SCI和EI收录∣中国化工学会会刊

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. 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. 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: 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