Ambient Pulsed Laser Augmentation to Enforce the 4-Electron Pathway for the Complete Reduction of Dioxygen into Water on Dicopper Nanohybrids

Oxygen reduction reaction (ORR) plays a critical role in many electrochemical energy conversion devices including low-temperature fuel cells. However, the sluggish nature of ORR has impeded the commercialization of fuel cells with high efficiency and low costs. At present, platinum-based materials are commonly used as ORR electrocatalysts, but the high cost associated with precious metals has prompted researchers to seek alternative catalysts based on earth-abundant metals, such as copper, supported on nitrogen-doped carbon materials. In this work, we investigated the use of a dicopper complex of 3,5-diamino-1,2,4-triazole (CuDAT) as an inorganic-organic nanohybrid electrocatalyst for ORR before and after direct nanosecond pulsed laser augmentation at room temperature under an ambient atmosphere. Compared to the metal-free Vulcan carbon control, the CuDAT electrode after emission-free pulsed laser augmentation (PL-CuDAT) exhibited an increase in onset potential by 120 mV and an increase in product selectivity for H2O by approximately 58% to 97%. This study suggests that solid-to-solid pulsed laser augmentation could be an effective and green approach to improving the catalytic performance of electrocatalysts.