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The conventional electrolytic water‐splitting process for hydrogen production is plagued by high energy consumption, low efficiency, and the requirement of expensive catalysts. Therefore, finding effective, affordable, and stable catalysts to drive this reaction is urgently needed. We report a nanosheet catalyst composed of carbon nanotubes encapsulated with MoC/Mo2C, the Ni@MoC‐700 nanosheet showcases low overpotentials of 275 mV for the oxygen evolution reaction and 173 mV for the hydrogen evolution reaction at a current density of 10 mA ⋅ cm−2. Particularly noteworthy is its outstanding performance in a two‐electrode system, where a cell potential of merely 1.64 V is sufficient to achieve the desired current density of 10 mA ⋅ cm−2. Furthermore, the catalyst demonstrates exceptional durability, maintaining its activity over a continuous operation of 40 hours with only minimal attenuation in overpotential. These outstanding activity levels and long‐term stability unequivocally highlight the promising potential of the Ni@MoC‐700 catalyst for large‐scale water‐splitting applications. [ABSTRACT FROM AUTHOR]

[Display omitted] Heterojunction can effectively improve oxygen evolution reaction (OER) activity by regulating the interfacial electronic structure of catalysts. However, p-p type heterojunction OER catalysts have obtained less attention, and the corresponding catalytic mechanisms are unclear either. Herein, the self-supported CoP-CoO p-p type heterojunction arrays are fabricated on carbon cloth substrate (CoP-CoO/CC). Band structure analysis shows that the formation of p-p heterojunction can drive the electrons from CoO to flow into CoP. This electronic modulation contributes to positively charged regions on the CoO and enhances the OH− adsorption during OER, proven by X-ray photoelectron spectroscopy and methanol molecular detection, respectively. As a result, the CoP-CoO/CC electrode only needs 210 mV overpotential to drive a current density of 10 mA cm−2 in an alkaline medium, superior to the most reported OER catalysts. Additionally, the CoP-CoO/CC also exhibits an ideal hydrogen evolution reaction response, and a water splitting system has been successfully constructed which can drive a 10 mA cm−2 within 1.65 V. This study supplies insight for catalytic origins p-p type heterojunctions OER catalyst, which provides a reference value for the efficient and reasonable design of heterojunction catalysts. [ABSTRACT FROM AUTHOR]

Developing efficient oxygen evolution reaction (OER) electrocatalysts with earth-abundant elements is very important for sustainable H 2 generation via electrochemical water splitting. Here we design a crystalline-amorphous Ni–Fe–Al hybrid phosphides nanosheet arrays grown on NiFe foam for efficient OER application. Dynamic surface reorganization of phosphides at anodic/cathodic polarizations is probed by in situ Raman spectroscopy. The reconstructed amorphous Ni(Fe)OOH species are determined as the active phases that facilitate the OER process. This unique electrode shows highly catalytic activity toward water oxidation, achieving the current densities of 10 and 100 mA cm−2 at 181 and 214 mV in 1 M KOH, respectively. Meanwhile, it also exhibits excellent stability at a large current density of 100 mA cm−2 for over 60 h. This work reveals the dynamic structural transformation of pre-catalyst in realistic conditions and highlights the important role of oxyhydroxides as real reactive species in OER process with high activity. [Display omitted] • Ni–Fe–Al hybrid phosphides nanosheet arrays were synthesized for OER. • Dynamic self-reconstruction was revealed by in situ Raman spectroscopy. • Amorphous Ni(Fe)OOH species act as the real active phases. • Regenerated pre-catalyst shows excellent OER activity. [ABSTRACT FROM AUTHOR]

Rational design of high efficient and low cost oxygen evolution reaction (OER) electrodes is critical for electrochemical water splitting. Herein, we report Reevesite Ni−Fe layered double hydroxide (NiFe‐(CO32−)‐LDH) nanosheet arrays as novel OER catalysts in alkaline electrolyte. These self‐supported nanosheet arrays with a composition of Ni6Fe2(CO3)(OH)16 ⋅ 4H2O on Ni foam (NF) were synthesized by a one‐pot hydrothermal method, in which NF served as both the conductive substrate and Ni source. The morphology and OER activity can be tuned by iron concentration. In 1 M KOH, the optimized NiFe‐(CO32−)‐LDH catalyst only required overpotentials of 228 and 264 mV to deliver current densities of 10 and 100 mA cm−2, respectively, with a small Tafel slope of 37 mV dec−1. Remarkably, this catalyst also showed outstanding durability by long‐term operation for 20 h with 96 % retention. Our work provides attractive cost‐effective 3D catalysts for efficient and robust water oxidation at alkaline media. [ABSTRACT FROM AUTHOR]

