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Dechloranes, like Dechlorane Plus® are commonly used flame retardants identified by the EU as substances of very high concern (SVHC) because of their persistence and bioaccumulation potential. To characterize the dechlorane exposure of Germans in the last two decades, 180 archived blood plasma samples of the German Environmental Specimen Bank (students aged 20-29 years) collected at six time points between 1995 and 2017 were analyzed for four dechloranes; namely Dechlorane Plus® (syn- and anti-DDC-CO), dechlorane 602 (DDC-DBF), and dechlorane 603 (DDC-Ant). These were quantified using a GC-MS/MS method. Overall, anti- and syn-DDC-CO were detected in 88% and 98% of the samples, whereas DDC-DBF and DDC-Ant were found in 40% and 37% of the samples, respectively. The median (95th percentile) values were 1.0 ng/g lipid weight (l.w.) (3.0 ng/g l.w.). for anti-DDC-CO, 0.6 ng/g l.w (1.9 ng/g l.w.). for syn-DDC-CO, 0.1 ng/g l.w (0.6 ng/g l.w.). for DDC-DBF, and 0.1 ng/g l.w (0.2 ng/g l.w.). for DDC-Ant. The 95th percentile concentrations of the sum of syn- and anti-DDC-CO decreased from 4.2 ng/g l.w. in 1995, to 2.9 ng/g l.w. in 1999, and subsequently increased to 3.7 ng/g l.w. in 2008, and up to 5.9 ng/g l.w. in 2017. A statistically significant decrease with time was observed for DDC-DBF and DDC-Ant, but not for DDC-CO. Our medians found in blood samples in 2017 are similar to those observed in Germany in 2013/14, but higher compared to values reported in other European countries. Overall, more toxicological and monitoring data is needed to better characterize the potential impact on health., (Copyright © 2020 Elsevier GmbH. All rights reserved.)

Frequent and persistent heavy metal pollution has profound effects on the composition and activity of microbial communities. Heavy metals select for metal resistance but can also co-select for resistance to antibiotics, which is a global health concern. We here document metal concentration, metal resistance and antibiotic resistance along a sediment archive from a pond in the North West of the United Kingdom covering over a century of anthropogenic pollution. We specifically focus on zinc, as it is a ubiquitous and toxic metal contaminant known to co-select for antibiotic resistance, to assess the impact of temporal variation in heavy metal pollution on microbial community diversity and to quantify the selection effects of differential heavy metal exposure on antibiotic resistance. Zinc concentration and bioavailability was found to vary over the core, likely reflecting increased industrialisation around the middle of the 20th century. Zinc concentration had a significant effect on bacterial community composition, as revealed by a positive correlation between the level of zinc tolerance in culturable bacteria and zinc concentration. The proportion of zinc resistant isolates was also positively correlated with resistance to three clinically relevant antibiotics (oxacillin, cefotaxime and trimethoprim). The abundance of the class 1 integron-integrase gene, intI1, marker for anthropogenic pollutants correlated with the prevalence of zinc- and cefotaxime resistance but not with oxacillin and trimethoprim resistance. Our microbial palaeontology approach reveals that metal-contaminated sediments from depths that pre-date the use of antibiotics were enriched in antibiotic resistant bacteria, demonstrating the pervasive effects of metal-antibiotic co-selection in the environment., (Copyright © 2019 The Authors. Published by Elsevier Ltd.. All rights reserved.)

Lead pollution in Arctic ice reflects midlatitude emissions from ancient lead-silver mining and smelting. The few reported measurements have been extrapolated to infer the performance of ancient economies, including comparisons of economic productivity and growth during the Roman Republican and Imperial periods. These studies were based on sparse sampling and inaccurate dating, limiting understanding of trends and specific linkages. Here we show, using a precisely dated record of estimated lead emissions between 1100 BCE and 800 CE derived from subannually resolved measurements in Greenland ice and detailed atmospheric transport modeling, that annual European lead emissions closely varied with historical events, including imperial expansion, wars, and major plagues. Emissions rose coeval with Phoenician expansion, accelerated during expanded Carthaginian and Roman mining primarily in the Iberian Peninsula, and reached a maximum under the Roman Empire. Emissions fluctuated synchronously with wars and political instability particularly during the Roman Republic, and plunged coincident with two major plagues in the second and third centuries, remaining low for >500 years. Bullion in silver coinage declined in parallel, reflecting the importance of lead-silver mining in ancient economies. Our results indicate sustained economic growth during the first two centuries of the Roman Empire, terminated by the second-century Antonine plague., Competing Interests: The authors declare no conflict of interest.

One of the major classes of pesticides is that of the organophosphates (OPs). Initial developments date back almost 2 centuries but it was only in the mid-1940s that OPs reached a prominent status as insecticides, a status that, albeit declining, is still ongoing. OPs are highly toxic to nontarget species including humans, the primary effects being an acute cholinergic toxicity (responsible for thousands of poisoning each year) and a delayed polyneuropathy. Several issues of current debate and investigation on the toxicology of OPs are discussed in this brief review. These include (1) possible additional targets of OPs, (2) OPs as developmental neurotoxicants, (3) OPs and neurodegenerative diseases, (4) OPs and the "aerotoxic syndrome," (5) OPs and the microbiome, and (6) OPs and cancer. Some of these issues have been debated and studied for some time, while others are newer, suggesting that the study of the toxicology of OPs will remain an important scientific and public health issue for years to come.

Recent decades have seen a rapid increase in reported toxic effects of drugs and pollutants on mitochondria. Researchers have also documented many genetic differences leading to mitochondrial diseases, currently reported to affect ∼1 person in 4,300, creating a large number of potential gene-environment interactions in mitochondrial toxicity. We briefly review this history, and then highlight cutting-edge areas of mitochondrial research including the role of mitochondrial reactive oxygen species in signaling; increased understanding of fundamental biological processes involved in mitochondrial homeostasis (DNA maintenance and mutagenesis, mitochondrial stress response pathways, fusion and fission, autophagy and biogenesis, and exocytosis); systemic effects resulting from mitochondrial stresses in specific cell types; mitochondrial involvement in immune function; the growing evidence of long-term effects of mitochondrial toxicity; mitochondrial-epigenetic cross-talk; and newer approaches to test chemicals for mitochondrial toxicity. We also discuss the potential importance of hormetic effects of mitochondrial stressors. Finally, we comment on future areas of research we consider critical for mitochondrial toxicology, including increased integration of clinical, experimental laboratory, and epidemiological (human and wildlife) studies; improved understanding of biomarkers in the human population; and incorporation of other factors that affect mitochondria, such as diet, exercise, age, and nonchemical stressors.

