The H2S removal characteristics of Taxada lime tinder the high temperature of 600-900℃ have been investigated. The test results indicated that this kind of sorbent almost was inert to H2S When temperature lowered dow...The H2S removal characteristics of Taxada lime tinder the high temperature of 600-900℃ have been investigated. The test results indicated that this kind of sorbent almost was inert to H2S When temperature lowered down to 600℃,while its reactivity increased with increased temperature and the equilibrium conversion reached up to over 60% at temperatLlre of 900℃.However, side reactions of H2S in conjunction with high-temperature decomposition and mineral catalysis to elemental sulfur and sulfur dioxide were testified.展开更多
Catalysts using α-FeOOH nanoparticles as the active ingredient were testedby a microreactor-chromatography assessing apparatus at atmospheric pressure between 25 and 60 ℃with a gas hourly space velocity of 10,000 h^...Catalysts using α-FeOOH nanoparticles as the active ingredient were testedby a microreactor-chromatography assessing apparatus at atmospheric pressure between 25 and 60 ℃with a gas hourly space velocity of 10,000 h^(-1), while the removal performance of H_2S withcatalysts was investigated using the thermal gravimetric method. The results show that the catalystsare highly active for COS hydrolysis at low temperatures (≤60 ℃) and high gas hourly spacevelocity, and the highest activity can reach 100%. The catalyst is particularly stable for 12 h, andno deactivation is observed. Nanoparticle α-FeOOH prepared using hydrated iron sulfate showshigher COS hydrolysis activity, and the optimum calcination temperature for the catalyst is 260 ℃.In addition, the catalysts can remove COS and H_2S simultaneously, and 60 ℃ is favorable for theremoval of H_2S. The compensation effect exists in nanoparticle-based catalysts.展开更多
Upgrading biogas into biomethane not only improves the biogas utilization as vehicle fuel or natural gas substitute,but also reduces the greenhouse gases emissions.Considering the principle of engineering green energy...Upgrading biogas into biomethane not only improves the biogas utilization as vehicle fuel or natural gas substitute,but also reduces the greenhouse gases emissions.Considering the principle of engineering green energy process,the renewable aqueous ammonia(RAA)solution obtained from biogas slurry was used to remove H_(2)S and CO_(2) simultaneously in the hollow fiber membrane contactor.RAA was mimicked in this study using the ammonia aqueous solution mixed with some typical impurities including ethanol,acetic acid,propionic acid,butyric acid and NH4HCO_(3).Compared with the typical physical absorption(i.e.,pure water)removing 48%of H_(2)S from biogas,RAA with 0.1 mol·L^(−1) NH_(3) could remove 97%of H_(2)S.Increasing the NH3 concentration from 0.1 to 0.5 mol·L^(−1) could elevate the CO_(2) absorption flux from 0.97 to 1.72 mol·m^(−2)·h^(−1) by 77.3%.Among the impurities contained in RAA,ethanol has a less impact on CO_(2) absorption,while other impurities like CO_(2) and acetic acid have significant negative impacts on CO_(2) absorption.Fortunately,the impurities have a less influence on H_(2)S removal efficiency,with more than 98%of H_(2)S could be removed by RAA.Also,the influences of operating parameters on acid gases removal were investigated to provide some engineering suggestions.展开更多
A series of ZnO/SiO_(2) adsorbents were prepared by a sol-gel method using tetraethyl orthosilicate,ethylene glycol(EG)and nitrates as precursors.The effect of gel drying temperature on the structure and desulfurizati...A series of ZnO/SiO_(2) adsorbents were prepared by a sol-gel method using tetraethyl orthosilicate,ethylene glycol(EG)and nitrates as precursors.The effect of gel drying temperature on the structure and desulfurization performance of the adsorbents were investigated in detail.It is found that the low drying temperature led to a weak interaction among EG,Si AOH/H_(2)O and the nitrates in the gel system,which caused the oxidation of EG by NO3-and formed zinc glyoxylate complex during the gel calcination process,whereas this oxidation process also occurred at a high drying temperature during the gel drying process.The