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Seawater electrolysis under alkaline conditions represents a sustainable approach to mass production of carbon-neutral hydrogen energy. However, the lack of efficient electrocatalysts restrict the development of this technology. Herein, core-shell-structured...

Exploring advanced electrocatalysts for overall water/seawater splitting is significant to massive green hydrogen production. Here, we report a novel self-sacrificing template strategy to fabricate a heterostructured NiMoO 4 @NiFeP electrode with superwetting properties as a bifunctional electrocatalyst for overall water/seawater splitting. Such an electrode exhibits superior intrinsic activity, more accessible active sites, effective charge transfer, and weak adhesion of gas bubbles. Its excellent corrosion resistance and superhydrophilic/superaerophobic nanoarrayed architecture ensure its catalytic performance under harsh seawater conditions. Accordingly, the electrode requires overpotentials of only 282 and 195 mV at 100 mA cm −2 for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) in 1 M KOH seawater together with its robust durability. Operando Raman spectroscopy together with ex situ characterization technologies reveal that NiMoO 4 @NiFeP was rapidly reconstructed to active Fe-doped β-Ni oxyhydroxides (β-Fe/NiOOH) during alkaline OER. Density functional theory calculations further disclose that Fe doping can optimize the energy barrier and modulate the d-band center of the catalyst, intrinsically boosting the OER performance. Consequently, the NiMoO 4 @NiFeP-assembled electrolyzer requires a voltage of 1.71 V at 100 mA cm −2 for seawater splitting and can stably maintain over 200 h without producing any hypochlorite. Our work holds great promise for constructing efficient non-noble-metal bifunctional electrodes toward water/seawater electrolysis applications.

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