Qingquan Zhang

Single Gold Nanoparticle-Based Colorimetric Detection of Picomolar Mercury Ion with Dark-Field Microscopy

Mercury severely damages the environment and human health, particularly when it accumulates in the food chain. Methods for the colorimetric detection of Hg(2+) have increasingly been developed over the past decade because of the progress in nanotechnology. However, the limits of detection (LODs) of these methods are mostly either comparable to or higher than the allowable maximum level (10 nM) in drinking water set by the US Environmental Protection Agency. In this study, we report a single Au nanoparticle (AuNP)-based colorimetric assay for Hg(2+) detection in solution. AuNPs modified with oligonucleotides were fixed on the slide. The fixed AuNPs bound to free AuNPs in the solution in the presence of Hg(2+) because of oligonucleotide hybridization. This process was accompanied by a color change from green to yellow as observed under an optical microscope. The ratio of changed color spots corresponded with Hg(2+) concentration. The LOD was determined as 1.4 pM, which may help guard against mercury accumulation. The proposed approach was applied to environmental samples with recoveries of 98.3 ± 7.7% and 110.0 ± 8.8% for Yuquan River and industrial wastewater, respectively.

Single gold nanoparticle localized surface plasmon resonance spectral imaging for quantifying binding constant of carbohydrate-protein interaction.

Quantifying carbohydrate-protein (ligand-receptor) interactions is important to understand diverse biological processes and to develop new diagnostic and therapeutic methods. We develop an approach to quantitatively study carbohydrate-protein interactions by Au nanoparticle localized surface plasmon resonance (LSPR) peak position shift at the single particles level. Unlike the previous techniques for single particle LSPR spectral imaging, only the first-order streak of an individual nanoparticle is needed to extract a LSPR spectrum, which has great potential to increase throughput to 500 single particle spectra in each frame. LSPR peak shift of protein modified single Au nanoparticles is found to be a function of its ligand concentration, which can be used to fit the binding constants of the interactions. The moderate interactions of Antithrombin III (AT III) and heparins including low molecular weight heparin (LMWH) are determined as well as the strong interaction of transferrin and antitransferrin and the weak interaction of bovine serum album (BSA) and heparin. The measured binding constants of transferrin to antitransferrin, heparin and LMWH to AT III, and BSA to heparin are (3.0 ± 0.6) × 10(9) M(-1), (3.1 ± 0.3) × 10(6) M(-1), (8.0 ± 0.5) × 10(5) M(-1), and (5.1 ± 0.1) × 10(3) M(-1), respectively, which are in good agreement with the reported values.

Sensing of hydrogen peroxide and glucose in human serum via quenching fluorescence of biomolecule-stabilized Au nanoclusters assisted by the Fenton reaction

Fe2+ can act as a catalyst to disproportionate hydrogen peroxide (H2O2) to produce extremely reactive hydroxyl radicals (˙OH) through the so-called Fenton reaction. Combining this reaction with the prominent sensitive nature of gold nanoclusters (Au NCs), we present herein a simple strategy of sensitive and rapid detection of H2O2. Compared with H2O2, the produced hydroxyl radical exhibits a much stronger oxidizing ability, and therefore could lead to a more efficient oxidation of the Au NCs and an improved sensitivity and oxidation rate. The results indicate that the detection limit for the determination of H2O2 was 0.2 μM (signal/noise = 3) and the linear range was 0.4–12 μM. Furthermore, in combination with the specific catalytic effect of glucose oxidase, the present sensing strategy can be successfully expanded to detect glucose in blood. The preliminary results are in good agreement with those provided by the hospital, which suggests the generalizability and great potential of the Au NCs/Fenton hybrid system for research and clinical diagnosis of diabetes.

A self-driven miniaturized liquid fuel cell

We present a miniaturized fuel cell driven by an evaporation pump. The prototype cell shows a net peak current density of 22 mA cm-2 and a net power density of 10.2 mW cm-2, both of which are the highest net values among passive-driven micro-fuel cells.

Viscosity based droplet size controlling in negative pressure driven droplets generator for large‐scale particle synthesis

The poor control and regulation of droplets limit the applications of negative pressure driven droplet generator (NPDDG). Here, we present a simple method to control droplet size in NPDDG via varying the oil viscosity. Depending on the infinite intersolubility of high viscous mineral oil and low viscous hexadecane, we obtain a series of oils with kinematic viscosities linearly varied from 4.2 to 194.6 mm2/s. By using these oils as continuous phases, monodisperse droplets are fabricated with controllable size in NPDDG. This viscosity‐based droplet regulation method is effective, reliable, and compatible with scale‐up processes. Compared with droplet generator driven by positive pressure, the presented method can fabricate hydrogel particles massively, without complicated multilayer chip structure and complex fluid controlling, which may extend the potential of NPDDG in droplets based high‐throughput assay or large‐scale materials synthesis.

Sensing Active Heparin by Counting Aggregated Quantum Dots at Single-Particle Level

Developing highly sensitive and highly selective assays for monitoring heparin levels in blood is required during and after surgery. In previous studies, electrostatic interactions are exploited to recognize heparin and changes in light signal intensity are used to sense heparin. In the present study, we developed a quantum dot (QD) aggregation-based detection strategy to quantify heparin. When cationic micelles and fluorescence QDs modified with anti-thrombin III (AT III) are added into heparin sample solution, the AT III-QDs, which specifically bind with heparin, aggregate around the micelles. The aggregated QDs are recorded by spectral imaging fluorescence microscopy and differentiated from single QDs based on the asynchronous process of blue shift and photobleaching. The ratio of aggregated QD spots to all counted QD spots is linearly related to the amount of heparin in the range of 4.65 × 10 -4 U/mL to 0.023 U/mL. The limit of detection is 9.3 × 10 -5 U/mL (∼0.1 nM), and the recovery of the spiked heparin at 0.00465 U/mL (∼5 nM) in 0.1% human plasma is acceptable.

A rapid and simple approach for glycoform analysis

Fast glycoform analysis is important for quality control of glycoproteins that account for over 40% of the approved biopharmaceuticals. Herein, we realized an Au nanoparticle-based lectin affinity chromatography (LAC) using simple standard laboratory equipment for fast glycoform analysis. Pisum sativum agglutinin (PA), a lectin derived from P. sativum, was covalently conjugated to Au nanoparticles via naturally formed carboxylic groups onto the surface of Au nanoparticles and amino groups of PA. Each model glycoprotein was separated into several fractions including the unbound, weakly bound, modestly bound, and strongly bound glycoforms based on affinity strength of the glycoform toward PA. A single run of Au nanoparticle-based LAC was finished within 18 min, which could be further decreased by centrifuging the mixture of the PA functionalized Au nanoparticles and the glycoproteins at a higher speed. To our knowledge, we are the first to use Au nanoparticles as LAC matrix.