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. 2023 Apr 24;62(18):e202218854.
doi: 10.1002/anie.202218854. Epub 2023 Mar 24.

Inverse CO2 /C2 H2 Separation with MFU-4 and Selectivity Reversal via Postsynthetic Ligand Exchange

Qiao Liu  1 , Sung Gu Cho  1 , Jordon Hilliard  1 , Ting-Yuan Wang  2 , Szu-Chia Chien  3 , Li-Chiang Lin  2 , Anne C Co  1 , Casey R Wade  1
Affiliations

Inverse CO2 /C2 H2 Separation with MFU-4 and Selectivity Reversal via Postsynthetic Ligand Exchange

Qiao Liu et al. Angew Chem Int Ed Engl. .

Abstract

Although many porous materials, including metal-organic frameworks (MOFs), have been reported to selectively adsorb C2 H2 in C2 H2 /CO2 separation processes, CO2 -selective sorbents are much less common. Here, we report the remarkable performance of MFU-4 (Zn5 Cl4 (bbta)3 , bbta=benzo-1,2,4,5-bistriazolate) toward inverse CO2 /C2 H2 separation. The MOF facilitates kinetic separation of CO2 from C2 H2 , enabling the generation of high purity C2 H2 (>98 %) with good productivity in dynamic breakthrough experiments. Adsorption kinetics measurements and computational studies show C2 H2 is excluded from MFU-4 by narrow pore windows formed by Zn-Cl groups. Postsynthetic F- /Cl- ligand exchange was used to synthesize an analogue (MFU-4-F) with expanded pore apertures, resulting in equilibrium C2 H2 /CO2 separation with reversed selectivity compared to MFU-4. MFU-4-F also exhibits a remarkably high C2 H2 adsorption capacity (6.7 mmol g-1 ), allowing fuel grade C2 H2 (98 % purity) to be harvested from C2 H2 /CO2 mixtures by room temperature desorption.

Keywords: Acetylene; CO2; Inverse Separation; Metal-Organic Frameworks; Molecular Sieving.

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