Spherical Hydrogel Sensor Based on PB@Fe-COF@Au Nanoparticles with Triplet Peroxidase-like Activity and Multiple Capture Sites for Effective Detection of Organophosphorus Pesticides

The residues of organophosphorus pesticides (OPs) have drawn worldwide increasing attention because of their potential fatal effects on human health and ecological systems. It is of great significance to develop an efficient and portable method for in-field detection of OPs. Herein, a novel core-shell nanocomposite of prussian blue@Fe-covalent organic framework@Au (PB@Fe-COF@Au) was constructed. Fe²⁺ and Fe³⁺ in PB nanoparticle (PBNP) cores, Fe-porphyrin in COF shells, and AuNPs grown on shells all acted as peroxidase-like catalytic active sites, enabling PB@Fe-COF@Au to possess triplet peroxidase-like activity. A colorimetric, affordable, sensitive, and selective strategy was designed to detect OPs. Compared with previous reports, this sensor realized a wider linear range for chlorpyrifos of 10-800 ng mL^-1 with a relatively lower detection limit of 0.61 ng mL^-1, which was attributed to the overlapping triple catalytic sites of PB@Fe-COF@Au and triple response sites to OPs. The assay was successfully employed to detect chlorpyrifos in food and environmental samples. Moreover, to meet the demand of in-field detection for OPs, a spherical hydrogel method based on PB@Fe-COF@Au with visual, portable, and equipment-free features was fabricated. This work provides a new pathway to design and apply effective nanozymes for on-site monitoring of pesticides.