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<p>Ethylene (C<sub>2</sub>H<sub>4</sub>) and propylene (C<sub>3</sub>H<sub>6</sub>), key products of the methanol-to-olefins (MTO) process, are vital chemical feedstocks. However, separating and purifying C<sub>3</sub>H<sub>6</sub>/C<sub>2</sub>H<sub>4</sub> mixtures remains highly challenging due to their similar physicochemical properties. Through the mixed-ligand strategy with both N,N′-bis(3,5-dicarboxyphenyl)-oxalamide (H<sub>4</sub>BDPO) and either 4,4′-bipyridine (bpy) or di(pyridin-4-yl)amine (dpa), respectively, two novel amide-functionalized MOFs, [Cu<sub>6</sub>(BDPO)<sub>3</sub>(bpy)<sub>2</sub>(H<sub>2</sub>O)]·<i>x</i>solvent (NJTU-Bai85, NJTU-Bai = Nanjing Tech University Bai’s group) and [Cu<sub>6</sub>(BDPO)<sub>3</sub>(dpa)<sub>2</sub>(H<sub>2</sub>O)]·<i>x</i>solvent (NJTU-Bai86) were synthesized with high C<sub>3</sub>H<sub>6</sub> capacities (181 and 191 cm<sup>3</sup>&#xa0;g<sup>−1</sup> at 298&#xa0;K and 1&#xa0;bar, respectively) and exceptional C<sub>3</sub>H<sub>6</sub>/C<sub>2</sub>H<sub>4</sub> selectivity (9.5 and 9.2, respectively), even at elevated temperatures. Furthermore, dynamic breakthrough experiments demonstrate that C<sub>3</sub>H<sub>6</sub>/C<sub>2</sub>H<sub>4</sub> mixture (50/50, 20/50, and 10/90, <i>v</i>/<i>v</i>) can be effectively separated in one step and obtain polymer-grade C<sub>2</sub>H<sub>4</sub> (≥ 99.5%) with ultra-high productivity (137 and 133 L kg<sup>−1</sup>, respectively) at 298&#xa0;K and very interestingly, the MOF-packed separation column shows markedly distinct retention times for C<sub>2</sub>H<sub>4</sub> and C<sub>3</sub>H<sub>6</sub>, highlighting their potential for industrial gas separation application.</p> Graphical abstract <p></p>

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Efficient separation of methanol-to-olefins products with two novel amide-functionalized Cu-MOFs

  • 期刊论文

  • 发表日期：

    2025年11月19日

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  • Rui-Rui Xie,
  • Jun-Feng Bai

摘要

Ethylene (C2H4) and propylene (C3H6), key products of the methanol-to-olefins (MTO) process, are vital chemical feedstocks. However, separating and purifying C3H6/C2H4 mixtures remains highly challenging due to their similar physicochemical properties. Through the mixed-ligand strategy with both N,N′-bis(3,5-dicarboxyphenyl)-oxalamide (H4BDPO) and either 4,4′-bipyridine (bpy) or di(pyridin-4-yl)amine (dpa), respectively, two novel amide-functionalized MOFs, [Cu6(BDPO)3(bpy)2(H2O)]·xsolvent (NJTU-Bai85, NJTU-Bai = Nanjing Tech University Bai’s group) and [Cu6(BDPO)3(dpa)2(H2O)]·xsolvent (NJTU-Bai86) were synthesized with high C3H6 capacities (181 and 191 cm3 g−1 at 298 K and 1 bar, respectively) and exceptional C3H6/C2H4 selectivity (9.5 and 9.2, respectively), even at elevated temperatures. Furthermore, dynamic breakthrough experiments demonstrate that C3H6/C2H4 mixture (50/50, 20/50, and 10/90, v/v) can be effectively separated in one step and obtain polymer-grade C2H4 (≥ 99.5%) with ultra-high productivity (137 and 133 L kg−1, respectively) at 298 K and very interestingly, the MOF-packed separation column shows markedly distinct retention times for C2H4 and C3H6, highlighting their potential for industrial gas separation application.

Graphical abstract