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Pseudo-capacitive negative electrodes remain a major bottleneck in the development of supercapacitor devices with high energy density because the electric double-layer capacitance of the negative electrodes does not match the pseudocapacitance of the corresponding positive electrodes. In the present study, a strategically improved Ni-Co-Mo sulfide is demonstrated to be a promising candidate for high energy density supercapattery devices due to its sustained pseudocapacitive charge storage mechanism. The pseudocapacitive behavior is enhanced when operating under a high current through the addition of a classical Schottky junction next to the electrode–electrolyte interface using atomic layer deposition. The Schottky junction accelerates and decelerates the diffusion of OH‒/K+ ions during the charging and discharging processes, respectively, to improve the pseudocapacitive behavior. The resulting pseudocapacitive negative electrodes exhibits a specific capacity of 2,114 C g−1 at 2 A g−1 matches almost that of the positive electrode’s 2,795 C g−1 at 3 A g−1. As a result, with the equivalent contribution from the positive and negative electrodes, an energy density of 236.1 Wh kg−1 is achieved at a power density of 921.9 W kg−1 with a total active mass of 15 mg cm−2. This strategy demonstrates the possibility of producing supercapacitors that adapt well to the supercapattery zone of a Ragone plot and that are equal to batteries in terms of energy density, thus, offering a route for further advances in electrochemical energy storage and conversion processes.

The rational design and development of novel electrode materials with promising nanostructures is an effective technique to improve their supercapacitive performance. This work presents high-performance core/shell electrodes based on three-dimensional hierarchical nanostructures coated with conformal thin transition-metal oxide layers using atomic layer deposition (ALD). This effective interface engineering creates disorder in the electronic structure and coordination environment at the interface of the heteronanostructure, which provides many more reaction sites and rapid ion diffusion. At 3 A g–1, the positive CuCo2O4/Ni4Mo/MoO2@ALD-Co3O4 electrode introduced here exhibits a specific capacity of 1029.1 C g–1, and the fabricated negative Fe3O4@ALD-TiO2 electrode significantly outperforms conventional carbon-based electrodes, with a maximum specific capacity of 372.6 C g–1. The supercapattery cell assembled from these two interface- and surface-tailored electrodes exhibits a very high energy density of 110.4 W h kg–1 with exceptional capacity retention over 20,000 cycles, demonstrating the immense potential of ALD for the next generation of supercapacitors.

Multifunctional materials are highly desirable not only for energy storage and conversion devices but also for integrated self-driven water-splitting systems. In this study, we propose a facile approach for developing...

Two essential characteristics that are required for hybrid electrocatalysts to exhibit higher oxygen and hydrogen evolution reaction (OER and HER, respectively) activity are a favorable electronic configuration and a sufficient density of active sites at the interface between the two materials within the hybrid. In the present study, a hybrid electrocatalyst is introduced with a novel architecture consisting of coral‐like iron nitride (Fe2N) arrays and tungsten nitride (W2N3) nanosheets that satisfies these requirements. The resulting W2N3/Fe2N catalyst achieves high OER activity (268.5 mV at 50 mA cm−2) and HER activity (85.2 mV at 10 mA cm−2) with excellent long‐term durability in an alkaline medium. In addition, density functional theory calculations reveal that the individual band centers experience an upshift in the hybrid W2N3/Fe2N structure, thus improving the OER and HER activity. The strategy adopted here thus provides a valuable guide for the fabrication of cost‐effective multi‐metallic crystalline hybrids for use as multifunctional electrocatalysts.