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不同温度焙烧的Au-Pd/SiO2催化剂上甲醇选择性氧化制备甲酸甲酯

师瑞萍,  王辉,  朱华青,  吴志伟,  秦张峰,  樊卫斌,  王建国

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文章导航 > 燃料化学学报（中英文）  > 2012 >  (08): 985-991
师瑞萍, 王辉, 朱华青, 吴志伟, 秦张峰, 樊卫斌, 王建国. 不同温度焙烧的Au-Pd/SiO2催化剂上甲醇选择性氧化制备甲酸甲酯[J]. 燃料化学学报（中英文）, 2012, (08): 985-991.
引用本文: 师瑞萍, 王辉, 朱华青, 吴志伟, 秦张峰, 樊卫斌, 王建国. 不同温度焙烧的Au-Pd/SiO2催化剂上甲醇选择性氧化制备甲酸甲酯[J]. 燃料化学学报（中英文）, 2012, (08): 985-991.
shu
SHI Rui-ping, WANG Hui, ZHU Hua-qing, WU Zhi-wei, QIN Zhang-feng, FAN Wei-bin, WANG Jian-guo. Methanol selective oxidation to methyl formate on Au-Pd/SiO2 catalysts with different calcination temperatures[J]. Journal of Fuel Chemistry and Technology, 2012, (08): 985-991.
Citation: SHI Rui-ping, WANG Hui, ZHU Hua-qing, WU Zhi-wei, QIN Zhang-feng, FAN Wei-bin, WANG Jian-guo. Methanol selective oxidation to methyl formate on Au-Pd/SiO2 catalysts with different calcination temperatures[J]. Journal of Fuel Chemistry and Technology, 2012, (08): 985-991.
shu

不同温度焙烧的Au-Pd/SiO2催化剂上甲醇选择性氧化制备甲酸甲酯

  • 1.

    中国科学院山西煤炭化学研究所 煤转化国家重点实验室, 山西 太原 030001;

  • 2.

    中国科学院研究生院, 北京 100049

基金项目: 国家自然科学基金(20773155); 山西省科技重大专项(20111101005); 山西省自然科学基金(201101106-3)。
详细信息
    通讯作者:

    朱华青, Tel: 0351-4046092; Fax: 0351-4041153; E-mail:zhuhq@sxicc.ac.cn; 王建国, Tel: 0351-4046092; Fax: 0351-4041153; E-mail:iccjgw@sxicc.ac.cn.

  • 中图分类号: O643.36

Methanol selective oxidation to methyl formate on Au-Pd/SiO2 catalysts with different calcination temperatures

  • 1.

    State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China;

  • 2.

