Investigating the Ionization of Dissolved Organic Matter by Electrospray.
Investigating the Ionization of Dissolved Organic Matter by Electrospray.
复制标题
电喷雾电离溶解有机物的研究。
DOI：
10.1021/acs.analchem.0c03438
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发表时间：
2020-10-20
影响因子：
7.4
通讯作者：
Hawkes JA
中科院分区：
文献类型：
--
作者：
Patriarca C;Balderrama A;Može M;Sjöberg PJR;Bergquist J;Tranvik LJ;Hawkes JA
电喷雾离子化（ESI）负离子模式与高分辨质谱联用是目前最常用的溶解性有机物（DOM）分析技术。这种复杂混合物的巨大分子异质性和官能团多样性阻止了有机材料通过单一电离源的有效电离，因此不可避免地存在未表征的材料。这种难以电离的碳池的程度是未知的，可能在样品之间是可变的，并且只能通过分析与统一的检测方法相结合来评估。荷电气溶胶检测（CAD），其响应是成比例的非挥发性物质的量，是独立于分析物的物理化学性质，是一个合适的候选人。在这项研究中，一个富里酸混合物进行了分馏和分析，通过高压液相色谱-质谱，以调查的极性和大小分布的高度和较差的电离材料在样品中。此外，对陆地和海洋来源的DOM样品进行了分析，以评估这些池在陆地-海洋水生连续体中的变异性。相对响应因子值表明，高度电离的组分的水生DOM混合物更亲水，具有较低的分子量比电离不良的组件。此外，发现陆地和海洋来源的样品之间的差异，表明海洋样品更好地代表ESI比陆地样品，其中有一个丰富的部分疏水性差电离材料。
Electrospray ionization (ESI) operating in the negative mode coupled to high-resolution mass spectrometry is the most popular technique for the characterization of dissolved organic matter (DOM). The vast molecular heterogeneity and the functional group diversity of this complex mixture prevents the efficient ionization of the organic material by a single ionization source, so the presence of uncharacterized material is unavoidable. The extent of this poorly ionizable pool of carbon is unknown, is presumably variable between samples, and can only be assessed by the combination of analysis with a uniform detection method. Charged aerosol detection (CAD), whose response is proportional to the amount of nonvolatile material and is independent from the physicochemical properties of the analytes, is a suitable candidate. In this study, a fulvic acid mixture was fractionated and analyzed by high-pressure liquid chromatography–mass spectrometry in order to investigate the polarity and size distributions of highly and poorly ionizable material in the sample. Additionally, DOM samples of terrestrial and marine origins were analyzed to evaluate the variability of these pools across the land–sea aquatic continuum. The relative response factor values indicated that highly ionizable components of aquatic DOM mixtures are more hydrophilic and have lower molecular weight than poorly ionizable components. Additionally, a discrepancy between the samples of terrestrial and marine origins was found, indicating that marine samples are better represented by ESI than terrestrial samples, which have an abundant portion of hydrophobic poorly ionizable material.
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影响因子：
7.4
作者：
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通讯作者：
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