摘要
Ni_2P/ZrO_2-SBA-15 catalysts with different zirconium n-propoxide/SBA-15 mass ratios were synthesized to evaluate their dibenzothiophene hydrodesulfurization catalytic activity. Effect of ZrO_2 introduction was investigated. Supports and catalysts were characterized by BET,XRD,^(29)SiNMR,XPS and FTIR. The results indicated that zirconium was incorporated into SBA-15 in the forms of [(–O–)_2 Si(–O–Zr)_2 ] and/or [(–O–)_3 Si–O–Zr],and that the SBA-15 framework structure was maintained after incorporation of ZrO_2. With zirconium content increasing,ZrO_2 was transformed from amorphous phase to tetragonal phase. Zirconium incorporation into SBA-15 supports could facilitate to form more dispersed Ni_2P active phase. There might be some interaction occurring between the P and Zr species. In addition to Ni_2P,another kind of active phase,ZrP,was formed,which might exhibit a better HDS activity than Ni_2P. It was observed that at a temperature of 280 °C,pressure of 3.0 MPa,WHSV of 6.5 h^(-1) and H_2 to oil ratio of 450,the Ni_2P/Zr-SBA(1.5) catalyst,where 1.5 represents zirconium n-propoxide/SBA-15 mass ratio,showed the highest DBT conversion,which was 86.6%,almost 35% higher than that of the Ni_2P/Zr-SBA(0) catalyst.
Ni_2P/ZrO_2-SBA-15 catalysts with different zirconium n-propoxide/SBA-15 mass ratios were synthesized to evaluate their dibenzothiophene hydrodesulfurization catalytic activity. Effect of ZrO_2 introduction was investigated. Supports and catalysts were characterized by BET,XRD,^(29)SiNMR,XPS and FTIR. The results indicated that zirconium was incorporated into SBA-15 in the forms of [(–O–)_2 Si(–O–Zr)_2 ] and/or [(–O–)_3 Si–O–Zr],and that the SBA-15 framework structure was maintained after incorporation of ZrO_2. With zirconium content increasing,ZrO_2 was transformed from amorphous phase to tetragonal phase. Zirconium incorporation into SBA-15 supports could facilitate to form more dispersed Ni_2P active phase. There might be some interaction occurring between the P and Zr species. In addition to Ni_2P,another kind of active phase,ZrP,was formed,which might exhibit a better HDS activity than Ni_2P. It was observed that at a temperature of 280 °C,pressure of 3.0 MPa,WHSV of 6.5 h^(-1) and H_2 to oil ratio of 450,the Ni_2P/Zr-SBA(1.5) catalyst,where 1.5 represents zirconium n-propoxide/SBA-15 mass ratio,showed the highest DBT conversion,which was 86.6%,almost 35% higher than that of the Ni_2P/Zr-SBA(0) catalyst.
