Spatially resolved electrochemiluminescence through a chemical lens.

Spatially resolved electrochemiluminescence through a chemical lens.
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DOI:
10.1039/d0sc04210b
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发表时间:
2020-09-14
期刊:
影响因子:
8.4
通讯作者:
Valenti G
Valenti G
中科院分区:
化学1区
文献类型:
--
作者:
Fiorani A;Han D;Jiang D;Fang D;Paolucci F;Sojic N;Valenti G

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电化学发光显微镜(ECL)是一种新兴的成像技术,具有高空间分辨率、表面受限和良好的信噪比等特点,具有广泛的成像应用前景。尽管它成功地应用于分析,但调谐景深(即ECL发射层的厚度)是一个关键问题。事实上,对ECL区域厚度的控制限制了细胞显微镜和生物检测的发展,ECL区域可以被认为是一个“逝去的”反应层。在这里,我们报道了一种基于化学透镜效应来调节[Ru(Bpy)3]2+/三正丙胺(TPrA)模型体系中ECL发光层的新策略。它由装饰有[Ru(Bpy)3]2+标记的微珠组成,经典地用于生物测定,并以TPrA作为牺牲共反应物。特别是,我们利用溶液的缓冲能力来修改ECL生成中涉及的反应的速度。首次通过绘制单个微米级微珠的发光反应性图,展示了对ECL光分布的精确控制。由此得到的ECL图像是定义ECL层的扩散TPrA自由基浓度分布的发光特征。因此,我们的发现为ECL的机制提供了洞察力,并为ECL显微镜和生物检测开辟了新的途径。事实上,报道的基于化学透镜的方法控制着“逝去的”ECL发射层的空间扩展,在概念上类似于逝去的波显微镜。因此,它应该允许在衬底或细胞中进行不同高度的探测和成像。提出了一种基于化学透镜控制电化学发光(ECL)空间分布的通用机制。改变缓冲容量会改变ECL反应的速度,从而改变ECL活性层的厚度。
Electrochemiluminescence (ECL) microscopy is an emerging technique with a wide range of imaging applications and unique properties in terms of high spatial resolution, surface confinement and favourable signal-to-noise ratio. Despite its successful analytical applications, tuning the depth of field (i.e., thickness of the ECL-emitting layer) is a crucial issue. Indeed, the control of the thickness of this ECL region, which can be considered as an “evanescent” reaction layer, limits the development of cell microscopy as well as bioassays. Here we report an original strategy based on chemical lens effects to tune the ECL-emitting layer in the model [Ru(bpy)3]2+/tri-n-propylamine (TPrA) system. It consists of microbeads decorated with [Ru(bpy)3]2+ labels, classically used in bioassays, and TPrA as the sacrificial coreactant. In particular we exploit the buffer capacity of the solution to modify the rate of the reactions involved in the ECL generation. For the first time, a precise control of the ECL light distribution is demonstrated by mapping the luminescence reactivity at the level of single micrometric bead. The resulting ECL image is the luminescent signature of the concentration profiles of diffusing TPrA radicals, which define the ECL layer. Therefore, our findings provide insights into the ECL mechanism and open new avenues for ECL microscopy and bioassays. Indeed, the reported approach based on a chemical lens controls the spatial extension of the “evanescent” ECL-emitting layer and is conceptually similar to evanescent wave microscopy. Thus, it should allow the exploration and imaging of different heights in substrates or in cells. A versatile mechanism based on a chemical lens to control the electrochemiluminescence (ECL) spatial distribution is presented. Changing the buffer capacity modifies the rate of ECL reactions, and therefore the thickness of the ECL-active layer.
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