Effect of oxidative/reductive pretreatment on the performance of Cu<sub>2</sub>O/AC catalyst for oxidative carbonylation of methnol

WANG Rui-yu; BAI Si-yu; ZHENG Chuan-yue; LI Zhong

Volume 43 Issue 10

Oct. 2015

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Article Navigation > Journal of Fuel Chemistry and Technology > 2015 > 43(10): 1245-1251

WANG Rui-yu, BAI Si-yu, ZHENG Chuan-yue, LI Zhong. Effect of oxidative/reductive pretreatment on the performance of Cu2O/AC catalyst for oxidative carbonylation of methnol[J]. Journal of Fuel Chemistry and Technology, 2015, 43(10): 1245-1251.

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WANG Rui-yu, BAI Si-yu, ZHENG Chuan-yue, LI Zhong. Effect of oxidative/reductive pretreatment on the performance of Cu₂O/AC catalyst for oxidative carbonylation of methnol[J]. Journal of Fuel Chemistry and Technology, 2015, 43(10): 1245-1251.

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Effect of oxidative/reductive pretreatment on the performance of Cu₂O/AC catalyst for oxidative carbonylation of methnol

1.
Key Laboratory of Coal-based CO₂ Capture and Geological Storage of Jiangsu province, China University of Mining and Technology, Xuzhou 221006, China;
2.
Key Laboratory of Coal Science and Technology, Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan 030024, China

Funds: The project was supported by the National Natural Science Foundation of China (21506249), the Jiangsu Postdoctoral Sustentantion Fund (1401096c) and the Fundamental Research Funds for the Central Universities (China University of Mining and Technology, 2014QNA19).

Received Date: 2015-03-24
Rev Recd Date: 2015-06-09
Publish Date: 2015-10-31

Abstract

Abstract

The Cu₂O/AC catalyst prepared by pyrolysis of copper acetate supported on activatede carbon was pretreated under oxidative (O₂/N₂) or reductive (H₂/N₂ and CO/N₂) atmospheres. The oxidation/reduction of Cu₂O was completed through pretreatment at 350 ℃ for 4 h, the Cu₂O in catalyst could be completely oxidized to CuO by oxidative atmosphere, or reduced to metallic copper by reductive atmosphere. The catalyst activities were evaluated in a continuous fixed-bed tubular micro reactor under atmospheric pressure at 140 ℃. The catalyst pretreated by CO/N₂ had good Cu⁰ dispersion on its surface and exhibited the highest activity. The space-time yield and selectivity of DMC reached 261.9 mg/(g·h) and 74.7%, respectively. After 58 h reaction, the valence state of copper species and the catalytic activity of catalysts pretreated by reductive atmosphere were found to be close to that of the Cu₂O/AC catalyst. Comparing the catalytic performance, the characterization of surface and bulk copper species before and after reaction, it was obvious that metallic copper exhibited a high initial activity, while Cu₂O was stable in catalytic activity and valence state, and CuO was low in activity.
- copper based catalyst,
- activated carbon,
- pretreatment,
- oxidative carbonylation,
- dimethyl carbonate,
- heterogeneous catalysis

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References(28)

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