To better understand the nature of reactive adsorption of thiophene on Ni/ZnO adsorbent,the effect of ZnO textural structure on the desulfurization activity was investigated.ZnO materials were synthesized by low-tempe...To better understand the nature of reactive adsorption of thiophene on Ni/ZnO adsorbent,the effect of ZnO textural structure on the desulfurization activity was investigated.ZnO materials were synthesized by low-temperature solid-state reaction and the corresponding Ni/ZnO adsorbents were prepared by incipient impregnation method.The analysis results showed that the crystalline sizes of ZnO as-synthesized as well as the BET surface areas varied obviously with the calcination temperature.The activity evaluations indicated that the Ni/ZnO adsorbents prepared with ZnO possessed a favorable textural structure as active component exhibited good activity of removing thiophene.The evolutions of the main crystalline phases of Ni/ZnO adsorbents before and after reaction confirmed that ZnO played a crucial role in taking up S element and converting it into ZnS in the reactive adsorption process.It was concluded that ZnO with larger surface area and smaller crystal particles resulted in better desulfurization activity,which may be the main reason for the different activities of the Ni/ZnO adsorbents prepared with ZnO calcined at different temperatures.展开更多
A Cu-Co-K/activated carbon （AC） adsorbent has been developed for the removal of carbonyl sulfide （COS）. The effects of COS concentration, reaction temperature and relative humidity were closely examined. A breakth...A Cu-Co-K/activated carbon （AC） adsorbent has been developed for the removal of carbonyl sulfide （COS）. The effects of COS concentration, reaction temperature and relative humidity were closely examined. A breakthrough of 33.23 mg COS .gl adsorbent at 60℃, under 30% relative humidity and in presence of 1.0% oxygen was exhibited in the Cu-Co-K/AC adsorbent prepared. Competitive adsorption studies for COS in the presence of CS2, and H2S were also conducted. TPD analysis was used to identify sulfur-containing products on the carbon surface, and the results indicated that H2S, COS and SO2 were all evident in the effluent gas generated from the exhausted Cu-Co-K/AC. Structure of the activated carbon samples has been characterized using nitrogen adsorption, and their surface chemical structures were also determined with X-ray photoelectron spectroscopy （XPS）. It turns out that the modification with Cu（OH）2CO3- CoPcS-KOH can significantly improve the COS removal capacity, forming SO2/4 species simultaneously. Regenera- tion of the spent activated carbon sorbents by thermal desorption has also been explored.展开更多
To investigate the effect of texture structure on the desulfurization performance in the Ni/ZnO reactive adsorption desulfurization（RADS） system,two kinds of ZnO porous materials with rod-shaped morphology were synt...To investigate the effect of texture structure on the desulfurization performance in the Ni/ZnO reactive adsorption desulfurization（RADS） system,two kinds of ZnO porous materials with rod-shaped morphology were synthesized and their structure was characterized by X-ray diffraction（XRD）,scanning electron microscopy（SEM）,transmission electron microscopy（TEM）,and N2 adsorption/desorption.The formation mechanisms of hierarchical porous ZnO（ZnO with meso and macro pores） were also studied.Their application performance was evaluated in the RADS process over Ni/ZnO absorbent.Due to the difference in structure between the two kinds of ZnO,the two ZnO based adsorbents showed different desulfurization activity.展开更多
A high-performance Ni/ZnO adsorbent was prepared by homogeneous precipitation using urea hydro- lysis and characterized by N2 adsorption-desorption, X-ray diffraction （XRD）, and scanning electron microscope （SEM）....A high-performance Ni/ZnO adsorbent was prepared by homogeneous precipitation using urea hydro- lysis and characterized by N2 adsorption-desorption, X-ray diffraction （XRD）, and scanning electron microscope （SEM）. The adsorbent was applied to the deep desulfur- ization of gasoline and showed a high breakthrough sulful capacity and a remarkably high volume hourly space velocity. The effects of coexisting olefins in gasoline as well as adsorptive conditions on the adsorptive perfor- mance were examined. It was found that olefins in gasoline had a slightly inhibiting effect on the desulfurization performance of the adsorbent. The optimum conditions were 673 K, 1.0 Mpa with a volume hourly space velocity of 60h^-1. Under the optimum conditions, ultralow sulfur gasoline could be produced and the breakthrough sulfur capacity of the adsorbent was 360 mg-s/g-sorb for the model gasoline.展开更多
