Nanozyme colorimetric sensor array based Au as electron bank facilitated surface charge redistribution of CeO2 for on-site detection and discrimination of sulfur-containing metal salts

Abstract

Developing a highly efficient array-based sensing platform for sulfur-containing metal salts (SCMs) analysis is imperious due to their potential to harm the environment and human health. Herein, we fabricate a ternary channel colorimetric sensor array technique to monitor multiple SCMs simultaneously, depending on Au nanoparticles loaded CeO2 nanobelts (Au/CeO2) heterostructure with excellent peroxidase-like (POD-like) activity. The results of XPS and DFT calculation revealed that Au NPs as electron bank can promote the charge redistribution on the surface of CeO2. This process increases the ratio of Ce3+/Ce4+, facilitates the release of OH* and the desorption of H2O, and significantly enhances the POD-like activity. Subsequently, a colorimetric-based sensor array based Au/CeO2 was developed, in integrating diverse degrees of TMB oxidation owing to their various catalysis behavior, leading to distinct patterns as "fingerprints" for different SCMs. The gained distinct patterns were recognized and processed via principal component analysis (PCA), enabling specific and sensitive identification and discrimination of different concentrations of SCMs with a detection limit of 5 µM. To advance the field determination of various SCMs concentrations, we creatively constructed a portable smartphone device-based autonomous sensing platform with a linear range of 5 - 110 μM, which further indicates the potential utility of colorimetric sensor arrays. This work opens new avenues for efficient on-site SCM detection and discrimination by enhancing POD-like activity of CeO2 through surface electron redistribution.