High-Performance CO2 Capture from Air by Harnessing the Power of CaO- and Superbase-Ionic-Liquid-Engineered Sorbents

Moitra, Debabrata; Mokhtari‐Nori, Narges; Siniard, Kevin M.; Qiu, Liqi; Fan, Juntian; Dong, Zhun; Hu, Wenda; Liu, Hongjun; Jiang, De‐en; Lin, Hongfei; Hu, Jianzhi; Li, Meijia; Yang, Zhenzhen; Dai, Sheng

doi:10.1002/cssc.202300808

High-Performance CO₂ Capture from Air by Harnessing the Power of CaO- and Superbase-Ionic-Liquid-Engineered Sorbents

Journal Article · Mon Jun 19 04:00:00 EDT 2023 · ChemSusChem

DOI:https://doi.org/10.1002/cssc.202300808· OSTI ID:1993676

Moitra, Debabrata ^[1]; Mokhtari‐Nori, Narges ^[1]; Siniard, Kevin M. ^[1]; Qiu, Liqi ^[1]; Fan, Juntian ^[1]; Dong, Zhun ^[2]; Hu, Wenda ^[3]; Liu, Hongjun ^[4]; Jiang, De‐en ^[4]; ^[2]; ^[5]; ^[6]; ^[6]; ^[7]

Univ. of Tennessee, Knoxville, TN (United States)
Washington State Univ., Pullman, WA (United States)
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Vanderbilt Univ., Nashville, TN (United States)
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Washington State Univ., Pullman, WA (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
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 by solid porous materials represents an attractive “negative emission” technology. However, state-of-the-art sorbents based on supported amines still suffer from unsolved high energy consumption and stability issues. For this work, taking clues from the CO₂ interaction with superbase-derived ionic liquids (SILs), high-performance and tunable sorbents in DAC of CO₂ was developed by harnessing the power of CaO- and SIL-engineered sorbents. Deploying mesoporous silica as the substrate, a thin CaO layer was first introduced to consume the surface-OH groups, and then active sites with different basicities (e. g., triazolate and imidazolate) were introduced as a uniformly distributed thin layer. The as-obtained sorbents displayed high CO₂ uptake capacity via volumetric (at 0.4 mbar) and breakthrough test (400 ppm CO₂ source), rapid interaction kinetics, facile CO₂ releasing, and stable sorption/desorption cycles. Operando diffuse reflectance infrared Fourier transformation spectroscopy (DRIFTS) analysis under simulated air atmosphere and solid-state NMR under ¹³CO₂ atmosphere demonstrated the critical roles of the SIL species in low-concentration CO₂ capture. The fundamental insights obtained in this work provide guidance on the development of high-performance sorbents in DAC of CO₂ by leveraging the combined advantages of porous solid scaffolds and the unique features of CO₂-philic ionic liquids.

View Accepted Manuscript (DOE)

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; SC0022273

OSTI ID:: 1993676

Alternate ID(s):: OSTI ID: 2439835
OSTI ID: 2248008

Journal Information:: ChemSusChem, Journal Name: ChemSusChem Journal Issue: 20 Vol. 16; ISSN 1864-5631

Publisher:: ChemPubSoc EuropeCopyright Statement

Country of Publication:: United States

Language:: English

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