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Effects of cobalt carbide on fischer–tropsch synthesis with MnO supported Co-based catalysts

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Journal of Energy Chemistry 2020年第3期29卷 227-232页

作者： Fanfei Sun Ruoou Yang Zhaoming Xia Yuqi Yang Ziang Zhao Songqi Gu Dongshuang Wu Yunjie Ding Zheng Jiang Shanghai Institute of Applied Physics Chinese Academy of SciencesShanghai 201204China Shanghai Synchrotron Radiation Facility Zhangjiang LaboratoryShanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201210China University of Chinese Academy of Sciences Beijing 100100China Center for Applied Chemical Research Frontier Institute of Science and TechnologyXi’an Jiaotong UniversityXi’an 710049ShaanxiChina Dalian National Laboratory for Clean Energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina Graduate school of science Kyoto UniversityKitashirakawaOiwake-choSakyo-kuKyoto-shiKyoto-fu606-8502Japan

Cobalt carbide(Co2C)was considered as potential catalysts available for large-scale industrialization of transforming syngas(H2 and CO)to clean fuels.Herein,we successfully synthesized Co-based catalysts with MnO supported,to comprehend the effects of Co2C for fischer–tropsch synthesis(FTS)under ambient conditions.The huge variety of product selectivity which was contained by different active sites(Co and Co2C)has been found.Furthermore,density functional theory(DFT)shows that Co2C is efficacious of CO adsorption,whereas is weaker for H adsorption than Co.Combining the advantages of Co and Co2C,the catalyst herein can not only obtain more C5+products but also suppress methane selectivity.It can be a commendable guide for the design of industrial application products in FTS.

关键词： Cobalt carbide fischer–tropsch synthesis X-ray absorption fine spectroscopy nanomaterials Density functional theory

Light olefin production by catalytic co-cracking of fischer–tropsch distillate with methanol and the reaction kinetics investigation

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Chinese Journal of Chemical Engineering 2020年第1期28卷 143-151页

作者： Hui Zou Teng Pan Yanwen Shi Youwei Cheng Lijun Wang Yu Zhang Xi Li Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027China Institute of Zhejiang University Jiuhua Boulevard NorthQzhou 324000China Ningxia Shenyao Technology Co. Ltd.China Energy Investment Co.West Desheng Road 1Yinchuan 750200China

Catalytic co-cracking of fischer–tropsch(FT) light distillate and methanol combines highly endothermic olefin cracking reaction with exothermic methanol conversion over ZSM-5 catalyst to produce light olefins through a nearly thermoneutral process. The kinetic behavior of co-cracking reactions was investigated by different feed conditions: methanol feed only, olefin feed only and co-feed of methanol with olefins or F–T distillate. The results showed that methanol converted to C2–C6 olefins in first-order parallel reaction at low space time, methylation and oligomerization–cracking prevailed for the co-feed of methanol and C2–C5 olefins, while for C6–C8 olefins,monomolecular cracking was the dominant reaction whether fed alone or co-fed with methanol. For FT distillate and methanol co-feed, alkanes were almost un-reactive, C3–C5 olefins were obtained as main products, accounting for 71 wt% for all products. A comprehensive co-cracking reaction scheme was proposed and the model parameters were estimated by the nonlinear least square method. It was verified by experimental data that the kinetic model was reliable to predict major product distribution for co-cracking of FT distillate with methanol and could be used for further reactor development and process design.

关键词： fischer–tropsch distillate Catalytic co-cracking Light olefins Methanol Reaction kinetics

Reduction and carburization of iron oxides for fischer–tropsch synthesis

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Journal of Energy Chemistry 2020年第12期29卷 48-61页

作者： Monia Runge Nielsen Asger Barkholt Moss Anton Simon Bjrnlund Xi Liu Axel Knop-Gericke Alexander YuKlyushin Jan-Dierk Grunwaldt Thomas LSheppard Dmitry EDoronkin Anna Zimina Thomas Eric Lyck Smitshuysen Christian Danvad Damsgaard Jakob Birkedal Wagner Thomas Willum Hansen DTU Nanolab Technical University of DenmarkDK-2800Kgs.LyngbyDenmark Department of Physics Technical University of DenmarkDK-2800Kgs.LyngbyDenmark SynCat@Beijing Synfuels China Technology Co.LtdBeijing 101407China School of Chemistry and Chemical Engineering Shanghai Jiao Tong UniversityShanghai 200240China Department of Inorganic Chemistry Fritz Haber Institute of the Max Planck SocietyD-14195 BerlinGermany Research Group Heterogeneous Reactions.Max Planck Institute for Chemical Energy Conversion D-45470 MulheimGermany Research Group Catalysis for Energy Helmholtz-Zentrum Berlin for Materials and Energy(BESSYⅡ)D-12489 BerlinGermany Institute for Chemical Technology and Polymer Chemistry Karlsruhe Institute of TechnologyD-76131 KarlsruheGermany Institute of Catalysis Research and Technology Karlsruhe Institute of TechnologyD-76344 Eggenstein-LeopoldshafenGermany

