The selective catalytic hydrogenation of naphthalene to high-value tetralin was systematically investigated.A series of Al2O3 catalysts containing different active metals(Co,Mo,Ni,W)were prepared by incipient wetness ...The selective catalytic hydrogenation of naphthalene to high-value tetralin was systematically investigated.A series of Al2O3 catalysts containing different active metals(Co,Mo,Ni,W)were prepared by incipient wetness impregnation.The effects of different active metals forms(oxidation,reduction,sulfuration)and reaction conditions on naphthalene hydrogenation were investigated and the catalysts were characterized by XRD,XPS,BET,NH3-TPD and SEM.Especially,Ni-Mo/Al2O3 was first used in this reactive system.The results show that the oxidative4%Ni O-20%MoO3/Al2O3 is the best catalyst for the preparation of tetralin.The conversion of naphthalene and the selectivity of tetralin can reach 95.62%and 99.75%respectively at 200℃,8 h and 6 MPa.Compared with reduced and sulfureted 4%Ni O-20%MoO3/Al2O3 catalysts,oxidative 4%Ni O-20%MoO3/Al2O3 has a well dispersed and uniform monolayer of the active metals,larger pore volume and size,and larger total acidity.NiO-MoO3/Al2O3 has a synergistic effect between NiO activity and MoO3 selectivity.展开更多
This work reports the enhancing effect of a highly cost effective and efficient metal, Fe, incorporation to Co or Ni based Mo/Al2O3 catalysts in the oxidative desulfurization （ODS） of dibenzothiophene （DBT） using ...This work reports the enhancing effect of a highly cost effective and efficient metal, Fe, incorporation to Co or Ni based Mo/Al2O3 catalysts in the oxidative desulfurization （ODS） of dibenzothiophene （DBT） using H2O2 and formic acid as oxidants. The influence of operating parameters i.e. reaction time, catalyst dose, reaction temperature and oxidant amount on oxidation process was investigated. Results revealed that 99% DBT conversion was achieved at 60℃ and 150 min reaction time over Fe-Ni-Mo/Al2O3. Fe tremendously enhanced the ODS activity of Co or Ni based Mo/Al2O3 catalysts following the activity order：Fe-Ni-Mo/Al2O3 〉 Fe-Co-Mo/Al2O3 〉 Ni-Mo/Al2O3 〉 Co-Mo/Al2O3, while H2O2 exhibited higher oxidation activity than formic acid over all catalyst systems. Insight about the surface morphology and textural properties of fresh and spent catalysts were achieved using scanning electron microscopy （SEM）, X-ray diffraction （XRD）, energy dispersive X-ray （EDX） analysis, Atomic Absorption Spectroscopy （AAS） and BET surface area analysis, which helped in the interpretation of experimental data. The present study can be deemed as an effective approach on industrial level for ODS of fuel oils crediting to its high efficiency, low process/catalyst cost, safety and mild operating condition.展开更多
基金supported by the Joint Funds of National Key R&D Program of China(2018YFB0604603)the National Natural Science Foundation of China(21536009,21776229)+2 种基金Science and Technology Plan Projects of Shaanxi Province(2017ZDCXL-GY-10-03,2018ZDXMGY-167)The Young Science and Technology Star Project of Shaanxi Province(2017KJXX-62)Science and Technology Program of Yulin(2018-2-22)。
文摘The selective catalytic hydrogenation of naphthalene to high-value tetralin was systematically investigated.A series of Al2O3 catalysts containing different active metals(Co,Mo,Ni,W)were prepared by incipient wetness impregnation.The effects of different active metals forms(oxidation,reduction,sulfuration)and reaction conditions on naphthalene hydrogenation were investigated and the catalysts were characterized by XRD,XPS,BET,NH3-TPD and SEM.Especially,Ni-Mo/Al2O3 was first used in this reactive system.The results show that the oxidative4%Ni O-20%MoO3/Al2O3 is the best catalyst for the preparation of tetralin.The conversion of naphthalene and the selectivity of tetralin can reach 95.62%and 99.75%respectively at 200℃,8 h and 6 MPa.Compared with reduced and sulfureted 4%Ni O-20%MoO3/Al2O3 catalysts,oxidative 4%Ni O-20%MoO3/Al2O3 has a well dispersed and uniform monolayer of the active metals,larger pore volume and size,and larger total acidity.NiO-MoO3/Al2O3 has a synergistic effect between NiO activity and MoO3 selectivity.
文摘This work reports the enhancing effect of a highly cost effective and efficient metal, Fe, incorporation to Co or Ni based Mo/Al2O3 catalysts in the oxidative desulfurization （ODS） of dibenzothiophene （DBT） using H2O2 and formic acid as oxidants. The influence of operating parameters i.e. reaction time, catalyst dose, reaction temperature and oxidant amount on oxidation process was investigated. Results revealed that 99% DBT conversion was achieved at 60℃ and 150 min reaction time over Fe-Ni-Mo/Al2O3. Fe tremendously enhanced the ODS activity of Co or Ni based Mo/Al2O3 catalysts following the activity order：Fe-Ni-Mo/Al2O3 〉 Fe-Co-Mo/Al2O3 〉 Ni-Mo/Al2O3 〉 Co-Mo/Al2O3, while H2O2 exhibited higher oxidation activity than formic acid over all catalyst systems. Insight about the surface morphology and textural properties of fresh and spent catalysts were achieved using scanning electron microscopy （SEM）, X-ray diffraction （XRD）, energy dispersive X-ray （EDX） analysis, Atomic Absorption Spectroscopy （AAS） and BET surface area analysis, which helped in the interpretation of experimental data. The present study can be deemed as an effective approach on industrial level for ODS of fuel oils crediting to its high efficiency, low process/catalyst cost, safety and mild operating condition.
