Elucidating the Composition and Transformation of Dissolved Organic Matter at the Sediment–Water Interface Using High-Resolution Mass Spectrometry

IF 3.1 2区 化学 Q2 BIOCHEMICAL RESEARCH METHODS
Jinfeng Ge, Yulin Qi, Sen Xu, Wenrui Yao, Jingyi Hou, Fu-Jun Yue, Dietrich A. Volmer, Pingqing Fu, Si-Liang Li
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Abstract

The exchange and transformation of dissolved organic matter (DOM) at the sediment–water interface are crucial factors in regulating watershed biogeochemistry, with the molecular composition of DOM serving as a pivotal determinant in elucidating this process. High-resolution mass spectrometry (HRMS) is an effective tool for resolving the composition of DOM. By analyzing the compositional characteristics of DOM at the sediment–water interface under three different salinities at the same latitude region in northern China, the findings indicate certain variations in component characteristics of DOM between low-salinity inland waters and high-salinity seawaters, with the former exhibiting greater molecular diversity and higher molecular weights, whereas the latter displayed a higher saturation and bioavailability. Notably, the presence of more CHOS substances in the low-salinity inland waters underscores the transformation of the DOM influenced by terrestrial inputs and anthropogenic activities. Conversely, the presence of more CHO and CHNO substances in high-salinity seawater underscores the microbial effects. The chemical transformation process from overlying water to pore water to sediments was characterized by methylation, hydrogenation, decarboxylation, and reduction, as determined by calculating the relations between the H/C and O/C ratios of different compound types. These findings indicate that HRMS can yield more refined results in revealing the process of DOM at the sediment–water interface under different environments, which provides a more reliable basis for a deeper understanding of the source–sink mechanism of sediment organic matter.

Abstract Image

利用高分辨率质谱分析法阐明沉积物-水界面溶解有机物的组成和转化过程
沉积物-水界面溶解有机物(DOM)的交换和转化是调节流域生物地球化学的关键因素,而溶解有机物的分子组成则是阐明这一过程的关键决定因素。高分辨率质谱(HRMS)是解析 DOM 成分的有效工具。通过分析中国北方同纬度地区三种不同盐度条件下沉积物-水界面 DOM 的组成特征,结果表明低盐度内陆水域和高盐度海水中 DOM 的组成特征存在一定差异,前者表现出更大的分子多样性和更高的分子量,而后者则表现出更高的饱和度和生物利用率。值得注意的是,低盐度内陆水域中存在较多的 CHOS 物质,这说明 DOM 的转化受到陆地输入和人为活动的影响。相反,高盐度海水中存在较多的 CHO 和 CHNO 物质,这突出表明了微生物的影响。从上覆水到孔隙水再到沉积物的化学转化过程包括甲基化、氢化、脱羧和还原,通过计算不同类型化合物的 H/C 和 O/C 比值之间的关系来确定。这些研究结果表明,HRMS 在揭示不同环境下沉积物-水界面 DOM 的转化过程方面可以得出更精细的结果,为深入了解沉积物有机质的源汇机制提供了更可靠的依据。
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来源期刊
CiteScore
5.50
自引率
9.40%
发文量
257
审稿时长
1 months
期刊介绍: The Journal of the American Society for Mass Spectrometry presents research papers covering all aspects of mass spectrometry, incorporating coverage of fields of scientific inquiry in which mass spectrometry can play a role. Comprehensive in scope, the journal publishes papers on both fundamentals and applications of mass spectrometry. Fundamental subjects include instrumentation principles, design, and demonstration, structures and chemical properties of gas-phase ions, studies of thermodynamic properties, ion spectroscopy, chemical kinetics, mechanisms of ionization, theories of ion fragmentation, cluster ions, and potential energy surfaces. In addition to full papers, the journal offers Communications, Application Notes, and Accounts and Perspectives
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