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基于无热解合成的 Fe-N/C 单原子纳米酶的比色传感器阵列用于识别抗氧化剂。

Colorimetric sensor array for identifying antioxidants based on pyrolysis-free synthesis of Fe-N/C single-atom nanozymes.

机构信息

Department of Chemisty, School of Science, Xihua University, Chengdu, 610039, PR China.

Department of Chemisty, School of Science, Xihua University, Chengdu, 610039, PR China.

出版信息

Talanta. 2024 Nov 1;279:126621. doi: 10.1016/j.talanta.2024.126621. Epub 2024 Jul 29.

Abstract

Iron-anchored nitrogen/doped carbon single-atom nanozymes (Fe-N/C), which possess homogeneous active sites and adjustable catalytic environment, represent an exemplary model for investigating the structure-function relationship and catalytic activity. However, the development of pyrolysis-free synthesis technique for Fe-N/C with adjustable enzyme-mimicking activity still presents a significant challenge. Herein, Fe-N/C anchored three carrier morphologies were created via a pyrolysis-free approach by covalent organic polymers. The peroxidase-like activity of these Fe-N/C nanozymes was regulated via the pores of the anchored carrier, resulting in varying electron transfer efficiency due to disparities in contact efficacy between substrates and catalytic sites within diverse microenvironments. Additionally, a colorimetric sensor array for identifying antioxidants was developed: (1) the Fe-N/C catalytically oxidized two substrates TMB and ABTS, respectively; (2) the development of a colorimetric sensor array utilizing oxTMB and oxABTS as sensing channels enabled accurate discrimination of antioxidants such as ascorbic acid (AsA), glutathione (GSH), cysteine (Cys), gallic acid (GA), and caffeic acid (CA). Subsequently, the sensor array underwent rigorous testing to validate its performance, including assessment of antioxidant mixtures and individual antioxidants at varying concentrations, as well as target antioxidants and interfering substances. In general, the present study offered valuable insights into the active origin and rational design of nanozyme materials, and highlighting their potential applications in food analysis.

摘要

铁锚定氮/掺杂碳单原子纳米酶(Fe-N/C)具有均匀的活性位点和可调的催化环境,是研究结构-功能关系和催化活性的典型模型。然而,开发具有可调酶模拟活性的无热解合成技术仍然是一个重大挑战。本文通过共价有机聚合物的无热解法构建了三种载体形态锚定的 Fe-N/C。通过锚定载体的孔来调节这些 Fe-N/C 纳米酶的过氧化物酶样活性,由于不同微环境中底物和催化位点之间的接触效果不同,导致电子转移效率不同。此外,还开发了一种用于识别抗氧化剂的比色传感器阵列:(1)Fe-N/C 分别催化氧化两种底物 TMB 和 ABTS;(2)利用 oxTMB 和 oxABTS 作为传感通道的比色传感器阵列的开发,能够准确区分抗氧化剂,如抗坏血酸(AsA)、谷胱甘肽(GSH)、半胱氨酸(Cys)、没食子酸(GA)和咖啡酸(CA)。随后,该传感器阵列经过严格测试以验证其性能,包括评估抗氧化剂混合物和不同浓度的单个抗氧化剂,以及目标抗氧化剂和干扰物质。总的来说,本研究为纳米酶材料的活性起源和合理设计提供了有价值的见解,并强调了它们在食品分析中的潜在应用。

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