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Environmental Forensics for Persistent Organic Pollutants
Environmental Forensics for Persistent Organic Pollutants
Environmental Forensics for Persistent Organic Pollutants
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Environmental Forensics for Persistent Organic Pollutants

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Environmental Forensics for Persistent Organic Pollutants represents the state-of-the-art in environmental forensics in relation to persistent organic pollutants (POPs). The book is a complete reference for practitioners and students, covering a range of topics from new analytical techniques to regulatory and legal status in the global community.

Through case studies from leading international experts, real-world issues — including the allocation of responsibility for release into the environment — are resolved through the application of advanced analytical and scientific techniques. This book introduces and assesses the development of new techniques and technologies to trace the source and fate of newly emerging and classic POPs (perfluoroalkyl substances, brominated flame retardants, organochlorine pesticides, perfluorinated chemicals, polycyclic aromatic hydrocarbons, and polychlorinated biphenyls) in environmental media, including atmospheric, marine, freshwater, and urban environments.

  • Real-world case studies show the application of advanced analytical and scientific techniques
  • Discussion of GC*GC provides an introduction and assessment of a novel technique from leaders in the field
  • Introduces the development of new analytical techniques (such as 2-D GC*HC and LC*LC) to trace the source and fate
  • Raises awareness about the health and environmental impact of persistent organic pollutants (POPs)
  • Outlines the development of international measures to control POPs so that chemists can understand the legal issues
LanguageEnglish
Release dateNov 20, 2013
ISBN9780444594518
Environmental Forensics for Persistent Organic Pollutants

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    Environmental Forensics for Persistent Organic Pollutants - Gwen O'Sullivan

    1

    Brief Overview

    Discovery, Regulation, Properties, and Fate of POPs

    Gwen O’Sullivana and David Megsonb,    aMount Royal University, Department of Environmental Science, Calgary, AB, Canada,    bUniversity of Plymouth, School of Geography Earth and Environmental Science, Drake Circus, Plymouth, UK

    Environmental forensics is a growing multidisciplinary field which combines traditional applied sciences, in particular analytical chemistry, with socioeconomic factors to identify the source, age, and timing of a contaminant into the environment. Persistent organic pollutants (POPs) are a group of priority pollutants which by their chemical nature are capable of long-range transport and biomagnification in food chains, including bioaccumulation in human and animal tissue. Mounting scientific evidence has suggested that they may be found not only in industrial locations but also in remote regions, such as deep ocean sediments and the Antarctic. They have been found to pose a significant risk to the environment and human health prompting the formation of environmental bodies like the United States Environmental Protection Agency and lead to the implementation of regulations to restrict their use. This chapter highlights significant discoveries of POPs in the environment, development of key analytical techniques and legislative milestones in the control of POPs in the environment. It also includes a brief description of the physical and chemical properties of POPs and finishes with a concise explanation of the main environmental processes that control the environmental behavior of POPs.

    Keywords

    Environmental forensics; persistent organic pollutants; biomagnification; bioaccumulation; LRAT

    1.1 Introduction

    The field of environmental forensics emerged in the 1980s as a consequence of legislative frameworks enacted to enable parties, either states or individuals, to seek compensation with regard to contamination or injury due to damage to the environment [1]. Environmental laws, including CERCLA (Superfund) [2] in the United States and Environmental Liability Directive [3] in the European Union (EU), are based on the polluter pays and precautionary principles and require the parties responsible for the release of hazardous substance to report the release, investigate the nature and extent of the release and to then remediate it to some objective cleanup standard [4]. Morrison and Murphy [5] define environmental forensics as a …systematic and scientific evaluation of physical, chemical, and historical information for the purpose of developing defensible scientific and legal conclusions regarding the source or age of a contaminant released into the environment.

