Abstract

Recent advances have allowed for greater investigation into microbial regulation of mercury toxicity in the environment. In wetlands in particular, dissolved organic matter (DOM) may influence methylmercury (MeHg) production both through chemical interactions and through substrate effects on microbiomes. We conducted microcosm experiments in two disparate wetland environments (oligotrophic unvegetated and high-C vegetated sediments) to examine the impacts of plant leachate and inorganic mercury loadings (20 mg/L HgCl2) on microbiomes and MeHg production in the St. Louis River Estuary. Our research reveals the greater relative capacity for mercury methylation in vegetated over unvegetated sediments. Further, our work shows how mercury cycling in oligotrophic unvegetated sediments may be susceptible to DOM inputs in the St. Louis River Estuary: unvegetated microcosms receiving leachate produced substantially more MeHg than unamended microcosms. We also demonstrate (1) changes in microbiome structure towards Clostridia, (2) metagenomic shifts toward fermentation, and (3) degradation of complex DOM; all of which coincide with elevated net MeHg production in unvegetated microcosms receiving leachate. Together, our work shows the influence of wetland vegetation in controlling MeHg production in the Great Lakes region and provides evidence that this may be due to both enhanced microbial activity as well as differences in microbiome composition.

Highlights

  • Mercury methylation in anoxic sediments is central to the bioaccumulation of mercury in plant and animal tissue (Benoit et al, 2003; Morel, Kraepiel & Amyot, 1998; Ullrich, Tanton & Abdrashitova, 2001) and poses a significant environmental and human health concern in the freshwater wetlands of the Great Lakes region (Branfireun et al, 1999; Harmon et al, 2005; Jeremiason et al, 2006)

  • Given the apparent shift in community structure towards Clostridia, and chemoorganotrophic Peptococcaceae in particular, we examined correlations of members of this family listed in the ORNL methylator database with the proportion of complex organic matter (HIX) and MeHg production within each environment

  • While substantially greater MeHg production is observed in vegetated sediments, unvegetated sediments stand to respond more strongly to Dissolved organic matter (DOM) additions in driving increases in MeHg production

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Summary

Introduction

Mercury methylation in anoxic sediments is central to the bioaccumulation of mercury in plant and animal tissue (Benoit et al, 2003; Morel, Kraepiel & Amyot, 1998; Ullrich, Tanton & Abdrashitova, 2001) and poses a significant environmental and human health concern in the freshwater wetlands of the Great Lakes region (Branfireun et al, 1999; Harmon et al, 2005; Jeremiason et al, 2006). With respect to mercury cycling in wetlands, mercury methylation is impacted both by binding properties of the humic DOM fraction, resulting either in increased dissolution of inorganic mercury complexes or in physical inhibition of mercury bioavailability (Drexel et al, 2002; Haitzer, Aiken & Ryan, 2002; Waples et al, 2005), and by the provisioning of organic substrate for microbial activity (Hsu-Kim et al, 2013; King et al, 2000; Lambertsson & Nilsson, 2006). Since mercury methylation is strongly impacted by DOM, environments such as the Great Lakes’ St. Louis River estuary, which contains areas of both vegetated and unvegetated sediments, may show differences in the capacity for MeHg production across vegetation gradients that exhibit pronounced differences in DOM content

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