Cascade Chromogenic System with Exponential Signal Amplification for Visual Colorimetric Detection of Acetone

The signal of the traditional chromogenic systems is directly proportional to analyte concentration, leading to an unsatisfactory sensitivity. Herein, we report a cascade chromogenic system to realize exponential amplification of colorimetric signal through coupling chemical oxidation with photoinduced radical chain reaction. The chemical oxidation of o-phenylenediamine (OPD) by Fe³⁺ generates Fe²⁺ and photoactive 2,3-diaminophenazine (DAP). Under blue-light irradiation, DAP initiates the formation of holes and H₂O₂ that reacts with Fe²⁺ to hydroxyl radicals (·OH) and Fe³⁺ via an intersystem crossing (ISC) process. Moreover, the holes oxidize water to yield ·OH as well. The resulting ·OH and regenerated Fe³⁺ in turn oxidize OPD to yield more DAP, leading to a self-propagating reaction cycle that continues to proceed until all the OPD molecules are consumed, along with a distinct color change from colorless to yellow. Through the generation of the complex between DAP and acetone that limits the ISC process, and therefore quenches the colorimetric signal, the highly sensitive and selective naked-eye detection of acetone is achieved from 50 μM to 3 mM, with a limit of detection of 35 μM. Additionally, the feasibility of this colorimetric assay to detect acetone in real water samples is also demonstrated.