Preferential Electroreduction at the Oil|Water|Conductor Interface.

Preferential Electroreduction at the Oil|Water|Conductor Interface.
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DOI:
10.1021/acs.jpclett.2c00545
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发表时间:
2022-04-21
影响因子:
5.7
通讯作者:
Dick, Jeffrey E.
Dick, Jeffrey E.
中科院分区:
化学2区
文献类型:
--
作者:
Clarke, Thomas B.;Dick, Jeffrey E.

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在有限体积内的化学反应,如水滴,不同于散装的、连续的水。然而,很少有技术可以在复杂的多相环境中探测界面反应性。在这里,我们证明了油|水|导体(三相)界面上的优先电还原。电沉积钴和镍的结果是环状结构,可以在扫描电子显微镜和能量色散x射线能谱中以几十纳米的精度进行表征。为了证明这些观察结果的普遍性,我们证明了雷扎脲电还原为荧光再间苯甲醚优先发生在三相边界,并且不强烈依赖于液滴的几何形状。我们认为我们的观察结果可以用液体|界面和界面电场的吸附来解释。这些基于三相边界反应的结果在化学和生物学的所有领域都非常重要,因为它们强调了界面如何以意想不到的方式改变化学。
Chemistry in confined volumes, such as aqueous droplets, is different from bulk, continuous water. However, few techniques are available to probe interfacial reactivity in complex, multiphase environments. Here, we demonstrate preferential electroreduction at the oil|water|conductor (three-phase) interface. Electrodeposition of cobalt and nickel results in ring-like structures that can be characterized with tens of nanometer precision in scanning electron microscopy and energy dispersive x-ray spectroscopy. To demonstrate the generalizability of these observations, we demonstrate that electroreduction of resazurin to fluorescent resorufin occurs preferentially at the three-phase boundary and does not strongly depend on droplet geometry. We suggest that our observations can be explained by adsorption to the liquid|liquid interface and the interfacial electric field. These results, grounded in three-phase boundary reactivity, are highly important across all fields of chemistry and biology because they highlight how the interface can change chemistry in unexpected ways.
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