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Deciphering Dissolved Organic Matter: Ionization, Dopant, and Fragmentation Insights via Fourier Transform-Ion Cyclotron Resonance Mass Spectrometry
Environmental Science & Technology ( IF 11.4 ) Pub Date : 2020-11-19 , DOI: 10.1021/acs.est.0c05206
Martin R. Kurek 1 , Brett A. Poulin 2, 3 , Amy M. McKenna 4 , Robert G. M. Spencer 1
Affiliation  

Fourier transform-ion cyclotron resonance mass spectrometry (FT-ICR MS) has been increasingly employed to characterize dissolved organic matter (DOM) across a range of aquatic environments highlighting the role of DOM in global carbon cycling. DOM analysis commonly utilizes electrospray ionization (ESI), while some have implemented other techniques, including dopant-assisted atmospheric pressure photoionization (APPI). We compared various extracted DOM compositions analyzed by negative ESI and positive APPI doped with both toluene and tetrahydrofuran (THF), including a fragmentation study of THF-doped riverine DOM using infrared multiple photon dissociation (IRMPD). DOM compositions followed the same trends in ESI and dopant-assisted APPI with the latter presenting saturated, less oxygenated, and more N-containing compounds than ESI. Between the APPI dopants, THF-doping yielded spectra with more aliphatic-like and N-containing compounds than toluene-doping. We further demonstrate how fragmentation of THF-doped DOM in APPI resolved subtle differences between riverine DOM that was absent from ESI. In both ionization methods, we describe a linear relationship between atomic and formulaic N-compositions from a range of DOM extracts. This study highlights that THF-doped APPI is useful for uncovering low-intensity aliphatic and peptide-like components in autochthonous DOM, which could aid environmental assessments of DOM across biolability gradients.

中文翻译:

解密溶解的有机物:通过傅立叶变换离子回旋加速器共振质谱法的电离,掺杂剂和碎片洞察力

傅立叶变换离子回旋共振质谱(FT-ICR MS)已被越来越多地用于表征一系列水生环境中的溶解有机物(DOM),从而突出了DOM在全球碳循环中的作用。DOM分析通常利用电喷雾电离(ESI),而有些则采用了其他技术,包括掺杂剂辅助的大气压光电离(APPI)。我们比较了通过负ESI和同时掺有甲苯和四氢呋喃(THF)的正APPI分析的各种提取的DOM组成,包括使用红外多光子离解(IRMPD)的THF掺杂河流DOM的碎裂研究。DOM组成在ESI和掺杂剂辅助的APPI中遵循相同的趋势,与ESI相比,后者呈现出饱和,含氧量少和含氮更多的化合物。在APPI掺杂剂之间,THF掺杂产生的光谱比甲苯掺杂的脂肪族类化合物和含N化合物更多。我们进一步证明了APPI中THF掺杂的DOM的片段化如何解决了ESI所缺乏的河流DOM之间的细微差异。在这两种电离方法中,我们都从一系列DOM提取物中描述了原子和分子式N组成之间的线性关系。这项研究强调,掺杂THF的APPI可用于揭示本地DOM中的低强度脂肪族和类肽成分,这可有助于在整个生物度梯度上对DOM进行环境评估。我们进一步证明了APPI中THF掺杂的DOM的片段化如何解决了ESI所缺乏的河流DOM之间的细微差异。在这两种电离方法中,我们都从一系列DOM提取物中描述了原子和分子式N组成之间的线性关系。这项研究强调,掺杂THF的APPI可用于揭示本地DOM中的低强度脂肪族和类肽成分,这可有助于在整个生物度梯度上对DOM进行环境评估。我们进一步证明了APPI中THF掺杂的DOM的片段化如何解决了ESI所缺乏的河流DOM之间的细微差异。在这两种电离方法中,我们都从一系列DOM提取物中描述了原子和分子式N组成之间的线性关系。这项研究强调,掺杂THF的APPI可用于揭示本地DOM中的低强度脂肪族和类肽成分,这可有助于在整个生物度梯度上对DOM进行环境评估。
更新日期:2020-12-15
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