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Advanced Solvent Based Methods for Molecular Characterization of Soil Organic Matter by High-Resolution Mass Spectrometry

机译:先进的基于溶剂的高分辨率有机质谱法表征土壤有机质的方法

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Soil organic matter (SOM), a complex, heterogeneous mixture of above and belowground plant litter and animal and microbial residues at various degrees of decomposition, is a key reservoir for carbon (C) and nutrient biogeochemical cycling in soil based ecosystems. A limited understanding of the molecular composition of SOM limits the ability to routinely decipher chemical processes within soil and accurately predict how terrestrial carbon fluxes will respond to changing climatic conditions and land use. To elucidate the molecular-level structure of SOM, we selectively extracted a broad range of intact SOM compounds by a combination of different organic solvents from soils with a wide range of C content. Our use of electrospray ionization (ESI) coupled with Fourier transform ion cyclotron resonance mass spectrometry (FTICR MS) and a suite of solvents with varying polarity significantly expands the inventory of the types of organic molecules present in soils. Specifically, we found that hexane is selective for lipid-like compounds with very low O/C ratios (<0.1); water (H2O) was selective for carbohydrates with high O/C ratios; acetonitrile (ACN) preferentially extracts lignin, condensed structures, and tannin polyphenolic compounds with O/C > 0.5; methanol (MeOH) has higher selectivity toward compounds characterized with low O/C < 0.5; and hexane, MeOH, ACN, and H2O solvents increase the number and types of organic molecules extracted from soil for a broader range of chemically diverse soil types. Our study of SOM molecules by ESI FTICR MS revealed new insight into the molecular-level complexity of organics contained in soils. We present the first comparative study of the molecular composition of SOM from different ecosystems using ultra high-resolution mass spectrometry.
机译:土壤有机物(SOM)是地上和地下植物凋落物以及动物和微生物残留物在不同程度分解下的复杂的异质混合物,是土壤生态系统中碳(C)和营养生物地球化学循环的重要储层。对SOM分子组成的有限了解限制了常规破译土壤中化学过程并准确预测陆地碳通量将如何响应不断变化的气候条件和土地利用的能力。为了阐明SOM的分子水平结构,我们通过从多种C含量不同的土壤中组合各种有机溶剂,选择性地提取了多种完整的SOM化合物。我们将电喷雾电离(ESI)与傅立叶变换离子回旋共振质谱(FTICR MS)结合使用,并使用一组极性不同的溶剂,可以大大增加土壤中存在的有机分子类型的数量。具体来说,我们发现己烷对O / C比率非常低(<0.1)的类脂质化合物具有选择性。水(H2O)对高O / C比的碳水化合物具有选择性;乙腈(ACN)优先提取O / C> 0.5的木质素,缩合结构和单宁多酚化合物;甲醇(MeOH)对O / C <0.5低的化合物具有更高的选择性;己烷,MeOH,ACN和H2O溶剂可增加从土壤中提取的有机分子的数量和类型,从而适用于更广泛的化学多样性土壤类型。我们通过ESI FTICR MS对SOM分子的研究揭示了对土壤中所含有机物的分子水平复杂性的新见解。我们使用超高分辨率质谱技术,对来自不同生态系统的SOM分子组成进行了首次比较研究。

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