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Speciation and hydrological transport of metals in non-acidic river systems of the Lake Baikal basin: Field data and model predictions
Stockholm University, Faculty of Science, Department of Physical Geography.ORCID iD: 0000-0001-6111-4819
Stockholm University, Faculty of Science, Department of Physical Geography.
Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
Stockholm University, Faculty of Science, Department of Geological Sciences.
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2017 (English)In: Regional Environmental Change, ISSN 1436-3798, E-ISSN 1436-378X, Vol. 17, no 7, 2007-2021 p.Article in journal (Refereed) Published
Abstract [en]

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.

Place, publisher, year, edition, pages
2017. Vol. 17, no 7, 2007-2021 p.
Keyword [en]
Metals, Speciation, River system, Non-acidic, Geochemical modelling, Lake Baikal
National Category
Geochemistry Oceanography, Hydrology, Water Resources
Research subject
Physical Geography
Identifiers
URN: urn:nbn:se:su:diva-145718DOI: 10.1007/s10113-016-0982-7OAI: oai:DiVA.org:su-145718DiVA: diva2:1134226
Funder
Swedish Research Council Formas, 2012-790
Available from: 2017-08-18 Created: 2017-08-18 Last updated: 2017-11-30Bibliographically approved
In thesis
1. Hydrological spreading of metal pollution and wetlands as nature-based solutions
Open this publication in new window or tab >>Hydrological spreading of metal pollution and wetlands as nature-based solutions
2017 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The quality of the Earth’s water resources have deteriorated due to human impacts. A key scientific challenge is to understand, quantify and predict the water-borne spreading of pollutants at relevant scales for freshwater management and water quality restoration programs. However, understanding the natural processes controlling large-scale hydrological transport of pollutants may be masked by river regulation schemes (in the form of dams and reservoirs), which are common in many large rivers. The main objective of this thesis is to increase the current knowledge regarding large-scale spreading of metals in hydrological systems. This objective is addressed through studying net impacts of mining (a main contributor to global metal pollution) on the spreading of metals in water systems and through investigating the mitigation opportunities of wetlands across the landscape. The main study region of this thesis is the Lake Baikal basin of Russia and Mongolia, which includes the large unregulated Selenga River and its delta-wetland areas. In addition, a set of global wetland sites are also studied. A multi-method approach is used in the four studies of this thesis. The methods include field-measurements, data synthesis, metal mass flow and water flow-path quantifications, as well as geochemical modelling. Results show that mining in the upstream part of the Lake Baikal basin is a significant contributor to riverine mass flows of several metals. The mass flows increased by an order of magnitude over the mining site. The observed speciation between dissolved (more bioavailable) and suspended (less bioavailable) phases could be well predicted for some metals (Fe, V, Pb and Zn) using a geochemical equilibrium model. However, the model failed to reproduce the speciation of other metals (Cr, Cu, Mn and Mo). In these cases, non-equilibrium processes may need to be considered, and adsorption databases may need to be developed, in order to make dependable predictions. Results also suggest that the concentration of dissolved organic carbon, which exhibits seasonal variability and long-term increasing trends due to climate change effects in the Arctic, can have a large impact on metal pollution transport. Further, observations showed that individual wetlands of the Selenga River delta locally retained between 77-99 % of incoming metal loads. However, a systematic analysis of current knowledge showed that large-scale net effects can differ considerably from the functions observed at individual wetlands on smaller scales. Along large-scale flow-paths, through which wetlands are connected with each other as well as with the larger landscape, key processes which can considerably contribute to such scale differences in function may occur. A survey of the current wetland research showed that relatively few studies have considered the larger scales at which key pollutant pressures and water quality changes take place. This thesis highlights the need for more research on large-scale wetland systems, which can aid in evaluating net pollution effects at landscape scales. This in turn can facilitate evaluations of how and when wetland systems may function as large-scale nature-based solutions.