formed zinc glyoxylate complex promoted the generation of monodentate carbonate on the surface of Zn O,which resulted in the inferior desulfurization performance of adsorbents despite they have smaller Zn O nanoparticles.The gel dried at 120°C formed the hydrogen bonds between EG and Si AOH/H_(2)O and a strong interaction between zinc oxo-clusters and NO3-was also found in the gel system,which avoided the oxidation of EG by NO3-during the preparation process and the Zn O nanoparticles with sizes of 6 nm were formed by a combustion method.The adsorbent affords a highest sulfur capacity of 104.9 mg·g^(-1) in this case.In addition,the gel drying temperature has a significant influence on the textural properties of the adsorbents except their surface area.展开更多
The primary aliphatic amine Primene JM-T was investigated as a potential absorbent for H2S removal. The solubility of HzS in JM-T was measured at 298, 313,333,353, and 368 K with H2S partial pressures from 20 to 760 k...The primary aliphatic amine Primene JM-T was investigated as a potential absorbent for H2S removal. The solubility of HzS in JM-T was measured at 298, 313,333,353, and 368 K with H2S partial pressures from 20 to 760 kPa and HzS loading from 0.02 to 0.8 mol H2S per mol JM-T. Relevant physical properties, such as density, viscoslty and dielectric constant, ot the matenal were measured. 'The thermodynamlc model with two-suttlX Margules equation was used to correlate the experimental vapor-liquid equilibrium data. Furthermore, the absorption mechanism in non-aqueous system is suggested and the difference between non-aqueous and aqueous absorption system is pointed out.展开更多
In order to decisively determine the adsorption selectivity of zirconium MOF(UiO-66) towards anionic versus cationic species, the adsorptive removal of the anionic dyes(Alizarin Red S.(ARS), Eosin(E), Fuchsin Acid(FA)...In order to decisively determine the adsorption selectivity of zirconium MOF(UiO-66) towards anionic versus cationic species, the adsorptive removal of the anionic dyes(Alizarin Red S.(ARS), Eosin(E), Fuchsin Acid(FA)and Methyl Orange(MO)) and the cationic dyes(Neutral Red(NR), Fuchsin Basic(FB), Methylene Blue(MB),and Safranine T(ST)) has been evaluated. The results clearly reveal a significant selectivity towards anionic dyes. Such an observation agrees with a plethora of reports of UiO-66 superior affinity towards other anionic species(Floride, PO_4^(3-), Diclofenac sodium, Methylchlorophenoxy-propionic acid, Phenols, CrO_4^(2-), SeO_3^(2-), and AsO_4^-). The adsorption process of ARS as an example has been optimized using the central composite design(CCD). The resultant statistical model indicates a crucial effect of both pH and sorbent mass. The optimum conditions were determined to be initial dye concentration 11.82 mg.L^(-1), adsorbent amount 0.0248 g, shaking time of 36 min and pH 2. The adsorption process proceeds via pseudo-second order kinetics(R^2= 0.999). The equilibrium data were fit to Langmuir and Tempkin models(R^2= 0.999 and 0.997 respectively). The results reveal an exceptional removal for the anionic dye(Alizarin Red S.) with a record adsorption capacity of400 mg·g^(-1). The significantly high adsorption capacity of UiO-66 towards ARS adds further evidence to the recently reported exceptional performance of MOFs in pollutants removal from water.展开更多
Hydrogen sulfide(H_(2)S)is a critical component of biogas formed under anaerobic conditions by sulfur and sulfate reducing bacteria from animal manure and renewable energy crops.H_(2)S causes high corrosion in equipme...Hydrogen sulfide(H_(2)S)is a critical component of biogas formed under anaerobic conditions by sulfur and sulfate reducing bacteria from animal manure and renewable energy crops.H_(2)S causes high corrosion in equipment,has a negative environmental impact,inhibits the biogas formation process and is furthermore odorous and toxic.Although several methods for internal and external desulfurization found their way into practice and had been explored at laboratory scale,no data were available on the performance of such methods in full scale practice,especially for an external fixed-bed trickling bioreactor(FBTB).The effects of temperature,pH and air ratio