Abstract

We have devised a unique strategy for highly sensitive, selective, and colorimetric detection of mercury based on analyte-induced enhancement of the photocatalytic activity of TiO2-Au nanospheres (TiO2-Au NSs) toward degradation of methylene blue (MB). Through electrostatic interactions, Au nanoparticles are attached to poly-(sodium 4-styreneulfonate)/poly(diallyldimethylammonium chloride) modified TiO2 nanoparticles, which then form an Au shell on each TiO2 core through reduction of Au3+ with ascorbic acid. Notably, the deposition of Hg species (Hg2+/CH3Hg+) onto TiO2-Au NSs through strong Au-Hg aurophilic interactions speeds up catalytic degradation of MB. The first-order degradation rates of MB by TiO2-Au NSs and TiO2-Au-Hg NSs are 1.4 × 10-2min-1 and 2.1 × 10-2min-1, respectively. Using a commercial absorption spectrometer, the TiO2-Au NSs/MB approach provides linearity (R2 = 0.98) for Hg2+ over a concentration range of 10.0 to 100.0nM, with a limit of detection (LOD) of 1.5nM. On the other hand, using a low-cost smartphone app that records the color changes (ΔRGB) of MB solution based on the red-blue-green (RGB) component values, the TiO2-Au NSs/MB approach provides an LOD of 2.0nM for Hg2+ and 5.0nM for CH3Hg+, respectively. Furthermore, the smartphone app sensing system has been validated for the analyses of various samples, including tap water, lake water, soil, and Dorm II, showing its great potential for on-line analysis of environmental and biological samples. Graphical Abstract ᅟ.

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