Tuning the Coordination Structure of Cu?N?C Single Atom Catalysts for Simultaneous Electrochemical Reduction of CO ₂ and NO ₃ ^– to Urea

Closing both the carbon and nitrogen loops is a critical venture to support establishment of circular, net-zero economy. Although single atom catalysts (SACs) have gained interest for electrochemical reduction reactions dioxide (CO2RR) nitrate (NO3RR), structure–activity relationship Cu SAC coordination these remains unclear should be explored such that fundamental understanding developed. To this end, role structure investigated in dictating activity selectivity CO2RR NO3RR. In agreement with density functional theory calculations, it revealed Cu-N4 sites exhibit higher intrinsic toward CO2RR, whilst Cu-N4?x-Cx are active Leveraging findings, NO3RR coupled formation urea on SACs, revealing importance *COOH binding as parameter determining catalytic production. best authors’ knowledge, first report employing SACs synthesis from NO3RR, which achieves Faradaic efficiency 28% production current ?27 mA cm–2 at ?0.9 V versus reversible hydrogen electrode.