A series of the Pt-Sn/SBA-15 catalysts were prepared and their properties characterized by using X-ray powder diffraction (XRD), N2 adsorption-desorption, high resolution transmission electron microscope, X-ray phot...A series of the Pt-Sn/SBA-15 catalysts were prepared and their properties characterized by using X-ray powder diffraction (XRD), N2 adsorption-desorption, high resolution transmission electron microscope, X-ray photoelectron spectroscopy (XPS) and H2-temperature programmed reduction. Their performances in long chain alkane dehydrogenation were evaluated in a fixed-bed microreactor with dodecane as a model alkane. The results indicated that SBA-15 maintained the well-order mesoporous structure during the reaction. The performance of the catalyst was found not dominated by its textural properties, but by the molar ratio of Sn to Pt which governed the degree of Sn reduction. Owing to the highest degree of Sn reduction, 1% (by mass) Pt-1.8% (by mass) Sn/SBA-15 showed the best catalytic activity. At 0.1 MPa and 470℃, the molar ratio of hydrogen to alkane at 4, and liquid hourly space velocity (LHSV) 20 h^-1, the dodecane conversion is 10%, and the dodecene selectivity is about 70%.展开更多
CoCu/TiO_2 catalysts promoted using alkali metals(Li, Na, K, Rb, and Cs) were prepared by the homogeneous deposition-precipitation method followed by the incipient wetness impregnation method. The influences of the ...CoCu/TiO_2 catalysts promoted using alkali metals(Li, Na, K, Rb, and Cs) were prepared by the homogeneous deposition-precipitation method followed by the incipient wetness impregnation method. The influences of the alkali metals on the physicochemical properties of the CoCu/TiO_2 catalysts and the catalytic performance for CO_2 hydrogenation to long-chain hydrocarbons(C_(5+))were investigated in this work. According to the characterization of the catalysts based on X-ray photoelectron spectroscopy, X-ray diffraction, CO_2 temperature-programmed desorption(TPD), and H_2-TPD, the introduction of alkali metals could increase the CO_2 adsorption and decrease the H_2 chemisorption, which could suppress the formation of CH_4, enhance the production of C_(5+), and decrease the hydrogenation activity. Among all the promoters, the Na-modified CoCu/TiO_2 catalyst provided the maximum C_(5+) yield of 5.4%, with a CO_2 conversion of 18.4% and C_(5+) selectivity of42.1%, because it showed the strongest basicity and a slight decrease in the amount of H_2 desorption;it also exhibited excellent catalytic stability of more than 200 h.展开更多
The acidic properties of aluminum phosphate (A1PO4-5) solid acid catalyst were characterized by tem- perature programmed desorption (TPD) of ammonia (NH3), n-propylamine (n-C3HTNH2), iso-propylamine [(CH3)2C...The acidic properties of aluminum phosphate (A1PO4-5) solid acid catalyst were characterized by tem- perature programmed desorption (TPD) of ammonia (NH3), n-propylamine (n-C3HTNH2), iso-propylamine [(CH3)2CHNH2] and n-dipropylamine [(C3H7)2NH] separately, and its catalytic performance in benzene alkylation with long chain olefin was studied in a fixed-bed reactor. The characterized acid amount of catalyst increased with the basicity of adsorbates. With increase of the activation temperature of catalyst, the acid amount characterized by NHa-TPD decreased, however, it increased when characterized by TPD using three other adsorbates. The desorption kinetics of TPD process and the deactivation kinetics of catalyst were investigated. The acidity and catalytic per- formance of catalyst was also correlated. The results showed that the acid amount and strength are well correlated with the activity and stability using NH3 as adsorbate, respectively, which indicated NH3 was a better basic adsorbate. It was also found that the catalyst with higher acid amount and lower acid strength on the surface exhibited the better catalytic performance and stability.展开更多
