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Influence of gas Components on the Formation of Carbonyl Sulfide over water-gas shift Catalyst B303Q

Journal of Natural gas Chemistry 2007年第1期16卷 53-59页

作者： Ju Shangguan Litong Liang Huiling Fan Fang Shen Key Laboratory of Coal Science and Technology Taiyuan University of Technology Ministry of Education and Shanxi Province Taiyuan 030024 Shanxi China

water-gas shift reaction catalyst at lower temperature （200-400 ℃） may improve the conversion of carbon monoxide. But carbonyl sulfide was found to be present over the sulfided cobaltmolybdenum/alumina catalyst for water-gas shift reaction. The influences of temperature, space velocity, and gas components on the formation of carbonyl sulfide over sulfided cobalt-molybdenum/alumina catalyst B303Q at 200-400 ℃ were studied in a tubular fixed-bed quartz-glass reactor under simulated water-gas shift conditions. The experimental results showed that the yield of carbonyl sulfide over B303Q catalyst reached a maximum at 220 ℃ with the increase in temperature, sharply decreased with the increase in space velocity and the content of water vapor, increased with the increase in the content of carbon monoxide and carbon dioxide, and its yield increased and then reached a stable value with the increase in the content of hydrogen and hydrogen sulfide. The formation mechanism of carbonyl sulfide over B303Q catalyst at 200-400 ℃ was discussed on the basis of how these factors influence the formation of COS. The yield of carbonyl sulfide over B303Q catalyst at 200-400 ℃ was the combined result of two reactions, that is, COS was first produced by the reaction of carbon monoxide with hydrogen sulfide, and then the as-produced COS was converted to hydrogen sulfide and carbon dioxide by hydrolysis. The mechanism of COS formation is assumed as follows： sulfur atoms in the Co9Ss-MoS2/Al2O3 crystal lattice were easily removed and formed carbonyl sulfide with CO, and then hydrogen sulfide in the water-gas shift gas reacted with the crystal lattice oxygen atoms in CoO-MoOa/Al2O3 to form Co9S8-MoS2/Al2O3. This mechanism for the formation of COS over water-gas shift catalyst B303Q is in accordance with the Mars-Van Krevelen＇s redox mechanism over metal sulfide.

关键词： formation carbonyl sulfide sulfided cobalt-molybdenum/alumina catalyst water-gas shift

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Effects of CeO_2 on structure and properties of Ni-Mn-K/bauxite catalysts for water-gas shift reaction

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Journal of Rare Earths 2008年第3期26卷 352-356页

作者：江莉龙叶炳火魏可镁 National Engineering Research Center For Chemical Fertilizer Catalysts Fuzhou University

Multiple-metal catalysts （Ni-Mn-Ce-K/bauxite） for water-gas shift （WGS） reaction were prepared by impregnation, and the catalytic structure and properties were investigated by N2 physical, XRD, H2-TPR, and CO-TPD. The results indicated that the addition of 7.5% CeO2 improved the activity of the WGS reaction obviously, and also increased the specific surface area and pore volume of the catalysts. The addition of CeO2 decreases the reduction temperature, enhanced the adsorption and activation of H2O2, and improved the adsorption content of CO. Besides, active sites were not changed and the number of active sites on catalysts did not increase obviously.

关键词： impregnated water-gas shift bauxite CeO2 rare earths

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Effects of ZrO_2 Content on Structure and Performance of Cu/CeO_2-ZrO_2 Catalysts for water-gas shift Reaction

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Journal of Rare Earths 2005年第6期23卷 685-689页

作者：郑云弟林性贻郑起詹瑛瑛李达林魏可镁 National Engineering Research Center of Chemical Fertilizer Catalyst Fuzhou University Fuzhou 350002 China National

