In the coke oven gas to methanol(CTM) process, boiling water(above 200 ℃) is generally used as the coolant in the methanol synthesis reactor, and thus, medium-pressure steam is generated as a by-product. In this pape...In the coke oven gas to methanol(CTM) process, boiling water(above 200 ℃) is generally used as the coolant in the methanol synthesis reactor, and thus, medium-pressure steam is generated as a by-product. In this paper, the influence of the coolant temperature on the CTM process is investigated from two aspects, which are the performance analyses of the reactor and the overall process and the energy integration of by-product steam. The results reveal that the coolant temperature plays a key role in the CTM process optimization. When the coolant temperature is reduced to 187 ℃, though low-pressure steam is generated, the techno-economic performance of the whole process is greatly improved: the energy/exergy efficiency is increased by 4-9%, energy cost is saved by 37.1%, income is increased by 5.4 M$/year, and the C02 emission is reduced by 21.3%.展开更多
Producing methanol from coke oven gas(COG) is one of the important applications of COG. Removal of sulfur from COG is a key step of this process. Conversion and reaction kinetics over a commercial Fe-Mo/Al2O3 catalyst...Producing methanol from coke oven gas(COG) is one of the important applications of COG. Removal of sulfur from COG is a key step of this process. Conversion and reaction kinetics over a commercial Fe-Mo/Al2O3 catalyst(T-202) were studied in a continuous flow fixed bed reactor under pressures of 1.6-2.8 MPa, space time of 1.32-3.55 s and temperatures of 240-360 °C. Though the COG contains about 0.6 mol/mol H2, hydrogenation of CO and CO2 is not significant on this catalyst. The conversions of unsaturated hydrocarbons depend on their molecular structures. Diolefins and alkynes can be completely hydrogenated even at relatively low temperature and pressure. Olefins, in contrast, can only be progressively hydrogenated with increasing temperature and pressure. The hydrodesulfurization(HDS) of CS2 on this catalyst is easy. Complete conversion of CS2 was observed in the whole range of the conditions used in this work. The original COS in the COG can also be easily converted to a low level. However, its complete HDS is difficult due to the relatively high concentration of CO in the COG and due to the limitation of thermodynamics. H2 S can react with unsaturated hydrocarbons to form ethyl mercaptan and thiophene, which are then progressively hydrodesulfurized with increasing temperature and pressure. Based on the experimental observations, reaction kinetic models for the conversion of ethylene and sulfur-containing compounds were proposed; the values of the parameters in the models were obtained by regression of the experimental data.展开更多
Perovskite-type oxygen-permeable membrane reactors of BaCo0.7Fe0.2Nb0.1O3-δ （BCFNO） packed with Ru-based catalyst had high oxygen permeability and could be used for hydrogen production by partial oxidation of metha...Perovskite-type oxygen-permeable membrane reactors of BaCo0.7Fe0.2Nb0.1O3-δ （BCFNO） packed with Ru-based catalyst had high oxygen permeability and could be used for hydrogen production by partial oxidation of methane in coke oven gas （COG）. At 1173 K, 94% of methane conversion, 85% of H2 selectivity, 107% of CO selectivity, and as high as 15.4 mL·cm^-2·min^-1 of oxygen permeation flux were obtained. The BCFNO membrane itself had poor catalytic activity to partial oxidation of CH4 in COG. During continuous operation for 70 h at 1173 K, no degradation of the membrane reaction performance was observed. XRD and SEM characterization also demonstrated that the BCFNO membrane reactor exhibited good stability in partial oxidation of methane in COG.展开更多
The effects of factors such as the molar ratio of H2O to CH4 (n(H2O)/n(CH4)), methane conversion temperature and time on methane conversion rate were investigated to build kinetic model for reforming of coke-oven gas ...The effects of factors such as the molar ratio of H2O to CH4 (n(H2O)/n(CH4)), methane conversion temperature and time on methane conversion rate were investigated to build kinetic model for reforming of coke-oven gas with steam. The results of experiments show that the optimal conditions for methane conversion are that the molar ratio of H2O to CH4 varies from 1.1 to 1.3 and the conversion temperature varies from 1 223 to 1 273 K. The methane conversion rate is more than 95% when the molar ratio of H2O to CH4 is 1.2, the conversion temperature is above 1 223 K and the conversion time is longer than 0.75 s. Kinetic model of methane conversion was proposed. All results demonstrate that the calculated values by the kinetic model accord with the experimental data well, and the error is less than 1.5%.展开更多
