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基于纳米酶比色传感器阵列的金作为电子库促进了二氧化铈的表面电荷重新分布,用于现场检测和鉴别含硫金属盐。

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

作者信息

Song Yang, Gu Zhongyuan, Wang Hao, Shi Xinxin, He Changchun, Li Tongxiang, Chen Yan, Li Zhao, Tian Lin

机构信息

School of Materials and Chemical Engineering, Xuzhou University of Technology, Xuzhou 221018, PR China.

School of Food (Biology) Engineering, Xuzhou University of Technology, Xuzhou 221018, PR China.

出版信息

Nanoscale. 2025 Jun 26;17(25):15214-15222. doi: 10.1039/d5nr01503k.

Abstract

Developing a highly efficient array-based sensing platform for sulfur-containing metal salt (SCM) analysis is imperious due to its potential to harm the environment and human health. Herein, we fabricated a ternary channel colorimetric sensor array technique to monitor multiple SCMs simultaneously, depending on the Au nanoparticle-loaded CeO nanobelt (Au/CeO) heterostructure with excellent peroxidase-like (POD-like) activity. The results of XPS and DFT calculations revealed that Au NPs as an electron bank can promote the charge redistribution on the surface of CeO. This process increases the ratio of Ce/Ce, facilitates the release of OH* and the desorption of HO, and significantly enhances the POD-like activity. Subsequently, colorimetry- and sensor array-based Au/CeO was developed, in integrating diverse degrees of TMB oxidation, owing to their various catalysis behaviors, leading to distinct patterns as "fingerprints" for different SCMs. The gained distinct patterns were recognized and processed 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 SCM 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 the POD-like activity of CeO through surface electron redistribution.

摘要

由于含硫金属盐(SCM)对环境和人类健康具有潜在危害,因此开发一种高效的基于阵列的传感平台用于SCM分析迫在眉睫。在此,我们构建了一种三元通道比色传感器阵列技术,用于同时监测多种SCM,该技术基于具有优异类过氧化物酶(POD-like)活性的负载金纳米颗粒的CeO纳米带(Au/CeO)异质结构。XPS和DFT计算结果表明,金纳米颗粒作为电子库可促进CeO表面的电荷重新分布。这一过程增加了Ce/Ce的比例,促进了OH*的释放和HO的解吸,并显著增强了类POD活性。随后,基于比色法和传感器阵列的Au/CeO得以开发,由于其不同的催化行为,整合了不同程度的TMB氧化,从而产生不同SCM的独特“指纹”图案。通过主成分分析(PCA)对获得的独特图案进行识别和处理,能够特异性且灵敏地识别和区分不同浓度的SCM,检测限为5 μM。为了推进对各种SCM浓度的现场测定,我们创新性地构建了一个基于便携式智能手机设备的自主传感平台,线性范围为5 - 110 μM,这进一步表明了比色传感器阵列的潜在实用性。这项工作通过表面电子重新分布增强CeO的类POD活性,为高效现场SCM检测和鉴别开辟了新途径。

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