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Student Number 983204024
Author Jiun Wang(王駿)
Author's Email Address No Public.
Statistics This thesis had been viewed 480 times. Download 11 times.
Department Chemical and Materials Engineering
Year 2010
Semester 2
Degree Master
Type of Document Master's Thesis
Language zh-TW.Big5 Chinese
Title Selective hydrogenation of α,β-unsaturated aldehydes on Ag/Mg2AlO-hydrotalcite catalyst
Date of Defense 2011-06-15
Page Count 112
Keyword
  • hydrotalcite
  • selective hydrogenation
  • silver catalyst
  • unsaturated aldehydes
  • Abstract Silver is dispersed on a solid base of Mg2AlO-hydrotalicite using a wet impregnation method to obtain a effective catalyst for selective hydrogenation of alpha,beta-unsaturated aldehydes.
    In the present study, 5wt% Ag/Mg2AlO catalysis on liquid-phase hydrogenation of a citral mode reactant. We disussed the experiment factors such as solvent effect, the whole phenomenon of hydrogenation, the molecular structure of reactants, steric effect and other impact from the experimental changes. The silver catalyst is characteristized by TGA, BET, TEM, XRD, TPR, TPD. In addition, we used γ-Al2O3, MgO, CeO2, SiO2 as support to observe the impact of support effect.
      The optimal catalyst, 5wt% Ag/Mg2AlO, was prepared by following process: Mg2AlO calcined at 100 °C as a support , 5wt% Ag/Mg2AlO catalyst calcined at 250 °C, and reducted at 400 oC before the catalysis. 5wt% Ag/Mg2AlO catalyst display effectively chemoselective hydrogenation of citral into unsaturated alcohols (Nerol and Geriol) for selectivity of 97%.
      The interaction force of unsaturated aldehyde molecule adsorbed on the surface of the silver metal catalyst, is different from the convalent force of conventional hydrogenation catalyst (Pt, Ni, etc), making the 5wt% Ag/Mg2AlO catalyst in citral reaction from a general catalytic behavior of metal catalysts. The C=O bond of conjugated C=C/C=O bond was hydrogenated prioritily; the remained C=C bond from conjugated C=C/C=O bond would not be hydrogenated continuously. The longer fuctional group of unsaturated aldehyde molecule, the greater catalytic activity.The 5wt% Ag/Mg2AlO has better citral hydrogenation activity in polar solvents than in nonpolar solvent. Higher alcohol carbon number can offer the catalytic better reactivity, but the unsaturated alcohol selectivity is slightly decreased.
      In the discussion of support effect, we conclude the activity of silver catalyst is proportional the relations with the base site concentration of support. The particle size of the silver catalyst is not affect the activity obviously. The base sites of support can promote hydrogen dissociated on the surface of silver-based catalyst. Among the supports in study, Mg2AlO-hydrotalcite in α,β-unsaturated aldehyde hydrogenation can be obtained the high potency silver catalyst.
    Table of Content 摘 要i
    目 錄v
    圖 目 錄viii
    表 目 錄xi
    第一章 緒論1
