BaCeO3 perovskite-incorporated Co catalyst for efficient NH3 synthesis under mild conditions

[Display omitted] •Co-incorporation of Ba and Ce onto Co drastically boosts NH3 synthesis.•Optimized Ba/CoCe catalyst shows excellent activity, durability, and cost-efficiency.•BaCeO3 perovskite formed during the synthesis is critical for promotion.•Co–BaCeO3 interface shows moderate N2 adsorption strength to activate N2.•The reaction occurs via N2H4-mediated associative mechanism. The growing demand for ammonia (NH3) as a carbon-free fuel and hydrogen carrier for decarbonization has increased interest in its synthesis under mild conditions to cope with the intermittent renewable supply of electricity and green hydrogen. Developing active and cost-efficient catalysts is crucial for achieving this goal. Herein, we investigated Ba and Ce incorporated Co (Ba/CoCe) as an efficient catalyst for ammonia synthesis. Our findings show that the optimal amount of Ba and Ce incorporation onto Co resulted in a drastic increase in catalytic activity compared to both pure Co and Ba or Ce singly promoted Co catalysts. Moreover, it exhibits superior catalytic performance and cost efficiency when compared to state-of-the-art benchmark catalysts. Co-incorporation of Ba and Ce forms BaCeO3 perovskite during catalyst preparation. Co–BaCeO3 interface bears a moderate adsorption strength of nitrogen, showing high adsorption–desorption reversibility of N atoms. Reaction studies coupled with structural characterizations give an insight into the presence of the kinetically favored associative mechanism, thereby significantly reducing the activation energy and boosting the NH3 synthesis rate. This work provides insight into the design of non-noble metal catalysts for ammonia synthesis under mild conditions, and also contributes to the potential design of the perovskite family for catalytic purposes.