    Globally there are many 100,000 existing chemicals on the market [6] and they are an integral part of our modern life. Since the 1960s, following the publication of Rachel Carson’s book Silent Spring [7], mounting scientific evidence has suggested that certain chemicals pose a significant risk to the environment and human health. The United Nations Environmental Programme (UNEP) has identified a number of these chemicals as substance of very high concern (SVHC) and categorizes them as persistent, bioaccumulative, and toxic (PBT). Chemicals categorized as PBT do not break down easily in the environment, accumulate in the tissues of organisms, and are toxic. Persistent organic pollutants (POPs) are a subset of the PBT category, others include trace metals and organo-metal compounds. As the name suggests POPs are compounds which are organic (natural or anthropogenic) in nature and resist biological, chemical, and photolytic degradation [8]. The UNEP defines POPs as …chemical substances that persist in the environment, bioaccumulate through the food web, and pose a risk of causing adverse effects to human health and the environment [9].

    There are thousands of chemicals which may be classified as POPs including whole families of chemicals, for example polychlorinated biphenyls (PCBs), polychlorinated dibenzo-p-dioxins and polychlorinated dibenzofurans (PCDD/PCDF), polybrominated diphenyl ethers (PBDEs), and organochlorinated pesticides (e.g., dichlorodiphenyltrichloroethane, DDT). Sources of POPs may be broadly classified as agrochemical (pesticides), industrial (synthesized for industrial use), or unintentional by-products (products of combustion or industrial synthesis of other chemicals).

    The following subsections will provide a brief overview of the history of POPs, introduce some of the key chemical and physical characteristics which help to define POPs, and outline the environmental fate and behavior of POPs. The purpose of this chapter is not to provide a comprehensive description of what POPs are but to provide you with a basic familiarity to assist you when reading the subsequent chapters.

    1.2 Brief History

    POPs have been used for more than a 100 years, with some of the infamous POPs discovered as early as the late 1800s (Table 1.1). A chronology for POPs, including when certain POPs were first discovered to be harmful, development of key analytical techniques and legislative milestones, may be found in Figure 1.1.

    Table 1.1

    The Discovery and Banning of Dirty Dozen POPs

    Figure 1.1 Chronology for POPs, including discoveries (blue text), development of key analytical techniques (green text) and legislative milestones (red text) [34–43].

    In the early 1960s, advancements in analytical techniques, including electron capture detectors, allowed for the detection of compounds such as DDT, Dichlorodiphenyldichloroethylene (DDE), dieldrin, and PCBs in environmental and biological samples at low levels [6]. In addition a number of key publications (e.g., Silent Spring by Rachel Carson [7]), scientific discoveries (e.g., Soeren Jensen finding PCBs in Baltic fish [44]), and human exposure incidents (the fatal poisoning in Turkey of 500 people with hexachlorobenzene (HCB)-treated seeds [45], poisoning of 1800 people in Japan with rice oil contaminated with Kanechlor 400 [46]) laid the foundations for discussions regarding the control of POPs. Initially action focused on individual specific industrial chemicals:

    • DDT: The US EPA (United States Environmental Protection Agency) issued a cancellation order based on adverse effect of its use (1972) [13].

    • Mirex: The US EPA issued regulations authorize restricted use by permit only (1972) [22].

    • Aldrin/dieldrin: The US Department of Agriculture cancels all use of aldrin and dieldrin in 1970, and in 1974 they were banned in the United States [10].

    • Heptachlor and chlordane: Banned in the United States in 1975 [17].

    • PCBs: Organization for Economic Development (OECD) was one of the first international groups to take steps to reduce the risk of specific chemicals through its decision to restrict the use of PCBs.

    However, in the 1970s, a number of legislative tools were implemented at a national level, including the Chemical Substance Control Law in Japan in 1973 and the Toxic Substance Control Act (TSCA) in United States of America (USA) in 1976. This continued into the 1980s with the development of the European Community (EC)-Existing Substances List in 1981 and the Domestic Substance List in Canada in 1986 which introduced the screening, e.g., examining structure and toxicity, of new chemicals to anticipate substance which could be of concern.

