The speciation of metals in aqueous systems is central to understanding their mobility, bioavailability, toxicity and fate. Although several geochemical speciation models exist for metals, the equilibrium conditions assumed by many of them may not prevail in field-scale hydrological systems with flowing water. Furthermore, the dominant processes and/or process rates in non-acidic systems might differ from well-studied acidic systems. We here aim to increase knowledge on geochemical processes controlling speciation and transport of metals under non-acidic river conditions. Specifically, we evaluate the predictive capacity of a speciation model to novel measurements of multiple metals and their partitioning, under high-pH conditions in mining zones within the Lake Baikal basin. The mining zones are potential hotspots for increasing metal loads to downstream river systems. Metals released from such upstream regions may be transported all the way to Lake Baikal, where increasing metal contamination of sediments and biota has been reported. Our results show clear agreement between speciation predictions and field measurements of Fe, V, Pb and Zn, suggesting that the partitioning of these metals mainly was governed by equilibrium geochemistry under the studied conditions. Systematic over-predictions of dissolved Cr, Cu and Mo by the model were observed, which might be corrected by improving the adsorption database for hydroxyapatite because that mineral likely controls the solubility of these metals. Additionally, metal complexation by dissolved organic matter is a key parameter that needs continued monitoring in the Lake Baikal basin because dependable predictions could not be made without considering its variability. Finally, our investigation indicates that further model development is needed for accurate As speciation predictions under non-acidic conditions, which is crucial for improved health risk assessments on this contaminant.
相似文献Mining has become one of the main causes of increased heavy metal loading of river systems throughout the world. There is however an evident gap between assessments of soil contamination and metal release at the mined sites and estimates of river pollution. The present work focuses on Zaamar Goldfield, which is one of the largest placer gold mines in the world, located along the Tuul River, Mongolia, which ultimately drains into Lake Baikal, Russia. It combines field observations in the river basin with soil erosion modelling and aims at quantifying the contribution from natural erosion of metal-rich soil to observed increases in mass flows of metals along the Tuul River. Results show that the sediment delivery from the mining area to the Tuul River is considerably higher than the possible contribution from natural soil erosion. This is primarily due to excessive mining-related water use creating turbid wastewaters, disturbed filtering functions of deposition areas (natural sediment traps) close to the river and disturbances from infrastructures such as roads. Furthermore, relative to background levels, soils within Zaamar Goldfield contained elevated concentrations of As, Sr, Mn,V, Ni, Cu and Cr. The enhanced soil loss caused by mining-related activities can also explain observed, considerable increases in mass flows of metals in the Tuul River. The present example from Tuul River may provide useful new insights regarding the erosion and geomorphic evolution of mined areas, as well as the associated delivery of metals into stream networks.
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