on H_(2)S removal efficiency(RE)were studied.The study was conducted at a research biogas plant with a given output of 96 m^(3) biogas per hour,and an H_(2)S concentration ranging between 500 ppm and 600 ppm(1 ppm=1 cm^(3)/m^(3))on average.The FBTB column has been designed to hold a packing volume of 2.21 m^(3) at a gas retention time of 84 seconds being loaded at an average of 32.88 g H_(2)S/(m^(3)·h).The highest H_(2)S RE of 98% was found at temperatures between 30℃ and 40℃.A major decline in RE to 21%-45%was observed at temperatures from 5℃ to 25℃.The results clearly showed a temperature optimum range for sulfate reducing bacteria.The results reveal that RE is little affected by different pH values and air ratios.During the experimental period,the practical suitability of the FBTB system could be proved while avoiding the disadvantages of internal biological desulfurization methods.展开更多
Higher concentrations of Hg can be emitted from coal pyrolysis or gasification than from coal combustion, especially elemental Hg. Highly efficient Hg removal technology from coal-derived fuel gas is thus of great imp...Higher concentrations of Hg can be emitted from coal pyrolysis or gasification than from coal combustion, especially elemental Hg. Highly efficient Hg removal technology from coal-derived fuel gas is thus of great importance. Based on the very excellent Hg removal ability of Pd and the high adsorption abilities of activated carbon(AC) for H2 S and Hg, a series of Pd/AC sorbents was prepared by using pore volume impregnation, and their performance in capturing Hg and H2 S from coal-derived fuel gas was investigated using a laboratory-scale fixed-bed reactor. The effects of loading amount, reaction temperature and reaction atmosphere on Hg removal from coal-derived fuel gas were studied. The sorbents were characterized by N2 adsorption, X-ray diffraction(XRD) and X-ray photoelectron spectroscopy(XPS). The results indicated that the efficiency of Hg removal increased with the increasing of Pd loading amount, but the effective utilization rate of the active component Pd decreased significantly at the same time. High temperature had a negative influence on the Hg removal. The efficiency of Hg removal in the N2-H2S-H2-CO-Hg atmosphere(simulated coal gas) was higher than that in N2-H2S-Hg and N2-Hg atmospheres, which showed that H2 and CO, with their reducing capacity, could benefit promote the removal of Hg. The XPS results suggested that there were two different ways of capturing Hg over sorbents in N2-H2S-Hg and N2-Hg atmospheres.展开更多
文摘The H2S removal characteristics of Taxada lime tinder the high temperature of 600-900℃ have been investigated. The test results indicated that this kind of sorbent almost was inert to H2S When temperature lowered down to 600℃,while its reactivity increased with increased temperature and the equilibrium conversion reached up to over 60% at temperatLlre of 900℃.However, side reactions of H2S in conjunction with high-temperature decomposition and mineral catalysis to elemental sulfur and sulfur dioxide were testified.
文摘Catalysts using α-FeOOH nanoparticles as the active ingredient were testedby a microreactor-chromatography assessing apparatus at atmospheric pressure between 25 and 60 ℃with a gas hourly space velocity of 10,000 h^(-1), while the removal performance of H_2S withcatalysts was investigated using the thermal gravimetric method. The results show that the catalystsare highly active for COS hydrolysis at low temperatures (≤60 ℃) and high gas hourly spacevelocity, and the highest activity can reach 100%. The catalyst is particularly stable for 12 h, andno deactivation is observed. Nanoparticle α-FeOOH prepared using hydrated iron sulfate showshigher COS hydrolysis activity, and the optimum calcination temperature for the catalyst is 260 ℃.In addition, the catalysts can remove COS and H_2S simultaneously, and 60 ℃ is favorable for theremoval of H_2S. The compensation effect exists in nanoparticle-based catalysts.
基金supports from the Natural Science Foundation of Hubei Province of China(2020CFA107,2020CFB209)the National Natural Science Foundation of China(32002222,52076101)the Fundamental Research Funds for the Central Universities(2662021JC004).