    第二章 文獻回顧4
    2-1 銀觸媒的發展史4
    2-2 MgxAlO-hydrotalcite 擔體6
    2-2-1 MgxAlO-hydrotalcite 結構性質6
    2-2-2 MgxAlO-hydrotalcite 之製備7
    2-2-3 MgxAlO-hydrotalcite 熱處理性質8
    2-2-4 MgxAlO-hydrotalcite 觸媒酸鹼性質11
    2-3 α,β-不飽和醛選擇性氫化反應14
    2-3-1 第VIII族過渡金屬15
    2-3-2 鉑金屬觸媒16
    2-3-2-(a) 擔體效應16
    2-3-2-(b) 金屬顆粒大小之影響18
    2-3-2-(c) 促進劑之影響20
    2-3-2-(d) 溶劑效應22
    2-3-3 金觸媒23
    2-3-3-(a) 金顆粒的大小與型態23
    2-3-3-(b) 擔體性質27
    2-3-4 銀觸媒28
    2-3-4-(a) 金屬顆粒大小與表面型態之影響28
    2-3-4-(b) 擔體性質31
    2-3-4-(c) 溶劑效應32
    第三章 實驗方法與設備33
    3-1 Mg2AlO-hydrotalcite擔體之製備33
    3-2 Ag/Mg2AlO-hydrotalcite 觸媒之製備34
    3-3 擔體與觸媒性質鑑定36
    3-3-1 熱重分析儀 (TGA)36
    3-3-2 X-射線繞射分析 (XRD)36
    3-3-3 比表面積測定 (BET)36
    3-3-4 Χ-射線光電子光譜 (XPS)37
    3-3-5 穿透式電子顯微鏡 (TEM)38
    3-3-6 氫氣程式升溫還原 (H2 - TPR)39
    3-3-7 二氧化碳程溫脫附 (CO2 - TPD)41
    3-4 反應活性測試43
    3-5 實驗藥品及氣體47
    第四章 結果與討論50
    4-1 Ag/Mg2AlO-hydrotalcite 於檸檬醛選擇性氫化反應50
    4-1-1 觸媒製備條件篩選51
    4-1-1-(a) Mg2AlO擔體煅燒溫度之影響51
    4-1-1-(b) 觸媒煅燒溫度之影響56
    4-1-1-(c) 觸媒氫氣還原之影響60
    4-1-1-(d) 銀負載量之影響71
    4-1-2 溶劑效應75
    4-1-3 全程氫化現象80
    4-2 反應物分子大小與立體障礙效應83
    4-3 擔體效應88
    第五章 結論94
    總 結95
    參考文獻96
    附錄一 Ag/support觸媒於檸檬醛氫化研究105
    Reference [1]V. Ponec, “On the role of promoters in hydrogenateon on metals: α,β-unsaturated aldehydes and ketones,” Appl. Catal. A 149 (1997) 27-48.
    [2]N. Mahata, F. Goncalves, M. Fernando, R. Pereira and J. L. Figueiredo, “Selective hydrogenation of cinnamaldehyde to cinnamyl alcohol over mesoporous carbon supported Fe and Zn promoted Pt catalyst,” Appl. Catal. A 339 (2008) 159-168.
    [3]D. Goupil, P. Fouilloux and R. Maurel, “Activity and selectivity of Pt-Fe/C alloys for the liquid phase hydrogenation of cinnamaldehyde to cinnamyl alcohol,” React. Kinet. Catal. Lett. 35 (1987) 185-193.
    [4]M. A. Vannice and B. Sen, “Metal-support effects on the intramolecular selectivity of crotonaldehyde hydrogenation over platinum,” J. Catal. 115 (1989) 65-78.
    [5]H. Yoshitake and Y. Iwasawa, “Active sites and reaction mechanisms for deuteration of acrolein on TiO2-, Y2O3-, ZrO2-, CeO2 and Na/SiO2- supported platinum catalysts,” J. Chem. Soc., Faraday Trans. 88 (3) (1992) 503-510.
    [6]A. Sepúlveda-Escribano, F. Coloma and F. Rodríguez-Reinoso, “Promoting effect of ceria on the gas phase hydrogenation of crotonaldehyde over platinum catalysts,” J. Catal. 178 (1998) 649-657.
    [7]李東穎, “Pd/hydrotalcite觸媒於苯酚一步合成環己酮之研究,” 國立中央大學, 化學工程與材料工程學系, 碩士論文 (1997).
    [8]蔡俊煌, “Ni/Mg-Al-O觸媒於CH4/CO2重組反應之研究,” 國立中央大學, 化學工程與材料工程學系, 碩士論文 (2002).
    [9]廖志偉, “一步合成甲基異丁基酮之多功能觸媒研究-Pd(Ni)/ hydrotalcite,” 國立中央大學, 化學工程與材料工程學系, 碩士論文 (1996).
    [10]C. T. Chang, B. J. Liaw, C.T. Huang and Y. Z. Chen, “Preparation of Au/MgxAlO hydrotalcite catalysts for CO oxidation,” Appl. Catal., A 332 (2007) 216-224.
    [11]游焜竣, “Au/MgxAlO-hydrotalcite觸媒於α,β-不飽和醛選擇性氫化反應之研究,” 國立中央大學, 化學工程與材料工程學系, 碩士論文 (2008).
    [12]吳佩珊, “Au觸媒於α,β-不飽和醛選擇性氫化反應之擔體效應研究,” 國立中央大學, 化學工程與材料工程學系, 碩士論文 (2010).
