Methane oxybromination over Rh-based catalysts: Effect of supports

doi:10.1016/j.cjche.2019.09.001

中国化学工程学报 ›› 2020, Vol. 28 ›› Issue (7): 1809-1815.DOI: 10.1016/j.cjche.2019.09.001

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

Methane oxybromination over Rh-based catalysts: Effect of supports

Peng Wang¹, Lang Chen¹, Sheng Shen¹, Chak-Tong Au², Shuangfeng Yin¹

1 State Key Laboratory of Chemo/Biosensing and Chemometrics, Hunan Provincial Key Laboratory for Cost-effective Utilization of Fossil Fuel Aimed at Reducing Carbon-dioxide Emissions, College of Chemistry and Chemical Engineering, Hunan University, Changsha 410082, China.;
2 College of Chemistry and Chemical Engineering, Hunan Institute of Engineering, Xiangtan 411104, China

收稿日期:2019-05-13 修回日期:2019-09-02 出版日期:2020-07-28 发布日期:2020-08-31
通讯作者: Shuangfeng Yin
基金资助:
This project was financially supported by the National Natural Science Foundation of China (Nos. 21725602, 21776064, 21671062 and 21476065), and the Innovative Research Groups of Hunan Province (2019JJ10001).

Methane oxybromination over Rh-based catalysts: Effect of supports

Peng Wang¹, Lang Chen¹, Sheng Shen¹, Chak-Tong Au², Shuangfeng Yin¹

1 State Key Laboratory of Chemo/Biosensing and Chemometrics, Hunan Provincial Key Laboratory for Cost-effective Utilization of Fossil Fuel Aimed at Reducing Carbon-dioxide Emissions, College of Chemistry and Chemical Engineering, Hunan University, Changsha 410082, China.;
2 College of Chemistry and Chemical Engineering, Hunan Institute of Engineering, Xiangtan 411104, China

Received:2019-05-13 Revised:2019-09-02 Online:2020-07-28 Published:2020-08-31
Contact: Shuangfeng Yin
Supported by:
This project was financially supported by the National Natural Science Foundation of China (Nos. 21725602, 21776064, 21671062 and 21476065), and the Innovative Research Groups of Hunan Province (2019JJ10001).

摘要/Abstract

摘要： Bromine mediation has been regarded as one of the most efficient ways to activate and convert methane to useful organics. This article reports the effects of active components (Rh, Ru, Pd and Pt) and supports (SiO₂, MgO and Al₂O₃) on the catalysis of methane oxybromination. Among the prepared catalysts, Rh/SiO₂ is the best in performance (CH₄ conversion of ca. 20% and CH₃Br selectivity exceeding 70%). The results reveal that support type has a notable influence on the catalytic performance of Rh, especially on product distribution. The high selectivity to CH₃Br over Rh/SiO₂ is attributed to its low propensity for CH₃Br oxidation. It was found that Rh small in particle size shows high catalytic activity and CH₃Br selectivity. Although silicalite-1 zeolite suffers from a certain degree of structural damage due to the presence of high temperature steam, the use of silicalite-1 as support results in a performance comparable to that of Rh/SiO₂.

关键词: Methane conversion, Oxybromination, Methyl bromide, Rhodium catalyst

Abstract: Bromine mediation has been regarded as one of the most efficient ways to activate and convert methane to useful organics. This article reports the effects of active components (Rh, Ru, Pd and Pt) and supports (SiO₂, MgO and Al₂O₃) on the catalysis of methane oxybromination. Among the prepared catalysts, Rh/SiO₂ is the best in performance (CH₄ conversion of ca. 20% and CH₃Br selectivity exceeding 70%). The results reveal that support type has a notable influence on the catalytic performance of Rh, especially on product distribution. The high selectivity to CH₃Br over Rh/SiO₂ is attributed to its low propensity for CH₃Br oxidation. It was found that Rh small in particle size shows high catalytic activity and CH₃Br selectivity. Although silicalite-1 zeolite suffers from a certain degree of structural damage due to the presence of high temperature steam, the use of silicalite-1 as support results in a performance comparable to that of Rh/SiO₂.

Key words: Methane conversion, Oxybromination, Methyl bromide, Rhodium catalyst

Peng Wang, Lang Chen, Sheng Shen, Chak-Tong Au, Shuangfeng Yin. Methane oxybromination over Rh-based catalysts: Effect of supports[J]. 中国化学工程学报, 2020, 28(7): 1809-1815.

Peng Wang, Lang Chen, Sheng Shen, Chak-Tong Au, Shuangfeng Yin. Methane oxybromination over Rh-based catalysts: Effect of supports[J]. Chinese Journal of Chemical Engineering, 2020, 28(7): 1809-1815.

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Methane oxybromination over Rh-based catalysts: Effect of supports

Methane oxybromination over Rh-based catalysts: Effect of supports

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