The sensitivity analysis of a polygeneration energy system fueled with duo fuel of coke oven gas and coal gas is performed in the study,and the focus is put on the relations among syngas composition,conversation rate ...The sensitivity analysis of a polygeneration energy system fueled with duo fuel of coke oven gas and coal gas is performed in the study,and the focus is put on the relations among syngas composition,conversation rate and performance.The impacts of the system configuration together with the fuel composition on the performance are investigated and discussed from the point of cascading utilization of fuel chemical energy.First,the main parameters affecting the performance are derived along with the analysis of the system configuration and the syngas composition.After the performance is being simulated by means of the Aspen Plus process simulator of version 11.1,the variation of the performance due to the composition of syngas and the conversion rate of chemical subsystem is obtained and discussed.It is obtained from the result that the proper conversion rate of the chemical subsystem according to the specific syngas composition results in better performance.And the syngas composition affects the optimal conversion rate of the chemical subsystem,the optimal point of which is around the stoichiometric composition for methanol production(CO/H_(2)=0.5).In all,the polygeneration system fueled with coke oven gas and coal gas,which can realize the reasonable conversion of syngas to power and chemical product according to the syngas composition,is a promising method for coal energy conversion and utilization.展开更多
Steam-reforming is an effective approach for upgrading methane and hydrocarbon of coke-oven gas into CO and HE, but the kinetic behavior needs more study. We investigated the conversion of methane in coke-oven gas by ...Steam-reforming is an effective approach for upgrading methane and hydrocarbon of coke-oven gas into CO and HE, but the kinetic behavior needs more study. We investigated the conversion of methane in coke-oven gas by steam reforming process in an electric tubular flow at 14 kPa with temperature varying from .500 ℃ to 9.50 ℃, and developed a kenetic model for, ignoring the effects of adsorption and diffusion. The optimal dynamic conditions for methane conversion 14 kPa are as follows： the ratio of the amount of water to the amount of methane is from 1.1 to 1.3; the reaction temperature is from 1 223 K to 1 273 K. The methane conversion rate is larger than 95% when the ratio of the amount of water to the amount of methane is 1.2 at a temperature above 1 223 K with the residence time up to 0.75 s.展开更多
文摘In the coke oven gas to methanol(CTM) process, boiling water(above 200 ℃) is generally used as the coolant in the methanol synthesis reactor, and thus, medium-pressure steam is generated as a by-product. In this paper, the influence of the coolant temperature on the CTM process is investigated from two aspects, which are the performance analyses of the reactor and the overall process and the energy integration of by-product steam. The results reveal that the coolant temperature plays a key role in the CTM process optimization. When the coolant temperature is reduced to 187 ℃, though low-pressure steam is generated, the techno-economic performance of the whole process is greatly improved: the energy/exergy efficiency is increased by 4-9%, energy cost is saved by 37.1%, income is increased by 5.4 M$/year, and the C02 emission is reduced by 21.3%.
文摘Producing methanol from coke oven gas(COG) is one of the important applications of COG. Removal of sulfur from COG is a key step of this process. Conversion and reaction kinetics over a commercial Fe-Mo/Al2O3 catalyst(T-202) were studied in a continuous flow fixed bed reactor under pressures of 1.6-2.8 MPa, space time of 1.32-3.55 s and temperatures of 240-360 °C. Though the COG contains about 0.6 mol/mol H2, hydrogenation of CO and CO2 is not significant on this catalyst. The conversions of unsaturated hydrocarbons depend on their molecular structures. Diolefins and alkynes can be completely hydrogenated even at relatively low temperature and pressure. Olefins, in contrast, can only be progressively hydrogenated with increasing temperature and pressure. The hydrodesulfurization(HDS) of CS2 on this catalyst is easy. Complete conversion of CS2 was observed in the whole range of the conditions used in this work. The original COS in the COG can also be easily converted to a low level. However, its complete HDS is difficult due to the relatively high concentration of CO in the COG and due to the limitation of thermodynamics. H2 S can react with unsaturated hydrocarbons to form ethyl mercaptan and thiophene, which are then progressively hydrodesulfurized with increasing temperature and pressure. Based on the experimental observations, reaction kinetic models for the conversion of ethylene and sulfur-containing compounds were proposed; the values of the parameters in the models were obtained by regression of the experimental data.