Abstract [sv]

Kvaliteten på jordens vattenresurser har försämrats på grund av mänsklig påverkan. En viktig vetenskaplig utmaning är att förstå, kvantifiera och förutsäga den vattenburna spridningen av föroreningar, på skalor som är relevanta för vattenresursförvaltning och åtgärdsprogram. De underliggande, naturliga processer som styr storskalig hydrologisk föroreningstransport kan dock maskeras av att de flesta stora floders flöden är reglerade med hjälp av dammar och reservoarer. Målet med den här avhandlingen är att öka kunskapen kring hydrologisk storskalig spridning av metaller. Detta görs genom att studera nettoeffekter av gruvverksamhet (en viktig källa till globala metallföroreningar) på metallers spridning i vattensystemet, samt att undersöka våtmarkers möjligheter att rena förorenade flöden i landskapet. Avhandlingens huvudstudieområde är Bajkalsjön och dess tillrinningsområde (i Ryssland och Mongoliet), vilket inkluderar den oreglerade Selengafloden och dess delta-våtmarksområden. Även en grupp av globala våtmarksområden har studerats. Flera metoder användes i de fyra studierna som ingår i denna avhandling, inklusive fältmätningar, datasyntes, massflödes- och flödesvägskvantifieringar, och geokemisk modellering. Resultaten visar att gruvdrift i uppströms-delar av Bajkalsjöns tillrinningsområde bidrar betydligt till förhöjda halter av flera metaller i flodsystemen. Massflödenena ökade en storleksordning över gruvområdet. Den observerade metall-specieringen mellan lösta (mer biotillgängliga) och partikulära (mindre biotillgängliga) faser kunde modelleras väl för vissa metaller (Fe, V, Pb och Zn) med en geokemisk jämviktsmodell. Modellen lyckades dock inte reproducera specieringen av andra metaller (Cr, Cu, Mn och Mo). I dessa fall kan icke-jämviktsprocesser behöva beaktas, och adsorptions-databaser kan behöva utvecklas för att förbättra prediktionerna. Resultaten visar också att koncentrationen av upplöst organiskt kol, som uppvisar stora årstidsvariationer samt långsiktigt ökande trender på grund av klimatpåverkan i Arktis, kan ha stor inverkan på metallföroreningars transport. Observationer visade att enskilda våtmarker i Selengafloden lokalt kunde minska inkommande massflöden av metaller med 77 till 99 %.  En systematisk genomgång av aktuellt kunskapsläge visade dock att storskaliga nettoeffekter kan skilja sig mycket från de funktioner som observeras vid enskilda våtmarker på mindre skalor. Längs storskaliga flödesvägar, genom vilka flera våtmarker är kopplade till varandra och till det större landskapet, kan viktiga processer ske, vilket avsevärt kan bidra till sådana skal-skillnader i funktion. En genomgång av aktuell våtmarksforskning visade att relativt få studier beaktade dessa större skalor där föroreningsspridning och vattenkvalitetsförändringar sker. Denna avhandling belyser behovet av ökat forskningsfokus på storskaliga våtmarkssystem. Detta kan hjälpa till att förstå föroreningars nettoeffekter på landskapsskalor, vilket underlättar vid bedömning av hur och när våtmarkssystem fungerar som storskaliga, så kallade naturbaserade lösningar. 

Place, publisher, year, edition, pages
Stockholm: Department of Physical Geography, Stockholm University, 2017
Series
Dissertations from the Department of Physical Geography, ISSN 1653-7211 ; 68
National Category
Oceanography, Hydrology, Water Resources
Research subject
Physical Geography
Identifiers
urn:nbn:se:su:diva-147613 (URN)978-91-7649-958-0 (ISBN)978-91-7649-959-7 (ISBN)
Public defence
2017-11-28, De Geersalen, Geovetenskapens hus, Svante Arrhenius väg 14, Stockholm, 13:00 (English)
Opponent
Supervisors
Available from: 2017-11-03 Created: 2017-10-06 Last updated: 2017-11-02Bibliographically approved

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