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2010, Vol. 19, No. 5　Online: 2010-09-30

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Journal of Natural Gas Chemistry begins to come off the press bimonthly in 2010 2010, 19(5): 0-0.  DOI: 摘要 ( 6133 )   PDF

Reviews

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The production of carbon nanotubes from carbon dioxide: challenges and opportunities Geoffrey S. Simate, Sunny E. Iyuke, Sehliselo Ndlovu, Clarence S. Yah, Lubinda F. Walubita 2010, 19(5): 453-460.  DOI: 10.1016/S1003-9953(09)60099-2 摘要 ( 12887 )   Recent advances in the production of carbon nanotubes (CNTs) are reviewed with an emphasis on the use of carbon dioxide (CO2) as a sole source of carbon. Compared to the most widely used carbon precursors such as graphite, methane, acetylene, ethanol, ethylene, and coal-derived hydrocarbons, CO2 is competitively cheaper with relatively high carbon yield content. However, CNT synthesis from CO2 is a newly emerging technology, and hence it needs to be explored further. A theoretical and analytical comparison of the currently existing CNT-CO2 synthesis techniques is given including a review of some of the process parameters (i.e., temperature, pressure, catalyst, etc.) that affect the CO2 reduction rate. Such analysis indicates that there is still a fundamental need to further explore the following aspects so as to realize the full potential of CO2 based CNT technology: (1) the CNT-CO2 synthesis and formation mechanism, (2) catalytic effects of transitional metals and mechanisms, (3) utilization of metallocenes in the CNT-CO2 reactions, (4) applicability of ferrite-organometallic compounds in the CNT-CO2 synthesis reactions, and (5) the effects of process parameters such as temperature, etc.

Communctions

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Continuous conversion of methanol to higher hydrocarbons at ambient pressure William W. Porterfield, Gordon M. Zrelak, L. Avery Moncure, Matthew D. Huff 2010, 19(5): 461-462.  DOI: 10.1016/S1003-9953(09)60114-6 摘要 ( 9657 )   An iodozincate ionic liquid solvent and catalyst is used to convert methanol continuously to a wide variety of hydrocarbons at atmospheric pressure.

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NF3 decomposition over some metal oxides in the absence of water Xianjun Niu, Liang Sun, Yanan Wang, Haipeng Wu, Xiufeng Xu 2010, 19(5): 463-467.  DOI: 10.1016/S1003-9953(09)60107-9 摘要 ( 10784 )   NF3 decomposition in the absence of water over Al2O3, Fe2O3, Co3O4 and NiO, and transition metal oxides (Fe2O3, Co3O4 and NiO) coated Al2O3 reagents was investigated. The results show that Al2O3 is an active reagent for NF3 decomposition with 100% conversion lasting for 8.5 h at 400 ℃. Fe2O3, Co3O4 and NiO coated Al2O3 reagents are superior to bare Al2O3, and 5%Co3O4/Al2O3 has a high reactivity with NF3 full conversion maintaining for 10.5 h. It is suggested that the presence of transition metal oxide is beneficial to the reactivity of Al2O3, and results in a significant enhancement in the fluorination of Al2O3.

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Catalytic performance of iron carbide for carbon monoxide hydrogenation Minglin Xiang, Juan Zou, Qinghua Li, Xichun She 2010, 19(5): 468-470.  DOI: 10.1016/S1003-9953(09)60113-4 摘要 ( 10403 )   Novel iron carbide and potassium-promoted iron carbide catalysts were prepared and investigated for CO hydrogenation. The iron carbide showed high activity for CO hydrogenation under high pressures; with the addition of potassium, activity and selectivity to C5+ hydrocarbons were greatly enhanced, and the selectivity to methane was suppressed.

Articles

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Facile synthesis of microporous carbon through a soft-template pathway and its performance in desulfurization and denitrogenation Bo Sun, Gang Li, Xiaoxing Wang 2010, 19(5): 471-476.  DOI: 10.1016/S1003-9953(09)60115-8 摘要 ( 10822 )   Wormlike/lamellar microporous carbons were prepared by using long alkyl chain primary amine hydrochloride as the template and resorcinol/formaldehyde as the carbon source under highly acidic conditions. The template can be eliminated by high temperature treatment under an inert atmosphere. The obtained carbon materials were characterized by N2 adsorption-desorption, transmission electron microscopy, thermogravimetry and scanning electron microscopy. The results show that dodecylamine hydrochloride surfactant can be used as the template of wormlike micropores structure while octadecylamine hydrochloride results in both lamellar and wormlike micropores. The obtained carbon materials have the similar pore size in the range of 0.5~0.59 nm, but with various morphologies such as monolith, spheres, and coralline. The microporous carbon obtained from dodecylamine hydrochloride surfactant shows good adsorption performance to remove the refractory sulfur compounds and nitrogen-containing compounds in fuel.

