Salt marshes: an important coastal sink for dissolved uranium

Abstract

The global budget for marine uranium demands another geochemical sink other than deep-sea systems, and the coastal environment may host some or all of this missing sink. In a previous paper (Sarin and Church, 1994), we have shown that some large subtidal estuaries are seasonal summer sinks at low salinities. In this paper, we show that intertidal salt marshes are even stronger sinks at all salinities, if for somewhat different reasons. Uranium was sampled in dissolved and particulate fractions over several tidal cycles and seasons for a lower Delaware Bay salt marsh (Canary Creek, Lewes, Delaware, USA), and uniquely, during summer months, the dissolved uranium is nonconservative. Moreover, because uranium extraction is greater on higher tides and occurs over the entire salinity gradient, this processing appears associated with surface of vegetated high marsh. We hypothesize that either (1) uranium scavenging occurs during the process of tidal mixing and attendant flocculation of humic acids and iron oxides-favoring this process is the presence of sulfonate complexes in salt marsh humic substances, and iron coprecipitation during its extensive redox cycling in the salt marsh-or (2) uranium extraction occurs at the marsh surface during extensive flooding of the salt marsh surface sediments-favoring this process is the increase in sulfuric acidity at the summer salt marsh surface that could destabilize the tetracarbonate species of U(VI). The latter option is favored by both field observations of maximum removal at the surface during the spring and summer tide conditions, and selective extraction of sediment phases where uranium is found as adsorbed and complexed forms in the ascorbate-citrate and humic acid fractions, respectively. Mass balance calculations show that under steady-state conditions, nearly two-thirds of the uranium extracted from tidal waters is retained in the sediments, while one-third is exported as U-enriched particles during ebbing tides. Independent confirmation of this balance comes from the measured accumulation rate of uranium buried at depth. This represents the net inventory buried below the geochemically reactive surface responsible for the initial extraction and redistribution of uranium onto sediment or tidally exported phases. Extrapolated globally, uranium burial in salt marshes alone or total marine wetlands including mangroves could comprise at least 10% and perhaps as much as 50% the total marine sink for uranium, or on an area specific basis, up to 50 times their marine areal extent.