Mo-Ni_2P/SBA-15催化剂的制备、表征及加氢脱硫催化性能（英文）

Preparation, Characterization and Hydrodesulfurization Catalytic Performances of Mo-Ni_2P/SBA-15 Catalysts

以介孔分子筛SBA-15为载体,通过分步浸渍硝酸镍、磷酸氢二铵、钼酸铵,然后在H2气流下程序升温还原(H2-TPR),制备了一系列不同Mo含量的Mo-Ni2P/SBA-15催化剂.采用X射线衍射(XRD)、氮气吸脱附(BET)、透射电子显微镜(TEM)和X射线光电子能谱(XPS)对催化剂的结构进行了表征,评价了催化剂对二苯并噻吩(DBT)的加氢脱硫(HDS)活性.结果表明,Mo-Ni2P/SBA-15催化剂仍然保留有介孔结构,催化剂的物相主要是Ni2P.催化剂表面的Ni以Niδ+和Ni2+形式存在;P以Pδ-和P5+形式存在;Mo以Moδ+和Mo6+形式存在.Mo能促进催化性能的提高,其中Mo含量为1%(w,质量分数)的Mo-Ni2P/SBA-15催化剂具有最好的二苯并噻吩加氢脱硫催化活性,在反应温度为380°C,反应压力为3.0 MPa的条件下,二苯并噻吩的转化率可达99.03%,所有考察的Mo-Ni2P/SBA-15都以直接加氢脱硫(DDS)途径为主.

A series of Mo-Ni2P/SBA-15 catalysts with various Mo loadings were prepared by impregnating nickel nitrate, diammonium hydrogen phosphate, and ammonium molybdate onto an SBA-15 support, followed by temperature-programmed reduction（TPR） under H2. The structure of the catalysts was characterized by Xray diffraction（XRD）, N2adsorption-desorption, transmission electron microscopy（TEM）, and X-ray photoelectron spectroscopy（XPS）. The catalytic performance was evaluated in the hydrodesulfurization（HDS） of dibenzothiophene（DBT）. The results indicate that the mesoporous structure was maintained and the Ni2 P phase was present in all of the catalysts. The chemical states of Ni were Niδ^＋and Ni2^＋, the chemical states of P were Pδ-and P5^＋, and the chemical states of Mo were Moδ^＋and Mo6^＋. Mo was shown to promote the HDS catalytic performance of Ni2P/SBA-15 catalysts. The Mo-Ni2P/SBA-15 catalysts with 1%（w, mass fraction） Mo loading exhibited the highest HDS activity. The conversion of the DBT reached 99.03% under reaction conditions of 380 °C and 3.0 MPa. The HDS of DBT proceeded mainly via the direct desulfurization（DDS） pathway over all of the tested Mo-Ni2P/SBA-15 catalysts.