The history of H 2 S - as an environmental toxin - dates back to 1700, to the observations of the Italian physician Bernardino Ramazzini, whose book "De Morbis Artificum Diatriba" described the painful eye irritation and inflammation of "sewer gas" in sewer workers. The gas has subsequently been identified as hydrogen sulfide (H 2 S), and opened three centuries of research into the biological roles of H 2 S. The current article highlights the key discoveries in the field of H 2 S research, including (a) the toxicological studies, which characterized H 2 S as an environmental toxin, and identified some of its modes of action, including the inhibition of mitochondrial respiration; (b) work in the field of bacteriology, which, starting in the early 1900s, identified H 2 S as a bacterial product - with subsequently defined roles in the regulation of periodontal disease (oral bacterial flora), intestinal epithelial cell function (enteral bacterial flora) as well as in the regulation of bacterial resistance to antibiotics; and (c), work in diverse fields of mammalian biology, which, starting in the 1940s, identified H 2 S as an endogenous mammalian enzymatic product, the functions of which - among others, in the cardiovascular and nervous system - have become subjects of intensive investigation for the last decade. The current review not only enumerates the key discoveries related to H 2 S made over the last three centuries, but also compiles the most frequently cited papers in the field which have been published over the last decade and highlights some of the current 'hot topics' in the field of H 2 S biology., (Copyright © 2017 Elsevier Inc. All rights reserved.)

The use of alkyl lead derivatives as antiknock agents in gasoline can be considered as one of the main pollution disasters of the 20th century because of both the global character of the pollution emitted and the seriousness of the impact on human health. Alkyl lead derivatives in themselves cannot be considered to be persistent pollutants because they readily degrade either before being released from the tailpipes or soon afterwards in the atmosphere. However, the inorganic lead they produced has been deposited in soils all over the planet, largely, but not exclusively in urban areas and along motorways, since the direct emission of lead into the atmosphere favored its dispersal over great distances: The signal of the massive use of alkyl lead derivatives has been found all over the world, including in remote sites such as polar areas. The short residence time of lead in the atmosphere implies that this compartment is highly responsive to changes in emissions. This was demonstrated when leaded gasoline was phased-out and is in striking contrast to the very long permanence of inorganic lead in soils, where resuspension is a permanent source of toxic lead.

Polychlorinated biphenyls (PCBs) were quantified in 18 surface sediment samples, 1 sediment core, and several mangrove tissue samples collected in Jobos Bay, Puerto Rico in September 2013. Total PCBs in surface sediments ranged from 0.42 to 1232ngg -1 dw. Generally, higher levels were observed near-shore close to urban and industrial areas. The levels suggest significant pollution in Jobos Bay with respect to PCBs. Two-thirds of the sites were dominated by lighter PCB congeners (tri- to penta-chlorinated PCBs) while one-third had heavy PCB congeners (hexa- to octa-chlorinated PCBs) dominant. Total PCBs in a sediment core indicated levels fluctuating according to historical usage patterns. Total PCBs were measured in mangal leaves (14-747ngg -1 dw), roots (0.26-120ngg -1 dw), and seeds (16-93ngg -1 dw), suggesting bioaccumulation from sediments. This is the first report of a historical profile of PCBs in the study area and of PCB bioaccumulation in mangroves. This article provides new and useful information on PCBs in the Caribbean area of the GRULAC region., (Copyright © 2016 Elsevier B.V. All rights reserved.)

Reconstructing trace metal historical trends are essential for better understanding anthropogenic impact on remote alpine ecosystems. We present results from an alpine lake sediment from the Eastern Tibetan Plateau to decipher the accumulation history of cadmium (Cd), lead (Pb) and zinc (Zn) over last century, from the preindustrial to the modern period. Cd, Pb and Zn in the sediment of Caohaizi Lake clearly suffered from atmospheric deposition, and the mining and smelting were regarded as the main anthropogenic sources. Since the mid-1990s, over 80% of trace metals were quantified from anthropogenic emissions. The temporal trends of anthropogenic metal fluxes showed that the contamination history of Pb was earlier than that of Cd and Zn, which was in agreement with the regional Pb emission history, but lagged behind the Pb decline in Europe and North America. The fluxes of anthropogenic Cd and Zn were relatively constant until the 1980s, increased sharply between the 1980s and the mid-1990s, and then kept the high values. The anthropogenic fluxes of Pb showed a marked rise around 1950, and increased sharply in the 1980s. In the mid-1990s, this flux reached the peak, and then decreased gradually. The Pb deposition flux at present in comparison with other lake records in the areas of Tibetan Plateau further demonstrated that trace metals in the Caohaizi Lake region were probably from Southwest China and South Asia. Economic development in these regions still puts pressure on the remote alpine ecosystems, and thus the impact of trace metals merits more attention., (Copyright © 2016 Elsevier Ltd. All rights reserved.)

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.

The concentrations of As, Sb, Hg, Pb, Cd, and Ba in the surface and core sediments of the oil and gas producing region of the Beibu Gulf were measured by Inductively Coupled Plasma Optical Emission Spectrometry (ICP-OES), Inductively Coupled Plasma Mass Spectrometry (ICP-MS) and Atomic Fluorescence Spectrometry (AFS), and the spatial distribution and historical trends of these elements are discussed. The results show that the concentrations of these elements are highest near the platforms. The results of Enrichment Factor (EF) and Potential Ecological Risk Index (PERI) also reveal significantly higher enrichment around the platforms, which imply that the offshore petroleum production was the cause of the unusual distribution and severe enrichment of these elements in the study area. The environment around the platforms was highly laden with toxic elements, thereby representing a very high ecological risk to the environment of the study area., (Copyright © 2014 Elsevier Ltd. All rights reserved.)

