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<p>The maturation of industrial methanol-to-olefins (MTO) technology intensifies the demand for highly-efficient separation of ethylene/propylene (C<sub>2</sub>H<sub>4</sub>/C<sub>3</sub>H<sub>6</sub>) mixture products. Addressing this challenge, a ligand-symmetry-guide molecular cage isomerism strategy is proposed and verified herein. The symmetry transition from C<sub>1</sub> to C<sub>2<i>v</i></sub> triggered by C/N exchange in organic linkers generated structure-related SNNU-5/5A materials containing two octahedral cage isomers ({[Fe<sub>3</sub>O]<sub>6</sub>L<sub>12</sub>}, defined as o-cage-α/β. Notably, the “isomer” in this paper specifically refer to the geometric spatial isomerism of metal-organic cages) and three tetradecahedral cage isomers ({[Fe<sub>3</sub>O]<sub>12</sub>L<sub>12</sub>}, defined as t-cage-α/β/γ). The structural modularity of two types of cage isomers with confined windows (≈6 Å) coupled with capacious cavities (&gt;12 Å) synergistically surmounts the persistent capacity-selectivity trade-off for C<sub>2</sub>H<sub>4</sub>/C<sub>3</sub>H<sub>6</sub> separation. Specially, SNNU-5A with three different cages exhibit ultra-high C<sub>3</sub>H<sub>6</sub> uptake capacities of 270.1 cm<sup>3</sup> g<sup>−1</sup> under ambient conditions along with separation productivity of 114 L kg<sup>−1</sup> for C<sub>2</sub>H<sub>4</sub> (purity &gt; 99.9%) and 107 L kg<sup>−1</sup> for C<sub>3</sub>H<sub>6</sub> (purity &gt; 99%), ranking second among all adsorbents for MTO products separation. This study offers a new perspective on cage engineering within MOFs and provides valuable guidance for designing practical adsorbents that overcome the trade-off barrier between adsorption capacity and separation efficiency.</p>

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Symmetry-induced cage isomerism in MOFs enables benchmark propylene storage and efficient propylene/ethylene separation

  • 期刊论文

  • 发表日期：

    2026年4月13日

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  • Yan-Ying Liu,
  • Fei Yuan,
  • Zhang-Lei Zhong,
  • Chen-Chen Xing,
  • Jia-Wen Wang,
  • Wen-Yu Yuan,
  • Ying Wang,
  • Quan-Guo Zhai

摘要

The maturation of industrial methanol-to-olefins (MTO) technology intensifies the demand for highly-efficient separation of ethylene/propylene (C2H4/C3H6) mixture products. Addressing this challenge, a ligand-symmetry-guide molecular cage isomerism strategy is proposed and verified herein. The symmetry transition from C1 to C2v triggered by C/N exchange in organic linkers generated structure-related SNNU-5/5A materials containing two octahedral cage isomers ({[Fe3O]6L12}, defined as o-cage-α/β. Notably, the “isomer” in this paper specifically refer to the geometric spatial isomerism of metal-organic cages) and three tetradecahedral cage isomers ({[Fe3O]12L12}, defined as t-cage-α/β/γ). The structural modularity of two types of cage isomers with confined windows (≈6 Å) coupled with capacious cavities (>12 Å) synergistically surmounts the persistent capacity-selectivity trade-off for C2H4/C3H6 separation. Specially, SNNU-5A with three different cages exhibit ultra-high C3H6 uptake capacities of 270.1 cm3 g−1 under ambient conditions along with separation productivity of 114 L kg−1 for C2H4 (purity > 99.9%) and 107 L kg−1 for C3H6 (purity > 99%), ranking second among all adsorbents for MTO products separation. This study offers a new perspective on cage engineering within MOFs and provides valuable guidance for designing practical adsorbents that overcome the trade-off barrier between adsorption capacity and separation efficiency.