Molybdenum-based catalysts supported on Al2O3 doped with Ni, Cu, or Fe oxide were synthesized and used in ethylbenzene dehydrogenation to produce styrene. The molybdenum oxide was sup-ported using an unconventional route that combined the polymeric precursor method (Pechini) and wet impregnation on commercial alumina. The samples were characterized by X-ray diffraction (XRD), N2 adsorption-desorption isotherms, temperature-programmed reduction of H2 (H2-TPR), and thermogravimetric (TG) analysis. XRD results showed that the added metals were well dis-persed on the alumina support. The addition of the metal oxide (Ni, Cu, or Fe) of 2 wt% by wet im-pregnation did not affect the texture of the support. TPR results indicated a synergistic effect be-tween the dopant and molybdenum oxide. The catalytic tests showed ethylbenzene conversion of 28%–53% and styrene selectivity of 94%–97%, indicating that the addition of the dopant improved the catalytic performance, which was related to the redox mechanism. Molybdenum oxides play a fundamental role in the oxidative dehydrogenation of ethylbenzene to styrene by its redox and acid–base properties. The sample containing Cu showed an atypical result with increasing conver-sion during the reaction, which was due to metal reduction. The Ni-containing solid exhibited the highest amount of carbon deposited, shown by TG analysis after the catalytic test, which explained its lower catalytic stability and selectivity.
参考文献
[1] | Baghalha M;Ebrahimpour O .[J].Applied Catalysis A:General,2007,326:143. |
[2] | Hirano T .[J].Applied Catalysis,1986,26:65. |
[3] | Mimura N;Saito M .[J].Catalysis Today,2000,55:173. |
[4] | Park S E;Han S C .[J].Journal of Industrial and Engineering Chemistry,2004,10:1257. |
[5] | Sun A L;Qin Z F;Wang J G .[J].Applied Catalysis A:General,2002,234:179. |
[6] | Sakurai Y;Suzaki T;Ikenaga N;Suzuki T .[J].Applied Catalysis A:General,2000,192:281. |
[7] | Sato S;Ohhara M;Sodesawa T;Nozaki F .[J].Applied Catalysis,1988,37:207. |
[8] | Fedorov G I;Sibgatullin S G;Solodova N L;Izmailov R I .[J].Petrol Chem,1976,16(03):162. |
[9] | Cavani F;Trifirò F .[J].Applied Catalysis A:General,1995,133:219. |
[10] | 李春光,缪长喜,聂颖颖,乐英红,顾松园,杨为民,华伟明,高滋.CO2气氛下MCF负载氧化钒催化剂上乙苯脱氢反应[J].催化学报,2010(08):993-998. |
[11] | 李惠云,乐英红,缪长喜,谢在库,华伟明,高滋.溶胶-凝胶法制备用于CO2气氛下乙苯胶氢反应的高活性Cr2O3-SiO2催化剂[J].催化学报,2006(01):4-6. |
[12] | Ikenaga N;Tsuruda T;Senma K;Yamaguchi T Sakurai Y Suzuki T .[J].Industrial and Engineering Chemistry Research,2000,39:1228. |
[13] | Carja G.;Nakamura R.;Aida T.;Niiyama H. .Mg-V-Al mixed oxides with mesoporous properties using layered double hydroxides as precursors: catalytic behavior for the process of ethylbenzene dehydrogenation to styrene under a carbon dioxide flow[J].Journal of Catalysis,2003(1):104-110. |
[14] | He X X;Fan C;Gu X Y;Zhou X G Chen D Zhu Y A .[J].Journal of Molecular Catalysis A:Chemical,2011,344:53. |
[15] | Braga T P;Pinheiro A N;Teixeira C V;Valentini A .[J].Applied Catalysis A:General,2009,366:193. |
[16] | Wong ST.;Mou CY.;Lin HP. .Tubular MCM-41-supported transition metal oxide catalysts for ethylbenzene dehydrogenation reaction[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2000(1/2):103-114. |
[17] | Morán C;González E;Sánchez J;Solano R Carruyo G Moronta A .[J].Journal of Colloid and Interface Science,2007,315:164. |