Litigation drives extensive historical research but often allows only select observers to see the results. Historians have conducted untold studies for litigation that become "secret histories" because these histories are not published. An example is the historical use and regulation of the chemical trichloroethylene (TCE), a hazardous chemical at issue in much environmental litigation, but a topic virtually absent in the secondary literature. This practice seems to contravene accepted standards of open scholarship. Although not directly aligned with the traditional academic model of historical practice, however, historical research and writing for litigation achieve legitimate and important results without abandoning the discipline's professional standards. History done by consultants for litigation is neither a history of compromised standards nor as "secret" as feared.

The European Variant Berkeley Trent (EVn-BETR) multimedia fugacity model is used to test the validity of previously derived emission estimates and predict environmental concentrations of the main decabromodiphenyl ether congener, BDE-209. The results are presented here and compared with measured environmental data from the literature. Future multimedia concentration trends are predicted using three emission scenarios (Low, Realistic and High) in the dynamic unsteady state mode covering the period 1970-2020. The spatial and temporal distributions of emissions are evaluated. It is predicted that BDE-209 atmospheric concentrations peaked in 2004 and will decline to negligible levels by 2025. Freshwater concentrations should have peaked in 2011, one year after the emissions peak with sediment concentrations peaking in 2013. Predicted atmospheric concentrations are in good agreement with measured data for the Realistic (best estimate of emissions) and High (worst case scenario) emission scenarios. The Low emission scenario consistently underestimates measured data. The German unilateral ban on the use of DecaBDE in the textile industry is simulated in an additional scenario, the effects of which are mainly observed within Germany with only a small effect on the surrounding areas. Overall, the EVn-BTER model predicts atmospheric concentrations reasonably well, within a factor of 5 and 1.2 for the Realistic and High emission scenarios respectively, providing partial validation for the original emission estimate. Total mean MEC:PEC shows the High emission scenario predicts the best fit between air, freshwater and sediment data. An alternative spatial distribution of emissions is tested, based on higher consumption in EBFRIP member states, resulting in improved agreement between MECs and PECs in comparison with the Uniform spatial distribution based on population density. Despite good agreement between modelled and measured point data, more long-term monitoring datasets are needed to compare predicted trends in concentration to determine the rate of change of POPs within the environment., (Copyright © 2014 Elsevier Ltd. All rights reserved.)

Quantifying the competing rates of intake and elimination of persistent organic pollutants (POPs) in the human body is necessary to understand the levels and trends of POPs at a population level. In this paper we reconstruct the historical intake and elimination of ten polychlorinated biphenyls (PCBs) and five organochlorine pesticides (OCPs) from Australian biomonitoring data by fitting a population-level pharmacokinetic (PK) model. Our analysis exploits two sets of cross-sectional biomonitoring data for PCBs and OCPs in pooled blood serum samples from the Australian population that were collected in 2003 and 2009. The modeled adult reference intakes in 1975 for PCB congeners ranged from 0.89 to 24.5ng/kgbw/day, lower than the daily intakes of OCPs ranging from 73 to 970ng/kgbw/day. Modeled intake rates are declining with half-times from 1.1 to 1.3years for PCB congeners and 0.83 to 0.97years for OCPs. The shortest modeled intrinsic human elimination half-life among the compounds studied here is 6.4years for hexachlorobenzene, and the longest is 30years for PCB-74. Our results indicate that it is feasible to reconstruct intakes and to estimate intrinsic human elimination half-lives using the population-level PK model and biomonitoring data only. Our modeled intrinsic human elimination half-lives are in good agreement with values from a similar study carried out for the population of the United Kingdom, and are generally longer than reported values from other industrialized countries in the Northern Hemisphere., (Copyright © 2014. Published by Elsevier Ltd.)

We identify eleven emission sources of perfluoroalkyl carboxylic acids (PFCAs) that have not been discussed in the past. These sources can be divided into three groups: [i] PFCAs released as ingredients or impurities, e.g., historical and current use of perfluorobutanoic acid (PFBA), perfluorohexanoic acid (PFHxA) and their derivatives; [ii] PFCAs formed as degradation products, e.g., atmospheric degradation of some hydrofluorocarbons (HFCs) and hydrofluoroethers (HFEs); and [iii] sources from which PFCAs are released as both impurities and degradation products, e.g., historical and current use of perfluorobutane sulfonyl fluoride (PBSF)- and perfluorohexane sulfonyl fluoride (PHxSF)-based products. Available information confirms that these sources were active in the past or are still active today, but due to a lack of information, it is not yet possible to quantify emissions from these sources. However, our review of the available information on these sources shows that some of the sources may have been significant in the past (e.g., the historical use of PFBA-, PFHxA-, PBSF- and PHxSF-based products), whereas others can be significant in the long-term (e.g., (bio)degradation of various side-chain fluorinated polymers where PFCA precursors are chemically bound to the backbone). In addition, we summarize critical knowledge and data gaps regarding these sources as a basis for future research., (Copyright © 2014 Elsevier Ltd. All rights reserved.)

Relative contributions of polycyclic aromatic hydrocarbons (PAHs) from combustion sources of wood, petroleum, and coal were computed in sediments from Central Park Lake in New York City (NY, USA) by chemical mass balance based on several reliable source indicators. These indicators are the ratio of retene to the sum of retene and chrysene, the ratio of 1,7-dimethylphenanthrene (DMP) to 1,7-DMP and 2,6-DMP, and the ratio of fluroanthene to fluroanthene and pyrene. The authors found that petroleum combustion-derived PAH fluxes generally followed the historical consumption data of New York State. Coal combustion-derived PAH flux peaked approximately in the late 1910s, remained at a relatively high level over the next 3 decades, then rapidly declined from the 1950s to the 1960s; according to historical New York State coal consumption data, however, there was a 2-peak trend, with peaks around the early 1920s and the mid-1940s. The 1940s peak was not observed in Central Park Lake, most likely because of the well-documented shift from coal to oil as the major residential heating fuel in New York City during the late 1930s. It was widely believed that the decreased PAH concentrations and fluxes in global sediments during the last century resulted from a major energy shift from coal to petroleum. The data, however, show that this shift occurred from 1945 through the 1960s and did not result in an obvious decline. The sharpest decrease, which occurred in the 1970s was not predominantly related to coal usage but rather was the result of multiple factors, including a decline in petroleum usage largely, the introduction of low sulfur-content fuel in New York City, and the introduction of emission-control technologies., (© 2013 SETAC.)

