Citation: GU Ying-ying, ZHANG Zhen-zhou, WANG Wen-feng, GAO Xiu-juan, ZHANG Qing-de, HAN Yi-zhuo, TAN Yi-sheng. Effects of calcination atmosphere on the structure and performance of MoO₃-SnO₂ catalyst for the oxidation of dimethyl ether at low temperature[J]. Journal of Fuel Chemistry and Technology, ;2017, 45(5): 572-580. shu

Effects of calcination atmosphere on the structure and performance of MoO₃-SnO₂ catalyst for the oxidation of dimethyl ether at low temperature

1.
State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China
2.
University of Chinese Academy of Sciences, Beijing 100049, China

Corresponding author: ZHANG Qing-de, qdzhang@sxicc.ac.cn
Received Date: 24 January 2017
Revised Date: 31 March 2017

Fund Project: Youth Innovation Promotion Association CAS 2014155the National Natural Science Foundation of China 20903114the National Natural Science Foundation of China 21373253

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MoO₃-SnO₂ catalysts with a Mo/Sn molar ratio of 1:3 was prepared by the co-precipitation method and calcined in different atmospheres (O₂, air, N₂ and H₂); the effect of calcination atmosphere on the catalytic performance of MoO₃-SnO₂ in the oxidation of dimethyl ether (DME) to methyl formate (MF) was investigated. The results show that the MoO₃-SnO₂ catalyst prepared by calcination in O₂ exhibits the highest activity; the conversion of DME reaches 25.10%, with the selectivity of 72.21% to MF. Over the catalyst calcined in H₂, the conversion of DME is only 7.01%, with the selectivity of 75.82% to MF. The activity of the MoO₃-SnO₂ catalysts calcined at different atmospheres follows the order of O₂ > air > N₂ > H₂. The results of XRD, Raman, XPS and ESR characterization indicate the presence of MoO_x domains on the surface of the MoO₃-SnO₂ catalyst with a Mo/Sn molar ratio of 1:3. The terminal Mo=O groups of oligomeric MoO₃ may be the active sites for the methoxy intermediate and the penta-coordinated Mo⁵⁺ species in the Mo-Sn interface may be able to promote the oxidation of DME to MF. Consequently, methoxy species are absorbed on the Mo⁵⁺ species in the Mo-Sn interfaces, which are oxidized to HCHO on the terminal Mo=O groups; after that, the absorbed HCHO may then react with the neighboring absorbed methoxy species, forming MF.
- MoO₃-SnO₂ catalysts,
- calcination atmosphere,
- dimethyl ether oxidation,
- methyl formate
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通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

Effects of calcination atmosphere on the structure and performance of MoO3-SnO2 catalyst for the oxidation of dimethyl ether at low temperature

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通讯作者: 陈斌, bchen63@163.com

Effects of calcination atmosphere on the structure and performance of MoO₃-SnO₂ catalyst for the oxidation of dimethyl ether at low temperature