Exploiting highly effective and low‐cost electrocatalysts for the hydrogen evolution reaction (HER) is a pressing challenge for the development of sustainable hydrogen energy. In this work, a facile and industrially compatible one‐pot corrosion strategy for the rapid synthesis of amorphous RuO2‐decorated FeOOH nanosheets on iron foam (FFNaRu) within 1 h is reported. Corrosion is a common and inevitable phenomenon that occurs on metal surfaces without electricity input, high temperature, and tedious synthetic procedures. The FFNaRu electrode is superhydrophilic and aerophobic, which guarantees intimate contact with the electrolyte and accelerates the instantaneous escape of produced gas bubbles during the electrocatalytic process. Moreover, the strong electronic interactions between RuO2 and FeOOH promote the electrocatalytic process via dramatically improving the electrochemical interfacial properties. Thus, the FFNaRu electrocatalyst presents excellent catalytic activity towards the HER (30 mV at 10 mA cm–2) and overall water‐splitting (230 mV at 10 mA cm–2) in 1 M KOH. The overall water‐splitting could be simply powered by sustainable and intermittent sunlight, wind, and thermal energies motivated Stirling engine. Density functional theory calculations confirm that coupling effects between RuO2 and FeOOH are also responsible for promoting the electrocatalytic HER performance.

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Exploiting efficient and stable electrocatalysts with trifunctional catalytic activity toward hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and oxygen reduction reaction (ORR) act has a crucial role with sustainable energy development. Therefore, this study fabricates Co3O4‐RuO2 hollow spheres using a facile and eco‐friendly solvothermal and low temperature oxidation procedure followed by ice water treatment (IW‐Co3O4‐RuO2‐HS). The specific hollow nanostructure could provide sufficient active sites and channels in the electrocatalytic procedure. Then, the IW‐Co3O4‐RuO2‐HS presents small overpotentials toward HER (40 mV@ 10 mA cm−2) and OER (250 mV@ 10 mA cm−2), and high half‐wave potential for ORR (E1/2@ 0.79 V). Remarkably, the IW‐Co3O4‐RuO2‐HS also presents superior catalytic performances toward water‐splitting and flexible rechargeable Zn–air batteries. Furthermore, the water electrolysis can be driven by sustainable energy, including solar, wind, thermal energy, and the assembled flexible rechargeable Zn–air battery. This study provides a valid path to synthesize multifunctional electrocatalysts on energy‐related devices.

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