uncertainty, variability and environmental risk...
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Uncertainty, variability and environmental risk analysis
Linnaeus University Dissertations
No 35/2011
UNCERTAINTY, VARIABILITY AND ENVIRONMENTAL RISK
ANALYSIS
MONIKA FILIPSSON
LINNAEUS UNIVERSITY PRESS
UNCERTAINTY, VARIABILITY AND ENVIRONMENTAL RISK ANALYSIS. Doctoral dissertation, School of Natural Sciences, Linnaeus University 2011. ISBN: 978-91-86491-63-5 Printed by: Intellecta Infolog, Gothenburg
Abstract Filipsson, Monika. (2011). Uncertainty, variability and environmental risk analysis. Linnaeus University Dissertations No 35/2011. ISBN: 978-91-86491-63-5. Written in English.
The negative effects of hazardous substances and possible measures that can be taken are evaluated in the environmental risk analysis process, consisting of risk assessment, risk communication and risk management. Uncertainty due to lack of knowledge and natural variability are always present in this process. The aim of this thesis is to evaluate some tools as well as discuss the management of uncertainty and variability, as it is necessary to treat them both in a reliable and transparent way to gain regulatory acceptance in decision making.
The catalytic effects of various metals on the formation of chlorinated aromatic compounds during the heating of fly ash were investigated (paper I). Copper showed a positive catalytic effect, while cobalt, chromium and vanadium showed a catalytic effect for degradation. Knowledge of the catalytic effects may facilitate the choice and design of combustion processes to decrease emissions, but it also provides valuable information to identify and characterize the hazard.
Exposure factors of importance in risk assessment (physiological parameters, time use factors and food consumption) were collected and evaluated (paper II). Interindividual variability was characterized by mean, standard deviation, skewness, kurtosis and multiple percentiles, while uncertainty in these parameters was estimated with confidence intervals.
How these statistical parameters can be applied was shown in two exposure assessments (papers III and IV). Probability bounds analysis was used as a probabilistic approach, which enables separate propagation of uncertainty and variability even in cases where the availability of data is limited. In paper III it was determined that the exposure cannot be expected to cause any negative health effects for recreational users of a public bathing place. Paper IV concluded that the uncertainty interval in the estimated exposure increased when accounting for possible changes in climate-sensitive model variables. Risk managers often need to rely on precaution and an increased uncertainty may therefore have implications for risk management decisions.
Paper V focuses on risk management and a questionnaire was sent to employees at all Swedish County Administrative Boards working with contaminated land. It was concluded that the gender, age and work experience of the employees, as well as the funding source of the risk assessment, all have an impact on the reviewing of risk assessments. Gender was the most significant factor, and it also affected the perception of knowledge.
Keywords: Contaminated land, exposure assessment, exposure factors, risk
analysis, risk perception, uncertainty, variability, probabilistic risk assessment
Sammanfattning Negativa effekter orsakade av skadliga ämnen och möjliga åtgärder bedöms och utvärderas i en miljöriskanalys, som kan delas i riskbedömning, riskkommunikation och riskhantering. Osäkerhet som beror på kunskapsbrist samt naturlig variabilitet finns alltid närvarande i denna process. Syftet med avhandlingen är att utvärdera några tillvägagångssätt samt diskutera hur osäkerhet och variabilitet hanteras då det är nödvändigt att båda hanteras trovärdigt och transparent för att riskbedömningen ska vara användbar för beslutsfattande. Metallers katalytiska effekt på bildning av klorerade aromatiska ämnen under upphettning av flygaska undersöktes (artikel I). Koppar visade en positiv katalytisk effekt medan kobolt, krom och vanadin istället katalyserade nedbrytningen. Kunskap om katalytisk potential för bildning av skadliga ämnen är viktigt vid val och design av förbränningsprocesser för att minska utsläppen, men det är också ett exempel på hur en fara kan identifieras och karaktäriseras. Information om exponeringsfaktorer som är viktiga i riskbedömning (fysiologiska parametrar, tidsanvändning och livsmedelskonsumtion) samlades in och analyserades (artikel II). Interindividuell variabilitet karaktäriserades av medel, standardavvikelse, skevhet, kurtosis (toppighet) och multipla percentiler medan osäkerhet i dessa parametrar skattades med konfidensintervall. Hur dessa statistiska parametrar kan tillämpas i exponeringsbedömningar visas i artikel III och IV. Probability bounds analysis användes som probabilistisk metod, vilket gör det möjligt att separera osäkerhet och variabilitet i bedömningen även när tillgången på data är begränsad. Exponeringsbedömningen i artikel III visade att vid nu rådande föroreningshalter i sediment i en badsjö så medför inte bad någon hälsofara. I artikel IV visades att osäkerhetsintervallet i den skattade exponeringen ökar när hänsyn tas till förändringar i klimatkänsliga modellvariabler. Riskhanterare måste ta hänsyn till försiktighetsprincipen och en ökad osäkerhet kan därmed få konsekvenser för riskhanteringsbesluten. Artikel V fokuserar på riskhantering och en enkät skickades till alla anställda som arbetar med förorenad mark på länsstyrelserna i Sverige. Det konstaterades att anställdas kön, ålder och erfarenhet har en inverkan på granskningsprocessen av riskbedömningar. Kön var den mest signifikanta variabeln, vilken också påverkade perceptionen av kunskap. Skillnader i de anställdas svar kunde också ses beroende på om riskbedömningen finansierades av statliga bidrag eller av en ansvarig verksamhetsutövare.
