The protection of Lake Baikal and the planning of water management measures in the Selenga River Basin require a comprehensive understanding of the current state and functioning of the delta's ecosystem and hydrogeochemical processes. This is particularly relevant in light of recent and expected future changes involving both the hydrology and water quality in the Lake Baikal basin causing spatiotemporal changes in water flow, morphology, and transport of sediments and metals in the Selenga River delta and thus impacting on delta barrier functions. The central part of the delta had been characterized by sediment storage, especially along the main channels, causing a continuous lift of the delta surface by about 0.75 cm/year-1. Theses morphological changes have a significant impact on hydrological conditions, with historical shifts in the bulk discharge from the left to the right parts of the delta which is distinguished by a relatively high density of wetlands. Regions with a high density of wetlands and small channels, in contrast to main channel regions, show a consistent pattern of considerable contaminant filtering and removal (between 77 and 99 % for key metals), during both high-flow and low-flow conditions. The removal is associated with a significant concentration increase (2-3 times) of these substances in the bottom sediment. In consequence, geomorphological processes, which govern the partitioning of flow between different channel systems, may therefore directly govern the barrier function of the delta.

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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 nonacidic river conditions. Specifically, we evaluate the predictive capacity of a speciation model to novel measurements of multiple metals and their partitioning, under highpH 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.

Lake Baikal is the largest freshwater body on Earth, once famous for its pristine conditions. However, the lake and its drainage basin with their unique ecosystems have in recent decades been subject to both climate warming above the world average and severe anthropogenic pressures from mining and agriculture. Although previous studies have targeted various hydroclimatic, geochemical, and biological conditions of the Lake Baikal basin, the heterogeneous nature and large size of the basin leave considerable knowledge gaps regarding ongoing metal contamination of the basin’s suspended sediments and waters. To address these knowledge gaps, the main objectives of this study are to (i) determine regional background values for water and suspended sediment quality with respect to multiple metals (representing undisturbed conditions) and (ii) further evaluate spatio-temporal concentration patterns of these metals, including regions with heavy anthropogenic impacts. We synthesize data from extensive field measurements within the Selenga River basin performed between 2011 and 2016, covering over 100 sampling locations. Results show that although the background metal concentrations (of both dissolved and suspended metal forms) in the alkaline Selenga River waters were close to the world averages, metal concentrations of up to two orders of magnitude above the background values were seen for Zn, As, Cd, Cu, Mo, and Pb in regions subject to anthropogenic impacts (cities and the mining industry). Specifically, dissolved As levels within the Selenga River basin were 2–5 times higher than the world average and well above the global guideline value in several regions. Notable hotspots for anthropogenic impacts of Cd were particularly found in Zakamensk and Ulaanbaatar. Our results highlight clear anthropogenic impacts and large-scale spreading of several pollutants of concern, with risks even to downstream parts including the Selenga delta and Lake Baikal. We expect that these results will aid in increasing the understanding of large-scale metal transport processes, as well as for designing relevant measures to mitigate further spreading of metals to Lake Baikal.

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