    International collaboration began in the 1970s as studies confirmed the transboundary migration of pollutants. In 1972, the United Nations Conference on the Human Environment in Stockholm signaled the start of active international cooperation which resulted in the signature of the Convention on Long-range Transboundary Air Pollution (CLRTAP) by 34 governments and the EC in 1979. As part of CLRTAP, the United Nations Economic Commission for Europe (UNECE) in 1998 adopted the Aarhus Protocol on Persistent Organic Pollutants with the ultimate objective of eliminating any discharges, emissions, and losses of POPs to the environment. The protocol banned the production and use of some POPs outright, e.g. aldrin, and severely restricts the use and disposal of others, e.g., DDT and Hexachlorocyclohexane (HCH). Initially the protocol focused on 16 POPs but seven more were included in 2009.

    In 1995, UNEP¹ called for global action to be taken on POPs which lead to a series of meetings of the Intergovernmental Negotiating Committee (INC) for a Treaty on Persistent Organic Pollutants. Following these negotiations the Stockholm convention, a United Nations (UN) treaty, was signed by over 90 countries and the EU in May 2001. Ratifying countries agreed to reduce or eliminate the production, use, and/or release of 12 POPs (Table 1.2). The initial 12 POPs, now infamously referred to as the dirty dozen, included pesticides, industrial chemicals, and unintended by-products. Following scientific review, a process specified in the convention, nine additional chemicals were added to the list in 2009.

    Table 1.2

    Categorization of Initial 12 POPs Listed in Stockholm Convention

    aParties must take measures to eliminate the production and use of chemicals listed.

    bMay also be categorized as by-product.

    cParties must take measures to restrict the production and use of chemicals listed.

    dMay also be categorized as industrial and by-product.

    eParties must take measures to reduce the unintentional production and releases of chemicals listed.

    With the development of global collaborations and conventions in recent years an emphasis has been placed on the completion of risk assessments and the development of national and international monitoring programs [6]. An important question for the success of these types of programs is to determine how we choose from the tens of thousands of chemicals on the markets which ones are priority to monitor [47]. In recent years, various lists of priority chemicals have been published including REACH’s SVHC [48], Substitute It Now (SIN) [49], and European Trade Union Confederation (ETUC) [50], and Oslo and Paris Conventions (OSPAR) [51]. However, there does not appear to be a consensus on the criteria for the selection of chemicals for each list as they differ considerably in their focus [47,52].

    The UNEP has established criteria for identifying new POPs (Table 1.3). They classified a substance as persistent if it has a half-life exceeding one of the thresholds in the following media [53]:

    • soil or sediment—180 days;

    • surface water—60 days;

    • air—2 days.

    Table 1.3

    Criteria for Assessment of POPs According to CLRTAPa and Stockholm Convention

    aCLRTAP, convention on long-range transboundary air pollution.

    Under the EU REACH chemical legislation, the half-life of a substance must be >120 days in freshwater sediment or soil to be classified as persistent and >180 days to be classified as very persistent (Table 1.3). Single media calculations of half-life are undertaken in controlled laboratory environments (Table 1.4). These single media criteria have been criticized by Gramatica and Papa [54] as being a simplistic approach to screening chemicals in the environment for POP-like behavior and often overpredict persistence when compared to environmental samples. However, with thousands of chemicals needing to be tested for persistence under REACH legislation single media half-life calculations provide a relatively quick and simple way to make an initial estimate of persistence.

    Table 1.4

    Estimated Half-Lives of Several POPs (to Two Significant Figures) in Different Media

    Source: Data obtained from supplementary material from Gramatica and Papa [54]

    Further discussion on the criteria used to create priority lists is beyond the scope of this chapter but further information and arguments may be found in Refs. [6,47,52,55–59].

    1.3 Chemistry and Properties of POPs

    All POPs are considered to be persistent in the environment, the following section outlines some of the key chemical and physical properties that give POPs their characteristic behavior. It provides a series of general rules to assist nonspecialists with the understanding of more complex discussions in further chapters.

    1.3.1 Aqueous Solubility (Sw)

    Aqueous solubility, sometimes referred to as water solubility, is the extent to which a compound will dissolve in water at a given pressure and temperature. POPs have a low aqueous solubility and as a result are rarely found in high concentrations in water samples instead they tend to partition to soil or sediment particles. As a general rule the greater the molecular weight the lower the solubility, and therefore the lower the proportion of the POP in the dissolved phase.

