ZrO_2/Mo-MCM-41中孔分子筛催化2-甲氧基萘乙酰化反应的研究
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摘要
在水热条件下制备了Mo-MCM-41中孔分子筛,以Zr(SO4_)_2·4H_2O为锆源,用浸泡和研磨两种方式制得ZrO_2/Mo-MCM-41催化剂。通过XRD、FT-IR、NH3-TPD及N2吸附-脱附技术对合成的材料进行了表征。结果表明:合成的中孔分子筛催化剂具有良好的中孔结构;在通过浸渍的方式制得的ZrO_2/Mo-MCM-41中孔分子筛中,ZrO_2分散于中孔分子筛的孔道内,在Mo-MCM-41分子筛外表面没有发现ZrO_2的结晶体;在通过研磨方式制得的ZrO_2/Mo-MCM-41中孔分子筛,ZrO_2仅存在于Mo-MCM-41分子筛的外表面;Mo原子没有进入分子筛骨架的内部,而是以氧化物的形式存在于分子筛表面。将合成的ZrO_2/Mo-MCM-41用于催化2-甲氧基萘的乙酰化反应,反应结果与SO42-/ZrO_2、HY及HZSM-5相比,以浸泡方式制得的ZrO_2/Mo-MCM-41中孔分子筛表现出良好的催化活性和对目的产物高的选择性。
The mesoporous molecular sieve Mo-MCM-41 was synthesized under hydrothermal conditions.ZrO_2/Mo-MCM-41 was prepared by impregnating and grinding using Zr(SO4)2 as the zirconium source. The obtained materials were characterized by XRD, FT-IR, NH3-TPD and N2 adsorption/desorption analysis techniques. The results indicated that ZrO_2/Mo-MCM-41 was of better mesoporous structure and that no crystalline ZrO_2 phase could be observed on the surface of Mo-MCM-41 prepared by impregnating. However, there was some crystalline ZrO_2 on the surface of Mo-MCM-41 prepared by grinding. Mo atom lay on the surface of Mo-MCM-41 in a form of MoO3.ZrO_2/Mo-MCM-41 was used the first time as catalyst in acetylation of 2-methoxynaphthalene. The catalytic results were compared with those obtained by using SO42-/ZrO_2, HY and HZSM-5 as catalysts. The ZrO_2/Mo-MCM-41 prepared by impregnation was found to be of best catalytic activity.
The mesoporous molecular sieve Mo-MCM-41 was synthesized under hydrothermal conditions.ZrO_2/Mo-MCM-41 was prepared by impregnating and grinding using Zr(SO4)2 as the zirconium source. The obtained materials were characterized by XRD, FT-IR, NH3-TPD and N2 adsorption/desorption analysis techniques. The results indicated that ZrO_2/Mo-MCM-41 was of better mesoporous structure and that no crystalline ZrO_2 phase could be observed on the surface of Mo-MCM-41 prepared by impregnating. However, there was some crystalline ZrO_2 on the surface of Mo-MCM-41 prepared by grinding. Mo atom lay on the surface of Mo-MCM-41 in a form of MoO3.ZrO_2/Mo-MCM-41 was used the first time as catalyst in acetylation of 2-methoxynaphthalene. The catalytic results were compared with those obtained by using SO42-/ZrO_2, HY and HZSM-5 as catalysts. The ZrO_2/Mo-MCM-41 prepared by impregnation was found to be of best catalytic activity.
引文
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[17] Li L, Li C H, Han B K, et al. Determination of InP(001)surfacereconstructions by STM and infrared spectroscopy of adsorbedhydrogen[J]. Physical Review B, 2000, 61(61):10223-10228.
[18]Xia Q H, Hidajat K, Kawi S. Effect of ZrO2, Loading on the Structure,Acidity, and Catalytic Activity of the SO42-/ZrO2/MCM-41 AcidCatalyst[J]. Journal of Catalysis, 2002, 205(2):318-331.
[19] Sayari A. Sulfated Zirconia-Based Strong Solid-Acid Catalysts:Recent Progress[J]. Catalysis Reviews, 1996, 38(3):329-412.
[20]Riemer T, Spielbauer D, Hunger M, et al. Super Acid Properties ofSulfated Zirconia as Measured by Raman and 1H MAS NMRSpectroscopy[J]. Journal of the Chemical Society ChemicalCommunications, 1994, 10(10):1181-1182.
[21] Morterra C, Cerrato G, Pinna F, et al. On the acid-catalysedisomerisation of light paraffins over a ZrO2/SO42-system:the effectof hydration[J]. Journal of Catalysis, 1994, 149(1):181-188.
[22]And R S D, Kob N. Acidity and Reactivity of Sulfated Zirconia andMetal-Doped Sulfated Zirconia[J]. Journal of Physical Chemistry B,1997, 101(17):3360-3364.
[23] Sohn J R, Decanio S J, Lunsford J H, et al. Determination offramework aluminium content in dealuminated Y-type zeolites:acomparison based on unit cell size and wavenumber of i.r. bands[J].Zeolites, 1986, 6(3):225-227.
[2]Costa J A S, de Jesus R A, da Silva C M P, et al. Efficient adsorption ofa mixture of polycyclic aromatic hydrocarbons(PAHs)bySi–MCM–41 mesoporous molecular sieve[J]. Powder Technology,2017, 308:434-441.
