Reconstructing Early Industrial Contributions to Legacy Trace Metal Contamination in Southwestern Pennsylvania.

Early industrial trace metal loadings are poorly characterized but potentially substantial sources of trace metals to the landscape. The magnitude of legacy contamination in southwestern Pennsylvania, the cradle of North American fossil fuel industrialization, is reconstructed from trace metal concentrations in a sediment core with proxies including major and trace metal chemistry, bulk density, and magnetic susceptibility. Trace metal chemistry in this sediment record reflects 19th and 20th century land use and industry. In particular, early 19th century arsenic loadings to the lake are elevated from pesticides used by early European settlers at a lakeside tannery. Later, sediment barium concentrations rise, likely reflecting the onset of acidic mine drainage from coal operations. Twentieth century zinc, cadmium, and lead concentrations are dominated by emissions from the nearby, infamous Donora Zinc Works yet record both the opening of a nearby coal-fired power plant and amendments to the Clean Air Act. The impact of early industry is substantial and rivals more recent metal fluxes, resulting in a significant potential source of contaminated sediments. Thus, modern assessments of trace metal contamination cannot ignore early industrial inputs, as the potential remobilization of legacy contamination would impact ecosystem and human health.

Environmental legacy of copper metallurgy and Mongol silver smelting recorded in Yunnan Lake sediments.

Geochemical measurements on well-dated sediment cores from Lake Er (Erhai) are used to determine the timing of changes in metal concentrations over 4500 years in Yunnan, a borderland region in southwestern China noted for rich mineral deposits but with inadequately documented metallurgical history. Our findings add new insight into the impacts and environmental legacy of human exploitation of metal resources in Yunnan history. We observe an increase in copper at 1500 BC resulting from atmospheric emissions associated with metallurgy. These data clarify the chronological issues related to links between the onset of Yunnan metallurgy and the advent of bronze technology in adjacent Southeast Asia, subjects that have been debated for nearly half a century. We also observe an increase from 1100 to 1300 AD in a number of heavy metals including lead, silver, zinc, and cadmium from atmospheric emissions associated with silver smelting. Culminating during the rule of the Mongols, known as the Yuan Dynasty (1271-1368 AD), these metal concentrations approach levels three to four times higher than those from industrialized mining activity occurring within the catchment today. Notably, the concentrations of lead approach levels at which harmful effects may be observed in aquatic organisms. The persistence of this lead pollution over time created an environmental legacy that likely contributes to known issues in modern day sediment quality. We demonstrate that historic metallurgical production in Yunnan can cause substantial impacts on the sediment quality of lake systems, similar to other paleolimnological findings around the globe.

Metal ratio mixing models clarify metal contamination sources to lake sediments in Yunnan, China.

Contaminated legacy sediments contribute to modern pollution loadings, particularly trace metals. These contributions are challenging to quantify as metal histories reconstructed from sediment records cannot be easily divided into legacy and concurrent contamination. In particular, the contribution from re-mobilization and delivery of legacy metals stored in catchment soil, colluvial, and fluvial environments are rarely considered or quantified when interpreting sediment records. Here, extended records of metals accumulation for a set of three lakes in Yunnan, China are compared with endmember chemistries using Monte Carlo-Markov Chain mixing models to help identify source contributions to the sediments. This approach allows attribution of metals transported by atmospheric and fluvial mechanisms in a region with a history of mining and metallurgy spanning millennia. These analyses reveal distinct source mixtures and demonstrate the sensitivity of lake records to basin sediment dynamics. In particular, substantial proportions of elevated metal concentrations in these lake systems seem to arise from soil contributions more than from atmospheric deposition of smelting emissions. The largest soil contributions seem to be in Erhai, a lake with erosion prone soils closely "connected" to the lake. Moreover, these invesigations illustrate the potential for mixing approaches to accommodate and clarify uncertainties in metal source and extraction as differences in extraction efficiency can be incorporated into source uncertainty estimates. Ultimately, these approaches emphasize the need to account for fluvial metal transport in interpretation of sediment histories.

Contrasting ecosystem responses to climatic events and human activity revealed by a sedimentary record from Lake Yilong, southwestern China.

Global climate change and human activities have significantly impacted lake ecosystems at an accelerating rate in recent decades, but the differences between the responses of lake ecosystems to these two stressors remain unclear. Thus an improved understanding of the long-term influences of climatic and anthropogenic disturbances is necessary for the management of lake ecosystems. In order to address these issues, a sedimentary record was obtained from Lake Yilong in Yunnan Province in southwestern China, where the climate and natural environment are dominated by the Indian Summer Monsoon and there is a long history of human occupation and intensive human activity. The chronology is based on AMS 14C dates from 13 samples of plant macrofossils and charcoal, which show that the record spans the last ~12,000 yr. Geochemical indices were used to reconstruct hydro-climatic variations and lake ecosystem responses. The results indicate that a cold and humid climate prevailed from the late Pleistocene to the beginning of the Holocene, which was interrupted by an abrupt decrease in precipitation during 9.7-8.7 ka (1 ka = 1000 cal yr BP, corresponding to the 9.3 ka event). A persistent drying trend occurred during the middle and late Holocene, and there was an increase in the intensity of human activity during the past 1500 years. A comparison of the effects of a natural climatic event and human disturbance reveals contrasting lake ecosystem responses. The lake ecosystem was resilient to the 9.3 ka event and subsequently recovered; however, long-term human activity in the watershed, including deforestation and cultivation, reduced the stability of the lake ecosystem and positive feedback effects were strengthened, leading to the deviation of the system far from its previous stable state. It is concluded that, compared to climate change, human activities have had a much more serious impact on lake ecosystem.

Severe Little Ice Age drought in the midcontinental United States during the Mississippian abandonment of Cahokia.

Drought has long been suspected as playing an important role in the abandonment of pre-Columbian Native American settlements across the midcontinental United States between 1350 and 1450 CE. However, high-resolution paleoclimatic reconstructions reflecting local effective moisture (the ratio of precipitation to evaporation) that are located in proximity to Mississippi period (1050-1450 CE) population centers are lacking. Here, we present a 1600-year-long decadally resolved oxygen isotope (δ18O) record from Horseshoe Lake (Collinsville, IL), an evaporatively influenced oxbow lake that is centrally located within the largest and mostly densely populated series of Mississippian settlements known as Greater Cahokia. A shift to higher δ18O in the Horseshoe Lake sediment record from 1200 to 1400 CE indicates that strongly evaporative conditions (i.e., low effective moisture) were persistent during the leadup to Cahokia's abandonment. These results support the hypothesis that climate, and drought specifically, strongly impacted agriculturally based pre-Columbian Native American cultures in the midcontinental US and highlights the susceptibility of this region, presently a global food production center, to hydroclimate extremes.