In Situ Engineered NiCoRu-CeO₂ Interfaces for Active and Stable Ammonia Conversion Toward High-Performance Direct...

Direct ammonia proton-conducting ceramic fuel cells (DA-PCFCs) emerge as one promising clean energy technology that directly utilizes ammonia as a hydrogen-rich, zero-carbon fuel. However, limited catalytic activity and structural instability of conventional Ni-based anode under ammonia atmospheres impose daunting challenges in the practical DA-PCFCs application. Here, we develop the stable NiCoRu-CeO₂ catalytic heterointerface using the facile strategy of infiltration coupled with in situ conversion of the Ce_0.9Co_0.09Ru_0.01O₂ (CCR) precursor on Ni-BaCe_0.7Zr_0.1Y_0.1Yb_0.1O_{3- δ} (Ni-BCZYYb) anode. The in situ engineered NiCoRu-CeO₂ heterointerface synergistically promotes efficient ammonia decomposition and proton conduction, achieving a near-complete and stable conversion efficiency close to 100% at 600°C under 300 h operation. Mechanism studies reveal that CCR-induced electronic modulation facilitates sufficient charge transfer and downshifts the Ni d-band center, thereby optimizing adsorption energetics of reactants and key intermediates, and mitigating the over-binding of NH₃ toward an efficient and stable ammonia conversion process. Using CCR@Ni-BCZYYb anodes, the assembled DA-PCFCs exhibit a high peak power density of 1.06 W cm^-2 at 650°C, and negligible degradation over 300 h of operation. This work provides an effective interface engineering strategy for developing highly active and durable ammonia-fueled PCFCs.