Highly photoluminescent silicon nanocrystals for rapid, label-free and recyclable detection of mercuric ions

摘要

Hydrothermal treatment of 3-aminopropyltrimethoxysilane (APTMS) in the presence of sodium citrate generates a suspension of highly fluorescent silicon nanocrystals that fluoresces blue under UV irradiation. The photoluminescent quantum yield of the as-prepared silicon nanocrystals was calculated to be 21.6%, with quinine sulfate as the standard reference. Only mercuric ions (Hg~(2+)) can readily prevent the fluorescence of the silicon nanocrystals, indicating a remarkably high selectivity towards Hg~(2+) over other metal ions. The optimized sensor system shows a sensitive detection range from 50 nM to 1 nM and a detection limit of 50 nM. The quenching mechanism was explained in terms of optical absorption spectra and time-resolved fluorescence decay spectra. Due to the strong interaction of Hg~(2+) with the thiol group, the fluorescence can be fully recovered by biothiols such as cysteine and glutathione, therefore, a regenerative strategy has been proposed and successfully applied to detect Hg~(2+) by the same sensor for at least five cycles. Endowed with relatively high sensitivity and selectivity, the present sensor holds the potential to be applied for mercuric assay in water.