Rational Design of Ultrahigh‐Loading Ir Single Atoms on Reconstructed Mn─NiOOH for Enhanced Catalytic Performance in Urea‐Water Electrolysis

Abstract Investigating advanced electrocatalysts is crucial for improving the efficacy of water splitting to generate environmentally friendly fuel. The discovery of highly effective electrocatalysts, capable of driving oxygen evolution reaction (OER) and urea oxidation reaction (UOR) in urea‐alkaline environments, is pivotal for advancing large‐scale hydrogen production. This study aims to introduce a new method that involves creating nanosheets of high‐loading iridium single atoms embedded in a manganese‐containing nickel oxyhydroxide matrix (Ir@Mn─NiOOH). These nanostructures are derived from self‐supported hydrate pre‐catalyst nanosheets grown on nickel foam and then activated through electrochemical etching pretreatment. The Ir@Mn─NiOOH nanoarchitecture displays outstanding electrocatalytic activity, having a low overpotential of just 258 mV and a potential of 1.319 V (at 10 mA cm −2 ) for OER and UOR, respectively. Such extraordinary catalytic characteristics of Ir@Mn─NiOOH is mainly owing to the strong synthetic electronic interaction between Ir single atoms and Mn─NiOOH, which can change its electronic characteristics and boost electrochemical catalytic sites. This research presents a new way to produce exceptionally efficient catalysts by adding a synergistic effect to complex multi‐electron processes.