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The human footprint on the global environment now touches every corner of the world. This book explores the myriad ways that environmental archives can be used to study the distribution and long-term trajectories of chemical contaminants. The volume first focuses on reviews that examine the integrity of the historic record, including factors related to hydrology, post-depositional diffusion, and mixing processes. This is followed by a series of chapters dealing with the diverse archives and methodologies available for long-term studies of environmental pollution, such as the use of sediments, ice cores, sclerochronology, and museum specimens.



Using Natural Archives to Track Sources and Long-Term Trends of Pollution: An Introduction

This book explores the myriad ways that environmental archives can be used to study the distribution and long-term trajectories of contaminants. The volume first focuses on reviews that examine the integrity of the historic record, including factors related to hydrology, post-depositional diffusion, and mixing processes. This is followed by a series of chapters dealing with the diverse archives available for long-term studies of environmental pollution.
Jules M. Blais, Michael R. Rosen, John P. Smol

The Influence of Hydrology on Lacustrine Sediment Contaminant Records

The way water flows to a lake, through streams, as runoff, or as groundwater, can control the distribution and mass of sediment and contaminants deposited. Whether a lake is large or small, deep or shallow, open or closed, the movement of water to a lake and the circulation patterns of water within a lake control how and where sediment and contaminants are deposited. Particle-associated contaminants may stay close to the input source of contamination or be transported by currents to bathymetric lows. A complex morphology of the lake bottom or shoreline can also affect how contaminants will be distributed. Dissolved contaminants may be widely dispersed in smaller lakes, but may be diluted in large lakes away from the source. Although dissolved contaminants may not be deposited in lake sediments, the impact of dissolved contaminants (such as nitrogen) may be reflected by the ecosystem. For instance, increased phosphorus and nitrogen may increase organic content or algal biomass, and contribute to eutrophication of the lake over time. Changes in oxidation-reduction potential at the sediment-water interface may either release some contaminants to the water column or conversely deposit other contaminants to the sediment depending on the compound’s chemical characteristics. Changes in land use generally affect the hydrology of the watershed surrounding a lake, providing more runoff if soil binding vegetation is removed or if more impervious cover (roads and buildings) is increased. Groundwater inputs may change if pumping of the aquifer connected to the lake occurs. Even if groundwater is only a small portion of the volume of water entering a lake, if contaminant concentrations in the aquifer are high compared to surface water inputs, the mass of contaminants from groundwater may be as, or more, important than surface water contributions.
Michael R. Rosen

The Stability of Metal Profiles in Freshwater and Marine Sediments

The stability of sedimentary metal profiles (defined as the absence of significant changes in profile shapes or concentrations as the accumulated metals are progressively buried), or the ability to reconstruct the original profiles following dispersion by diagenetic processes, is a key requirement for the robust interpretation of metal deposition histories from these natural archives. Diagenesis is a common problem in the study of metals in freshwater and marine sediments, but its effects are difficult to generalize because they are metal- and site-specific. There are two types of diagenetic processes, both of which may be strongly influenced by benthic biological activity: (1) physical processes, involving the mixing of surface and deeper sediments by bioturbation or wind and wave action, which may affect all metals in upper sediment layers; and (2) geochemical processes which involve chemical reactions between certain metals in solid-phases and in porewater, the vertical redistribution of dissolved metals, and their precipitation/adsorption elsewhere in the sediment column. A minority of the metals of environmental interest, such as Hg and to a lesser extent Pb, are thought to be geochemically stable in most settings. Others, such as As, Cd, Cu, Mo, Ni, Re, U and Zn, are relatively sensitive to changes in oxic-anoxic (oxidation- reduction) conditions down-core and are often redistributed during burial. This review has several aims: (1) to describe the patterns and mechanisms of physical and geochemical diagenesis; (2) to describe three tests of metal profile stability; (3) to review environmental and geochemical factors that influence the occurrence and severity of diagenesis; (4) to present case studies that illustrate working approaches for correcting diagenetically-altered profiles so that part or all of the original history of accumulation can be reconstructed; and (5) to present practical recommendations concerning study site selection, and approaches to detecting diagenesis, which may assist in minimizing or at least identifying the severity of metal redistribution.
Peter M. Outridge, Feiyue Wang

