Effect of the particle size of MoO3 on the catalytic activity of Mo/ZSM-5 in methane non-oxidative aromatization

被引:31
|
作者
Hu, Jing [1 ]
Wu, Shujie [1 ]
Ma, Yuanyuan [1 ,2 ]
Yang, Xiaoyuan [1 ]
Li, Zhifang [1 ]
Liu, Heng [1 ]
Huo, Qisheng [3 ]
Guan, Jingqi [1 ]
Kan, Qiubin [1 ]
机构
[1] Jilin Univ, Coll Chem, Changchun 130023, Peoples R China
[2] Qiqihar Univ, Coll Heilongjiang Prov, Key Lab Fine Chem, Qiqihar 161006, Peoples R China
[3] Jilin Univ, Coll Chem, State Key Lab Inorgan Synth & Preparat Chem, Changchun 130012, Peoples R China
基金
中国国家自然科学基金;
关键词
MO/HZSM-5; CATALYSTS; DEHYDRO-AROMATIZATION; ZEOLITE CATALYSTS; MAS NMR; DEHYDROAROMATIZATION; CONVERSION; BENZENE; CO; NAPHTHALENE; DEHYDROGENATION;
D O I
10.1039/c5nj00672d
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Three types of molybdenum oxide with different sizes (i.e. 10-20 mu m, 0.1-1 mu m and 30-150 nm) were used to modify ZSM-5, which were investigated in the methane non-oxidative aromatization reaction. The structure and surface properties of the prepared catalysts were studied using XRD, SEM, N-2 adsorption/desorption, ICP-AES, NH3-TPD and the IR spectra of pyridine adsorption. The characterization results showed that MoO3 with smaller size calcined at 500 degrees C more easily sublimated to form Mo-species at a atomic/molecular level, diffused into the channels of ZSM-5 and reacted with the Bronsted acid to form Mo-O-Al species, which resulted in the decrease of the Bronsted acid sites in the catalysts. The catalytic results confirmed that nano MoO3 modified ZSM-5 zeolites calcined at 500 degrees C showed higher methane conversion (14.1%) and aromatics yield (9.5%) than micron MoO3 modified ZSM-5. In addition, micron MoO3 modified ZSM-5 calcined under higher temperature (i.e. 550 degrees C) or calcined at 500 degrees C for longer time did not achieve the higher catalytic behaviour. Moreover, nano-MoO3 modified ZSM-5 showed better catalytic stability when compared with micron-MoO3 modified ZSM-5.
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页码:5459 / 5469
页数:11
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