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Autothermal reforming of biogas over a monolithic catalyst Sadao Araki, Naoe Hino, Takuma Mori, Susumu Hikazudani 2010, 19(5): 477-481.  DOI: 10.1016/S1003-9953(09)60102-X 摘要 ( 11306 )   This study focused on measurement of the autothermal reforming of biogas over a Ni based monolithic catalyst. The effects of the steam/CH4 (S/C) ratio, O2/CH4 (O2/C) ratio and temperature were investigated. The CH4 conversions were higher under all examined temperatures than the equilibrium conversion calculated using the blank outlet temperature, because the catalyst layer was heated by the exothermic catalytic partial oxidation reaction. The CH4 conversion increased with increasing O2/C ratio. Moreover, the CH4 conversion was higher than the equilibrium conversion calculated using the blank outlet temperature for O2/C>0.42 and reached about 100% at O2/C=0.55. However, the hydrogen concentration decreased for O2/C>0.45 because hydrogen was combusted to steam in the presence of excess oxygen. On the other hand, the hydrogen and CO2 concentrations increased and the CO concentration decreased with increasing S/C ratio. As a result, it was found that the highest hydrogen concentrations and CH4 conversions were attained at the O2/C ratios of 0.45-0.55 and the S/C ratios of 1.5-2.5. Moreover, the H2/CO ratio could also be controlled in the range from about 2 to 3.5 to give at least 90% CH4 conversion, by regulating the O2/C or S/C ratios.

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Cross metathesis of butene-2 and ethene to propene over Mo/MCM-22-Al2O3 catalysts with different Al2O3 contents Shenglin Liu, Xiujie Li, Wenjie Xin, Sujuan Xie, Peng Zeng, Lixin Zhang, Longya Xu 2010, 19(5): 482-486.  DOI: 10.1016/S1003-9953(09)60095-5 摘要 ( 12118 )   A series of 3.0Mo/MCM-22-Al2O3 catalysts with γ-Al2O3 contents in the range of 0-100 wt% were prepared and applied in the metathesis reaction of ethene and butene-2. Addition of γ-Al2O3 did not affect the structure of MCM-22 zeolite as evidenced by XRD and N2 adsorption measurements. It was deduced from TPR experiments that γ-Al2O3 phase favored the formation of polymolybdate or multilayered Mo oxide, while more Al2(MoO4)3 species were generated over MCM-22 zeolites. Alumina content in the support was directly related to the metathesis activity of ethene and butene-2 to propene. Mo species with higher valence (Mo6+or Mo5+) contributed more to the excellent performance of catalyst than metallic Mo. The best catalyst activity and stability was obtained over 3.0Mo/(MCM-22-30%Al2O3) under the reaction condition of 1.0 MPa and 125 ℃ using N2 as the pretreatment gas.

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Effect of preparation methods of aluminum emulsions on catalytic performance of copper-based catalysts for methanol synthesis from syngas Lili Wang, Wen Ding, Yingwei Liu, Weiping Fang, Yiquan Yang 2010, 19(5): 487-492.  DOI: 10.1016/S1003-9953(09)60105-5 摘要 ( 11373 )     Various Cu/ZnO/Al2O3 catalysts have been synthesized by different aluminum emulsions as aluminum sources and their performances for methanol synthesis from syngas have been investigated. The influences of preparation methods of aluminum emulsions on physicochemical and catalytic properties of catalysts were studied by XRD, SEM, XPS, N2 adsorption--desorption techniques and methanol synthesis from syngas. The preparation methods of aluminum emulsions were found to influence the catalytic activity, CuO crystallite size, surface area and Cu0 surface area and reduction process. The results show that the catalyst CN using the aluminum source prepared by addition the ammonia into the aluminum nitrate (NP) exhibited the best catalytic performance for methanol synthesis from syngas.

