SCI和EI收录∣中国化工学会会刊

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. 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. 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: 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