    1.3.2 Air–Water Partition Coefficient (Kaw or H)

    The air–water partition coefficient, also known as the Henry’s law constant, is a measure of the equilibrium distribution of a substance between air and water (i.e., how much of the gas dissolves in a solvent at a set temperature). The units for Henry’s law constants are reported in Pa m³/mol; however, the dimensionless Henry’s law constant (Kaw) is also sometimes used (recorded in cm³/cm³). The Kaw of POPs is variable, however, they are rarely at the extremes of the spectrum. POPs are not often found in high concentrations in the aqueous phase or atmosphere and so this is not a major pathway, however, some flux does occur between both phases. There is only a weak correlation, however, as a general rule the greater the degree of chlorination (or bromination) the lower the Kaw and therefore the lower the rate of transport from water to the atmosphere.

    1.3.3 Melting Point

    The melting point of a substance is defined as the point at which a solid becomes a liquid at a standard pressure. The units for melting point are often reported in degree Celsius or Fahrenheit, although in environmental models it is more common for units to be expressed in kelvin. Most POPs are solids (waxes) at environmental temperatures although they have often been manufactured into more practical forms like liquids (PCBs in transformer oils). Larger compounds with the strongest intermolecular forces will generally have higher melting points.

    1.3.4 Vapor Pressure

    The boiling point of a substance is defined as the point at which a liquid becomes a gas at a standard pressure. This occurs when the vapor pressure of a liquid equals the pressure surrounding the liquid. The vapor pressure is therefore the driving factor determining the proportion of a compound in the gaseous and liquid phases. There are various units for vapor pressure that include torr (mm Hg), pascals (Pa), atmospheres (atm), and bar (bar). Most POPs have relatively low vapor pressures which results in a minimal flux to the atmosphere. However, POPs are incredibly resistant to degradation and even though the flux is low, atmospheric transport is a significant pathway which has resulted in the global distribution of POPs [55]. Larger compounds with the strongest intermolecular forces will have lower vapor pressures.

    1.3.5 Octanol Water Partition Coefficient

    The octanol water partition coefficient is a dimensionless number defined as the ratio of a chemical's concentration in the octanol phase to its concentration in the aqueous phase. Most POPs have a high Kow which explains the partitioning of POPs in lipids. POPs with a higher Kow will be less polar than those with a lower Kow. As a general rule the higher the degree of chlorination (or bromination) the higher the Kow, and therefore the more lipophilic the POP.

    1.3.6 Organic Carbon Water Partition Coefficient (log Koc)

    The organic carbon water partition coefficient is a dimensionless number defined as the ratio of a chemical’s concentration absorbed per unit mass of soil, to its concentration in the aqueous phase. It represents the distribution coefficient (Kd) normalized to total organic carbon content. Most POPs have a high Koc which explains the partitioning of POPs in soils with high organic matter contents. As a general rule, the higher the degree of chlorination (or bromination) the higher the Koc, and therefore the more a chemical will bind to organic matter.

    1.4 Environmental Behavior

    Chemicals may now be considered as POPs if they, once released to the environment, have long half-lives persisting in the environment (soils, sediments, air, or biota) for extended periods. Combining POPs stability and inclination/tendency to exist in the gas phase means that POPs are subject to long-range transportation [52] and have accumulated in food chains. The physiochemical properties described in the previous section begin to explain why POPs behave the way they do. The main environmental processes that control the persistence of a compound can be roughly separated into three areas:

    • Transport: volatilization, dilution, and advection;

    • Partitioning: sorption, uptake by organisms;

    • Degradation: biodegradation (aerobic, anaerobic, and metabolism) and abiotic degradation (hydrolysis, photolysis, oxidation, and reduction).

    POPs in the environment are not present in just one phase. There is a constant dynamic equilibrium whereby POPs are shifting through the different phases. The proportion of a POP in each phase is dependent upon the chemicals physiochemical parameters. The main processes are summarized in Figure 1.2. Subsequent chapters will examine in more detail the environmental fate and behavior of individual POPs in different media, e.g., biological, terrestrial, air, and aquatic. The following sections will, however, briefly introduce the concepts of transportation and degradation.

