Moriau Leonard, Bele Marjan, Marinko Živa, Ruiz-Zepeda Francisco, Koderman Podboršek Gorazd, Šala Martin, Šurca Angelja Kjara, Kovač Janez, Arčon Iztok, Jovanovič Primož, Hodnik Nejc, Suhadolnik Luka
Department of Materials Chemistry, National Institute of Chemistry, Hajdrihova 19, SI-1000 Ljubljana, Slovenia.
Jožef Stefan International Postgraduate School, Jamova 39, SI-1000 Ljubljana, Slovenia.
ACS Catal. 2021 Jan 15;11(2):670-681. doi: 10.1021/acscatal.0c04741. Epub 2020 Dec 30.
The development of affordable, low-iridium-loading, scalable, active, and stable catalysts for the oxygen-evolution reaction (OER) is a requirement for the commercialization of proton-exchange membrane water electrolyzers (PEMWEs). However, the synthesis of high-performance OER catalysts with minimal use of the rare and expensive element Ir is very challenging and requires the identification of electrically conductive and stable high-surface-area support materials. We developed a synthesis procedure for the production of large quantities of a nanocomposite powder containing titanium oxynitride (TiON ) and Ir. The catalysts were synthesized with an anodic oxidation process followed by detachment, milling, thermal treatment, and the deposition of Ir nanoparticles. The anodization time was varied to grow three different types of nanotubular structures exhibiting different lengths and wall thicknesses and thus a variety of properties. A comparison of milled samples with different degrees of nanotubular clustering and morphology retention, but with identical chemical compositions and Ir nanoparticle size distributions and dispersions, revealed that the nanotubular support morphology is the determining factor governing the catalyst's OER activity and stability. Our study is supported by various state-of-the-art materials' characterization techniques, like X-ray photoelectron spectroscopy, scanning and transmission electron microscopies, X-ray powder diffraction and absorption spectroscopy, and electrochemical cyclic voltammetry. Anodic oxidation proved to be a very suitable way to produce high-surface-area powder-type catalysts as the produced material greatly outperformed the IrO benchmarks as well as the Ir-supported samples on morphologically different TiON from previous studies. The highest activity was achieved for the sample prepared with 3 h of anodization, which had the most appropriate morphology for the effective removal of oxygen bubbles.
开发用于析氧反应(OER)的价格合理、低铱负载、可扩展、活性高且稳定的催化剂是质子交换膜水电解槽(PEMWE)商业化的必要条件。然而,以最少使用稀有且昂贵的元素铱来合成高性能OER催化剂极具挑战性,并且需要确定导电且稳定的高表面积载体材料。我们开发了一种合成程序,用于大量生产包含氧氮化钛(TiON)和铱的纳米复合粉末。通过阳极氧化工艺,随后进行分离、研磨、热处理以及铱纳米颗粒的沉积来合成催化剂。改变阳极氧化时间以生长出三种不同类型的纳米管结构,它们具有不同的长度和壁厚,因而具有多种性能。对具有不同程度纳米管聚集和形态保留但化学成分相同且铱纳米颗粒尺寸分布和分散情况相同的研磨样品进行比较,结果表明纳米管载体形态是决定催化剂OER活性和稳定性的因素。我们的研究得到了各种先进材料表征技术的支持,如X射线光电子能谱、扫描和透射电子显微镜、X射线粉末衍射和吸收光谱以及电化学循环伏安法。阳极氧化被证明是制备高表面积粉末型催化剂的一种非常合适的方法,因为所制备的材料在性能上大大优于IrO基准以及先前研究中在形态不同的TiON上负载铱的样品。阳极氧化3小时制备的样品具有最高活性,其形态最适合有效去除氧气气泡。