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Iron isotope pathways in the boreal landscape: Role of the riparian zone
Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.ORCID iD: 0000-0003-2276-0564
Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.ORCID iD: 0000-0002-7313-5833
Department of Forest Ecology and Management, Swedish University of Agricultural Sciences, Umeå.
Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
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2018 (English)In: Geochimica et Cosmochimica Acta, ISSN 0016-7037, E-ISSN 1872-9533, Vol. 239, p. 49-60Article in journal (Refereed) Published
Abstract [en]

Stable Fe isotope compositions have been measured in water samples of the subarctic Kalix River, a first-order stream, and soil water samples from a riparian soil profile adjacent to the first-order stream (Northern Sweden). In the first-order stream, dominated by forest, both the particulate (>0.22 µm) and dissolved (<0.22 µm) phase showed negative δ56Fe values (relative to IRMM-014) during base flow and meltwater discharge in May (−0.97 to −0.09‰). The Fe isotope composition in the water from the riparian soil profile varied between −0.20 and +0.91‰ with sharp gradients near the groundwater table. A linear correlation between the δ56Fe values and the TOC/Febulk ratio was measured during snowmelt in the unfiltered river waters (δ56Fe from −0.02 to +0.54‰), suggesting mixing of two Fe components. Two groups of Fe aggregates, with different Fe isotope compositions, are formed in the boreal landscape. We propose that carbon-rich aggregates, Fe(II)(III)-OC, have negative δ56Fe values and Fe-oxyhydroxides have positive δ56Fe values. A mixture of these two components can explain temporal variations of the Fe isotope composition in the Kalix River. This study suggests that stable Fe isotopes can be used as a tool to track and characterize suspended Fe-organic carbon aggregates during transport from the soil, via first-order streams and rivers, to coastal sediment. Furthermore, the differences in Fe isotope values in the Kalix River and the first-order stream during base flow conditions suggest that the primary Fe sources for river water change throughout the year. This model is combining the Fe isotope composition of first-order streams and rivers to weathering and transport processes in the riparian soil.

Place, publisher, year, edition, pages
Elsevier, 2018. Vol. 239, p. 49-60
National Category
Geochemistry
Research subject
Applied Geochemistry
Identifiers
URN: urn:nbn:se:ltu:diva-70367DOI: 10.1016/j.gca.2018.07.030ISI: 000445036400003Scopus ID: 2-s2.0-85051391721OAI: oai:DiVA.org:ltu-70367DiVA, id: diva2:1238556
Note

Validerad;2018;Nivå 2;2018-08-14 (andbra)

Available from: 2018-08-14 Created: 2018-08-14 Last updated: 2019-04-25Bibliographically approved
In thesis
1. Iron isotopes in aquatic systems
Open this publication in new window or tab >>Iron isotopes in aquatic systems
2019 (English)Doctoral thesis, comprehensive summary (Other academic)
Alternative title[sv]
Järnisotoper i akvatiska system
Abstract [en]

The cycling of iron (Fe) is a key component for understanding water quality and biogeochemical processes. It serves as mediator during biotic and abiotic processes, as electron acceptor during the degradation of organic matter, as surface for trace element and organic matter adsorption, and is necessary for primary production processes. Since the beginning of Fe isotope studies, researchers focussed on the ratios in soils, rivers and oceans in various environments. The aim of this study was to characterize the Fe isotope ratios from the source (e.g. soils), along the river course, through the estuaries and into the adjacent sea within the boreal landscape. Therefore, seasonal sampling of water from Swedish headwater streams (2016/2017), rivers (2016), estuaries (2013/2014) and the Baltic Sea (2013/2014) were conducted, with the purpose to better understand the role and fate of riverine Fe export. Fe is transported in two main phases from the headwater streams into the oceans: organic Fe complexes and Fe(oxy)hydroxide. It has been proposed that these Fe phases varies in response to seasonal differences in hydrology.

                      This thesis includes the first Fe isotope dataset describing seasonal variations of headwater streams on a regional scale. In the headwater streams positive and negative Fe isotopes ratios can be used to distinguish between different Fe phases. Furthermore, Fe isotope ratios in headwater streams could verify regional drought periods and the subsequent rewetting of the subsurface soils.

Within the rivers and estuaries, we found positive Fe isotopes in the dissolved phase (< 0.22µm) and negative Fe isotopes (> 0.22µm) in the particulate phase during high discharge. The correlation between different chemical parameters, Fe and DOC showed that the Fe isotope composition during spring flood is evolving in the upper soil layers of headwater streams. Therefore, the lighter Fe isotope signal is correlated to the organic-rich soil layers of the riparian zones in forested catchments. During baseflow, particulate Fe has a positive Fe isotope signal. This shows that the Fe has different origin throughout the season within one catchment.

Salt-induced flocculation in the estuaries and under experimental conditions, is removing about 80 % of the dissolved and particulate Fe. Newly formed colloids and particles aggregate and sediment due to small changes in salinity. This major flocculation at low salinities might cause an underestimation of riverine Fe flux. Interestingly, salinity-induced aggregation experiments revealed that Fe(oxy)hydroxide, which dominated aggregates, displayed lower Fe isotope ratios than in the river samples Fe, while organic Fe complexes in the suspension had higher Fe isotope values. The seasonal variability in Fe isotope values could not be simply linked to Fe phases but was probably also influenced by variation in source areas of Fe and processes along the flow-path that alter both Fe phases and isotopic composition.

Within the estuarine mixing zone, no Fe isotope fractionation was observed. The Fe isotope signal is constant over time and space, which excludes fractionation processes for example by oxidation. The Fe isotope signal within the Bothnian Bay was positive showing that different surface properties of Fe-OC and Fe(oxy)hydroxide aggregates lead to the flocculation of negative Fe aggregates.

Place, publisher, year, edition, pages
Luleå: Luleå University of Technology, 2019
Series
Doctoral thesis / Luleå University of Technology 1 jan 1997 → …, ISSN 1402-1544
National Category
Geochemistry
Research subject
Applied Geochemistry
Identifiers
urn:nbn:se:ltu:diva-73763 (URN)978-91-7790-376-5 (ISBN)978-91-7790-377-2 (ISBN)
Public defence
2019-06-20, F531, Luleå, 10:00 (English)
Opponent
Supervisors
Available from: 2019-04-25 Created: 2019-04-25 Last updated: 2019-06-05Bibliographically approved

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Ingri, JohanConrad, SarahEngström, Emma

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