Calculating Rates and Dates and Interpreting Contaminant Profiles in Biomixed Sediments

Contaminant profiles in well-dated sediment cores represent extremely valuable natural archives of environmental contamination, by which contaminant sources, history and cycling may be determined and contaminant concentrations in surface sediments projected into the future. However, most marine and estuarine sediments are mixed by benthic organisms to a depth of at least 2–20 cm, which introduces significant risks of misinterpreting and misapplying these archives if biomixing is not explicitly taken into account. This chapter offers a step-by-step guide to avoiding common pitfalls and appropriately applying biomixed sediment archives to reconstructing contaminant inputs to the environment. By the use of simple models, radioisotope tracers (210Pb, 137Cs) may still be applied to establish geochronologies in biomixed cores and to validate the sedimentation rates and dates derived. Having obtained (and validated) sedimentation and mixing rates for biomixed cores, contaminant profiles may then be interpreted through the further use of models in a way that explicitly accounts for mixing. As with any sediment core, the main caution when one attempts to infer contaminant releases from deposition histories reconstructed from biomixed sediment cores are the unknown possible impacts of environmental variation and change.
Zou Zou A. Kuzyk, Robie W. Macdonald, Sophia C. Johannessen

Contaminants in Marine Sedimentary Deposits from Coal Fly Ash During the Latest Permian Extinction

The Latest Permian Extinction (LPE) event, the greatest mass extinction in Earth history, was marked by major explosive volcanic eruptions through thick layers of coal and carbonaceous deposits at the time. This resulted in significant dispersion of volcanic-derived ash and other particulate and gaseous hazardous substances, which may have caused extensive contamination of the global marine ecosystem.
A continuous geological sedimentary record from the Canadian High Arctic revealed evidence of unprecedented mercury loading that may have contributed to the extinction. Mercury loading is attributed to combined effects of volcanic emissions in association with volcanic combustion of surface and subsurface coal and carbonaceous deposits.
Mercury influx exceeded the scavenging capacity of organic matter (OM) in the Late Permian ocean, leading to major disruption of mercury drawdown processes mediated by organic carbon. This resulted in buildup of dissolved mercury to maximum levels at the LPE boundary. The transition of the Latest Permian ocean to euxinic conditions allowed sulphide scavenging of mercury from ocean water, beginning a self-mitigation process that led to gradual recovery from toxic marine conditions.
Hamed Sanei, Stephen E. Grasby, Benoit Beauchamp

Lake Sediment Records of Preindustrial Metal Pollution

The extraction of mineral resources has been occurring for millennia in both the Old and New Worlds. Lake sediments can archive the environmental legacy of these preindustrial activities, offering an independent method for understanding the magnitude and spatial extent of metal pollution through time. A number of geochemical records of past metal pollution within lake sediments have now been completed across especially Europe and the South American Andes, revealing histories of metal pollution that extend back over millennia. The use of paleolimnological techniques is refining our understanding of spatial and temporal differences in mineral resource extractions and use, and offers the opportunity to understand the degree to which human activities have mobilized metals from geologic stores into the biosphere.
Colin A. Cooke, Richard Bindler

Lacustrine Archives of Metals from Mining and Other Industrial Activities—A Geochemical Approach