[3]Armengol E, Cano M L, Corma A, et al. Mesoporous aluminosilicateMCM-41 as a convenient acid catalyst for Friedel–Crafts alkylation ofa bulky aromatic compound with cinnamyl alcohol[J]. Journal of theChemical Society, Chemical Communications, 1995(5):519-520.
[4]Huang Z, Miao H, Li J, et al. Modifier-enhanced supercritical CO2extraction of organic template from aluminosilicate MCM-41materials:Effect of matrix Al/Si ratios and different modifiers[J].Separation and Purification Technology, 2013, 118:170-178.
[5]Chen P, Wang W, Zhai Y. Friedel–Crafts acylation of 2-methoxynaphthalene with acetic anhydride over Al-HMS[J]. Journal of Porous Materials, 2014, 21(4):441-448.
[6] VitvarováD, LupínkováL, Kub?M. Alkylation of phenols andacylation 2-methoxynaphthalene over SSZ-33, SSZ-35 and SSZ-42zeolites[J]. Microporous and Mesoporous Materials, 2015, 210:133-141.
[7]Cahyono E, Priatmoko S, Haryani S. Acetylation of 2-Methoxynaphtalene with Acetic anhidryde over Zr4+-Zeolite beta[J]. OrientalJournal of Chemistry, 2015, 31(Special Issue 1(2015)):79-83.
[8]Zhang B, Xie F, Yuan J, et al. Meerwein-Ponndorf-Verley reaction ofacetophenone over ZrO2-La2O3/MCM-41:Influence of loading orderof ZrO2 and La2O3[J]. Catalysis Communications, 2017, 92:46-50.
[9]Hodala J L, Halgeri A B, Shanbhag G V. Enhancement in activity andshape selectivity of zeolite BEA by phosphate treatment for2-methoxynaphthalene acylation[J]. Rsc Advances, 2016, 6(93):90579-90586.
[10]Wang X X, Lefebvre F, Basset J M, et al. Synthesis and characterization of zirconium containing mesoporous silicas:I. Hydrothermal synthesis of Zr-MCM-41-type materials[J]. Microporous&Mesoporous Materials, 2001, 42(2):269-276.
[11] Miao C X, Gao Z. Preparation and properties of ultrafine SO42-/ZrO2,superacid catalysts[J]. Materials Chemistry&Physics, 1997,50(1):15-19.
[12] Sayari A. Sulfated Zirconia-Based Strong Solid-Acid Catalysts:Recent Progress[J]. Catalysis Reviews, 1996, 38(3):329-412.
[13]Bachari K, Chebout R., Lamouchi, M(2016)Efficient synthesis ofzinc-containing mesoporous silicas by microwave irradiation methodand their high activities in acetylation of 1, 2-dimethoxybenzenewith acetic anhydride[C]. Arabian Journal of Chemistry 9:2016:S893-S900.
[14]Hino M, Arata K, Synthesis of solid superacid of molybdenum oxidesupported on zirconia and its catalytic action[J]. hemistry Letters,1989,18:971-972.
[15]Sun Y, Zhu L, Lu H, et al. Sulfated zirconia supported in mesoporousmaterials[J]. Applied Catalysis A General, 2002, 237(1):21-31.
[16]Pauly T R, Liu Y, Pinnavaia T J, et al. Textural Mesoporosity and theCatalytic Activity of Mesoporous Molecular Sieves with WormholeFramework Structures[J]. Journal of the American Chemical Society,1999, 121(38):8835-8842.
[17] Li L, Li C H, Han B K, et al. Determination of InP(001)surfacereconstructions by STM and infrared spectroscopy of adsorbedhydrogen[J]. Physical Review B, 2000, 61(61):10223-10228.
[18]Xia Q H, Hidajat K, Kawi S. Effect of ZrO2, Loading on the Structure,Acidity, and Catalytic Activity of the SO42-/ZrO2/MCM-41 AcidCatalyst[J]. Journal of Catalysis, 2002, 205(2):318-331.
[19] Sayari A. Sulfated Zirconia-Based Strong Solid-Acid Catalysts:Recent Progress[J]. Catalysis Reviews, 1996, 38(3):329-412.
[20]Riemer T, Spielbauer D, Hunger M, et al. Super Acid Properties ofSulfated Zirconia as Measured by Raman and 1H MAS NMRSpectroscopy[J]. Journal of the Chemical Society ChemicalCommunications, 1994, 10(10):1181-1182.
[21] Morterra C, Cerrato G, Pinna F, et al. On the acid-catalysedisomerisation of light paraffins over a ZrO2/SO42-system:the effectof hydration[J]. Journal of Catalysis, 1994, 149(1):181-188.
[22]And R S D, Kob N. Acidity and Reactivity of Sulfated Zirconia andMetal-Doped Sulfated Zirconia[J]. Journal of Physical Chemistry B,1997, 101(17):3360-3364.
[23] Sohn J R, Decanio S J, Lunsford J H, et al. Determination offramework aluminium content in dealuminated Y-type zeolites:acomparison based on unit cell size and wavenumber of i.r. bands[J].Zeolites, 1986, 6(3):225-227.