    [13]P. Claus, “Selective hydrogenation of α,β-unsaturated aldehydes and other C=O and C=C bonds containing compounds,” Top. Catal. 5 (1998) 51-62.
    [14]M. E. Eberhart, M. J. Donovan and R. A. Outlaw, “Ab initio calculations of oxygen diffusivity in Group IB transition metals,” Phys. Rev. B: Condens. Matter Mater. Phys. 46 (1992) 12744-12747.
    [15]L. Gang, B. G. Anderson, J. V. Grandelle and R. A. Santen, “Low temperature selective oxidation of ammonia to nitrogen on silver-based catalysts,” Appl. Catal., B 40 (2003) 101-110.
    [16]O. Blank, German Patent 228 (1910) 697.
    [17]T. E. Lefort, United States Patent (1935) US1998878.
    [18]S. R. Seyedmonir, J. K. Plischke, M. A. Vannice, et al. “Ethylene oxidation over small silver crystallines,” J. Catal. 123 (1990) 534-549.
    [19]V. I. Bukhtiyarov, I. P. Prosvirin and R. I. Kvon, “Study of reactivity of oxygen states adsorbed at a silver surface towards C2H4 by XPS, TPD and TPR,” Surf. Sci. 320 (1994) 47-50.
    [20]B. Hammer and J. K. Norskov, “Electronic factors determining the reactivity of metal surfaces,” Surf. Sci. 343 (1995) 211.
    [21]A. B. Mohammad, I. V. Yudanov, K. H. Lim, K. M. Neyman and N. Rsch, “Hydrogen activation on silver: A computational study on surface and subsurface sxygen species,” J. Phys. Chem. C 112 (2008) 1628-1635.
    [22]A. Montoya, A. Schlunke and B. S. Haynes, “Reaction of hydrogen with Ag(111): binding states, minimum energy paths and kinetics,” J. Phys. Chem. B 110 (2006) 17145-17154.
    [23]R. J. Mikovsky, M. Boudart and H. S. Taylor, “Hydrogen-deuterium exchange on copper, silver, gold and alloy surface,” J. Am. Chem. Soc. 76 (1954) 3814-3819.
    [24]V. Ponec and G. C. Bond, “Catalysis by Metals and Alloys,” Elsevier: Amsterdam (1996)
    [25]A. Metcalfe and M. W. Rowden, “Hydrogenation of nitrobenzene over palladium-silver catalysts,” J. Catal. 22 (1971) 30-34.
    [26]C. Fragalea, M. Garganoa, N. Ravasioa, M. Rossi1 and I. Santoa, “Selective hydrogenation of penta-1,3-diene and cyclooctadienes catalyzed by silver-modified palladium catalysts,” J. Mol. Catal. 24 (1984) 211-216.
    [27]Q. Zhanga, J. Li, X. Liu and Q. Zhu, “Synergetic effect of Pd and Ag dispersed on Al2O3 in the selective hydrogenation of acetylene.” Appl. Catal., A 197 (2000) 221-228.
    [28]B. Ngamsom, N. Bogdanchikova, M. A. Borja and P. Praserthdam, “Characterisations of Pd-Ag/Al2O3 catalysts for selective acetylene hydrogenation: effect of pretreatment with NO and N2O,” Catal. Commun. 5 (2004) 243-248.
    [29]S. Karski, I. Wito´nska, J. Rogowski and J. Gołuchowska, “Interaction between Pd and Ag on the surface of silica,” J. Mol. Catal. A: Chem. 240 (2005) 155-163.
    [30]D. D. Miller and S. S. C. Chuang, “In situ infrared study of NO reduction over Pd/Al2O3 and Ag-Pd/Al2O3 catalysts under H2-rich and lean-burn conditions,” J. Taiwan Inst. Chem. Eng. 40 (2009) 613-621.
    [31]S. S. C. Chuanga, S. Piena and R. Narayanana, “C2 oxygenate synthesis from CO hydrogenation on AgRh/SiO2,” Appl. Catal. 57 (1990) 241-251.
    [32]S. Sugawa, K. Sayama, K. Okabe and H. Arakawa, “Methanol synthesis from CO2 and H2 over silver catalyst,” Energy Convers. Manage. 36 (1995) 665-668.
