Revisiting the Aluminum Trimesate-based MOF (MIL-96): from Structure Determination to the Processing of Mixed Matrix Membranes for CO2 Capture.

Marvin Benzaqui, Renjith S. Pillai, Anahid Sabetghadam, Virginie Benoit, Périne Normand, Jerome Marrot, Nicolas Menguy, David Montero, William Shepard, Antoine Tissot, Charlotte Martineau-Corcos, Clémence Sicard, Mihail Mihaylov, Florent Carn, Isabelle Beurroeis, Philip L. Llewellyn, Guy De Weireld, Konstantin Hadjiivanov, Jorge Gascon, Freek KapteijnGuillaume Maurin, Nathalie Steunou, Christian Serre

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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/N-2 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/N-2 coadsorption experiments, calorimetry, and molecular simulations revealed that MIL-96-(Al) nanoparticles show a relatively high CO2 affinity over N-2 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/N-2 separation.
Original languageEnglish (US)
Pages (from-to)10326-10338
Number of pages13
JournalChemistry of Materials
Volume29
Issue number24
DOIs
StatePublished - Dec 4 2017

ASJC Scopus subject areas

  • Materials Chemistry
  • Chemical Engineering(all)
  • Chemistry(all)

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  • CCDC 1558833: Experimental Crystal Structure Determination : catena-[hexakis(mu-benzene-1,3,5-tricarboxylato)-dodecakis(mu-hydroxo)-(mu-oxo)-pentaaqua-tetrakis(hydroxy)-dodeca-aluminium hydrate]

    Benzaqui, M. (Creator), S. Pillai, R. (Creator), Sabetghadam, A. (Creator), Benoit, V. (Creator), Normand, P. (Creator), Marrot, J. (Creator), Menguy, N. (Creator), Montero, D. (Creator), Shepard, W. (Creator), Tissot, A. (Creator), Martineau-Corcos, C. (Creator), Sicard, C. (Creator), Mihaylov, M. (Creator), Carn, F. (Creator), Beurroeis, I. (Creator), Llewellyn, P. L. (Creator), De Weireld, G. (Creator), Hadjiivanov, K. (Creator), Gascon, J. (Creator), Kapteijn, F. (Creator), Maurin, G. (Creator), Steunou, N. (Creator), Serre, C. (Creator), Benzaqui, M. (Creator), S. Pillai, R. (Creator), Sabetghadam, A. (Creator), Benoit, V. (Creator), Normand, P. (Creator), Marrot, J. (Creator), Menguy, N. (Creator), Montero, D. (Creator), Shepard, W. (Creator), Tissot, A. (Creator), Martineau-Corcos, C. (Creator), Sicard, C. (Creator), Mihaylov, M. (Creator), Carn, F. (Creator), Beurroeis, I. (Creator), Llewellyn, P. L. (Creator), De Weireld, G. (Creator), Hadjiivanov, K. (Creator), Kapteijn, F. (Creator), Maurin, G. (Creator), Steunou, N. (Creator) & Serre, C. (Creator), Cambridge Crystallographic Data Centre, 2018

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