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首页> 外文期刊>Environmental Science & Technology >Facet-Mediated Adsorption and Molecular Fractionation of Humic Substances on Hematite Surfaces
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Facet-Mediated Adsorption and Molecular Fractionation of Humic Substances on Hematite Surfaces

机译：面介导的赤铁矿表面腐殖质的吸附和分子分级

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摘要

Interactions between dissolved organic matter (DOM) and iron oxyhydroxides have important environmental and geochemical implications. The present study employed two hematite nanocrystals to investigate the adsorption and molecular fractionation of two typical humic substances (HSs) using electrospray ionization coupled with Fourier transform ion cyclotron resonance mass spectrometry (ESI-FT-ICR-MS). Hematite with a predominant exposure of {100} facets induced more pronounced adsorption and molecular fractionation of HSs than {001} facets, indicating that the interfacial adsorptive fractionation process of HSs was mediated by exposed facets of hematite. Further exploration of the surface OH groups of the two hematite nanocrystals confirms that the facet-mediated molecular fractionation of HSs was attributable to the abundance of singly iron-atom coordinated -OH sites on the hematite surfaces. Molecules with a high oxidation state and high aromaticity such as oxidized black carbon, polyphenollike, and tannic-like compounds preferentially formed ligand-exchange complexes with singly coordinated -OH groups on the hematite surfaces, inducing the selective binding and molecular fractionation of HSs at the mineral water interface. These results demonstrate that singly iron-atom coordinated -OH sites determine DOM adsorption and mediate molecular fractionation on hematite surfaces, and this contributes substantially to our understanding of the molecular mechanisms of iron oxyhydroxide-mediated molecular exchange of DOM in soils and/or sediments.
机译：溶解性有机物（DOM）和羟基氧化铁之间的相互作用具有重要的环境和地球化学意义。本研究使用两种赤铁矿纳米晶体，通过电喷雾电离和傅立叶变换离子回旋共振质谱（ESI-FT-ICR-MS）研究两种典型的腐殖质（HSs）的吸附和分子分离。与{001}晶面相比，{100}晶面主要暴露的赤铁矿诱导HS的更明显的吸附和分子分馏，这表明HS的界面吸附分馏过程是由暴露的赤铁矿晶面介导的。对两个赤铁矿纳米晶体的表面OH基团的进一步研究证实，HS的介面分子分馏可归因于赤铁矿表面上单个铁原子配位的-OH位置。具有高氧化态和高芳香性的分子（例如氧化的黑碳，多酚类和单宁类化合物）优先在赤铁矿表面上形成带有单配位-OH基团的配体交换复合物，从而诱导HS的选择性结合和分子分馏矿泉水界面。这些结果表明，单个铁原子配位的-OH位点决定DOM吸附并介导赤铁矿表面上的分子分级分离，这在很大程度上有助于我们理解羟基氧化铁介导的土壤和/或沉积物中DOM分子交换的分子机制。

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  • 来源
    《Environmental Science & Technology》 |2018年第20期|11660-11669|共10页
  • 作者

    Lv Jitao; Miao Yuexia; Huang Zaoquan; Han Ruixia; Zhang Shuzhen;

  • 作者单位

    Chinese Acad Sci, Res Ctr Ecoenvironm Sci, State Key Lab Environm Chem & Ecotoxicol, Beijing 100085, Peoples R China;

    Chinese Acad Sci, Res Ctr Ecoenvironm Sci, State Key Lab Environm Chem & Ecotoxicol, Beijing 100085, Peoples R China;

    Chinese Acad Sci, Res Ctr Ecoenvironm Sci, State Key Lab Environm Chem & Ecotoxicol, Beijing 100085, Peoples R China;

    Chinese Acad Sci, Res Ctr Ecoenvironm Sci, State Key Lab Environm Chem & Ecotoxicol, Beijing 100085, Peoples R China;

    Chinese Acad Sci, Res Ctr Ecoenvironm Sci, State Key Lab Environm Chem & Ecotoxicol, Beijing 100085, Peoples R China;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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