Regulating Extra‐Framework Cations in Faujasite Zeolites for Capture of Trace Carbon Dioxide

Abstract The development of cost‐effective sorbents for direct capture of trace CO 2 (<1 %) from the atmosphere is an important and challenging task. Natural or commercial zeolites are promising sorbents, but their performance in adsorption of trace CO 2 has been poorly explored to date. A systematic study on capture of trace CO 2 by commercial faujasite zeolites reveals that the extra‐framework cations play a key role on their performance. Under dry conditions, Ba−X displays high dynamic uptake of 1.79 and 0.69 mmol g −1 at CO 2 concentrations of 10000 and 1000 ppm, respectively, and shows excellent recyclability in the temperature‐swing adsorption processes. K−X exhibits perfect moisture resistance, and >95 % dry CO 2 uptake can be preserved under relative humidity of 74 %. In situ solid‐state NMR spectroscopy, synchrotron X‐ray diffraction and neutron diffraction reveal two binding sites for CO 2 in these zeolites, namely the basic framework oxygen atoms and the divalent alkaline earth metal ions. This study unlocks the potential of low‐cost natural zeolites for applications in direct air capture.