SCI和EI收录∣中国化工学会会刊

中国化学工程学报 ›› 2024, Vol. 69 ›› Issue (5): 192-198.DOI: 10.1016/j.cjche.2024.02.001

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Efficient adsorption separation of methane from C2-C3 hydrocarbons in a Co(II)-nodes metal-organic framework

Jie Zhang1, Xingzhe Guo2, Bing Lin2, Guangzu Xiong2, Hanshuang Wang1, Min Zhang1, Liwen Fan1, Bingwen Li3, Shuisheng Chen2   

  1. 1. Department of Chemistry and Chemical Engineering, Taiyuan Institute of Technology, Taiyuan 030008, China;
    2. Engineering Research Center of Oligosaccharides, Fuyang Normal University, Fuyang 236041, China;
    3. Shandong Key Laboratory of Biophysics, Institute of Biophysics, Dezhou University, Dezhou 253023, China
  • 收稿日期:2023-08-29 修回日期:2024-02-01 出版日期:2024-05-28 发布日期:2024-07-01
  • 通讯作者: Xingzhe Guo,E-mail:guoxingzhe2014@gmail.com;Bingwen Li,E-mail:libingwen@dzu.edu.cn;Shuisheng Chen,E-mail:chenss@fynu.edu.cn
  • 基金资助:
    This work was supported by the National Natural Science Foundation of China (21401099), the Natural Science Foundation of Shanxi Province (202203021212331), Science and Technology Innovation Project of Colleges and Universities of Shanxi Province (2022L532), the National Natural Science Foundation of Anhui Province (2008085MB32 and KJ2021ZD0073), Natural Science Foundation of Shandong Province (ZR2021QB159). This work is also supported by the Talent Program Foundation of Dezhou University (2021xjrc102).

Efficient adsorption separation of methane from C2-C3 hydrocarbons in a Co(II)-nodes metal-organic framework

Jie Zhang1, Xingzhe Guo2, Bing Lin2, Guangzu Xiong2, Hanshuang Wang1, Min Zhang1, Liwen Fan1, Bingwen Li3, Shuisheng Chen2   

  1. 1. Department of Chemistry and Chemical Engineering, Taiyuan Institute of Technology, Taiyuan 030008, China;
    2. Engineering Research Center of Oligosaccharides, Fuyang Normal University, Fuyang 236041, China;
    3. Shandong Key Laboratory of Biophysics, Institute of Biophysics, Dezhou University, Dezhou 253023, China
  • Received:2023-08-29 Revised:2024-02-01 Online:2024-05-28 Published:2024-07-01
  • Contact: Xingzhe Guo,E-mail:guoxingzhe2014@gmail.com;Bingwen Li,E-mail:libingwen@dzu.edu.cn;Shuisheng Chen,E-mail:chenss@fynu.edu.cn
  • Supported by:
    This work was supported by the National Natural Science Foundation of China (21401099), the Natural Science Foundation of Shanxi Province (202203021212331), Science and Technology Innovation Project of Colleges and Universities of Shanxi Province (2022L532), the National Natural Science Foundation of Anhui Province (2008085MB32 and KJ2021ZD0073), Natural Science Foundation of Shandong Province (ZR2021QB159). This work is also supported by the Talent Program Foundation of Dezhou University (2021xjrc102).

摘要: Methane (CH4) as a substitute for other mineral fuels plays a crucial role in reducing energy consumption and preventing environmental pollution. The present study employs a solvothermal method to fabricate a porous framework Co-metal-organic framework (Co-MOF) containing two distinct secondary building units (SBUs): an anionic [Co22-OH)(COO)4(H2O)] and a neutral [CoN2(COO)2]. Notably, within the anionic SBUs, the coordinated water molecules induce the generation of divergent unsaturated Co(II) centers in the unidirectional porous channels, thereby creating open metal sites. The adsorption performance of Co-MOF towards pure component gases was systematically investigated. The results demonstrated that Co-MOF exhibits superior adsorption capacity for C2-C3 hydrocarbons compared to CH4, which offers the potential for efficient adsorption and separation of CH4 from C2-C3 hydrocarbons. The gas selectivity separation ratios of Co-MOF for C2H6/CH4 and C3H8/CH4 were calculated using the ideal adsorbed solution theory method at 273/298 K and 0.1 MPa. The results revealed that Co-MOF achieved remarkable equilibrium separation selectivity for CH4 and C2-C3 hydrocarbon gases among non-modified MOFs, signifying the potential of the synthesized Co-MOF for efficient recovery and purification of CH4 from C2-C3 hydrocarbons. Breakthrough experiments further demonstrate the ability of Co-MOF to purify methane from C2-C3 hydrocarbons in practical gas separation scenarios. Additionally, molecular simulation calculations further substantiate the propensity of anionic SBUs to interact with C2-C3 hydrocarbon compounds. This study provides a novel paradigm for the development of porous MOF materials in the application of gas mixture separation.

关键词: Co-MOF, Separation hydrocarbons, Dynamic breakthrough curves, Molecular simulations adsorbent, Monte Carlo simulation

Abstract: Methane (CH4) as a substitute for other mineral fuels plays a crucial role in reducing energy consumption and preventing environmental pollution. The present study employs a solvothermal method to fabricate a porous framework Co-metal-organic framework (Co-MOF) containing two distinct secondary building units (SBUs): an anionic [Co22-OH)(COO)4(H2O)] and a neutral [CoN2(COO)2]. Notably, within the anionic SBUs, the coordinated water molecules induce the generation of divergent unsaturated Co(II) centers in the unidirectional porous channels, thereby creating open metal sites. The adsorption performance of Co-MOF towards pure component gases was systematically investigated. The results demonstrated that Co-MOF exhibits superior adsorption capacity for C2-C3 hydrocarbons compared to CH4, which offers the potential for efficient adsorption and separation of CH4 from C2-C3 hydrocarbons. The gas selectivity separation ratios of Co-MOF for C2H6/CH4 and C3H8/CH4 were calculated using the ideal adsorbed solution theory method at 273/298 K and 0.1 MPa. The results revealed that Co-MOF achieved remarkable equilibrium separation selectivity for CH4 and C2-C3 hydrocarbon gases among non-modified MOFs, signifying the potential of the synthesized Co-MOF for efficient recovery and purification of CH4 from C2-C3 hydrocarbons. Breakthrough experiments further demonstrate the ability of Co-MOF to purify methane from C2-C3 hydrocarbons in practical gas separation scenarios. Additionally, molecular simulation calculations further substantiate the propensity of anionic SBUs to interact with C2-C3 hydrocarbon compounds. This study provides a novel paradigm for the development of porous MOF materials in the application of gas mixture separation.

Key words: Co-MOF, Separation hydrocarbons, Dynamic breakthrough curves, Molecular simulations adsorbent, Monte Carlo simulation