    Graduate University of Chinese Academy of Sciences, Beijing 100049, China

    摘要
  • 摘要: 以溶胶固定法制备了Au-Pd/SiO2催化剂,考察了催化剂焙烧温度对甲醇选择氧化制甲酸甲酯反应性能的影响。在200~500℃,400℃焙烧的Au-Pd/SiO2具有最好的低温催化性能,在室温下就有活性,反应温度为100℃时甲醇转化率为25.3%,甲酸甲酯的选择性为100%。采用BET、XRD、UV-vis DRS、XPS、TEM和DRIFTS技术对催化剂进行表征,结果表明,催化剂中活性组分Au和Pd的高分散性,合适的Au和Pd粒径,Au-Pd合金的形成以及Au和Pd之间的强相互作用力,有利于甲醇氧化为甲酸甲酯反应的进行。初步推测出了甲醇在Au-Pd/SiO2上氧化为甲酸甲酯的反应机理,甲醇在Au-Pd/SiO2催化剂上是通过甲氧基中间体得到甲酸甲酯的。
    Abstract: Au-Pd/SiO2 catalysts with different calcination temperatures were prepared by sol-immobilization method; their catalytic performance in oxidation of methanol to methyl formate was investigated. Among 200~500℃, Au-Pd/SiO2 catalyst calcined at 400℃ exhibits the best catalytic activity in the topic reaction at room temperature, and 25.3% methanol conversion with 100% selectivity to methyl formate can be achieved at100℃. They were characterized by BET, XRD, UV-vis DRS, XPS, TEM and DRIFTS. Good dispersity of Au and Pd, proper particle size of Au and Pd, the formation of Au-Pd bimetallic nanoparticles, and strong interaction between Au and Pd in the Au-Pd/SiO2 catalyst are beneficial to the oxidation of methanol to methyl formate. Furthermore, a preliminary reaction mechanism of methanol oxidation to methyl formate on the Au-Pd/SiO2 catalyst is inferred and methyl formate is gained from intermediate species methoxy in this reaction mechanism.
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  • HUGHES M D, XU Y J, JENKINS P, MCMORN P, LANDON P, ENACHE D I, CARLEY A F, ATTARD G A, HUTCHINGS G J, KING F, STITT E H, JOHNSTON P, GRIFFIN K, KIELY C J. Tunable gold catalysts for selective hydrocarbon oxidation under mild conditions[J]. Nature, 2005, 437(7062): 1132-1135.
    GERARD E, GOTZ H, PELLEGRINI S, CASTANET Y, MORTREUX A. Epoxide-tertiary amine combinations as efficient catalysts for methanol carbonylation into methyl formate in the presence of carbon dioxide[J]. Appl Catal A, 1998, 170(2): 297-306.
    LIU J L, ZHAN E S, CAI W J, LI J, SHEN W J. Methanol selective oxidation to methyl formate over ReOx/CeO2 catalysts[J]. Catal Lett, 2008, 120(3/4): 274-280.
    AI M. The production of methyl formate by the vapor-phase oxidation of methanol[J]. J Catal, 1982, 77(1): 279-288.
    BUSCA G, AHMED S, ELMI, FORZATTI P. Mechanism of selective methanol oxidation over vanadium oxide-titanium oxide catalysts: A FT-IR and flow reactor study[J]. J Phys Chem, 1987, 91(20): 5263-5269.
    ROYER S, SCORDEL X, BRANDHORST M, DUMEIGNIL F, CRISTOL S, DUJARDIN C, CAPRON M, PAYEN E, DUBOIS J. Amorphous oxide as a novel efficient catalyst for direct selective oxidation of methanol to dimethoxymethane[J]. Chem Commun, 2008, 7(6): 865-867.
    WANG H, ZHU H Q, QIN Z F, LIANG F X, WANG G F, WANG J G. Deactivation of a Au/CeO2-Co3O4 catalyst during CO preferential oxidation in H2-rich stream[J]. J Catal, 2009, 264(2): 154-162.
    YI N, SI R, SALTSBURG H, FLYTZANI-STEPHANOPOULOS M, ENERGY ENVIRON. Active gold species on cerium oxide nanoshapes for methanol steam reforming and the water gas shift reactions[J]. Energy Environ Sci, 2010, 3(6): 831-837.
    HUTCHINGS G J. Nanocrystalline gold and gold palladium alloy catalysts for chemical synthesis[J]. Chem Commun, 2008, 10(7): 1148-1164.
    WITTSTOCK A, ZIELASEK V, BIENER J, FRIEND C. M, BUMER M. Nanoporous gold catalysts for selective gas-phase oxidative coupling of methanol at low temperature[J]. Science, 2010, 327(5963): 319-322.
