A series of Mo-based catalysts prepared by sol-gel method using citric acid as complexant were successfully applied in the high efficient production of mixed alcohols from bio-syngas, derived from the biomass gasifica...A series of Mo-based catalysts prepared by sol-gel method using citric acid as complexant were successfully applied in the high efficient production of mixed alcohols from bio-syngas, derived from the biomass gasification. The Cu1Co1Fe1MO1Zn0.5-6%K catalyst exhibited a higher activity on the space-time yield of mixed alcohols, compared with the other Mobased catalysts. The carbon conversion significantly increases with rising temperature below 340 ℃, but the alcohol selectivity has an opposite trend. The maximum mixed alcohols yield derived from biomass gasification is 494.8 g/(kg catal·h) with the C2+ (C2-C6 higher alcohols) alcohols of 80.4% under the tested conditions. The alcohol distributions are consistent with the Schulz-Flory plots, except methanol. In the alcohols products, the C2+ alcohols (higher alcohols) dominate with a weight ratio of 70%-85%. The Mo-based cata- lysts have been characterized by X-ray diffraction and N2 adsorption/desorption. The clean bio-fules of mixed alcohols derived from bio-syngas with higher octane values could be used as transportation fuels or petrol additives.展开更多
Since the minimum-boiling azeotropes of C2-C8 alcohols with water and high-water content(up to 95%(mass))in the Fischer-Tropsch aqueous by-products,the separation is energy-intensive and challenging.The energy-saving ...Since the minimum-boiling azeotropes of C2-C8 alcohols with water and high-water content(up to 95%(mass))in the Fischer-Tropsch aqueous by-products,the separation is energy-intensive and challenging.The energy-saving strategy for the complete separation of the Fischer-Tropsch aqueous by-products has received massive attention in recent decades.In this study,a stripper-sidestream decanter process is proposed by exploiting homogeneous azeotropes(C2-C3 alcohols-water)and heterogeneous azeotropes(C4-C8 alcohols-water).The introduction of the stripping column for pre-dehydration avoids the revaporization of the mixture,and energy carried by the overhead vapor is conserved instead of being removed in a condenser.The precise fraction cutting of C1-C3 alcohol-water mixture,C4-C8 alcohols,and water is realized by the sidestream distillation column.The C4-C8 alcohols rich mixture withdrawn from the sidestream flows into the decanter to break the distillation boundary,where the organic phase returns to the sidestream distillation column to obtain the dehydrated C4-C8 alcohols,and the aqueous phase enters the stripping column.Steady-state optimization based on total annual cost(TAC)minimization shows that the stripper-sidestream decanter process reduces TAC by 17.00%and saves energy by 21.27%compared with the conventional three-column distillation process.Further,a control structure of the process is established,and dynamic simulations show that the control structure combining a differential controller with a low-selector exhibits robust co ntrol.This study provides a novel design scheme and deepens the insights into the efficient separation of aqueous by-products of the Fischer-Tropsch synthesis.展开更多
A series of molybdenum carbide catalysts promoted by potassium and cobalt,supported on carbon nanotubes(CNTs) were prepared by carbothermal hydrogen reduction method using CNTs as a carbon precursor.Firstly,molybden...A series of molybdenum carbide catalysts promoted by potassium and cobalt,supported on carbon nanotubes(CNTs) were prepared by carbothermal hydrogen reduction method using CNTs as a carbon precursor.Firstly,molybdenum and cobalt were loaded by co-precipitation method,and then potassium and additional molybdenum were impregnated to previous resultant.Different Mo/Co and K/Co molar ratio were used in catalyst synthesis.All the catalysts were characterized by ICP,BET,TEM,TPR,XRD and XPS,and the catalysts performances for higher alcohols synthesis(HAS) were investigated in a fixed-bed micro-reactor.The maximum selectivity to higher alcohols(C2+OH) was obtained at Mo/Co and K/Mo molar ratios of 1.66 and 0.6,respectively.XRD results confirmed the formation of K-Mo-C site and Co3Mo3 C phase that might play important role in producing C2+OH.展开更多
Porous carbon nanospheres have been widely used in different fields such as electric devices, catalysts, and water treatment. Here we will introduce a template-free process for the preparation of porous carbon nanosph...Porous carbon nanospheres have been widely used in different fields such as electric devices, catalysts, and water treatment. Here we will introduce a template-free process for the preparation of porous carbon nanospheres starting from a direct 3-aminophenol formaldehyde polymerization in a mixed solution. We identify that the addition of different alcohols, particularly ethanol and nbutanol, is able to change the growth habit of the polymer nanospheres and introduce a favorable inner compositional homogeneity for the preparation of porous structure. After the carbonization of the polymer nanospheres, the obtained porous carbon exhibits promising electrochemical performance when used as electrode material in super capacitor.展开更多
基金This work is supported Technical Research and by the National High Development Program (No.2009AA05Z435), the National Basic Research Program of Ministry of Science and Technology of China (No.2007CB210206), and the National Natural Science Foundation of China (No.50772107).