Cu/CeO2-ZrO2 catalysts for water-gas shift （WGS） reaction were prepared with co-precipitation method, and the influence of ZrO2 content on the catalytic structure and properties was investigated by the techniques of N2 physical adsorption analysis, XRD and H2-TPR. The results indicate that the BET surface areas of the catalysts are increased in varying degrees due to the presence of ZrO2. With increasing ZrO2 content, the pore size distribution is centered on 1.9 nm. ZrO2 can efficiently restrain the growth of Cu crystal particles. The appropriate amount of ZrO2 in the Cu/CeO2 catalysts can help the catalyst keep better copper dispersion in the WGS reaction, which can lead to both higher catalytic activity and better thermal stability. When ZrO2 content is 10% （atom fraction）, Cu/CeO2-Zr02 catalyst reaches a CO conversion rate of 73.7% at the reaction temperature of 200℃.

关键词： water-gas shift Cu/CeO2-ZrO2 catalyst rare earths

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Potassium-decorated active carbon supported Co-Mo-based catalyst for water-gas shift reaction

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Journal of Natural gas Chemistry 2011年第1期20卷 77-83页

作者： Yixin Lian RuiFen Xiao Weiping Fang Yiquan Yang National Engineering Laboratory for Green Chemical Productions of Alcohols Ethers and Esters College of Chemistry and Chemical Engineering Xiamen University Xiamen 361005 Fujian China Minnan Science and Technology Institute Fujian Normal University Quanzhou 362332 Fujian China

The effect of potassium-decoration was studied on the activity of water-gas shift （WGS） reaction over the Co-Mo-based catalysts supported on active carbon （AC）, which was prepared by incipient wetness co-impregnation method. The decoration of potassium on active carbon in advance enhances the activities of the CoMo-K/AC catalysts for WGS reaction. Highest activity （about 92% conversion） was obtained at 250 ？ C for the catalyst with an optimum K 2 O/AC weight ratio in the range from 0.12 to 0.15. The catalysts were characterized by TPR and EPR, and the results show that activated carbon decorated with potassium makes Co-Mo species highly dispersed, and thus easily reduced and sulfurized. XRD results show that an appropriate content of potassium-decoration on active carbon supports may favors the formation of highly dispersed Co 9 S 8 -type structures which are situated on the edge or a site in contact with MoS 2 , K-Mo-O-S, Mo-S-K phase. Those active species are responsible for the high activity of CoMo-K/AC catalysts.

关键词： active carbon potassium-decorated active phase Co-Mo-based catalyst water-gas shift

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Effect of yttrium addition on water-gas shift reaction over CuO/CeO_2 catalysts

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Journal of Rare Earths 2009年第3期27卷 412-418页

作者：佘育生李雷詹瑛瑛林性贻郑起魏可镁 National Engineering Research Center of Chemical Fertilizer Catalysts Fuzhou University

This paper presented a study on the role of yttrium addition to CuO/CeO2 catalyst for water-gas shift reaction. A single-step co-precipitation method was used for preparation of a series of yttrium doped CuO/CeO2 catalysts with yttrium content in the range of 0-5wt.%. Properties of the obtained samples were characterized and analyzed by X-ray diffraction （XRD）, Raman spectroscopy, H2-TPR, cyclic voltammetry （CV） and the BET method. The results revealed that catalytic activity was increased with the yttrium content at first, but then decreased with the further increase of yttrium content. Herein, CuO/CeO2 catalyst doped with 2wt.% of yttrium showed the highest catalytic activity （CO conversion reaches 93.4% at 250 ℃） and thermal stability for WGS reaction. The catalytic activity was correlated with the surface area, the area of peak γ of H2-TPR profile （i.e., the reduction of surface copper oxide （crystalline forms） interacted with surface oxygen vacancies on ceria）, and the area of peak C2 and A1 （Cu^0→←Cu^2＋ in cyclic voltammetry process）, respectively. Besides, Raman spectra provided evidences for a synergistic Cu-Ovacancy interaction, and it was indicated that doping yttrium may facilitate the formation of oxygen vacancies on ceria.

