Oxygen Vacancy Engineering in Europia Clusters/Graphite-Like Carbon Nitride Nanostructures Induced Signal...

Oxygen vacancy is an intrinsic defect in metal oxide semiconductors and has a crucial influence on their physicochemical and electronic properties. To boost the electrochemiluminescence (ECL) efficiency of the graphite-like carbon nitride (g-C₃N₄), the wet-chemical-calcination method was developed to introduce an oxygen vacancy in Eu-doped g-C₃N₄ nanostructures for the first time. The morphology and structure characterization suggest that the Eu element was present in the matrix of the europia (Eu₂O₃) clusters. Because of the effect of oxygen vacancy promoting catalytic activity, the doping of Eu caused a great positive shift of onset potential and large signal amplification in cathodic ECL signals compared with pure g-C₃N₄. Furthermore, a novel and ultrasensitive ECL aptasensor was realized with 17β-estradiol (E2) as a prototype target by adsorption of E2 aptamer onto the Eu₂O₃-doped g-C₃N₄ (Eu₂O₃- g-C₃N₄) surface via van der Waals force. Given the specific recognition between aptamer and E2, the ECL signal decreased with the increasing concentration of E2, because the formation of E2-aptamer complex impeded the diffusion of luminophor molecules and the electrons approaching the surface of the electrode. Under the optimal cases, the as-prepared ECL aptasensor showed superior performances and also manifested outstanding selectivity toward E2. The present conceptual strategy offers a novel methodology to boost the sensitivity of the ECL sensor and promote the activity of ECL reagents.