It may be a coincidence, but it is a fact that the first clear characterization of hay fever began in England where modern industrialization started in Europe. Only at the end of the 20th century were associations of the increasing prevalence of allergy with outdoor air pollution discussed. The seminal study came from Japan from the group of T. Miyamoto linking the increase in Japanese cedar pollinosis to an increased prevalence of Diesel cars and probably exposure to Diesel exhaust in epidemiological, animal experimental and in vitro studies. In Germany first epidemiological studies were done in North Rhine-Westphalia and Bavaria in 1987 and 1988 showing a striking prevalence of allergic disease of up to 10-20% in preschool children. After German reunification the most surprising observation was a lower prevalence of hay fever in East German children compared to the West, although there was a much higher air pollution with SO2 and large particulate matter. Modern smog as found over West German cities most likely originating from traffic exhaust and consisting of fine and ultrafine particles was shown to be associated with higher incidence rates of allergy and allergic sensitization. In the 10 years after reunification there was a steep increase of allergy prevalence in East German children reaching almost the same level as in West Germany. Obviously, a multitude of lifestyle factors - beyond air pollution - may be involved in the explanation of this phenomenon. Surprisingly the skin manifestation of atopy, namely atopic eczema, was more frequent in East German children compared to the West, thus differing from airway allergy. Meanwhile in vitro studies and animal experiments have shown that a variety of air pollutants mostly from environmental tobacco smoke (indoors) and from traffic exhaust (outdoors) can stimulate immune cells inducing a Th2-dominated response besides their irritative effects. While 50 years ago in allergy textbooks a clear distinction was made between 'toxic' or 'allergic', the newly developed concept of allergotoxicology has stimulated research tremendously, meaning 'the investigation of effects of toxic substances upon the induction, elicitation and maintenance of allergic reactions'., (© 2014 S. Karger AG, Basel.)

Atmospheric particle associated with pyrogenic polycyclic aromatic hydrocarbons (PAHs) poses serious threats to human health by inhalation exposure, especially in semiarid areas. Hence, the distributions of PAHs and particle size in two core sediments collected from Lake Lianhuan, Northeast China were studied. The sediments were dated radiometrically, and particle size distribution and PAH concentration were evaluated and potential human health risk was assessed. From 1980 to 2007, the dominant PAHs in the two cores were 2- and 3-ring PAHs, and the concentrations of 3-6 ring PAHs gradually increased from the early 1990s. Diagnostic ratios indicated that pyrogenic PAHs were the main sources of PAHs which changed over time from combustions of wood and coal to liquid fossil fuel sources. Fine particles (<65 μm) were the predominant particle size (56-97%). Lacustrine source (with the peak towards 200-400 μm) and eolian sources derived from short (2.0-10 and 30-65 μm) and long (0.4-1.0 μm) distance suspension were indentified from frequency distribution pattern of particle size. Significant correlations between 3-6 ring PAHs (especially carcinogenic 5-6 ring PAHs) and 10-35 μm particulate fractions indicated that eolian particles played an important role in adsorbing pyrogenic PAHs. Petroleum source of PAHs was only identified during the 1980s in one core sediments, in which positive correlations between 2-ring PAHs and particulate fractions of >125 μm were found. Future research should focus on the seven carcinogenic pyrogenic PAHs due to a rapidly increasing trend since 1995 based on the assessment of toxic equivalency factors., (Copyright © 2013 Elsevier B.V. All rights reserved.)

Legacy organochlorine contaminants were determined in adipose tissues from 294 polar bears (Ursus maritimus) sampled in East Greenland in 23 of the 28years between 1983 and 2010. Of 19 major legacy contaminants and congeners (ΣPCB, 4 PCB congeners (CB153, 180, 170/190), ΣDDT, p,p'-DDE, p,p' -DDD and p,p'-DDT, α- and β-hexachlorocyclohexane (HCH), HCB, octachlorostyrene, dieldrin, oxychlordane, cis- and trans-chlordane, cis- and trans-nonachlor, heptachlor epoxide and BB-153), 18 showed statistically significant average yearly declines of -4.4% (range: -2.0 to -10.8%/year) among subadult polar bears (i.e. females<5years, males<6years). For example, the ∑PCB concentrations declined 2.7 fold from 22730ng/g lw (95% C.I.: 12470-32990ng/g lw) in 1983-1986 to 8473ng/g lw (95% C.I.: 6369-9776ng/g lw) in 2006-2010. Similar but fewer statistically significant trends were found for adult females and adult males likely due to smaller sample size and years. Despite declines as a result of international regulations, relatively high levels of these historic pollutants persist in East Greenland polar bear tissues., (Copyright © 2012 Elsevier Ltd. All rights reserved.)

The German system of a health-related environmental monitoring is based upon two instruments: The German Environmental Survey (GerES) and the Environmental Specimen Bank (ESB). The ESB is a tool to describe time trends of human exposure. Each year approx. 500 students from 4 sampling locations are analysed for their heavy metal contents in blood, blood plasma, and urine. GerES is a nationwide representative cross-sectional study that has been conducted four times up to now. Both instruments have been used to measure heavy metals over the last decades and thus provide complementary information. Both instruments are useful to describe time trends. However, combining the two has an added value, which is demonstrated for heavy metals for the first time in this paper. Major results and the changing importance of sources of exposure to heavy metals (Pb, Cd, Hg, Au, Pt, U and Ni) are shown. This leads to the following conclusion about the today's relevance of exposure in Germany. For the study participants of the city of Muenster, lead in whole blood decreased from about 70 μg/l in 1981 to levels below 15 μg/l in 2009. GerES data of young adults confirmed this time trend and GerES IV on children revealed the decreasing relevance of lead in outdoor air and in drinking water. The concentrations of mercury in urine decreased because in Germany it is no longer recommended to use amalgam fillings for children. However, GerES IV and ESB data also demonstrate that despite the decline of these heavy metals exposures to nickel and uranium originating from drinking water are still of importance., (Copyright © 2013 Elsevier GmbH. All rights reserved.)

