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首页> 外文期刊>Environmental Science & Technology >Citrate Controls Fe(Ⅱ)-Catalyzed Transformation of Ferrihydrite by Complexation of the Labile Fe(Ⅲ) Intermediate
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Citrate Controls Fe(Ⅱ)-Catalyzed Transformation of Ferrihydrite by Complexation of the Labile Fe(Ⅲ) Intermediate

机译：柠檬酸盐对照Fe（Ⅱ）通过粘合粘合的铁矿石（Ⅲ）中间体络合转化Ferrihydrite

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摘要

Ferrihydrite (Fh) is generally associated with dissolved organic matter (DOM) in natural environments due to a strong sorption affinity at circumneutral pH and its high specific surface area. In suboxic conditions, aqueous Fe(Ⅱ) (Fe(Ⅱ)_(aq)) can catalyze transformation of Fh into more stable crystalline Fe(Ⅲ) phases, but how DOM influences the transformation kinetics and pathway is still unclear. Using citrate as a surrogate, we have examined Fh transformation with 1 mM Fe(Ⅱ)_(aq) and 0-60 μM citrate at pH 7.2. We focus on quantifying the time-dependent concentrations of sorbed Fe(Ⅱ), structural Fe(Ⅱ), and a key intermediate species, labile Fe(Ⅲ) (Fe(Ⅲ)_(labile)), resulting from interfacial electron transfer (IET), and how these species correlate with the evolution of lepidocrocite (Lp), magnetite (Mt), and goethite (Gt) products. Low concentrations of citrate significantly impact the proportions of Lp/Gt, and the collective results reveal that its effect is primarily through its ability to complex labile Fe(Ⅲ) and thereby disrupt polymerization into product crystallites, as opposed to modifying the surface properties of Fh or inhibiting IET. The emergence of a Mt coprecipitate is observed in the transformation experiments with 5-10 μM citrate, when the Fe(Ⅱ)/Fe(Ⅲ)_(labile) ratio onear the Fh surface is close to 0.5, the stoichiometric Fe(Ⅱ)/Fe(Ⅲ) ratio in Mt. At the molecular level, the findings suggest that citrate, and by extension DOM, can modify the relative rates of olation and oxolation reactions that assemble labile Fe(Ⅲ) into various product minerals.
机译：由于在循环pH和其高比表面积的强吸附亲和力，Ferrihydrite（FH）通常与天然环境中的溶解有机物质（DOM）相关。在中药条件下，Fe（Ⅱ）（Fe（Ⅱ）_（aq））可以将FH的转化催化为更稳定的结晶Fe（Ⅲ）阶段，但如何影响转化动力学和途径尚不清楚。使用柠檬酸盐作为替代物，我们已经检查了用1mm FE（Ⅱ）_（aq）和0-60μm柠檬酸盐在pH 7.2中的FH转化。我们专注于量化吸附含量（Ⅱ），结构Fe（Ⅱ）和关键中间物种的时间依赖性浓度，不稳定的Fe（Ⅲ）（Fe（Ⅲ）_（Labile）），由界面电子转移产生（ IET），以及这些物种如何与鳞片（LP），磁铁矿（MT）和碎石（GT）产品的演变相关。低浓度的柠檬酸盐显着影响LP / GT的比例，并且集体结果表明，其作用主要是通过其复杂不稳定Fe（Ⅲ）的能力，从而破坏了产品微晶的聚合，而不是改变FH的表面性质或抑制IET。在5-10μm柠檬酸盐的转化实验中观察到Mt共沉淀的出现，当FH表面上/近/附近的Fe（Ⅱ）/ Fe（Ⅲ）_（Labile）比率接近0.5时，化学计量计量（ Ⅱ）/ Fe（Ⅲ）比例在Mt.在分子水平下，调查结果表明，柠檬酸盐和延伸DOM可以改变将不稳定Fe（Ⅲ）组装成各种产品矿物质的橄榄油和原子化反应的相对速率。

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  • 来源
    《Environmental Science & Technology》 |2020年第12期|7309-7319|共11页
  • 作者

    Anxu Sheng; Xiaoxu Li; Yuji Arai; Yuefei Ding; Kevin M. Rosso; Juan Liu;

  • 作者单位

    The Key Laboratory of Water and Sediment Sciences College of Environmental Sciences and Engineering Peking University Beijing 100871 China;

    The Key Laboratory of Water and Sediment Sciences College of Environmental Sciences and Engineering Peking University Beijing 100871 China;

    Department of Natural Resources and Environmental Sciences University of Illinois at Urbana-Champaign Urbana Illinois 61801 United States;

    The Key Laboratory of Water and Sediment Sciences College of Environmental Sciences and Engineering Peking University Beijing 100871 China;

    Physical and Computational Sciences Directorate Pacific Northwest National Laboratory Richland Washington 99354 United States;

    The Key Laboratory of Water and Sediment Sciences College of Environmental Sciences and Engineering Peking University Beijing 100871 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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