Commercially available coal-based activated carbon was treated by nitric acid with different concentrations and the resultant samples were used as catalysts for the direct hydroxylation of benzene to phenol in acetoni...Commercially available coal-based activated carbon was treated by nitric acid with different concentrations and the resultant samples were used as catalysts for the direct hydroxylation of benzene to phenol in acetonitrile. Boehm titration, X-ray photoelectron spectroscopy, scanning electron microscope coupled with an energy dispersive X-ray microanalyzer, and Brunauer-Emmett-Teller method were used to characterize the samples. The number of carboxyl groups on the surface was found to be the main factor affecting the catalytic activity. An optimum catalytic performance with a yield of 15.7% and a selectivity of 87.2% to phenol was obtained.展开更多
Coal-based Magnetic Activated Carbons （CMAC＇s） were prepared from three representative coal samples of various ranks： Baorigele lignite from Inner Mongolia; Datong bitumite from Shanxi province; and Taixi anthraci...Coal-based Magnetic Activated Carbons （CMAC＇s） were prepared from three representative coal samples of various ranks： Baorigele lignite from Inner Mongolia; Datong bitumite from Shanxi province; and Taixi anthracite from Ningxia Hui Auto- nomous Region. Fe3O4 was used as a magnetic additive. A nitrogen-adsorption analyzer was used to determine the specific surface area and pore structure of the resulting activated carbons. The adsorption capacity was assessed by the adsorption of iodine and methylene blue. X-ray diffraction was used to measure the evolution behavior of Fe304 during the preparation process. Magnetic properties were characterized with a vibrating-sample magnetometer. The effect of the activation temperature on the performance of CMAC＇s was also studied. The results show that, compared to Baorigele lignite and Taixi anthracite, the Datong bitumite is more appropriate for the preparation of CMAC＇s with a high specific surface area, an advanced pore structure and suitable magnetic properties. Fe304 can effectively enhance the magnetic properties and control the pore structure by increasing the ratio of meso- pores. An addition of 6.0% Fe304 and an activation temperature of 880 ℃ produced a CMAC having a specific surface area, an iodine adsorption, a methylene blue adsorption and a specific saturation magnetization of 1152.0 m2/g, 1216.7 mg/g, 229.5 mg/g and 4.623 emu/g, respectively. The coal used to prepare this specimen was Datong bitumite.展开更多
The preparation of activated carbon from Chinese fir sawdust by zinc chloride activation under both nitrogen atmosphere and vacuum conditions was carded out in a self-manufactured vacuum pyrolysis reactor. The effects...The preparation of activated carbon from Chinese fir sawdust by zinc chloride activation under both nitrogen atmosphere and vacuum conditions was carded out in a self-manufactured vacuum pyrolysis reactor. The effects of the system pressure and the activation condition （nitrogen or vacuum） on pore development were investigated. The results show that both high quality activated carbon and high added-value bio-oil can be obtained simultaneously via vacuum chemical activation. The characteristics of the activated carbons produced under vacuum conditions are better than those prepared under nitrogen atmosphere. The performance parameters of the activated carbon obtained under vacuum conditions are as follows： the pore size distribution is mainly microporous, the Brunauer-Emmett-Teller （BET） surface area is 1 070.59 m^2/g, the microporous volume is 0.502 4 cm^3/g, the average pore size is 2.085 nm, and the iodine adsorption value and the methylene blue adsorption value are 1 142.92 and 131.34 mg/g, respectively. The activated carbon from vacuum chemical activation has developed micropores, and the N2 adsorption equilibrium constant of the corresponding activated carbon gradually increases with the decrease of reaction system pressure.展开更多
To obtain the pyrolysis characteristics and kinetics of preparation process of sludge-based activated carbon by ZnCl2 activation method （i.e.the pyrolysis process of the sludge with ZnCl2 activation）,the characteris...To obtain the pyrolysis characteristics and kinetics of preparation process of sludge-based activated carbon by ZnCl2 activation method （i.e.the pyrolysis process of the sludge with ZnCl2 activation）,the characteristic of mass loss and gas products generated during pyrolysis of the sludge with ZnCl2 activation were analyzed by thermogravimetric analysis coupled with Fourier Transform Infrared Spectroscopy （TG-FTIR）.The kinetic parameters were calculated by the Coats-Redfem method and the mechanism models were established.The role of ZnCl2 in the pyrolysis process of the sludge with ZnCl2 activation was also illustrated through the comparison of the pyrolysis characteristics and kinetics of the sludge with and without ZnCl2 activation.The results showed that the pyrolysis process of the sludge with ZnCl2 activation can be divided into four stages including the dehydration of sludge and initial depolymerization of a small portion of organics matters,the decomposition of large molecular organic matters into small molecular intermediates,the further degradation of intermediates and volatilization of ZnCl2,and the decomposition of inorganic minerals and undecomposed organic matters.CO2,CO,CH4,H2O,some aldehydes and carboxylic acids are the major pyrolysis gaseous products.The activation energies and pre-exponential factors are in the range of 28.84-206.42 kJ/mol and 9885.16-8.08× 1011 min-1,respectively.During the pyrolysis of sludge,ZnC12 not only can function as a dehydration agent and inhibit the formation of tar,but also can peptize the organic matters in the sludge,making them easier to be decomposed.展开更多