Since the first studies reporting recent stratigraphic changes of metal concentration in lake sediments, many hundreds of studies have been published in the peer-reviewed literature. It is an impossible task to do justice to all of these works here; instead we: (1) examine recent methodological advances and place these in the context of the historical development of the discipline; and (2) explore the various purposes to which such methods have been applied. Such a historical emphasis may appear in conflict with the needs of a review of new approaches; however, this is not in fact the case for two main reasons. First, most new advances supplement rather than replace traditional methods, such that a thorough understanding of the practical and theoretical issues impacting these is still essential for reliable interpretation of palaeolimnological data. Second, while many of the new methods purport to circumvent problems, they achieve this only under favourable conditions, not dissimilar to the conditions that influence the earlier methods, so the same lesson must be learned anyway. Consequently, we use this historical narrative to address the fundamentals of the discipline.
The chapter comprises two main parts; methodology and applications. The methodological section has three subsections: (1) Introduction to processes controlling natural variations in metal fluxes and concentrations in lake sediments; (2) Measurement of metal concentrations in sediments; (3) Calculation of enrichment or fluxes from sediment metal concentration data.
There are four main applications subsections focusing on the value of lake sediment records of metals derived from mining or industry. They are: (1) Geochronological markers in sediments providing chronology for other research goals; (2) Lake sediment heavy metal records to quantify pollution loading histories, or to identify pollutant sources; (3) Identifying and quantifying pre- and post-mining baseline conditions; (4) Identifying pollutant pathways or environmental processes regulating heavy metals.
John Boyle, Richard Chiverrell, Dan Schillereff

Organic Pollutants in Sediment Core Archives

Organic contaminant profiles in lake and marine sediment cores are important for understanding the persistence of pollutants in aquatic ecosystems, as well as for evaluating the success of emission restrictions and regulations. Several different classes of organic contaminants can be reconstructed from cores. The earliest studies measured PCBs, DDT, and polycyclic aromatic hydrocarbons, but paleolimnological approaches are now common for a suite of organochlorines and brominated flame retardants, as well as emerging studies on fluorinated persistent organic pollutants and historical sewage indicators (fecal sterols). In order for the history of organic contaminant inputs to be successfully reconstructed from sediment cores, the contaminant must have a high affinity for sedimentary particulates and low water solubility, ensuring its rapid delivery and incorporation into the sediment record, and minimal porewater migration once it is deposited. In addition, the compound must be resistant to microbial degradation and post-depositional transformation, so that any changes in composition and abundance down-core may be confidently attributed to changing contaminant inputs to the aquatic environment. Using several independent lines of evidence, we review the reliability of sediment cores as historical archives for organochlorines, brominated flame retardants, perfluoroalkyl substances, polycyclic aromatic hydrocarbons, and fecal sterols. The objective of this chapter is to provide a framework for researchers to critically evaluate the reliability of sediment cores for reflecting historical inputs of legacy and emerging organic contaminants.
Jennifer B. Korosi, Wenhan Cheng, Jules M. Blais

Environmental Archives of Contaminant Particles

Particulates in the environment may be contaminants or pollutants. They may affect climate through: the absorption of energy in the atmosphere and by reducing the albedo of ice and snow surfaces; may enhance the transfer and distribution of pollutants such as trace metals and persistent organic pollutants via absorption and adsorption to their surfaces; may adversely impact the health of aquatic life and consequently other biota that depend upon it; in the atmosphere they may have direct effects on human health via respiratory disease and the transfer of substances deep into the respiratory system. Therefore, it is important to be able to determine temporal trends in particulate emissions and deposition. Natural archives such as ice, sediment and peat cores can provide well-resolved records, but research has mainly focussed on a few particle types, and predominantly black carbon. In this chapter we review the environmental records of black carbon and other industrially-derived particles, their analysis, interpretation and relative strengths and weaknesses. Finally we consider two emerging particle types: microplastics and nanoparticles. These latter groups have, so far, received little attention from palaeoecological perspectives but their direct impacts on aquatic biota and ability to transport pollutants within the atmosphere and aquatic ecosystems is becoming increasingly apparent in the literature and are predicted to further increase in coming decades.
Neil L. Rose, Meri Ruppel

Tracking Long-range Atmospheric Transport of Contaminants in Arctic Regions Using Lake Sediments

