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首页> 外文期刊>Marine Chemistry >Novel insights into the molecular structure of non-volatile marine dissolved organic sulfur
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Novel insights into the molecular structure of non-volatile marine dissolved organic sulfur

机译：非易失性海洋溶解有机硫分子结构的新颖见解

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摘要

Abiotic sulfurization likely contributes to the preservation of organic matter in fossil deposits. It is unknown whether this mechanism also stabilizes dissolved organic matter (DOM) in the oceanic water column. Knowledge of the structure of the sulfur-containing compounds in DOM could help to understand the observed stability of at least a fraction of refractory DOM in the ocean. Structural analysis of dissolved organic sulfur (DOS) is complicated by it's great molecular diversity and the low concentration of each compound. Two contrasting marine DOM samples, one deep-sea sample from the North Pacific Ocean and one surface sample from the marginal North Sea (Germany), were examined in this study. Selective alteration experiments targeting different sulfur-containing functional groups were applied prior to Fourier-transform ion cyclotron resonance mass spectrometry (FT-ICR-MS). All treatments were also carried out with corresponding model compounds, in order to test for the applicability of the chosen reactions and for matrix effects, and to confirm the types of changes caused by the treatments. Alteration experiments were composed of harsh hydrolysis, selective derivatization of thiols, oxidation, and deoxygenation. None of these treatments induced detectable changes to DOS, indicating the absence of thioesters, sulfonic acid esters, alkylsulfates, thiols, non-aromatic thioethers, and sulfoxides in solid-phase-extractable DOM (SPE-DOM). Collision-induced fragmentation of isolated nominal masses in the FT-ICR-MS confirmed these findings and revealed the presence of sulfonic acids in both samples. Additionally, the presence of thiophenes and possibly also sulfones is likely, while the presence of any other form of sulfur in SPE-DOM can be ruled out based on our results. In conclusion, only unreactive (fully oxidized and hydrolyzed) sulfur compounds resist in the water column as part of refractory DOM. There was no detectable difference in molecular structure between DOS of the marginal North Sea and the deep North Pacific, indicating that the chemical inertness and the presence of sulfonic acids are global features of DOS residing in the oxic water column.
机译：非生物硫化可能有助于保存化石沉积物中的有机物。尚不清楚该机制是否也稳定了海洋水柱中的溶解有机物（DOM）。了解DOM中含硫化合物的结构可能有助于了解海洋中至少一部分难熔DOM的稳定性。溶解性有机硫（DOS）的结构分析因其分子多样性大且每种化合物的浓度低而变得复杂。在这项研究中，检查了两个相对的海洋DOM样本，一个来自北太平洋的深海样本，另一个是来自边缘北海（德国）的地表样本。在进行傅立叶变换离子回旋共振质谱（FT-ICR-MS）之前，应用了针对不同含硫官能团的选择性改变实验。还用相应的模型化合物进行所有处理，以测试所选反应的适用性和基质效应，并确认由处理引起的变化类型。改变实验包括苛刻的水解，硫醇的选择性衍生，氧化和脱氧。这些处理均未引起DOS的可检测变化，表明在固相可萃取DOM（SPE-DOM）中不存在硫代酸酯，磺酸酯，烷基硫酸盐，硫醇，非芳族硫醚和亚砜。 FT-ICR-MS中碰撞引起的分离的标称质量碎片证实了这些发现，并揭示了两个样品中均存在磺酸。此外，根据我们的结果，可以排除噻吩以及可能还有砜的存在，同时可以排除SPE-DOM中任何其他形式的硫的存在。总之，只有不活泼的（完全氧化和水解的）硫化合物才能作为难熔DOM的一部分在水柱中抵抗。边缘北海的DOS和北太平洋深部的DOS之间的分子结构没有可检测到的差异，表明化学惰性和磺酸的存在是DOS在氧气水柱中的整体特征。

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