Heymans, N., Bourrelly, S., Normand, P., Bloch, E., Mkhadder, H., Cooper, L., Gorman, M., Bouzidi, I., Guillou, N., De Weireld, G. & Devic, T. (2020) Small-Pore Gallates MOFs for Environmental Applications: Sorption Behaviors and Structural Elucidation of Their High Affinity for CO2. J. Phys. Chem. C, 124 3188–3195.
Added by: Richard Baschera (2020-02-28 09:15:43) Last edited by: Richard Baschera (2020-02-28 09:18:10)
|Type de référence: Article
Numéro d'identification (ISBN etc.): 1932-7447
Clé BibTeX: Heymans2020
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|Catégories: INTERNATIONAL, ST2E
Mots-clés: 3, 4, 5-trihydroxybenzoate, adsorption, binding, building unit, capture, carbon-dioxide separation, metal-organic frameworks, performance, Porous materials, thermodynamics
Créateurs: Bloch, Bourrelly, Bouzidi, Cooper, De Weireld, Devic, Gorman, Guillou, Heymans, Mkhadder, Normand
Collection: J. Phys. Chem. C
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The ability of two structurally related small-pore metal-organic frameworks (MOFs) to capture CO2 was investigated by a combination of gas sorption measurements, X-ray powder diffraction (XRPD) analysis, microcalorimetry experiments, and ideal adsorbed solution theory (LAST) calculations. The title solids, formulated Mg(H(2)gal) and Fe(Hgal) (H(4)gal = gallic acid), are made of a naturally occurring ligand and were both prepared on the multigram scale under mild conditions. They both present very similar structures, with identical channels of ca 3.5 angstrom diameter, but present different amounts of acidic protons on the surface of the pores. These compounds were found to be extremely hydrophilic and exhibit moderate stability toward the water. While their ability to adsorb CH4 and N-2 is very limited, they both adsorb significant amounts of CO2 even at atmospheric pressure (3 and 5 mmol g(-1) at 303 K for the Fe and Mg derivatives, respectively). As a consequence, these compounds present high CO2/N-2 and CO2/CH4 selectivities (380-910 and 190-460, respectively) together with good working capacities, making them of interest for the capture of CO2 from flue gas or for landfill gas upgrading in pressure swing adsorption or vacuum swing adsorption processes. Finally, the analysis of the Mg derivative by X-ray diffraction (XRD) and adsorption microcalorimetry revealed that its high affinity for CO2 relies on a strong and specific site of adsorption involving double hydrogen bonds between the CO2 molecules and the acidic protons of the framework.