Co Single Atoms and CoOx Nanoclusters Anchored on Ce0.75Zr0.25O2 Synergistically Boosts the NO Reduction by CO

Abstract Achieving high NO conversion and N 2 selectivity in selective catalytic reduction of NO by CO (CO‐SCR) in a wide operating temperature window, particularly in the presence of high O 2 concentration, remains a big challenge. Herein, guided by density functional theory (DFT) calculations, a catalyst is rationally developed with dual active centers consisting of both Co single‐atoms (SAs) and CoO x nanoclusters (NCs) co‐anchored on Ce 0.75 Zr 0.25 O 2 support (CZO), which show above 99.7% NO conversion and 100% N 2 selectivity at 250–400 °C under 5 vol% O 2 . DFT calculation and experimental results confirm a strong interaction among Co SAs, CoO x NCs, and CZO support. Co SAs enhance CO adsorption and accompany the oxygen vacancies (OVs) formation in CZO, while the CoO x NCs promote both NO conversion to nitrate intermediate and the breakage of the NO bond at OVs, thus synergistically boosting the N 2 formation.