Human mobilization and use of reactive nitrogen (Nr) has been one of the major aspects of global change over the past century. Nowhere has that change been more dramatic than in China, where annual net Nr creation increased from 9.2 to 56 Tg from 1910 to 2010. Since 1956, anthropogenic Nr creation exceeded natural Nr creation, contributing over 80% of total Nr until 2010. There is great interest and uncertainty in the fate and effects of this Nr in China. Here, a comprehensive inventory of Nr in China shows that Nr (including recycled Nr) has continuously and increasingly accumulated on land (from 17 to 45 Tg), accompanied by increasing transfers to the atmosphere (before deposition; from 7.6 to 20 Tg), inland waters (from 2.7 to 9.6 Tg), and coastal waters (from 4.5 to 7.7 Tg) over the past 30 y. If current trends continue, Nr creation from human activities will increase to 63 Tg by 2050, raising concerns about deleterious environmental consequences for land, air, and water at regional and global scales. Tremendous amounts of Nr have accumulated in plants, soils, and waters in China over the past 30 y, but the retention capacity of the terrestrial landscape seems to be declining. There is a possibility that the negative environmental effects of excessive Nr may accelerate in coming decades, increasing the urgency to alter the trajectory of increasing Nr imbalance. Here, a conceptual framework of the relationships between human drivers and Nr cycling in China is oriented and well-targeted to Chinese abatement strategies for Nr environmental impact.

Rachel Carson's Silent Spring is often depicted as the beginning of a broad societal concern about the dangers of DDT and other pesticides. Attention to the other chlorinated hydrocarbons, specifically PCBs, is seen as an outgrowth of the late 1960s environmental movement. Carson's work was clearly critical in broadening the history to include the environmental impact and set the stage for the path breaking work decades later by Theo Colburn and others on endocrine disruptions associated with other synthetic chemicals. This article reviews the development of the understanding the dangers of the chlorinated hydrocarbons in the decades preceding Carson's book. Although little noticed, Rachel Carson makes this observation herself., (Copyright © 2012 Elsevier Inc. All rights reserved.)

(210)Pb-dated sediment cores taken from lakes on the Falkland Islands, the South Orkney Islands, and the Larsemann Hills in Antarctica were analyzed for fly ash particles to assess the temporal record of contamination from high temperature fossil-fuel combustion sources. Very low, but detectable, levels were observed in the Antarctic lakes. In the Falkland Island lakes, the record of fly ash extended back to the late-19th century and the scale of contamination was considerably higher. These data, in combination with meteorological, modeling, and fossil-fuel consumption data, indicate most likely sources are in South America, probably Chile and Brazil. Other southern hemisphere sources, notably from Australia, contribute to a background contamination and were more important historically. Comparing southern polar data with the equivalent from the northern hemisphere emphasizes the difference in contamination of the two circumpolar regions, with the Falkland Island sites only having a level of contamination similar to that of northern Svalbard.

A tension exists between damage caused to the environment by novel chemicals and the advance in industrial and economic progress based on the same products. This was brought to the fore in Rachel Carson's Silent Spring. However, this was not altogether a new story. For some, such as Robert Angus Smith, concerns arose in the nineteenth century with the polluting vapours from chemical processes. Smith and colleagues in the Alkali Inspectorate, with support from medical officers of health and occupational health officers, exercised vigilance and diligence to ensure wider and tighter regulations in order to protect workers and the public. This article reviews the changes in British regulatory approaches adopted during the second half of the nineteenth century in response to the increasing proliferation of harmful chemicals released into the environment.

Human activities have significantly altered atmospheric Pb concentrations and thus, its geochemical cycle, for thousands of years. Whereas historical Pb emissions from Western Europe, North America, and Asia are well documented, there is no equivalent data for Eastern Europe. Here, we present ice-core Pb concentrations for the period 1680-1995 from Belukha glacier in the Siberian Altai, assumed to be representative of emissions in Eastern Europe and the Altai. Pb concentrations and (207)Pb/(206)Pb ratios were strongly enhanced during the period 1935-1995 due to the use of Pb additives in Russian gasoline mined in the Rudny Altai. Comparable to Western Europe and North America, Eastern European Pb emissions peaked in the 1970s. However, the subsequent downward trend in Eastern Europe was mainly caused by the economic crisis in the U.S.S.R. and not by a phase-out of leaded gasoline. Pb concentrations in the period 1680-1935, preceding the era of intensified industrialization in Russia, reflect the history of local emissions from Rudny Altai mining and related metallurgical processing primarily for the production of Russian coins. During this time, Altai ore Pb contributed about 40% of the regional atmospheric Pb.

Clair Patterson and colleagues demonstrated already four decades ago that the lead cycle was greatly altered on a global scale by humans. Moreover, this change occurred long before the implementation of monitoring programs designed to study lead and other trace metals. Patterson and colleagues also developed stable lead isotope analyses as a tool to differentiate between natural and pollution-derived lead. Since then, stable isotope analyses of sediment, peat, herbaria collections, soils, and forest plants have given us new insights into lead biogeochemical cycling in space and time. Three important conclusions from our studies of lead in the Swedish environment conducted over the past 15 years, which are well supported by extensive results from elsewhere in Europe and in North America, are: (1) lead deposition rates at sites removed from major point sources during the twentieth century were about 1,000 times higher than natural background deposition rates a few thousand years ago (~10 mg Pb m(-2) year(-1) vs. 0.01 mg Pb m(-2) year(-1)), and even today (~1 mg Pb m(-2) year(-1)) are still almost 100 times greater than natural rates. This increase from natural background to maximum fluxes is similar to estimated changes in body burdens of lead from ancient times to the twentieth century. (2) Stable lead isotopes ((206)Pb/(207)Pb ratios shown in this paper) are an effective tool to distinguish anthropogenic lead from the natural lead present in sediments, peat, and soils for both the majority of sites receiving diffuse inputs from long range and regional sources and for sites in close proximity to point sources. In sediments >3,500 years and in the parent soil material of the C-horizon, (206)Pb/(207)Pb ratios are higher, 1.3 to >2.0, whereas pollution sources and surface soils and peat have lower ratios that have been in the range 1.14-1.18. (3) Using stable lead isotopes, we have estimated that in southern Sweden the cumulative anthropogenic burden of atmospherically deposited lead is ~2-5 g Pb m(-2) and ~1 g Pb m(-2) in the "pristine" north. Half of this cumulative total was deposited before industrialization. (4) In the vicinity of the Rönnskär smelter in northern Sweden, a major point source during the twentieth century, there is an isotopic pattern that deviates from the general trends elsewhere, reflecting the particular history of ore usage at Rönnskär, which further demonstrates the chronological record of lead loading recorded in peat and in soil mor horizons.

