Stilianos Papadopoulos Lambidis, Tilman Schramm, Karoline Steuer-Lodd, Shane Farrell, Paolo Stincone, Robin Schmid, Irina Koester, Ralph Torres, Thorsten Dittmar, Lihini Aluwihare, Carsten Simon, Daniel Petras
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引用次数: 0
摘要
溶解有机物(DOM)是一种超复杂的混合物,在全球生物地球化学循环中发挥着核心作用。尽管溶解有机物非常重要,但人们对它的分子水平仍然知之甚少。过去几十年来,人们一直在努力通过高分辨率质谱法(HR-MS)和液相色谱法(LC)结合串联质谱法(MS/MS)来破译 DOM 的化学成分。然而,DOM 的复杂性和高度非解析异构体仍然阻碍着对其进行全面的结构分析。为了应对这一挑战,我们开发了一种离线二维(2D)液相色谱法,使用两个具有正交 pH 值的反相层面,然后进行 MS/MS 数据采集和分子联网。2D-LC-MS/MS 降低了 DOM 的复杂性,提高了 MS/MS 图谱的质量并增加了光谱注释率。将我们的方法应用于分析美国南加州的沿海表层 DOM 和北太平洋中部(夏威夷)的公海 DOM,我们通过 MS/MS 图谱匹配总共注释了 600 多个结构,在总运行时间相同的情况下,比 1D LC-MS/MS 迭代分析多出 90%。我们的数据为了解海洋 DOM 的分子组成提供了前所未有的视角,并凸显了二维液相色谱-质谱/质谱方法在破译超复杂样品化学组成方面的潜力。
Two-Dimensional Liquid Chromatography Tandem Mass Spectrometry Untangles the Deep Metabolome of Marine Dissolved Organic Matter
Dissolved organic matter (DOM) is an ultracomplex mixture that plays a central role in global biogeochemical cycles. Despite its importance, DOM remains poorly understood at the molecular level. Over the last decades, significant efforts have been made to decipher the chemical composition of DOM by high-resolution mass spectrometry (HR-MS) and liquid chromatography (LC) coupled with tandem mass spectrometry (MS/MS). Yet, the complexity and high degree of nonresolved isomers still hamper the full structural analysis of DOM. To address this challenge, we developed an offline two-dimensional (2D) LC approach using two reversed-phase dimensions with orthogonal pH levels, followed by MS/MS data acquisition and molecular networking. 2D-LC-MS/MS reduced the complexity of DOM, enhancing the quality of MS/MS spectra and increasing spectral annotation rates. Applying our approach to analyze coastal-surface DOM from Southern California (USA) and open-ocean DOM from the central North Pacific (Hawaii), we annotated in total more than 600 structures via MS/MS spectrum matching, which was up to 90% more than that in iterative 1D LC-MS/MS analysis with the same total run time. Our data offer unprecedented insights into the molecular composition of marine DOM and highlight the potential of 2D-LC-MS/MS approaches to decipher the chemical composition of ultracomplex samples.
期刊介绍:
Environmental Science & Technology (ES&T) is a co-sponsored academic and technical magazine by the Hubei Provincial Environmental Protection Bureau and the Hubei Provincial Academy of Environmental Sciences.
Environmental Science & Technology (ES&T) holds the status of Chinese core journals, scientific papers source journals of China, Chinese Science Citation Database source journals, and Chinese Academic Journal Comprehensive Evaluation Database source journals. This publication focuses on the academic field of environmental protection, featuring articles related to environmental protection and technical advancements.