文摘A series of Mo-based catalysts prepared by sol-gel method using citric acid as complexant were successfully applied in the high efficient production of mixed alcohols from bio-syngas, derived from the biomass gasification. The Cu1Co1Fe1MO1Zn0.5-6%K catalyst exhibited a higher activity on the space-time yield of mixed alcohols, compared with the other Mobased catalysts. The carbon conversion significantly increases with rising temperature below 340 ℃, but the alcohol selectivity has an opposite trend. The maximum mixed alcohols yield derived from biomass gasification is 494.8 g/(kg catal·h) with the C2+ (C2-C6 higher alcohols) alcohols of 80.4% under the tested conditions. The alcohol distributions are consistent with the Schulz-Flory plots, except methanol. In the alcohols products, the C2+ alcohols (higher alcohols) dominate with a weight ratio of 70%-85%. The Mo-based cata- lysts have been characterized by X-ray diffraction and N2 adsorption/desorption. The clean bio-fules of mixed alcohols derived from bio-syngas with higher octane values could be used as transportation fuels or petrol additives.
文摘Since the minimum-boiling azeotropes of C2-C8 alcohols with water and high-water content(up to 95%(mass))in the Fischer-Tropsch aqueous by-products,the separation is energy-intensive and challenging.The energy-saving strategy for the complete separation of the Fischer-Tropsch aqueous by-products has received massive attention in recent decades.In this study,a stripper-sidestream decanter process is proposed by exploiting homogeneous azeotropes(C2-C3 alcohols-water)and heterogeneous azeotropes(C4-C8 alcohols-water).The introduction of the stripping column for pre-dehydration avoids the revaporization of the mixture,and energy carried by the overhead vapor is conserved instead of being removed in a condenser.The precise fraction cutting of C1-C3 alcohol-water mixture,C4-C8 alcohols,and water is realized by the sidestream distillation column.The C4-C8 alcohols rich mixture withdrawn from the sidestream flows into the decanter to break the distillation boundary,where the organic phase returns to the sidestream distillation column to obtain the dehydrated C4-C8 alcohols,and the aqueous phase enters the stripping column.Steady-state optimization based on total annual cost(TAC)minimization shows that the stripper-sidestream decanter process reduces TAC by 17.00%and saves energy by 21.27%compared with the conventional three-column distillation process.Further,a control structure of the process is established,and dynamic simulations show that the control structure combining a differential controller with a low-selector exhibits robust co ntrol.This study provides a novel design scheme and deepens the insights into the efficient separation of aqueous by-products of the Fischer-Tropsch synthesis.
文摘A series of molybdenum carbide catalysts promoted by potassium and cobalt,supported on carbon nanotubes(CNTs) were prepared by carbothermal hydrogen reduction method using CNTs as a carbon precursor.Firstly,molybdenum and cobalt were loaded by co-precipitation method,and then potassium and additional molybdenum were impregnated to previous resultant.Different Mo/Co and K/Co molar ratio were used in catalyst synthesis.All the catalysts were characterized by ICP,BET,TEM,TPR,XRD and XPS,and the catalysts performances for higher alcohols synthesis(HAS) were investigated in a fixed-bed micro-reactor.The maximum selectivity to higher alcohols(C2+OH) was obtained at Mo/Co and K/Mo molar ratios of 1.66 and 0.6,respectively.XRD results confirmed the formation of K-Mo-C site and Co3Mo3 C phase that might play important role in producing C2+OH.
基金supported by the National Natural Science Foundation of China(51672282,21373238)the Major State Basic Research Program of China(2013CB934000)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDA09010101)
文摘Porous carbon nanospheres have been widely used in different fields such as electric devices, catalysts, and water treatment. Here we will introduce a template-free process for the preparation of porous carbon nanospheres starting from a direct 3-aminophenol formaldehyde polymerization in a mixed solution. We identify that the addition of different alcohols, particularly ethanol and nbutanol, is able to change the growth habit of the polymer nanospheres and introduce a favorable inner compositional homogeneity for the preparation of porous structure. After the carbonization of the polymer nanospheres, the obtained porous carbon exhibits promising electrochemical performance when used as electrode material in super capacitor.