The element phosphorus has no substitute in sustaining all life and food production on our planet. Yet today's phosphorus use patterns have resulted in both a global environmental epidemic of eutrophication and led to a situation where the future availability of the world's main sources of phosphorus is uncertain. This paper examines the important history of human interference with the phosphorus cycle from initial discovery to present, highlighting key interrelated events and consequences of the Industrial Revolution, Sanitation Revolution and Green Revolution. Whilst these events led to profound advances in technology, public health and food production, they have fundamentally broken the global phosphorus cycle. It is clear a 'Fourth Revolution' is required to resolve this dilemma and ensure humanity can continue to feed itself into the future while protecting environmental and human health., (Copyright © 2011 Elsevier Ltd. All rights reserved.)

Methylmercury cycling in the Pacific Ocean has garnered significant attention in recent years, especially with regard to rising mercury emissions from Asia. Uncertainty exists concerning whether increases in anthropogenic emissions over time may have caused increased mercury bioaccumulation in the biota. To address this, we measured total mercury and, for a subset of samples, methylmercury (the bioaccumulated form of mercury) in museum feathers from an endangered seabird, the black-footed albatross (Phoebastria nigripes), spanning a 120-y period. We analyzed stable isotopes of nitrogen (δ(15)N) and carbon (δ(13)C) to control for temporal changes in trophic structure and diet. In post-1940 and -1990 feathers, we detected significantly higher mean methylmercury concentrations and higher proportions of samples exhibiting above deleterious threshold levels (∼ 40,000 ng · g(-1)) of methylmercury relative to prior time points, suggesting that mercury toxicity may undermine reproductive effort in the species. We also found higher levels of (presumably curator-mediated) inorganic mercury in older specimens of albatross as well as two nonpelagic species lacking historical exposure to bioavailable mercury, patterns suggesting that studies on bioaccumulation should measure methylmercury rather than total mercury when using museum collections. δ(15)N contributed substantially to models explaining the observed methylmercury variation. After simultaneously controlling for significant trends in δ(13)C over time and δ(15)N with methylmercury exposure, year remained a significant independent covariate with feather methylmercury levels among the albatrosses. These data show that remote seabird colonies in the Pacific basin exhibit temporal changes in methylmercury levels consistent with historical global and recent regional increases in anthropogenic emissions.

Background, Aim, and Scope: In the 50 years or so that polychlorinated biphenyls (PCBs) were manufactured in the USA and elsewhere, they were widely used in numerous applications because of their desirable properties. The purpose of this paper is to review and summarize in one place the factual information about the uses of PCBs, as well as to correct some misconceptions that have arisen over the years. The focus is on applications in the USA for which there is ample documentation. However, use patterns were probably similar worldwide., Materials and Methods: Review., Results: PCBs were used primarily as electrical insulating fluids in capacitors and transformers and also as hydraulic, heat transfer, and lubricating fluids. PCBs were blended with other chemicals as plasticizers and fire retardants and used in a range of products including caulks, adhesives, plastics, and carbonless copy paper. In the USA, PCBs were manufactured from 1929 through mid-1977, although many products remained in service for decades after the manufacture of PCBs was terminated. This article reviews the historic uses of PCBs in the USA and discusses, where possible, the relative sales volumes. Especially with smaller volume, military, and third-party uses, documenting a use and/or differentiating between a commercial use and an experimental test batch is not possible., Discussion: A major contribution of this paper is to differentiate reported commercial applications of PCBs that can be documented from those which cannot. Undocumented uses may include actual minor uses as well as reported applications that are unlikely ever to have been commercialized.

Between 1950 and 1963 approximately 11 million kilograms of mercury (Hg) were used at the Oak Ridge Y-12 National Security Complex (Y-12 NSC) for lithium isotope separation processes. About 3% of the Hg was lost to the air, soil and rock under facilities, and East Fork Poplar Creek (EFPC) which originates in the plant site. Smaller amounts of Hg were used at other Oak Ridge facilities with similar results. Although the primary Hg discharges from Y-12 NSC stopped in 1963, small amounts of Hg continue to be released into the creek from point sources and diffuse contaminated soil and groundwater sources within Y-12 NSC. Mercury concentration in EFPC has decreased 85% from ∼2000 ng/L in the 1980s. In general, methylmercury concentrations in water and in fish have not declined in response to improvements in water quality and exhibit trends of increasing concentration in some cases., (Published by Elsevier Ltd.)

Here I explore how the experience of place at a First Nations reserve in Ontario, located in the middle of Canada's "Chemical Valley," is disrupted by the extraordinary levels of pollution found there. In so doing, I give special attention to air pollution and residents' responses to associated odors - that is, to the sense of smell. Focusing on a unique feature of smell - that it operates primarily through indexicality - I draw on C. S. Peirce's semiotic framework to highlight ways in which perception of odors entails embodiment of the perceived substance, thus connecting self and surroundings in profound and transformative ways. Ultimately, I argue that the local smellscape, while having reinforced a sense of positive emplacement on the reserve in the past, is now, because of the constant presence of toxic fumes, instilling in residents a profound sense of alienation from the ancestral landscape - a condition I call "dysplacement."