Owing to the unique electronic properties, rare‐earth modulations in noble‐metal electrocatalysts emerge as a critical strategy for a broad range of renewable energy solutions such as water‐splitting and metal–air batteries. Beyond the typical doping strategy that suffers from synthesis difficulties and concentration limitations, the innovative introduction of rare‐earth is highly desired. Herein, a novel synthesis strategy is presented by introducing CeO2 support for the nickel–iron–chromium hydroxide (NFC) to boost the oxygen evolution reaction (OER) performance, which achieves an ultralow overpotential at 10 mA cm−2 of 230.8 mV, the Tafel slope of 32.7 mV dec−1, as well as the excellent durability in alkaline solution. Density functional theory calculations prove the established d–f electronic ladders, by the interaction between NFC and CeO2, evidently boosts the high‐speed electron transfer. Meanwhile, the stable valence state in CeO2 preserves the high electronic reactivity for OER. This work demonstrates a promising approach in fabricating a nonprecious OER electrocatalyst with the facilitation of rare‐earth oxides to reach both excellent activity and high stability. [ABSTRACT FROM AUTHOR]

Metal foams with high surface/volume ratio and excellent electrical conductivity are widely used in water splitting. Herein, we report a redox process sculpturing commercial NiFe foams with dual-scale porosities as high efficient catalysts for water oxidation reactions. Through the oxidation-reduction process, many pores of few micrometres in size were formed on a porous NiFe backbone with a pore size of 50–300 μm. The pore morphology can be reasonably controlled by varying the oxidation temperature. Electrochemical measurement demonstrates that redox-NiFe foam exhibits greatly enhanced activity towards oxygen evolution reaction. Specifically, the redox-NiFe foam oxidized at 900 °C yields the best catalytic activity with an overpotential of 294 ± 3 mV to achieve the current density of 100 mA cm−2 in 1 M KOH, which is much lower than 402 ± 2 mV of initial NiFe foam. This work highlights the formation of highly porous microstructure in the original skeleton of NiFe foam. Furthermore, the redox sculptured NiFe foams can also function as effective skeletons for the loading of active catalysts, which thus can find wide applications in electrocatalysis and energy storage. • NiFe foams with dual-scale porosities were fabricated by a redox process. • Micropore structure can be engineered by controlling oxidation temperature. • Redox-NiFe foams exhibited greatly enhanced water oxidation activity. • Redox NiFe foam showed excellent durability. [ABSTRACT FROM AUTHOR]

Interfacial engineering is an effective strategy for the design of active oxygen evolution electrode. Yet the intrinsic mechanism of heterogeneous interfaces remains largely unclear for the lack of direct evidence of real active phases. Herein, operando ultraviolet-visible (UV–vis) and Raman spectroscopies were used to probe the surface reconstruction behaviors of FeOOH@NiFe layered double hydroxides (LDH) hybrid catalysts, which revealed that FeOOH@NiFe LDH was converted into highly active FeOOH@ β-Ni(Fe)OOH phases during the OER process. The FeOOH-NiFe LDH interface can promote interfacial charge transfer, delay the Ni oxidation and induce the NiFe LDH phases to highly reactive β-Ni(Fe)OOH. The FeOOH@ β-Ni(Fe)OOH exhibited excellent OER performance (252 mV at 100 mA cm−2) and a 1.6 times increase (at overpotential of 300 mV) in turnover frequency (TOF) with respect to the active phase γ-Ni(Fe)OOH of NiFe LDH. This work clarifies that ration interface engineering can regulate the generation of highly active phases in the OER process. [Display omitted] • Reconstruction of FeOOH@NiFe LDH was study by operando UV–vis and Raman spectroscopies. • FeOOH induced the phase transformation of NiFe LDH to β-Ni(Fe)OOH at the interface. • The interfacial electric field of NiFe LDH and FeOOH promoted the charge transfer. • As-formed FeOOH@ β-Ni(Fe)OOH showed superior OER activity to γ-Ni(Fe)OOH. [ABSTRACT FROM AUTHOR]

Oxygen evolution reaction (OER) is a key step for electrochemical water splitting and understanding the surface reconstruction of OER pre-catalysts is of vital importance. Herein, hybrid Ni 5 P 4 @FeP nanosheet arrays were evaluated as promising OER pre-catalysts. The dynamic surface evolution was probed by in situ Raman spectroscopy, which revealed that Ni 5 P 4 @FeP was rapidly reconstructed to NiFe 2 O 4 during the anodic scan. The structural instability of amorphous NiFe 2 O 4 led to partial reconstitution to Ni/FeOOH at high oxidation potentials. As-formed Ni/FeOOH@NiFe 2 O 4 hybrid with high structural reversibility was established as a truly active species, which exhibited excellent alkaline OER performance with a low overpotential of 205 and 242 mV under current densities of 10 and 100 mA cm−2, respectively. This work provides a facile strategy to in situ construct an amorphous spinel/oxyhydroxide hybrid structure using electrochemical activation that holds strong promise for potential application in electrochemical water splitting and related energy devices. [Display omitted] • Surface reconstruction of Ni 5 P 4 @FeP was probed by in situ Raman spectroscopy. • Ni 5 P 4 @FeP was oxidized to NiFe 2 O 4 and further to Ni/FeOOH at high potentials. • The real active intermediate was identified as Ni/FeOOH and NiFe 2 O 4 hybrid. • High structural reversibility between NiFe 2 O 4 and Ni/FeOOH was found. • As-formed amorphous NiOOH and NiFe 2 O 4 hybrid showed superior OER activity. [ABSTRACT FROM AUTHOR]