Origin of dissolved organic matter in the Harz Mountains (Germany): A thermally assisted hydrolysis and methylation (THM-GC–MS) study
Origin of dissolved organic matter in the Harz Mountains (Germany): A thermally assisted hydrolysis and methylation (THM-GC–MS) study
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哈尔茨山脉（德国）溶解有机物的起源：热辅助水解和甲基化 (THM-GCâMS) 研究
DOI：
10.1016/j.geoderma.2020.114635
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发表时间：
2020
期刊：
影响因子：
6.1
通讯作者：
Biester
中科院分区：
文献类型：
--
作者：
Nierop;Pérez-Rodríguez;Biester
环境变化正在增加北半球流域中溶解有机物 (DOM) 的浓度。本研究旨在通过热辅助水解和甲基化 (THM-GC-MS) 进行分子表征，评估哈尔茨国家公园（德国）溪流和水库中 DOM 浓度高的原因。为了制定多酚、碳水化合物、蛋白质、脂肪族大分子、树脂和其他 DOM 前体的众多 THM 产品的普遍来源的代理，我们创建了该地区潜在来源（云杉、桦树、蓝莓、石南花、泥炭藓、土壤）的参考样本集。除了固态参考样品（大块有机物；BOM）外，我们还获得并分析了它们的渗滤液（可水提取的 OM；WEOM）。最后，使用主成分分析 (PCA) 对奥得河（跨越哈尔茨泥炭和森林生物群落之间的边界）现有的 DOM THM-GC-MS 数据集进行了扩展和探索，以测试河流 DOM 评估的代理。结果显示 BOM 和 WEOM 之间存在巨大差异，这表明固体到渗滤液的转变具有高度选择性或显着改变主要生物分子成分。 WEOM 中比 BOM 中更丰富的 THM 化合物是 G 型酚类化合物（来自木质素和单宁的 1,2-二甲氧基苯）、含氮部分和苯甲酸，而 WEOM 中多糖、紫丁香基木质素和脂肪族大分子（角质和木栓质）的产物较少。 WEOM 的木质素指纹也与 BOM 显着不同，绝大多数大分子木质素的典型产物（G7、G8、G14、G15）都被耗尽，而酸部分（G6，主要来自香草酸）丰富，尤其是云杉木。奥得河森林部分的 DOM 的 THM 色谱图显示出异常丰富的 G6，最有可能来自云杉衍生的木质素。这可能表明腐烂的云杉原木和森林土壤释放的 DOM 发挥了主要作用。结果强调了使用 THM-GC-MS 进行 DOM 来源识别的潜力和缺陷。
Environmental change is increasing the concentration of dissolved organic matter (DOM) in catchments of the Northern Hemisphere. This study aims to assess the causes of high DOM concentrations in streams and reservoirs of the Harz National Park (Germany), by means of molecular characterization using thermally assisted hydrolysis and methylation (THM-GC–MS). In order to formulate proxies of the prevailing origin of the numerous THM products of polyphenols, carbohydrates, proteins, aliphatic macromolecules, resins and other DOM precursors, we created a reference sample set of potential sources (spruce, birch, blueberry, heather, peat moss, soils) from the area. Besides solid-state reference samples (bulk organic matter; BOM) we obtained and analyzed their leachates (water-extractable OM; WEOM). Finally, an existing THM-GC–MS dataset of the DOM from the Oder river, which crosses the boundary between peat and forest biomes in the Harz, was extended and explored chemometrically using Principal Component Analysis (PCA) to test the proxies for stream DOM assessment. The results show large differences between BOM and WEOM, which suggests that the solid-to-leachate transition is highly selective or significantly alters the major biomolecular constituents. THM compounds that tend to be more abundant in WEOM than in BOM are G-type phenolic compounds (1,2-dimethoxybenzenes, from lignin and tannin), nitrogen-containing moieties and benzene carboxylic acids, whereas WEOM is depleted in products of polysaccharides, syringyl lignin and aliphatic macromolecules (cutin and suberin). The lignin fingerprint of the WEOM also differs significantly from that of BOM, being depleted in the vast majority of the typical products of macromolecular lignin (G7, G8, G14, G15) and enriched in the acid moiety (G6, predominantly from vanillic acid), especially for spruce wood. THM chromatograms of DOM from the forest section of the Oder show an extraordinary abundance of G6, most probably from spruce-derived lignin. This may indicate a major role of DOM released from decaying spruce logs and forest soils. The results highlight both the potential and the pitfalls associated with source identification of DOM using THM-GC–MS.
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