Bt cotton is accused of being responsible for an increase of farmer suicides in India. In this article, we provide a comprehensive review of evidence on Bt cotton and farmer suicides. Available data show no evidence of a 'resurgence' of farmer suicides. Moreover, Bt cotton technology has been very effective overall in India. Nevertheless, in specific districts and years, Bt cotton may have indirectly contributed to farmer indebtedness, leading to suicides, but its failure was mainly the result of the context or environment in which it was planted.

Mercury has a long history, fascinating in its many aspects. Through the centuries--from ancient times to the present day--the metal in its various forms, also known under the name "quicksilver", accompanied the man and was used for diversified purposes. Today, mercury is employed in manufacturing thermometers, barometers, vacuum pumps and explosives. It is also used in silver and gold mining processes. Mercury compounds play a significant role in dentistry, pharmaceutical industry and crop protection. The contemporary use of mercury markedly decreases, but historically speaking, the archives abound in materials that document facts and events occurring over generations and the immense intellectual effort aiming at discovering the true properties and mechanisms of mercury activity. Mercury toxicity, manifested in destruction of biological membranes and binding of the element with proteins, what disturbs biochemical processes occurring in the body, was discovered only after many centuries of the metal exerting its effect on the lives of individuals and communities. For centuries, mercury was present in the work of alchemists, who searched for the universal essence or quintessence and the so-called philosopher's stone. In the early modern era, between the 16th and 19th centuries, mercury was used to manufacture mirrors. Mercury compounds were employed as a medication against syphilis, which plagued mankind for more than four hundred years--from the Middle Ages till mid 20th century, when the discovery of penicillin became the turning point. This extremely toxic therapy resulted in much suffering, individual tragedies, chronic poisonings leading to fatalities and dramatic sudden deaths. In the last fifty years, there even occurred attempts of mentally imbalanced individuals at injecting themselves with metallic mercury, also as a performance-enhancing drug. Instances of mass mercury poisoning occurred many times in the past in consequence of eating food products poisoned with organic mercury compounds originating from the natural environment.

As the most widely scattered toxic metal in the world, the sources of lead (Pb) observed in contamination investigation are often difficult to identify. This review presents an overview of the principles, analysis, and applications of Pb isotopic fingerprinting in tracing the origins and transport pathways of Pb in the environment. It also summarizes the history and current status of lead pollution in China, and illustrates the power of Pb isotopic fingerprinting with examples of its recent applications in investigating the effectiveness of leaded gasoline phase-out on atmospheric lead pollution, and the sources of Pb found in various environmental media (plants, sediments, and aquatic organisms) in China. The limitations of Pb isotopic fingerprinting technique are discussed and a perspective on its development is also presented. Further methodological developments and more widespread instrument availability are expected to make isotopic fingerprinting one of the key tools in lead pollution investigation., (Copyright 2009 Elsevier Ltd. All rights reserved.)

Radishes cut to look like roses, watermelons carved into fruit baskets, apples made into swans, cakes frosted to look like dolls—when did this game of food masquerade start and how? This essay speculates about food's on-going history of disguise, of pretending to be what it's not. From the Renaissance courtier's delight in confections disguised as beasts, birds, and other fancies to our present day fascination with Japanese bento lunch boxes, food masquerade would seem to be a fanciful part of the history of food.Food masquerade injects some levity into our growing seriousness about food, our suspicion that most supermarket food is riddled with toxins and bad karma. It proposes that eating food should be fun. Food masquerade also gets to the very heart of artistic visual representation: the magical transformation of paint, clay or wood into an image of something else. It is a synecdoche for art itself.

The first health effects of cadmium (Cd) were reported already in 1858. Respiratory and gastrointestinal symptoms occurred among persons using Cd-containing polishing agent. The first experimental toxicological studies are from 1919. Bone effects and proteinuria in humans were reported in the 1940's. After World War II, a bone disease with fractures and severe pain, the itai-itai disease, a form of Cd-induced renal osteomalacia, was identified in Japan. Subsequently, the toxicokinetics and toxicodynamics of Cd were described including its binding to the protein metallothionein. International warnings of health risks from Cd-pollution were issued in the 1970's. Reproductive and carcinogenic effects were studied at an early stage, but a quantitative assessment of these effects in humans is still subject to considerable uncertainty. The World Health Organization in its International Program on Chemical Safety, WHO/IPCS (1992) (Cadmium. Environmental Health Criteria Document 134, IPCS. WHO, Geneva, 1-280.) identified renal dysfunction as the critical effect and a crude quantitative evaluation was presented. In the 1990's and 2000 several epidemiological studies have reported adverse health effects, sometimes at low environmental exposures to Cd, in population groups in Japan, China, Europe and USA (reviewed in other contributions to the present volume). The early identification of an important role of metallothionein in cadmium toxicology formed the basis for recent studies using biomarkers of susceptibility to development of Cd-related renal dysfunction such as gene expression of metallothionein in peripheral lymphocytes and autoantibodies against metallothionein in blood plasma. Findings in these studies indicate that very low exposure levels to cadmium may give rise to renal dysfunction among sensitive subgroups of human populations such as persons with diabetes.

The finding in 1972 of two World War II mustard gas artillery shells in crushed shell sediment dredged in the Faxaflói Bay and transported as raw material for cement production at Akranes (Western Iceland) is reported. One of the shells was wedged in a stone crusher in the raw material processing line and was ruptured. As a result dark fluid with a garlic like smell seeped out from the metal canister. The attending employees believed the metal object to be inert and tried to cut it out with a blow torch. This resulted in the explosion of the shell charge and in the exposure of four employees to mustard gas. All suffered burns on their hands and two of them in the eyes also. The second shell was detonated in the open at a distance from the factory. Emphasis is given to the fact that instant, or at least as soon as possible, cleansing and washing is the most efficient measure to be taken against the debilitating effects of mustard gas. It is also pointed out that the active principle in mustard gas (dichlorodiethyl sulphide) can easily be synthesized and none of the precursor substances are subjected to any restrictions of use. The authors conclude that mustard gas bombs may still be found in the arsenals of some military powers in spite of an international convention that prohibits the production, stockpiling and the use of chemical weapons. Terrorist groups have also seemingly tried to aquire mustard gas bombs and other chemical weapons. Therefore cases of mustard gas poisoning might still occur.