文摘Upgrading biogas into biomethane not only improves the biogas utilization as vehicle fuel or natural gas substitute,but also reduces the greenhouse gases emissions.Considering the principle of engineering green energy process,the renewable aqueous ammonia(RAA)solution obtained from biogas slurry was used to remove H_(2)S and CO_(2) simultaneously in the hollow fiber membrane contactor.RAA was mimicked in this study using the ammonia aqueous solution mixed with some typical impurities including ethanol,acetic acid,propionic acid,butyric acid and NH4HCO_(3).Compared with the typical physical absorption(i.e.,pure water)removing 48%of H_(2)S from biogas,RAA with 0.1 mol·L^(−1) NH_(3) could remove 97%of H_(2)S.Increasing the NH3 concentration from 0.1 to 0.5 mol·L^(−1) could elevate the CO_(2) absorption flux from 0.97 to 1.72 mol·m^(−2)·h^(−1) by 77.3%.Among the impurities contained in RAA,ethanol has a less impact on CO_(2) absorption,while other impurities like CO_(2) and acetic acid have significant negative impacts on CO_(2) absorption.Fortunately,the impurities have a less influence on H_(2)S removal efficiency,with more than 98%of H_(2)S could be removed by RAA.Also,the influences of operating parameters on acid gases removal were investigated to provide some engineering suggestions.
基金financially supported by the National Natural Science Foundation of China(22078223 and 21878209)Shanxi Province Science Foundation for Youths(20210302123065)。
文摘A series of ZnO/SiO_(2) adsorbents were prepared by a sol-gel method using tetraethyl orthosilicate,ethylene glycol(EG)and nitrates as precursors.The effect of gel drying temperature on the structure and desulfurization performance of the adsorbents were investigated in detail.It is found that the low drying temperature led to a weak interaction among EG,Si AOH/H_(2)O and the nitrates in the gel system,which caused the oxidation of EG by NO3-and formed zinc glyoxylate complex during the gel calcination process,whereas this oxidation process also occurred at a high drying temperature during the gel drying process.The formed zinc glyoxylate complex promoted the generation of monodentate carbonate on the surface of Zn O,which resulted in the inferior desulfurization performance of adsorbents despite they have smaller Zn O nanoparticles.The gel dried at 120°C formed the hydrogen bonds between EG and Si AOH/H_(2)O and a strong interaction between zinc oxo-clusters and NO3-was also found in the gel system,which avoided the oxidation of EG by NO3-during the preparation process and the Zn O nanoparticles with sizes of 6 nm were formed by a combustion method.The adsorbent affords a highest sulfur capacity of 104.9 mg·g^(-1) in this case.In addition,the gel drying temperature has a significant influence on the textural properties of the adsorbents except their surface area.
基金Supported by the National Natural Science Foundation of China(51178446,21206168)
文摘The primary aliphatic amine Primene JM-T was investigated as a potential absorbent for H2S removal. The solubility of HzS in JM-T was measured at 298, 313,333,353, and 368 K with H2S partial pressures from 20 to 760 kPa and HzS loading from 0.02 to 0.8 mol H2S per mol JM-T. Relevant physical properties, such as density, viscoslty and dielectric constant, ot the matenal were measured. 'The thermodynamlc model with two-suttlX Margules equation was used to correlate the experimental vapor-liquid equilibrium data. Furthermore, the absorption mechanism in non-aqueous system is suggested and the difference between non-aqueous and aqueous absorption system is pointed out.