    Figure 1.2 A schematic of the dynamic equilibriums influencing the proportion of a POPs in each phase.

    1.4.1 Transportation/Long-Range Atmospheric Transportation

    POPs are typically hydrophobic and lipophilic. In soils they tend to bind to organic matter and tend to be fairly localized contaminants as transportation in ground water is minimal. In aquatic environments, they tend to bind strongly to solid particles and are therefore only detected in low concentrations in the dissolved phase. Based on their semi-volatile character, these compounds can be found in the gas phase, in association with atmospheric particles or distributed between these two phases [60]. The atmosphere therefore is the main transport media for the global distribution of POPs. Once released into the environment, they travel in multiple cycles of evaporation, transport by air and condensation (Figure 1.3). Global distillation and cold condensation describe the process whereby semi-volatile chemicals like POPs would volatilize from warm source areas, undergo long-range atmospheric transport (LRAT), and subsequently condense onto surfaces, such as soil, vegetation, or snow, at low temperatures, effectively accumulating in the polar regions. This migration of POPs to higher latitudes in a series of relatively short jumps is colloquially referred as the grasshopper effect. The compounds migrate, rest, and migrate again in tune with seasonal temperature changes at mid latitudes.

    Figure 1.3 Multiple cycles of evaporation, transport by air, and condensation of POPs (grasshopper effect).

    The more volatile POP compounds tend to remain airborne and migrate faster. Less volatile POPs will partition into water, snow, soil, or vegetation. Thus POPs can be found all over the world, including areas where they have never been used and in remote regions, such as the middle of oceans and polar region. In the cold climate of the Arctic and Antarctic, low evaporation rates trap POPs resulting in their entry in the food chain. The composition of contaminant mixtures thus will vary along a temperature or latitudinal gradient [55]. The ability of POPs to travel great distances along with remobilization from soils, which can now act as sources, is part of the explanation for why countries that banned the use of specific POPs are no longer experiencing a decline in their concentrations; the wind may carry chemicals into the country from places that still use them [61,62] (Figure 1.4).

    Figure 1.4 The grasshopper effect and out of Canada sources. Reproduced with permission from House of Commons Proceedings [61].

    1.4.2 Bioaccumulation and Biomagnification

    POPs lipophilic and hydrophobic nature means that once they enter a biological system they are not easily excreted. In biological systems, POPs tend to partition into lipids which results in accumulation of POPs in organs and adipose tissue. Over time POPs accumulate (bioaccumulation) in the living tissue of organism. Biomagnification is the increase in concentration of POPs as contaminated materials (plant and animals) pass up the trophic levels of the food chain.

    Because POPs can bioaccumulate and magnify in the food chain, concern centers around impacts to top predators, including humans. Probably the best documented and clearest evidence of POP effects have been in birds and marine mammals. Various papers have documented and reviewed how organochlorines (OCs), for instance DDE, a metabolic breakdown product of DDT, can affect egg-shell thickness in birds of prey [63,64]. In humans, it has been well documented that the lipophilic nature of POPs can result in transport to a developing fetus and suckling infants.

    1.5 How to Use This Book

    Environmental Forensics for Persistent Organic Pollutants was written for a diverse audience with the objective of acting as a reference guide for practitioners and students. The book presents a compilation of the state of the art in environmental forensics in relation to POPs presented by leading international experts. Each chapter is supported and supplemented with references from the relevant literature and presentation of case studies. The following is a brief overview of each chapter in the book.

    1.5.1 Brief Overview: Discovery, Regulation, Properties, and Fate of POPs

    This chapter introduces the concept of environmental forensics and describes significant discoveries of POPs in the environment, development of key analytical techniques and legislative milestones in the control of POPs in the environment. The chapter also includes a brief description of the physical and chemical properties which define POPs and finishes with a concise explanation of the main environmental processes that control the environmental behavior of POPs.

