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Iridium–Tungsten Alloy Nanodendrites as pH-UniversalWater-Splitting Electrocatalysts

机译:通用的铱钨合金纳米枝晶分解水的电催化剂

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摘要

The development of highly efficient and durable electrocatalysts for high-performance overall water-splitting devices is crucial for clean energy conversion. However, the existing electrocatalysts still suffer from low catalytic efficiency, and need a large overpotential to drive the overall water-splitting reactions. Herein, we report an iridium–tungsten alloy with nanodendritic structure (IrW ND) as a new class of high-performance and pH-universal bifunctional electrocatalysts for hydrogen and oxygen evolution catalysis. The IrW ND catalyst presents a hydrogen generation rate ∼2 times higher than that of the commercial Pt/C catalyst in both acid and alkaline media, which is among the most active hydrogen evolution reaction (HER) catalysts yet reported. The density functional theory (DFT) calculations reveal that the high HER intrinsic catalytic activity results from the suitable hydrogen and hydroxyl binding energies, which can accelerate the rate-determining step of the HER in acid and alkaline media. Moreover, the IrW NDs show superb oxygen evolutionreaction (OER) activity and much improved stability over Ir. The theoreticalcalculation demonstrates that alloying Ir metal with W can stabilizethe formed active iridium oxide during the OER process and lower thebinding energy of reaction intermediates, thus improving the Ir corrosionresistance and OER kinetics. Furthermore, the overall water-splittingdevices driven by IrW NDs can work in a wide pH range and achievea current density of 10 mA cm–2 in acid electrolyteat a low potential of 1.48 V.
机译:用于高性能整体水分解装置的高效耐用的电催化剂的开发对于清洁能源的转化至关重要。然而,现有的电催化剂仍然遭受低催化效率的困扰,并且需要大的超电势来驱动整个水分解反应。在本文中,我们报告了具有纳米树枝状结构的铱钨合金(IrW ND),它是一类新型的可在氢和氧逸出催化中使用的高性能且具有pH值通用性的双功能电催化剂。 IrW ND催化剂在酸性和碱性介质中的产氢率均比市售Pt / C催化剂高约2倍,这是迄今报道的活性最高的析氢反应(HER)催化剂之一。密度泛函理论(DFT)计算表明,较高的HER固有催化活性是由合适的氢和羟基结合能产生的,这可以加快HER在酸和碱性介质中的速率确定步骤。此外,IrW NDs显示出极好的氧气释放反应(OER)活性并大大提高了Ir的稳定性。理论上计算表明,与钨合金化的铱金属可以稳定在OER过程中形成的活性氧化铱并降低反应中间体的结合能,从而改善Ir腐蚀阻力和OER动力学。此外,总的水分解IrW ND驱动的设备可以在很宽的pH范围内工作并达到酸性电解液中的电流密度为10 mA cm –2 在1.48 V的低电位下

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