Picomolar-Level Melamine Detection via ATP Regulated CeO2 Nanorods Tunable Peroxidase-Like Nanozyme-Activity-Based Colorimetric Sensor: Logic Gate Implementation and Real Sample Analysis

Abstract

The capability of functional logic operations is highly intriguing, but far from being realized owing to limited recognition element (RE) and complex readout signals, which limit their applications. In this contribution, for a visual colorimetric sensor for melamine (MEL) we described the construction of two- and three-input AND logic gate by exploiting the intrinsic peroxidase (POD)-like activity of CeO2 nanorods (NRs) (~23.04% Ce3+ fraction and aspect ratio (RTEM) of 3.85 ± 0.18) as RE at acidic pH (4.5). Further ATP piloted catalytic tuning of POD-like activity in CeO2 NRs employed for a functional logic gate-controlled MEL sensing at neutral pH (7.4). AND logic circuit operated MEL sensing record colorimetric response time of 15 min to produce blue color proportionate to MEL concentration. The fabricated nanozyme (CeO2)-based logic gate sensor probe for MEL at pH 4.5 showed a linear response from 0.004 nM to 1.56 nM with a limit of detection (LOD) of 4 pM; while translation from acidic to neutral pH (at 7.4) sensor exhibited linear response ranging from 0.2 nM to 3.12 nM with a LOD value of 17 pM. Through CeO2 POD-like nanozyme behavior under acidic and neutral pH, the fabricated logic gate sensor showed high affinity for MEL, generating prominent visual output with picomolar sensitivity, good reproducibility, and stability with relative standard deviation (RSD) <1% and 2%, respectively. A feasibility study in real samples (raw milk and milk powder) showed good recoveries with negligible matrix effect, an anti-interference experiment revealed sensor selectivity, highlighting robust sensor practical utility. With the merits of high sensitivity, specificity, low cost, and simplified sample processing, the developed logic-controlled colorimetric MEL sensing platform with appropriate modifications can be recognized as a potent methodology for on-site analysis of various food adulterants and related applications.