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Creating Highly Active Atomic Layer Deposited NiO Electrocatalysts for the Oxygen Evolution Reaction

机译：创建用于氧气析出反应的高活性原子层沉积NiO电催化剂

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摘要

Atomic layer deposition (ALD) provides a promising route for depositing uniform thin coatings of electrocatalysts useful in many technologies, including the splitting of water. For materials such as NiO x that readily form hydrous oxides, however, the smooth, compact films deposited by ALD may result in higher overpotentials due to low catalyst surface area compared to other deposition methods. Here, the use of ALD–NiO thin films as oxygen evolution reaction (OER) electrocatalysts is explored. Thin films of crystalline ALD­–NiO are deposited and OER activity is tested using cyclic voltammetry (CV). Fe incorporated from the electrolyte can increase the activity of NiO, and it is shown that the turnover frequency (TOF) increases tenfold by going from an Fe-poor to Fe-rich KOH electrolyte. Applying a potential exfoliates the NiO, increasing the number of electrochemically accessible Ni sites. Interestingly, by X-ray photoelectron spectroscopy (XPS) and CV, it is found that an Fe-rich electrolyte reduces the amount of restructuring and oxidation is found. It is shown that a high surface area, high TOF catalyst may be created by using a two-step process in which the sample is sequentially conditioned in Fe-poor then Fe-rich KOH. This work highlights the importance of pretreatment on catalytic activity for compact NiO films deposited by ALD.
机译：原子层沉积（ALD）提供了一种有前途的方法，用于沉积均匀的电催化剂薄涂层，可用于许多技术，包括水分解。但是，对于像NiO x这样易于形成水合氧化物的材料，与其他沉积方法相比，由于催化剂表面积低，通过ALD沉积的光滑致密膜可能会导致较高的超电势。在这里，探索了使用ALD-NiO薄膜作为氧释放反应（OER）电催化剂。沉积ALD­–NiO晶体薄膜，并使用循环伏安法（CV）测试OER活性。从电解质中掺入的Fe可以提高NiO的活性，并且表明通过从贫铁到富铁的KOH电解质，转换频率（TOF）增加了十倍。施加电势会使NiO剥落，从而增加电化学可访问的Ni位置的数量。有趣的是，通过X射线光电子能谱（XPS）和CV，发现富含铁的电解质减少了重组和氧化的量。结果表明，可以通过使用两步法制备高表面积，高TOF催化剂，在该过程中，先在贫铁然后富铁的KOH中依次处理样品。这项工作凸显了预处理对于由ALD沉积的致密NiO膜的催化活性的重要性。

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