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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

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

Mass Transfer Characteristics of H_2 and CO in Mimicked F-T Slurry Bubble Column Reactor

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China Petroleum Processing & Petrochemical Technology 2018年第2期20卷 111-118页

作者： Wu Jianmin sun qiwen Zhang Zongsen Yankuang Energy R&D Co. Ltd.State Key Laboratory of Coal Liquefaction and Coal Chemical Technology

The equilibrium solubilities,volumetric gas-liquid mass transfer coefficients kLa of H_2 and CO were measured as functions of temperature(298―513 K),pressure(1―3 MPa),superficial gas velocity(0.5―3 cm/s) and solid volume fraction(5%―25%) in liquid paraffin/iron-based catalyst slurry bubble column *** volumetric mass transfer coefficients kLa were obtained by measuring the dissolution rate of H_2 and *** influences of the operation conditions,such as pressure,temperature,superficial gas velocity and catalyst concentration on kLa,were *** empirical correlations were proposed to predict kLa values of H_2 and CO in liquid paraffin/solid particles slurry bubble column *** results showed that the equilibrium solubilities of H-2 and CO increased with an increasing temperature and pressure,and the solubility of CO was greater than that for H_*** was found that the equilibrium solubility can be expressed by Henry's *** volumetric mass transfer coefficients of H_2 and CO were of the same order of magnitude,and increased with the increase of pressure,temperature and superficial gas *** presence of solid particles decreased kLa values of both H_2 and CO.

关键词： slurry bubble column reactor solubility volumetric mass transfer coeffcient iron-based catalyst

Effect of the operation parameters on the Fischer-Tropsch synthesis in fluidized bed reactors

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Chinese Journal of Chemical Engineering 2018年第2期26卷 245-251页

作者： Xiaolai Zhang Weixin Qian Haitao Zhang qiwen sun Weiyong Ying Engineering Research Center of Large Scale Reactor Engineering and Technology Ministry of EducationState Key Laboratory of Chemical EngineeringEast China University of Science and TechnologyShanghai 200237China State Key Laboratory of Coal Liquefaction and Coal Chemical Technology Shanghai 201203China

For the Fischer-Tropsch synthesis （FrS）, this paper presents a numerical investigation in a 3D fiuidized bed reactor. The effect of the operation parameters such as bed temperature, superficial gas velocities, particle size and bed heights is discussed. A 3D-CFD model coupled with FTS chemical kinetics was set up. The computational resuits are compared with experimental data in terms of the components production rates, etc. The analysis shows that the bed heights, the bed temperature, the superficial gas velocities and particle sizes affect the C5 ＋ selectivity and the reaction rates. Product yields are dependent on the operating conditions especially the temperature.

关键词： Fluidized bed Fischer-Tropsch synthesis CFD

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

Online measurement of solids motion in fluidized bed reactor with different distributor for Fischer–Tropsch synthesis

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Chinese Journal of Chemical Engineering 2018年第10期26卷 2003-2008页

作者： Xiaolai Zhang Weixin Qian Haitao Zhang qiwen sun Weiyong Ying Engineering Research Centre of Large Scale Reactor Engineering and Technology Ministry of Education State Key Laboratory of Chemical Engineering East China University of Science and Technology Shanghai 200237 China State Key Laboratory of Coal Liquefaction and Coal Chemical Technology Shanghai 201203 China

In this paper, the distributions of particle velocity in a gas–solid fluidized bed with branched pipe distributor or circle distributor were measured by using a laser Doppler velocimetry. Our results show that, within a certain range of superficial gas velocity, when using circle distributor, the particle velocity is large and the distribution of the particle velocity is even more compared with the branched pipe distributor. On the basis of the amplitude of tangential movement statistics, the amplitude of tangential movement statistics(AVATMS) decreases with increasing the axial height under the appropriate superficial gas velocity.

关键词： Fischer–Tropsch synthesis Laser Doppler velocimetry Fluidized bed

Numerical simulation of effect of gas distributor on Fischer-Tropsch synthesis in fluidized-bed reactor

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Particuology 2019年第4期17卷 98-104页

作者： Xiaolai Zhang Guangwei Zhai Weixin Qian Haitao Zhang qiwen sun Weiyong Ying Engineering Research Center of Large Scale Reactor Engineering and Technology Ministry of Education State Key Laboratory of Chemical Engineering East China University of Science and Technology Shanghai 200237 China State Key Laboratory of Coal Liquefaction and Coal Chemical Technology Shanghai 201203 China

Circular and branched pipe distributors were designed for Fischer-Tropsch synthesis in a fluidized-bed reactor. A numerical investigation of the effects of these distributors on product selectivity and production rate was performed. Under the same conditions, the circular distributor gave higher production rates for small diameter particles. For superficial gas velocities ranging from 5 to 15 times the minimum fluidization velocity, the production rates of methane and C5+(the sum of C10H22 and C22H46)were 18%, which was 2% higher than those using the branched pipe distributor, while the C5+ selectivity was 1% lower. For deeper beds, the circular distributor led to higher production rates and the selectivity for C5+ was 5% lower than that using the branched pipe distributor.

