Laser-Induced Atomic Engineering Activates and Stabilizes Single and Paired Metal Sites for Efficient Electrocatalytic H₂O₂ Production

Electrochemical H2O2 production in acid is attractive for its higher product stability and direct compatibility with downstream use; however, the acidic two-electron oxygen reduction reaction (2e− ORR) is often limited by slow kinetics and poor catalyst durability. Here we report a laser-induced atomic engineering strategy that generates Pt and Pd single-atom sites as well as heteronuclear Pt-Pd dual-atom sites. The process relies on mild, spatially confined heating and avoids pyrolysis or post-synthetic treatment. Relative to untreated precursor electrodes, laser processing activates metal sites and delivers higher activity, higher H2O2 selectivity and improved stability. Structural and spectroscopic analyses confirm that the atomically dispersed oxygen coordination environment is altered compared to the metal acetylacetonate precursors (M(acac)₂) precursor; simultaneously, Pt-Pd pairing drives electron redistribution, breaking local symmetry and modulating the adsorption energy. The Pt-Pd catalyst achieves up to 94% selectivity and high mass activity, sustaining 97 mol gPGM-1 h-1 at 95% Faradaic efficiency for 24 h under bulk H2O2 electrocatalysis, surpassing the performance of most state-of-the-art benchmark catalysts. These results establish laser engineering as a practical route to stable isolated and paired noble-metal sites for decentralized acidic H2O2 electrosynthesis.