Abstract
AbstractLake 227 of the Experimental Lakes Area (ELA) in Ontario, Canada, has been fertilized with phosphorus (P) since 1969, which resulted in a rapid transition from oligotrophic to eutrophic conditions. Sediment cores collected from the oxygenated epilimnion, and the mostly anoxic hypolimnion of this unique lake contain a historical record of the changes in sediment P speciation and burial rates across the trophic transition. To elucidate these changes, results of chemical extractions were combined with 210Pb sediment dating, and with 31P NMR, Mössbauer, and XANES spectroscopies. Prior to 1969, organic P (POrg) was the major sedimentary P sink in Lake 227. Eutrophication of the lake coincided with marked increases in the burial rate of total P (TP), as well as in the relative contribution of the NaHCO3‐extractable P pool (humic‐bound P, PHum). Together, PHum and POrg account for ≥70% of total P burial in the sediments deposited since artificial fertilization started. The PHum fraction likely comprises phosphate complexes with humic substances. The strong linear correlation between P and iron (Fe) extracted by NaHCO3 implies a close association of the two elements in the humic fraction. Mössbauer and XANES spectra further indicate that most Fe in the post‐1969 sediments remained in the Fe (III) oxidation state, which is attributed to the stabilization of reducible Fe by organic matter, in part via the formation of phosphate‐Fe (III)‐humic complexes. Importantly, our results show that the eutrophication experimentation of Lake 227 caused the accumulation of a large reservoir of reactive sediment P, which may continue to fuel internal P loading to the water column once artificial fertilization is terminated.
Highlights
Strict environmental regulations in many countries have contributed to substantial decreases in external phosphorus (P) loading to lakes from agriculture and urban activities
The aims of this study were to (1) compare the effect of prefertilization and postfertilization on P speciation before and after 1969 in dated sediment cores collected from deep and shallow regions of the lake, using sequential chemical extractions, complemented by spectroscopic techniques [31P nuclear magnetic resonance (NMR), Mössbauer, and X‐ray Adsorption Near‐Edge Structure (XANES)], and (2) assess how the pools of P associated with sedimentary organic matter and ferric iron (Fe) responded to the large shift in external P loading accompanying the long‐term fertilization experiment
We report on the changes in sediment accumulation and speciation of P and associated elements, including C, Fe, and S, which accompanied the rapid transition of Lake 227 from oligotrophic to eutrophic conditions
Summary
Strict environmental regulations in many countries have contributed to substantial decreases in external phosphorus (P) loading to lakes from agriculture and urban activities. A reduction in external P supply may amplify the role of internal P loading (Van der Molen & Boers, 1994). Because of the importance of internal P loading in lentic ecosystems, many studies have investigated the factors that affect benthic P release (Ahlgren et al, 2006; Orihel et al, 2017; Søndergaard et al, 2002). Phosphorus cycling in aquatic sediments is usually explained with the classic (Mortimer, 1941) model, where P release from sediments is controlled largely by the oxidation‐reduction cycle of iron (Fe). This model is based on the strong affinity of phosphate anions
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