    [33]M. A. Ulibarri, I. Pavlovic, C. Barriga, M. C. Hermosin and J. Cornejo, “Adsorption of anionic species on hydrotalcite-like compounds: Effect of interlayer anion and crystallinity,” Appl. Clay Sci. 18 (2001) 17-27.
    [34]F. Cavani, F. Trifiro and A. Vacari, “Hydrotalcite-type anionic clays: Preparation, properties and applications,” Catal. Today. 11 (1911) 173-301.
    [35]A. Corma, V. Fornes and F. Rey, “Hydrotalcite as base catalyst: Influence of the chemical composition and synthesis condition on the dehydrogenation of isopropanol,” J. Catal. 148 (1994) 205-212.
    [36]N. Bejoy, “Hydrotalcite: The clay that cures,” Resonance, 6 (2001) 57-61.
    [37]W. T. Reichle, “Catalytic reactions by thermally activated anionic clay minerals,” J. Catal. 94 (1985) 547-577.
    [38]A. L. McKenzie , C. T. Fishel and T. J. Davis, “Investigation of the surface structure and basic properties of calcined hydrotalcite,” J. Catal. 138 (1992) 547-561.
    [39]S. P. Liab and Z. P. Zhouc, “Synthesis and Characterization of the Mixed Mg/Al hydrotalcite-like compounds,” J. Dispersion Sci. Technol. 27 (2006) 1079-1084.
    [40]D. Tichit , M. H. Lhouty, A. Guida, B. H. Chiche, F. Figueras, A. Auroux, D. Bartalini and E. Farronn, “Textural properties and catalytic activity of hydrotalcite,” J. Catal. 151 (1995) 50-59.
    [41]W. Yanga, Y. Kim, P. K. T. Liub, M. Sahimia and T. T. Tsotsisa, “A study by in situ techniques of the thermal evolution of the structure of a Mg-Al-CO3 layered double hydroxide,” Chem. Eng. Sci. 57 (2002) 2945-2953.
    [42]C. P. Keikar and A. A. Schutz, “Ni-, Mg- and Co-containing hydrotalcite-like materials with a sheet-like morphology: Synthesis and characterization,” Microporous Mater. 10 (1997) 163-172.
    [43]M. Bolognini, F. Cavania, D. Scagliarini, C. Flego, C. Perego and M. Saba, “Heterogeneous basic catalysts as alternatives to homogeneous catalysts: Reactivity of Mg/Al mixed oxides in the alkylation of m-cresol with methanol,” Catal. Today 75 (2002) 103-111
    [44]A. Corma, V. Fornes, R. M. Martin-Aranda and F. Rey, “Determination of base properties of hydrotalcite: Condensation of benzaldehyde with ethyl acetoacetate,” J. Catal. 134 (1992) 58-65.
    [45]J. I. Di Cosimo, V. K. Díez, M. Xu, E. Iglesia and C. R. Apestegu´ıa, “Structure and surface and catalytic properties of Mg-Al basic oxides,” J. Catal. 178, (1998) 499-510.
    [46]N. D. Hutson and B. C. Attwood, “High temperature adsorption of CO2 on various hydrotalcite-like compounds,” Adsorption 14 (2008) 781-789.
    [47]V. K. Díez, J. I. Di Cosimo and C. R. Apesteguía, “Study of the citral/acetone reaction on MgyAlOx oxides: Effect of the chemical composition on catalyst activity, selectivity and stability,” Appl. Catal., A 345 (2008) 143-151.
    [48]C. Mohr and P. Claus, “Hydrogenation properties of supported nanosized gold particles,” Sci. Prog. 84 (2001) 311-334.
    [49]R. A. V. Santan and M. Neurock, “Concepts in theoretical heterogeneous catalytic reactivity,” Catal. Rev.-Sci. Eng. 37 (1995) 557-698.
    [50]D. V. Sokol’skii, N. V. Anisimova, A. K. Zharmagambetova, S.G. Mukhamedzhanova and L. N. Edygenova, “Pt−Fe2O3 catalytic system for hydrogenation reactions,” React. Kinet. Catal. Lett. 33 (1987) 399-403.
    [51]G. Cordier, Y. Colleuille, P. Fouilloux, in Catalyse par les Metaux (B. Imelik et al., eds.), “Editions du CNRS, Paris,” (1984) 349.
