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Metal–Organic Framework Based Hydrogen-Bonding Nanotrap for Efficient Acetylene Storage and Separation
Open accessAbstract
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 tradeoff 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 a 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 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 an ultrahigh 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 those for the other two isostructural MOFs (86 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 (Δ q break = 5.02 mol/kg) and C 2 H 2 productivity (6.8 mol/kg). In addition, in situ FT-IR experiments and computational modeling further reveal that the unique host–guest multiple hydrogen-bonding interaction between the nanotrap and C 2 H 2 is the key factor for achieving the extraordinary acetylene storage capacity and superior C 2 H 2 /CO 2 selectivity. This work provides a novel and powerful approach to address the tradeoff of this extremely challenging gas separation.
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Metadata
- Authors
- Ye, Y., Xian, S., Cui, H., Tan, K., Gong, L., Liang, B., Pham, T., Pandey, H., Krishna, R., Lan, P. C., Forrest, K. A., Space, B., Thonhauser, T., Li, J., & Ma, S.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2021-12-29
- Volume
- 144
- Issue
- 4
- Pages
- 1681-1689
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W4200219264
- Cited by
- 359
- References
- 77
- FWCI
- 18.43
- Type
- journal article
- Language
- en
- Open access
- green
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