The activation of iron oxide fischer–tropsch Synthesis(FTS) catalysts was investigated during pretreatment: reduction in hydrogen followed by carburization in either CO or syngas mixture, or simultaneously reduction and carburization in syngas. A combination of different complementary in situ techniques was used to gain insight into the behavior of Fe-based FTS catalysts during activation. In situ XRD was used to identify the crystalline structures present during both reduction in hydrogen and carburization. An increase in reduction rate was established when increasing the temperature. A complete reduction was demonstrated in the ETEM and a grain size dependency was proven, i.e. bigger grains need higher temperature in order to reduce. XPS and XAS both indicate the formation of a small amount of carbonaceous species at the surface of the bulk metallic iron during carburization.

关键词： In situ characterization fischer–tropsch Catalyst reduction and carburization Iron oxides

Research Trends in fischer-tropsch Catalysis for Coal to Liquids Technology

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Frontiers of Engineering Management 2016年第4期3卷 321-330页

作者： Emiel J.M.Hensen Peng Wang Wayne Xu Laboratory of Inorganic Materials Chemistry Schuit Institute of CatalysisDepartment of Chemical Engineering and ChemistryEindhoven University of Technology National Institute of Clean-and-Low-Carbon Energy (NICE) Shenhua NICEFuture Science & Technology City

fischer–tropsch Synthesis(FTS) constitutes catalytic technology that converts synthesis gas to synthetic liquid fuels and chemicals.While synthesis gas can be obtained from any carbonaceous feedstock,current industrial FTS operations are almost exclusively based on natural gas.Due to the energy structure of China where cheap coal is abundant,coal to liquids(CTL) technology involving coal gasification,FTS and syncrude upgrading is increasingly being considered as a viable option to convert coal to clean transportation fuels.In this brief paper,we review some pertinent issues about Fe-and Co-based FTS catalysts.Fe is better suited to convert synthesis gas derived from coal gasification into fuels.The authors limit themselves to noting some important trends in the research on Fe-based catalysts.They focus on the preparation of phase-pure carbides and innovative cheap synthesis methods for obtaining active and stable catalysts.These approaches should be augmented by(1) computational investigations that are increasingly able to predict not only mechanism,reaction rates and selectivity but also optimum catalyst composition,as well as(2) characterization of the catalytic materials under conditions close to the operation in real reactors.

关键词： fischer–tropsch FTS CTL Fe catalyst iron carbide computational modeling

Polyaniline-supported iron catalyst for selective synthesis of lower olefins from syngas

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Journal of Energy Chemistry 2017年第4期26卷 608-615页

作者： Bang Gu Shun He Wei Zhou Jincan Kang Kang Cheng Qinghong Zhang Ye Wang State Key Laboratory of Physical Chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy MaterialsNational Engineering Laboratory for Green Chemical Productions of AlcoholsEthers and EstersCollege of Chemistry and Chemical EngineeringXiamen University

Uniform iron nanoparticles dispersed on polyaniline have been used as catalysts for the direct conversion of synthesis gas into lower olefins. As compared to active carbon and N-doped active carbon, polyaniline as a support of Fe catalysts showed higher selectivity of lower olefins(C;=). The C;=selectivity reached;0% at a CO conversion of 79% over a 10 wt% Fe/polyaniline catalyst without any promoters.The XRD, H;-TPR, TEM and HRTEM studies revealed that the presence of nitrogen-containing groups in polyaniline structure could promote the dispersion and reduction of iron oxides, forming higher fraction of iron carbides with smaller mean sizes and narrower size distributions. The propylene-TPD result indicates that the use of polyaniline support facilitates the desorption of lower olefins, thus suppressing the consecutive hydrogenation to form undesirable lower paraffins.

关键词： Polyaniline Iron catalyst Lower olefins fischer–tropsch Electron effect