Knežević Sara, Totoricaguena-Gorriño Joseba, Gajjala Rajendra Kumar Reddy, Hermenegildo Bruno, Ruiz-Rubio Leire, Vilas-Vilela José Luis, Lanceros-Méndez Senentxu, Sojic Neso, Del Campo Francisco Javier
University of Bordeaux, Bordeaux INP, ISM, UMR CNRS 5255, Pessac 33607, France.
BCMaterials, Basque Center for Materials, Applications and Nanostructures, UPV/EHU Science Park, Leioa, Vizcaya 48940, Spain.
J Am Chem Soc. 2024 Aug 14;146(32):22724-22735. doi: 10.1021/jacs.4c07566. Epub 2024 Aug 1.
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.
电化学发光(ECL)通常局限于电极表面的微米级区域。本研究表明,利用电生成的氯气泡,ECL发射可延伸至距电极几毫米远的地方。使用金微电极在含氯和无氯电解质溶液中研究了这种气泡增强ECL背后的机制。我们发现,气/液界面处的ECL发射由两种平行效应驱动。首先,气泡电晕效应有助于在气泡附着于表面时生成能够氧化鲁米诺的羟基自由基。其次,由氯生成的次氯酸盐在气泡脱离后能使鲁米诺发射持续200多秒,并将发射范围扩展至溶液中5毫米深处。与传统方法相比,这种新方法可使基于鲁米诺的检测的发射强度提高5倍。通过葡萄糖生物检测证明了这一点,使用中档手机摄像头进行检测。这些发现通过在时间和空间上扩展其有效范围,显著扩大了ECL的潜在应用。