Probing the Structure of a Water-Oxidizing Anodic Iridium Oxide Catalyst using Raman Spectroscopy

催化作用 拉曼光谱 化学 氧化剂 氧化物 析氧 过渡金属 红外光谱学 光化学 氧气 无机化学 物理化学 电化学 光学 物理 有机化学 生物化学 电极
作者
Zoran Pavlović,Chinmoy Ranjan,Qiang Gao,Maurice van Gastel,Robert Schlögl
出处
期刊:ACS Catalysis [American Chemical Society]
卷期号:6 (12): 8098-8105 被引量:134
标识
DOI:10.1021/acscatal.6b02343
摘要

Iridium oxide is one of the most important catalysts for water oxidation. The atomic structure of this catalyst remains unknown. We have studied anodically grown iridium oxide catalyst films using Raman spectroscopy. In addition to deuteration and 18O substitution experiments, theoretical models were also constructed using density functional theory to interpret the experimental data. The material was characterized over a large potential range which included that for the oxygen evolution reaction (0.0–1.8 V). The material was found to be composed of [IrO6]n edge-sharing polyhedra (with n ≥ 3). Ir centers are connected to each other via μ-O type oxygen linkages that allow for the Ir centers to electronically couple to each other. The most intense peaks in Raman spectra were characterized by stretching movement of Ir−μ-O bonds in the basal plane of the octahedra coupled to OH bending movements of hydroxyl groups bound to the Ir centers. Oxidation of Ir3+ to Ir4+ at 0.7–1.2 V within a μ-O linked polymeric geometry results in a blue coloration of the material at high potentials. Theoretical calculations indicate that the optical transition responsible for the color is essentially an Ir to Ir charge transfer transition. The active compound that carries out oxygen evolution is resistant to further structure-directing influence of oxidation. In the course of oxidation, it was observed that IrO2 with a rutile structure could form at potentials greater than 1.2 V as a side product of the reaction.
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