SCI和EI收录∣中国化工学会会刊

中国化学工程学报 ›› 2022, Vol. 42 ›› Issue (2): 49-54.DOI: 10.1016/j.cjche.2021.09.001

• Recent Advances in Adsorptive Separation Materials and Technologies • 上一篇    下一篇

Efficient separation of C4 olefins using tantalum pentafluor oxide anion-pillared hybrid microporous material

Bin Gao1, Zhaoqiang Zhang1, Jianbo Hu1, Jiyu Cui1, Liyuan Chen1, Xili Cui1,2, Huabin Xing1,2   

  1. 1. Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, China;
    2. Hangzhou Global Scientific and Technological Innovation Center, Zhejiang University, Hangzhou 311215, China
  • 收稿日期:2021-05-29 修回日期:2021-08-31 出版日期:2022-02-28 发布日期:2022-03-30
  • 通讯作者: Huabin Xing,E-mail:xinghb@zju.edu.cn
  • 基金资助:
    This work was supported by Natural Science Foundation of Zhejiang Province (LR20B060001 and LZ18B060001), the National Natural Science Foundation of China (21725603, 21938011), the Entrepreneur Team Introduction Program of Zhejiang (2019R01006), and the Research Computing Center in College of Chemical and Biological Engineering at Zhejiang University.

Efficient separation of C4 olefins using tantalum pentafluor oxide anion-pillared hybrid microporous material

Bin Gao1, Zhaoqiang Zhang1, Jianbo Hu1, Jiyu Cui1, Liyuan Chen1, Xili Cui1,2, Huabin Xing1,2   

  1. 1. Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, China;
    2. Hangzhou Global Scientific and Technological Innovation Center, Zhejiang University, Hangzhou 311215, China
  • Received:2021-05-29 Revised:2021-08-31 Online:2022-02-28 Published:2022-03-30
  • Contact: Huabin Xing,E-mail:xinghb@zju.edu.cn
  • Supported by:
    This work was supported by Natural Science Foundation of Zhejiang Province (LR20B060001 and LZ18B060001), the National Natural Science Foundation of China (21725603, 21938011), the Entrepreneur Team Introduction Program of Zhejiang (2019R01006), and the Research Computing Center in College of Chemical and Biological Engineering at Zhejiang University.

摘要: With the increasing demand for synthetic rubber, the purification of 1,3-butadiene (C4H6) is of great industrial significance. Herein, the successful removal of n-butene (n-C4H8) and iso-butene (iso-C4H8) from 1,3-butadiene (C4H6) was realized by synthesizing a novel TaOF52- anion-pillared ultramicroporous material TaOFFIVE-3-Ni (also referred to as ZU-96, TaOFFIVE=TaOF52-, 3=pyrazine). Single-component adsorption isotherms show that TaOFFIVE-3-Ni can achieve the exclusion of n-C4H8 and iso-C4H8 in the low pressure region (0-30 kPa), and uptake C4H6 with a high capacity of 92.78 cm3·cm-3 (298 K and 100 kPa). The uptake ratio of C4H6/iso-C4H8 on TaOFFIVE-3-Ni was 20.83 (298 K and 100 kPa), which was the highest among the state-of-the-art adsorbents reported so far. With the rotation of anion and pyrazine ring, the pore size changes continuously, which makes smaller-size C4H6 enter the channel while larger-size n-C4H8 and iso-C4H8 are completely blocked. The excellent breakthrough performance of TaOFFIVE-3-Ni shows great potential in industrial separation of C4 olefins. The specific adsorption binding sites within ZU-96 was further revealed through the modeling calculation.

关键词: Adsorptive separation, C4 olefin, 1,3-Butadiene, Anion-pillared hybrid microporous material

Abstract: With the increasing demand for synthetic rubber, the purification of 1,3-butadiene (C4H6) is of great industrial significance. Herein, the successful removal of n-butene (n-C4H8) and iso-butene (iso-C4H8) from 1,3-butadiene (C4H6) was realized by synthesizing a novel TaOF52- anion-pillared ultramicroporous material TaOFFIVE-3-Ni (also referred to as ZU-96, TaOFFIVE=TaOF52-, 3=pyrazine). Single-component adsorption isotherms show that TaOFFIVE-3-Ni can achieve the exclusion of n-C4H8 and iso-C4H8 in the low pressure region (0-30 kPa), and uptake C4H6 with a high capacity of 92.78 cm3·cm-3 (298 K and 100 kPa). The uptake ratio of C4H6/iso-C4H8 on TaOFFIVE-3-Ni was 20.83 (298 K and 100 kPa), which was the highest among the state-of-the-art adsorbents reported so far. With the rotation of anion and pyrazine ring, the pore size changes continuously, which makes smaller-size C4H6 enter the channel while larger-size n-C4H8 and iso-C4H8 are completely blocked. The excellent breakthrough performance of TaOFFIVE-3-Ni shows great potential in industrial separation of C4 olefins. The specific adsorption binding sites within ZU-96 was further revealed through the modeling calculation.

Key words: Adsorptive separation, C4 olefin, 1,3-Butadiene, Anion-pillared hybrid microporous material