Carbon and Oxygen Double Defects Enhanced Ru‐based Catalyst for Ammonia Decomposition

Although ammonia is widely recognized as one of the most promising candidates for hydrogen storage and transformation, the catalytic mechanisms involved in ammonia decomposition remain insufficiently understood, and the stability of catalysts continues to present significant challenges. In this study, Ru/CeO2‐CNTs catalysts with double defect sites were synthesized by a straightforward method, achieving an outstanding hydrogen production rate of 2,230 mmol/gRu/min at 500 °C, outperforming most Ru‐based catalysts. Experimental characterization and theoretical calculations revealed that the CeO2‐CNT interface promotes the formation of oxygen vacancies (Ov) and carbon defects (Cd) through carbon‐oxygen interactions. These defects enhance electron transfer from the support to Ru nanoparticles (NPs), modulate NH3 adsorption and activation, as well as the recombination and desorption of adsorbed N species (N*). Moreover, the coating of CeO2 significantly improved the stability of CNTs, which weakens undesired reaction under high temperature and hydrogen‐rich conditions. The study introduced a rational design strategy that enhance the multiple elementary stages of the NH3 decomposition by constructing double defect sites, and offering new insights into the design of efficient and durable catalysts under harsh environment.