Flue gas and coal bed methane are two important sources of greenhouse gases.Pressure swing adsorption process has a wide range of application in the field of gas separation,and the selection of adsorbent is crucial.In...Flue gas and coal bed methane are two important sources of greenhouse gases.Pressure swing adsorption process has a wide range of application in the field of gas separation,and the selection of adsorbent is crucial.In this regard,in order to assess the better adsorbent for separating CO_(2) from flue gas and CH_(4) from coal bed methane,adsorption isotherms of CO_(2),CH_(4) and N_(2) on activated carbon and carbon molecular sieve are measured at 303.15,318.15 and 333.15 K,and up to 250 kPa.The experimental data fit better with Langmuir 2 compared to Langmuir 3 and Langmuir-Freundlich models,and Clausius-Clapeyron equation was used to calculate the isosteric heat.Both the order of the adsorbed amount and the adsorption heat on the two adsorbents are CO_(2)>CH_(4)>N_(2).The adsorption kinetics are calculated by the pseudo-first kinetic model,and the order of adsorption rates on activated carbon is N_(2)-CH_(4)>CO_(2),while on carbon molecular sieve,it is CO_(2)-N_(2)>CH_(4).It is shown that relative molecular mass and adsorption heat are the primary effect on kinetics for activated carbon,while kinetic diameter is the main resistance factor for carbon molecular sieve.Moreover,the adsorption selectivity of CH_(4)/N_(2) and CO_(2)/N_(2) were estimated with the ideal adsorption solution theory,and carbon molecular sieve performed best at 318.15 K for both CO_(2) and CH_(4) separation.The study suggested that activated carbon is a better choice for separating flue gas and carbon molecular sieve can be a strong candidate for separating coal bed methane.展开更多
The adsorption of CO2 on a raw activated carbon A and three modified activated carbon samples B, C, and D at temperatures ranging from 303 to 333 K and the thermodynamics of adsorption have been investigated using a v...The adsorption of CO2 on a raw activated carbon A and three modified activated carbon samples B, C, and D at temperatures ranging from 303 to 333 K and the thermodynamics of adsorption have been investigated using a vacuum adsorption apparatus in order to obtain more information about the effect of CO2 on removal of organic sulfur-containing compounds in industrial gases. The active ingredients impregnated in the carbon samples show significant influence on the adsorption for CO2 and its volumes adsorbed on modified carbon samples B, C, and D are all larger than that on the raw carbon sample A. On the other hand, the physical parameters such as surface area, pore volume, and micropore volume of carbon samples show no influence on the adsorbed amount of CO2. The Dubinin-Radushkevich (D-R) equation was the best model for fitting the adsorption data on carbon samples A and B, while the Freundlich equation was the best fit for the adsorption on carbon samples C and D. The isosteric heats of adsorption on carbon samples A, B, C, and D derived from the adsorption isotherms using the Clapeyron equation decreased slightly increasing surface loading. The heat of adsorption lay between 10.5 and 28.4 kJ/mol, with the carbon sample D having the highest value at all surface coverages that were studied. The observed entropy change associated with the adsorption for the carbon samples A, B, and C (above the surface coverage of 7 ml/g) was lower than the theoretical value for mobile adsorption. However, it was higher than the theoretical value for mobile adsorption but lower than the theoretical value for localized adsorption for carbon sample D.展开更多
Principal side factors as well as technical and procedural peculiarities capable of distorting the results of measurements of adsorbed and desorbed amounts, of falsifying the nature of the processes proceeding in the ...Principal side factors as well as technical and procedural peculiarities capable of distorting the results of measurements of adsorbed and desorbed amounts, of falsifying the nature of the processes proceeding in the systems under study, and of promoting artifacts in calorimetric and other studies of gas chemisorption on powders are considered. Modified techniques and procedures allowing the elimination of sources of side phenomena and artifacts and freeing traditional glass static adsorption apparatuses and experimental procedures from undesirable factors and peculiarities are proposed. Some available chemisorption and calorimetric data representing artifacts and also some data that are not artifacts but, due to imperfections of chemisorption techniques, show up as artifacts are presented and discussed. Several applications of the improved techniques and procedures to calorimetric and adsorption studies of the steps of catalytic processes proceeding on the basis of natural gas and of products of its processing are presented and discussed.展开更多
