Oxidative coupling of methane to C2 hydrocarbons on the Mg-Ti mixed oxide-supported catalysts at the lower reaction temperature: Role of surface oxygen atoms

被引:42
|
作者
Jeon, Wonjin [1 ]
Lee, Jong Yeol [1 ]
Lee, Maro [1 ,2 ]
Choi, Jae-Wook [1 ]
Ha, Jeong-Myeong [1 ,3 ,4 ]
Suh, Dong Jin [1 ,3 ,4 ]
Kim, Il Won [2 ]
机构
[1] Korea Inst Sci & Technol, Clean Energy Res Ctr, Seoul 136791, South Korea
[2] Soongsil Univ, Dept Chem Engn, Seoul 156743, South Korea
[3] Univ Sci & Technol, Dept Clean Energy & Chem Engn, Taejon 305350, South Korea
[4] Korea Univ, Green Sch, Seoul 136701, South Korea
关键词
Oxidative coupling of methane; Mg-Ti mixed oxide; Catalyst; Surface lattice oxygen; ALKALINE-EARTH; BASICITY; PERFORMANCE; GAS; MN/NA2WO4/SIO2; DIFFRACTION; ETHYLENE; NEUTRON; LA2O3; PRESSURE;
D O I
10.1016/j.apcata.2013.05.020
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
The oxidative coupling of methane (OCM) couples methane molecules, which are the major components of natural gas, to form ethane and ethylene in order to produce fuels and chemicals. Because of the high reaction temperature (700-900 degrees C) to obtain high yields of desirable products, the OCM process has been difficult to commercialize. We have developed a less energy-intensive OCM process that exhibits higher activity at a lower reaction temperature using Mg-Ti mixed oxide-supported Na/W/Mn catalysts. The catalyst consisting of Mg/(Mg + Ti) = 0.5 (mol/mol) exhibited the highest C-2 hydrocarbons yields (i.e., 18.1% at 825 degrees C and 16.5% at 775 degrees C) among the mixed oxide-supported catalysts, which were higher than those of the conventional SiO2-supported catalyst particularly at a low temperature of 775 degrees C (12.8%). Based on catalyst characterization by transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), UV-vis spectroscopy (UV-vis), O-2-temperature programmed desorption (O-2-TPD), and CO2-temperature programmed desorption (CO2-TPD), the improved catalytic activity of the mixed oxide-supported catalysts was attributed to more active surface lattice O atoms. (C) 2013 Elsevier B.V. All rights reserved.
引用
收藏
页码:68 / 77
页数:10
相关论文
共 22 条
  • [1] OXIDATIVE COUPLING OF METHANE TO C2 HYDROCARBONS OVER DOPED TITANIA CATALYSTS
    PAPAGEORGIOU, D
    VAMVOUKA, D
    VERYKIOS, XE
    STUDIES IN SURFACE SCIENCE AND CATALYSIS, 1993, 75 : 2269 - 2272
  • [2] SUPPORTED PbO CATALYSTS FOR THE OXIDATIVE COUPLING OF METHANE - THE EFFECT OF SURFACE ACIDITY OF THE SUPPORT ON C2 + SELECTIVITY.
    Bytyn, W.
    Baerns, M.
    1600, (28): : 1 - 2
  • [3] Effect of Mg substitution on LaTi1-xMgxO3+δ catalysts for improving the C2 selectivity of the oxidative coupling of methane
    Lopes, Larissa B.
    Vieira, Luiz H.
    Assaf, Jose M.
    Assaf, Elisabete M.
    CATALYSIS SCIENCE & TECHNOLOGY, 2021, 11 (01) : 283 - 296
  • [4] OXIDATIVE COUPLING OF METHANE OVER CAO-CEO2 CATALYSTS - EFFECT OF OXYGEN-ION CONDUCTIVITY ON C2 SELECTIVITY
    ZHANG, ZL
    BAERNS, M
    JOURNAL OF CATALYSIS, 1992, 135 (01) : 317 - 320
  • [5] SUPPORTED PBO CATALYSTS FOR THE OXIDATIVE COUPLING OF METHANE - THE EFFECT OF SURFACE-ACIDITY OF THE SUPPORT ON C2+ SELECTIVITY
    BYTYN, W
    BAERNS, M
    APPLIED CATALYSIS, 1986, 28 (1-2): : 199 - 207
  • [6] Oxidative coupling of methane under microwave: core-shell catalysts for selective C2 production and homogeneous temperature control
    Kaneda, Reina
    Palomo, Jose
    Hu, Lingjun
    Urakawa, Atsushi
    CATALYSIS SCIENCE & TECHNOLOGY, 2023, 13 (19) : 5757 - 5766
  • [7] Oxidative Coupling of Methane Using Mg/Ti-Doped SiO2-Supported Na2WO4/Mn Catalysts
    Yunarti, Rika Tri
    Gu, Sangseo
    Choi, Jae-Wook
    Jae, Jungho
    Suh, Dong Jin
    Ha, Jeong-Myeong
    ACS SUSTAINABLE CHEMISTRY & ENGINEERING, 2017, 5 (05): : 3667 - 3674
  • [8] Methane-water redox reaction on A2SnO4 (A=Mg, Ca, Sr, Ba) oxide to produce C2 hydrocarbons
    K. Omata
    T. Ehara
    I. Kawai
    M. Yamada
    Catalysis Letters, 1997, 45 : 245 - 248
  • [10] Optimal oxygen concentration strategy through an isothermal oxidative coupling of methane plug flow reactor to obtain a high yield of C2 hydrocarbons
    Amideddin Nouralishahi
    Hassan Pahlavanzadeh
    Mohammadmehdi Choolaei
    Elaheh Esmaeili
    Amir Yadegari
    Korean Journal of Chemical Engineering, 2013, 30 : 1213 - 1221