The bioconversion of coal at ambient conditions is a promising technology for coal processing, although the mechanisms of coal degradation are still not understood fully. In this work, the bioconversion of lig- nite w...The bioconversion of coal at ambient conditions is a promising technology for coal processing, although the mechanisms of coal degradation are still not understood fully. In this work, the bioconversion of lig- nite was studied using a fungus isolated from decaying wood. The lignite samples were oxidized with nitric acid under moderate conditions and then the oxidized samples were placed on a potato medium with isolated fungus for lignite bioconversion. Lignite, oxidized lignite and residual products after bioconversion of lignite were sequentially extracted with petroleum ether, CS2, methanol, acetone and tetrahydrofuran (THt:), and then each extract was characterized by gas chromatography-mass spectrom- etry (GC/MS). The differences in composition and structure among the samples were inferred by compar- ing the differences between the extracts. The results show that aromatics with one or several benzene rings and their derivatives; and some long-chain alkanes containing oxygen decreased in the metha- nol-, acetone-, and THF-soluble fraction from residual lignite, whereas long chain or a few branched alkanes and small quantities of aromatic compounds increased in petroleum ether and CS2 soluble fractions.展开更多
In our previous paper we extended the Tao and Mason equation of state (TM EOS) to refrigerant fluids, using the speed of sound data. This is a continuation for evaluating TM EOS in predicting PVT properties of heavy n...In our previous paper we extended the Tao and Mason equation of state (TM EOS) to refrigerant fluids, using the speed of sound data. This is a continuation for evaluating TM EOS in predicting PVT properties of heavy n-alkanes. Liquid density of long-chain n-alkane systems from C 9 to C 20 have been calculated using an analytical equation of state based on the statistical-mechanical perturbation theory. The second virial coefficients of these n-alkanes are scarce and there is no accurate potential energy function for their theoretical calculation. In this work the second virial coefficients are calculated using a corresponding state correlation based on surface tension and liquid density at the freezing point. The deviation of calculated densities of these alkanes is within 0.5% from experimental data. The densities of n-alkanes obtained from the TM EOS are compared with those calculated from Ihm-Song-Mason equation of state and the corresponding-states liquid densities (COSTALD). Our results are in favor of the preference of the TM EOS over other two equations of state.展开更多
V/SiO2 catalysts compared to Cr/SiO2 catalysts were studied for dehydrogenation of n-butane to butenes. Several methods for characterization of catalysts such as FT-IR, UV-vis and Raman spectroscopies were used. Some ...V/SiO2 catalysts compared to Cr/SiO2 catalysts were studied for dehydrogenation of n-butane to butenes. Several methods for characterization of catalysts such as FT-IR, UV-vis and Raman spectroscopies were used. Some differences between two catalysts were showed, including the performances of catalysts, distribution of products and mechanism of reactions. The results showed that prepared catalysts with 12m% of active component loading all demonstrated best conversion of n-butane to butene at a reaction temperature of around 590 ℃. Two different reaction mechanisms were mentioned to well explain why iso-butene was produced on V/SiO2 catalysts but not on Cr/SiO2 catalysts.展开更多
Carbon preference index (CPI) of long-chain n-alkanes preserved in surface soil increases gradually from southeastern China to the north margin of Loess Plateau.Along this latitudinal transect,the CPI value correlates...Carbon preference index (CPI) of long-chain n-alkanes preserved in surface soil increases gradually from southeastern China to the north margin of Loess Plateau.Along this latitudinal transect,the CPI value correlates to relative humidity,precipitation,and temperature with a negative linear relationship,respectively,whereas the correlation of CPI to temperature is relatively weak.In the Wuyi,Shennongjia,and Tianshan Mountains,CPI values do not change systemically with altitude increasing (or temperature decreasing).However,mean value of CPI for the individual mountain increases in turn from the humid mountain to the arid.These results jointly suggest that aridity (or humidity) is a dominate climate factor in altering soil CPI value.High CPI values of geological records therefore indicate the arid paleoclimate.Though long-chain n-alkanes in soil are derived mainly from leaf wax of terrestrial vascular plants,the regular latitudinal variations of soil CPI might not be caused by the change of vegetation.We speculate that increased long-chain n-alkanes from microbes and/or enhanced biodegradation in the humid climate lead to the decrease of soil CPI.展开更多
基金Supported by the National Natural Science Foundation of China (20376005).
