1f:T40d,Efficient oxygen-evolution reaction catalysts are required for the cost-effective generation of solar fuels. Metal selenides have been reported as promising oxygen-evolution catalysts; however, their active forms are yet to be elucidated. Here we show that a representative selenide catalyst, nickel selenide, is entirely converted into nickel hydroxide under oxygen-evolution conditions. This result indicates that metal selenides are unstable during oxygen evolution, and the in situ generated metal oxides are responsible for their activity. This knowledge inspired us to synthesize nanostructured nickel iron diselenide, a hitherto unknown metal selenide, and to use it as a templating precursor to a highly active nickel iron oxide catalyst. This selenide-derived oxide catalyses oxygen evolution with an overpotential of only 195 mV for 10 mA cm(-2). Our work underscores the importance of identifying the active species of oxygen-evolution catalysts, and demonstrates how such knowledge can be applied to develop better catalysts.20:T4be,Rational design of the catalysts is impressive for sustainable energy conversion. However, there is a grand challenge to engineer active sites at the interface. Herein, hierarchical transition bimetal oxides/sulfides heterostructure arrays interacting two-dimensional MoO_x/MoS₂ nanosheets attached to one-dimensional NiO_x/Ni₃S₂ nanorods were fabricated by oxidation/hydrogenation-induced surface reconfiguration strategy. The NiMoO_x/NiMoS heterostructure array exhibits the overpotentials of 38 mV for hydrogen evolution and 186 mV for oxygen evolution at 10 mA cm^-2, even surviving at a large current density of 500 mA cm^-2 with long-term stability. Due to optimized adsorption energies and accelerated water splitting kinetics by theory calculations, the assembled two-electrode cell delivers the industrially relevant current densities of 500 and 1000 mA cm^-2 at record low cell voltages of 1.60 and 1.66 V with excellent durability. This research provides a promising avenue to enhance the electrocatalytic performance of the catalysts by engineering interfacial active sites toward large-scale water splitting.21:T4c9,The establishment of electrocatalysts with bifunctionality for efficient oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) in acidic environments is necessary for the development of proton exchange membrane (PEM) water electrolyzers for the production of clean hydrogen fuel. RuIr alloy is considered to be a promising electrocatalyst because of its favorable OER performance and potential for HER. Here, the design of a bifunctional electrocatalyst with greatly boosted water-splitting performance from doping RuIr alloy nanocrystals with transition metals that modify electronic structure and binding strength of reaction intermediates is reported. Significantly, Co-RuIr results in small overpotentials of 235 mV for OER and 14 mV for HER (@ 10 mA cm^-2 current density) in 0.1 m HClO₄ media. Therefore a cell voltage of just 1.52 V is needed for overall water splitting to produce hydrogen and oxygen. More importantly, for a series of M-RuIr (M = Co, Ni, Fe), the catalytic activity dependence at fundamental level on the chemical/valence states is used to establish a novel composition-activity relationship. This permits new design principles for bifunctional electrocatalysts.22:T4e6,Electrocatalytic performance can be enhanced by engineering a purposely designed nanoheterojunction and fine-tuning the interface electronic structure. Herein a new approach of developing atomic epitaxial in-growth in Co-Ni₃ N nanowires array is devised, where a nanoconfinement effect is reinforced at the interface. The Co-Ni₃ N heterostructure array is formed by thermal annealing NiCo₂ O₄ precursor nanowires under an optimized condition, during which the nanowire morphology is retained. The epitaxial in-growth structure of Co-Ni₃

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