Metal-Nanoparticle-Supported Nanozyme-Based Colorimetric Sensor Array for Precise Identification of Proteins and Oral Bacteria.

Convenient, precise, and high-throughput discrimination of multiple bioanalytes is of great significance for an early diagnosis of diseases. Array-based pattern recognition has proven to be a powerful tool to detect diverse analytes, but developing sensing elements featuring favorable surface diversity still remains a challenge. In this work, we presented a simple and facile method to prepare programmable metal-nanoparticle (NP)-supported nanozymes (MNNs) as artificial receptors for the accurate identification of multiple proteins and oral bacteria. The in situ reduction of metal NPs on hierarchical MoS2 on polypyrrole (PPy), which generated differential nonspecific interactions with bioanalytes, was envisaged as the encoder to break through the limited supply of the receptor's quantity. As a proof of concept, three metal NPs, i.e., Au, Ag, and Pd NPs, were taken as examples to deposit on PPy@MoS2 as colorimetric probes to construct a cross-reactive sensor array. Based on the principal component analysis (PCA), the proposed MNN sensor array could well discriminate 11 proteins with unique fingerprint-like patterns at a concentration of 250 nM and was sufficiently sensitive to determine individual proteins with a detection limit down to the nanomolar level. Remarkably, two highly similar hemoglobins from different species (hemoglobin and bovine hemoglobin) have been precisely identified. Additionally, five oral bacteria were also well separated from each other without cross-classification at the level of 107 CFU mL-1. Furthermore, the sensor array allowed effective discrimination of complex protein mixtures either at different molar ratios or with minor varying components. Most importantly, the blind samples, proteins in human serums, proteins in simulated body fluid environment, the heat-denatured proteins, and even clinical cancer samples all could be well distinguished by the sensor array, demonstrating the real-world applications in clinical diagnosis.

Simultaneous detection of dual biomarkers using hierarchical MoS2 nanostructuring and nano-signal amplification-based electrochemical aptasensor toward accurate diagnosis of prostate cancer.

Accurate and reliable quantification of tumor biomarkers in clinical samples is of vital importance for early stage diagnosis and treatment of cancer. However, a poor specificity of prostate specific antigen (PSA) testing alone fostering overdetection and overtreatment, remains a great controversy in prostate cancer (PCa) screening. Here we report an electrochemical aptasensor using hierarchical MoS2 nanostructuring and SiO2 nano-signal amplification for simultaneous detection of dual PCa biomarkers, PSA and sarcosine, to enhance the diagnostic performance of PCa. In this strategy, hierarchical flower-like MoS2 nanostructures as functional interface accelerated intermolecular accessibility and improved DNA hybridization efficiency. Moreover, the spherical SiO2 nanoprobe that conjugated with both electroactive tags and DNA probes, allowed effective electrochemical signal amplification. By deliberately designing different hybridization modes, we individually implemented the optimization of PSA and sarcosine sensing system. Based on this, simultaneous determination of PSA and sarcosine was achieved, with limit of detection (LOD) down to 2.5 fg/mL and 14.4 fg/mL, respectively, as well as excellent selectivity. More importantly, using this approach, we could directly differentiate cancer patients with healthy ones for clinical serum samples. The ultrasensitive biosensor provides single-step analysis with simple operation and a small sample volume (∼12 µL), shedding new light on accurate diagnosis and early-detection of cancer in clinical applications.