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<p>One-step removal of multiple impurities implemented by adsorptive separation is an efficient and simple process to afford high purity products, but is hindered by the lack of advanced porous materials that could capture different types of molecules. Herein, a series of novel metal-organic frameworks ZU-921 to ZU-924 with cooperative binding environment of integrated aromaticity surface and fluorine/oxygen electronegative sites are designed, and ZU-921 is presented as the demonstration that solves the long-standing challenge in one-step propylene (C<sub>3</sub>H<sub>6</sub>) purification from the C3 quaternary mixture. The selective recognition ability towards alkyne, allene, alkane than alkene implemented by ZU-921 is attributed to the optimal interaction contribution from polarizability and dipole/quadruple moments that is realized by the fine-tuned density of parallelly-distributed electronegative sites via ligand engineering strategy. Ultra-high purity (99.99%) C<sub>3</sub>H<sub>6</sub> could be directly obtained from the C3 quaternary mixture (C<sub>3</sub>H<sub>4</sub>/C<sub>3</sub>H<sub>4</sub>(PD)/C<sub>3</sub>H<sub>8</sub>/C<sub>3</sub>H<sub>6</sub> 1 v/1 v/3 v/95 v) with the productivity of 17.27 L/kg derived from the 10-times scale-up column (1.0 cm × 50 cm) breakthrough experiment. This work not only presents a common strategy in advanced adsorbents design for multiple impurities capture but also provides an energy-efficient alternative for C<sub>3</sub>H<sub>6</sub> purification.</p>

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One-step propylene purification from a quaternary mixture by a single physisorbent

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年12月13日

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  • Peixin Zhang,
  • Zhensong Qiu,
  • Yechen Liu,
  • Sen Chen,
  • Lifeng Yang,
  • Xian Suo,
  • Xili Cui,
  • Huabin Xing

摘要

One-step removal of multiple impurities implemented by adsorptive separation is an efficient and simple process to afford high purity products, but is hindered by the lack of advanced porous materials that could capture different types of molecules. Herein, a series of novel metal-organic frameworks ZU-921 to ZU-924 with cooperative binding environment of integrated aromaticity surface and fluorine/oxygen electronegative sites are designed, and ZU-921 is presented as the demonstration that solves the long-standing challenge in one-step propylene (C3H6) purification from the C3 quaternary mixture. The selective recognition ability towards alkyne, allene, alkane than alkene implemented by ZU-921 is attributed to the optimal interaction contribution from polarizability and dipole/quadruple moments that is realized by the fine-tuned density of parallelly-distributed electronegative sites via ligand engineering strategy. Ultra-high purity (99.99%) C3H6 could be directly obtained from the C3 quaternary mixture (C3H4/C3H4(PD)/C3H8/C3H6 1 v/1 v/3 v/95 v) with the productivity of 17.27 L/kg derived from the 10-times scale-up column (1.0 cm × 50 cm) breakthrough experiment. This work not only presents a common strategy in advanced adsorbents design for multiple impurities capture but also provides an energy-efficient alternative for C3H6 purification.