    [52]G. Cordier, French Patent F 2,329,628 (1975), to Rhone-Poulene S. A.; Chem. Abstr. 87, 38862s (1997).
    [53]U. K. Singh and M. A. Vannice, “Liquid-phase citral hydrogenation over SiO2-supported group VIII metals,” J. Catal. 199 (2001) 73-84.
    [54]A. Giroir-Fendler, D. Richard and P. Gallezot, “In heterogeneous catalysis and fine chemicals, studies in surface science and catalysis Vol.41, Elsevier, Amsterdam,” (1988) 171-178.
    [55]A. Sepúlveda-Escribano, F. Coloma and F. Rodríguez-Reinoso, “Promoting effect of ceria on the gas phase hydrogenation of crotonaldehyde over platinum catalysts,” J. Catal. 178 (1998) 649-657.
    [56]M. Consonni, D. Jokic, D. Y. Murzin and R. Touroude, “High performances of Pt/ZnO catalysts in selective hydrogenation of crotonaldehyde,” J. Catal. 188 (1999) 165-175.
    [57]A. Grioir-Fendler, D. Richard and P. Gallezot, “Chemioselectivity in the catalytic hydrogenateon of cinnamaldehyde: effect of metal particle morphology,” Catal. Lett. 5 (1990) 175-181.
    [58]M. Englisch, A. Jentys and J. A. Lercher, “Structure sensitivity of the hydrogenation of crotonaldehyde over Pt/SiO2 and TiO2,” J. Catal. 166 (1997) 25-35.
    [59]M. Englisch, V. S. Ranade and J. A. Lercher, “Liquid phase hydrogenation of crotonaldehyde over Pt/SiO2,” Appl. Catal., A 163 (1997) 111-122.
    [60]M. Abid, V. Paul-Boncour, and R. Touroude, “Pt/CeO2 catalysts in crotonaldehyde hydrogenation: Selectivity, metal particle size and SMSI states,” Appl. Catal. A 297 (2006) 48-59.
    [61]F. Delbecq and P. Sautet, “Competitive C=C and C=O adsorption of α,β-unsaturated aldehydes on Pt and Pd surfaces in relation with the selectivity of hydrogenation reactions: a theoretical approach,” J. Catal. 152 (1995) 217-236.
    [62]V. Ponec, “On the role of promoters in hydrogenateon on metals: α,β-unsaturated aldehydes and ketones,” Appl. Catal. A 149 (1997) 27-48.
    [63]D. Goupil, P. Fouilloux and R. Maurel, “Activity and selectivity of Pt-Fe/C alloys for the liquid phase hydrogenation of cinnamaldehyde to cinnamyl alcohol,” React. Kinet. Catal. Lett. 35 (1987) 185-193.
    [64]N. Mahata, F. Goncalves, M. Fernando, R. Pereira and J. L. Figueiredo, “Selective hydrogenation of cinnamaldehyde to cinnamyl alcohol over mesoporous carbon supported Fe and Zn promoted Pt catalyst,” Appl. Catal. A 339 (2008) 159-168.
    [65]V. Satagopan and S.B. Chandalia, “Selectivity aspects in the multi-phase hydrogenation of α,β-unsaturated aldehydes over supported noble metal catalysts: Part II ,” J. Chem. Tech. Biotechnol. 60 (1994) 17-21.
    [66]W. Koo-Amornpattana amd J.M. Winterbottom, “Pt and Pt-alloy catalysts and their properties for the liquid-phase hydrogenation of cinnamaldehyde,” Catal. Today 66 (2001) 277-287.
    [67]F. Zhao, Y. Ikushimab, M. Chatterjeeb, O. Satob and M. Arai, “Hydrogenation of an α,β-unsaturated aldehyde catalyzed with ruthenium complexes with different fluorinated phosphine compounds in supercritical carbon dioxide and conventional organic solvents, ” J. Supercrit Fluid 27 (2003) 65-72.
    [68]M. Shirai, T. Tanaka and M. Arai, “Selective hydrogenation of α,β-unsaturated aldehyde to unsaturated alcohol with supported platinum catalysts at high pressures of hydrogen,” J. Mol. Catal. A: Chem. 168 (2001) 99-103.
