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Abstract Sodium all‐solid‐state batteries (NaSSBs) with an alloy‐type anode (e.g., Sn and Sb) offer superior capacity and energy density compared to hard carbon anode. However, the irreversible loss of Na⁺at the alloy anode during the initial cycle results in diminished capacity and stability, impairing full‐cell performance. This study presents an easy‐to‐implement cathode presodiation strategy by employing a Na‐rich material to address these challenges. Leveraging the high theoretical capacity and suitable voltage window, Na₂S is chosen as the Na donor, which is activated by creating a mixed electron‐ion conducting network, delivering a high capacity of 511.7 mAh g⁻¹. By adding a small amount (i.e., 3 wt.%) of Na₂S to the cathode composite, a NaCrO₂|| Sn full cell demonstrated capacity improvement from 90.8 to 118.2 mAh g⁻¹(based on cathode mass). The capacity‐balanced full cell can thus cycle to more than 300 times with >90% capacity retention. This work provides a practical solution to enhance the full‐cell performance and advance the transformation from half‐cell to full‐cell applications of NaSSBs. 

Abstract Porous electrodes that conduct electrons, protons, and oxygen ions with dramatically expanded catalytic active sites can replace conventional electrodes with sluggish kinetics in protonic ceramic electrochemical cells. In this work, a strategy is utilized to promote triple conduction by facilitating proton conduction in praseodymium cobaltite perovskite through engineering non‐equivalent B‐site Ni/Co occupancy. Surface infrared spectroscopy is used to study the dehydration behavior, which proves the existence of protons in the perovskite lattice. The proton mobility and proton stability are investigated by hydrogen/deuterium (H/D) isotope exchange and temperature‐programmed desorption. It is observed that the increased nickel replacement on the B‐site has a positive impact on proton defect stability, catalytic activity, and electrochemical performance. This doping strategy is demonstrated to be a promising pathway to increase catalytic activity toward the oxygen reduction and water splitting reactions. The chosen PrNi_0.7Co_0.3O_3−δoxygen electrode demonstrates excellent full‐cell performance with high electrolysis current density of −1.48 A cm⁻²at 1.3 V and a peak fuel‐cell power density of 0.95 W cm⁻²at 600 °C and also enables lower‐temperature operations down to 350 °C, and superior long‐term durability.