TY - JOUR
T1 - Revisiting the Aluminum Trimesate-Based MOF (MIL-96)
T2 - From Structure Determination to the Processing of Mixed Matrix Membranes for CO2 Capture
AU - Benzaqui, Marvin
AU - Pillai, Renjith S.
AU - Sabetghadam Esfahani, A.
AU - Benoit, Virginie
AU - Normand, Perine
AU - Marrot, Jérôme
AU - Menguy, Nicolas
AU - Montero, David
AU - Shepard, William
AU - Tissot, Antoine
AU - Martineau-Corcos, Charlotte
AU - Sicard, Clémence
AU - Mihaylov, Mihail
AU - Carn, Florent
AU - Beurroies, Isabelle
AU - Llewellyn, Philip L.
AU - De Weireld, Guy
AU - Hadjiivanov, Konstantin
AU - Gascon, Jorge
AU - Kapteijn, Freek
AU - Maurin, Guillaume
AU - Steunou, Nathalie
AU - Serre, Christian
PY - 2017/12/26
Y1 - 2017/12/26
N2 - 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.
AB - 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.
UR - http://resolver.tudelft.nl/uuid:643d07bf-475a-43bc-b325-9b76ff9fd65c
UR - http://www.scopus.com/inward/record.url?scp=85040087174&partnerID=8YFLogxK
U2 - 10.1021/acs.chemmater.7b03203
DO - 10.1021/acs.chemmater.7b03203
M3 - Article
AN - SCOPUS:85040087174
SN - 0897-4756
VL - 29
SP - 10326
EP - 10338
JO - Chemistry of Materials
JF - Chemistry of Materials
IS - 24
ER -