Thermal stable Pt clusters anchored by K/TiO2-Al2O3 for efficient cycloalkane dehydrogenation

doi:10.1016/j.cjche.2024.05.018

中国化学工程学报 ›› 2024, Vol. 72 ›› Issue (8): 187-198.DOI: 10.1016/j.cjche.2024.05.018

Thermal stable Pt clusters anchored by K/TiO₂-Al₂O₃ for efficient cycloalkane dehydrogenation

Zhendong Wang¹, Bofeng Zhang¹, Guozhu Liu^1,2, Xiangwen Zhang^1,2

1 Key Laboratory for Green Chemical Technology of the Ministry of Education, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China;
2 Zhejiang Institute of Tianjin University, Ningbo 315201, China

收稿日期:2023-12-23 修回日期:2024-05-22 出版日期:2024-08-28 发布日期:2024-10-17
通讯作者: Guozhu Liu,E-mail:gliu@tju.edu.cn;Xiangwen Zhang,E-mail:zhangxiangwen@tju.edu.cn.Tel./Fax:+86 022 85356099
基金资助:
This work was supported by the National Natural Science Foundation of China (22025802).

Thermal stable Pt clusters anchored by K/TiO₂-Al₂O₃ for efficient cycloalkane dehydrogenation

Zhendong Wang¹, Bofeng Zhang¹, Guozhu Liu^1,2, Xiangwen Zhang^1,2

1 Key Laboratory for Green Chemical Technology of the Ministry of Education, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China;
2 Zhejiang Institute of Tianjin University, Ningbo 315201, China

Received:2023-12-23 Revised:2024-05-22 Online:2024-08-28 Published:2024-10-17
Contact: Guozhu Liu,E-mail:gliu@tju.edu.cn;Xiangwen Zhang,E-mail:zhangxiangwen@tju.edu.cn.Tel./Fax:+86 022 85356099
Supported by:
This work was supported by the National Natural Science Foundation of China (22025802).

摘要/Abstract

摘要： Catalytic dehydrogenation of cycloalkanes is considered a valuable endothermic process for alleviating the thermal barrier issue of hypersonic vehicles. However, conventional Pt-based catalysts often face the severe problem of metal sintering under high-temperature conditions. Herein, we develop an efficient K₂CO₃-modified Pt/TiO₂-Al₂O₃ (K-Pt/TA) for cycloalkane dehydrogenation. The optimized K-Pt/TA showed a high specific activity above 27.9 mol·mol^-1·s^-1(H₂/Pt), with toluene selectivity above 90.0% at 600 °C with a high weight hourly space velocity of 266.4 h^-1. The introduction of alkali metal ions could generate titanate layers after high-temperature hydrogen reduction treatment, which promotes the generation of oxygen vacancy defects to anchored Pt clusters. In addition, the titanate layers could weaken the surface acidity of catalysts and inhibit side reactions, including pyrolysis, polymerization, and isomerization reactions. Thus, this work provides a modification method to develop efficient and stable dehydrogenation catalysts under high-temperature conditions.

关键词: Cycloalkane dehydrogenation, Pt clusters, Oxygen vacancy defects, Coking, Stability, Deactivation

Abstract: Catalytic dehydrogenation of cycloalkanes is considered a valuable endothermic process for alleviating the thermal barrier issue of hypersonic vehicles. However, conventional Pt-based catalysts often face the severe problem of metal sintering under high-temperature conditions. Herein, we develop an efficient K₂CO₃-modified Pt/TiO₂-Al₂O₃ (K-Pt/TA) for cycloalkane dehydrogenation. The optimized K-Pt/TA showed a high specific activity above 27.9 mol·mol^-1·s^-1(H₂/Pt), with toluene selectivity above 90.0% at 600 °C with a high weight hourly space velocity of 266.4 h^-1. The introduction of alkali metal ions could generate titanate layers after high-temperature hydrogen reduction treatment, which promotes the generation of oxygen vacancy defects to anchored Pt clusters. In addition, the titanate layers could weaken the surface acidity of catalysts and inhibit side reactions, including pyrolysis, polymerization, and isomerization reactions. Thus, this work provides a modification method to develop efficient and stable dehydrogenation catalysts under high-temperature conditions.

Key words: Cycloalkane dehydrogenation, Pt clusters, Oxygen vacancy defects, Coking, Stability, Deactivation

Zhendong Wang, Bofeng Zhang, Guozhu Liu, Xiangwen Zhang. Thermal stable Pt clusters anchored by K/TiO₂-Al₂O₃ for efficient cycloalkane dehydrogenation[J]. 中国化学工程学报, 2024, 72(8): 187-198.

Zhendong Wang, Bofeng Zhang, Guozhu Liu, Xiangwen Zhang. Thermal stable Pt clusters anchored by K/TiO₂-Al₂O₃ for efficient cycloalkane dehydrogenation[J]. Chinese Journal of Chemical Engineering, 2024, 72(8): 187-198.

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Thermal stable Pt clusters anchored by K/TiO₂-Al₂O₃ for efficient cycloalkane dehydrogenation

Thermal stable Pt clusters anchored by K/TiO₂-Al₂O₃ for efficient cycloalkane dehydrogenation

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