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Developing highly efficient and low‐cost photocatalysts for overall water splitting has long been a pursuit for converting solar power into clean hydrogen energy. Herein, we demonstrate that a nonstoichiometric nickel–cobalt double hydroxide can achieve overall water splitting by itself upon solar light irradiation, avoiding the consumption of noble‐metal co‐catalysts. We employed an intensive laser to ablate a NiCo alloy target immersed in alkaline solution, and produced so‐called L‐NiCo nanosheets with a nonstoichiometric composition and O2−/Co3+ ions exposed on the surface. The nonstoichiometric composition broadens the band gap, while O2− and Co3+ ions boost hydrogen and oxygen evolution, respectively. As such, the photocatalyst achieves a H2 evolution rate of 1.7 μmol h−1 under AM 1.5G sunlight irradiation and an apparent quantum yield (AQE) of 1.38 % at 380 nm. [ABSTRACT FROM AUTHOR]

Exploiting low-cost and high-activity catalysts is crucial for lowering energy consumption for hydrogen evolution reaction (HER). Herein, we reported a pure Nickel catalyst with high activity and long-term stability at a large current density in an alkaline medium. We employed an industrial machining technology, turning processing, to generate Ni-chips, a self-supported catalyst, with mostly close-packed planes exposed and high compressive strain. The close-packed plane and compressive strain jointly lower the d -band center of the nickel catalyst and overcome the excessive adsorption for reactive intermediates. As such, Ni-chip achieves ultralow overpotentials of 70 mV at 10 mA cm−2 and 297 mV at 1000 mA cm−2. Particularly, the catalyst exhibits outstanding stability at high current density (1 A cm−2), after working for one and a half months (ca. 1070 h), the initial current density merely declined by 7.3%. With its remarkable catalytic activity, excellent stability, ease of synthesis, and utilization of metallic scraps, the Ni-chip catalyst may serve as a promising catalyst for industrial applications. Ni-chip catalysts with high compressive strain and predominantly close-packed planes were prepared through turning processing. This combination effectively mitigated the excessive adsorption of *OH and *H on the Ni surface, enabling an ultralow overpotential of 297 mV at 1000 mA cm-2, and excellent stability at 1 A cm-2 for 1070 h, demonstrating potential as an efficient and durable electrocatalyst. [Display omitted] [ABSTRACT FROM AUTHOR]

• Single nickel atom is in-situ oxidized and embedded into Ru matrix. • NiRu-0.2 SAC exhibits a low overpotential of 17 mV @ 10 mA cm−2 which is much superior to that of commercial Pt/C (42 mV @ 10 mA cm−2) in alkaline media. • The introduction of oxidized single nickel atom creates a unique atomical interface which boosts water dissociation and H evolution during HER progress. [Display omitted] It is desirable but challenging to fine adjust the electronic structure of single atom to enhance the activity of single atom catalysts (SACs). Herein, we embedded an oxidized single nickel atom into pure ruthenium (Ru) metal (NiRu SAC), thereby constructing an atomic-level interface with high catalytic activity. NiRu SAC exhibits a long-term durability and an extremely low overpotential for hydrogen evolution reaction (optimal value reaches 17 mV) at 10 mA cm−2 which is superior to that of the commercial Pt/C catalyst and most reported Ru-based catalysts. NiRu-0.2 SAC also shows a remarkable oxygen evolution reaction (OER) performance of 210 mV at 10 mA cm−2, and a resulted excellent water splitting property (1.5 V vs. RHE @ 10 mA cm−2). Density functional theory (DFT) calculations demonstrate the fabricated oxidized single-nickel-atomic interface (between single nickel atom and neighboring Ru/O atom) not only lowers the energy barrier for water dissociation but also optimizes the H adsorption through the interaction between the interfacial Ru and O atoms. The single-atomic tailoring provides a new idea to further enhance the performance of single atom catalysts to satisfy the industrial applications. [ABSTRACT FROM AUTHOR]