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Forecasting China's natural gas consumption based on a combination model Gang Xu, Weiguo Wang 2010, 19(5): 493-496.  DOI: 10.1016/S1003-9953(09)60100-6 摘要 ( 8345 )     Ensuring a sufficient energy supply is essential to a country. Natural gas constitutes a vital part in energy supply and therefore forecasting natural gas consumption reliably and accurately is an essential part of a country's energy policy. Over the years, studies have shown that a combinative model gives better projected results compared to a single model. In this study, we used Polynomial Curve and Moving Average Combination Projection (PCMACP) model to estimate the future natural gas consumption in China from 2009 to 2015. The new proposed PCMACP model shows more reliable and accurate results: its Mean Absolute Percentage Error (MAPE) is less than those of any previous models within the investigated range. According to the PCMACP model, the average annual growth rate will increase for the next 7 years and the amount of natural gas consumption will reach 171600 million cubic meters in 2015 in China.

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Selective CO methanation over amorphous Ni-Ru-B/ZrO2 catalyst for hydrogen-rich gas purification Qihai Liu, Zili Liu, LieWen Liao, Xinfa Dong 2010, 19(5): 497-502.  DOI: 10.1016/S1003-9953(09)60106-7 摘要 ( 10534 )     Amorphous Ni-Ru-B/ZrO2 catalysts were prepared by chemical reduction method. The effects of Ni-Ru-B loading and Ru/Ni mole ratio on the catalytic performance for selective CO methanation from reformed fuel were studied, and the catalysts were characterized by BET, ICP, XRD and TPD. The results showed that Ru strongly affected the catalytic activity and selectivity by increasing the thermal stability of amorphous structure, promoting the dispersion of the catalyst particle, and intensifying the CO adsorption. For the catalysts with Ru/Ni mole ratio under 0.15, the CO methanation conversion and selectivity increased significantly with the increasing Ru/Ni mole ratio. Among all the catalysts investigated, the 30 wt% Ni-Ru-B loading amorphous Ni61Ru9B30/ZrO2 catalyst with 0.15 Ru/Ni mole ratio presented the best catalytic performance, over which higher than 99.9% of CO conversion was obtained in the temperature range of 230℃~250℃, and the CO2 conversion was kept under the level of 0.9%.

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Fischer-Tropsch synthesis over ruthenium-promoted Co/Al2O3 catalyst with different reduction procedures Ali Karimi, Ali Nakhaei Pour, Farshad Torabi, Behnam Hatami, Ahmad Tavasoli, Mohammad Reza Alaei, Mohammad Irani 2010, 19(5): 503-508.  DOI: 10.1016/S1003-9953(09)60111-0 摘要 ( 13242 )   The effect of reduction procedure on catalyst properties, activity and products selectivity of ruthenium-promoted Co/γ-Al2O3 catalyst in Fischer-Tropsch synthesis (FTS) was investigated. Catalyst samples were reduced with different reduction gas compositions and passivated before being characterized by TPR and XRD techniques. Different activity and product selectivity analyses were also performed. These results showed that the catalyst dispersion, particle size, and the degree of reduction changed with different reduction gas compositions, which were resulted from the water partial pressures in reduction process that give varying degrees of interaction with the support. It has been suggested that the FTS activity of cobalt catalyst was directly dependent on the catalyst reducibility. A reduction gas with a molar ratio of H2/He = 1 was used to prevent the formation of Co-support compound during catalyst reduction.

