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Limiting the increase of CO₂ in the atmosphere is one of the largest challenges of our generation. Because carbon capture and storage is one of the few viable technologies that can mitigate current CO₂ emissions, much effort is focused on developing solid adsorbents that can efficiently capture CO₂ from flue gases emitted from anthropogenic sources. One class of materials that has attracted considerable interest in this context is metal–organic frameworks (MOFs), in which the careful combination of organic ligands with metal-ion nodes can, in principle, give rise to innumerable structurally and chemically distinct nanoporous MOFs. However, many MOFs that are optimized for the separation of CO₂ from nitrogen^{, , –} do not perform well when using realistic flue gas that contains water, because water competes with CO₂ for the same adsorption sites and thereby causes the materials to lose their selectivity. Although …