Coal-water interactions have profound influences on gas extraction from coal and coal utilization.Experimental measurements on three coals using X-ray photoelectron spectroscopy(XPS),low-temperature nitrogen adsorptio...Coal-water interactions have profound influences on gas extraction from coal and coal utilization.Experimental measurements on three coals using X-ray photoelectron spectroscopy(XPS),low-temperature nitrogen adsorption and dynamic water vapor sorption(DVS)were conducted.A mechanism-based isotherm model was proposed to estimate the water vapor uptake at various relative humidities,which is well validated with the DVS data.The validated isotherm model of sorption was further used to derive the isosteric heat of water vapor sorption.The specific surface area of coal pores is not the determining parameter that controls water vapor sorption at least during the primary adsorption stage.Oxidation degree dominates the primary adsorption,and which togethering with the cumulative pore volume determine the secondary adsorption.Higher temperature has limited effects on primary adsorption process.The isosteric heat of water adsorption decreases as water vapor uptake increases,which is found to be close to the latent heat of bulk water condensation at higher relative humidity.The results confirmed that the primary adsorption is controlled by the stronger bonding energy while the interaction energy between water molecules during secondary adsorption stage is relatively weak.However,the thermodynamics of coal-water interactions are complicated since the internal bonding interactions within the coal are disrupted at the same time as new bonding interactions take place within water molecules.Coal has a shrinkage/swelling colloidal structure with moisture loss/gain and it may exhibit collapse behavior with some collapses irreversible as a function of relative humidity,which further plays a significant role in determining moisture retention.展开更多
Ordered mesoporous carbon(OMC) with high specific surface area and large pore volume was synthesized and tested for use as an adsorbent for volatile organic compound(VOC)disposal. Benzene, cyclohexane and hexane w...Ordered mesoporous carbon(OMC) with high specific surface area and large pore volume was synthesized and tested for use as an adsorbent for volatile organic compound(VOC)disposal. Benzene, cyclohexane and hexane were selected as typical adsorbates due to their different molecular sizes and extensive utilization in industrial processes. In spite of their structural differences, high adsorption amounts were achieved for all three adsorbates, as the pore size of OMC is large enough for the access of these VOCs. In addition, the unusual bimodal-like pore size distribution gives the adsorbates a higher diffusion rate compared with conventional adsorbents such as activated carbon and carbon molecular sieve. Kinetic analysis suggests that the adsorption barriers mainly originated from the difficulty of VOC vapor molecules entering the pore channels of adsorbents. Therefore, its superior adsorption ability toward VOCs, together with a high diffusion rate, makes the ordered mesoporous carbon a promising potential adsorbent for VOC disposal.展开更多
基金supported by the renewable energy and hydrogen projects in National Key Research and Development Plan of China(2019YFB1505000).
文摘Flue gas and coal bed methane are two important sources of greenhouse gases.Pressure swing adsorption process has a wide range of application in the field of gas separation,and the selection of adsorbent is crucial.In this regard,in order to assess the better adsorbent for separating CO_(2) from flue gas and CH_(4) from coal bed methane,adsorption isotherms of CO_(2),CH_(4) and N_(2) on activated carbon and carbon molecular sieve are measured at 303.15,318.15 and 333.15 K,and up to 250 kPa.The experimental data fit better with Langmuir 2 compared to Langmuir 3 and Langmuir-Freundlich models,and Clausius-Clapeyron equation was used to calculate the isosteric heat.Both the order of the adsorbed amount and the adsorption heat on the two adsorbents are CO_(2)>CH_(4)>N_(2).The adsorption kinetics are calculated by the pseudo-first kinetic model,and the order of adsorption rates on activated carbon is N_(2)-CH_(4)>CO_(2),while on carbon molecular sieve,it is CO_(2)-N_(2)>CH_(4).It is shown that relative molecular mass and adsorption heat are the primary effect on kinetics for activated carbon,while kinetic diameter is the main resistance factor for carbon molecular sieve.Moreover,the adsorption selectivity of CH_(4)/N_(2) and CO_(2)/N_(2) were estimated with the ideal adsorption solution theory,and carbon molecular sieve performed best at 318.15 K for both CO_(2) and CH_(4) separation.The study suggested that activated carbon is a better choice for separating flue gas and carbon molecular sieve can be a strong candidate for separating coal bed methane.
基金National Basic Research Program of China (2005CB221203).
