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As a new family of adsorbent materials, porous metal–organic frameworks (MOFs) have attracted enormous attention over the past decade.[1] Having a large surface area,[2] tunable pore size and shape,[3] adjustable composition and functionalizable pore surface,[4] MOFs show unique advantages and promises for potential applications in adsorption-based storage and separation technologies for small gas molecules such as H2, CO2, and CH4.[1b, d, 5]

CO2 capture from flue gases is of particular importance in reducing greenhouse gas emissions and in preserving environmental health. A flue gas mixture is composed of nitrogen, carbon dioxide, water vapor, oxygen, and other minor components such as carbon monoxide, nitrogen oxides, and sulfur oxides.[1b, 6] Separation of low-concentration CO2 (about 10–15%) from nitrogen-rich streams remains a challenging task at the present time. Adsorption-based …