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Journal of Natural Gas Chemistry 2007年第2期16卷 193-199页

作者： Dianhua Liu Xing Hua dingye fang College of Chemical Engineering East China University of Science and Technology Shanghai 200237 China

A three-phase reactor mathematical model was set up to simulate and design a three-phase bubble column reactor for direct synthesis of dimethyl ether （DME） from syngas, considering both the influence of part inert carrier backmixing on transfer and the influence of catalyst grain sedimentation on reaction. On the basis of this model, the influences of the size and reaction conditions of a 100000 t/a DME reactor on capacity were investigated. The optimized size of the 10000 t/a DME synthesis reactor was proposed as follows： diameter 3.2 m, height 20 m, built-in 400 tube heat exchanger （Ф 38×2 mm）, and inert heat carrier paraffin oil 68 t and catalyst 34.46 t. Reaction temperature and pressure were important factors influencing the reaction conversion for different size reactors. Under the condition of uniform catalyst concentration distribution, higher pressure and temperature were proposed to achieve a higher production capacity of DME. The best ratio of fresh syngas for DME synthesis was 2.04.

关键词： dimethyl ether syngas three-phase reactor DME synthesis slurry bed mathematical simulation model

Simulation and model design of pipe-shell reactor for the direct synthesis of dimethyl ether from syngas

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Journal of Natural Gas Chemistry 2008年第2期17卷 195-200页

作者： Yanfang Hu Zhaoguang Nie dingye fang College of Chemical Engineering and Environment Qingdao University Qingdao 266071 Shandong China Department of Chemical Engineering East China University Science and Technology Shanghai 200237 China

The simulation was made based on the model of pipe-shell reactor that was established by the model of global kinetics of synthesis of dimethyl ether from syngas over a bifunctional catalyst. The results of simulation showed that the selectivity for dimethyl ether （DME） and the conversion of CO were higher but the hot spot was kept below the temperature limit of the pipe-shell reactor. The suitable diameter of the pipe was φ38×2 mm, and the length of the pipe was 5.8 m. The optimal process conditions of the reactor were that the pressure was 5 MPa, the temperature of the cooling water was 240 ℃, and the temperature of the raw gas at inlet of the reactor was 220 ℃. The production of this reactor was 102800 t/y （ton per year） under these conditions.

关键词： simulation model dimethyl ether pipe-shell reactor syngas

Reaction and deactivation kinetics of methanol-to-olefins process based on a special TGA reactor

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Journal of Natural Gas Chemistry 2010年第4期19卷 409-416页

作者： Hao Hu Weiyong Ying dingye fang Engineering Research Center of Large Scale Reactor Engineering and Technology Ministry Education East China University of Science and Technology Shanghai 200237 China State Key Laboratory of Chemical Engineering East China University of Science and Technology Shanghai 200237 China

Thermax 700 thermo gravimetric analysis （TGA） instrument is introduced for the investigation of the reaction and deactivation kinetics of Methanol-to-Olefins （MTO） process with SAPO-34 *** the use of a special sample basket,the TGA instrument can be viewed as a plug flow fixed-bed reactor,while the weight change of SAPO-34 during reaction can be recorded *** data are acquired in the temperature range of 648.2？748.2 K and space velocities of 7.08？35.91 h^-1 （WHSV）.Catalyst activity is expressed with average coke content,and selectivity for different products is related as a function of coke content and *** is also introduced into the lumping kinetic model,and power exponent function with first-order reaction is adopted for model *** function is tested to give the best fit for catalyst activity and product selectivity with the highest correlation *** nicely agreed results between experimental and calculated data suggest that the overall kinetic model would be meaningful in both product distribution prediction and reactor simulation.

关键词： methanol-to-olefins SAPO-34 kinetic model deactivation coking

Effects of the ratio of Fe to Co over Fe-Co/SiO_2 bimetallic catalysts on their catalytic performance for Fischer-Tropsch synthesis

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Journal of Natural Gas Chemistry 2009年第2期18卷 232-236页

作者： Xiangdong Ma Qiwen Sun Weiyong Ying dingye fang Chemical Engineering ＆ Pharmaceutics College Henan University of Science and Technology Luoyang 471003 Henan China School of Chemical Engineering East China University of Science and Technology Shanghai 200237 China Shanghai Yankuang Energy R＆ D Co. Ltd Shanghai 201203 China

