Abstract

In this study, introducing Fe-MOFs as reactants to the electrode surface creates a novel mode for modulating interface performance that can lead to rapid enrichment of reactants in the proximity of electrodes by electrochemical-induced confinement effect. A facile, controllable, and room temperature electrochemical approach utilizes Fe-MOFs as nanotemplates to produce porous Prussian blue (PB) nanolayers on the electrode surfaces. Unlike conventional chemical conversion that needs a supply of exogenous acid regents, the electrochemical method creates a solid acidic condition in the oxygen evolution reaction cycle to release Fe3+ from the Fe-MOFs, improving conversion efficiency and electrochemical activity of PB. Furthermore, small oxygen bubbles generated by splitting H2O near the electrodes are also good templates, promoting the formation of porous structures that can increase effective surface area and mass-transfer efficiency. As a conceptional application, using Fe-MOFs as self-sacrificial tags, an ultrasensitive electrochemical platform with triple amplification is developed to detect Pb2+ and S. aureus based on DNAzyme-CHA cascade reaction. The designed platform shows low detection limits of 8.5 fM and 1 CFU/mL for Pb2+ and S. aureus, respectively. Moreover, the platform has high selectivity, stability and reproducibility, and also shows satisfactory recovery rates when validated using actual samples.

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