Human activities over the last several centuries have transferred vast quantities of mercury (Hg) from deep geologic stores to actively cycling earth-surface reservoirs, increasing atmospheric Hg deposition worldwide. Understanding the magnitude and fate of these releases is critical to predicting how rates of atmospheric Hg deposition will respond to future emission reductions. The most recently compiled global inventories of integrated (all-time) anthropogenic Hg releases are dominated by atmospheric emissions from preindustrial gold/silver mining in the Americas. However, the geophysical evidence for such large early emissions is equivocal, because most reconstructions of past Hg-deposition have been based on lake-sediment records that cover only the industrial period (1850-present). Here we evaluate historical changes in atmospheric Hg deposition over the last millennium from a suite of lake-sediment cores collected from remote regions of the globe. Along with recent measurements of Hg in the deep ocean, these archives indicate that atmospheric Hg emissions from early mining were modest as compared to more recent industrial-era emissions. Although large quantities of Hg were used to extract New World gold and silver beginning in the 16th century, a reevaluation of historical metallurgical methods indicates that most of the Hg employed was not volatilized, but rather was immobilized in mining waste.

Both cinnabar (HgS) and metallic mercury (Hg(0)) were important resources throughout Andean prehistory. Cinnabar was used for millennia to make vermillion, a red pigment that was highly valued in pre-Hispanic Peru; metallic Hg(0) has been used since the mid-16th century to conduct mercury amalgamation, an efficient process of extracting precious metals from ores. However, little is known about which cinnabar deposits were exploited by pre-Hispanic cultures, and the environmental consequences of Hg mining and amalgamation remain enigmatic. Here we use Hg isotopes to source archeological cinnabar and to fingerprint Hg pollution preserved in lake sediment cores from Peru and the Galápagos Islands. Both pre-Inca (pre-1400 AD) and Colonial (1532-1821 AD) archeological artifacts contain cinnabar that matches isotopically with cinnabar ores from Huancavelica, Peru, the largest cinnabar-bearing district in Central and South America. In contrast, the Inca (1400-1532 AD) artifacts sampled are characterized by a unique Hg isotopic composition. In addition, preindustrial (i.e., pre-1900 AD) Hg pollution preserved in lake sediments matches closely the isotopic composition of cinnabar from the Peruvian Andes. Industrial-era Hg pollution, in contrast, is distinct isotopically from preindustrial emissions, suggesting that pre- and postindustrial Hg emissions may be distinguished isotopically in lake sediment cores.

We present unambiguous records of preindustrial atmospheric mercury (Hg) pollution, derived from lake-sediment cores collected near Huancavelica, Peru, the largest Hg deposit in the New World. Intensive Hg mining first began ca. 1400 BC, predating the emergence of complex Andean societies, and signifying that the region served as a locus for early Hg extraction. The earliest mining targeted cinnabar (HgS) for the production of vermillion. PreColonial Hg burdens peak ca. 500 BC and ca. 1450 AD, corresponding to the heights of the Chavín and Inca states, respectively. During the Inca, Colonial, and industrial intervals, Hg pollution became regional, as evidenced by a third lake record Ϸ225 km distant from Huancavelica. Measurements of sediment-Hg speciation reveal that cinnabar dust was initially the dominant Hg species deposited, and significant increases in deposition were limited to the local environment. After conquest by the Inca (ca. 1450 AD), smelting was adopted at the mine and Hg pollution became more widely circulated, with the deposition of matrix-bound phases of Hg predominating over cinnabar dust. Our results demonstrate the existence of a major Hg mining industry at Huancavelica spanning the past 3,500 years, and place recent Hg enrichment in the Andes in a broader historical context.

Air temperatures in the tropical Andes have risen at an accelerated rate relative to the global average over recent decades. However, the effects of climate change on Andean lakes, which are vital to sustaining regional biodiversity and serve as an important water resource to local populations, remain largely unknown. Here, we show that recent climate changes have forced alpine lakes of the equatorial Andes towards new ecological and physical states, in close synchrony to the rapid shrinkage of glaciers regionally. Using dated sediment cores from three lakes in the southern Sierra of Ecuador, we record abrupt increases in the planktonic thalassiosiroid diatom Discostella stelligera from trace abundances to dominance within the phytoplankton. This unprecedented shift occurs against the backdrop of rising temperatures, changing atmospheric pressure fields, and declining wind speeds. Ecological restructuring in these lakes is linked to warming and/or enhanced water column stratification. In contrast to seasonally ice-covered Arctic and temperate alpine counterparts, aquatic production has not increased universally with warming, and has even declined in some lakes, possibly because enhanced thermal stability impedes the re-circulation of hypolimnetic nutrients to surface waters. Our results demonstrate that these lakes have already passed important ecological thresholds, with potentially far-reaching consequences for Andean water resources.

The mining and processing of the Athabasca oil sands (Alberta, Canada) has been occurring for decades; however, a lack of consistent regional monitoring has obscured the long-term environmental impact. Here, we present sediment core results to reconstruct spatial and temporal patterns in trace element deposition to lakes in the Athabasca oil sands region. Early mining operations (during the 1970s and 1980s) led to elevated V and Pb inputs to lakes located <50 km from mining operations. Subsequent improvements to mining and upgrading technologies since the 1980s have reduced V and Pb loading to near background levels at many sites. In contrast, Hg deposition increased by a factor of ∼3 to all 20 lakes over the 20th century, reflecting global-scale patterns in atmospheric Hg emissions. Base cation deposition (from fugitive dust emissions) has not measurably impacted regional lake sediments. Instead, results from a principal components analysis suggest that the presence of carbonate bedrock underlying lakes located close to development appears to exert a first-order control over lake sediment base cation concentrations and overall lake sediment geochemical composition. Trace element concentrations generally did not exceed Canadian sediment quality guidelines, and no spatial or temporal trends were observed in the frequency of guideline exceedence. Our results demonstrate that early mining efforts had an even greater impact on trace element cycling than has been appreciated previously, placing recent monitoring efforts in a critical long-term context.