Ruth Ebenbauer, Therese Adam Møller, Jakob Bjørn, Clemens Kaußler, Craig Day, Hongwei Sun, Dennis Wilkens Juhl, Niels Chr. Nielsen, Kim Daasbjerg, Simon Stampe Kildahl, Troels Skrydstrup
Here, we report the transition-metal-catalyzed post-functionalization of consumer polystyrene plastics using a gold-catalyzed bromination followed by a copper-catalyzed Ullmann-type C–N coupling to access self-supported solid amine CO 2 sorbents. The method enables selective control over the degree of functionalization and amine motifs, and it yields macroporous amine networks with up to 15 wt % nitrogen incorporation. The resulting materials display competitive CO 2 -capture performance under both flue gas and direct-air-capture conditions, with capacities up to 2.5 mmol g −1 at 25°C and excellent cyclability over 48 thermal swing cycles. Furthermore, the protocol was successfully demonstrated on a series of end-of-life polystyrene samples, including expanded polystyrene packaging and other single-use plastics, in order to showcase its robustness and broad applicability. We anticipate that this upcycling strategy will advance catalytic polymer amination methods and provide a sustainable route to next-generation CO 2 sorbents.