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

doi:10.1021/jacs.1c10620

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

Journal Article · Wed Dec 29 00:00:00 EST 2021 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.1c10620· OSTI ID:1863378

^[1]; Xian, Shikai ^[2]; ^[3]; ^[4]; Gong, Lingshan ^[5]; Liang, Bin ^[5]; ^[6]; Pandey, Haardik ^[7]; ^[8]; Lan, Pui Ching ^[5]; Forrest, Katherine A. ^[6]; Space, Brian ^[9]; ^[7]; ^[10]; ^[5]

Univ. of North Texas, Denton, TX (United States); Rutgers University
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 North Texas, Denton, 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)

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 (Δq_break = 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.

View Accepted Manuscript (DOE)

Research Organization:: Wake Forest Univ., Winston-Salem, NC (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0019902

OSTI ID:: 1863378

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 4 Vol. 144; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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