TABLE OF CONTENTS
LIST OF PAPERS................................................................................................. 3
ABBREVIATIONS ............................................................................................... 4
INTRODUCTION ............................................................................................... 5
The risk analysis process .................................................................................... 5
Uncertainty and variability ................................................................................. 7
Characterization of uncertainty and variability in risk assessments ................... 9
Aims of the included papers in a risk-analysis context .................................... 11
METHODS ......................................................................................................... 13
Catalytic effects of metal oxides....................................................................... 13
Variability and uncertainty in exposure factors ................................................ 14
Exposure assessments ...................................................................................... 16
Risk management of contaminated land ......................................................... 20
RESULTS AND DISCUSSION ........................................................................ 22
Catalytic effects of metal oxides....................................................................... 22
Variability and uncertainty in exposure factors ................................................ 22
Exposure assessments ...................................................................................... 24
Risk management of contaminated land ......................................................... 30
CONCLUSIONS................................................................................................. 32
ACKNOWLEDGEMENTS .............................................................................. 34
REFERENCES.................................................................................................... 35
APPENDIX.......................................................................................................... 43
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LIST OF PAPERS
The following papers, referred to in the text by roman numerals, form the basis of this thesis. Published papers are reprinted with permission from Elsevier (papers I and III) and John Wiley and Sons (paper II).
I. Öberg, T., Bergbäck, B., Filipsson, M. 2008. Catalytic effects by metal
oxides on the formation and degradation of chlorinated aromatic compounds in fly ash. Chemosphere, 71, 1135–1143.
II. Filipsson, M., Öberg, T., Bergbäck, B. 2011. Variability and
uncertainty in Swedish exposure factors for use in quantitative exposure assessments. Risk Analysis, 31, 108-119.
III. Filipsson, M., Lindström, M., Peltola, P., Öberg, T. 2009. Exposure to
contaminated sediments during recreational activities at a public bathing place. Journal of Hazardous Materials, 171, 200-207.
IV. Augustsson, A., Filipsson, M., Öberg, T., Bergbäck, B. Climate change
– an uncertainty factor in risk analysis of contaminated land. Submitted.
V. Filipsson, M., Ljunggren, L., Öberg, T. Gender differences in risk management of contaminated land. Manuscript.
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ABBREVIATIONS
ABS Absorption factor (no unit) AF Sediment-to-skin adherence factor (mg/cm2) ANOVA Analysis of variance AT Period over which exposure is averaged (days) BaP equivalents Benzo[a]pyrene equivalents BW Body weight (kg) CAB County Administrative Board (Länsstyrelsen) Cd Cadmium CF Conversion factor (10-6 kg/mg) CI Confidence interval CR Contact rate, i.e. the amount of water swallowed while
swimming (L/h) CS Chemical concentration in sediment (mg/kg) CW Chemical concentration in water (mg/L) ED Exposure duration (year) EF Exposure frequency (days/year) ET Exposure time, i.e. time spent in water (h/day) IR Ingestion rate, i.e. intake of sediment from the
contaminated source (mg/day) Kd Soil-water distribution coefficient MLR Multiple linear regression PAH Polycyclic aromatic hydrocarbons PBA Probability bounds analysis P-boxes Probability boxes PCA Principal component analysis PCDD Polychlorinated dibenzo-p-dioxins PCDF Polychlorinated dibenzofurans PLSR Partial least squares regression RME Reasonable maximum exposure SA Skin surface area available for contact (cm2/day) SD Standard deviation TRV Toxicological reference value US EPA United States Environmental Protection Agency WHO World Health Organization
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INTRODUCTION
The release of hazardous substances may have negative effects on humans and the environment. These effects, as well as possible measures taken, are evaluated in a risk analysis process. Uncertainty and variability are inevitably included in this process. Knowledge and reliable methods to deal with uncertainty and variability are essential for transparency and trust in the risk analysis process, which is necessary in order to gain regulatory acceptance in decision making. This thesis aims to evaluate some of the tools available and provide insight into how knowledge about uncertainty and variability in the environmental risk analysis process can be managed.
