Identification of molybdenum oxide nanostructures on zeolites for natural gas conversion

被引:318
作者
Gao, Jie [1 ]
Zheng, Yiteng [1 ]
Jehng, Jih-Mirn [2 ,3 ]
Tang, Yadan [2 ]
Wachs, Israel E. [2 ]
Podkolzin, Simon G. [1 ]
机构
[1] Stevens Inst Technol, Dept Chem Engn & Mat Sci, Hoboken, NJ 07030 USA
[2] Lehigh Univ, Dept Chem Engn, Operando Mol Spect & Catalysis Lab, Bethlehem, PA 18015 USA
[3] Natl Chung Hsing Univ, Dept Chem Engn, Taichung 40227, Taiwan
基金
美国国家科学基金会;
关键词
BRONSTED ACID SITES; METHANE DEHYDROAROMATIZATION; ZSM-5; ZEOLITES; CATALYSTS; BENZENE; AROMATIZATION; DEHYDROGENATION; SPECTROSCOPY; ACTIVATION; AROMATICS;
D O I
10.1126/science.aaa7048
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Direct methane conversion into aromatic hydrocarbons over catalysts with molybdenum (Mo) nanostructures supported on shape-selective zeolites is a promising technology for natural gas liquefaction. We determined the identity and anchoring sites of the initial Mo structures in such catalysts as isolated oxide species with a single Mo atom on aluminum sites in the zeolite framework and on silicon sites on the zeolite external surface. During the reaction, the initial isolated Mo oxide species agglomerate and convert into carbided Mo nanoparticles. This process is reversible, and the initial isolated Mo oxide species can be restored by a treatment with gas-phase oxygen. Furthermore, the distribution of the Mo nanostructures can be controlled and catalytic performance can be fully restored, even enhanced, by adjusting the oxygen treatment.
引用
收藏
页码:686 / 690
页数:5
相关论文
共 29 条
  • [1] [Anonymous], 2012, GOLD RUL GOLD AG GAS
  • [2] Methane dehydroaromatization over Mo-modified H-MFI for gas to liquid catalysts
    Aritani, Hirofumi
    Shibasaki, Hiromi
    Orihara, Hitoshi
    Nakahira, Atsushi
    [J]. JOURNAL OF ENVIRONMENTAL SCIENCES, 2009, 21 (06) : 736 - 740
  • [3] DEHYDRO-OLIGOMERIZATION OF METHANE TO ETHYLENE AND AROMATICS OVER MOLYBDENUM/HZSM-5 CATALYST
    CHEN, LY
    LIN, LW
    XU, ZS
    LI, XS
    ZHANG, T
    [J]. JOURNAL OF CATALYSIS, 1995, 157 (01) : 190 - 200
  • [4] Nonoxidative activation of methane
    Choudhary, TV
    Aksoylu, E
    Goodman, DW
    [J]. CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 2003, 45 (01): : 151 - 203
  • [5] Siting and Distribution of Framework Aluminium Atoms in Silicon-Rich Zeolites and Impact on Catalysis
    Dedecek, J.
    Sobalik, Z.
    Wichterlova, B.
    [J]. CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 2012, 54 (02): : 135 - 223
  • [6] Structure of Mo2Cx and Mo4Cx), Molybdenum Carbide Nanoparticles and Their Anchoring Sites on ZSM-5 Zeolites
    Gao, Jie
    Zheng, Yiteng
    Fitzgerald, George B.
    de Joannis, Jason
    Tang, Yadan
    Wachs, Israel E.
    Podkolzin, Simon G.
    [J]. JOURNAL OF PHYSICAL CHEMISTRY C, 2014, 118 (09) : 4670 - 4679
  • [7] Direct, Nonoxidative Conversion of Methane to Ethylene, Aromatics, and Hydrogen
    Guo, Xiaoguang
    Fang, Guangzong
    Li, Gang
    Ma, Hao
    Fan, Hongjun
    Yu, Liang
    Ma, Chao
    Wu, Xing
    Deng, Dehui
    Wei, Mingming
    Tan, Dali
    Si, Rui
    Zhang, Shuo
    Li, Jianqi
    Sun, Litao
    Tang, Zichao
    Pan, Xiulian
    Bao, Xinhe
    [J]. SCIENCE, 2014, 344 (6184) : 616 - 619
  • [8] Identification of diverse silanols on protonated ZSM-5 zeolites by means of FTIR spectroscopy
    Hoffmann, Pedro
    Lobo, Jose A.
    [J]. MICROPOROUS AND MESOPOROUS MATERIALS, 2007, 106 (1-3) : 122 - 128
  • [9] Direct conversion of methane to fuels and chemicals
    Holmen, Anders
    [J]. CATALYSIS TODAY, 2009, 142 (1-2) : 2 - 8
  • [10] Direct conversion of methane on Mo/ZSM-5 catalysts to produce benzene and hydrogen: achievements and perspectives
    Ismagilov, Zinfer R.
    Matus, Ekaterina V.
    Tsikoza, Lidia T.
    [J]. ENERGY & ENVIRONMENTAL SCIENCE, 2008, 1 (05) : 526 - 541