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Harnessing the Hybridization of a Metal-Organic Framework and Superbase-Derived Ionic Liquid for High-Performance Direct Air Capture of CO2

Journal Article · · Small
 [1];  [2];  [1];  [3];  [4];  [5];  [6];  [3];  [3];  [5];  [7];  [8];  [9];  [9];  [9];  [9];  [10]
  1. Univ. of Tennessee, Knoxville, TN (United States)
  2. Xiamen Univ. (China)
  3. Vanderbilt Univ., Nashville, TN (United States)
  4. Univ. of California, Riverside, CA (United States)
  5. Washington State Univ., Pullman, WA (United States)
  6. Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
  7. Washington State Univ., Pullman, WA (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
  8. University of Wisconsin, Stevens Point, WI (United States)
  9. Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
  10. Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division

Direct air capture (DAC) of CO2 has emerged as the most promising “negative carbon emission” technologies. Despite being state-of-the-art, sorbents deploying alkali hydroxides/amine solutions or amine-modified materials still suffer from unsolved high energy consumption and stability issues. Here, in this work, composite sorbents are crafted by hybridizing a robust metal-organic framework (Ni-MOF) with superbase-derived ionic liquid (SIL), possessing well maintained crystallinity and chemical structures. The low-pressure (0.4 mbar) volumetric CO2 capture assessment and a fixed-bed breakthrough examination with 400 ppm CO2 gas flow reveal high-performance DAC of CO2 (CO2 uptake capacity of up to 0.58 mmol g-1 at 298 K) and exceptional cycling stability. Operando spectroscopy analysis reveals the rapid (400 ppm) CO2 capture kinetics and energy-efficient/fast CO2 releasing behaviors. The theoretical calculation and small-angle X-ray scattering demonstrate that the confinement effect of the MOF cavity enhances the interaction strength of reactive sites in SIL with CO2, indicating great efficacy of the hybridization. The achievements in this study showcase the exceptional capabilities of SIL-derived sorbents in carbon capture from ambient air in terms of rapid carbon capture kinetics, facile CO2 releasing, and good cycling performance.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1993672
Alternate ID(s):
OSTI ID: 2217526
OSTI ID: 1985194
Journal Information:
Small, Journal Name: Small Journal Issue: 41 Vol. 19; ISSN 1613-6810
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

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