Fluorido-bridged robust metal–organic frameworks for efficient C2H2/CO2 separation under moist conditions†
ab
Cai-Lin
Chen,
d
Sheng-Sheng
Zhao,
a
Tian-Jun
Sun,
a
Yu
Han,
d
Xiao-Wei
Liu,
*d
Zhiping
Lai
*d
and
Shu-Dong
Wang
*a
Abstract
The modern technology for acetylene production is inevitably accompanied by the contamination of carbon dioxide and moisture impurities. Metal–organic frameworks (MOFs), with rational configurations of fluorine as the hydrogen-bonding acceptor (HBA), exhibit excellent affinities to capture acetylene from the gas mixtures. Currently, most research studies feature anionic fluorine groups as structural pillars (e.g., SiF62−, TiF62−, NbOF52−), whereas in situ insertion of fluorine into metal clusters is rather challenging. Herein, we report a unique fluorine-bridged Fe-MOF, i.e., DNL-9(Fe), which is assembled by mixed-valence FeIIFeIII clusters and renewable organic ligands. The fluorine species in the coordination-saturated structure offer superior C2H2-favored adsorption sites facilitated by hydrogen bonding, with a lower C2H2 adsorption enthalpy than other reported HBA-MOFs, demonstrated by static/dynamic adsorption tests and theoretical calculations. Importantly, DNL-9(Fe) shows exceptional hydrochemical stability under aqueous, acidic, and basic conditions, and its intriguing performance for C2H2/CO2 separation was even maintained at a high relative humidity of 90%.
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