Iron (Fe) concentrations are increasing in lakes and running waters over a broad geographical scale (Björnerås et al., 2017). Together with dissolved organic matter (DOM), Fe is contributing to an ongoing browning-that is, an increase in water color in freshwaters-with consequences for light penetration and thermal stratification, affecting ecosystem functions such as primary productivity, as well as for the ecosystem services that aquatic systems provide (Kritzberg et al., 2019). Fe originates primarily from sources in the catchment, and the association with DOM is a prerequisite for the transport of Fe from soils to waters, since DOM increases Fe solubility in oxic circum-neutral waters (Stumm & Morgan, 1996). However, lake-internal processes, such as aggregation and sedimentation, remove Fe from the water column (Neubauer et al., 2013;von Wachenfeldt et al., 2008) and are important in determining the distribution of Fe between the water column and the sediments (Björnerås Abstract Increasing iron (Fe) concentrations are found in lakes on a wide geographical scale but exact causes are still debated. The observed trends might result from increased Fe loading from the terrestrial catchment, but also from changes in how Fe distributes between the water column and the sediments. To get a better understanding of the causes we investigated whether there has been any change in the sediment formation of Fe sulfides (FeS) as an Fe sink in response to declining atmospheric sulfur (S) deposition during recent decades. For our study, we chose Lake Bolmen in southern Sweden, a lake for which we confirmed that Fe concentrations in the water column have strongly increased along with water color during 1966-2018. Our investigations showed that Fe accumulation and speciation varied independently of S accumulation patterns in the Lake Bolmen sediment record. Thus, we were not able to relate the positive trend in Fe concentrations to reduced FeS binding in the sediments. Furthermore, we found that Fe accumulation rates increased along with lake water Fe concentrations, indicating that increased catchment loading rather than a change in the distribution between the sediments and the water column has driven the increase in Fe concentrations. The increased loading may be due to land-use change in the form of an extensive expansion of coniferous forest during the past century. Altered forest management practices and increased precipitation may have led to enhanced weathering and erosion of organic soil layers under aging coniferous forest.
Plain Language Summary Iron concentrations are increasing in freshwaters in the NorthernHemisphere. One possible explanation is a decline in sulfur deposition in recent decades, which may have led to lower iron sulfide formation in soils and sediments, and thus to increased lake water iron concentrations. We tested this hypothesis by exploring iron concentrations in water and sediments of Lake Bolmen in southern Sweden in relation to changes in sulfur deposition, climate and catchment land-use. We ...