Ane Etxebarria, Mauricio Lopez Luna, Andrea Martini, Uta Hejral, Martina Rüscher, Chao Zhan, Antonia Herzog, Afshan Jamshaid, David Kordus, Arno Bergmann, Helmut Kuhlenbeck, Beatriz Roldan Cuenya
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引用次数: 0
Abstract
Water splitting has emerged as a promising route for generating hydrogen as an alternative to conventional production methods. Finding affordable and scalable catalysts for the anodic half-reaction, the oxygen evolution reaction (OER), could help with its industrial widespread implementation. Iron-containing Ni-based catalysts have a competitive performance for the use in commercial alkaline electrolyzers. Due to the complexity of studying the catalysts at working conditions, the active phase and the role that iron exerts in conjunction with Ni are still a matter of investigation. Here, we study this topic with NiO(001) and Ni0.75Fe0.25Ox(001) thin film model electrocatalysts employing surface-sensitive techniques. We show that iron constrains the growth of the oxyhydroxide phase formed on top of the Ni or NiFe oxide, which is considered the active phase for the OER. Besides, operando Raman and grazing incidence X-ray absorption spectroscopy experiments reveal that the presence of iron affects both, the disorder level of the active phase and the oxidative charge around Ni during OER. The observed compositional, structural, and electronic properties of each system have been correlated with their electrochemical performance.
作为传统制氢方法的一种替代方法,水分裂已成为一种前景广阔的制氢途径。为阳极半反应--氧进化反应(OER)寻找经济实惠且可扩展的催化剂,有助于其在工业上的广泛应用。含铁的镍基催化剂在商用碱性电解槽中的使用性能极具竞争力。由于在工作条件下研究催化剂的复杂性,活性相以及铁与镍结合所发挥的作用仍是一个研究课题。在此,我们采用表面敏感技术,对 NiO(001)和 Ni0.75Fe0.25Ox(001)薄膜模型电催化剂进行了研究。我们发现,铁限制了在镍或镍铁氧化物顶部形成的氢氧化物相的生长,而氢氧化物相被认为是 OER 的活性相。此外,操作拉曼和掠入射 X 射线吸收光谱实验表明,铁的存在会影响 OER 期间活性相的无序水平和镍周围的氧化电荷。观察到的每个体系的组成、结构和电子特性都与其电化学性能相关联。
期刊介绍:
ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels.
The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.