Due to the nature of global atmospheric circulation patterns, numerous contaminants of concern, including mercury (Hg) and persistent organic pollutants (POPs), undergo long-range transport to the Arctic where they can be deposited to landscapes and water bodies. As a result, both mercury and POPs have recently reached levels in Arctic mammals and fishes that are high enough to pose health risks to Northern peoples consuming these animals as traditional country foods. Dated lake sediment cores provide a valuable tool for examining temporal trends in atmospheric contaminant deposition. In addition, the recent application of novel multi-proxy approaches is allowing atmospheric contaminant deposition to be examined within the context of numerous climate-induced alterations to contaminant cycling, such as increased catchment contaminant inputs driven by climate-induced erosion. Here, we review current information on the use of dated sediment cores to examine post-industrial (post-~ 1850) changes to atmospheric mercury and POPs deposition, including atmospheric contaminant transport and deposition processes, the impacts of climate-induced changes on these processes, and the application of novel lake sediment core analyses to untangle trends in contaminant deposition due to multiple sources and environmental stressors. Hg and POPs are compared and contrasted throughout the chapter, as, although these contaminants are both of great concern in the Arctic, their differing physical-chemical properties and emission sources result in differing transport and deposition pathways. Finally, we make suggestions for future research that will allow dated lake sediment cores to continue to provide valuable information on contaminant deposition in the face of a changing Arctic climate.
Jane Kirk, Amber Gleason

Tracking Long-Range Atmospheric Transport of Trace Metals, Polycyclic Aromatic Hydrocarbons, and Organohalogen Compounds Using Lake Sediments of Mountain Regions

High mountain regions may be perceived as areas of high environmental quality, yet many contaminants are ubiquitous on the planet through long-range atmospheric transportation. Mountain lake sediments record and archive how this global contamination is proceeding and have developed throughout history, particularly since rapid industrialization in the 1950s. Action against diffuse atmospheric contamination transported far away from the sources requires the development of national and international protocols, which must be based on reliable scientific evidence. Research on mountain lake sediments aims to provide long-term references, models for interpretation of results, and sound understanding of the mechanisms that lie behind the observed patterns of contamination. Mountains offer an excellent setting for environmental research because short distances may provide marked physical gradients (e.g., air temperature), and ecosystems are relatively amenable to observation and modelling. The lake sediment contributions are important complements to other observational approaches used in global change research. This chapter focuses on trace metals, polycyclic aromatic hydrocarbons (PAHs) and organohalogen compounds (OHCs). After a short introduction regarding contaminants and the several operative ways to examine the sediment archive, the main features of contaminant distribution in mountain lake sediments are described, followed by a section on the understanding of the processes behind the patterns (e.g., atmospheric transport, catchment interactions, air-water exchange, water column dynamics and eventual sediment archiving), and finishes with a section on biological assessment.
Jordi Catalan

Using Peat Records as Natural Archives of Past Atmospheric Metal Deposition

Over the last decades, scientists throughout Europe and beyond have been increasingly using peat as archives of past atmospheric metal deposition. Since the pioneering studies using herbaria moss collections to evidence atmospheric metal pollution in the late sixties, the improvements in analytical techniques, as well as chronological controls, have allowed investigations of a variety of scientific questions in various fields, e.g. elemental biogeochemical cycles, atmospheric pollution and archaeology. In this chapter we summarize the various applications and usage of peat cores as archives of past atmospheric metal deposition. The chapter contains an introduction followed by a section addressing the state of the art in the field, providing examples of various elements and a variety of study sites. We then continue with a brief description of the application of metal records stored in peat, i.e. applications to archaeology. To end we present some confounding factors affecting the integrity of the peat record, which must be carefully considered, and lastly we give a few examples of challenges and perspectives for future generations of peat geochemists.
Sophia V. Hansson, Richard Bindler, François De Vleeschouwer

