Bipolar Electrochemiluminescence at the Water/Organic Interface

IF 7.6 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Yuheng Fu, Bingbing Xie, Miaoxia Liu, Shaojuan Hou, Qunyan Zhu, Alexander Kuhn, Lin Zhang, Wensheng Yang, Neso Sojic
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Abstract

Electrochemiluminescence (ECL) has emerged as a valuable tool for understanding multiphasic and compartmentalized systems, which have crucial wide-ranging applications across diverse fields. However, ECL reactions are limited to the vicinity of the electrode surface due to spatial constraints of electron transfer and the short lifetime of radical species, making ECL emission in bulk multiphasic solution challenging. To address this limitation, we propose a novel bipolar electrochemistry (BPE) approach for wireless dual-color ECL emission at the water/oil (w/o) interface. Firstly, amphiphilic glass carbon (GC) microbeads with distinct hydrophilic and hydrophobic regions are prepared by bipolar electrografting of hydrophobic trifluoromethyl diazonium salt, then the resulting Janus beads are positioned at the w/o interface. Subsequently, two model ECL systems containing luminol and H2O2 in the aqueous phase, and [Ru(bpy)3]²⁺ and benzoyl peroxide (BPO) in the organic phase, are selected based on their solubility to confine light-emitting reactions to their respective phases. Upon application of an electric field perpendicular to the interface, the Janus microbeads get polarized, triggering simultaneous oxidative blue ECL (425 nm) and reductive red ECL (620 nm) in the aqueous and organic phases, respectively. Taking advantage of ECL imaging, the potential gradient distribution on the GC microbead at the w/o interface is revealed, indicating a "pseudo-closed" bipolar system due to limited ion transfer between phases. We also investigate the effect of changing the electric field direction parallel to the interface, which alters the ECL emission area from a hemisphere to a quarter of the microbead's surface. This bipolar ECL approach at the w/o interface not only offers opportunities for imaging the aqueous phase and organic phase simultaneously, but also enables ECL imaging and light generation in the bulk solution, thus overcoming the usual spatial limitation requiring proximity to the electrode surface.
水/有机物界面的双极电化学发光
电化学发光(ECL)已成为了解多相系统和区隔系统的重要工具,在各个领域都有着至关重要的广泛应用。然而,由于电子传递的空间限制和自由基物种的短寿命,ECL 反应仅限于电极表面附近,这使得在大体积多相溶液中进行 ECL 发射具有挑战性。为解决这一局限性,我们提出了一种新型的双极电化学(BPE)方法,用于在水/油(w/o)界面实现无线双色 ECL 发射。首先,通过疏水性三氟甲基重氮盐的双极电接枝,制备出具有不同亲水区和疏水区的两亲玻璃碳(GC)微珠,然后将得到的 Janus 微珠置于水/油界面。随后,根据它们的溶解度选择了两个模型 ECL 系统,水相中含有发光酚和 H2O2,有机相中含有[Ru(铋)3]²⁺和过氧化苯甲酰 (BPO),以便将发光反应限制在各自的相中。当施加垂直于界面的电场时,Janus 微珠被极化,分别在水相和有机相中同时触发氧化性蓝色 ECL(425 纳米)和还原性红色 ECL(620 纳米)。利用 ECL 成像的优势,我们揭示了 GC 微珠在 w/o 界面上的电位梯度分布,这表明由于相间离子转移有限,形成了一个 "伪封闭 "双极系统。我们还研究了改变平行于界面的电场方向的效果,这将改变 ECL 发射区域,从半球形变为微珠表面的四分之一。这种在 W/o 界面上的双极 ECL 方法不仅为水相和有机相同时成像提供了机会,而且还能在大体积溶液中进行 ECL 成像和发光,从而克服了通常要求靠近电极表面的空间限制。
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来源期刊
Chemical Science
Chemical Science CHEMISTRY, MULTIDISCIPLINARY-
CiteScore
14.40
自引率
4.80%
发文量
1352
审稿时长
2.1 months
期刊介绍: Chemical Science is a journal that encompasses various disciplines within the chemical sciences. Its scope includes publishing ground-breaking research with significant implications for its respective field, as well as appealing to a wider audience in related areas. To be considered for publication, articles must showcase innovative and original advances in their field of study and be presented in a manner that is understandable to scientists from diverse backgrounds. However, the journal generally does not publish highly specialized research.
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