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Interacting Effect of pH, Phosphate and Time on the Release of Arsenic from Polluted River Sediments (Anllóns River, Spain)

机译:pH,磷酸盐和时间对污染河流沉积物中砷释放的相互作用(西班牙,安利斯河)

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The interacting effect of pH, phosphate and time on the release of arsenic (As) from As-rich river bed sediments was studied. Arsenic release edges and kinetic release experiments (pH range 3–10), in the absence and presence of phosphate, coupled with sequential extraction procedures, SEM/EDX analyses and geochemical calculations, were carried out to evaluate As remobilisation and to elucidate the mechanisms involved. The results showed that As release underwent pronounced kinetic effects, which were strongly influenced by pH and phosphate. Remobilisation of As after 24 h was low (between ~1 and 5%) and varied slightly with pH, whereas alkaline conditions generally promoted As remobilisation after 168 h, with up to 12–21% of total As released. The results showed that depending on the pH and sediment considered, the release of As increased dramatically after ~48–72 h, suggesting that different processes are involved at different reaction periods. The addition of phosphate (1 mM) increased both the amount of As released (between 2 and 8 times) and the rate of As release from the sediments within the entire pH range (3–10) and period (168 h) studied. Moreover, in some cases, it also affected the shape of the As release edges and kinetic profiles. The similarities in the release profiles and the positive correlations between As and some sediment components, especially Fe and Al hydroxides, and organic matter—which appears to play a key role at high pH—suggest that As release from the studied sediments may be associated with solid phase dissolution processes under both acid and alkaline pH, whereas desorption plays a key role in the short term and at natural pH conditions, especially in the presence of phosphate, which acts as an As-displacing ligand. Evaluation of As mobility based on short-time leaching experiments may seriously underestimate the mobilisation of As from sediments.
机译:研究了pH,磷酸盐和时间对富砷河床沉积物中砷(As)释放的相互作用。在不存在磷酸盐的情况下,进行砷释放边缘和动力学释放实验(pH范围3-10),并结合顺序萃取程序,SEM / EDX分析和地球化学计算,以评估砷的迁移并阐明所涉及的机理。结果表明,As的释放具有明显的动力学效应,这受到pH和磷酸盐的强烈影响。 24小时后As的迁移率较低(约1%至5%),并且随pH值而略有变化,而碱性条件通常在168 h后促进As迁移,最多释放12-21%的As。结果表明,取决于所考虑的pH和沉积物,As的释放在〜48–72 h后急剧增加,表明在不同的反应时期涉及到不同的过程。在研究的整个pH范围(3-10)和周期(168 h)内,添加磷酸盐(1 mM)既增加了As释放量(2至8倍),又增加了As从沉积物中的释放速率。而且,在某些情况下,它还影响了As释放边缘的形状和动力学曲线。释放曲线的相似性以及砷与某些沉积物成分之间的正相关性,尤其是铁和氢氧化铝,以及有机物(在高pH下似乎起着关键作用),这表明所研究沉积物中的砷释放可能与在酸性和碱性pH值下固相溶解过程,而脱附在短期和自然pH条件下(尤其是在作为As置换配体的磷酸盐存在下)起着关键作用。基于短时浸出实验的砷迁移率评估可能严重低估了沉积物中砷的迁移。

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