Electrochemiluminescence Biosensor for Hyaluronidase Based on the Adjustable Electrostatic Interaction between the Surface-Charge-Controllable Nanoparticles and Negatively Charged Electrode

Abstract

A novel electrochemiluminescence (ECL) biosensor for hyaluronidase (HAase) based on the adjustable electrostatic interaction between the surface-charge-controllable nanoparticles and negatively charged electrode has been devised. Hyaluronic acid (HA)-coated amino-modified ruthenium bipyridine-doped silica nanoparticles (Ru@SiO 2 −NH 2 @HA NPs) have been synthesized and act as ECL indicators, and the surface of this particle is negatively charged because HA contains a large amount of OH− and COO−. The strong electrostatic repulsion between the Ru@ SiO 2 −NH 2 @HA NPs and negatively charged indium tin oxide (ITO) electrode surface leads to the detection of a low-intensity ECL signal. In the presence of HAase, the HA on the surface of the Ru@SiO 2 −NH 2 @HA NPs can be decomposed, and the particles can be transformed into positively charged amino-modified ruthenium bipyridine-doped silica nanoparticles (Ru@SiO 2 −NH 2 NPs), which can be concentrated near the surface of the ITO electrode through electrostatic attraction, and result in the detection of an enhanced ECL signal. The ECL of the system has a good linear relationship with HAase concentration in the range of 2.0−60 U/ mL, and the limit of detection was 0.37 U/mL. The designed biosensor had been applied to detect the target in real samples with satisfied results.

Low-Background Signal-On Homogeneous Electrochemiluminescence Biosensor for Hepatitis B Virus Detection Based on the Regulation of the Length of DNA Modified on the Nanoparticles by CRISPR/Cas12a and Hybridization Chain Reaction

“…In this study, CRISPR/Cas12a was combined with HCR amplification technology to develop a homogeneous ECL sensor, which regulates the electrostatic interaction between emitters (with variable surface charges) and negatively charged electrodes. By synthesizing ruthenium bipyridine-doped silica nanoparticles (Ru@SiO 2 NPs) with porous structures on their surface and then modifying the carefully designed nucleic acid (initiator chain) on the nanoparticles, Ru@SiO 2 can be made into a charge-controlled luminescent body . As shown in Scheme , in the presence of the target, the trans-cleavage activity of Cas12a is triggered, and the trigger DNA on the surface of the luminescent body is cleaved by Cas12a; thus, HCR amplification cannot occur.…”

“…By synthesizing ruthenium bipyridinedoped silica nanoparticles (Ru@SiO 2 NPs) with porous structures on their surface and then modifying the carefully designed nucleic acid (initiator chain) on the nanoparticles, Ru@SiO 2 can be made into a charge-controlled luminescent body. 25 As shown in Scheme 1, in the presence of the target, the trans-cleavage activity of Cas12a is triggered, and the trigger DNA on the surface of the luminescent body is cleaved by Cas12a; thus, HCR amplification cannot occur. Consequently, the electronegativity of the luminescent body is reduced, resulting in less electrostatic repulsion with the negatively charged indium tin oxide (ITO) electrode, allowing the luminescent body to approach the working electrode more easily.…”

Photocurrent Polarity Switchable Sensing of Hyaluronidase Activity by Regulating Electrostatic Interactions between Two Semiconductors

“…Through the degradation of HA, HAase can increase the permeability of the cell membrane, reduce the viscosity of the extracellular environment, and enhance the diffusion of drugs in cells . HAase is closely related to the physiological and pathological processes such as maintenance of tissue elastic viscosity, embryogenesis, inflammation, and wound healing. , Overexpression of HAase is associated with bladder, rectal, and prostate cancers, so HAase is considered as an important tumor marker. − Methods for HAase activity detection include colorimetry, viscosity, fluorescence, surface-enhanced Raman scattering, and electrochemiluminescence. − However, these methods often have the problems of expensive instruments, long analysis time, and complicated operation. Therefore, it is highly desirable to develop a simple and efficient method for detecting the HAase activity.…”

“…Electrostatic interactions, including electrostatic attraction and electrostatic repulsion, exist universally between two charged particles. Electrostatic interaction regulation has been extensively used for constructing fluorescence, electrochemiluminescence, and electrochemical biosensors. ,,− As far as we are aware, electrostatic interaction regulation has not been used for constructing photocurrent polarity switchable PEC sensors.…”

Slippery Viscosity-Sensing Platform with Time Readout for the Detection of Hyaluronidase and Its Inhibitor

“…Hence, as a potential tumor marker, the evaluation of HAase activity is crucial for the diagnosis and early therapy of cancer. Up to now, significant efforts have been made toward the development of HAase detection methods, such as turbidimetric, viscometric, colorimetric, , spectrophotometric, − electrochemiluminescence, immunoassays methods, and so on . Although these methods have been proven with various advantages for detecting HAase, they usually require time-consuming multistep preparation, expensive instruments, and the synthesis of complex molecules/nanoparticles.…”