Historical Contaminant Records from Sclerochronological Archives

A number of marine and freshwater organisms, including scleractinian and proteinacious corals, coralline algae, sclerosponges, and bivalve mollusks, secrete skeletons that grow larger over time and may record environmental contaminants over the lifespan of an individual. Most of these organisms also form periodic growth patterns (growth increments, lines or bands) that can be used to accurately date contaminant archives produced from chemical or physical analysis of sequential skeletal samples (termed sclerochronology). The majority of records produced from these organisms thus far have focused on paleoclimate reconstructions, but there is a vast potential for information on changes in contaminant levels over time. Importantly, sclerochronological archives offer the potential for pre-anthropogenic baselines of naturally occurring substances to estimate the magnitude of anthropogenic pollution. This chapter presents an overview of existing contaminant records and discusses the limitations and potential for future work using archives derived from marine organism skeletons.
Jessica Carilli, Branwen Williams, Bernd R. Schöne, Richard A. Krause, Stewart J. Fallon

Contaminant Records in Ice Cores

Ice cores extracted in polar regions and in high altitude glaciers at low and mid latitudes are important recorders of global to regional changes in climate, ecosystems and human activities (e.g. industry, mining, transport). All of the contaminants found in ice cores are transported through the atmosphere, with the transport mechanism and atmospheric lifetime of these contaminants determining their spatial extent. In this chapter, we consider such ice core impurities as lead, mercury, platinum group elements, other trace elements, black carbon, organic and radioactive species. These contaminants are evaluated over the past few centuries, from the pre-industrial period through the Industrial Revolution and up to the most recent years of atmospheric monitoring, pollutant moratoria and/or abatement technologies. Contamination by most of these compounds is widespread from the higher latitudes of the Northern Hemisphere down to the remotest locations of Antarctica, suggesting that today there are no glaciers on Earth where atmospheric depositions of anthropogenic origin cannot be detected.
Paolo Gabrielli, Paul Vallelonga

Use of Catalogued Long-term Biological Collections and Samples for Determining Changes in Contaminant Exposure to Organisms

For decades, biological materials have been collected and held in museum collections, natural history collections (NHC), herbaria and environmental specimen banks (ESB). Those biological materials and accompanying data represent a potentially important source of retrospective analyses of contaminants and other chemical tracers. In ideal situations, those can provide valuable insights into changes in contaminant accumulation and concentrations over time and space. This chapter explores the benefits of such curated and catalogued specimens for contaminant research, as well as limitations and key considerations which must be kept in mind when using such samples. Three case studies examining temporal trends in contaminants using long-term biological collections are also presented.
Linda M. Campbell, Paul E. Drevnick

Tracking Contaminant Transport From Biovectors

We investigated contaminant transport and accumulation into ecosystems via migrating and invasive organisms. This review examines contaminant bioaccumulation and biomagnification in the context of physico-chemical properties of pollutants, the ecology, life cycles, and behavioural aspects of the carrier organisms (i.e. biovectors). Lake sediment profiles can provide an important historical archive for biovectors, such as the accumulation of metals and persistent organic pollutants, because these sediment profiles may be influenced by biological inputs (including fish carcases, animal waste, and other biological materials). Future research priorities are recommended based on the knowledge gaps identified. This chapter aims to provide science-based information for environmental scientists and regulators for the development of new coordinated research strategies, monitoring and research programs as well as international regulations for the mitigation of hazardous effects of anthropogenic pollutants.
Roland Kallenborn, Jules M. Blais

Using Natural Archives to Track Sources and Long-Term Trends of Pollution: Some Final Thoughts and Suggestions for Future Directions

Newly produced, as well as some so-called legacy contaminants, continue to be released into the environment at an accelerated rate. Given the general lack of integrated, direct monitoring programs, the use of natural archival records of contaminants will almost certainly continue to increase. We conclude this volume with a short chapter highlighting some of our final thoughts, with a focus on a call to action to develop and apply methodologies to assess the fidelity of the archival record.
Jules M. Blais, Michael R. Rosen, John P. Smol

Erratum to: The Stability of Metal Profiles in Freshwater and Marine Sediments

Without Abstract
Peter M. Outridge, Feiyue Wang


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