Revisiting the Aluminum Trimesate-based MOF (MIL-96): from Structure Determination to the Processing of Mixed Matrix Membranes for CO2 Capture.
S. Pillai, Renjith
Llewellyn, Philip L.
De Weireld, Guy
KAUST DepartmentKAUST Catalysis Center (KCC)
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AbstractA 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.
CitationBenzaqui M, Pillai RS, Sabetghadam A, Benoit V, Normand P, et al. (2017) Revisiting the Aluminum Trimesate-Based MOF (MIL-96): From Structure Determination to the Processing of Mixed Matrix Membranes for CO2 Capture. Chemistry of Materials 29: 10326–10338. Available: http://dx.doi.org/10.1021/acs.chemmater.7b03203.
SponsorsWe acknowledge the European Community Seventh Framework Program (FP7/2007-2013) for funding the research presented in this article under Grant Agreement No. 608490 (Project M4CO2). We thank IMPC FR2482 for SEM-FEG instrumentation funded by CNRS, UPMC, and C'Nano projects of Region Ile-de-France. We also acknowledge synchrotrons SOLEIL (Saint-Aubin, France) and ALBA (Barcelona, Spain) for SAXS beam time allocation. We additionally thank Thomas Bizien (SWING, SOLEIL) for his help during SAXS experiments and the staff of the PROMMA 2A at SOLEIL for technical assistance. G.M. thanks Institut Universitaire de France for its support.
PublisherAmerican Chemical Society (ACS)
JournalChemistry of Materials