Membrane-based gas separations are energy efficient processes; however, major challenges remain to develop high-performance membranes enabling the replacement of conventional separation processes. Herein, a new fluorinated MOF-based mixed-matrix membrane is reported, which is formed by incorporating the MOF crystals into selected polymers via a facile mixed-matrix approach. By finely controlling the molecular transport in the channels through the MOF apertures tuned by metal pillars and at the MOF-polymer interfaces, the resulting fluorinated MOF-based membranes exhibit excellent molecular sieving properties. These materials significantly outperform state-of-the-art membranes for simultaneous removal of H S and CO from natural gas-a challenging and economically important application. The robust fluorinated MOFs (NbOFFIVE-1-Ni, AlFFIVE-1-Ni), pave a way to efficient membrane separation processes that require precise discrimination of closely sized molecules.
MOF-based
mixed-matrix membranes (MMMs) prepared using standard
routes often exhibit poor adhesion between polymers and MOFs. Herein,
we report an unprecedented systematic exploration on polymer functionalization
as the key to achieving defect-free MMMs. As a case study, we explored
computationally MMMs based on the combination of the prototypical
UiO-66(Zr) MOF with polymer of intrinsic porosity-1 (PIM-1) functionalized
with various groups including amidoxime, tetrazole, and N-((2-ethanolamino)ethyl)carboxamide. Distinctly, the amidoxime-derivative
PIM-1/UiO-66(Zr) MMM was predicted to express the desired enhanced
MOF/polymer interfacial interactions and thus subsequently prepared
and evaluated experimentally. Prominently, high-resolution transmission
electron microscopy confirmed optimal adhesion between the two components
in contrast to the nanometer-sized voids/defects shown by the pristine
PIM-1/UiO-66(Zr) MMM. Notably, single-gas permeation measurements
further corroborated the need of optimal MOF/polymer adhesion in order
to effectively enable the MOF to play a role in the gas transport
of the resulting MMM.
Membrane-based gas separations are energy efficient processes; however, major challenges remain to develop highperformance membranes enabling replacement of conventional separation processes. Here, a new fluorinated MOF-based mixedmatrix membrane is reported, which is formed by incorporating the MOF crystals into selected polymers via a facile mixed-matrix approach. By finely controlling the molecular transport in the channels through MOF apertures tuned by metal pillars and at the MOFpolymer interfaces, the resulting fluorinated MOF-based membranes exhibit excellent molecular sieving properties. We show that these materials significantly outperform state-of-the-art membranes for simultaneous removal of H 2 S and CO 2 from natural gas-a challenging and economically-important application. The robust fluorinated MOFs (NbOFFIVE-1-Ni, AlFFIVE-1-Ni), with tunable channel apertures provided by tuning the metal pillars and/or organic linker, pave a new avenue to efficient membrane separation processes that require precise discrimination of closely sized molecules.
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