Activated carbon(AC) was prepared from surplus sludge using chemical activation method with the assistance of ZnCl2. The influences of process parameters on the AC's specific surface area and adsorption capacity f...Activated carbon(AC) was prepared from surplus sludge using chemical activation method with the assistance of ZnCl2. The influences of process parameters on the AC's specific surface area and adsorption capacity for Pb2+ were examined to optimize these parameters. The optimal conditions for the preparation of AC were determined to be activation temperature of 500 °C, activation time of 1 h, impregnation ratio of 1:1(solid-to-liquid volume) with the 30% ZnCl2 solution(mass fraction), giving the BET surface area of 393.85 m2/g and yield of 30.14% with 33.45% ash. Also, the pyrolysis temperature was found to be the most important parameter in chemical activation. FTIR spectra provided the evidence of some surface structures such as C=C and C—O—C. In the adsorption studies, a rise in solution pH led to a significant increase in adsorption capacity when the pH value varied from 3.0 to 7.0, and the optimal pH for removal of Pb2+ was 7.0. It was observed that the pseudo-second-order equation provided better correlation for the adsorption rate than the pseudo-first-order and the Langmuir model fitted better than the Freundlich model for adsorption isotherm. The adsorption capacity of AC to Pb2+ was 11.75 mg/L at solution pH 7.0, the equilibrium time 480 min and 25 °C. Moreover, the adsorption process is endothermic according to the value of enthalpy change.展开更多
Surface chemical properties of typical commercial coal-based activated cokes were characterized by Xray photoelectron spectroscopy(XPS) and acid-base titration, and then the influence of surface chemical properties on...Surface chemical properties of typical commercial coal-based activated cokes were characterized by Xray photoelectron spectroscopy(XPS) and acid-base titration, and then the influence of surface chemical properties on catalytic performance of activated cokes of NO reduction with NH3 was investigated in a fixed-bed quartz micro reactor at 150 ℃. The results indicate that the selective catalytic reduction(SCR) activity of activated cokes with the increase of its surface acidic sites and oxygen content,obviously, a correlation between catalytic activity and surface acidic sites content by titration has higher linearity than catalytic activity and surface oxygen content by XPS. While basic sites content by acid-base titration have not correlation with SCR activity. It has been proposed that surface basic sites content measured by titration may not be on adjacent of acidic surface oxides and then cannot form of NO2-like species, thus the reaction of reduction of NO with NH3 have been retarded.展开更多
基金This work was supported by the National Natural Science Foundation of China （No.20502017, No.20872102, and No.21021001）, the Program for Changjiang Scholars and Innovative Research Team in University （No.IRT0846）, and the characterization of the catalyst from Analytic and Testing Center of Sichuan University are greatly appreciated.
文摘Commercially available coal-based activated carbon was treated by nitric acid with different concentrations and the resultant samples were used as catalysts for the direct hydroxylation of benzene to phenol in acetonitrile. Boehm titration, X-ray photoelectron spectroscopy, scanning electron microscope coupled with an energy dispersive X-ray microanalyzer, and Brunauer-Emmett-Teller method were used to characterize the samples. The number of carboxyl groups on the surface was found to be the main factor affecting the catalytic activity. An optimum catalytic performance with a yield of 15.7% and a selectivity of 87.2% to phenol was obtained.
基金supported by the National Natural Science Foundation of China (No20776150)the National High Technology Research and Development Program of China (No2008AA05Z308)
文摘Coal-based Magnetic Activated Carbons （CMAC＇s） were prepared from three representative coal samples of various ranks： Baorigele lignite from Inner Mongolia; Datong bitumite from Shanxi province; and Taixi anthracite from Ningxia Hui Auto- nomous Region. Fe3O4 was used as a magnetic additive. A nitrogen-adsorption analyzer was used to determine the specific surface area and pore structure of the resulting activated carbons. The adsorption capacity was assessed by the adsorption of iodine and methylene blue. X-ray diffraction was used to measure the evolution behavior of Fe304 during the preparation process. Magnetic properties were characterized with a vibrating-sample magnetometer. The effect of the activation temperature on the performance of CMAC＇s was also studied. The results show that, compared to Baorigele lignite and Taixi anthracite, the Datong bitumite is more appropriate for the preparation of CMAC＇s with a high specific surface area, an advanced pore structure and suitable magnetic properties. Fe304 can effectively enhance the magnetic properties and control the pore structure by increasing the ratio of meso- pores. An addition of 6.0% Fe304 and an activation temperature of 880 ℃ produced a CMAC having a specific surface area, an iodine adsorption, a methylene blue adsorption and a specific saturation magnetization of 1152.0 m2/g, 1216.7 mg/g, 229.5 mg/g and 4.623 emu/g, respectively. The coal used to prepare this specimen was Datong bitumite.
