Enhanced Electrochemiluminescence at the Gas/Liquid Interface of Bubbles Propelled into Solution.

IF 14.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Journal of the American Chemical Society Pub Date : 2024-08-14 Epub Date: 2024-08-01 DOI:10.1021/jacs.4c07566
Sara Knežević, Joseba Totoricaguena-Gorriño, Rajendra Kumar Reddy Gajjala, Bruno Hermenegildo, Leire Ruiz-Rubio, José Luis Vilas-Vilela, Senentxu Lanceros-Méndez, Neso Sojic, Francisco Javier Del Campo
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Abstract

Electrochemiluminescence (ECL) is typically confined to a micrometric region from the electrode surface. This study demonstrates that ECL emission can extend up to several millimeters away from the electrode employing electrogenerated chlorine bubbles. The mechanism behind this bubble-enhanced ECL was investigated using an Au microelectrode in chloride-containing and chloride-free electrolyte solutions. We discovered that ECL emission at the gas/solution interface is driven by two parallel effects. First, the bubble corona effect facilitates the generation of hydroxyl radicals capable of oxidizing luminol while the bubble is attached to the surface. Second, hypochlorite generated from chlorine sustains luminol emission for over 200 s and extends the emission range up to 5 mm into the solution, following bubble detachment. The new approach can increase the emission intensity of luminol-based assays 5-fold compared to the conventional method. This is demonstrated through a glucose bioassay, using a midrange mobile phone camera for detection. These findings significantly expand the potential applications of ECL by extending its effective range in time and space.

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被推进溶液中的气泡在气/液界面上的增强电化学发光。
电化学发光(ECL)通常局限于电极表面的微米区域。本研究表明,利用电生氯气泡,ECL 发射可以延伸到距离电极几毫米的地方。我们在含氯和不含氯的电解质溶液中使用金微电极研究了这种气泡增强 ECL 背后的机制。我们发现,气体/溶液界面上的 ECL 发射是由两个平行效应驱动的。首先,当气泡附着在表面上时,气泡电晕效应促进了能够氧化发光酚的羟基自由基的产生。其次,在气泡脱离后,氯产生的次氯酸盐会使发光酚的发射持续 200 秒以上,并将发射范围扩大到溶液中的 5 毫米处。与传统方法相比,新方法可将基于发光酚的检测的发射强度提高 5 倍。使用中档手机摄像头进行检测的葡萄糖生物测定证明了这一点。这些发现大大扩展了 ECL 在时间和空间上的有效范围,从而拓展了其潜在的应用领域。
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来源期刊
CiteScore
24.40
自引率
6.00%
发文量
2398
审稿时长
1.6 months
期刊介绍: The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.
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