Organic matter, eutrophication, and increased mass accumulation rates in the Anthropocene are the main drivers of mercury concentrations and historical enrichment in Canadian lake sediments

Mercury (Hg) contamination in the environment is a persistent issue as emissions from industry are ongoing and legacy cycling is prolonged. To quantify total mercury (total Hg) and methylmercury (MeHg) concentrations in lake sediments across a wide suite of temperate to subarctic lakes, measurements and modeling were conducted for 320 sites across Canada. Total Hg varied from 7 to 567 ng g-1 dry sediment with a mean (median) value of 148 (128) ng g-1 dry sediment, with lowest concentrations observed in eutrophic lakes of the Prairies and Boreal Plains. Average total Hg concentrations have increased twofold in contemporary sediments relative to their preindustrial pair. MeHg concentrations were generally low, with a mean of 0.8 ng g-1 dry sediment and this form representing on average 0.6% of the total contemporary mercury concentrations. Water column variables related to eutrophication were among the strongest predictors of contemporary total Hg, MeHg, and total Hg enrichment in the sediments. In lakes where sediment radiometric data were collected, contemporary total Hg accumulation rates were strongly related to longitude(+) and Hg atmospheric deposition(+). Latitude(-) and Hg atmospheric deposition(+) were the best predictors of MeHg accumulation rates. Chromophoric dissolved organic matter optical properties were key predictors of both total Hg concentrations and accumulation rates. Our work highlights the paramount importance of lake trophic state and the nature of organic matter as key predictors of lake sediment mercury metrics.