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Catalytic properties of Ni/ceria-yttria electrode materials for partial oxidation of methane Shaohua Zeng, Lei Wang, Maochu Gong, Yaoqiang Chen 2010, 19(5): 509-514.  DOI: 10.1016/S1003-9953(09)60098-0 摘要 ( 12625 )   The catalytic properties of electrode materials Ni/Ce1-xYxO2-δ (x = 0.05, 0.10, 0.15 and 0.20) were investigated for partial oxidation of methane (POM). The CeO2-Y2O3 solid solutions were prepared by co-precipitaion method. The Ni-based catalysts supported on the solid solutions were obtained using the impregnation method. Structural, surface and redox characteristics of the prepared catalysts were systematically examined by means of X-ray diffraction (XRD), N2 adsorption-desorption (Brunauer-Emmet-Teller BET method), H2 temperature-programmed reduction (H2-TPR) and X-ray photoelectron spectroscopy (XPS) methods. The results indicated that yttria doped in the ceria system, forming a good solid solution, readily induced more defects and oxygen vacancies that favored the improvement of catalytic activity and coking resistance. In the temperature range of 600-850 ℃, Ni/Ce0.90Y0.10O1.95 catalyst exhibited the best catalytic activity among the four tested catalysts, with the CH4 conversion, CO selectivity and H2 selectivity of 78.8%, 90.6% and 89.8%, respectively, at 850 ℃. And the H2/CO molar ratio in products of Ni/Ce0.90Y0.10O1.95 catalyst was closer to the theoretical value of 2.0. The excellent coking resistant behaviors for all catalysts were clearly manifested by Thermal Analysis.

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Characterization and catalytic behavior of Na-W-Mn-Zr-S-P/SiO2 prepared by different methods in oxidative coupling of methane Wen Zheng, Dangguo Cheng, Fengqiu Chen, Xiaoli Zhan 2010, 19(5): 515-521.  DOI: 10.1016/S1003-9953(09)60101-8 摘要 ( 12339 )     Na-W-Mn-Zr-S-P/SiO2 catalysts for oxidative coupling of methane (OCM) were prepared by incipient wetness impregnation, sol-gel and mixture slurry methods. The catalyst prepared by mixture slurry method showed the best catalytic performance among all samples. In addition, the effects of different addition sequences of Na, W, Mn, Zr, S and P on the catalytic performance were studied. The absence of Na before the addition of Mn and Zr in the catalysts preparation depressed the formation of the active phases of Mn2O3 and ZrO2 and decreased the activities of the catalysts significantly.

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Product oriented oxidative bromination of methane over Rh/SiO2 catalysts Zhen Liu, Wensheng Li, Xiaoping Zhou 2010, 19(5): 522-529.  DOI: 10.1016/S1003-9953(09)60112-2 摘要 ( 11358 )   Rh/SiO2 was prepared for the oxidative bromination of methane. The catalyst was prepared by calcination at different temperatures and for different times to obtain catalysts with different specific surface areas for the purposes of producing either CH3Br or CH3Br and CO. It was found that the catalyst having a low specific surface area (calcined at relatively high temperature) favors the selective oxidation of methane to prepare CH3Br, while the catalyst having a high specific surface area favors the deeper partial oxidation of methane, which is good for CH3Br and CO preparation. The 650 h on stream life-time test revealed that the catalytic performance of the 0.4Rh/SiO2--900-10 catalyst was excellent. Both methane conversion and CH3Br selectivity kept increasing trends during the life-time test. No matter how serious was the Rh leaching during the reaction, the 0.4Rh/SiO2--900-10 catalyst did not deactivate at all.

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Synthesis, characterization and hydrodesulfurization activity of silica-dispersed NiMoW trimetallic catalysts Di Liu, Lihua Liu, Guangci Li, Chenguang Liu 2010, 19(5): 530-533.  DOI: 10.1016/S1003-9953(09)60108-0 摘要 ( 11368 )   Silica-dispersed NiMoW trimetallic hydrodesulfurization catalysts were prepared by deposition-precipitation method. For comparative purposes, bulk NiMoW trimetallic catalysts were obtained by co-precipitation. Silica was employed to disperse active metals for full utilization of active components and silica-dispersed NiMoW catalyst had high active metal content. BET analysis showed that silica-dispersed NiMoW trimetallic catalysts had a high surface area (165.1 m2/g) and pore volume (0.27 ml/g). Transmission electron microscopy results proved that active components were well dispersed. Hydrodesulfurization activity of silica-dispersed NiMoW catalysts was much higher than that of comparative catalysts and up to twice greater than those of commercial NiMo alumina-supported systems per gram of catalyst.

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Direct oxidation of methyl radicals in OCM process deduced from correlation of product selectivities Zhiming Gao, Yuanyuan Ma 2010, 19(5): 534-538.  DOI: 10.1016/S1003-9953(09)60110-9 摘要 ( 9738 )     Selectivity of hydrogen in oxidative coupling of methane (OCM) was evaluated over the MxOy-BaCO3 (MxOy: La2O3, Sm2O3, MgO, CaO) catalysts. Correlation of product selectivities was thus discussed. From correlation of product selectivities, it is revealed that the carbon oxides (CO and CO2) were most probably formed from the direct oxidation of methyl radicals under the conditions adopted in the present work. This is also in accordance with the OCM mechanism proposed in literature.

