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通过直接热解普鲁士蓝类似物来制备 FeCo 合金@N 掺杂碳层:用于化学发光葡萄糖生物传感的新型过氧化物酶模拟物。

Engineering FeCo alloy@N-doped carbon layers by directly pyrolyzing Prussian blue analogue: new peroxidase mimetic for chemiluminescence glucose biosensing.

机构信息

The Key Laboratory of Luminescence and Real-Time Analytical Chemistry, Ministry of Education, College of Chemistry and Chemical Engineering, Southwest University, Chongqing 400715, China.

出版信息

J Mater Chem B. 2019 Jul 31;7(30):4661-4668. doi: 10.1039/c9tb00797k.

Abstract

Herein, we report the synthesis of FeCo alloy@N-doped carbon layers (FeCo@NC), a new peroxidase mimetic, by directly pyrolyzing the FeIII-Co Prussian blue analogue (FeIII-Co PBA). The FeCo@NC composite showed excellent peroxidase-like activity due to its highly active FeCo alloy, M-N species (Co-N and Fe-N) and N-doped carbon layers with hierarchical pore nanostructures, which were formed via simple heat treatment of FeIII-Co PBA without additional C and N sources. In particular, the obtained FeCo@NC hybrid presented high CL activity with more than 85-fold enhancement in the CL emission of the H2O2-luminol system, and long-term stability compared with FeCo alloy nanoparticles. The CL response showed a linear range of 0.01-40 μM H2O2 with a limit of detection of 2.5 nM. When coupled with glucose oxidase, we developed a new CL sensing method for the detection of glucose in the linear range of 10 nM to 10 μM with a detection limit of 8.5 nM. This FeCo@NC-based glucose biosensor displayed rapidity, high precision and good reproducibility when utilized to analyze real biological samples. Expectedly, FeCo@NC, as a new peroxidase mimetic, exhibits great potential for monitoring glucose levels in clinical diagnosis.

摘要

在此,我们通过直接热解 FeIII-Co 普鲁士蓝类似物(FeIII-Co PBA),合成了一种新的过氧化物酶模拟物 FeCo 合金@N 掺杂碳层(FeCo@NC)。由于其具有高活性的 FeCo 合金、M-N 物种(Co-N 和 Fe-N)以及具有分级孔纳米结构的 N 掺杂碳层,FeCo@NC 复合材料表现出优异的过氧化物酶样活性,这些结构是通过简单的热处理 FeIII-Co PBA 形成的,无需额外的 C 和 N 源。特别是,所获得的 FeCo@NC 杂化材料具有很高的 CL 活性,在 H2O2-鲁米诺体系的 CL 发射中增强了 85 倍以上,并且与 FeCo 合金纳米粒子相比具有长期稳定性。CL 响应呈现出 0.01-40 μM H2O2 的线性范围,检测限为 2.5 nM。当与葡萄糖氧化酶偶联时,我们开发了一种新的 CL 传感方法,用于检测 10 nM 至 10 μM 范围内的葡萄糖,检测限为 8.5 nM。当用于分析实际生物样品时,基于 FeCo@NC 的葡萄糖生物传感器显示出快速性、高精度和良好的重现性。预计,作为一种新的过氧化物酶模拟物,FeCo@NC 在临床诊断中监测葡萄糖水平方面具有巨大潜力。

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