Dye/Peroxalate Aggregated Nanoparticles with Enhanced and Tunable Chemiluminescence for Biomedical Imaging of Hydrogen Peroxide

Abstract

Hydrogen peroxide (H(2)O(2)) is an endogenous molecule that plays diverse physiological and pathological roles in living systems. Here we report multimolecule integrated nanoprobes with the enhanced chemiluminescence (CL) response to H(2)O(2) that is produced in cells and in vivo. This approach is based on the nanoscopic coaggregation of a dye exhibiting aggregation-enhanced fluorescence (AEF) with a H(2)O(2)-responsive peroxalate that can convert chemical reaction energy into electronic excitation. The coaggregated CL nanoparticles (FPOA NPs) with an average size of ~20 nm were formulated by aqueous self-assembly of a ternary mixture of a surfactant (Pluronic F-127) and concentrated hydrophobic dye/peroxalte payloads. Spectroscopic studies manifest that FPOA NPs as a reagent-concentrated nanoreactor possess the signal enhancement effect by AEF, as well as the optimized efficiencies for H(2)O(2) peroxalate reaction and subsequent intraparticle energy transfer to the dye aggregates, to yield greatly enhanced CL generation with a prolonged lifetime. It is shown that the enhanced CL signal thereby is capable of detecting intracellular H(2)O(2) overproduced during immune response. We also demonstrate that the densely integrated nature of FPOA NPs facilitates further intraparticle CL energy transfer to a low-energy dopant to red shift the spectrum toward the biologically more transparent optical window, which enables the high-sensitivity in vivo visualization of H(2)O(2) associated with early stage inflammation.

In situ diselenide-crosslinked polymeric micelles for ROS-mediated anticancer drug delivery

“…Physically self-assembled micelles with ROS-sensitive molecules such as thioketal [23], boronic ester [22], peroxylate ester [24], thioether [25], selenoether [26], and tellurium [27], have been extensively investigated for biomedical applications. However, crosslinking might be required to achieve biostability of these polymeric micelles.…”

Nanoparticles of Conjugated Molecules and Polymers for Biomedical Applications

“…12) [142]. Dye/peroxalateaggregated Pluronic nanoparticles (FPOA NPs), which were formulated with excess loading of 9,10-distyrylanthracene derivative (BLSA) and a peroxalate (CPPO), exhibited enhanced CL by the characteristic SSF of BLSA upon addition of H 2 O 2 .…”

Electrochemical K-562 cells sensor based on origami paper device for point-of-care testing

“…It is the most common representative of ROS studied in cell environments because of its stability and penetration through cell membranes. A variety of techniques, including colorimetry [17], chemiluminescence [18], fluorescence [19,20], electrochemical methods [21,22] etc., have been developed for the determination of cellular H 2 O 2 . In this paper, a lowcost, simple, portable and sensitive paper-based electrochemical sensor was developed for the detection of K-562 cells (one of the most aggressive human chronic myelogenous leukemia cell lines) based on the release of H 2 O 2 from cells on origami paper device.…”