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<p>The rational design of metal-organic frameworks capable of simultaneous reverse C<sub>2</sub>H<sub>2</sub>/CO<sub>2</sub> separation and one-step C<sub>2</sub>H<sub>4</sub> purification from ternary C<sub>2</sub>H<sub>2</sub>/CO<sub>2</sub>/C<sub>2</sub>H<sub>4</sub> mixtures has never been realized. Herein, we report a novel 2D carborane hybrid metal-organic framework ZNU-13 featuring zigzag 1D channel with contracted neck dimensions (3.9 Å × 3.9 Å) and expanded cavities (8.9 Å × 5.9 Å) to tackle this challenge. The robust porous structure was sustained through mortise-tenon interlocking of the neighboring carborane dicarboxylic-zinc 2D layers. Gas adsorption analysis reveals a rare adsorption selectivity hierarchy of CO<sub>2</sub> &gt; C<sub>2</sub>H<sub>2</sub> &gt; C<sub>2</sub>H<sub>4</sub>, contrasting sharply with the analogue ZNU-14’s conventional selectivity pattern (C<sub>2</sub>H<sub>2</sub> &gt; C<sub>2</sub>H<sub>4</sub> &gt; CO<sub>2</sub>). <i>In-situ</i> gas-loaded single-crystal X-ray diffraction (SCXRD) combined with density functional theory (DFT) calculations elucidates the higher CO<sub>2</sub> binding affinity. CO<sub>2</sub> is tightly trapped in the contracted channel pores with multiple interactions, while C<sub>2</sub>H<sub>2</sub> is located at the large cage cavity with weaker interactions. Various breakthrough experiments validate ZNU-13’s exceptional reverse C<sub>2</sub>H<sub>2</sub>/CO<sub>2</sub> separation performance, exhibiting a dynamic separation factor of 3–5 and maintaining capacity under humid conditions for multiple cycles. Moreover, ZNU-13 enables direct production of polymer-grade C<sub>2</sub>H<sub>4</sub> from equimolar ternary gas mixtures through a single adsorption process, establishing a new benchmark for integrated gas purification systems.</p>

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A novel carborane hybrid metal-organic framework with mortise-tenon architecture for reverse C2H2/CO2 separation and ternary C2H4 purification

  • 期刊论文

  • 发表日期：

    2025年8月1日

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  • Changhong Liu,
  • Shuangshuang Wu,
  • Wenlei Yang,
  • Xue Li,
  • Jéssica Bayer,
  • Binquan Luan,
  • Lingyao Wang,
  • Xiaolei Huang,
  • Yuanbin Zhang

摘要

The rational design of metal-organic frameworks capable of simultaneous reverse C2H2/CO2 separation and one-step C2H4 purification from ternary C2H2/CO2/C2H4 mixtures has never been realized. Herein, we report a novel 2D carborane hybrid metal-organic framework ZNU-13 featuring zigzag 1D channel with contracted neck dimensions (3.9 Å × 3.9 Å) and expanded cavities (8.9 Å × 5.9 Å) to tackle this challenge. The robust porous structure was sustained through mortise-tenon interlocking of the neighboring carborane dicarboxylic-zinc 2D layers. Gas adsorption analysis reveals a rare adsorption selectivity hierarchy of CO2 > C2H2 > C2H4, contrasting sharply with the analogue ZNU-14’s conventional selectivity pattern (C2H2 > C2H4 > CO2). In-situ gas-loaded single-crystal X-ray diffraction (SCXRD) combined with density functional theory (DFT) calculations elucidates the higher CO2 binding affinity. CO2 is tightly trapped in the contracted channel pores with multiple interactions, while C2H2 is located at the large cage cavity with weaker interactions. Various breakthrough experiments validate ZNU-13’s exceptional reverse C2H2/CO2 separation performance, exhibiting a dynamic separation factor of 3–5 and maintaining capacity under humid conditions for multiple cycles. Moreover, ZNU-13 enables direct production of polymer-grade C2H4 from equimolar ternary gas mixtures through a single adsorption process, establishing a new benchmark for integrated gas purification systems.