首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Ligand-Promoted Photoreductive Dissolution of Goethite by Atmospheric Low-Molecular Dicarboxylates
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Ligand-Promoted Photoreductive Dissolution of Goethite by Atmospheric Low-Molecular Dicarboxylates

机译:通过大气低分子二羧酸盐促进聚光淀粉的光电溶解

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Recent evidence suggested that organic ligands in atmosphere water play an important role in the mobilization of iron from mineral aerosol. In this study, the dissolution of goethite (alpha-FeOOH) was investigated in the presence of three low molecular dicarboxylates enriched in the atmosphere, as well as a reference organic acid of methanesulfonate (MSA), which is especially abundant in marine atmospheric boundary layer. Iron mobilized from a-FeOOH was promoted under the irradiation and the deaerated condition, and the soluble Fe(II) concentration was enhanced greatly in the ligand-containing suspensions exposed to light. Irrespective of the reaction conditions, the capacities of the dicarboxylates on Fe mobilization were in the following order: oxalate > malonate > succinate, which were closely correlated with the carbon chain length of dicarboxylates: n = 2 > 3 > 4. The space barrier action of carbon atoms inhibited ligand-promoted Fe dissolution by affecting the structure and stability of the complexes. MSA also acted as an organic ligand to mobilize iron and showed weak capacity to reduce Fe(III) under the irradiation. The reactive oxygen species (ROS) analysis indicated that OH, O-2(.) (-), and H2O2 could be involved in the Fe(II) Fe(III) redox circle, and the ligand-promoted photoreductive dissolution process could be an important source of ROS in atmosphere water. Both transmission electron microscopy analysis and zeta potential data supported that the adsorption of oxalate molecules onto the surface would change the aggregation state of goethite nanoparticles, which increased the effective surface area, and therefore facilitated Fe mobilization from the oxide. The data shown herein deepens our understanding on the ligand-promoted dissolution mechanisms, which could be an important formation pathway of bioavailable Fe in the atmosphere.
机译:最近的证据表明,大气中的水的有机配体中铁的动员从矿物气溶胶中发挥重要作用。在这项研究中,针铁矿(α-针铁矿)的溶解在大气中,以及甲磺酸盐的参考有机磺酸(MSA),它是在海洋大气边界层中特别丰富富集三个低分子量二羧酸的存在下进行了研究。铁动员从-的FeOOH在辐照和脱气条件下促进,和可溶的Fe(II)浓度是在暴露于光的含配位体的悬浮液大大增强。不管反应条件,对Fe动员二羧酸的能力是按以下顺序:草酸盐>丙二>琥珀酸盐,将其紧密地与二羧酸的碳链长度相关:N = 2> 3> 4空间阻隔作用碳原子通过影响复合物的结构和稳定性抑制配体促进的铁溶解。 MSA还作为有机配位体动员铁和呈弱能力以减少的Fe(III)的照射下。活性氧物质(ROS)分析表明,OH,O-2(。)( - ),和H 2 O 2可以参与的Fe(II)的Fe(III)氧化还原循环,和配体促进的光还原性溶解过程可以是ROS在大气中水的重要来源。两个透射电子显微镜分析和ζ电位数据支持该草酸盐分子吸附到表面上会改变针铁矿纳米颗粒,其增加的有效表面积,并因此从氧化物促进铁动员的聚集状态。本文所示的数据加深我们对配体促进的溶解机制,其可以是在大气中的生物可利用的铁的重要形成途径的了解。

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