Research Articles (Chemistry and Polymer Science)

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Breaking the trade-off between selectivity and adsorption capacity for gas separation
(Elsevier Inc., 2021-11) Soumya, Naveen Kumar; Mukherjee, Nathan C.; Bezrukov, Andrey A.; Tan, Kui; Martins, Vinicius; Vandichel, Matthias; Pham, Tony; Van Wyk, Lisa M.; Oyekan, Kolade; Kumar, Amrit; Forrest, Katherine A.; Patil, Komal M.; Barbour, Leonard J.; Space, Brian; Huang, Yining; Kruger, Paul E.; Zaworotko, Michael J.
The trade-off between selectivity and adsorption capacity with porous materials is a major roadblock to reducing the energy footprint of gas separation technologies. To address this matter, we report herein a systematic crystal engineering study of C2H2 removal from CO2 in a family of hybrid ultramicroporous materials (HUMs). The HUMs are composed of the same organic linker ligand, 4-(3,5-dimethyl-1H-pyrazol-4-yl)pyridine, pypz, three inorganic pillar ligands, and two metal cations, thereby affording six isostructural pcu topology HUMs. All six HUMs exhibited strong binding sites for C2H2 and weaker affinity for CO2. The tuning of pore size and chemistry enabled by crystal engineering resulted in benchmark C2H2/CO2 separation performance. Fixed-bed dynamic column breakthrough experiments for an equimolar (v/v = 1:1) C2H2/CO2 binary gas mixture revealed that one sorbent, SIFSIX-21-Ni, was the first C2H2 selective sorbent that combines exceptional separation selectivity (27.7) with high adsorption capacity (4 mmol·g−1).