Suhadolnik Luka, Bele Marjan, Čekada Miha, Jovanovič Primož, Maselj Nik, Lončar Anja, Dražić Goran, Šala Martin, Hodnik Nejc, Kovač Janez, Montini Tiziano, Melchionna Michele, Fornasiero Paolo
Department of Chemical and Pharmaceutical Sciences, CNR-ICCOM Trieste and INSTM Trieste Research Units, University of Trieste, via L. Giorgieri 1, 34127 Trieste, Italy.
Department of Materials Chemistry, National Institute of Chemistry, Hajdrihova 19, SI-1000 Ljubljana, Slovenia.
Chem Mater. 2023 Mar 9;35(6):2612-2623. doi: 10.1021/acs.chemmater.3c00125. eCollection 2023 Mar 28.
A versatile approach to the production of cluster- and single atom-based thin-film electrode composites is presented. The developed TiO N -Ir catalyst was prepared from sputtered Ti-Ir alloy constituted of 0.8 ± 0.2 at % Ir in α-Ti solid solution. The Ti-Ir solid solution on the Ti metal foil substrate was anodically oxidized to form amorphous TiO-Ir and later subjected to heat treatment in air and in ammonia to prepare the final catalyst. Detailed morphological, structural, compositional, and electrochemical characterization revealed a nanoporous film with Ir single atoms and clusters that are present throughout the entire film thickness and concentrated at the Ti/TiO N -Ir interface as a result of the anodic oxidation mechanism. The developed TiO N -Ir catalyst exhibits very high oxygen evolution reaction activity in 0.1 M HClO, reaching 1460 A g at 1.6 V vs reference hydrogen electrode. The new preparation concept of single atom- and cluster-based thin-film catalysts has wide potential applications in electrocatalysis and beyond. In the present paper, a detailed description of the new and unique method and a high-performance thin film catalyst are provided along with directions for the future development of high-performance cluster and single-atom catalysts prepared from solid solutions.
本文提出了一种制备基于团簇和单原子的薄膜电极复合材料的通用方法。所开发的TiO N -Ir催化剂由溅射的Ti-Ir合金制备而成,该合金在α-Ti固溶体中的Ir含量为0.8±0.2原子%。将Ti金属箔基底上的Ti-Ir固溶体进行阳极氧化,形成非晶态的TiO-Ir,随后在空气和氨中进行热处理,以制备最终的催化剂。详细的形态、结构、成分和电化学表征表明,该纳米多孔膜具有Ir单原子和团簇,它们存在于整个膜厚度中,并由于阳极氧化机制而集中在Ti/TiO N -Ir界面处。所开发的TiO N -Ir催化剂在0.1 M HClO中表现出非常高的析氧反应活性,相对于参比氢电极,在1.6 V时达到1460 A g 。基于单原子和团簇的薄膜催化剂的新制备概念在电催化及其他领域具有广泛的潜在应用。在本文中,详细描述了这种新颖独特的方法和一种高性能薄膜催化剂,并给出了由固溶体制备高性能团簇和单原子催化剂的未来发展方向。