    LICHTENBERGER J, LEE D, IGLESIA E. Catalytic oxidation of methanol on Pd metal and oxide clusters at near-ambient temperatures[J]. Phys Chem Chem Phys, 2007, 9(35): 4902-4906.
    KESAVAN L, TIRUVALAM R, RAHIM M A B, SAIMAN M I B, ENACHE D I, JENKINS R L, DIMITRATOS N, LOPEZ-SANCHEZ J A, TAYLOR S H, KNIGHT D W, KIELY C J, HUTCHINGS G J. Solvent-free oxidation of primary carbon-hydrogen bonds in toluene using Au-Pd alloy nanoparticles[J]. Science, 331(6014): 195-199.
    TAN L F, CHEN D, LIU H Y, TANG F Q. A silica nanorattle with a mesoporous shell: An ideal nanoreactor for the preparation of tunable gold cores[J]. Adv Mater, 2010, 22(43): 4885-4889.
    XU J, WHITE T, LI P, HE C H, YU J G, YUAN W K, HAN Y F. Biphasic Pd-Au alloy catalyst for low-temperature CO oxidation[J]. J Am Chem Soc, 2010, 132(30): 10398-10406.
    WANG A Q, CHANG C M, MOU C Y. Evolution of catalytic activity of Au-Ag bimetallic nanoparticles on mesoporous support for CO oxidation[J]. J Phys Chem B, 2005, 109(40): 18860-18867.
    LU C L, PRASAD K S, WU H L, HO J A, HUANG M H. Au nanocube-directed fabrication of Au-Pd core-shell nanocrystals with tetrahexahedral, concave octahedral, and octahedral structures and their electrocatalytic activity[J]. J Am Chem Soc, 2010, 132(41): 14546-14553.
    XU J G, WILSON A R, RATHMELL A R, HOWE J, CHI M F, WILEY B J. Synthesis and catalytic properties of Au-Pd nanoflowers[J]. Acs Nano, 2011, 5(8): 6119-6127.
    WU M L, CHEN D H, HUANG T C. Synthesis of Au/Pd bimetallic nanoparticles in reverse micelles[J]. Langmuir, 2001, 17(13): 3877-3883.
    HU J W, ZHANG Y, LI J F, LIU Z, REN B, SUN S G, TIAN Z Q, LIAN T. Synthesis of Au@Pd core-shell nanoparticles with controllable size and their application in surface-enhanced raman spectroscopy[J]. Chem Phys Lett, 2005, 408(4/6): 354-359.
    MULVANEY P, GIERSIG M, HENGLEIN A. Surface chemistry of colloidal gold: Deposition of lead and acompanying optical effects[J]. J Phys Chem, 1992, 96(25): 10419-10424.
    LEE Y S, JEONY Y S, CHUNG Y D, LIM K Y, WHANG C N, OH S J. Charge redistribution and electronic behavior in Pd-Au aloys[J]. J Korean Chem Soc, 2000, 37(4): 451-455.
    PRITCHARD J, KESAVAN L, PICCININI M, HE Q, TIRUVALAM R, DIMITRATOS N, LOPEZ-SANCHEZ J A, CARLEY A F, EDWARDS J K, KIELY C J, AND HUTCHINGS G J. Direct synthesis of hydrogen peroxide and benzyl alcohol oxidation using Au-Pd catalysts prepared by sol immobilization[J]. Langmuir, 2010, 26(21): 16568-16577.
    RASKJ, BONTOVICS J, SOLYMOSI F. FTIR study of the interaction of methanol with clean and potassium-doped Pd/SiO2 catalysts[J]. J Catal, 1994, 146(1): 22-33.
    GRISELDA G C, ADRIÁN L, BONIVARDI A L, BALTANÁS M A. FTIR study of the adsorption of methanol on clean and Ca-promoted Pd/SiO2 catalysts[J]. J Catal, 2001, 201(2): 213-220.
    LOCHARV. FT-IR study of methanol, formaldehyde and methyl formate adsorption on the surface of Mo/Sn oxide catalyst[J]. Appl Catal A, 2006, 309(1): 33-36.
    XU B Q, LIU X Y, HAUBRICH J, MADIX R J, FRIEND C M. Selectivity control in gold-mediated esterification of methanol[J]. Angew Chem Int Ed, 2009, 48(23): 4206-4209.
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出版历程
  • 收稿日期:  2011-11-03
  • 修回日期:  2012-02-17
  • 刊出日期:  2012-08-31

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