文摘A series of the Pt-Sn/SBA-15 catalysts were prepared and their properties characterized by using X-ray powder diffraction (XRD), N2 adsorption-desorption, high resolution transmission electron microscope, X-ray photoelectron spectroscopy (XPS) and H2-temperature programmed reduction. Their performances in long chain alkane dehydrogenation were evaluated in a fixed-bed microreactor with dodecane as a model alkane. The results indicated that SBA-15 maintained the well-order mesoporous structure during the reaction. The performance of the catalyst was found not dominated by its textural properties, but by the molar ratio of Sn to Pt which governed the degree of Sn reduction. Owing to the highest degree of Sn reduction, 1% (by mass) Pt-1.8% (by mass) Sn/SBA-15 showed the best catalytic activity. At 0.1 MPa and 470℃, the molar ratio of hydrogen to alkane at 4, and liquid hourly space velocity (LHSV) 20 h^-1, the dodecane conversion is 10%, and the dodecene selectivity is about 70%.
文摘CoCu/TiO_2 catalysts promoted using alkali metals(Li, Na, K, Rb, and Cs) were prepared by the homogeneous deposition-precipitation method followed by the incipient wetness impregnation method. The influences of the alkali metals on the physicochemical properties of the CoCu/TiO_2 catalysts and the catalytic performance for CO_2 hydrogenation to long-chain hydrocarbons(C_(5+))were investigated in this work. According to the characterization of the catalysts based on X-ray photoelectron spectroscopy, X-ray diffraction, CO_2 temperature-programmed desorption(TPD), and H_2-TPD, the introduction of alkali metals could increase the CO_2 adsorption and decrease the H_2 chemisorption, which could suppress the formation of CH_4, enhance the production of C_(5+), and decrease the hydrogenation activity. Among all the promoters, the Na-modified CoCu/TiO_2 catalyst provided the maximum C_(5+) yield of 5.4%, with a CO_2 conversion of 18.4% and C_(5+) selectivity of42.1%, because it showed the strongest basicity and a slight decrease in the amount of H_2 desorption;it also exhibited excellent catalytic stability of more than 200 h.
文摘The acidic properties of aluminum phosphate (A1PO4-5) solid acid catalyst were characterized by tem- perature programmed desorption (TPD) of ammonia (NH3), n-propylamine (n-C3HTNH2), iso-propylamine [(CH3)2CHNH2] and n-dipropylamine [(C3H7)2NH] separately, and its catalytic performance in benzene alkylation with long chain olefin was studied in a fixed-bed reactor. The characterized acid amount of catalyst increased with the basicity of adsorbates. With increase of the activation temperature of catalyst, the acid amount characterized by NHa-TPD decreased, however, it increased when characterized by TPD using three other adsorbates. The desorption kinetics of TPD process and the deactivation kinetics of catalyst were investigated. The acidity and catalytic per- formance of catalyst was also correlated. The results showed that the acid amount and strength are well correlated with the activity and stability using NH3 as adsorbate, respectively, which indicated NH3 was a better basic adsorbate. It was also found that the catalyst with higher acid amount and lower acid strength on the surface exhibited the better catalytic performance and stability.