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Prediction and measurement of pollutant emissions in CNG fired internal combustion engine M. Mansha, A. R. Saleemi, Javed S. H, Badar M. Ghauri 2010, 19(5): 539-547.  DOI: 10.1016/S1003-9953(09)60103-1 摘要 ( 10296 )   In the present study, the detailed reaction mechanisms were developed and Chemkin 4.1.1 was implemented to predict the formation of pollutant species in compressed natural gas (CNG) fired internal combustion (IC) engine. The proposed mechanisms were developed by coupling the EXGAS (an automatic mechanism generation tool for alkane oxidation) mechanisms with the Leed's NOx mechanism (version 2.0). The simulation results of each proposed mechanism were validated by the experimental measurements for profiles of temperature, pressure and pollutant species (CO, NOx). The rate of production analysis of each mechanism identified the important reactions in each mechanism which contributed to the formation of pollutant species. In spite of some discrepancies, the experimental measurements indicate that Mechanism-IV (consisting of 208 reactions and 78 species) showed closer agreement for each of the predicted profiles of temperature, pressure and pollutant species (CO, NOx).

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Syntheis of SWNTs over Co-Mo/MgO Nanoporous and using as a catalyst support for selective hydrogenation of syn gas to hydrocarbon A. M. Rashidi, A. Karimi, H. R. Bozorgzadeh, K. Kashefi, M. Zare 2010, 19(5): 548-551.  DOI: 10.1016/S1003-9953(09)60104-3 摘要 ( 12546 )   Single-wall carbon nanotubes (SWNTs) with high surface area were synthesized over nanoporous Co-Mo/MgO by a chemical vapor deposition (CVD) method. The SWNTs were used as catalyst support for selective hydrogenation of syngas to hydrocarbons. Here an extensive study of Fischer-Tropsch synthesis (FTS) on CNT-supported cobalt catalysts with different amounts of cobalt loading up to 40 wt% is reported. The catalysts were characterized by different methods including N2 adsorption-desorption, X-ray diffraction, hydrogen chemisorption, inductively coupled plasma (ICP) and temperature-programmed reduction. Enhancement of the reducibility of Co3O4 to CoO, CoO to Coo and small cobalt oxide particles, dispersion of the cobalt, and activity and selectivity of FTS were investigated and compared with a conventional support. The CNT supported catalysts achieve a high dispersion and high loading of the active metal, cobalt in particular, so that the bulk formation of cobalt metal, which tends to occur in conventional support, can be avoided. The results showed that the specific activity of CNT supported catalysts increase significantly (there is a two fold increase in CO Conversion per gram of the active metal) with respect to the conventional supported catalyst.

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A new and reliable model for predicting methane viscosity at high pressures and high temperatures Ehsan Heidaryan, Jamshid Moghadasi, Amir Salarabadi 2010, 19(5): 552-556.  DOI: 10.1016/S1003-9953(09)60109-2 摘要 ( 11769 )   In recent years, there has been an increase of interest in the flow of gases at relatively high pressures and high temperatures. Hydrodynamic calculation of the energy losses in the flow of gases in conduits, as well as through the porous media constituting natural petroleum reservoirs, requires knowledge of the viscosity of the fluid at the pressure and temperature involved. Although there are numerous publications concerning the viscosity of methane at atmospheric pressure, there appears to be little information available relating to the effect of pressure and temperature upon the viscosity. A survey of the literature reveals that the disagreements between published data on the viscosity of methane are common and that most investigations have been conducted over restricted temperature and pressure ranges. Experimental viscosity data for methane are presented for temperatures from 320 to 400 K and pressures from 3000 to 140000 kPa by using falling body viscometer. A summary is given to evaluate the available data for methane, and a comparison is presented for that data common to the experimental range reported in this paper. A new and reliable correlation for methane gas viscosity is presented. Predicted values are given for temperatures up to 400 K and pressures up to 140000 kPa with Average Absolute Percent Relative Error (EABS) of 0.794.