A series of Al‐containing mesostructured cellular silica foams(Al‐MCFs)with different Si/Al molar ratios(x;x=10,20,30,40,or50)were prepared by a post synthetic method using aluminum isopropoxide as an alumina source...A series of Al‐containing mesostructured cellular silica foams(Al‐MCFs)with different Si/Al molar ratios(x;x=10,20,30,40,or50)were prepared by a post synthetic method using aluminum isopropoxide as an alumina source.The corresponding NiMo catalysts supported on Al‐MCFs were prepared and evaluated using dibenzothiophene(DBT)as the probe reactant.All the synthesized samples were characterized by small‐angle X‐ray scattering,scanning electron microscopy,nitrogen adsorption‐desorption,UV‐Vis diffuse reflectance spectroscopy,H2temperature‐programmed reduction,27Al MAS NMR,temperature‐programmed desorption of ammonia,pyridine‐FTIR,Raman spectroscopy,HRTEM,and X‐ray photoelectron spectroscopy to analyze their physicochemical properties and to gain a deeper insight of the interrelationship between the structures and the catalytic performance.The synthesis mechanism was proposed to involve the formation of Br?nsted acid and Lewis acid sites through the replacement of Si4+with Al3+.Aluminum introduced into MCFs by the post synthetic method has a negligible influence on the mesostructure of the parent MCFs but can form silicoaluminate materials with moderate Br?nsted acidity.For Al‐MCFs(x)materials,the detection of tetrahedrally coordinated Al3+cations demonstrated that the Al species had been successfully incorporated into the silicon frameworks.Furthermore,the DBT hydrodesulfurization(HDS)catalytic activity of the NiMo/Al‐MCFs(x)catalysts increased with increasing Si/Al molar ratio,and reached a maximum at a Si/Al molar ratio of20.The interaction of Ni and Mo species with the support became stronger when Al was incorporated into the MCFs supports.The high activities of the NiMo/Al‐MCFs catalysts for the DBT HDS were attributed to the suitable acidity properties and good dispersions of the Ni and Mo active phases.展开更多
Hydrodesulfurization(HDS)catalysts are widely used in petrochemical industries,playing a crucial role in desulfurization process to get high-quality oil.The generation of Al-based spent HDS catalyst is estimated to be...Hydrodesulfurization(HDS)catalysts are widely used in petrochemical industries,playing a crucial role in desulfurization process to get high-quality oil.The generation of Al-based spent HDS catalyst is estimated to be 1.2×105 tons per year around the world.The spent HDS catalysts have been regarded as an important secondary resource due to their abundant output,considerable metal value,and regeneration potential;however,if improperly handled,it would severely pollute the environment due to high content of heavy metals.Thus,the recovery of valuable metals from spent HDS catalysts is of great importance from both resource utilization and environmental protection points of view.In this work,recent advances in the spent HDS catalyst treatment technologies have been reviewed,focusing on the recovery of valuable transition metals and environmental impacts.Finally,typical commercial processes have been discussed,providing in-depth information for peer researchers to facilitate their future research work in designing more effective and environmentally friendly recycling processes.展开更多
This articles refers to the development of the technology for hydrodesulfurization (HDS) and aromatization of FCC naphtha This technology adopts a catalyst with aromatization performance, which does not reduce the oct...This articles refers to the development of the technology for hydrodesulfurization (HDS) and aromatization of FCC naphtha This technology adopts a catalyst with aromatization performance, which does not reduce the octane rating of gasoline in the course of HDS of FCC naphtha. Experimental results have shown that the sulfur removal rate of FCC naphtha could reach over 85%, with the RON of gasoline increased by 0.2-0.6 units, the MON increased by 1.3-1.8 units and the antiknock index of the gasoline increased by around one unit. The total C5+ liquid yield was over 95%. The activity of regenerated catalyst could be restored to be equal to that of fresh one after coke burning on the spent catalyst.展开更多
基金supported by National Natural Science Foundation of China (21276277,U1463207)CNOOC Project+1 种基金CNPC major projectthe Opening Project of Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology (2015K003)~~
文摘A series of Al‐containing mesostructured cellular silica foams(Al‐MCFs)with different Si/Al molar ratios(x;x=10,20,30,40,or50)were prepared by a post synthetic method using aluminum isopropoxide as an alumina source.The corresponding NiMo catalysts supported on Al‐MCFs were prepared and evaluated using dibenzothiophene(DBT)as the probe reactant.All the synthesized samples were characterized by small‐angle X‐ray scattering,scanning electron microscopy,nitrogen adsorption‐desorption,UV‐Vis diffuse reflectance spectroscopy,H2temperature‐programmed reduction,27Al MAS NMR,temperature‐programmed desorption of ammonia,pyridine‐FTIR,Raman spectroscopy,HRTEM,and X‐ray photoelectron spectroscopy to analyze their physicochemical properties and to gain a deeper insight of the interrelationship between the structures and the catalytic performance.The synthesis mechanism was proposed to involve the formation of Br?nsted acid and Lewis acid sites through the replacement of Si4+with Al3+.Aluminum introduced into MCFs by the post synthetic method has a negligible influence on the mesostructure of the parent MCFs but can form silicoaluminate materials with moderate Br?nsted acidity.For Al‐MCFs(x)materials,the detection of tetrahedrally coordinated Al3+cations demonstrated that the Al species had been successfully incorporated into the silicon frameworks.Furthermore,the DBT hydrodesulfurization(HDS)catalytic activity of the NiMo/Al‐MCFs(x)catalysts increased with increasing Si/Al molar ratio,and reached a maximum at a Si/Al molar ratio of20.The interaction of Ni and Mo species with the support became stronger when Al was incorporated into the MCFs supports.The high activities of the NiMo/Al‐MCFs catalysts for the DBT HDS were attributed to the suitable acidity properties and good dispersions of the Ni and Mo active phases.
基金financially supported by National Key Research and Development Program of China(Grant No.2020YFC1909703)S&T Program of Hebei(Grant Nos.20373808D and 206Z4401G)+1 种基金Fangchenggang Key R&D Program Grant No.AB20014008National Natural Science Foundation of China(Grant No.52074256)
文摘Hydrodesulfurization(HDS)catalysts are widely used in petrochemical industries,playing a crucial role in desulfurization process to get high-quality oil.The generation of Al-based spent HDS catalyst is estimated to be 1.2×105 tons per year around the world.The spent HDS catalysts have been regarded as an important secondary resource due to their abundant output,considerable metal value,and regeneration potential;however,if improperly handled,it would severely pollute the environment due to high content of heavy metals.Thus,the recovery of valuable metals from spent HDS catalysts is of great importance from both resource utilization and environmental protection points of view.In this work,recent advances in the spent HDS catalyst treatment technologies have been reviewed,focusing on the recovery of valuable transition metals and environmental impacts.Finally,typical commercial processes have been discussed,providing in-depth information for peer researchers to facilitate their future research work in designing more effective and environmentally friendly recycling processes.
文摘This articles refers to the development of the technology for hydrodesulfurization (HDS) and aromatization of FCC naphtha This technology adopts a catalyst with aromatization performance, which does not reduce the octane rating of gasoline in the course of HDS of FCC naphtha. Experimental results have shown that the sulfur removal rate of FCC naphtha could reach over 85%, with the RON of gasoline increased by 0.2-0.6 units, the MON increased by 1.3-1.8 units and the antiknock index of the gasoline increased by around one unit. The total C5+ liquid yield was over 95%. The activity of regenerated catalyst could be restored to be equal to that of fresh one after coke burning on the spent catalyst.