    1.5.2 Environmental Regulation and Litigation

    This chapter identifies key treaties, statutes, regulations, and case law pertaining to the control of POPs by the federal governments in the United States and Canada. The chapter also discusses the standards for use and presentation of forensic science in the courtroom during legal proceedings involving POPs, and legal remedies potentially available to individuals alleging harm due to exposure to POPs.

    1.5.3 Analytical Methodology of POPs

    An important goal in the field of analytical chemistry is to use the proper extraction, preparation, and instrumental techniques such that the accuracy and uncertainty of the technique is acceptable to meet the required data quality objectives and the analytical method used is fit for the purpose for which it was intended. A variety of techniques, procedures, and instruments are introduced, including discussion on optimum conditions important to ensure that analytes are quantitatively extracted, matrix co-extractables and interferences are removed and instruments are used most effectively and efficiently.

    1.5.4 Sample Collection and Management for Environmental Forensic Investigations

    This chapter provides an overview of quality systems, which includes project planning, field documentation, and data verification and validation. There are no specific documentation requirements for environmental forensic investigations; however, a robust and defensible investigation must comply with the framework of quality systems established by the governing agency. The project manager must clearly understand how these affect the investigation.

    Planning for a forensic field event is motivated by two objectives: remediation planning and litigation assignment. The design of an investigation is guided by compliance with both of these needs on a case-by-case basis. This is discussed in the context of analytical data needs. Currently, the field documentation and data management of environmental investigations is slowly advancing from physical to electronic forms of information gathering, storage, and transfer. Examples are provided where new developments in technology can make these processes cheaper, more secure, and less error-prone.

    1.5.5 Biomonitoring for POPs

    This chapter discusses the various aspects of human biomonitoring, including toxicokinetics—absorption, distribution, metabolism, and elimination; sensitive analytical chemistry methods; characterizing normal background population levels such as in the US National Report on Human Exposure to Environmental Chemicals as well as in other countries; development of reference values and biomonitoring equivalents; and environmental exposure pathways, such as food, soil, dust, clay, and beef. Human exposures are then discussed related to accidental exposures, poisonings, food contamination incidents, and occupational exposures.

    1.5.6 Atmospheric Fate and Behavior of POPs

    This chapter discusses the sources to the atmosphere, chemical transformations during atmospheric transport, levels found in ambient air, and levels found in settled dust for five families of POPs: polycyclic aromatic hydrocarbons (PAHs), PCBs, polybrominated compounds, polyfluorinated compounds, and PCDD/PCDFs (aka dioxins and furans). For each of the chemical groups, environmental forensic case studies are also presented to support discussion.

    1.5.7 POPs in the Terrestrial Environment

    This chapter examines a variety of terrestrial environments, including soil and sediments, herbage, wildlife, and humans. It includes discussion on the major pathways in which POPs enter each media, the changes which may occur within the media, background concentrations and patterns which may be used to interpret the potential sources of POPs in each media. Two case studies are presented to provide context to the discussion and highlight how environmental forensic investigations in the terrestrial environment may be carried out using different tools.

    1.5.8 POPs in the Marine and Freshwater Environments

    This chapter provides a summary of POPs in the aquatic environment. POPs generally have low solubility and are thus found at very low concentrations in these environments in the dissolved phase, making detection of these chemicals relatively difficult. In aquatic environments, POPs are found bound to particles, colloids, and debris in these environments providing a complex exposure scenario for risk assessment. POPs covered in this chapter include emerging chemicals, such as polyfluoroalkyl compounds, pharmaceuticals and personal care products (PPCPs), nanomaterials, marine debris and microplastics as well as flame retardants and PAHs.

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    2. Comprehensive Environmental, Response, Compensation, and Liability Act, 42 U.S.C. § 9601 et seq.

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    25. Aboriginal Affair and Northern Development Canada (AANDC), Persistent Organic Pollutants (POPs) Fact Sheet Series: Toxaphene. Available from: <http://www.aadnc-aandc.gc.ca/eng/1290437720770/1290437887650>, 2011 (accessed 01.11.12).

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