关键词： CuO/CeO2 catalyst water-gas shift yttrium cyclic voltammetry rare earths

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Zirconia modified monolithic macroporous Pt/CeO_2/Al_2O_3 catalyst used for water-gas shift reaction

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Journal of Rare Earths 2011年第8期29卷 753-757页

作者：梁皓苑宏刚魏枫张喜文刘源 Fushun Research Institute of Petroleum and Petrochemicals SINOPEC Fushun Environmental Science Academy Tianjin Key Laboratory of Applied Catalysis Science and Engineering Department of Catalysis Science and Technology School of Chemical Engineering and Technology Tianjin University

Monolithic macroporous Pt/CeO2/Al2O3 and zirconia modified Pt/CeO2/Al2O3 catalysts were prepared by using concentrated emulsions synthesis route. The catalytic performances over the platinum-based catalysts were investigated by water-gas shift （WGS） reaction in a wide temperature range （180–300 oC）. The samples were characterized with thermogravimetry （TG）, X-ray diffraction （XRD）, scanning electron microscopy （SEM）, high resolution transmission electron microscopy （HRTEM） and temperature programmed reduction （TPR） techniques as well. The SEM and HRTEM results indicated that the monoliths possessed macroporosity, in size of 5–50 μm, and platinum particles were homogeneously dispersed on macroporous materials. XRD and TPR results showed that the interaction between ceria and zirconia oxide was formed and the addition of zirconia could promote the reducibility of platinum oxide on the interface of ceria and zirconia particles, which led to an improvement of catalytic activity in WGS reaction. The results indicated that zirconia modified monolithic macroporous Pt/CeO2/Al2O3 could be fabricated in small size （from millimeter lever to centimeter） and had good reaction activity, which was a potential new route for miniaturization of the WGS reactor.

关键词： macroporous monolithic water-gas shift platinum zirconia rare earths

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Three-dimensionally ordered macro-porous Pt/TiO_2 catalyst used for water-gas shift reaction

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Journal of Natural gas Chemistry 2008年第4期17卷 403-408页

作者： Hao Liang Yuan Zhang Yuan Liu Department of Catalysis Science and Technology School of Chemical Engineering and Technology Tianjin University Tianjin 300072 China

Three-dimensionally ordered macro-porous （3DOM） Pt/TiO2 catalysts were prepared by template and impregnation methods, and the resultant samples were characterized by using TG-DTA, XRD, SEM, TEM, and TPR techniques. The catalytic performance for water-gas shift （WGS） reaction was tested, and the influences of some conditions, such as reduction temperature of catalysts, the amount of Pt loadings and space velocity on catalytic performance were investigated. It was shown that Pt particles were homogeneously dispersed on 3DOM TiO2. The reduction of TiO2 surface was important for the catalytic performance. The activity test results showed that the 3DOM Pt/TiO2 catalysts exhibited very good catalytic performance for WGS reaction even at high space velocity, which was owing to the better mass transfer of 3DOM porous structure besides the high intrinsic activity of Pt/TiO2.

关键词： three-dimensionally ordered macro-porous water-gas shift platinum titania

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A Modified Co-precipitation Method to Prepare Cu/ZnO/Al2O3 Catalyst and Its Application in Low Temperature water-gas shift(LT-WGS)Reaction

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Journal of Wuhan University of Technology(Materials Science) 2018年第4期33卷 876-883页

作者：许龙龙 PENG Dong LIU Wenhui FENG Yimin HOU Yanan LI Xiongjian 黄驰 Tianhua Chemical Branch Xi'an Sunward Aeromat Co.Ltd.Xi'an 710065China Sanjiang Chemical Factory of CSSG Yuanan 444200China College of Chemistry and Molecular Scienees Wuhan UniversityWuhan 430072China

