Metal–Organic Framework Based Hydrogen-Bonding Nanotrap for Efficient Acetylene Storage and Separation
Abstract
The removal of carbon dioxide (CO2) from acetylene (C2H2) is a critical industrial process for manufacturing high purity C2H2. 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 C2H2/CO2 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 C2H2 storage capacity (191 cm3 g–1, or 213 cm3 cm–3) but much less CO2 uptake (90 cm3 g–1) under ambient conditions. The C2H2 adsorption amount of MIL-160 is remarkably higher than the other two isostructural MOFs (86 cm3 g–1 and 119 cm3 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 C2H2/CO2 separation in terms of the separation potential (Δqbreak = 5.02 mol/kg) and C2H2 productivity (6.8 mol/kg). In addition, in-situ FT-IR experiments combined with computational modeling further reveal that the uniquemore »
- Authors:
-
[1];
[3];
[4];
[5];
[7];
[6];
[9];
[1]
- Univ. of North Texas, Denton, TX (United States)
- Rutgers Univ., Piscataway, NJ (United States); Shenzhen Polytechnic, Guangdong (China)
- Univ. of Texas, San Antonio, TX (United States)
- Univ. of Texas at Dallas, Richardson, TX (United States)
- Univ. of South Florida, Tampa, FL (United States)
- Wake Forest Univ., Winston-Salem, NC (United States)
- Univ. of Amsterdam (The Netherlands)
- North Carolina State Univ., Raleigh, NC (United States)
- Rutgers Univ., Piscataway, NJ (United States)
- Publication Date:
- Research Org.:
- Wake Forest Univ., Winston-Salem, NC (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1863378
- Grant/Contract Number:
- SC0019902
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 144; Journal Issue: 4; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Adsorption; Hydrocarbons; Metal organic frameworks; Mixtures; Molecules
Citation Formats
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, and Ma, Shengqian. Metal–Organic Framework Based Hydrogen-Bonding Nanotrap for Efficient Acetylene Storage and Separation. United States: N. p., 2021.
Web. doi:10.1021/jacs.1c10620.
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. Metal–Organic Framework Based Hydrogen-Bonding Nanotrap for Efficient Acetylene Storage and Separation. United States. https://doi.org/10.1021/jacs.1c10620
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, and Ma, Shengqian. Wed .
"Metal–Organic Framework Based Hydrogen-Bonding Nanotrap for Efficient Acetylene Storage and Separation". United States. https://doi.org/10.1021/jacs.1c10620. https://www.osti.gov/servlets/purl/1863378.
@article{osti_1863378,
title = {Metal–Organic Framework Based Hydrogen-Bonding Nanotrap for Efficient Acetylene Storage and Separation},
author = {Ye, Yingxiang and Xian, Shikai and Cui, Hui and Tan, Kui and Gong, Lingshan and Liang, Bin and Pham, Tony and Pandey, Haardik and Krishna, Rajamani and Lan, Pui Ching and Forrest, Katherine A. and Space, Brian and Thonhauser, Timo and Li, Jing and Ma, Shengqian},
abstractNote = {The removal of carbon dioxide (CO2) from acetylene (C2H2) is a critical industrial process for manufacturing high purity C2H2. 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 C2H2/CO2 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 C2H2 storage capacity (191 cm3 g–1, or 213 cm3 cm–3) but much less CO2 uptake (90 cm3 g–1) under ambient conditions. The C2H2 adsorption amount of MIL-160 is remarkably higher than the other two isostructural MOFs (86 cm3 g–1 and 119 cm3 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 C2H2/CO2 separation in terms of the separation potential (Δqbreak = 5.02 mol/kg) and C2H2 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 C2H2 is the key factor for achieving extraordinary acetylene storage capacity and superior C2H2/CO2 selectivity. Furthermore, this work provides a novel and powerful approach to address the trade-off of this extremely challenging gas separation.},
doi = {10.1021/jacs.1c10620},
journal = {Journal of the American Chemical Society},
number = 4,
volume = 144,
place = {United States},
year = {Wed Dec 29 00:00:00 EST 2021},
month = {Wed Dec 29 00:00:00 EST 2021}
}
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