基金supported by the National High-Tech Research and Development Program of China (No. 2006AA11A189)the Research on Novel Technology of Hydrogen Production from Oven Gas from Metallurgy Process (No. 07DZ12036)the National Key Technolo-gies Research and Development Program of China (No. 2006BA103A05)
文摘Perovskite-type oxygen-permeable membrane reactors of BaCo0.7Fe0.2Nb0.1O3-δ （BCFNO） packed with Ru-based catalyst had high oxygen permeability and could be used for hydrogen production by partial oxidation of methane in coke oven gas （COG）. At 1173 K, 94% of methane conversion, 85% of H2 selectivity, 107% of CO selectivity, and as high as 15.4 mL·cm^-2·min^-1 of oxygen permeation flux were obtained. The BCFNO membrane itself had poor catalytic activity to partial oxidation of CH4 in COG. During continuous operation for 70 h at 1173 K, no degradation of the membrane reaction performance was observed. XRD and SEM characterization also demonstrated that the BCFNO membrane reactor exhibited good stability in partial oxidation of methane in COG.
基金Project(291054) supported by Postdoctoral Fund of China
文摘The effects of factors such as the molar ratio of H2O to CH4 (n(H2O)/n(CH4)), methane conversion temperature and time on methane conversion rate were investigated to build kinetic model for reforming of coke-oven gas with steam. The results of experiments show that the optimal conditions for methane conversion are that the molar ratio of H2O to CH4 varies from 1.1 to 1.3 and the conversion temperature varies from 1 223 to 1 273 K. The methane conversion rate is more than 95% when the molar ratio of H2O to CH4 is 1.2, the conversion temperature is above 1 223 K and the conversion time is longer than 0.75 s. Kinetic model of methane conversion was proposed. All results demonstrate that the calculated values by the kinetic model accord with the experimental data well, and the error is less than 1.5%.
基金supported by the National Natural Science Foundation of China(Grant No.50706052)the State Key Development Program for Basic Research of China(Grant No.2005CB221207).
文摘The sensitivity analysis of a polygeneration energy system fueled with duo fuel of coke oven gas and coal gas is performed in the study,and the focus is put on the relations among syngas composition,conversation rate and performance.The impacts of the system configuration together with the fuel composition on the performance are investigated and discussed from the point of cascading utilization of fuel chemical energy.First,the main parameters affecting the performance are derived along with the analysis of the system configuration and the syngas composition.After the performance is being simulated by means of the Aspen Plus process simulator of version 11.1,the variation of the performance due to the composition of syngas and the conversion rate of chemical subsystem is obtained and discussed.It is obtained from the result that the proper conversion rate of the chemical subsystem according to the specific syngas composition results in better performance.And the syngas composition affects the optimal conversion rate of the chemical subsystem,the optimal point of which is around the stoichiometric composition for methanol production(CO/H_(2)=0.5).In all,the polygeneration system fueled with coke oven gas and coal gas,which can realize the reasonable conversion of syngas to power and chemical product according to the syngas composition,is a promising method for coal energy conversion and utilization.
基金the Postdoctoral Foundation of China under the grant No. 2910001
文摘Steam-reforming is an effective approach for upgrading methane and hydrocarbon of coke-oven gas into CO and HE, but the kinetic behavior needs more study. We investigated the conversion of methane in coke-oven gas by steam reforming process in an electric tubular flow at 14 kPa with temperature varying from .500 ℃ to 9.50 ℃, and developed a kenetic model for, ignoring the effects of adsorption and diffusion. The optimal dynamic conditions for methane conversion 14 kPa are as follows： the ratio of the amount of water to the amount of methane is from 1.1 to 1.3; the reaction temperature is from 1 223 K to 1 273 K. The methane conversion rate is larger than 95% when the ratio of the amount of water to the amount of methane is 1.2 at a temperature above 1 223 K with the residence time up to 0.75 s.