    [69]M. A. Aramendia, V. Borau, C. Jimenez, J.M. Marinas, A. Porras and F. J. Urbano, “Selective liquid-phase hydrogenation of citral over supported palladium,” J. Catal. 172 (1997) 46-54.
    [70]I. Kun, G. Szöllösi and M. Bartók, “Crotonaldehyde hydrogenation over clay-supported platinum catalysts,” J. Mol. Catal. A: Chem. 169 (2001) 235-246.
    [71]J. Hájek, N. Kumar, P. Mäki-Arvela, T. Salmi, and D.Y. Murzin, “Selective hydrogenation of cinnamaldehyde over Ru/Y zeolite,” J. Mol. Catal. A: Chem. 217 (2004) 145-154.
    [72]J. Hájek, N. Kumar, P. Mäki-Arvela, T. Salmi D. Y. Murzin, I. Paseka, T. Heikkilä, E. Laine, P. Laukkanen and J. Väyrynen, “Ruthenium-modified MCM-41 mesoporous molecular sieve and Y zeolite catalysts for selective hydrogenation of cinnamaldehyde,” Appl. Catal. A 251 (2003) 385-396.
    [73]S. Mukherjee and M. A. Vannice, “Solvent effects in liquid-phase reactions I. Activity and selectivity during citral hydrogenation on Pt/SiO2 and evaluation of mass transfer effects,” J. Catal. 243 (2006) 108-130.
    [74]J. Jia, K. Haraki, J. N. Kondo, K. Domen and K. Tamaru, “Selective hydrogenation of acetylene over Au/Al2O3 catalyst,” J. Phys. Chem. B 104 (2000) 11153-11156.
    [75]M. Okumura, T. Akita and M. Haruta, “Hydrogenation of 1,3-butadiene and of crotonaldehyde over highly dispersed Au catalysts,” Catal. Today 74 (2002) 265-269.
    [76]J. E. Bailie and G. J. Hutchings, “Promotion by sulfur of gold catalysts for crotyl alcohol formation from crotonaldehyde hydrogenation,” Chem. Commun. (1999) 2151.
    [77]S. Schimpf, M. Lucas, C. Mohr, U. Rodemerck, A. Brückner, J. Radnik, H. Hofmeister and P. Claus, “Supported gold nanoparticles: in-depth catalyst characterization and application in hydrogenation and oxidation reactions,” Catal.Today 72 (2002) 63-78.
    [78]C. Mohr, H. Hofmeister and P. Claus, “The influence of real structure of gold catalysts in the partial hydrogenation of acrolein,” J. Catal. 213 (2003) 86-94.
    [79]J. Radnik, C. Mohr and P. Claus, “On the origin of binding energy shifts of core levels of supported gold nanoparticles and dependence of pretreatment and material synthesis,” Phys. Chem. Chem. Phys. 5 (2003) 172-177.
    [80]C. Mohr, H. Hofmeister, J. Radnik and P. Claus, “Identification of active sites in gold-catalyzed hydrogenation of acrolein,” J. Am. Chem. Soc. 125 (2003) 1905-1911.
    [81]J. E. Bailie, H. A. Abdullah, J. A. Anderson, C. H. Rochester, N.V. Richardson, N. Hodge, Jian-Guo Zhang, A. Burrows, C.J. Kiel, and G.J. Hutchings, “Hydrogenation of but-2-enal over supported Au/ZnO catalysts,” Phys. Chem. Chem. Phys. 3 (2001) 4113-4121.
    [82]R. Zanella, C. Louis, S. Giorgio and R. Touroude, “Crotonaldehyde hydrogenation by gold supported on TiO2: Structure sensitivity and mechanism,” J. Catal. 223 (2004) 328-339.
    [83]B. Campo, C. Petit and M. A. Volpe, “Hydrogenation of crotonaldehyde on different Au/CeO2 catalysts,” J. Catal. 254 (2008) 71-78.
    [84]E. Bus, R. Prins and J. A. van Bokhoven, “Origin of the cluster-size effect in the hydrogenation of cinnamaldehyde over supported Au catalysts,” Catal. Commun. 8 (2007) 1397-1402.
    [85]C. Milone, C. Crisafulli, R. Ingoglia, L. Schipilliti and S. Galvagno, “A comparative study on the selective hydrogenation of α,β unsaturated aldehyde and ketone to unsaturated alcohols on Au supported catalysts,” Catal. Today 122 (2007) 341-351.
