High-Throughput Color Imaging Hg²⁺ Sensing via Amalgamation-Mediated Shape Transition of Concave Cube Au...

Mercury, as one type of toxic heavy metal, represents a great threat to environmental and biological metabolic systems. Thus, reliable and sensitive quantitative detection of mercury levels is particularly meaningful for environmental protection and human health. We proposed a high-throughput single-particle color imaging strategy under dark-field microscopy (DFM) for mercury ions (Hg²⁺) detection by using individual concave cube Au nanoparticles as optical probes. In the presence of ascorbic acid (AA), Hg²⁺ was reduced to Hg which forms Au-Hg amalgamate with Au nanoparticles, altering their localized surface plasmon resonance (LSPR). Transmission electron microscopy (TEM) images demonstrated that the concave cube Au nanoparticles were approaching to sphere upon increasing the concentration of Hg²⁺. The nanoparticles underwent an obvious color change from red to yellow, green, and finally blue under DFM due to the shape-evolution and LSPR changes. In addition, we demonstrated for the first time that the LSPR of Au-Hg amalgamated below 400 nm. Inspired by the above-mentioned results, single-particle color variations were digitalized by converting the color image into RGB channels to obtain (green+blue)/red intensity ratios [(G+B)/R]. The concentration-dependence change was quantified by statistically analyzing the (G+B)/R ratios of a large number of particles. A linear range from 10 to 2000 nM (R² = 0.972) and a limit of detection (LOD) of 1.857 nM were acquired. Furthermore, many other metal ions, like Cu²⁺, Cr³⁺, etc., did not interfere with Hg²⁺ detection. More importantly, Hg²⁺ content in industrial wastewater samples and in the inner regions of human HepG2 cells was determined, showing great potential for developing a single-particle color imaging sensor in complex biological samples using concave cube Au nanoparticles as optical probes.