The search for efficient oxygen evolution reaction (OER) electrocatalysts capable of high-current-density water electrolysis is critical for scalable hydrogen production. Herein, we present a rationally designed FeCo-LDH@Ni3S2 heterostructure on nickel foam (NF), synthesized through a controlled approach. This electrode delivers ultralow overpotentials of 220, 235, and 245 mV at 10 mA cm-2 in alkaline freshwater, simulated seawater, and natural seawater, respectively, alongside remarkable 100 h stability at industrial-level conditions (100 mA cm-2 in seawater). Furthermore, a symmetric electrolyzer utilizing FeCo-LDH@Ni3S2 as both cathode and anode achieves low voltages of 1.60, 1.64, and 1.69 V at 10 mA cm-2 in the corresponding electrolytes and exhibits over 100 h stability at 50 mA cm-2. Density-functional theory (DFT) analysis confirms that the FeCo-LDH@Ni3S2 heterointerface enables charge redistribution, optimizes the d-band center, and reduces the energy barrier for OER rate-determining steps. This study demonstrates an effective interface engineering strategy for d-band center reduction via heterostructure design, offering a durable electrocatalyst for marine hydrogen production.
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Heterojunction structures improve the intrinsic activity of electrocatalysts by enhancing the charge transfer between the catalyst and the electrode. In this paper, the NiS/FeS2 heterostructured electrocatalyst is fabricated by a simple sulfidation method using an interface engineering strategy to adjust the surface electron density of the electrocatalyst. As expected, NiS/FeS2 electrocatalyst exhibits superior activity and durable oxygen evolution reaction (OER) stability, requiring only a low overpotential of 183 mV to achieve a current density of 10 mA·cm−2 and can be stable for more than 80 h, superior to NiS, FeS2 electrocatalyst individually, and precious RuO2. Notably, NiS/FeS2 is also a good bifunctional electrocatalyst with good overall water splitting performance, and it only requires a voltage 1.56 V to obtain a current density of 10 mA·cm−2 for more than 12 h. Remarkably, the NiS/FeS2 hybridization facilitates the formation of coral-like structures, increasing the electrochemical surface area (ECSA) and enhancing the charge transfer efficiency, thus leading to excellent electrocatalytic performance. This work proposes a constructive strategy for designing efficient electrocatalysts based on interface engineering, and lays a foundation for designing a new class of electrocatalysts.
Electrocatalytic oxygen reduction reaction (ORR) provides an attractive alternative to anthraquinone process for H2O2 synthesis. Rational design of earth-abundant electrocatalysts for H2O2 synthesis via a two-electron ORR process in acids is attractive but still very challenging. In this work, we report that nitrogen-doped carbon nanotubes as a multi-functional support for CoSe2 nanoparticles not only keep CoSe2 nanoparticles well dispersed but alter the crystal structure, which in turn improves the overall catalytic behaviors and thereby renders high O2-to-H2O2 conversion efficiency. In 0.1 M HClO4, such CoSe2@NCNTs hybrid delivers a high H2O2 selectivity of 93.2% and a large H2O2 yield rate of 172 ppm·h−1 with excellent durability up to 24 h. Moreover, CoSe2@NCNTs performs effectively for organic dye degradation via electro-Fenton process.
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