    [86]B. Campo, M. Volpe, S. Ivanova and R. Touroude, “Selective hydrogenation of crotonaldehyde on Au/HSA-CeO2 catalysts,” J. Catal. 242 (2006) 162-171.
    [87]J. L. Solomon and R. J. Madix, “π bonded intermediates in alcohol oxidation: Orientations of allyloxy and propargyloxy on Ag(110) by near edge X-ray absorption fine structure,” J. Chem. Phys. 89 (1998) 5316-5322.
    [88]J. L. Solomon and R. J. Madix, “Kinetlcs and mechanism of the oxidation of allyl alcohol on Ag(110),” J. Phys. Chem. 91 (1987) 6241-6244.
    [89]P. Claus and H. Hofmeister, “Electron microscopy and catalytic study of silver catalysts: Structure sensitivity of the hydrogenation of crotonaldehyde,” J. Phys. Chem. B 1999, 103, 2766-2775.
    [90]B. C. Khanra, Y. Jugnet and J. C. Bertolini “Energetics of acrolein hydrogenation on Pt(111) and Ag(111) surfaces: a BOC-MP model study,” J. Mol. Catal. A: Chem. 208 (2004) 167-174.
    [91]M. Bron, D. Teschner, A. Knop-Gericke, F. C. Jentoft, J. Kröhnert, J. Hohmeyer, C. Volckmar, B. Steinhauer, R. Schlögl and P. Claus, “Silver as acrolein hydrogenation catalyst: Intricate effects of catalyst nature and reactant partial pressures,” Phys. Chem. Chem. Phys. 9 (2007) 3559-3569.
    [92]K. Brandt, M. E. Chiu, D. J. Watson, M. S. Tikhov and R. M. Lambert, “Chemoselective catalytic hydrogenation of acrolein on Ag(111): Effect of molecular orientation on reaction selectivity,” J. Am. Chem. Soc. 131 (2009) 17286-17290.
    [93]R. Ferullo, M. M. Branda and F. Illas, “Coverage dependence of the structure of acrolein adsorbed on Ag(111),” J. Phys. Chem. Lett. 1 (2010) 2546-2549.
    [94]K. H. Lim, Z. X. Chen, K. M. Neyman and N. Rösch, “Adsorption of acrolein on single-crystal surfaces of silver: Density functional studies,” Chem. Phys. Lett. 420 (2006) 60-64.
    [95]M. Lucas and P.Claus, “Hydrogenations over silver: A highly active and chemoselective Ag-In/SiO2 catalyst for the one-step synthesis of allyl alcohol from acrolein,” Chem. Eng. Technol. 28 (2005) 867-870.
    [96]F. Haass, M. Bron, H. Fuess and P. Claus, “In situ X-ray investigations on AgIn/SiO2 hydrogenation catalysts,” Appl. Catal. A 318 (2007) 9-16.
    [97]W. Gru1nert, A. Bru1ckner, H. Hofmeister and P. Claus, “Structural properties of Ag/TiO2 catalysts for acrolein hydrogenation,” J. Phys. Chem. B 18 (2004) 5709-5717.
    [98]C. E. Volckmar, M. Bron, U. Bentrup, A. Martinb and P. Claus, “Influence of the support composition on the hydrogenation of acrolein over Ag/SiO2-Al2O3 catalysts,” J. Catal. 261 (2009) 1-8.
    [99]M. Steffan, M. Lucas, A. Brandner, M. Wollny, N. Oldenburg and P. Claus, “Selective hydrogenation of citral in an organic solvent, in a ionic liquid, and in substance,” Chem. Eng. Technol. 30 (2007) 481-486.
    [100]P. G. N. Mertens, F. Cuypers, P.Vandezande, X.Ye, F.Verpoort, I. F. J. Vankelecom and D. E. De Vos, “Ag0 and Co0 nanocolloids as recyclable quasihomogeneous metal catalysts for the hydrogenation of α,β-unsaturated aldehydes to allylic alcohol fragrances,” Appl. Catal. A 325 (2007) 130-139.
    Advisor
  • Yin-Zu Chen(陳吟足)
  • Files
  • 983204024.pdf
  • disapprove authorization
    Date of Submission 2011-07-13

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