基金supported by the Fundamental Research Funds for the Central Universities (No. 2010QNB12)the National Natural Science Foundation of China (No. 50921002)
文摘The bioconversion of coal at ambient conditions is a promising technology for coal processing, although the mechanisms of coal degradation are still not understood fully. In this work, the bioconversion of lig- nite was studied using a fungus isolated from decaying wood. The lignite samples were oxidized with nitric acid under moderate conditions and then the oxidized samples were placed on a potato medium with isolated fungus for lignite bioconversion. Lignite, oxidized lignite and residual products after bioconversion of lignite were sequentially extracted with petroleum ether, CS2, methanol, acetone and tetrahydrofuran (THt:), and then each extract was characterized by gas chromatography-mass spectrom- etry (GC/MS). The differences in composition and structure among the samples were inferred by compar- ing the differences between the extracts. The results show that aromatics with one or several benzene rings and their derivatives; and some long-chain alkanes containing oxygen decreased in the metha- nol-, acetone-, and THF-soluble fraction from residual lignite, whereas long chain or a few branched alkanes and small quantities of aromatic compounds increased in petroleum ether and CS2 soluble fractions.
基金H. Karimi and F. Yousefi would like to thank Yasouj University for supporting this project
文摘In our previous paper we extended the Tao and Mason equation of state (TM EOS) to refrigerant fluids, using the speed of sound data. This is a continuation for evaluating TM EOS in predicting PVT properties of heavy n-alkanes. Liquid density of long-chain n-alkane systems from C 9 to C 20 have been calculated using an analytical equation of state based on the statistical-mechanical perturbation theory. The second virial coefficients of these n-alkanes are scarce and there is no accurate potential energy function for their theoretical calculation. In this work the second virial coefficients are calculated using a corresponding state correlation based on surface tension and liquid density at the freezing point. The deviation of calculated densities of these alkanes is within 0.5% from experimental data. The densities of n-alkanes obtained from the TM EOS are compared with those calculated from Ihm-Song-Mason equation of state and the corresponding-states liquid densities (COSTALD). Our results are in favor of the preference of the TM EOS over other two equations of state.
基金The Program for New Century Excellent Talents in University (Grant No.NCET-04-0987)Doctor Fund of Science Research of Xinjiang University (Grant No. BS060101)
文摘V/SiO2 catalysts compared to Cr/SiO2 catalysts were studied for dehydrogenation of n-butane to butenes. Several methods for characterization of catalysts such as FT-IR, UV-vis and Raman spectroscopies were used. Some differences between two catalysts were showed, including the performances of catalysts, distribution of products and mechanism of reactions. The results showed that prepared catalysts with 12m% of active component loading all demonstrated best conversion of n-butane to butene at a reaction temperature of around 590 ℃. Two different reaction mechanisms were mentioned to well explain why iso-butene was produced on V/SiO2 catalysts but not on Cr/SiO2 catalysts.
基金supported jointly by National Natural Science Foundation of China (Grant No. 41103001)Knowledge Innovation Program of Chinese Academy of Sciences (Grant Nos. KZCX2-YW-Q1-15,KZCX2-YW-Q1-03)
文摘Carbon preference index (CPI) of long-chain n-alkanes preserved in surface soil increases gradually from southeastern China to the north margin of Loess Plateau.Along this latitudinal transect,the CPI value correlates to relative humidity,precipitation,and temperature with a negative linear relationship,respectively,whereas the correlation of CPI to temperature is relatively weak.In the Wuyi,Shennongjia,and Tianshan Mountains,CPI values do not change systemically with altitude increasing (or temperature decreasing).However,mean value of CPI for the individual mountain increases in turn from the humid mountain to the arid.These results jointly suggest that aridity (or humidity) is a dominate climate factor in altering soil CPI value.High CPI values of geological records therefore indicate the arid paleoclimate.Though long-chain n-alkanes in soil are derived mainly from leaf wax of terrestrial vascular plants,the regular latitudinal variations of soil CPI might not be caused by the change of vegetation.We speculate that increased long-chain n-alkanes from microbes and/or enhanced biodegradation in the humid climate lead to the decrease of soil CPI.