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Disclosed is a method and device for separating carbon dioxide, wherein carbon dioxide adsorption ability can be maintained over the long term by means of recovering and re-supporting on a carbon dioxide adsorption material amine compounds that vaporize during operation. An amine recovery device (11) and an aqueous amine solution preparation device (14) are connected to an adsorption-material-filled tank (1), which has been filled with the carbon dioxide adsorption material (2), amine compounds vaporized from the carbon dioxide adsorption material (2) during operation are recovered to the aqueous amine solution preparation device (14) by means of the amine recovery device (11), and recovered amine compounds are re-supported on the carbon dioxide adsorption material (2) via a supply line (7).