Journal of Guangdong University of Technology ›› 2017, Vol. 34 ›› Issue (02): 28-33.doi: 10.12052/gdutxb.160025

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A Research of Mesoporous Copper-Manganese Mixed Oxides for Selective Oxidation of Benzyl Alcohol to Benzaldehyde

Zheng Hai-long, Liao Shu-huan, Yu Lin   

  1. School of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou 510006, China
  • Received:2016-03-02 Online:2017-03-09 Published:2017-03-09

Abstract:

A novel template-free co-precipitation method was applied to synthesize mesoporous copper-manganese mixed oxides with high surface area, which can be obtained in large quantities. Catalytic activity of copper-manganese mixed oxides (Cu-Mn-x, x=1, 2, 4) has been studied in selective oxidation of benzyl alcohol using molecular oxygen as oxidizing agent and toluene as solvent. The catalysts exhibited highest activity, in which 90% conversion of the benzyl alcohol was achieved with 98% selectivity to benzaldehyde within a short reaction period only in 20 min at 102℃, when the design mole ratio of Cu/Mn was 1:2. The physicochemical properties of the catalysts were characterized by XRD, SEM, TEM, BET, H2-TPR and EDS techniques. It shows that Cu and Mn can improve the catalytic performance each other effectively but there must be an appropriate mole ratio of Cu/Mn. In addition, there is a great relationship between the activity and the amount of catalysts, which shows that the higher activity the more catalysts.

Key words: mesoporous, copper-manganese mixed oxides, benzyl alcohol, selective oxidation

CLC Number: 

  • TQ244

[1] 张昕, 吴伟伟, 黄启权, 等. 苯甲醇液相氧化制苯甲醛催化剂的研究进展[J]. 石油化工, 2010, 02:215-223.ZHANG X, WU W W, HUANG Q Q, et al. Advance in catalysts for green liquid-phase oxidation of benzyl alcohol to benzaldehyde[J]. Electrochemical Technology, 2010, 02:215-223.
[2] KÖCKRITZ A, SEBEK M, DITTMAR A, et al. Ru-catalyzed oxidation of primary alcohol[J]. J Mol Catal A:Chem, 2006, 246(1~2):85-99.
[3] STUCHINSKAYA T L, KOZHEVNIKOV I V. Liquid-phase oxidation of alcohols with oxygen catalysed by modified palladium (Ⅱ) oxide[J]. Catal Commum, 2003, 4(8):417-422.
[4] SU F Z, CHEN M, WANG L C, et al. Aerobic oxidation of alcohols catalyzed by gold nanoparticles supported on gallia[J]. Polymorphs Catal Commum, 2008, 9(6):1027-1032.
[5] BEIER M J, HANSEN T W, GRUNWALDT J D. Selective liquid-phase oxidation of alcohols catalyzed by a silver-based catalyst promoted by the presence of ceria[J]. Journal of Catalysis, 2009, 266(2):320-330.
[6] MENG X J, LIN K F, YANG X Y, et al. Catalytic oxidation of olefins and alcohols by molecular oxygen under air pressure over Cu2(OH)PO4 and Cu4O(PO4)2 catalysts[J]. J Catal, 2003, 218(2):460-464.
[7] CHOUDHARY V R, DUMBRE D K, UPHADE B S, et al. Solvent-free oxidation of benzyl alcohol to benzaldehyde by tert-butyl hydroper oxide using transition metal containing layered double hydroxides and/or mixed hydroxides[J]. J Mol Catal A:Chem, 2004, 215(1-2):129-135.
[8] HU J, SUN K Q, HE D P, et al. Amorphous manganese oxide for catalytic selective oxidation of benzyl alcohol[J]. Chinese Journal of Catalysis, 2007, 28(12):1025-1027.
[9] TANG Q H, HUANG X N, WU C M, et al. Structure and catalytic properties of K-doped manganese oxide supported on alumina[J]. J Mol Catal A:Chem, 2009, 306(1-2):48-53.
[10] SHEN Y F, SUIB S L, O'YONG C L. Cu containing octahedral molecular sieves and octahedral layered materials[J]. J Catal, 1996, 161(1):115-122.
[11] 符志伟, 程高, 林婷, 等. 二氧化锰制备及催化燃烧甲苯性能研究[J]. 广东工业大学学报, 2016, 33(02):85-90.FU Z W, CHENG G, LIN T, et al. The preparation of MnO2 and application in catalytic combustion of toluene[J]. Journal of Guangdong University of Technology, 2016, 33(02):85-90.
[12] FANG D, XIE J L. Effect of CuMn2O4 spinel in Cu-Mn oxide catalysts on selective catalytic reduction of NOx with NH3 at low temperature[J]. RSC Adv, 2014, 4(49):25540-25551.
[13] TANG W X, WU X F, LI S D. Porous Mn-Co mixed oxide nanorod as a novel catalyst with enhanced catalytic activity for removal of VOCs[J]. Catalysis Communications, 2014, 56(56):134-138.
[14] LI G N, LI L, SHI J J. One-pot pyrolytic synthesis of mesoporous MCo2O4(4.5)(M=Mn, Ni, Fe, Cu) spinels and its high efficient catalytic properties for CO oxidation at low temperature[J]. Journal of Molecular Catalysis A-Chemical, 2014, 390(8):97-104.
[15] TANG W X, WU X F, LI S D, et al. Co-nanocasting synthesis of mesoporous Cu-Mn composite oxides and their promoted catalytic activities for gaseous benzene removal[J]. Applied Catalysis B-Environmental, 2015, 162:110-121.
[16] LIU X S, JIN Z N, LU J Q, et al. Highly active CuO/OMS-2 catalysts for low-temperature CO oxidation[J]. Chemical Engineering Journal, 2010, 162(1):151-157.
[17] KRÄMER M, SCHMIDT T, STÖWE K, et al. Structural and catalytic aspects of sol-gel derived copper manganese oxides as low-temperature CO oxidation catalyst[J]. Applied Catalysis A:General, 2006, 302(2):257-263.
[18] TANG Q H, GONG X N, ZHAO P Z, et al. Copper-manganese oxide catalysts supported on alumina:Physicochemical features and catalytic performances in the aerobic oxidation of benzyl alcohol[J]. Applied Catalysis A-General, 2010, 389(1-2):101-107.
[19] TANG W X, WU X F, CHEN Y F, et al. Oxalate route for promoting activity of manganese oxide catalysts in total VOCs' oxidation:effect of calcination temperature and preparation method[J]. Mater Chem A, 2014, 2(8):2544-2554.
[20] SHU Z, HUANG W M, SHI J L, et al. Template-free synthesis of mesoporous X-Mn (X=Co, Ni, Zn) bimetal oxides and catalytic application in the room temperature removal of low-concentration NO[J]. Mater Chem A, 2013, 1(35):10218-10227.
[21] ALI R, SIDDIQUI M R, WARTHAN A A. Selective oxidation of benzyl alcohol with molecular oxygen over copper-manganese oxide catalyst[J]. Oxidation Communications, 2011, 34(4):778-787.
[22] PAPAVASILIOU J, AVGOUROPOULOS G, IOANNIDES T. Combined steam reforming of methanol over Cu-Mn spinel oxide catalysts[J]. Journal of Catalysis, 2007, 251(1):7-20.

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