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Selective nitrogen adsorption via backbonding in a metal-organic framework with exposed vanadium sites.

  • Jaramillo, David E
  • Reed, Douglas A
  • Jiang, Henry ZH
  • Oktawiec, Julia
  • Mara, Michael W
  • Forse, Alexander C
  • Lussier, Daniel J
  • Murphy, Ryan A
  • Cunningham, Marc
  • Colombo, Valentina
  • Shuh, David K
  • Reimer, Jeffrey A
  • Long, Jeffrey R
Publication Date
May 01, 2020
eScholarship - University of California
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Industrial processes prominently feature π-acidic gases, and an adsorbent capable of selectively interacting with these molecules could enable important chemical separations1-4. Biological systems use accessible, reducing metal centres to bind and activate weakly π-acidic species, such as N2, through backbonding interactions5-7, and incorporating analogous moieties into a porous material should give rise to a similar adsorption mechanism for these gaseous substrates8. Here, we report a metal-organic framework featuring exposed vanadium(II) centres capable of back-donating electron density to weak π acids to successfully target π acidity for separation applications. This adsorption mechanism, together with a high concentration of available adsorption sites, results in record N2 capacities and selectivities for the removal of N2 from mixtures with CH4, while further enabling olefin/paraffin separations at elevated temperatures. Ultimately, incorporating such π-basic metal centres into porous materials offers a handle for capturing and activating key molecular species within next-generation adsorbents.

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