Theoretical calculations unveil the charge redistribution over abundant interfaces and the enhanced electronic states of Ru/RuS2 heterostructure. The resulting surface electron‐deficient Ru sites display optimized adsorption behavior toward diverse reaction intermediates, thereby reducing the thermodynamic energy barriers. Experimentally, for the first time the laminar Ru/RuS2 heterostructure is rationally engineered by virtue of the synchronous reduction and sulfurization under eutectic salt system. Impressively, it exhibits extremely high catalytic activity for both OER (201 mV @ 10 mA cm−2) and HER (45 mV @ 10 mA cm−2) in acidic media due to favorable kinetics and excellent specific activity, consequently leading to a terrific performance in acidic overall water splitting devices (1.501 V @ 10 mA cm−2). The in‐depth insight into the internal activity origin of interfacial effect could offer precise guidance for the rational establishment of hybrid interfaces.

The highly efficient energy conversion of the polymer-electrolyte-membrane fuel cell (PEMFC) is extremely limited by the sluggish oxygen reduction reaction (ORR) kinetics and poor electrochemical stability of catalysts. Hitherto, to replace costly Pt-based catalysts, non-noble-metal ORR catalysts are developed, among which transition metal-heteroatoms-carbon (TM-H-C) materials present great potential for industrial applications due to their outstanding catalytic activity and low expense. However, their poor stability during testing in a two-electrode system and their high complexity have become a big barrier for commercial applications. Thus, herein, to simplify the research, the typical Fe-N-C material with the relatively simple constitution and structure, is selected as a model catalyst for TM-H-C to explore and improve the stability of such a kind of catalysts. Then, different types of active sites (centers) and coordination in Fe-N-C are systematically summarized and discussed, and the possible attenuation mechanism and strategies are analyzed. Finally, some challenges faced by such catalysts and their prospects are proposed to shed some light on the future development trend of TM-H-C materials for advanced ORR catalysis.

Theoretical calculations unveil the charge redistribution over abundant interfaces and the enhanced electronic states of Ru/RuS2 heterostructure. The resulting surface electron‐deficient Ru sites display optimized adsorption behavior toward diverse reaction intermediates, thereby reducing the thermodynamic energy barriers. Experimentally, for the first time the laminar Ru/RuS2 heterostructure is rationally engineered by virtue of the synchronous reduction and sulfurization under eutectic salt system. Impressively, it exhibits extremely high catalytic activity for both OER (201 mV @ 10 mA cm−2) and HER (45 mV @ 10 mA cm−2) in acidic media due to favorable kinetics and excellent specific activity, consequently leading to a terrific performance in acidic overall water splitting devices (1.501 V @ 10 mA cm−2). The in‐depth insight into the internal activity origin of interfacial effect could offer precise guidance for the rational establishment of hybrid interfaces.

Developing high‐efficiency electrocatalysts toward overall water splitting is an increasingly important area for sustainable energy evolution. Theoretical calculation results demonstrate that the incorporation of Ru optimizes the Gibbs free energy of adsorption of H2O molecules and intermediates for the hydrogen/oxygen evolution reactions (HER/OER) on metal selenide sites, thus boosting electrocatalytic overall water splitting. Accordingly, ruthenium modified nickel diselenide nanosheet arrays are designed and construct on nickel foam (Ru–NiSe2/NF). The obtained Ru–NiSe2/NF electrode with a stable 3D structure shows greatly improved OER and HER activity in alkaline solution. Particularly, toward OER, it only requires 210 mV to obtain a current density of 10 mA cm−2, and the formation of the intermediate nickel oxyhydroxide as active center during the OER process is captured by in situ Raman. Moreover, the overall water splitting can be driven by a voltage of merely 1.537 V to obtain 10 mA cm−2. This work provides an available strategy for selenides to enhance electrochemical properties and inspires more studies to explore highly efficient electrocatalysts toward full water splitting.

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