The waste gas evolved from biodegradation of animal urine contains ammonia causing environmental concerns. A new and effective method for removing ammonia from such waste gas using reactive adsorption is presented. In...The waste gas evolved from biodegradation of animal urine contains ammonia causing environmental concerns. A new and effective method for removing ammonia from such waste gas using reactive adsorption is presented. In the process, activated carbon impregnated with H2SO4（H2SO4/C） is employed. Ammonia in the waste gas reacts with H2SO4 on the adsorbent instantaneously and completely to form （NIL）2SO4. The H2SO4/C adsorbent is high in NH3 adsorption capacity and regenerable. The NH3 removal capacity of this regenerable adsorbent is more than 30 times that of the adsorbents used normally in the industry. The spent H2SO4/C is regenerated by flowing low-pressure steam through the adsorbent bed to remove the （NH4）2SO4 from the adsorbent. The regeneration by-product is concentrated （NH4）2SO4 solution, which is a perfect liquid fertilizer for local use. Re-soaking the activated carbon with H2SO4 solution rejuvenates the activity of the adsorbent. Thus the H2SOJC can be reused repeatedly. In the mechanism of this reactive adsorption process, trace of H20 in the waste gas is a required, which lends itself to treating ammonia gas saturated with moisture from biodegradation of animal urine.展开更多
Aiming to improve the reactive adsorption desulfurization（RADS） performances of Ni/Zn O adsorbents,ZnxAly（OH）2（CO3）z·x H2 O precursor is synthesized by coprecipitation of Zn2＋,AlO-2,and CO2-3; the Zn OZn6A...Aiming to improve the reactive adsorption desulfurization（RADS） performances of Ni/Zn O adsorbents,ZnxAly（OH）2（CO3）z·x H2 O precursor is synthesized by coprecipitation of Zn2＋,AlO-2,and CO2-3; the Zn OZn6Al2O9 composite oxides are obtained by the calcination of ZnxAly（OH）2（CO3）z·x H2 O precursor,and the Ni/Zn O-Zn6Al2O9（6.0 wt% Ni O） adsorbents are prepared by wetness impregnation method. The phase,acid strength,acid type and quantity,morphology,and thermal properties were characterized by X-ray diffraction,temperature-programmed desorption of ammonia,pyridine-adsorbed infrared spectrum,high-resolution transmission electron microscopy,and Thermo Gravimetry-Derivative Thermo Gravimetry（TG-DTG）,respectively. The breakthrough sulfur capacities of six adsorbents are between 34.2 and 47.9 mg/gcat. The kinetic studies indicated that the active energy of RADS（49.4 k J/mol） could reach nano-sized Zn O,the particle size of is about 12.0 nm. All the excellent RADS performances can be due to the high SBET. Also,there are some extents of aromatization reactions that occur,which can be contributed to the B？nsted acid rooted in Zn6Al2O9 composite oxide,and the octane number of products can be preserved well.展开更多
基金supported by National Key Fundamental Research development Plan ("973" Plan, No. 2010CB226905)the Postgraduate Innovation Fund of China University of petroleumthe Postgraduate Innovation Fund of China University of petroleum
文摘To better understand the nature of reactive adsorption of thiophene on Ni/ZnO adsorbent,the effect of ZnO textural structure on the desulfurization activity was investigated.ZnO materials were synthesized by low-temperature solid-state reaction and the corresponding Ni/ZnO adsorbents were prepared by incipient impregnation method.The analysis results showed that the crystalline sizes of ZnO as-synthesized as well as the BET surface areas varied obviously with the calcination temperature.The activity evaluations indicated that the Ni/ZnO adsorbents prepared with ZnO possessed a favorable textural structure as active component exhibited good activity of removing thiophene.The evolutions of the main crystalline phases of Ni/ZnO adsorbents before and after reaction confirmed that ZnO played a crucial role in taking up S element and converting it into ZnS in the reactive adsorption process.It was concluded that ZnO with larger surface area and smaller crystal particles resulted in better desulfurization activity,which may be the main reason for the different activities of the Ni/ZnO adsorbents prepared with ZnO calcined at different temperatures.
基金This work was supported by the National Natural Science Foundation of China （Grant Nos. Ul137603, 51268021 and 51368026）, the National High Technology Research and Development Program of China （No. 2012AA062504） and the Applied Basic Research Program of Yunnan （Nos. 2011FB027 and 2011FA010）.
文摘A Cu-Co-K/activated carbon （AC） adsorbent has been developed for the removal of carbonyl sulfide （COS）. The effects of COS concentration, reaction temperature and relative humidity were closely examined. A breakthrough of 33.23 mg COS .gl adsorbent at 60℃, under 30% relative humidity and in presence of 1.0% oxygen was exhibited in the Cu-Co-K/AC adsorbent prepared. Competitive adsorption studies for COS in the presence of CS2, and H2S were also conducted. TPD analysis was used to identify sulfur-containing products on the carbon surface, and the results indicated that H2S, COS and SO2 were all evident in the effluent gas generated from the exhausted Cu-Co-K/AC. Structure of the activated carbon samples has been characterized using nitrogen adsorption, and their surface chemical structures were also determined with X-ray photoelectron spectroscopy （XPS）. It turns out that the modification with Cu（OH）2CO3- CoPcS-KOH can significantly improve the COS removal capacity, forming SO2/4 species simultaneously. Regenera- tion of the spent activated carbon sorbents by thermal desorption has also been explored.
