Ca2MnO4-layered perovskite modified by NaNO3 for chemical-looping oxidative dehydrogenation of ethane to ethylene

doi:10.1016/j.cjche.2023.12.021

Chinese Journal of Chemical Engineering ›› 2024, Vol. 68 ›› Issue (4): 53-64.DOI: 10.1016/j.cjche.2023.12.021

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Ca₂MnO₄-layered perovskite modified by NaNO₃ for chemical-looping oxidative dehydrogenation of ethane to ethylene

Weixiao Ding^1,2,3, Kun Zhao², Shican Jiang^1,2, Zhen Huang², Fang He¹

1. College of Chemistry and Bioengineering, Guilin University of Technology, Guilin 541006, China;
2. Guangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou 510640, China;
3. School of Chemistry and Chemical Engineering, Nanjing University of Science and Technology, Nanjing 210094, China

Received:2023-09-25 Revised:2023-11-30 Online:2024-06-28 Published:2024-04-28
Contact: Kun Zhao,E-mail address:zhaokun@ms.giec.ac.cn;Fang He,E-mail address:hefang@glut.edu.cn
Supported by:
The financial support of National Natural Science Foundation of China (22179027) is gratefully acknowledged. This work was also supported by the Natural Science Foundation of Guangxi Province (2021GXNSFAA075063, 2018GXNSFDA281005), and the National Key Research and Development Program of China (2017YFE0105500), Science & Technology Research Project of Guangdong Province (2017A020216009).

Ca₂MnO₄-layered perovskite modified by NaNO₃ for chemical-looping oxidative dehydrogenation of ethane to ethylene

Weixiao Ding^1,2,3, Kun Zhao², Shican Jiang^1,2, Zhen Huang², Fang He¹

1. College of Chemistry and Bioengineering, Guilin University of Technology, Guilin 541006, China;
2. Guangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou 510640, China;
3. School of Chemistry and Chemical Engineering, Nanjing University of Science and Technology, Nanjing 210094, China

通讯作者: Kun Zhao,E-mail address:zhaokun@ms.giec.ac.cn;Fang He,E-mail address:hefang@glut.edu.cn
基金资助:
The financial support of National Natural Science Foundation of China (22179027) is gratefully acknowledged. This work was also supported by the Natural Science Foundation of Guangxi Province (2021GXNSFAA075063, 2018GXNSFDA281005), and the National Key Research and Development Program of China (2017YFE0105500), Science & Technology Research Project of Guangdong Province (2017A020216009).

Abstract

Abstract: Chemical-looping oxidative dehydrogenation (CL-ODH) is a process designed for the conversion of alkanes into olefins through cyclic redox reactions, eliminating the need for gaseous O₂. In this work, we investigated the use of Ca₂MnO₄-layered perovskites modified with NaNO₃ dopants, serving as redox catalysts (also known as oxygen carriers), for the CL-ODH of ethane within a temperature range of 700-780 ℃. Our findings revealed that the incorporation of NaNO₃ as a modifier significantly enhanced the selectivity for ethylene generation from Ca₂MnO₄. At 750 ℃ and a gas hourly space velocity of 1300 h^-1, we achieved an ethane conversion up to 68.17%, accompanied by a corresponding ethylene yield of 57.39%. X-ray photoelectron spectroscopy analysis unveiled that the doping NaNO₃ onto Ca₂MnO₄ not only played a role in reducing the oxidation state of Mn ions but also increased the lattice oxygen content of the redox catalyst. Furthermore, formation of NaNO₃ shell on the surface of Ca₂MnO₄ led to a reduction in the concentration of manganese sites and modulated the oxygen-releasing behavior in a step-wise manner. This modulation contributed significantly to the enhanced selectivity for ethylene of the NaNO₃-doped Ca₂MnO₄ catalyst. These findings provide compelling evidence for the potential of Ca₂MnO₄-layered perovskites as promising redox catalysts in the context of CL-ODH reactions.

Key words: Chemical-looping oxidative dehydrogenation, Ethane, Ethylene, NaNO₃-doped Ca₂MnO₄ redox catalyst, Layered perovskites

摘要： Chemical-looping oxidative dehydrogenation (CL-ODH) is a process designed for the conversion of alkanes into olefins through cyclic redox reactions, eliminating the need for gaseous O₂. In this work, we investigated the use of Ca₂MnO₄-layered perovskites modified with NaNO₃ dopants, serving as redox catalysts (also known as oxygen carriers), for the CL-ODH of ethane within a temperature range of 700-780 ℃. Our findings revealed that the incorporation of NaNO₃ as a modifier significantly enhanced the selectivity for ethylene generation from Ca₂MnO₄. At 750 ℃ and a gas hourly space velocity of 1300 h^-1, we achieved an ethane conversion up to 68.17%, accompanied by a corresponding ethylene yield of 57.39%. X-ray photoelectron spectroscopy analysis unveiled that the doping NaNO₃ onto Ca₂MnO₄ not only played a role in reducing the oxidation state of Mn ions but also increased the lattice oxygen content of the redox catalyst. Furthermore, formation of NaNO₃ shell on the surface of Ca₂MnO₄ led to a reduction in the concentration of manganese sites and modulated the oxygen-releasing behavior in a step-wise manner. This modulation contributed significantly to the enhanced selectivity for ethylene of the NaNO₃-doped Ca₂MnO₄ catalyst. These findings provide compelling evidence for the potential of Ca₂MnO₄-layered perovskites as promising redox catalysts in the context of CL-ODH reactions.

关键词: Chemical-looping oxidative dehydrogenation, Ethane, Ethylene, NaNO₃-doped Ca₂MnO₄ redox catalyst, Layered perovskites

Weixiao Ding, Kun Zhao, Shican Jiang, Zhen Huang, Fang He. Ca₂MnO₄-layered perovskite modified by NaNO₃ for chemical-looping oxidative dehydrogenation of ethane to ethylene[J]. Chinese Journal of Chemical Engineering, 2024, 68(4): 53-64.

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Ca₂MnO₄-layered perovskite modified by NaNO₃ for chemical-looping oxidative dehydrogenation of ethane to ethylene

Ca₂MnO₄-layered perovskite modified by NaNO₃ for chemical-looping oxidative dehydrogenation of ethane to ethylene

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