Effect of CO2 on the structural variation of Na2WO4/Mn/SiO2 catalyst for oxidative coupling of methane to ethylene

能源化学(英文) ›› 2015, Vol. 21 ›› Issue (4): 394-400.

Effect of CO₂ on the structural variation of Na₂WO₄/Mn/SiO₂ catalyst for oxidative coupling of methane to ethylene

Jia Shi, Lu Yao, Changwei Hu

Key Laboratory of Green Chemistry and Technology, Ministry of Education, College of Chemistry, Sichuan University, Chengdu 610064, Sichuan, China

收稿日期:2015-03-29 修回日期:2015-06-30 发布日期:2015-08-21
通讯作者: Changwei Hu
基金资助:
The authors are grateful for financial support from the Ministry of Science and Technology (Nos. 2012BAC20B10) and the National Natural Science Foundation of China (Nos. 21321061 and 20976109). The characterization of the catalysts from Analytical and Testing Center of Sichuan University was also appreciated.

Effect of CO₂ on the structural variation of Na₂WO₄/Mn/SiO₂ catalyst for oxidative coupling of methane to ethylene

Jia Shi, Lu Yao, Changwei Hu

Key Laboratory of Green Chemistry and Technology, Ministry of Education, College of Chemistry, Sichuan University, Chengdu 610064, Sichuan, China

Received:2015-03-29 Revised:2015-06-30 Published:2015-08-21
Contact: Changwei Hu
Supported by:
The authors are grateful for financial support from the Ministry of Science and Technology (Nos. 2012BAC20B10) and the National Natural Science Foundation of China (Nos. 21321061 and 20976109). The characterization of the catalysts from Analytical and Testing Center of Sichuan University was also appreciated.

摘要/Abstract

摘要： In this work, the influence of CO₂ on the structural variation and catalytic performance of Na₂WO₄/Mn/SiO₂ for oxidative coupling of methane to ethylene was investigated. The catalyst was prepared by impregnation method and characterized by XRD, Raman and XPS techniques. Appropriate amount of CO₂ in the reactant gases enhanced the formation of surface tetrahedral Na₂WO₄ species and promoted the migration of O in MO_x, Na,Wfrom the catalyst bulk to surface, which were favorable for oxidative coupling of methane. When the molar ratio of CH₄/O₂/CO₂ was 3/1/2, enriched surface tetrahedral Na₂WO₄ species and high surface concentration of O in MO_x, Na, W were detected, and then high CH₄ conversion of 33.1% and high C₂H₄ selectivity of 56.2% were obtained. With further increase of CO₂ in the reagent gases, the content of active surface tetrahedral Na₂WO₄ species and surface concentration of O in MO_x, Na, W decreased, while that of inactive species (MnWO₄ and Mn₂O₃) increased dramatically, leading to low CH₄ conversion and low C₂H₄ selectivity. It could be speculated that Na₂WO₄ crystal was transformed into MnWO₄ crystal with excessive CO₂ added under the reaction conditions. Pretreatment of Na₂WO₄/Mn/SiO₂ catalyst by moderate amount of CO₂ before OCM also promoted the formation of Na₂WO₄ species.

关键词: Oxidative coupling of methane, CO₂, C₂H₄, Na₂WO₄/Mn/SiO₂ catalyst, Structural variation

Abstract: In this work, the influence of CO₂ on the structural variation and catalytic performance of Na₂WO₄/Mn/SiO₂ for oxidative coupling of methane to ethylene was investigated. The catalyst was prepared by impregnation method and characterized by XRD, Raman and XPS techniques. Appropriate amount of CO₂ in the reactant gases enhanced the formation of surface tetrahedral Na₂WO₄ species and promoted the migration of O in MO_x, Na,Wfrom the catalyst bulk to surface, which were favorable for oxidative coupling of methane. When the molar ratio of CH₄/O₂/CO₂ was 3/1/2, enriched surface tetrahedral Na₂WO₄ species and high surface concentration of O in MO_x, Na, W were detected, and then high CH₄ conversion of 33.1% and high C₂H₄ selectivity of 56.2% were obtained. With further increase of CO₂ in the reagent gases, the content of active surface tetrahedral Na₂WO₄ species and surface concentration of O in MO_x, Na, W decreased, while that of inactive species (MnWO₄ and Mn₂O₃) increased dramatically, leading to low CH₄ conversion and low C₂H₄ selectivity. It could be speculated that Na₂WO₄ crystal was transformed into MnWO₄ crystal with excessive CO₂ added under the reaction conditions. Pretreatment of Na₂WO₄/Mn/SiO₂ catalyst by moderate amount of CO₂ before OCM also promoted the formation of Na₂WO₄ species.

Key words: Oxidative coupling of methane, CO₂, C₂H₄, Na₂WO₄/Mn/SiO₂ catalyst, Structural variation

Jia Shi, Lu Yao, Changwei Hu. Effect of CO₂ on the structural variation of Na₂WO₄/Mn/SiO₂ catalyst for oxidative coupling of methane to ethylene[J]. 能源化学(英文), 2015, 21(4): 394-400.

Jia Shi, Lu Yao, Changwei Hu. Effect of CO₂ on the structural variation of Na₂WO₄/Mn/SiO₂ catalyst for oxidative coupling of methane to ethylene[J]. Journal of Energy Chemistry, 2015, 21(4): 394-400.

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Effect of CO₂ on the structural variation of Na₂WO₄/Mn/SiO₂ catalyst for oxidative coupling of methane to ethylene

Effect of CO₂ on the structural variation of Na₂WO₄/Mn/SiO₂ catalyst for oxidative coupling of methane to ethylene

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