Metal–organic frameworks (MOFs) represent the largest known class of porous crystalline materials ever synthesized. Their narrow pore windows and nearly unlimited structural and chemical features have made these materials of significant interest for membrane-based gas separations. In this comprehensive review, we discuss opportunities and challenges related to the formation of pure MOF films and mixed-matrix membranes (MMMs). Common and emerging separation applications are identified, and membrane transport theory for MOFs is described and contextualized relative to the governing principles that describe transport in polymers. Additionally, cross-cutting research opportunities using advanced metrologies and computational techniques are reviewed. To quantify membrane performance, we introduce a simple membrane performance score that has been tabulated for all of the literature data compiled in this review. These data are reported on upper bound plots, revealing classes of MOF materials that consistently demonstrate promising separation performance. Recommendations are provided with the intent of identifying the most promising materials and directions for the field in terms of fundamental science and eventual deployment of MOF materials for commercial membrane-based gas separations.

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Zirconiumv (IV)-carboxylate metal-organic framework (MOF) UiO-66 nanoparticles were successfully synthesized and incorporated in the polyamide (PA) selective layer to fabricate novel thin-film nanocomposite (TFN) membranes. Compared to unmodified pure polyamide thin-film composite (TFC) membranes, the incorporation of UiO-66 nanoparticles significantly changes the membrane morphology and chemistry, leading to an improvement of intrinsic separation properties due to the molecular sieving and superhydrophilic nature of UiO-66 particles. The best performing TFN-U2 (0.1 wt % particle loading) membrane not only shows a 52% increase of water permeability but also maintains salt rejection levels (∼95%) similar to the benchmark. The effects of UiO-66 loading on the forward osmosis (FO) performance were also investigated. Incorporation of 0.1 wt % UiO-66 produced a maximum water flux increase of 40% and 25% over the TFC control under PRO and FO modes, when 1 M NaCl was used as the draw solution against deionized water feed. Meanwhile, solute reverse flux was maintained at a relatively low level. In addition, TFN-U2 membrane displayed a relatively linear increase in FO water flux with increasing NaCl concentration up to 2.0 M, suggesting a slightly reduced internal concentration polarization effect. To our best knowledge, the current study is the first to consider implementation of Zr-MOFs (UiO-66) onto TFN-FO membranes.

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