Electronic single-molecule identification of carbohydrate isomers by recognition tunnelling.

Electronic single-molecule identification of carbohydrate isomers by recognition tunnelling.
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通过识别隧道效应对碳水化合物异构体进行电子单分子识别。

DOI:
10.1038/ncomms13868
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发表时间:
2016-12-21
影响因子:
16.6
通讯作者:
--
中科院分区:
综合性期刊1区
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碳水化合物是生命的四个主要组成部分之一,分为单糖(糖)、低聚糖和多糖。每个糖可以存在于两个不同的异构体中(其中C-1上的羟基具有不同的取向),并且每对糖可以形成不同的同分异构体(连接糖的立体中心周围的异构体)。这导致了巨大的组合复杂性,对于质谱学来说很难处理,并且需要大量的样品来进行核磁共振表征。将碰撞截面的测量与质谱仪(IM-MS)相结合是有帮助的,但许多异构体仍然很难分离。在这里,我们表明,识别隧道(RT)可以通过许多异构体和差向异构体在识别分子功能化的隧道结中捕获时产生的电流波动来分类。最重要的是,RT是一种纳米级的技术,利用亚皮摩尔量的分析物。如果整合到纳米孔中,RT将提供一种独特的方法来对线性多糖进行测序。碳水化合物是常见的生物分子,但表现出巨大的立体化学复杂性,往往无法用质谱学来解释。在这里,作者表明,识别隧道可以区分单独的立体异构体,利用皮摩尔量的分析物。
Carbohydrates are one of the four main building blocks of life, and are categorized as monosaccharides (sugars), oligosaccharides and polysaccharides. Each sugar can exist in two alternative anomers (in which a hydroxy group at C-1 takes different orientations) and each pair of sugars can form different epimers (isomers around the stereocentres connecting the sugars). This leads to a vast combinatorial complexity, intractable to mass spectrometry and requiring large amounts of sample for NMR characterization. Combining measurements of collision cross section with mass spectrometry (IM–MS) helps, but many isomers are still difficult to separate. Here, we show that recognition tunnelling (RT) can classify many anomers and epimers via the current fluctuations they produce when captured in a tunnel junction functionalized with recognition molecules. Most importantly, RT is a nanoscale technique utilizing sub-picomole quantities of analyte. If integrated into a nanopore, RT would provide a unique approach to sequencing linear polysaccharides. Carbohydrates are common biological molecules, but display huge stereochemical complexity that often cannot be elucidated by mass spectrometry. Here the authors show that recognition tunnelling can distinguish individual stereoisomers, utilizing picomole quantities of analytes.
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影响因子: 3.7
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期刊: ACS NANO
影响因子: 17.1
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