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A gating ultramicroporous metal-organic framework showing high adsorption selectivity, capacity and rate for xylene separation

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Abstract

Adsorptive separation of p-xylene (pX) from xylene isomers is a key process in chemical industry, but known adsorbents cannot simultaneously achieve high adsorption selectivity, capacity, and rate. Here, we demonstrate gating ultramicropore as a solution for this challenge. Slight modification of the synthetic condition gives rise to isomeric metal-organic frameworks α-[Zn(pba)] (MAF-88, H2pba = 4-(1H-pyrazol-4-yl)benzoic acid) and β-[Zn(pba)] (MAF-89) possessing similar pillared-column structures, porosities, and high pX capacities of 2.0 mmol g−1, but very different framework/pore topologies, pore sizes, and pX selectivities. For binary and ternary mixtures of liquid xylene isomers, MAF-88 with narrow one-dimensional (1D) channels shows pX selectivity of 11 and 1.6, while MAF-89 with 3D-connected quasi-discrete pores shows pX selectivity up to 221 and 46, respectively. Thermogravimetry, differential scanning calorimetry, and time-dependent separation experiments reveal that the kinetic effects of the gating pores play more important roles than the thermodynamic effects, which is further confirmed by single-crystal X-ray diffraction and computational simulations.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (21731007, 22090061, 21821003, 22161021). C.-T. He acknowledges the support of Jiangxi Province (jxsq2018106041) and the “Young Elite Scientists Sponsorship Program” by CAST. We thank the staffs of BL17B/BL18U/BL19U1/BL19U2/BL01B beamlines at National Center for Protein Sciences Shanghai and Shanghai Synchrotron Radiation Facility, for assistance in collecting the single-crystal diffraction data of MAF-89, and thank Prof. Ming-Liang Tong and Mr. Kai-Ping Xie from Sun Yat-Sen University for assistance in collecting the single-crystal diffraction data of MAF-88.

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Authors and Affiliations

  1. Key Laboratory of Bioinorganic and Synthetic Chemistry (Ministry of Education), School of Chemistry, Sun Yat-Sen University, Guangzhou, 510275, China

    Zi-Ming Ye, De-Xuan Liu, Yan-Tong Xu, Chao Wang, Kai Zheng, Dong-Dong Zhou, Chun-Ting He & Jie-Peng Zhang

  2. Key Lab of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of Education/National Engineering Research Center for Carbohydrate Synthesis, Jiangxi Normal University, Nanchang, 330022, China

    Xue-Feng Zhang & Chun-Ting He

  3. Guangdong Provincial Key Laboratory of New and Renewable Energy Research and Development, Guangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou, 510640, China

    Yan-Tong Xu

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  1. Zi-Ming Ye
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  2. Xue-Feng Zhang
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  4. Yan-Tong Xu
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Correspondence to Chun-Ting He or Jie-Peng Zhang.

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Supporting information The supporting information is available online at http://chem.scichina.com and http://link.springer.com/journal/11426. The supporting materials are published as submitted, without typesetting or editing. The responsibility for scientific accuracy and content remains entirely with the authors.

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A gating ultramicroporous metal-organic framework showing high adsorption selectivity, capacity and rate for xylene separation

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Ye, ZM., Zhang, XF., Liu, DX. et al. A gating ultramicroporous metal-organic framework showing high adsorption selectivity, capacity and rate for xylene separation. Sci. China Chem. 65, 1552–1558 (2022). https://doi.org/10.1007/s11426-022-1304-1

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