文摘The preparation of activated carbon from Chinese fir sawdust by zinc chloride activation under both nitrogen atmosphere and vacuum conditions was carded out in a self-manufactured vacuum pyrolysis reactor. The effects of the system pressure and the activation condition （nitrogen or vacuum） on pore development were investigated. The results show that both high quality activated carbon and high added-value bio-oil can be obtained simultaneously via vacuum chemical activation. The characteristics of the activated carbons produced under vacuum conditions are better than those prepared under nitrogen atmosphere. The performance parameters of the activated carbon obtained under vacuum conditions are as follows： the pore size distribution is mainly microporous, the Brunauer-Emmett-Teller （BET） surface area is 1 070.59 m^2/g, the microporous volume is 0.502 4 cm^3/g, the average pore size is 2.085 nm, and the iodine adsorption value and the methylene blue adsorption value are 1 142.92 and 131.34 mg/g, respectively. The activated carbon from vacuum chemical activation has developed micropores, and the N2 adsorption equilibrium constant of the corresponding activated carbon gradually increases with the decrease of reaction system pressure.
基金Sponsored by the National Natural Science Foundation of China(Grant No.51008106)
文摘To obtain the pyrolysis characteristics and kinetics of preparation process of sludge-based activated carbon by ZnCl2 activation method （i.e.the pyrolysis process of the sludge with ZnCl2 activation）,the characteristic of mass loss and gas products generated during pyrolysis of the sludge with ZnCl2 activation were analyzed by thermogravimetric analysis coupled with Fourier Transform Infrared Spectroscopy （TG-FTIR）.The kinetic parameters were calculated by the Coats-Redfem method and the mechanism models were established.The role of ZnCl2 in the pyrolysis process of the sludge with ZnCl2 activation was also illustrated through the comparison of the pyrolysis characteristics and kinetics of the sludge with and without ZnCl2 activation.The results showed that the pyrolysis process of the sludge with ZnCl2 activation can be divided into four stages including the dehydration of sludge and initial depolymerization of a small portion of organics matters,the decomposition of large molecular organic matters into small molecular intermediates,the further degradation of intermediates and volatilization of ZnCl2,and the decomposition of inorganic minerals and undecomposed organic matters.CO2,CO,CH4,H2O,some aldehydes and carboxylic acids are the major pyrolysis gaseous products.The activation energies and pre-exponential factors are in the range of 28.84-206.42 kJ/mol and 9885.16-8.08× 1011 min-1,respectively.During the pyrolysis of sludge,ZnC12 not only can function as a dehydration agent and inhibit the formation of tar,but also can peptize the organic matters in the sludge,making them easier to be decomposed.
基金Project supported by the Open Fund of State Key Laboratory of Photocatalysis,China
文摘Activated carbon(AC) was prepared from surplus sludge using chemical activation method with the assistance of ZnCl2. The influences of process parameters on the AC's specific surface area and adsorption capacity for Pb2+ were examined to optimize these parameters. The optimal conditions for the preparation of AC were determined to be activation temperature of 500 °C, activation time of 1 h, impregnation ratio of 1:1(solid-to-liquid volume) with the 30% ZnCl2 solution(mass fraction), giving the BET surface area of 393.85 m2/g and yield of 30.14% with 33.45% ash. Also, the pyrolysis temperature was found to be the most important parameter in chemical activation. FTIR spectra provided the evidence of some surface structures such as C=C and C—O—C. In the adsorption studies, a rise in solution pH led to a significant increase in adsorption capacity when the pH value varied from 3.0 to 7.0, and the optimal pH for removal of Pb2+ was 7.0. It was observed that the pseudo-second-order equation provided better correlation for the adsorption rate than the pseudo-first-order and the Langmuir model fitted better than the Freundlich model for adsorption isotherm. The adsorption capacity of AC to Pb2+ was 11.75 mg/L at solution pH 7.0, the equilibrium time 480 min and 25 °C. Moreover, the adsorption process is endothermic according to the value of enthalpy change.
基金the High Technology Research and Development Program of China(No.2011AA060803)the Beijing Key Laboratory Annual Program(No.Z121103009212039)
文摘Surface chemical properties of typical commercial coal-based activated cokes were characterized by Xray photoelectron spectroscopy(XPS) and acid-base titration, and then the influence of surface chemical properties on catalytic performance of activated cokes of NO reduction with NH3 was investigated in a fixed-bed quartz micro reactor at 150 ℃. The results indicate that the selective catalytic reduction(SCR) activity of activated cokes with the increase of its surface acidic sites and oxygen content,obviously, a correlation between catalytic activity and surface acidic sites content by titration has higher linearity than catalytic activity and surface oxygen content by XPS. While basic sites content by acid-base titration have not correlation with SCR activity. It has been proposed that surface basic sites content measured by titration may not be on adjacent of acidic surface oxides and then cannot form of NO2-like species, thus the reaction of reduction of NO with NH3 have been retarded.
