Title: Cold Temperature Direct Air CO ₂ Capture with Amine-Loaded Metal–Organic Framework Monoliths

Abstract

Zeolites, silica-supported amines, and metal– organic frameworks (MOFs) have been demonstrated as promising adsorbents for direct air CO₂ capture (DAC), but the shaping and structuring of these materials into sorbent modules for practical processes have been inadequately investigated compared to the extensive research on powder materials. Furthermore, there have been relatively few studies reporting the DAC performance of sorbent contactors under cold, subambient conditions (temperatures below 20 °C). In this work, we demonstrate the successful fabrication of adsorbent monoliths composed of cellulose acetate (CA) and adsorbent particles such as zeolite 13X and MOF MIL- 101(Cr) by a 3D printing technique: solution-based additive manufacturing (SBAM). These monoliths feature interpenetrated macroporous polymeric frameworks in which microcrystals of zeolite 13X or MIL-101(Cr) are evenly distributed, highlighting the versatility of SBAM in fabricating monoliths containing sorbents with different particle sizes and density. Branched poly(ethylenimine) (PEI) is successfully loaded into the CA/MIL-101(Cr) monoliths to impart CO₂ uptakes of 1.05 mmol g_monolith ^–1 at –20 °C and 400 ppm of CO₂. Kinetic analysis shows that the CO₂ sorption kinetics of PEI-loaded MIL-101(Cr) sorbents are not compromised in the monoliths compared to the powder sorbents. Importantly, these monoliths exhibit promising working capacities (0.95 mmol g_monolith ^–1) overmore » 14 temperature swing cycles with a moderate regeneration temperature of 60 °C. Dynamic breakthrough experiments at 25 °C under dry conditions reveal a CO₂ uptake capacity of 0.60 mmol g_monolith ^–1, which further increases to 1.05 and 1.43 mmol g_monolith ^–1 at –20 °C under dry and humid (70% relative humidity) conditions, respectively. Our work showcases the successful implementation of SBAM in making DAC sorbent monoliths with notable CO₂ capture performance over a wide range of sorption temperatures, suggesting that SBAM can enable the preparation of efficient sorbent contactors in various form factors for other important chemical separations« less

Authors:

Wang, Yuxiang  ^[1];

• Search DOE PAGES for author "Wang, Yuxiang"
• Search DOE PAGES for ORCID "0000-0002-6945-6431"

Rim, Guanhe  ^[1];

• Search DOE PAGES for author "Rim, Guanhe"
• Search DOE PAGES for ORCID "0000-0001-8244-8308"

Song, MinGyu ^[1]; Holmes, Hannah E.  ^[1];

• Search DOE PAGES for author "Holmes, Hannah E."
• Search DOE PAGES for ORCID "0000-0002-3199-1711"

Jones, Christopher W.  ^[1];

• Search DOE PAGES for author "Jones, Christopher W."
• Search DOE PAGES for ORCID "0000-0003-3255-5791"

Lively, Ryan P.  ^[1]

• Search DOE PAGES for author "Lively, Ryan P."
• Search DOE PAGES for ORCID "0000-0002-8039-4008"

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1. School of Chemical & Biomolecular Engineering, Georgia Institute of Technology, 311 Ferst Dr., Atlanta, Georgia 30332, United States

Publication Date:

Mon Dec 18 00:00:00 EST 2023

Research Org.:

Georgia Institute of Technology, Atlanta, GA (United States)

Sponsoring Org.:

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

OSTI Identifier:

2242550

Alternate Identifier(s):

OSTI ID: 2280770

Grant/Contract Number:  

FE-FE0031952; FE0031952

Resource Type:

Published Article

Journal Name:

ACS Applied Materials and Interfaces

Additional Journal Information:

Journal Name: ACS Applied Materials and Interfaces Journal Volume: 16 Journal Issue: 1; Journal ID: ISSN 1944-8244

Publisher:

American Chemical Society

Country of Publication:

United States

Language:

English

Subject:

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 3D printing; carbon capture; direct air capture; metal−organic frameworks; subambient conditions; adsorption; catalysts supports; polyethylenimine; sorbents