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首页> 外文期刊>Environmental Science & Technology >Mutual Interactions between Reduced Fe-Bearing Clay Minerals and Humic Acids under Dark, Oxygenated Conditions: Hydroxyl Radical Generation and Humic Acid Transformation
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Mutual Interactions between Reduced Fe-Bearing Clay Minerals and Humic Acids under Dark, Oxygenated Conditions: Hydroxyl Radical Generation and Humic Acid Transformation

机译：减少粘土矿物质和腐殖酸在暗，含氧条件下的相互相互作用：羟基自由基产生和腐殖酸转化

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摘要

Hydroxyl radicals (•OH) exert a strong impact on the carbon cycle due to their nonselective and highly oxidizing nature. Reduced iron-containing clay minerals (RIC) are one of the major contributors to the formation of •OH in dark environments, but their interactions with humic acids (HA) are poorly known. Here, we investigate the mutual interactions between RIC and HA under dark and oxygenated conditions. HA decreased the oxidation rate of structural Fe(Ⅱ) in RIC but significantly promoted the •OH yield. HA dissolved a fraction of Fe(Ⅱ) from RIC to form an aqueous Fe(Ⅱ)-HA complex. •OH were generated through both heterogeneous (through oxidation of structural Fe(Ⅱ)) and homogeneous pathways (through oxidation of aqueous Fe(Ⅱ)-HA species). RIC-mediated •OH production by providing H_2O_2 to react with Fe(Ⅱ)-HA and electrons to regenerate Fe(Ⅱ)-HA. This highly efficient homogeneous pathway was responsible for increased •OH yield. Abundant •OH significantly decreased the molecular size, bleached chromophores, and increased the oxygen-containing functional groups of HA. These molecular changes of HA resembled photochemical transformation of HA. The mutual interaction between RIC and HA in dark and redox-fluctuating environments provides a new pathway for fast turnover of recalcitrant organic matters in clay- and HA-rich ecosystems such as tropical forest soils and tidal marsh sediments.
机译：由于它们的非选择性和高度氧化性质，羟基自由基（•OH）对碳循环产生强烈影响。还原含铁粘土矿物（RIC）是在黑暗环境中形成的主要贡献者之一，但它们与腐殖酸（HA）的相互作用是众所周知的。在这里，我们研究了在黑暗和含氧条件下RIC和HA之间的相互相互作用。 HA在RIC中降低了结构Fe（Ⅱ）的氧化率，但显着促进了oh产量。 HA溶解来自RIC的Fe（Ⅱ）的一部分Fe（Ⅱ）以形成含水Fe（Ⅱ）-Ha复合物。 •哦是通过异质的（通过结构Fe（Ⅱ））和均相途径（通过氧化Fe（Ⅱ）-HA物种）产生的。 RIC介导•OH生产通过提供H_2O_2以与Fe（Ⅱ）-HA和电子反应再生Fe（Ⅱ）-Ha。这种高效均匀的途径负责哦产量增加。丰富•oh显着降低了分子大小，漂白发色团，并增加了含氧官能团的HA。 HA的这些分子变化类似于HA的光化学转化。 Ric和HA之间的相互相互作用在暗和氧化还原环境中提供了一种新的岩石和富含热带森林土壤和潮汐沼泽沉积物的顽固性有机物的快速营业速度的新途径。

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  • 来源
    《Environmental Science & Technology》 |2020年第23期|15013-15023|共11页
  • 作者

    Qiang Zeng; Xi Wang; Xiaolei Liu; Liuqin Huang; Jinglong Hu; Rosalie Chu; Nikola Tolic; Hailiang Dong;

  • 作者单位

    Center for Geomicrobiology and Biogeo chemistry Research State Key Laboratory of Biogeology and Environmental Geology and School of Earth Sciences and Resources China University of Geosciences Beijing 100083 China;

    Center for Geomicrobiology and Biogeochemistry Research State Key Laboratory of Biogeology and Environmental Geology and School of Earth Sciences and Resources China University of Geosciences Beijing 100083 China;

    Center for Geomicrobiology and Biogeochemistry Research State Key Laboratory of Biogeology and Environmental Geology and School of Water Resources and Environment China University of Geosciences Beijing 100083 China;

    State Key Laboratory of Biogeology and Environmental Geology China University of Geosciences Wuhan 430074 China Environmental Molecular Sciences Laboratory Pacific Northwest National Laboratory Richland Washington 99352 United States;

    Center for Geomicrobiology and Biogeochemistry Research State Key Laboratory of Biogeology and Environmental Geology and School of Earth Sciences and Resources China University of Geosciences Beijing 100083 China;

    Environmental Molecular Sciences Laboratory Pacific Northwest National Laboratory Richland Washington 99352 United States;

    Environmental Molecular Sciences Laboratory Pacific Northwest National Laboratory Richland Washington 99352 United States;

    Center for Geomicrobiology and Biogeochemistry Research State Key Laboratory of Biogeology and Environmental Geology and School of Earth Sciences and Resources China University of Geosciences Beijing 100083 China;

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