One-step ethylene separation from ternary C2 hydrocarbon mixture with a robust zirconium metal-organic framework

doi:10.1016/j.cjche.2023.01.001

中国化学工程学报 ›› 2023, Vol. 59 ›› Issue (7): 9-15.DOI: 10.1016/j.cjche.2023.01.001

• Full Length Article • 上一篇下一篇

One-step ethylene separation from ternary C₂ hydrocarbon mixture with a robust zirconium metal-organic framework

Yuan Liu¹, Hanting Xiong¹, Jingwen Chen¹, Shixia Chen¹, Zhenyu Zhou¹, Zheling Zeng¹, Shuguang Deng², Jun Wang¹

1. School of Chemistry and Chemical Engineering, Nanchang University, Nanchang 330031, China;
2. School for Engineering of Matter, Transport and Energy, Arizona State University, Tempe, AZ 85287, United States

收稿日期:2022-11-15 修回日期:2022-12-25 出版日期:2023-07-28 发布日期:2023-10-14
通讯作者: Jingwen Chen,E-mail:chenjw@ncu.edu.cn;Jun Wang,E-mail:jwang7@ncu.edu.cn
基金资助:
This research work was supported by the National Natural Science Foundation of China (21908090, 22008099, 22108243, and 22168023) and Natural Science Foundation of Jiangxi Province (20224ACB204003).

One-step ethylene separation from ternary C₂ hydrocarbon mixture with a robust zirconium metal-organic framework

Yuan Liu¹, Hanting Xiong¹, Jingwen Chen¹, Shixia Chen¹, Zhenyu Zhou¹, Zheling Zeng¹, Shuguang Deng², Jun Wang¹

1. School of Chemistry and Chemical Engineering, Nanchang University, Nanchang 330031, China;
2. School for Engineering of Matter, Transport and Energy, Arizona State University, Tempe, AZ 85287, United States

Received:2022-11-15 Revised:2022-12-25 Online:2023-07-28 Published:2023-10-14
Contact: Jingwen Chen,E-mail:chenjw@ncu.edu.cn;Jun Wang,E-mail:jwang7@ncu.edu.cn
Supported by:
This research work was supported by the National Natural Science Foundation of China (21908090, 22008099, 22108243, and 22168023) and Natural Science Foundation of Jiangxi Province (20224ACB204003).

摘要/Abstract

摘要： One-step separation of high-purity ethylene (C₂H₄) from C₂ hydrocarbon mixture is critical but challenging because of the very similar molecular sizes and physical properties of C₂H₄, ethane (C₂H₆), and acetylene (C₂H₂). Herein, we report a robust zirconium metal-organic framework (MOF) Zr-TCA (H₃TCA = 4,4',4″-tricarboxytriphenylamine) with suitable pore size (0.6 nm×0.7 nm) and pore environment for direct C₂H₄ purification from C₂H₄/C₂H₂/C₂H₆ gas-mixture. Computational studies indicate that the abundant oxygen atoms and non-polar phenyl rings created favorable pore environments for the preferential binding of C₂H₂ and C₂H₆ over C₂H₄. As a result, Zr-TCA exhibits not only high C₂H₆ (2.28 mmol·g^-1) and C₂H₂ (2.78 mmol·g^-1) adsorption capacity but also excellent C₂H₆/C₂H₄ (2.72) and C₂H₂/C₂H₄ (5.64) selectivity, surpassing most of one-step C₂H₄ purification MOF materials. Dynamic breakthrough experiments confirm that Zr-TCA can produce high-purity C₂H₄ (>99.9%) from a ternary gas mixture (1/9/90 C₂H₂/C₂H₆/C₂H₄) in a single step with a high C₂H₄ productivity of 5.61 L·kg^-1.

关键词: Zirconium metal–organic framework, Adsorption, Separation, One-step ethylene purification

Abstract: One-step separation of high-purity ethylene (C₂H₄) from C₂ hydrocarbon mixture is critical but challenging because of the very similar molecular sizes and physical properties of C₂H₄, ethane (C₂H₆), and acetylene (C₂H₂). Herein, we report a robust zirconium metal-organic framework (MOF) Zr-TCA (H₃TCA = 4,4',4″-tricarboxytriphenylamine) with suitable pore size (0.6 nm×0.7 nm) and pore environment for direct C₂H₄ purification from C₂H₄/C₂H₂/C₂H₆ gas-mixture. Computational studies indicate that the abundant oxygen atoms and non-polar phenyl rings created favorable pore environments for the preferential binding of C₂H₂ and C₂H₆ over C₂H₄. As a result, Zr-TCA exhibits not only high C₂H₆ (2.28 mmol·g^-1) and C₂H₂ (2.78 mmol·g^-1) adsorption capacity but also excellent C₂H₆/C₂H₄ (2.72) and C₂H₂/C₂H₄ (5.64) selectivity, surpassing most of one-step C₂H₄ purification MOF materials. Dynamic breakthrough experiments confirm that Zr-TCA can produce high-purity C₂H₄ (>99.9%) from a ternary gas mixture (1/9/90 C₂H₂/C₂H₆/C₂H₄) in a single step with a high C₂H₄ productivity of 5.61 L·kg^-1.

Key words: Zirconium metal–organic framework, Adsorption, Separation, One-step ethylene purification

Yuan Liu, Hanting Xiong, Jingwen Chen, Shixia Chen, Zhenyu Zhou, Zheling Zeng, Shuguang Deng, Jun Wang. One-step ethylene separation from ternary C₂ hydrocarbon mixture with a robust zirconium metal-organic framework[J]. 中国化学工程学报, 2023, 59(7): 9-15.

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One-step ethylene separation from ternary C₂ hydrocarbon mixture with a robust zirconium metal-organic framework

One-step ethylene separation from ternary C₂ hydrocarbon mixture with a robust zirconium metal-organic framework

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