Precision Engineering for Optimizing Multi-Metallic IrRuOX Catalysts via Electronic Structure Quantification for Sustainable Hydrogen Production

Abstract

This study introduces a novel quantitative framework—the Electronic Structure Modification Index (ESMI)—for rational design and optimization of mixed metal oxide catalysts. Through controlled synthesis of IryRu1-yOx compositions (y = 0.2, 0.6, 0.7), we establish correlations between electronic structure modifications and electrocatalytic activity. Comprehensive characterization analysizes reveals that Ir0.6Ru0.4OX exhibits optimal structural and electronic properties. The ESMI, derived from XPS analysis of binding energy shifts and hydroxyl-to-lattice oxygen ratios, demonstrates perfect correlation (R2 = 0.994) with Tafel slope values, providing a predictive tool for catalyst optimization. Electrochemical measurements confirm that Ir0.6Ru0.4OX delivers high mass activity (7152.60 mA mgIr-1 at 1.6 V), outperforming benchmark catalysts. Density functional theory (DFT) calculations support experimental findings, revealing enhanced density of states near the Fermi level for the optimized composition. This work establishes ESMI as a powerful approach for predicting and enhancing the catalytic activity of mixed oxide systems, offering a pathway toward more efficient and durable OER catalysts for sustainable hydrogen production.