文摘The adsorption of CO2 on a raw activated carbon A and three modified activated carbon samples B, C, and D at temperatures ranging from 303 to 333 K and the thermodynamics of adsorption have been investigated using a vacuum adsorption apparatus in order to obtain more information about the effect of CO2 on removal of organic sulfur-containing compounds in industrial gases. The active ingredients impregnated in the carbon samples show significant influence on the adsorption for CO2 and its volumes adsorbed on modified carbon samples B, C, and D are all larger than that on the raw carbon sample A. On the other hand, the physical parameters such as surface area, pore volume, and micropore volume of carbon samples show no influence on the adsorbed amount of CO2. The Dubinin-Radushkevich (D-R) equation was the best model for fitting the adsorption data on carbon samples A and B, while the Freundlich equation was the best fit for the adsorption on carbon samples C and D. The isosteric heats of adsorption on carbon samples A, B, C, and D derived from the adsorption isotherms using the Clapeyron equation decreased slightly increasing surface loading. The heat of adsorption lay between 10.5 and 28.4 kJ/mol, with the carbon sample D having the highest value at all surface coverages that were studied. The observed entropy change associated with the adsorption for the carbon samples A, B, and C (above the surface coverage of 7 ml/g) was lower than the theoretical value for mobile adsorption. However, it was higher than the theoretical value for mobile adsorption but lower than the theoretical value for localized adsorption for carbon sample D.
文摘Principal side factors as well as technical and procedural peculiarities capable of distorting the results of measurements of adsorbed and desorbed amounts, of falsifying the nature of the processes proceeding in the systems under study, and of promoting artifacts in calorimetric and other studies of gas chemisorption on powders are considered. Modified techniques and procedures allowing the elimination of sources of side phenomena and artifacts and freeing traditional glass static adsorption apparatuses and experimental procedures from undesirable factors and peculiarities are proposed. Some available chemisorption and calorimetric data representing artifacts and also some data that are not artifacts but, due to imperfections of chemisorption techniques, show up as artifacts are presented and discussed. Several applications of the improved techniques and procedures to calorimetric and adsorption studies of the steps of catalytic processes proceeding on the basis of natural gas and of products of its processing are presented and discussed.
基金This study was sponsored by the Open Fund Project Funded by State Key Laboratory of Coal Mine Disaster Dynamics and Control,Chongqing University(Grant#2011DA105287-FW201903)We also want to thank the China Scholarship Council(CSC)for the financial support(Grant#201806430028).
文摘Coal-water interactions have profound influences on gas extraction from coal and coal utilization.Experimental measurements on three coals using X-ray photoelectron spectroscopy(XPS),low-temperature nitrogen adsorption and dynamic water vapor sorption(DVS)were conducted.A mechanism-based isotherm model was proposed to estimate the water vapor uptake at various relative humidities,which is well validated with the DVS data.The validated isotherm model of sorption was further used to derive the isosteric heat of water vapor sorption.The specific surface area of coal pores is not the determining parameter that controls water vapor sorption at least during the primary adsorption stage.Oxidation degree dominates the primary adsorption,and which togethering with the cumulative pore volume determine the secondary adsorption.Higher temperature has limited effects on primary adsorption process.The isosteric heat of water adsorption decreases as water vapor uptake increases,which is found to be close to the latent heat of bulk water condensation at higher relative humidity.The results confirmed that the primary adsorption is controlled by the stronger bonding energy while the interaction energy between water molecules during secondary adsorption stage is relatively weak.However,the thermodynamics of coal-water interactions are complicated since the internal bonding interactions within the coal are disrupted at the same time as new bonding interactions take place within water molecules.Coal has a shrinkage/swelling colloidal structure with moisture loss/gain and it may exhibit collapse behavior with some collapses irreversible as a function of relative humidity,which further plays a significant role in determining moisture retention.
基金the State Key program of National Natural Science Foundation (No. 21337003)the Strategic Priority Research Program (No. XDB05050200)+2 种基金the National High Technology Research and Development Program of China (2012AA063101)the Special Environmental Protection Foundation for Public Welfare Project (No. 201309073)the Team Interaction and Cooperation of the Science and Technology Program of the Chinese Academy of Sciences
文摘Ordered mesoporous carbon(OMC) with high specific surface area and large pore volume was synthesized and tested for use as an adsorbent for volatile organic compound(VOC)disposal. Benzene, cyclohexane and hexane were selected as typical adsorbates due to their different molecular sizes and extensive utilization in industrial processes. In spite of their structural differences, high adsorption amounts were achieved for all three adsorbates, as the pore size of OMC is large enough for the access of these VOCs. In addition, the unusual bimodal-like pore size distribution gives the adsorbates a higher diffusion rate compared with conventional adsorbents such as activated carbon and carbon molecular sieve. Kinetic analysis suggests that the adsorption barriers mainly originated from the difficulty of VOC vapor molecules entering the pore channels of adsorbents. Therefore, its superior adsorption ability toward VOCs, together with a high diffusion rate, makes the ordered mesoporous carbon a promising potential adsorbent for VOC disposal.