A modified co-precipitation method for the production of Cu/ZnO/Al2O3 complex was studied. The modification was that part of Al was introduced by adding Al^（3＋） into Cu^（2＋）/Zn^（2＋） solution, and the rest of Al was added after co-precipitation step in the form of pseudo-boehmite. The prepared samples were characterized by different techniques such as X-ray diffraction, N2 adsorption, H2-N2O titration, temperature programmed reduction and scanning electron microscopy. X-ray diffraction characterizations revealed that Al^（3＋） can be doped in aurichalcite lattice, and the maximum doping amount of Al^（3＋） was 5.0% of total Cu and Zn atoms. The Cu/ZnO/Al2O3 sample produced by the modified method, in which co-precipitated Al^（3＋） was 2.5% of total Cu and Zn atoms showed much better activity and stability in water-gas shift reaction than commercial sample. The high Cu surface area（26.1 m^2/g） obtained by decompositon of doped aurichalcite is believed to be responsible for the activity enhancement. The stability was enhanced mainly because of the support effect of γ-Al2O3, which was decomposed from pseudo-boehmite in the calcination step.

关键词： Cu/ZnO/Al2O3 co-precipitation water-gas shift aurichalcite

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water gas shift activity of Co-Mo/MgO-Al_2O_3 catalysts presulfided with ammonium sulfide

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Journal of Natural gas Chemistry 2010年第1期19卷 61-66页

作者： Yixin Lian, Huifang Wang, Weiping Fang, Yiquan Yang Department of Chemistry, College of Chemistry and Chemical Engineering, National Engineering Laboratory for Green Chemical Productions of Alcohols, Ethers and Esters, Xiamen University, Xiamen 361005, Fujian, China Department of Chemistry College of Chemistry and Chemical Engineering National Engineering Laboratory for Green Chemical Productions of Alcohols Ethers and Esters Xiamen University Xiamen 361005 Fujian China

Co-Mo/MgO-Al2O3 catalyst was presulfided with ammonium sulfide in aqueous solution and activated with synthesis gas for water gas shift reaction. The assay results indicate that the presulfided Co-Mo/MgO-Al2O3 catalyst exhibits an excellent catalytic activity and stability. XRD and EPR characterization results show that the O-S exchange might occur during the impregnation, leading to the formation of （NH4）2MoS4 （or （NH4）zMoxSy） precursor, which was then thermally decomposed and reduced to MoS2. The higher catalytic performance is attributed to an optimization formation of active Co-Mo sulfides, consisting of well dispersed MoS2 and Co-Mo-S phase due to the redispersion of Co sulfide particles over the edges of newly formed MoS2 crystallites.

关键词： Co-Mo-based catalyst ammonium sulfide presulfidation water-gas shift

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Steam effects over Pd/Ce_(0.67)Zr_(0.33)O_2 three-way catalyst

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Journal of Rare Earths 2011年第3期29卷 217-224页

作者：王建强沈美庆王军王务林 Key Laboratory for Green Chemical Technology of State Education Ministry School of Chemical Engineering&TechnologyTianjin University China Automotive Technology&Research Center State Key Laboratory of Engines Tianjin University

In the purification process of automobile exhaust,existing water plays an important role as an oxidant,which converts CO and hydrocarbons（HCs） by the water-gas shift（WGS） and the steam reforming（SR） reactions,respectively,especially at high *** it is major component of the exhaust which can affect significantly the thermal stability of the three-way *** experiments were carried out close to the real operation conditions（GHSV,concentration,etc.） with a Pd/Ce0.67Zr0.33O2 catalyst supplying information on the CO and C3H8 oxidation reactions in feedstream formed by different reactant *** obtained results showed that the activity of the CO and C3H8 oxidation was promoted by the addition of steam due to the WGS and SR *** WGS and SR reaction were competitive under oxygen-lean *** kinetic analysis was considered for WGS and SR reactions.

关键词： three-way catalysts water-gas shift steam reforming turnover frequency compensation effect rare earths

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