文摘In order to decisively determine the adsorption selectivity of zirconium MOF(UiO-66) towards anionic versus cationic species, the adsorptive removal of the anionic dyes(Alizarin Red S.(ARS), Eosin(E), Fuchsin Acid(FA)and Methyl Orange(MO)) and the cationic dyes(Neutral Red(NR), Fuchsin Basic(FB), Methylene Blue(MB),and Safranine T(ST)) has been evaluated. The results clearly reveal a significant selectivity towards anionic dyes. Such an observation agrees with a plethora of reports of UiO-66 superior affinity towards other anionic species(Floride, PO_4^(3-), Diclofenac sodium, Methylchlorophenoxy-propionic acid, Phenols, CrO_4^(2-), SeO_3^(2-), and AsO_4^-). The adsorption process of ARS as an example has been optimized using the central composite design(CCD). The resultant statistical model indicates a crucial effect of both pH and sorbent mass. The optimum conditions were determined to be initial dye concentration 11.82 mg.L^(-1), adsorbent amount 0.0248 g, shaking time of 36 min and pH 2. The adsorption process proceeds via pseudo-second order kinetics(R^2= 0.999). The equilibrium data were fit to Langmuir and Tempkin models(R^2= 0.999 and 0.997 respectively). The results reveal an exceptional removal for the anionic dye(Alizarin Red S.) with a record adsorption capacity of400 mg·g^(-1). The significantly high adsorption capacity of UiO-66 towards ARS adds further evidence to the recently reported exceptional performance of MOFs in pollutants removal from water.
文摘Hydrogen sulfide(H_(2)S)is a critical component of biogas formed under anaerobic conditions by sulfur and sulfate reducing bacteria from animal manure and renewable energy crops.H_(2)S causes high corrosion in equipment,has a negative environmental impact,inhibits the biogas formation process and is furthermore odorous and toxic.Although several methods for internal and external desulfurization found their way into practice and had been explored at laboratory scale,no data were available on the performance of such methods in full scale practice,especially for an external fixed-bed trickling bioreactor(FBTB).The effects of temperature,pH and air ratio on H_(2)S removal efficiency(RE)were studied.The study was conducted at a research biogas plant with a given output of 96 m^(3) biogas per hour,and an H_(2)S concentration ranging between 500 ppm and 600 ppm(1 ppm=1 cm^(3)/m^(3))on average.The FBTB column has been designed to hold a packing volume of 2.21 m^(3) at a gas retention time of 84 seconds being loaded at an average of 32.88 g H_(2)S/(m^(3)·h).The highest H_(2)S RE of 98% was found at temperatures between 30℃ and 40℃.A major decline in RE to 21%-45%was observed at temperatures from 5℃ to 25℃.The results clearly showed a temperature optimum range for sulfate reducing bacteria.The results reveal that RE is little affected by different pH values and air ratios.During the experimental period,the practical suitability of the FBTB system could be proved while avoiding the disadvantages of internal biological desulfurization methods.
基金supported by the National Natural Science Foundation of China (Nos. 21006067, 21276170)the Shanxi Province Natural Science Foundation (Nos. 2010021008-1, 201101008-4)the National High-Tech Research and Development Program (863) of China (No. 2013AA065404E)
文摘Higher concentrations of Hg can be emitted from coal pyrolysis or gasification than from coal combustion, especially elemental Hg. Highly efficient Hg removal technology from coal-derived fuel gas is thus of great importance. Based on the very excellent Hg removal ability of Pd and the high adsorption abilities of activated carbon(AC) for H2 S and Hg, a series of Pd/AC sorbents was prepared by using pore volume impregnation, and their performance in capturing Hg and H2 S from coal-derived fuel gas was investigated using a laboratory-scale fixed-bed reactor. The effects of loading amount, reaction temperature and reaction atmosphere on Hg removal from coal-derived fuel gas were studied. The sorbents were characterized by N2 adsorption, X-ray diffraction(XRD) and X-ray photoelectron spectroscopy(XPS). The results indicated that the efficiency of Hg removal increased with the increasing of Pd loading amount, but the effective utilization rate of the active component Pd decreased significantly at the same time. High temperature had a negative influence on the Hg removal. The efficiency of Hg removal in the N2-H2S-H2-CO-Hg atmosphere(simulated coal gas) was higher than that in N2-H2S-Hg and N2-Hg atmospheres, which showed that H2 and CO, with their reducing capacity, could benefit promote the removal of Hg. The XPS results suggested that there were two different ways of capturing Hg over sorbents in N2-H2S-Hg and N2-Hg atmospheres.