

Through a mild pyrolysis‐free route, cooperative coupling of single cobalt atoms (CoSA) and fully exposed platinum nanoclusters (PtNC) is assembled. As expected, the as‐prepared catalysts PtNC/CPF‐Co exhibit dual‐functional performance and high adaptability, demonstrating low overpotentials of 44 mV for HER and 340 mV for OER at 10 mA cm−2 in saline electrolysis. Abstract The development of large‐scale and low‐cost hydrogen production based on water splitting necessitates the design of well‐defined and highly adaptable catalytic materials. Advancements in synthesis strategies are crucial for the preparation of efficient catalysts and the understanding of underlying mechanisms. Here, a pyrolysis‐free strategy is present toward the directive assembly of cooperative coupling single cobalt atoms and fully exposed platinum nanoclusters as active sites. The catalysts possess dual functionality and high adaptability for overall saline electrolysis. As expected, both the electrode and the symmetric cell deliver good catalytic activity and stability. Additionally, the rational and controllable synthesis leads to comprehensive analysis, which reveals that the cooperative coupling between Pt‐Co sites can regulate the interaction between the intermediates and active centers to improve the activity, prevent the Cl− poisoning, and ensure the efficient selectivity. The catalytic performance has been well‐maintained in not only saline water, but also fluctuant and extreme concentrations of hydroxide. This work expedites the research progress and future deployment of rationally designed and efficient saline or seawater electrolyzers. Through a mild pyrolysis-free route, cooperative coupling of single cobalt atoms (CoSA) and fully exposed platinum nanoclusters (PtNC) is assembled. As expected, the as-prepared catalysts PtNC/CPF-Co exhibit dual-functional performance and high adaptability, demonstrating low overpotentials of 44 mV for HER and 340 mV for OER at 10 mA cm −2 in saline electrolysis. Abstract The development of large-scale and low-cost hydrogen production based on water splitting necessitates the design of well-defined and highly adaptable catalytic materials. Advancements in synthesis strategies are crucial for the preparation of efficient catalysts and the understanding of underlying mechanisms. Here, a pyrolysis-free strategy is present toward the directive assembly of cooperative coupling single cobalt atoms and fully exposed platinum nanoclusters as active sites. The catalysts possess dual functionality and high adaptability for overall saline electrolysis. As expected, both the electrode and the symmetric cell deliver good catalytic activity and stability. Additionally, the rational and controllable synthesis leads to comprehensive analysis, which reveals that the cooperative coupling between Pt-Co sites can regulate the interaction between the intermediates and active centers to improve the activity, prevent the Cl − poisoning, and ensure the efficient selectivity. The catalytic performance has been well-maintained in not only saline water, but also fluctuant and extreme concentrations of hydroxide. This work expedites the research progress and future deployment of rationally designed and efficient saline or seawater electrolyzers. Advanced Science, Volume 12, Issue 48, December 29, 2025.
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