载体性质对Pd催化剂加氢脱硫性能的影响

发布时间：2018-09-08 21:10

【摘要】：以Si O2、全硅MCM-41(Si-MCM-41)、通过机械混合Si-MCM-41与ZSM-5得到的Z-MCM-41-M以及通过在ZSM-5外部包覆MCM-41制备得到的Z-MCM-41四种材料为载体,制备了四种负载型Pd催化剂。采用XRD、HRTEM、N2吸附-脱附、NH3-TPD手段对Pd催化剂进行了表征;以二苯并噻吩(DBT)为模型化合物,在固定床反应器上对四种催化剂的加氢脱硫(HDS)活性、加氢路径选择性和加氢裂化活性进行了考察,研究了不同类型载体对Pd催化剂加氢脱硫性能的影响。结果表明,载体的性质会显著影响负载型Pd催化剂的加氢脱硫性能。载体的比表面积对负载型Pd催化剂加氢脱硫活性影响不大,但是HYD路径的选择性与载体的孔道结构有关;具有介孔孔道结构有利于加氢路径选择性的提高。酸性载体负载的Pd催化剂表现出较好加氢脱硫活性和加氢选择性,这与氢溢流有关。介孔材料的孔道结构与微孔沸石的酸性有机结合,所得到的Z-M CM-41复合材料是是潜在的贵金属Pd加氢脱硫催化剂优良载体,可有效提升其加氢脱硫活性。
[Abstract]:Four kinds of supported Pd catalysts were prepared on the support of Si O _ 2, all-silicon MCM-41 (Si-MCM-41), Z-MCM-41-M obtained by mechanically mixing Si-MCM-41 with ZSM-5 and Z-MCM-41 prepared by coating ZSM-5 with MCM-41. The XRD,HRTEM,N2 adsorption-desorption NH _ 3-TPD method was used to characterize the Pd catalyst, and the hydrodesulfurization (HDS) activity of the four catalysts was studied in a fixed-bed reactor using dibenzothiophene (DBT) as a model compound. The hydrogenation path selectivity and hydrocracking activity were investigated and the effects of different kinds of supports on the hydrodesulfurization performance of Pd catalysts were studied. The results showed that the properties of the support significantly affected the hydrodesulfurization performance of the supported Pd catalyst. The specific surface area of the support has little effect on the hydrodesulfurization activity of the supported Pd catalyst, but the selectivity of the HYD path is related to the pore structure of the carrier, and the mesoporous structure is conducive to the improvement of the hydrogenation path selectivity. The hydrodesulfurization activity and hydrogenation selectivity of the Pd catalyst supported on acid carrier are better, which is related to the hydrogen overflow. The pore structure of mesoporous materials is combined with the acidity of microporous zeolites. The Z-M CM-41 composite is an excellent carrier for potential noble metal Pd hydrodesulfurization catalysts, which can effectively enhance its hydrodesulfurization activity.
【作者单位】：中国石油石油化工研究院大庆化工研究中心;
【基金】：中国石油天然气股份公司基金(2013E-1502、2014B-2508)资助~~
【分类号】：TE624.9

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