Revisiting the Aluminum Trimesate-Based MOF (MIL-96)
From Structure Determination to the Processing of Mixed Matrix Membranes for CO2 Capture
Marvin Benzaqui (ENS-PSL Research University & CNRS, Institut Lavoisier de Versailles)
Renjith S. Pillai (Institut Charles Gerhardt Montpellier)
A. Sabetghadam Esfahani (TU Delft - Applied Sciences)
Virginie Benoit (Aix Marseille Université)
Perine Normand (Université de Mons)
Jérôme Marrot (Institut Lavoisier de Versailles)
Nicolas Menguy (Universite Pierre et Marie Curie (UPMC))
David Montero (Universite Pierre et Marie Curie (UPMC))
William Shepard (L'Orme les Merisiers Saint-Aubin)
Antoine Tissot (ENS-PSL Research University & CNRS, Institut Lavoisier de Versailles)
Charlotte Martineau-Corcos (Université d'Orléans, Institut Lavoisier de Versailles)
Clémence Sicard (Institut Lavoisier de Versailles)
Mihail Mihaylov (Bulgarian Academy of Sciences)
Florent Carn (Universite Paris Diderot)
Isabelle Beurroies (Aix Marseille Université)
Philip L. Llewellyn (Aix Marseille Université)
Guy De Weireld (Université de Mons)
Konstantin Hadjiivanov (Bulgarian Academy of Sciences)
Jorge Gascon (King Abdullah University of Science and Technology, TU Delft - Applied Sciences)
Freek Kapteijn (TU Delft - Applied Sciences)
Guillaume Maurin (Institut Charles Gerhardt Montpellier)
Nathalie Steunou (Institut Lavoisier de Versailles)
Christian Serre (ENS-PSL Research University & CNRS, Institut Lavoisier de Versailles)
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Abstract
A microporous Al trimesate-based metal-organic framework (MOF), denoted MIL-96-(Al), was selected as a porous hybrid filler for the processing of mixed matrix membranes (MMMs) for CO2/N2 postcombustion separation. First, the structural model of MIL-96-(Al) initially reported was revisited using a combination of synchrotron-based single-crystal X-ray diffraction, solid-state nuclear magnetic resonance spectroscopy, and density functional theory (DFT) calculations. In a second step, pure MIL-96-(Al) crystals differing by their size and aspect ratio, including anisotropic hexagonal platelets and nanoparticles of about 70 nm in diameter, were prepared. Then, a combination of in situ IR spectroscopy, single-gas, and CO2/N2 coadsorption experiments, calorimetry, and molecular simulations revealed that MIL-96-(Al) nanoparticles show a relatively high CO2 affinity over N2 owing to strong interactions between CO2 molecules and several adsorption sites such as Al3+ Lewis centers, coordinated water, and hydroxyl groups. Finally, the high compatibility between MIL-96-(Al) nanoparticles and the 6FDA-DAM polymer allowed the processing of homogeneous and defect-free MMMs with a high MOF loading (up to 25 wt %) that outperform pure polymer membranes for CO2/N2 separation.