Enhanced hydrogen spillover effect in low-temperature ammonia decomposition via N-coordination and O-vacancy-activated Co/La_xCe_{1-x}AlO_{3-y}N_z catalyst

• • Achieved 92.6% NH3 conversion and 9.7 mmol g−1 min−1 H2 production rate at 425 °C (GHSV=9000 mL h−1 g_cat−1), a 125 °C reduction in operating temperature vs. conventional Co catalysts, enabling lower energy costs for on-demand hydrogen generation. • • The LA-L(A+B)-LB active site configuration, formed by Ce and N co-modification, lowers the Schottky barrier at the Co-support interface, facilitating hydrogen spillover and shifting the reaction to a Mars-van Krevelen mechanism, which bypasses the rate-limiting N2 desorption step. • • Isotopic labeling and in-situ DRIFTS confirm the interfacial mechanism, providing direct evidence for the promotional effect of O-vacancies and N-coordination on hydrogen spillover, which is critical for rational catalyst design. • • The catalyst demonstrates exceptional low-temperature activity, making it a promising candidate for industrial ammonia decomposition units that operate at reduced temperatures, thereby improving process efficiency and catalyst longevity.