Two sediment cores, one at middle of the bay (core 1) and another at an outfall of a wastewater treatment plant (WWTP; core 2) were collected in Masan Bay, Korea, to investigate the historical records of contamination by polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs), dioxin-like polychlorinated biphenyls (dl-PCBs), and nonylphenols (NPs). Vertical profiles of PCDD/Fs, dl-PCBs, and NPs in the two cores, dated using (210)Pb technique, were different but they had similar vertical profiles within the same core. The overall concentrations of these contaminants were greater in core 2 (0.05-110ng TEQkg(-1) dry wt for PCDD/Fs; 0.02-4.4ng TEQkg(-1) dry wt for dl-PCBs; 1.0-470microgkg(-1) dry wt for NPs) than in core 1 (0.72-8.0ng TEQkg(-1) dry wt for PCDD/Fs; 0.03-1.4ng TEQkg(-1) dry wt for dl-PCBs; 1.3-110microgkg(-1) dry wt for NPs). In particular, PCDD/F concentrations in core 2 were an order of magnitude greater than the concentrations in core 1. The highest concentrations of all target contaminants in cores1 and 2 were found at the surface layer (dated as 2005) and at 8-10cm ( approximately 2000), respectively. For sediment core 2, rapid changes in the concentrations and sources of target contaminants coincide with the establishment and operation of a WWTP; this suggested that discharges from WWTP contributed to contamination by PCDD/Fs, dl-PCBs and NPs in the bay. Analysis of data by non-parametric multidimensional scaling ordination showed that both the cores were influenced by different PCDD/F sources over time. Inventories and fluxes of PCDD/Fs, dl-PCBs, and NPs have rapidly increased since establishment of the WWTP, indicating that the discharge of WWTP is an important source of sediment contamination in aquatic environment.

An assessment of community exposure to 2,3,7,8-tetrachlorodibenzo-p-dioxin (TCDD) was undertaken in Paritutu, New Zealand. The suburb lies adjacent to an agrichemical facility that produced 2,4,5-trichlorophenoxyacetic acid (2,4,5-T), between 1962 and 1987. Soil TCDD measurements from 73 nearby addresses demonstrated a pattern of TCDD deposition consistent with an aerial plume following the prevailing local wind patterns and the agrichemical plant as the point source. Blood samples were taken from 52 volunteers having lived for three or more years in Paritutu between 1962 and 1987. Candidate selection focused primarily on individuals who were most likely to show elevated TCDD blood lipid levels when compared to age and gender stratified national average blood concentrations, and secondarily on individuals that provided additional information about specific exposure periods, potential exposures of younger age groups, and specific dietary patterns. A multipathway exposure model was used to estimate serum TCDD levels in each participant. Age and gender-specific TCDD elimination kinetics were also considered. Historical TCDD environmental concentrations were back-calculated from soil concentrations at each residence assuming TCDD releases occurred pre-dominantly between 1962 and 1975. Serum was analysed for chlorinated dibenzodioxins and dibenzofurans, and a subset was analysed for dioxin-like polychlorinated biphenyls. TCDD in serum lipid exceeded two standard deviations above national background levels for 14 participants, and 3 standard deviations for 10 participants. The highest TCDD lipid concentration was 33.3 ng/kg-lipid, or 11 times higher than the comparative 1997 national average. Elevated TCDD concentrations were observed primarily, but not exclusively, in the older study participants who had been in residence in Paritutu before 1968. The study demonstrated TCDD exposure in this community, occurring most likely through the aerial route, and most probably from fugitive emissions during manufacture.

Editor's Note: This is 1 of 4 papers from the US Environmental Protection Agency Science Advisory Board's Ecological Processes and Effects Committee workshop on the current and future practice of ecological risk assessment. The workshop was held in Washington, DC in February 2006. Risk assessment originated with the insurance industry and spread to the estimation of risks to people and property in other contexts, including the regulation of environmental contamination. Ecological assessment became an important component of environmental management in the United States with the legal mandate for environmental impact assessment in 1970. Risk assessment and ecological assessment merged in the 1980s to form ecological risk assessment (ERA). Since then, ERA has been institutionalized with the development of the US Environmental Protection Agency's (hereafter, USEPA or Agency) framework and guidance documents. Ecological risk assessment has been adapted by the Agency's program offices to fit their legal and policy contexts. The future of ERA will inevitably include the incorporation of more complex and demanding methods. However, the biggest challenge for future risk assessors will be to make ecological risks more compelling to decision makers.

Prior to the advent of scientific aquaculture in the mid-nineteenth century, English farming manuals of the seventeenth and eighteenth centuries instructed American colonists in the "art of husbandry," imparting advice and passing on the best-known strategies for keeping and rearing fish in enclosed ponds. The development of such ponds in the New England and Mid-Atlantic colonies during the eighteenth century marked the culmination of a long process by which British-American colonists adapted to declines in natural fish populations brought on by over-fishing and disruption of habitat by water-powered mills. The development of private fishponds as an increasingly important component of American mixed husbandry practices in long-settled areas by the end of the eighteenth century illustrates early American farmers' ability to successfully adapt to self-wrought changes in their physical environment.

Laser-ablation inductively coupled-plasma mass-spectrometry analysis of red oak (Quercus rubra) from a well documented heavy metal contaminated United States Environmental Protection Agency superfund site in Woburn, Massachusetts reveals decade-long trends in Pb contaminant sources. Lead isotope ratios (207Pb/206Pb and 208Pb/206Pb) in tree rings plot along a linear trend bracketed by several local and regional contamination sources. Statistically significant interannual variations in 207Pb/206Pb suggest that atmospheric Pb is rapidly incorporated into wood, with minimal mobility subsequent to deposition in annual growth rings. We interpret the decadal trends in our record as a changing mixture of local pollution sources and gasoline-derived Pb. Between 1940 and 1970, Pb was predominantly derived from remobilization of local industrial Pb sources. An abrupt shift in 207Pb/206Pb may indicate that local Pb sources were overwhelmed by gasoline-derived Pb during the peak of leaded gasoline emissions in the late 1960s and early 1970s.