基金Financial support from the National Basic Research Program of China (No. 2010CB226905)the National Natural Science Foundation of China (Nos. 21176258, U1162203)the Specialized Research Fund for the Doctoral Program of Higher Education (20110133110002)
文摘To investigate the effect of texture structure on the desulfurization performance in the Ni/ZnO reactive adsorption desulfurization（RADS） system,two kinds of ZnO porous materials with rod-shaped morphology were synthesized and their structure was characterized by X-ray diffraction（XRD）,scanning electron microscopy（SEM）,transmission electron microscopy（TEM）,and N2 adsorption/desorption.The formation mechanisms of hierarchical porous ZnO（ZnO with meso and macro pores） were also studied.Their application performance was evaluated in the RADS process over Ni/ZnO absorbent.Due to the difference in structure between the two kinds of ZnO,the two ZnO based adsorbents showed different desulfurization activity.
文摘A high-performance Ni/ZnO adsorbent was prepared by homogeneous precipitation using urea hydro- lysis and characterized by N2 adsorption-desorption, X-ray diffraction （XRD）, and scanning electron microscope （SEM）. The adsorbent was applied to the deep desulfur- ization of gasoline and showed a high breakthrough sulful capacity and a remarkably high volume hourly space velocity. The effects of coexisting olefins in gasoline as well as adsorptive conditions on the adsorptive perfor- mance were examined. It was found that olefins in gasoline had a slightly inhibiting effect on the desulfurization performance of the adsorbent. The optimum conditions were 673 K, 1.0 Mpa with a volume hourly space velocity of 60h^-1. Under the optimum conditions, ultralow sulfur gasoline could be produced and the breakthrough sulfur capacity of the adsorbent was 360 mg-s/g-sorb for the model gasoline.
文摘The waste gas evolved from biodegradation of animal urine contains ammonia causing environmental concerns. A new and effective method for removing ammonia from such waste gas using reactive adsorption is presented. In the process, activated carbon impregnated with H2SO4（H2SO4/C） is employed. Ammonia in the waste gas reacts with H2SO4 on the adsorbent instantaneously and completely to form （NIL）2SO4. The H2SO4/C adsorbent is high in NH3 adsorption capacity and regenerable. The NH3 removal capacity of this regenerable adsorbent is more than 30 times that of the adsorbents used normally in the industry. The spent H2SO4/C is regenerated by flowing low-pressure steam through the adsorbent bed to remove the （NH4）2SO4 from the adsorbent. The regeneration by-product is concentrated （NH4）2SO4 solution, which is a perfect liquid fertilizer for local use. Re-soaking the activated carbon with H2SO4 solution rejuvenates the activity of the adsorbent. Thus the H2SOJC can be reused repeatedly. In the mechanism of this reactive adsorption process, trace of H20 in the waste gas is a required, which lends itself to treating ammonia gas saturated with moisture from biodegradation of animal urine.
文摘Aiming to improve the reactive adsorption desulfurization（RADS） performances of Ni/Zn O adsorbents,ZnxAly（OH）2（CO3）z·x H2 O precursor is synthesized by coprecipitation of Zn2＋,AlO-2,and CO2-3; the Zn OZn6Al2O9 composite oxides are obtained by the calcination of ZnxAly（OH）2（CO3）z·x H2 O precursor,and the Ni/Zn O-Zn6Al2O9（6.0 wt% Ni O） adsorbents are prepared by wetness impregnation method. The phase,acid strength,acid type and quantity,morphology,and thermal properties were characterized by X-ray diffraction,temperature-programmed desorption of ammonia,pyridine-adsorbed infrared spectrum,high-resolution transmission electron microscopy,and Thermo Gravimetry-Derivative Thermo Gravimetry（TG-DTG）,respectively. The breakthrough sulfur capacities of six adsorbents are between 34.2 and 47.9 mg/gcat. The kinetic studies indicated that the active energy of RADS（49.4 k J/mol） could reach nano-sized Zn O,the particle size of is about 12.0 nm. All the excellent RADS performances can be due to the high SBET. Also,there are some extents of aromatization reactions that occur,which can be contributed to the B？nsted acid rooted in Zn6Al2O9 composite oxide,and the octane number of products can be preserved well.
