Global-scale patterns in anthropogenic Pb contamination reconstructed from natural archives.

During the past two centuries metal loads in the Earth's atmosphere and ecosystems have increased significantly over pre-industrial levels. This has been associated with deleterious effects to ecosystem processes and human health. The magnitude of this toxic metal burden, as well as the spatial and temporal patterns of metal enrichment, is recorded in sedimentary archives across the globe. This paper presents a compilation of selected Pb contamination records from lakes (n = 10), peat mires (n = 10) and ice fields (n = 7) from Europe, North and South America, Asia, Australia and the Northern and Southern Hemisphere polar regions. These records quantify changes in Pb enrichment in remote from source environments. The presence of anthropogenic Pb in the environment has a long history, extending as far back as the early to mid-Holocene in North America, Europe and East Asia. However, results show that Pb contamination in the Earth's environment became globally ubiquitous at the beginning of the Second Industrial Revolution (c.1850-1890 CE), after which the magnitude of Pb contamination increased significantly. This date therefore serves as an effective global marker for the onset of the Anthropocene. Current global average Pb enrichment rates are between 6 and 35 times background, however Pb contamination loads are spatially variable. For example, they are >100 times background in Europe and North America and 5-15 times background in Antarctica. Despite a recent decline in Pb loads in some regions, most notably Europe and North America, anthropogenic Pb remains highly enriched and universally present in global ecosystems, while concentrations are increasing in some regions (Australia, Asia and parts of South America and Antarctica). There is, however, a paucity of Pb enrichment records outside of Europe, which limits assessments of global contamination.

A landscape-scale approach to examining the fate of atmospherically derived industrial metals in the surficial environment.

Industrial metals are now ubiquitous within the atmosphere and their deposition represents a potential source of contamination to surficial environments. Few studies, however, have examined the environmental fate of atmospheric industrial metals within different surface environments. In this study, patterns of accumulation of atmospherically transported industrial metals were investigated within the surface environments of the Snowy Mountains, Australia. Metals, including Pb, Sb, Cr and Mo, were enriched in aerosols collected in the Snowy Mountains by 3.5-50 times pre-industrial concentrations. In sedimentary environments (soils, lakes and reservoirs) metals showed varying degrees of enrichment. Differences were attributed to the relative degree of atmospheric input, metal sensitivity to enrichment, catchment area and metal behaviour following deposition. In settings where atmospheric deposition dominated (ombrotrophic peat mires in the upper parts of catchments), metal enrichment patterns most closely resembled those in collected aerosols. However, even in these environments significant dilution (by 5-7 times) occurred. The most sensitive industrial metals (those with the lowest natural concentration; Cd, Ag, Sb and Mo) were enriched throughout the studied environments. However, in alpine tarn-lakes no other metals were enriched, due to the dilution of pollutant-metals by catchment derived sediment. In reservoirs, which were located lower within catchments, industrial metals exhibited more complex patterns. Particle reactive metals (e.g. Pb) displayed little enrichment, implying that they were retained up catchment, whereas more soluble metals (e.g., Cu and Zn) showed evidence of concentration. These same metals (Cu and Zn) were depleted in soils, implying that they are preferentially transported through catchments. Enrichment of other metals (e.g. Cd) varied between reservoirs as a function of contributing catchment area. Overall this study showed that the fate of atmospherically derived metals is complex, and depends upon metal behaviour and geomorphic processes operating at landscape scales.

Attribution of sources to metal accumulation in an alpine tarn, the Snowy Mountains, Australia.

This study analyses 1800 years of heavy metal accumulation in a remote alpine lake experiencing long-range atmospheric contamination and additional inputs of Ag from cloud seeding. In comparison to previous work undertaken on peats, lake sediments show limited post-industrial metal enrichment with enrichment factors of Ag: 1.3, Pb: 1.3, Zn: 1.1, Cu: 1.2 compared to Ag: 2.2, Pb: 3.3, Zn: 2.1, Cu: 4.1 for peat. We show this to be the result of substantial fluvial lithogenic flux of metals (92-97% of total metal flux) to the lake. Total annual metal flux to the lake ranges from: Ag: 4-12 ng/cm(2)/yr to Zn: 3 383-11 313 ng/cm(2)/yr. As a result, any contribution of cloud seeding to additional enrichment of Ag in lake sediments is considered negligible. Results show that metal enrichment is not necessarily ubiquitous through a landscape. This has implications for predicting the impacts of atmospheric metal pollution to complex environmental systems.

Using trace elements in particulate matter to identify the sources of semivolatile organic contaminants in air at an alpine site.

An approach using trace elements in particulate matter (PM) to identify the geographic sources of atmospherically transported semivolatile organic contaminants (SOCs) was investigated. Daily samples of PM and SOCs were collected with high-volume air samplers from 16 January to 16 February 2009 at Temple Basin, a remote alpine site in New Zealand's Southern Alps. The most commonly detected pesticides were dieldrin, trans-chlordane, endosulfan I, and chlorpyrifos. Polycyclic aromatic hydrocarbons and polychlorinated biphenyls were also detected. For each sampling day, the relative contribution of PM from regional New Zealand versus long-range Australian sources was determined using trace element profiles and a binary mixing model. The PM approach indicated that endosulfan I, indeno[1,2,3-c,d]pyrene, and benzo[g,h,i]perylene found at Temple Basin were largely of Australian origin. Local wind observations indicated that the chlorpyrifos found at Temple Basin primarily came from the Canterbury Plains in New Zealand.

Atmospheric pollutants in alpine peat bogs record a detailed chronology of industrial and agricultural development on the Australian continent.

Two peat bogs from remote alpine sites in Australia were found to contain detailed and coherent histories of atmospheric metal pollution for Pb, Zn, Cu, Mo, Ag, As, Cd, Sb, Zn, In, Cr, Ni, Tl and V. Dramatic increases in metal deposition in the post-1850 AD portion of the cores coincide with the onset of mining in Australia. Using both Pb isotopes and metals, pollutants were ascribed to the main atmospheric pollution emitting sources in Australia, namely mining and smelting, coal combustion and agriculture. Results imply mining and metal production are the major source of atmospheric metal pollution, although coal combustion may account for up to 30% of metal pollutants. A novel finding of this study is the increase in the otherwise near-constant Y/Ho ratio after 1900 AD. We link this change to widespread and increased application of marine phosphate fertiliser in Australia's main agricultural area (the Murray Darling Basin).