The Fe-Co/SiO2 bimetallic catalysts with different ratios of Fe to Co were prepared by aqueous incipient wetness impregnation. The catalysts of 10%Fe：0%Co/SiO2, 10%Fe：6%Co/SiO2, 10%Fe：2%Co/SiO2, 10%Fe：10%Co/SiO2, 6%Fe：10%Co/SiO2, 2%Fe：10%Co/SiO2 and 0%Fe： 10%Co/SiO2 by mass were tested in a fixed reactor by the Fischer-Tropsch synthesis. Activity and hydrocarbon distribution were found to be determined by the ratio of iron to cobalt of the catalysts. Higher iron content inhibited the activity, whereas higher cobalt content enhanced the activity of the Fe-Co/SiO2 catalysts. On the other hand, for the catalysts of 10%Fe：6%Co/SiO2, 10%Fe：10%Co/SiO2, 6%Fe：10%Co/SiO2, and 2%Fe：10%Co/SiO2, the total C2-C4 fraction increased （from 10.65% to 26.78%） and C5＋ fraction decreased （from 75.75% to 57.63%） at 523 K. Temperature programmed reduction revealed that the addition of cobalt enhanced the reducibility of the Fe-Co/SiO2 catalyst. Metal oxides were present in those catalysts as shown by XRD. The Fe-Co alloy phase was found in the 2%Fe：10%Co/SiO2, 6%Fe：10%Co/SiO2, 10%Fe： 10%Co/SiO2, 10%Fe：6%Co/SiO2 catalysts and their crystals were perfect.

关键词： Fischer-Tropsch bimetallic iron cobalt

Product distributions of Fischer-Tropsch synthesis over Co/AC catalyst

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Journal of Natural Gas Chemistry 2011年第4期20卷 389-396页

作者： Weixin Qian Haitao Zhang Weiyong Ying dingye fang Engineering Research Center of Large Scale Reactor Engineering and Technology Ministry of EducationState Key Laboratory of Chemical Engineering East China University of Science and Technology Shanghai 200237 China

The product distributions of Fischer-Tropsch synthesis over Co/AC catalyst are investigated under different reaction conditions in an integral fixed bed *** is found that the product distributions deviate from the ASF *** deviation from ASF distribution is analyzed by taking the readsorption of alkenes and the following secondary reaction into *** is noted that the contents of alcohol,alkene and alkane decline with the increasing carbon number,showing a slighter declining tendency of alkanes than those of alkenes and *** is also found that high temperature,space velocity,H2/CO in feed gas and low pressure are preferential for light hydrocarbons and alcohols while against the chain *** effect of space velocity on the product distributions especially on the light products is not *** is noticed that low temperature,space velocity,H2/CO and high pressure lead to high contents of alcohols;high temperature,H2/CO and low space velocity lead to high contents of *** effect of pressure on the amounts of alkanes is not significant;high space velocity and low temperature,pressure,H2/CO are preferential for alkenes.

关键词： Fischer-Tropsch synthesis product distribution Co/AC catalyst

Effects of promoters on catalytic performance of Fe-Co/SiO_2 catalyst for Fischer-Tropsch synthesis

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Journal of Natural Gas Chemistry 2009年第3期18卷 354-358页

作者： Xiangdong Ma Qiwen Sun Weiyong Ying dingye fang Chemical Engineering ＆ Pharmaceutics College Henan University of Science and Technology Luoyang 471003 Henan China Shanghai Yankuang Energy RD Co.Ltd Shanghai 201203 China School of Chemical Engineering East China University of Science and Technology Shanghai 200237 China

2%Fe-10%Co/SiO2 catalysts with different potassium or zirconium loadings were prepared by aqueous incipient wetness impregnation and tested for Fischer-Tropsch synthesis in a flow reactor, using H2/CO = 1.6 （molar ratio） in the feed, under the condition of an overall pressure of 1 MPa, GHSV of 600 h^-1 and temperature of 503 K. The zirconium and potassium promoters remarkably influenced hydrocarbon distribution of the products. CO conversion increased on the catalysts with the increase of zirconium loadings, which indicated that zirconium enhanced the activity of iron-cobalt catalysts. Low potassium loadings also enhanced the activity of the catalysts. However, high potassium loading made CO conversion on the catalysts decrease and weakened the secondary hydrogenations. The catalyst was characterized by BET, XRD and TPR. The catalyst characterization revealed that the Co3O4 phase was presented on the fresh catalyst, whereas the spinel phase of Fe-Co alloy and CoO existed on the used catalyst.

关键词： Fischer-Tropsch synthesis bimetallic iron cobalt promoter potassium zirconium

Intrinsic kinetics of methane aromatization under non-oxidative conditions over modified Mo/HZSM-5 catalysts

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Journal of Natural Gas Chemistry 2008年第1期17卷 64-68页

作者： Benzhen Yao Jin Chen Dianhua Liu dingye fang State Key Laboratory of Chemical Engineering East China University of Science and Technology Shanghai 200237 China

The intrinsic reaction kinetics of methane aromatization under non-oxidative conditions over modified Mo/HZSM-5 catalysts was studied in the quartz pipe-reactor under ordinary pressure with the temperature ranging from 913.15 to 973.15 K and the space velocity from 700 to 2100 ml/（g·h）. The Langmuir-Hinshelwood model was chosen to describe the intrinsic kinetics while Levenberg-Marquardt method was selected to determine the parameters in the kinetic model. Statistical test and residual error distribution diagrams showed that experimental data were in good agreement with calculated data, and Langmuir-Hinshelwood model was suitable for the description of the intrinsic kinetics of methane aromatization under the reaction conditions discussed in this article.

