Author(s) Jaramillo, D.E.; Reed, D.A.; Jiang, H.Z.H.; Oktawiec, J.; Mara, M.W.; Forse, A.C.; Lussier, D.J.; Murphy, R.A.; Cunningham, M.; Colombo, V.; Shuh, D.K.; Reimer, J.A.; Long, J.R.
Journal Nat Mater
Date Published 2020 Feb 03

Industrial processes prominently feature π-acidic gases, and an adsorbent capable of selectively interacting with these molecules could enable important chemical separations. Biological systems use accessible, reducing metal centres to bind and activate weakly π-acidic species, such as N, through backbonding interactions, and incorporating analogous moieties into a porous material should give rise to a similar adsorption mechanism for these gaseous substrates. 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 N capacities and selectivities for the removal of N from mixtures with CH, 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.

DOI 10.1038/s41563-019-0597-8
ISSN 1476-1122
Citation Nat Mater. 2020.

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