBA-15 catalysts exhibited good catalytic performance of deep hydrodesulfurization of dibenzothiophene over 360℃,in which the direct desulfurization was the main desulfurization mechanism.
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