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DOE OSTI · 1863378

Metal–Organic Framework Based Hydrogen-Bonding Nanotrap for Efficient Acetylene Storage and Separation

Ye, Yingxiang·Xian, Shikai·Cui, Hui·Tan, Kui·Gong, Lingshan·Liang, Bin·Pham, Tony·Pandey, Haardik·Krishna, Rajamani·Lan, Pui Ching·Forrest, Katherine A.·Space, Brian·Thonhauser, Timo·Li, Jing·Ma, Shengqian
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Abstract

The removal of carbon dioxide (CO 2 ) from acetylene (C 2 H 2 ) is a critical industrial process for manufacturing high purity C 2 H 2 . However, it remains challenging to address the trade-off between adsorption capacity and selectivity, on account of their similar physical properties and molecular sizes. To overcome this difficulty, here we report a novel strategy involving the regulation of hydrogen-bonding nanotrap on the pore surface to promote the separation of C 2 H 2 /CO 2 mixtures, in three isostructural metal-organic frameworks (MOFs, named as MIL-160, CAU-10H, and CAU-23, respectively). Among them, MIL-160, which has abundant hydrogen-bonding acceptors as nanotraps, can selectively capture acetylene molecules and demonstrates ultra-high C 2 H 2 storage capacity (191 cm 3 g –1 , or 213 cm 3 cm –3 ) but much less CO 2 uptake (90 cm 3 g –1 ) under ambient conditions. The C 2 H 2 adsorption amount of MIL-160 is remarkably higher than the other two isostructural MOFs (86 cm 3 g –1 and 119 cm 3 g –1 for CAU-10H and CAU-23 respectively) under the same conditions. More importantly, both simulation and experimental breakthrough results show that MIL-160 sets a new benchmark for equimolar C 2 H 2 /CO 2 separation in terms of the separation potential (Δq break = 5.02 mol/kg) and C 2 H 2 productivity (6.8 mol/kg). In addition, in-situ FT-IR experiments combined with computational modeling further reveal that the unique host-guest multiple hydrogen-bonding interactions between the nanotrap and C 2 H 2 is the key factor for achieving extraordinary acetylene storage capacity and superior C 2 H 2 /CO 2 selectivity. Furthermore, this work provides a novel and powerful approach to address the trade-off of this extremely challenging gas separation.

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRYAdsorptionHydrocarbonsMetal organic frameworksMixturesMolecules

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Ye, Yingxiang, Xian, Shikai, Cui, Hui, Tan, Kui, Gong, Lingshan, Liang, Bin, Pham, Tony, Pandey, Haardik, Krishna, Rajamani, Lan, Pui Ching, Forrest, Katherine A., Space, Brian, Thonhauser, Timo, Li, Jing, Ma, Shengqian. 2021-12-29. Metal–Organic Framework Based Hydrogen-Bonding Nanotrap for Efficient Acetylene Storage and Separation. https://doi.org/10.1021/jacs.1c10620

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