关键词： Fischer-Tropsch synthesis Fluidized bed Gas distributor Numerical simulation

Diffusion and Reaction Model of Catalyst Pellets for Fischer-Tropsch Synthesis

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China Petroleum Processing & Petrochemical Technology 2013年第4期15卷 77-86页

作者： Wu Jianmin sun qiwen Zhang Zongsen Pang Lifeng Yankuang Energy R&D Co. Ltd. State Key Laboratory of Coal Liquefaction and Coal Chemical Technology

The diffusion and reaction phenomenon in a Fe-based catalyst pellet for Fischer-Tropsch synthesis was studied. It was considered that the pores of catalyst pellets were full of liquid wax under Fischer-Tropsch synthesis conditions. The re- actants diffused from the bulk gas phase to the external surface of the pellet, and then the reactants diffused through the wax inside the pellet and reacted on the internal surface formed along the pore passages of the pellet. On the basis of reaction kinetics and double a-ASF product distribution model, a diffusion and reaction model of catalyst pellet was established. The effects of diffusion and reaction interaction in a catalyst pellet, the bulk temperature, the reaction pressure and the pellet size on the reactivity were further investigated. The relationship between the internal diffusion effectiveness factor of spherical catalyst pellet and the Thiele modulus were also discussed. The bulk temperature and pellet size have significant effects on the reactivity, while the pressure shows only a slight influence on the reactivity. The internal diffusion effectiveness factor decreases with an increasing Thiele modulus.

关键词： Fischer-Tropsch synthesis diffusion and reaction catalyst pellet internal diffusion effectiveness factor

Effects of the Different Supports on the Activity and Selectivity of Iron-Cobalt Bimetallic Catalyst for Fischer-Tropsch Synthesis

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Journal of Natural Gas Chemistry 2006年第4期15卷 335-339页

作者： Xiangdong Ma 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 Shanghai Yankuang Energy R＆D Co. Ltd. Shanghai 201203 China

Silica, alumina, and activated carbon supported iron-cobalt catalysts were prepared by incipient wetness impregnation. These catalysts have been characterized by BET, X-ray diffraction （XRD）, and temperature-programmed reduction （TPR）. Activity and selectivity of iron-cobalt supported on different carriers for CO hydrogenation were studied under the conditions of 1.5 MPa, 493 K, 630 h^-1, and H2/CO ratio of 1.6. The results indicate that the activity, C4 olefin/（C4 olefin＋C4 paraffin） ratio, and C5 olefin/（C5 olefin＋C5 paraffin） decrease in the order of Fe-Co/SiO2, Fe-Co/AC1, Fe-Co/Al2O3 and Fe- Co/AC2. The activity of Fe-Co/SiO2 reached a maximum. The results of TPR show that the Fe-Co/SiO2 catalyst is to some extent different. XRD patterns show that the Fe-Co/SiO2 catalyst differs significantly from the others; it has two diffraction peaks. The active spinel phase is correlated with the supports.

关键词： Fischer-Tropsch synthesis bimetallic catalyst iron cobalt support silica alumina active carbon syngas

LDV measurements of particle velocity distribution in an annular stripper

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Chinese Journal of Chemical Engineering 2019年第10期27卷 2293-2303页

作者： Yongzheng Li Xiaolai Zhang Guangwei Zhai Haitao Zhang Tao Li qiwen sun Weiyong Ying Engineering Research Center of Large Scale Reactor Engineering and Technology Ministry of EducationState Key Laboratory of Chemical EngineeringEast China University of Science and TechnologyShanghai 200237China School of Chemistry and Chemical Engineering Shandong UniversityJinan 250100China State Key Laboratory of Coal Liquefaction and Coal Chemical Technology Shanghai 201203China

Particle descent velocities in an annular stripper were measured by a laser Doppler velocimetry(LDV)*** the radial direction,particle descent velocity was relatively constant in the mid-region of the stripper and increased towards the walls on both sides,exhibiting an anti-U-shaped *** descent velocity in the radial mid-region increased with the increase of superficial gas velocity,and the maximum in the outer wall region increased significantly with the increase of solid mass *** stripping gas velocity had stronger effect on particle velocity distributions near the stripper gas distributor,and such effect weakened with the increase of the distance from the *** particle velocity and its radial profiles could be adjusted by changing the superficial stripping gas *** formulas were established to describe the relationships between the local particle velocity and cross-sectional averaged velocity based on the effects of operating conditions and measuring *** result showed that the predicted data was in good agreement with the experimental value.

关键词： Annular stripper Flow Hydrodynamics Particle velocity Laser Doppler velocimeter