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Micrometer-Sized Water Droplets Induce Spontaneous Reduction

机译:微米尺寸的水滴可自发减少

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摘要

Bulk water serves as an inert solvent for many chemical and biological reactions. Here, we report a striking exception. We observe that in micrometer-sized water droplets (microdroplets), spontaneous reduction of several organic molecules occurs, pyruvate to lactate, lipoic acid to dihydrolipoic acid, fumarate to succinate, and oxaloacetate to malate. This reduction proceeds in microdroplets without any added electron donors or acceptors and without any applied voltage. In three of the four cases, the reduction efficiency is 90% or greater when the concentration of the dissolved organic species is less than 0.1 mu M. None of these reactions occurs spontaneously in bulk water. One example demonstrating the possible broad application of reduction in water micro droplets to organic molecules is the reduction of acetophenone to form 1-phenylethanol. Taken together, these results show that microdroplets 'provide a new foundation for green chemistry by rendering water molecules to be highly electrochemically active without any added reducing agent or applied potential. In this manner, aqueous microdroplets might have provided a route for abiotic reduction reactions in the prebiotic era, thereby providing organic molecules with a reducing power before the advent of biotic reducing machineries.
机译:大量水可作为许多化学和生物反应的惰性溶剂。在这里,我们报告了一个惊人的例外。我们观察到,在微米大小的水滴(微滴)中,发生了几种有机分子的自发还原,丙酮酸转化为乳酸,硫辛酸转化为二氢硫辛酸,富马酸酯转化为琥珀酸酯,草酰乙酸转化为苹果酸。在没有任何添加的电子供体或受体并且没有施加任何电压的情况下,这种减少在微滴中进行。在四种情况中的三种情况下,当溶解的有机物的浓度小于0.1μM时,还原效率为90%或更高。在散装水中,这些反应都不是自发发生的。苯乙酮的还原反应生成1-苯基乙醇表明了水微滴还原法可能广泛应用于有机分子的一个例子。综上,这些结果表明,微滴通过使水分子具有高度的电化学活性而无需添加任何还原剂或施加电势,从而为绿色化学奠定了新的基础。以这种方式,水性微滴可能已经为益生元时代的非生物还原反应提供了一条途径,从而在生物还原机制出现之前为有机分子提供了还原能力。

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  • 来源
    《Journal of the American Chemical Society》 |2019年第27期|10585-10589|共5页
  • 作者单位

    Stanford Univ, Dept Chem, Stanford, CA 94305 USA;

    Stanford Univ, Dept Chem, Stanford, CA 94305 USA|Northwestern Univ, Dept Chem, 2145 Sheridan Rd, Evanston, IL 60208 USA|Northwestern Univ, Int Inst Nanotechnol, 2145 Sheridan Rd, Evanston, IL 60208 USA;

    Inst Basic Sci, Ctr Plant Aging Res, Daegu 42988, South Korea|DGIST, Dept New Biol, Daegu 42988, South Korea;

    Stanford Univ, Dept Chem, Stanford, CA 94305 USA;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
  • 原文格式 PDF
  • 正文语种 eng
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  • 入库时间 2022-08-18 04:27:56

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