Research Center of Analytical Instrumentation, Key Laboratory of Synthetic and Natural Functional Molecule of Ministry of Education, College of Chemistry and Materials Science, Northwest University, Xi'an, 710127, People's Republic of China.
Anal Chem. 2022 Apr 12;94(14):5615-5623. doi: 10.1021/acs.analchem.1c05377. Epub 2022 Mar 30.
In recent years, semiconducting polymer dots (Pdots) as environmentally friendly and high-brightness electrochemiluminescence (ECL) nanoemitters have attracted intense attention in ECL biosensing and imaging. However, most of the available Pdots have a high ECL excitation potential in the aqueous phase (>1.0 V vs Ag/AgCl), which causes poor selectivity in actual sample detection. Therefore, it is particularly important to construct a simple and universal strategy to lower the trigger potential of Pdots. This work has realized the ECL emission of Pdots at low-trigger-potential based on the electrochemiluminescence resonance energy transfer (ERET) strategy. By covalently coupling the Pdots with a luminol analogue, -(4-aminobutyl)--ethylisoluminol (ABEI), the ABEI-Pdots showed an anodic ECL emission with a low onset potential of +0.34 V and a peak potential at +0.45 V (vs Ag/AgCl), which was the lowest trigger potential reported so far. We further explored this low-triggering-potential ECL for imaging detection of glucose in buffer and serum. By imaging the ABEI-Pdots-modified screen-printed electrodes (SPCE) at +0.45 V for 16 s, the ECL imaging method could quantify the glucose concentration in buffer from 10 to 200 μM with detection limits of 3.3 μM, while exhibiting excellent selectivity. When applied to real serum, the results of our method were highly consistent with a commercial blood glucose meter, with the relative errors ranging from 3.2 to 13%. This work provided a universal strategy for constructing low potential Pdots and demonstrated its application potential in complex biological sample analysis.
近年来,作为环保型和高光亮度电致化学发光(ECL)纳米发射器的半导体聚合物点(Pdots)在 ECL 生物传感和成像中引起了强烈关注。然而,大多数可用的 Pdots 在水相中的 ECL 激发电位较高(>1.0 V 相对于 Ag/AgCl),这导致在实际样品检测中选择性较差。因此,构建一种简单通用的策略来降低 Pdots 的触发电位尤为重要。本工作基于电化学发光共振能量转移(ERET)策略,实现了 Pdots 在低触发电位下的 ECL 发射。通过将 Pdots 与鲁米诺类似物,即 -(4-氨基丁基)-乙基异鲁米诺(ABEI)共价偶联,ABEI-Pdots 表现出具有低起始电位为 +0.34 V 和峰电位为 +0.45 V(相对于 Ag/AgCl)的阳极 ECL 发射,这是迄今为止报道的最低触发电位。我们进一步探索了这种低触发电位 ECL 用于缓冲液和血清中葡萄糖的成像检测。通过在 +0.45 V 下对 ABEI-Pdots 修饰的丝网印刷电极(SPCE)进行 16 s 的成像,ECL 成像方法可以从 10 到 200 μM 的缓冲液中定量葡萄糖浓度,检测限为 3.3 μM,同时表现出优异的选择性。当应用于实际血清时,我们方法的结果与商业血糖计高度一致,相对误差范围为 3.2 至 13%。这项工作为构建低电位 Pdots 提供了一种通用策略,并展示了其在复杂生物样品分析中的应用潜力。