Ethylbenzene dehydrogenation with CO2 over Fe-doped MgAl2O4 spinel catalysts: Synergy effect between Fe2+ and Fe3+

被引:34
作者
Ji, Min [1 ]
Zhang, Xiaoyan [1 ]
Wang, Junhu [2 ]
Park, Sang-Eon [3 ,4 ]
机构
[1] Dalian Univ Technol, Sch Chem, Dalian 116023, Peoples R China
[2] Chinese Acad Sci, Dalian Inst Chem Phys, Mossbauer Effect Data Ctr, Dalian 116023, Peoples R China
[3] Inha Univ, Lab Nanogreen Catalysis, Inchon 402751, South Korea
[4] Inha Univ, Dept Chem, Nano Ctr Fine Chem Fus Technol, Inchon 402751, South Korea
关键词
Ethylbenzene dehydrogenation; Spinel; Fe-57 Mossbauer spectroscopy; Synergy; IRON-OXIDE CATALYSTS; AL MIXED OXIDES; OXIDATIVE DEHYDROGENATION; CARBON-DIOXIDE; STYRENE; HYDROTALCITE; PRECURSORS; OXYDEHYDROGENATION; CONVERSION; REDUCTION;
D O I
10.1016/j.molcata.2013.01.025
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Fe-doped MgAl2O4 spinet catalyst of MgFe0.1Al1.9O4 and supported catalyst of Fe2O3-MgO/gamma-Al2O3 for ethylbenzene dehydrogenation in the presence of CO2 were studied by Mossbauer spectroscopy (MS) combining with the partial reduction method in the presence of H-2, and the catalytic activity of the ferrous iron species was discussed. The results showed that the catalytic performance of Fe3+ existing in spinel is superior to alpha-Fe2O3, and the synergistic effect between Fe2+ and Fe3+ might indeed increase the catalytic activity since Fe2+-O2- formed in the process of reduction has moderate basicity, which was more favorable for desorption of CO2 compared with Mg2+-O2-. The reduced MgFe0.1Al1.9O4 containing Fe2+ of around 25% exhibits much higher catalytic activity than unreduced catalyst, with improved styrene yield nearly 2 times to 45.0%. MgxFe1-xO as another ferrous iron species formed in the reduction process of Fe2O3-MgO/gamma-Al2O3 showed inconspicuously catalytic activity. (C) 2013 Elsevier B.V. All rights reserved.
引用
收藏
页码:36 / 41
页数:6
相关论文
共 34 条
  • [1] Bragg L., 1965, CRYSTAL STRUCTURE MI, P103
  • [2] 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
    Carja, G
    Nakamura, R
    Aida, T
    Niiyama, H
    [J]. JOURNAL OF CATALYSIS, 2003, 218 (01) : 104 - 110
  • [3] Elaboration and characterization of submicronic magnesio-wustite (Mg1-xFex)O powders
    Carles, V
    Rousset, A
    [J]. SOLID STATE IONICS, 1996, 83 (3-4) : 309 - 321
  • [4] KINETICS OF THE DEHYDROGENATION OF ETHYLBENZENE TO STYRENE OVER UNPROMOTED AND K-PROMOTED MODEL IRON-OXIDE CATALYSTS
    COULTER, K
    GOODMAN, DW
    MOORE, RG
    [J]. CATALYSIS LETTERS, 1995, 31 (01) : 1 - 8
  • [5] Courty Ph., 1979, STUD SURF SCI CATAL, V3, P293
  • [6] Dehydrogenation of ethylbenzene with CO2 to produce styrene over Fe-containing ceramic composites
    de Araujo, Jesuina C. S.
    Sousa, Charllys B. A.
    Oliveira, Alcemira C.
    Freire, Francisco N. A.
    Ayala, Alejandro P.
    Oliveira, Alcineia C.
    [J]. APPLIED CATALYSIS A-GENERAL, 2010, 377 (1-2) : 55 - 63
  • [7] Mesoporous MAl2O4 (M = Cu, Ni, Fe or Mg) spinels: Characterisation and application in the catalytic dehydrogenation of ethylbenzene in the presence of CO2
    de Morais Batista, Andressa H.
    Ramos, Francisca S. O.
    Braga, Tiago P.
    Lima, Cleanio L.
    de Sousa, Francisco F.
    Barros, Eduardo B. D.
    Mendes Filho, Josue
    de Oliveira, Aldenor S.
    de Sousa, Jackson R.
    Valentini, Antoninho
    Oliveira, Alcineia C.
    [J]. APPLIED CATALYSIS A-GENERAL, 2010, 382 (02) : 148 - 157
  • [8] Ethylbenzene to chemicals: Catalytic conversion of ethylbenzene into styrene over metal-containing MCM-41
    de Morais Batista, Andressa H.
    de Sousa, Francisco F.
    Honorato, Sara B.
    Ayala, Alejandro P.
    Mendes Filho, Josue
    de Sousa, Francisco W.
    Pinheiro, Antonio N.
    de Araujo, J. C. S.
    Nascimento, Ronaldo F.
    Valentini, Antoninho
    Oliveira, Alcineia C.
    [J]. JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2010, 315 (01) : 86 - 98
  • [9] Studies of catalytic activity and coke deactivation of spinel oxides during ethylbenzene dehydrogenation
    Freire, Rafael M.
    de Sousa, Francisco F.
    Pinheiroa, Anderson L.
    Longhinotti, Elisane
    Mendes Filho, J.
    Oliveira, Alcemira C.
    Freire, Paulo de Tarso C.
    Ayala, Alejandro P.
    Oliveira, Alcineia C.
    [J]. APPLIED CATALYSIS A-GENERAL, 2009, 359 (1-2) : 165 - 179
  • [10] The reduction of Mg-Fe-O and Mg-Fe-Al-O complex oxides studied by temperature-programmed reduction combined with in situ Mossbauer spectroscopy
    Ge, X
    Li, MS
    Shen, JY
    [J]. JOURNAL OF SOLID STATE CHEMISTRY, 2001, 161 (01) : 38 - 44