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The stability of Fe isotope signatures during low salinity mixing in subarctic estuaries
Luleå tekniska universitet, Institutionen för samhällsbyggnad och naturresurser, Geovetenskap och miljöteknik.ORCID-id: 0000-0002-7313-5833
GEOMAR Helmholtz Centre for Ocean Research Kiel, Kiel, Germany. Antarctic Climate and Ecosystems Cooperative Research Centre, University of Tasmania, Hobart, Australia.ORCID-id: 0000-0003-4010-5918
GEOMAR Helmholtz Centre for Ocean Research Kiel, Kiel, Germany. Institute for Marine and Antarctic Studies, University of Tasmania, Hobart, Australia.
ALS Laboratory Group, ALS Scandinavia AB, Luleå, Sweden.ORCID-id: 0000-0003-4505-4590
Visa övriga samt affilieringar
2019 (Engelska)Ingår i: Aquatic geochemistry, ISSN 1380-6165, E-ISSN 1573-1421, Vol. 25, nr 5-6, s. 195-218Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

We have studied iron (Fe)-isotope signals in particles (> 0.22 µm) and the dissolved phase (< 0.22 µm) in two subarctic, boreal rivers, their estuaries and the adjacent sea in northern Sweden. Both rivers, the Råne and the Kalix, are enriched in Fe and organic carbon (up to 29 µmol/L and up to 730 µmol/L, respectively). Observed changes in the particulate and dissolved phase during spring flood in May suggest different sources of Fe to the rivers during different seasons. While particles show a positive Fe-isotope signal during winter, during spring flood, the values are negative. Increased discharge due to snowmelt in the boreal region is most times accompanied by flushing of the organic-rich sub-surface layers. These upper podzol soil layers have been shown to be a source for Fe-organic carbon aggregates with a negative Fe-isotope signal. During winter, the rivers are mostly fed by deep groundwater, where Fe occurs as Fe(oxy)hydroxides, with a positive Fe-isotope signal. Flocculation during initial estuarine mixing does not change the Fe-isotope compositions of the two phases. Data indicate that the two groups of Fe aggregates flocculate diversely in the estuaries due to differences in their surface structure. Within the open sea, the particulate phase showed heavier δ56Fe values than in the estuaries. Our data indicate the flocculation of the negative Fe-isotope signal in a low salinity environment, due to changes in the ionic strength and further the increase of pH.

Ort, förlag, år, upplaga, sidor
Springer, 2019. Vol. 25, nr 5-6, s. 195-218
Nyckelord [en]
Fe-isotopes, Fe geochemistry, Dissolved and particulate Fe, Organically complexed Fe, Fe(oxy)hydroxides, Salinity gradient, Spring flood
Nationell ämneskategori
Geokemi
Forskningsämne
Tillämpad geokemi
Identifikatorer
URN: urn:nbn:se:ltu:diva-73760DOI: 10.1007/s10498-019-09360-zISI: 000494758500001Scopus ID: 2-s2.0-85074857809OAI: oai:DiVA.org:ltu-73760DiVA, id: diva2:1306841
Anmärkning

Validerad;2019;Nivå 2;2019-12-06 (johcin)

Tillgänglig från: 2019-04-25 Skapad: 2019-04-25 Senast uppdaterad: 2021-10-24Bibliografiskt granskad
Ingår i avhandling
1. Iron isotopes in aquatic systems
Öppna denna publikation i ny flik eller fönster >>Iron isotopes in aquatic systems
2019 (Engelska)Doktorsavhandling, sammanläggning (Övrigt vetenskapligt)
Alternativ titel[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.

Ort, förlag, år, upplaga, sidor
Luleå: Luleå University of Technology, 2019
Serie
Doctoral thesis / Luleå University of Technology 1 jan 1997 → …, ISSN 1402-1544
Nationell ämneskategori
Geokemi
Forskningsämne
Tillämpad geokemi
Identifikatorer
urn:nbn:se:ltu:diva-73763 (URN)978-91-7790-376-5 (ISBN)978-91-7790-377-2 (ISBN)
Disputation
2019-06-20, F531, Luleå, 10:00 (Engelska)
Opponent
Handledare
Tillgänglig från: 2019-04-25 Skapad: 2019-04-25 Senast uppdaterad: 2019-06-05Bibliografiskt granskad

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Conrad, SarahRodushkin, IliaIngri, Johan

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Conrad, SarahWuttig, KathrinRodushkin, IliaIngri, Johan
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