Misoriented high-entropy iridium ruthenium oxide for acidic water splitting

Abstract

Designing an efficient catalyst for acidic oxygen evolution reaction (OER) is of critical importance in manipulating proton exchange membrane water electrolyzer (PEMWE) for hydrogen production. Here, we report a fast, nonequilibrium strategy to synthesize quinary high-entropy ruthenium iridium-based oxide (M-RuIrFeCoNiO₂) with abundant grain boundaries (GB), which exhibits a low overpotential of 189 millivolts at 10 milliamperes per square centimeter for OER in 0.5 M H₂SO₄. Microstructural analyses, density functional calculations, and isotope-labeled differential electrochemical mass spectroscopy measurements collectively reveal that the integration of foreign metal elements and GB is responsible for the enhancement of activity and stability of RuO₂ toward OER. A PEMWE using M-RuIrFeCoNiO₂ catalyst can steadily operate at a large current density of 1 ampere per square centimeter for over 500 hours. This work demonstrates a pathway to design high-performance OER electrocatalysts by integrating the advantages of various components and GB, which breaks the limits of thermodynamic solubility for different metal elements.