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Chemical fractionation of a terrestrial humic acid upon sorption on alumina by high resolution mass spectrometry

机译：高分辨率质谱法对氧化铝吸附时的陆地腐殖酸的化学分馏

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摘要

Understanding the fractionation of humic acids (HA) during their sorption at mineral-solution interfaces is one of the major issues of soil and environmental sciences. Molecular-scale investigations have been conducted on the fractionation of a terrestrial HA (more precisely, of the water-soluble fraction of Aldrich HA denoted WSAHA) - rich in highly condensed aromatic compounds - during its sorption at acidic pH on alumina particles, which were taken as surrogates of Al oxide hydrates existing in soils. High-resolution mass spectrometry combined with electrospray ionization and atmospheric pressure chemical ionization was used for analysing WSAHA solutions before and after their contact with alumina. The sorption process was found to lead to enrichment of the highly reactive, acidic, oxygen-functionalized aromatic and aliphatic molecules, and of highly condensed aromatic compounds depleted in hydrogen carrying only a few oxygenated groups on the alumina surface. In contrast, the poorly oxygenated aliphatic constituents and aromatic compounds of O/C values in the range 0.2 to 0.5 remained preferentially in the solution. By comparing results obtained for homologous compounds whose elemental composition differed only by the number of CO2 groups, evidence is found that both molecular acidity and degree of molecular hydrophobicity influence the degree of sorption (via ligand exchange on the surface and hydrophobic interactions, respectively) of WSAHA compounds of highly condensed aromatic type. Evidence at the molecular scale is provided that molecular acidity and hydrophobicity are the determining factors that control the size-fractionation of WSAHA during sorption on alumina.
机译：在矿物液界面的吸附过程中了解的腐殖酸（HA）的分馏的土壤和环境科学的主要问题之一。在酸性pH下其吸附期间氧化铝粒子，这是 - 分子级的研究已在地面HA的分馏已进行（更精确地，Aldrich公司HA的水溶性级分的表示WSAHA） - 富含高度缩合的芳族化合物作为现有土壤Al氧化物水合物的替代物。高分辨率质谱与电喷雾电离和大气压化学电离组合被用于之前以及它们与氧化铝接触后，分析WSAHA解决方案。吸附过程被发现导致富集高反应性的，酸性的，氧 - 官能的芳族和脂族分子，并且在氧化铝表面上带有只有少数含氧基团中的氢贫化高度缩合芳族化合物。与此相反，该范围内的含氧脂族差成分和O / C值的芳族化合物为0.2〜0.5的溶液优选保持。通过比较用于同源化合物，其元素组成仅由CO 2基团的数目不同所获得的结果，证据发现两个分子酸度和分子的疏水性的程度影响吸附的程度（通过表面和疏水性相互作用的配体交换，分别地）的高度浓缩的芳族型的WSAHA化合物。证据在分子尺度提供了分子酸度和疏水性是在氧化铝上的吸附过程中控制WSAHA的大小分级分离的决定性因素。

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  • 来源
    《RSC Advances》 |2015年第89期|共10页
  • 作者

    Galindo Catherine; Del Nero Mirella;

  • 作者单位

    UdS CNRS Inst Pluridisciplinaire Hubert Curien UMR 7178 F-67037 Strasbourg 2 France;

    UdS CNRS Inst Pluridisciplinaire Hubert Curien UMR 7178 F-67037 Strasbourg 2 France;

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  • 正文语种 eng
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