[18] | Moronta A;Troconis ME;Gonzalez E;Moran C;Sanchez J;Gonzalez A;Quinonez J .Dehydrogenation of ethylbenzene to styrene catalyzed by Co, Mo and CoMo catalysts supported on natural and aluminum-pillared clays - Effect of the metal reduction[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2006(0):199-204. |
[19] | Pramod C V;Raghavendra C;Reddy K H P;Babu G V R Rao K S R Raju B D .[J].JChem Sci,2014,126:311. |
[20] | 孙晓岩,王锐,苏党生.纳米碳材料非金属催化的研究进展[J].催化学报,2013(03):508-523. |
[21] | Chen D;Holmen A;Sui Z J;Zhou X G .[J].催化学报,2014,35:824. |
[22] | Cavani F;Trifiro F .[J].Applied Catalysis A:General,1995,133:219. |
[23] | 辛勤;林励吾 .[J].催化学报,2013,34:401. |
[24] | Dalmaschio, C.J.;Mastelaro, V.R.;Nascente, P.;Bettini, J.;Zotin, J.L.;Longo, E.;Leite, E.R. .Oxide surface modification: Synthesis and characterization of zirconia-coated alumina[J].Journal of Colloid and Interface Science,2010(1):256-262. |
[25] | Chary KVR;Reddy KR;Kishan G;Niemantsverdriet JW;Mestl G .Structure and catalytic properties of molybdenum oxide catalysts supported on zirconia[J].Journal of Catalysis,2004(2):283-291. |
[26] | Al-Shihry S S;Halawy S A .[J].Journal of Molecular Catalysis A:Chemical,1996,113:479. |
[27] | Humblot F.;Le Peltier F.;Didillon B.;Basset JM.;Candy JP. .Surface organometallic chemistry on metals: Selective dehydrogenation of isobutane into isobutene on bimetallic catalysts prepared by reaction of tetra n-butyltin on silica-supported platinum catalyst[J].Journal of Catalysis,1998(2):459-468. |
[28] | Kaneko S;Arakawa T;Ohshima M;Kurokawa H Miura H .[J].Applied Catalysis A:General,2009,356:80. |
[29] | Men Y;Yang M .[J].CATALYSIS COMMUNICATIONS,2012,22:68. |
[30] | Delgado J J;Chen X;Tessonnier J P;Schuster M E Del Rio E Schl?gl R Su D S .[J].Catalysis Today,2010,150:49. |
[31] | Nederlof C;Kapteijn F;Makkee M .[J].Applied Catalysis A:General,2012,417-418:163. |
[32] | Zarubina V;Nederlof C;Van der Linden B;Kapteijn F Heeres H J Makkee M Melian-Cabrera I .[J].Journal of Molecular Catalysis A:Chemical,2014,381:179. |
[33] | Braga T P;Sales B M C;Pinheiro A N;Herrera W T Bag-gio-Saitovitch E Valentini A .[J].Catal Sci Technol,2011,1:1383. |
[34] | Pochamoni R;Narani A;Gurram V R B;Gudimella M D Potharaju P S S P Burri D R Rao K S R .[J].INDIAN Journal OF CHEMISTRY SECTION A-INORGANIC BIO-INORGANIC PHYSICAL TH,2014,53A:493. |
[35] | Oganowski W;Hanuza J;Drulis H;Mista W Macalik L .[J].Applied Catalysis A:General,1996,133:143. |
[36] | Irún O;Sadosche S A;Lasobras J;Soler J Francés E Herguido J Menéndez M .[J].Catalysis Today,2013,203:53. |
[37] | Park M S;Vislovskiy V P;Chang J S;Shul Y G Yoo J S Park S E .[J].Catalysis Today,2003,87:205. |
[38] | Abello MC.;Ferretti O.;Gomez MF. .Mo/gamma-Al2O3 catalysts for the oxidative dehydrogenation of propane. Effect of Mo loading[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2001(1/2):421-431. |
[39] | Nederlof C;Talay G;Kapteijn F;Makkee M .[J].Applied Catalysis A:General,2012,423-424:59. |
[40] | Watanabe R;Sekine Y;Kojima J;Matsukata M Kikuchi E .[J].Applied Catalysis A:General,2011,398:66. |
[41] | He X X;Fan C;Gu X Y;Zhou X G Chen D Zhu Y A .[J].Journal of Molecular Catalysis A:Chemical,2011,344:53. |
[42] | Hanuza J;Jezowska-Trzebiatowska B;Oganowski W .[J].Journal of Molecular Catalysis,1978,4:271. |
[43] | Abello MC.;Ferretti O.;Gomez MF. .Mo/gamma-Al2O3 catalysts for the oxidative dehydrogenation of propane. Effect of Mo loading[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2001(1/2):421-431. |
[44] | Vedrine J C;Millet J M M;Volta J C .[J].Catalysis Today,1996,32:115. |
- 下载量()
- 访问量()
- 您的评分:
-
10%
-
20%
-
30%
-
40%
-
50%