Dual‐Site Interaction Tailoring Dynamic Reconstruction of Pt‐Ni Dual‐Site Catalysts for Advanced Zn‐Urea‐Air Batteries

ABSTRACT Dynamic reconstruction of single‐atom sites generates high‐activity species but typically leads to irreversible aggregation and degradation during prolonged operation, presenting a fundamental dilemma for durable electrocatalysis. Here, we propose and demonstrate a strategy to master this reconstruction by constructing synergistic dual single‐atom sites, where one stable site guides the evolution of a neighboring reconstruction‐prone site. Using an underpotential electrodeposition method, a Pt‐Ni dual single‐atom (DSA) catalyst with locally coupled PtO 4 and NiO 6 sites was fabricated. In situ characterizations and theoretical calculations reveal that the Pt‐Ni interaction guides a self‐optimizing reconstruction for enhanced activity. During oxygen evolution and urea oxidation reactions (OER/UOR), Ni sites are dynamically transformed into ultrafine and stabilized NiOOH clusters anchored around PtO 4 ‐SA sites, forming an integrated PtO 4 ‐SA/NiOOH active center; while PtO 4 sites demonstrate enhanced oxygen reduction reaction (ORR) activity due to the dual‐site electronic interaction. When deployed in a zinc‐urea‐air battery (ZUAB), the catalyst enables a superior energy efficiency (61%) and long‐term durability (> 500 h). This work not only offers fundamental insights into the dual‐site interaction guiding the self‐optimization in DSAs, but also provides a generalizable design principle for creating active and stable catalysts by proactively tailoring dynamic site reconstruction.