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Carbon capture and storage (CCS) from large point sources such as power plants is one option for reducing anthropogenic CO<jats:sub>2<\/jats:sub> emissions; however, currently the capture alone will increase the energy requirements of a plant by 25\u201340\u2009%. This Review highlights the challenges for capture technologies which have the greatest likelihood of reducing CO<jats:sub>2<\/jats:sub> emissions to the atmosphere, namely postcombustion (predominantly CO<jats:sub>2<\/jats:sub>\/N<jats:sub>2<\/jats:sub> separation), precombustion (CO<jats:sub>2<\/jats:sub>\/H<jats:sub>2<\/jats:sub>) capture, and natural gas sweetening (CO<jats:sub>2<\/jats:sub>\/CH<jats:sub>4<\/jats:sub>). The key factor which underlies significant advancements lies in improved materials that perform the separations. 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