Abstract

Anthropogenic releases of mercury (Hg)1–3 are a human health issue4 because the potent toxicant methylmercury (MeHg), formed primarily by microbial methylation of inorganic Hg in aquatic ecosystems, bioaccumulates to high concentrations in fish consumed by humans5,6. Predicting the efficacy of Hg pollution controls on fish MeHg concentrations is complex because many factors influence the production and bioaccumulation of MeHg7–9. Here we conducted a 15-year whole-ecosystem, single-factor experiment to determine the magnitude and timing of reductions in fish MeHg concentrations following reductions in Hg additions to a boreal lake and its watershed. During the seven-year addition phase, we applied enriched Hg isotopes to increase local Hg wet deposition rates fivefold. The Hg isotopes became increasingly incorporated into the food web as MeHg, predominantly from additions to the lake because most of those in the watershed remained there. Thereafter, isotopic additions were stopped, resulting in an approximately 100% reduction in Hg loading to the lake. The concentration of labelled MeHg quickly decreased by up to 91% in lower trophic level organisms, initiating rapid decreases of 38–76% of MeHg concentration in large-bodied fish populations in eight years. Although Hg loading from watersheds may not decline in step with lowering deposition rates, this experiment clearly demonstrates that any reduction in Hg loadings to lakes, whether from direct deposition or runoff, will have immediate benefits to fish consumers.

Highlights

  • Changing climatic conditions can influence MeHg production[8], as well as restructure food webs, alter the dominant pathways of energy flow and cause size-dependent changes in fish growth rates that shift population size structure[14,17,18]

  • METAALICUS addresses the relationship between changes in inorganic Hg loadings to a lake and MeHg

  • Lake white sh Northern pike Surface sediments concentrations in fish using highly enriched inorganic Hg isotopes that enabled us to follow a change in loading against a background of previously deposited Hg and present-day, relatively constant, Hg inputs from direct deposition to the lake surface and from the watershed

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Summary

Methods

METAALICUS was conducted on the Lake 658 catchment at the Experimental Lakes Area (ELA; IISD-ELA), a remote area in the Precambrian Shield of northwestern Ontario, Canada (49° 43′ 95′′ N, 93° 44′ 20′′ W) set aside for whole-ecosystem research[31]. Sampling for determination of MeHg concentrations (measured as total mercury (THg), see below) occurred each autumn (August–October; that is, the end of the growing season in north temperate lakes) for all fish species in Lake 658, and for northern pike and yellow perch in nearby reference Lake 240 (Extended Data Tables 2, 3). MeHg concentration of prey items were averaged from samples collected throughout the open-water season immediately prior to autumn sampling of fish species to represent an integrated exposure for calculation of BMF. To account for differences among individuals and between individuals and the population, we normalized the data to examine the mean proportion of original (t0) lake spike MeHg burden present in northern pike each year of the recovery period (2008–2015). Reporting summary Further information on research design is available in the Nature Research Reporting Summary linked to this paper

Experiments of concern
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