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DOI

  • Marvin Benzaqui
  • Renjith S. Pillai
  • A. Sabetghadam Esfahani
  • Virginie Benoit
  • Perine Normand
  • Jérôme Marrot
  • Nicolas Menguy
  • David Montero
  • William Shepard
  • Antoine Tissot
  • Charlotte Martineau-Corcos
  • Clémence Sicard
  • Mihail Mihaylov
  • Florent Carn
  • Isabelle Beurroies
  • Philip L. Llewellyn
  • Guy De Weireld
  • Konstantin Hadjiivanov
  • Guillaume Maurin
  • Nathalie Steunou
  • Christian Serre

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.

Original languageEnglish
Pages (from-to)10326-10338
Number of pages13
JournalChemistry of Materials
Volume29
Issue number24
DOIs
Publication statusPublished - 26 Dec 2017

ID: 36834533