Centuries of anthropogenic releases have resulted in a global legacy of mercury (Hg) contamination. Here we use a global model to quantify the impact of uncertainty in Hg atmospheric emissions and cycling on anthropogenic enrichment and discuss implications for future Hg levels. The plausibility of sensitivity simulations is evaluated against multiple independent lines of observation, including natural archives and direct measurements of present-day environmental Hg concentrations. It has been previously reported that pre-industrial enrichment recorded in sediment and peat disagree by more than a factor of 10. We find this difference is largely erroneous and caused by comparing peat and sediment against different reference time periods. After correcting this inconsistency, median enrichment in Hg accumulation since pre-industrial 1760 to 1880 is a factor of 4.3 for peat and 3.0 for sediment. Pre-industrial accumulation in peat and sediment is a factor of ∼ 5 greater than the precolonial era (3000 BC to 1550 AD). Model scenarios that omit atmospheric emissions of Hg from early mining are inconsistent with observational constraints on the present-day atmospheric, oceanic, and soil Hg reservoirs, as well as the magnitude of enrichment in archives. Future reductions in anthropogenic emissions will initiate a decline in atmospheric concentrations within 1 year, but stabilization of subsurface and deep ocean Hg levels requires aggressive controls. These findings are robust to the ranges of uncertainty in past emissions and Hg cycling.

Background: Colonial cinnabar mining and refining began in Huancavelica, Peru, in 1564. With a local source of mercury, the amalgamation process was adopted to refine silver in Potosí, Bolivia, in the early 1570s. As a result, large quantities of mercury were released into the environment. Objectives: We used archival, primary, and secondary sources to develop the first estimate of mercury emissions from cinnabar refining in Huancavelica and to revise previous estimates of emissions from silver refining in Potosí during the colonial period (1564–1810). Discussion: Although other estimates of historical mercury emissions have recognized Potosí as a significant source, Huancavelica has been overlooked. In addition, previous estimates of mercury emissions from silver refining under-estimated emissions because of unrecorded (contra-band) production and volatilization of mercury during processing and recovery. Archival descriptions document behavioral and health issues during the colonial period that are consistent with known effects of mercury intoxication. Conclusions: According to our calculations, between 1564 and 1810, an estimated 17,000 metric tons of mercury vapor were emitted from cinnabar smelting in Huancavelica, and an estimated 39,000 metric tons were released as vapor during silver refining operations in Potosí. Huancavelica and Potosí combined contributed > 25% of the 196,000 metric tons of mercury vapor emissions in all of Latin America between 1500 and 1800. The historical record is laden with evidence of mercury intoxication consistent with effects recognized today. Our estimates serve as the foundation of investigations of present-day contamination in Huancavelica and Potosí resulting from historical emissions of mercury.

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