Approaching Durable Single-Layer Fuel Cells: Promotion of Electroactivity and Charge Separation via Nanoalloy Redox Exsolution.

Single-layer fuel cells (SLFCs) based on mixed semiconductors and ionic conductors demonstrate  simplified material preparation and fabrication procedure and possess high performance potentially. However, the operational stability and principle of SLFCs have not yet been convinced of either commercialization or fundamental interests. We hereby report on the employment of a perovskite oxide-based phase-structured redox-stable semiconductor prior to determining a possible solution that improves the durability of the SLFC. Feasible working principles are established and an in-depth understanding of the short-circuit-free phenomenon in SLFCs with the mixed ionic and electronic conductors is provided. Additionally, a smart material design and cell structure processing are also proposed. An extended nonstop testing period of up to 2 days confirms the project feasibility and improved durability of the SLFCs, achieved by replacing the unstable lithiated oxide phase with redox-stable perovskite oxide, though the electrochemical performance is sacrificed. The precipitated metal/alloy nanoparticle on perovskite oxide not only improves the electrode reaction kinetics but also facilitates the charge separation and ionic conduction in SLFCs, consequently enhancing the fuel cell performance and electrical efficiency. The results confirmed the potential of stable operation for future practical deployment of SLFCs via appropriate selection of material and cell structure design. It is greatly believed that the physical junction plays a crucial role in overcoming the internal short-circuit issue of SLFCs.