@misc{10481/97480,
year = {2024},
month = {11},
url = {https://hdl.handle.net/10481/97480},
abstract = {Capturing carbon dioxide from diluted streams, such as flue gas originating from natural gas combustion, can be
achieved using recyclable, humidity-resistant porous materials. Three such materials were synthesized by chemically modifying the
pores of metal−organic frameworks (MOFs) with Lewis basic functional groups. These materials included aluminum 1,2,4,5-
tetrakis(4-carboxylatophenyl) benzene (Al-TCPB) and two novel MOFs: Al-TCPB(OH), and Al-TCPB(NH2), both isostructural to
Al-TCPB, and chemically and thermally stable. Single-component adsorption isotherms revealed significantly increased CO2 uptakes
upon pore functionalization. Breakthrough experiments using a 4/96 CO2/N2 gas mixture humidified up to 75% RH at 25 °C
showed that Al-TCPB(OH) displayed the highest CO2 dynamic breakthrough capacity (0.52 mmol/g) followed by that of Al-
TCPB(NH2) (0.47 mmol/g) and Al-TCPB (0.26 mmol/g). All three materials demonstrated excellent recyclability over eight
humid breakthrough-regeneration cycles. Solid-state nuclear magnetic resonance spectra revealed that upon CO2/H2O loading, H2O
molecules do not interfere with CO2 physisorption and are localized near the Al-O(H) chain and the −NH2 functional group,
whereas CO2 molecules are spatially confined in Al-TCPB(OH) and relatively mobile in Al-TCPB(NH2). Density functional theory
calculations confirmed the impact of the adsorbaphore site between of two parallel ligand-forming benzene rings for CO2 capture.
Our study elucidates how pore functionalization influences the fundamental adsorption properties of MOFs, underscoring their
practical potential as porous sorbent materials.},
organization = {College of Science for the Industrial Partnership Award},
organization = {Saudi Aramco},
publisher = {ACS Publications},
keywords = {pore functionalization},
keywords = {CO2 capture},
keywords = {H2O isotherms},
title = {Enhanced Carbon Dioxide Capture from Diluted Streams with Functionalized Metal−Organic Frameworks},
doi = {10.1021/jacsau.4c00923},
author = {Gładysiak, Andrzej and Song, Ah-Young and Vismara, Rebecca and Waite, Madison and M. Alghoraibi, Nawal and H. Alahmed, Ammar and Younes, Mourad and Huang, Hongliang and A. Reimer, Jeffrey and C. Stylianou, Kyriakos},
}