Departments of †Chemical and Biochemical Engineering and ‡Chemistry, University of Iowa , Iowa City, Iowa 52242, United States.
Environ Sci Technol. 2013 Sep 17;47(18):10312-21. doi: 10.1021/es401285s. Epub 2013 Aug 29.
Atmospheric organic acids potentially display different capacities in iron (Fe) mobilization from atmospheric dust compared with inorganic acids, but few measurements have been made on this comparison. We report here a laboratory investigation of Fe mobilization of coal fly ash, a representative Fe-containing anthropogenic aerosol, and Arizona test dust, a reference source material for mineral dust, in pH 2 sulfuric acid, acetic acid, and oxalic acid, respectively. The effects of pH and solar radiation on Fe dissolution have also been explored. The relative capacities of these three acids in Fe dissolution are in the order of oxalic acid > sulfuric acid > acetic acid. Oxalate forms mononuclear bidentate ligand with surface Fe and promotes Fe dissolution to the greatest extent. Photolysis of Fe-oxalate complexes further enhances Fe dissolution with the concomitant degradation of oxalate. These results suggest that ligand-promoted dissolution of Fe may play a more significant role in mobilizing Fe from atmospheric dust compared with proton-assisted processing. The role of atmospheric organic acids should be taken into account in global-biogeochemical modeling to better access dissolved atmospheric Fe deposition flux at the ocean surface.
大气有机酸在从大气尘埃中迁移铁(Fe)方面可能表现出与无机酸不同的能力,但对此比较的测量很少。我们在这里报告了一项实验室研究,比较了 pH 值为 2 的硫酸、乙酸和草酸中,煤飞灰(一种代表性的含 Fe 人为气溶胶)和亚利桑那州测试尘(一种矿物尘的参考源材料)中 Fe 的迁移情况。还探讨了 pH 值和太阳辐射对 Fe 溶解的影响。这三种酸溶解 Fe 的相对能力顺序为草酸>硫酸>乙酸。草酸盐与表面 Fe 形成单核双齿配体,促进 Fe 溶解的程度最大。Fe-草酸盐配合物的光解进一步增强了 Fe 的溶解,同时草酸盐的降解。这些结果表明,与质子辅助过程相比,配体促进的 Fe 溶解可能在从大气尘埃中迁移 Fe 方面发挥更重要的作用。在全球生物地球化学模型中应考虑大气有机酸的作用,以便更好地了解海洋表面溶解大气 Fe 的沉积通量。