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ACS Appl Mater Interfaces ; 11(26): 23192-23197, 2019 Jul 03.
Artigo em Inglês | MEDLINE | ID: mdl-31184107


Inspired by the structure of carbonic anhydrase, we developed a robust ultramicroporous lanthanide metal-organic framework (MOF) platform (NKMOF-3-Ln), which possesses a porous pocket to selectively bind with CO2 at ambient conditions. Notably, CO2 molecules can be precisely observed in the single-crystal structure of NKMOF-3-Ln. Highly ordered CO2 molecules can strongly interact with the framework via electrostatic interaction of nitrates. We found that the CO2 adsorption capacity and binding energy were gradually enhanced as lanthanide contraction. The strong CO2 binding affinity endows NKMOF-3-Ln with excellent CO2 separation performance, which is verified by experimental breakthrough results. Moreover, because of the specific binding affinity of CO2, NKMOF-3-Eu showed a fluorescence response to CO2.

Angew Chem Int Ed Engl ; 58(30): 10209-10214, 2019 Jul 22.
Artigo em Inglês | MEDLINE | ID: mdl-31059186


Simultaneous removal of trace amounts of propyne and propadiene from propylene is an important but challenging industrial process. We report herein a class of microporous metal-organic frameworks (NKMOF-1-M) with exceptional water stability and remarkably high uptakes for both propyne and propadiene at low pressures. NKMOF-1-M separated a ternary propyne/propadiene/propylene (0.5 : 0.5 : 99.0) mixture with the highest reported selectivity for the production of polymer-grade propylene (99.996 %) at ambient temperature, as attributed to its strong binding affinity for propyne and propadiene over propylene. Moreover, we were able to visualize propyne and propadiene molecules in the single-crystal structure of NKMOF-1-M through a convenient approach under ambient conditions, which helped to precisely understand the binding sites and affinity for propyne and propadiene. These results provide important guidance on using ultramicroporous MOFs as physisorbent materials.