关键词： methane aromatization intrinsic kinetics Mo/HZSM-5 non-oxidative

Pretreatment of Alumina and Its Influence on the Properties of Co/Alumina Catalysts for Fischer-Tropsch Synthesis

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Journal of Natural Gas Chemistry 2007年第3期16卷 308-315页

作者： Chen Li Qiwen Sun Fahai Cao Weiyong Ying dingye fang State key Laboratory of Chemical Engineering School of Chemical Engineering East China University of Science and Technology Shanghai 200237 China School of Chemistry and Chemical Engineering Henan University of Technology Zhengzhou 450001 Henan China Yankuang Energy R ＆ D Co. Ltd. Shanghai 201203 China

16.6%Co/γ-Al2O3 catalysts prepared by incipient wetness impregnation method were used for Fischer-Tropsch synthesis. The support was pre-treated with different concentration of NH4NO3 aqueous solution. The effect of support pre-treatment on the properties of support and performance of supportedcobalt-based catalysts was investigated. To treat the support with NH4NO3 aqueous solution enlarged the pore of γ-Al2O3, decreased the impurity Na2O content, and weakened the surface acidity of γ-Al2O3. The change in the properties of the support decreased the interaction between cobalt species and support, enhanced the CO hydrogenation rate and the C5＋ selectivity. For all catalysts, increasing the reaction temperature increased the CO hydrogenation rate or the CO conversion, slightly decreased the total hydrocarbon selectivity, and favored the formation of methane and light hydrocarbons, while the chain growth probability decreased. For 16.6%Co/γ-Al2O3 catalysts, prepared with the support treated with 100 g/L NH4NO3 aqueous solution, the CO conversion, the CH4 selectivity, and the C5＋ selectivity were 83.13%, 6.86% and 82.75% respectively, and the chain growth probability was 0.83 under the condition of 493 K, 1.5 MPa, 500 h-1 and the molar ratio of H2 to CO being 2.0 in feed.

关键词： Fischer-Tropsch synthesis support pretreatment characterization C0/γ-Al2O3 CO conversion heavy hydrocarbon synthesis

Ni/Al_2O_3 catalysts for syngas methanation: Effect of Mn promoter

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Journal of Natural Gas Chemistry 2012年第2期21卷 170-177页

作者： Anmin Zhao Weiyong Ying Haitao Zhang Hongfang Ma dingye fang State Key Laboratory of Chemical Engineering Engineering Research Center of Large Scale Reactor Engineering and TechnologyMinistry of EducationEast China University of Science and TechnologyShanghai 200237China

Ni/Al2O3 catalysts with different amounts of manganese ranging from 1 to 3 wt% as promoter were prepared by co-impregnation method. The catalysts were characterized by N2 physisorption, XRD, TPR, SEM and TEM. Their catalytic activity towards syngas methanation reaction was also investigated using a fixed-bed integral reactor. It was demonstrated that the addition of manganese to Ni/Al2O3 catalysts can increase the catalyst surface area and average pore volume, but decrease NiO crystallite size, leading to higher activity and stability. The effects of reaction temperature, pressure and weight hourly space velocity （WHSV） on carbon oxides conversion and CH4 formation rate were also studied. High carbon oxides conversion, CH4 selectivity and formation rate were achieved at the reaction temperature range of 280 300℃.

关键词： manganese promotion nickel catalysts syngas methanation

Effect of copper loading on texture,structure and catalytic performance of Cu/SiO_2 catalyst for hydrogenation of dimethyl oxalate to ethylene glycol

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Journal of Natural Gas Chemistry 2012年第5期21卷 563-570页

作者： Bo Zhang Shengguo Hui Suhua Zhang Yang Ji Wei Li dingye fang State Key Laboratory of Chemical Engineering East China University of Science and TechnologyShanghai 200237China Pujing Chemical Industry(Sha)Limited Shanghai 200231China

Cu/SiO2 catalysts prepared by a convenient and efficient method using the urea hydrolysis deposition-precipitation （UHDP） technique have been proposed focusing on the effect of copper *** texture,structure and composition are systematically characterized by ICP,FTIR,N 2-physisorption,N2O chemisorption,TPR,XRD and *** formation of copper phyllosilicate is observed in Cu/SiO2 catalyst by adopting UHDP method,and the amount of copper phyllosilicate is related to copper *** is found the structure properties and catalytic performance is profoundly affected by the amount of copper *** excellent catalytic activity is attributed to the synergetic effect between Cu0 and Cu ＋.DMO conversion and EG selectivity are determined by the amount of Cu0 and Cu＋,*** proper copper loading （30 wt%） provides with the highest ratio of Cu ＋ /Cu0,giving rise to the highest EG yield of 95% under the reaction conditions of p=2.0 MPa,T=473 K,H2/DMO=80 and LHSV=1.0h-1.

关键词： Cu/SiO2 copper loading dimethyl oxalate ethylene glycol copper phyllosilicate