Understanding electrocatalytic mechanisms and ultra-trace uranyl detection with Pd nanoparticles electrodeposited in deep eutectic solvents

Abstract

This research paper investigates the electrocatalytic mechanisms and ultra-trace detection abilities of uranyl ions (UO₂²⁺) using palladium nanoparticles (PdNPs) electrodeposited in deep eutectic solvents (DESs). The unique properties of DESs, such as their adjustable viscosity and ionic conductivity, offer an advantageous and environmentally friendly medium for Pd nanoparticle electrodeposition, resulting in highly active and stable electrocatalysts. Various characterization techniques, including scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), and X-ray diffraction (XRD), were used to examine the morphology, size distribution, and crystallographic structure of the Pd nanoparticles. Electrochemical tests revealed that the Pd-modified electrodes show exceptional electrocatalytic activity and current sensitivity towards uranyl ions, with detection limits as low as 3.4 nM. Density functional theory (DFT) calculations were conducted to elucidate the mechanism of the electrocatalytic reduction of UO₂²⁺ by the PdNPs, providing a plausible explanation for the high sensitivity of PdNPs in detecting uranyl ions based on the calculated structural parameters and reaction energetics. This study underscores the potential of Pd nanoparticles electrodeposited in DESs as a promising method for sensitive uranyl ion detection, contributing to advancements in environmental monitoring and nuclear safety.