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基于聚鲁米诺-金纳米复合物的无共反应物自增强固态电化学发光平台用于汞离子的信号开启检测。

Co-reactant-free self-enhanced solid-state electrochemiluminescence platform based on polyluminol-gold nanocomposite for signal-on detection of mercury ion.

机构信息

Electrodics and Electrocatalysis Division, CSIR-Central Electrochemical Research Institute (CECRI), Karaikudi, Tamil Nadu, 630003, India.

Academy of Scientific and Innovative Research (AcSIR), Ghaziabad, Uttar Pradesh, 201002, India.

出版信息

Sci Rep. 2021 Mar 25;11(1):6932. doi: 10.1038/s41598-021-86195-1.

DOI:10.1038/s41598-021-86195-1
PMID:33767245
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC7994561/
Abstract

Development of a self-enhanced solid-state ECL platform creates a straightforward experimental design for the fabrication of point-of-care applications. Herein, we develop a promising method for self-enhanced solid-state ECL platform of polyluminol gold nanocomposite on glassy carbon electrode [(PL-Au)/GCE] via simple one-step electrochemical deposition process without involving any additional co-reactants. The presence of gold nanoparticles (AuNPs) augments the electron transfer kinetics of PL (polyluminol) and enhances the solid-state ECL intensity and promotes label-free, excellent sensitivity, and selectivity to detect Hg in physiological pH through signal-on mode. Unlike pristine PL/GCE, electrochemically co-deposited AuNPs in the (PL-Au)/GCE composite, enable the co-reactant accelerator by improving the catalytic activity of PL towards oxygen reduction reaction (ORR) yielding in-situ ROS (co-reactant) generation. Further, the ECL intensity of (PL-Au)/GCE composite, gradually increases with each addition of Hg ion. This is because of the formation of an amalgamation of Au-Hg on (PL-Au)/GCE composite surface which further accelerates the yield of in-situ ROS and enhances the intensity of ECL. Whereas no ECL signals changes were observed for PL/GCE composite. The proposed self-enhanced solid-state ECL platform is selectively sensing the Hg ion in the linear range of 0.3-200 nM with a detection limit of 0.1 nM. The demonstrated (PL-Au)/GCE platform might pave new avenues for further studies in the solid-state ECL platform which could be more useful in on-site monitoring of clinical bioassay and immunosensors.

摘要

开发自增强型固态电化学发光 (ECL) 平台为制备即时检测应用创造了一种简单的实验设计。在此,我们通过简单的一步电化学沉积过程,在玻碳电极上开发了一种有前途的聚[对苯二甲酰亚胺-金纳米复合材料] (PL-Au)/GCE 的自增强型固态 ECL 平台的方法,无需涉及任何额外的共反应物。金纳米粒子 (AuNPs) 的存在增强了 PL (聚[对苯二甲酰亚胺])的电子转移动力学,并增强了固态 ECL 强度,并通过信号开启模式促进了无标记、优异的灵敏度和选择性,以在生理 pH 下检测 Hg。与原始的 PL/GCE 不同,电化学共沉积的 AuNPs 在 (PL-Au)/GCE 复合材料中作为共反应物的加速剂,通过提高 PL 对氧还原反应 (ORR) 的催化活性来产生原位 ROS (共反应物)。此外,(PL-Au)/GCE 复合材料的 ECL 强度随着每加入一个 Hg 离子而逐渐增加。这是因为在 (PL-Au)/GCE 复合材料表面形成了 Au-Hg 的汞齐,进一步加速了原位 ROS 的产生,并增强了 ECL 的强度。而对于 PL/GCE 复合材料,没有观察到 ECL 信号的变化。所提出的自增强型固态 ECL 平台能够选择性地在 0.3-200 nM 的线性范围内检测 Hg 离子,检测限为 0.1 nM。所展示的 (PL-Au)/GCE 平台可能为进一步研究固态 ECL 平台开辟新途径,这在临床生物测定和免疫传感器的现场监测中可能更有用。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0f0b/7994561/1434bd5ad751/41598_2021_86195_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0f0b/7994561/16f624237ad1/41598_2021_86195_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0f0b/7994561/bf89de68712f/41598_2021_86195_Sch1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0f0b/7994561/6e7b9bff2fbd/41598_2021_86195_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0f0b/7994561/a5ea7394d468/41598_2021_86195_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0f0b/7994561/521c68bc0ed6/41598_2021_86195_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0f0b/7994561/1434bd5ad751/41598_2021_86195_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0f0b/7994561/16f624237ad1/41598_2021_86195_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0f0b/7994561/bf89de68712f/41598_2021_86195_Sch1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0f0b/7994561/6e7b9bff2fbd/41598_2021_86195_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0f0b/7994561/a5ea7394d468/41598_2021_86195_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0f0b/7994561/521c68bc0ed6/41598_2021_86195_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0f0b/7994561/1434bd5ad751/41598_2021_86195_Fig5_HTML.jpg

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