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
  • [21] Surface Oxygen Vacancies Induced by Calcium Substitution in Macroporous La2Ce2-x Ca x O7-δ Catalysts for Boosting Low-Temperature Oxidative Coupling of Methane
    Wu, Tongtong
    Zhang, Peng
    Wei, Yuechang
    Xiong, Jing
    Han, Dawei
    Li, Tao
    Yang, Yitao
    Zhao, Zhen
    Liu, Jian
    ACS CATALYSIS, 2024, 14 (03) : 1882 - 1902
  • [22] Existence and Properties of Isolated Catalytic Sites on the Surface of β-Cristobalite-Supported, Doped Tungsten Oxide Catalysts (WOx/β-SiO2, Na-WOx/β-SiO2, Mn-WOx/β-SiO2) for Oxidative Coupling of Methane (OCM): A Combined Periodic DFT and Experimental Study
    Kiani, Daniyal
    Sourav, Sagar
    Taifan, William
    Calatayud, Monica
    Tielens, Frederik
    Wachs, Israel E.
    Baltrusaitis, Jonas
    ACS CATALYSIS, 2020, 10 (08) : 4580 - 4592