Influence of extra-framework Al in Fe-MOR catalysts for the direct conversion of methane to oxygenates by nitrous oxide

doi:10.1016/j.cjche.2020.06.007

中国化学工程学报 ›› 2021, Vol. 33 ›› Issue (5): 132-138.DOI: 10.1016/j.cjche.2020.06.007

• Catalysis, Kinetics and Reaction Engineering • 上一篇下一篇

Influence of extra-framework Al in Fe-MOR catalysts for the direct conversion of methane to oxygenates by nitrous oxide

Shenglai Li¹, Lisong Fan¹, Lina Song^1,2, Dangguo Cheng^1,2, Fengqiu Chen^1,2

1 College of Chemical and Biological Engineering, Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology, Zhejiang University, Hangzhou 310027, China;
2 Institute of Zhejiang University-Quzhou, 78 Jiuhua Boulevard North, Quzhou 324000, China

收稿日期:2020-04-12 修回日期:2020-05-28 出版日期:2021-05-28 发布日期:2021-08-19
通讯作者: Dangguo Cheng
基金资助:
This research was supported by the Zhejiang Provincial Natural Science Foundation of China (LR18B060001), Basic Research Project of Sinopec Group (415025) and the Fundamental Research Funds for the Central Universities.

Influence of extra-framework Al in Fe-MOR catalysts for the direct conversion of methane to oxygenates by nitrous oxide

Shenglai Li¹, Lisong Fan¹, Lina Song^1,2, Dangguo Cheng^1,2, Fengqiu Chen^1,2

1 College of Chemical and Biological Engineering, Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology, Zhejiang University, Hangzhou 310027, China;
2 Institute of Zhejiang University-Quzhou, 78 Jiuhua Boulevard North, Quzhou 324000, China

Received:2020-04-12 Revised:2020-05-28 Online:2021-05-28 Published:2021-08-19
Contact: Dangguo Cheng
Supported by:
This research was supported by the Zhejiang Provincial Natural Science Foundation of China (LR18B060001), Basic Research Project of Sinopec Group (415025) and the Fundamental Research Funds for the Central Universities.

摘要/Abstract

摘要： Iron-containing zeolites play an important role in the selective oxidation of methane to oxygenates by nitrous oxide. A solid-state ion exchange method is adopted to prepare Fe-MOR zeolite catalysts with different amounts of extra-framework Al. EPR spectra and UV-vis spectra show that the percentage of iron ions in tetrahedral or octahedral coordination increases while those of clustered Fe species decrease by the addition of extra-framework Al species. Nitrous oxide titration reveals that more active Fe centers are formed, which promote the nitrous oxide consumption. The number of active centers in the catalyst with the introduction of extra-framework Al is about four times that of the catalyst without the addition of extra-framework Al. Due to this, there is an increase in the methane conversion, total selectivity and yield of oxygenates.

关键词: Extra-framework Al, Methane conversion, α-site, Nitrous oxide, Oxygenates

Abstract: Iron-containing zeolites play an important role in the selective oxidation of methane to oxygenates by nitrous oxide. A solid-state ion exchange method is adopted to prepare Fe-MOR zeolite catalysts with different amounts of extra-framework Al. EPR spectra and UV-vis spectra show that the percentage of iron ions in tetrahedral or octahedral coordination increases while those of clustered Fe species decrease by the addition of extra-framework Al species. Nitrous oxide titration reveals that more active Fe centers are formed, which promote the nitrous oxide consumption. The number of active centers in the catalyst with the introduction of extra-framework Al is about four times that of the catalyst without the addition of extra-framework Al. Due to this, there is an increase in the methane conversion, total selectivity and yield of oxygenates.

Key words: Extra-framework Al, Methane conversion, α-site, Nitrous oxide, Oxygenates

Shenglai Li, Lisong Fan, Lina Song, Dangguo Cheng, Fengqiu Chen. Influence of extra-framework Al in Fe-MOR catalysts for the direct conversion of methane to oxygenates by nitrous oxide[J]. 中国化学工程学报, 2021, 33(5): 132-138.

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Influence of extra-framework Al in Fe-MOR catalysts for the direct conversion of methane to oxygenates by nitrous oxide

Influence of extra-framework Al in Fe-MOR catalysts for the direct conversion of methane to oxygenates by nitrous oxide

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