The risk analysis process The risk analysis process can be divided into the following three sub-processes: risk assessment, risk communication and risk management (figure 1) (WHO 2004). The overall process can be seen as an iterative procedure, since previous assessments may be altered and re-evaluated, and new hazards are also continuously identified.
Risk assessment
Hazard identification
Hazard characterization
Exposure assessment
Risk characterization
Risk
communication
Risk management
Risk evaluation
Risk reduction
Risk monitoring
Figure 1. The risk analysis process.
The risk assessment itself can be further divided into different stages: hazard identification, hazard characterization (dose-response assessment), exposure assessment and risk characterization (figure 1) (National Research Council 1983, WHO 2004).
In the first step, hazard identification, potentially harmful factors are identified. The question in the hazard identification is whether a factor can cause negative effects in a system, (sub)population or an organism. A hazard can be defined as a source with potential to cause harm, which can be
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differentiated from the risk, which is the probability to harm or injure and can thereby be expressed as a combination of probability and consequences (Kaplan and Garrick 1981). According to the IPCS (International Programme on Chemical Safety) risk assessment terminology a hazard is defined as an “inherent property of an agent or situation having the potential to cause adverse effects when an organism, system, or (sub)population is exposed to that agent” and a risk as “the probability of an adverse effect in an organism, system, or (sub)population caused under specified circumstances by exposure to an agent” (WHO 2004).
The aim of the second step, hazard characterization, is to further describe and characterize the hazard. It aims to determine possible adverse effects caused by the identified hazard, qualitative or if possible, quantitative. This can be done by determining the relationship between the dose of a substance and the negative effects (dose-response assessment). These first two steps in the risk assessment, hazard identification and hazard characterization, can also be summarized and called hazard assessment.
Even though exposure is often quantified in an exposure assessment, the next step of the risk assessment, it is necessary to bear in mind that this is an assessment that aims to approximate an exposure scenario, not an exact calculation of reality. These assessments are often based on models including input variables that are associated with varying degrees of uncertainty and variability. Questions to be answered in the exposure assessment are, for example: which are the exposure pathways and who is exposed, how is the pollutant transferred, and what is the magnitude of the exposure?
In the fourth and final stage of a risk assessment, risk characterization, the previous stages are pulled together and conclusions are drawn regarding the risk to the environment or the exposed population or organism. This can be done qualitatively, or when possible quantitatively. Risk characterization forms the final and conclusive part of a risk assessment.
Risk communication is the part of the risk analysis process where the outcome of the risk assessment is transmitted to the parties concerned. It is an interactive process which includes the exchange of information between risk assessors, risk managers (decision makers), the media, stakeholders and the public. This stage does not necessarily need to occur only after the risk assessment, but can also be integrated into the assessment, as well as in the next part of the risk analysis, risk management.
Factors such as knowledge and expertise, openness and honesty as well as concern and care increase the perception of trust and credibility, which affect the risk communication (Peters et al. 1997). Risk communication is also closely linked to risk perception. Trust and confidence has shown to reduce the risk perceived (Siegrist et al. 2005). Risk perception is affected by other factors; for example if the risk is unknown (e.g. not possible to observe, delayed effect, new risks), and if the risk is uncontrollable, global, catastrophic or may be high for future generations (dread risk) (Slovic 1987). Several
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studies point out gender as a factor that influences not only risk perception, but also risk judgments (Davidson and Freudenburg 1996, Slovic 1999).
Risk management is the decision making process where political, social, economic and technical factors are considered together with the outcome of the risk assessment (WHO 2004). Transparency is an important factor in the risk management process and has the potential to affect the perceived risk (Sparrevik et al. 2011). In risk management, the risk is evaluated and if necessary reduced and monitored in three different stages (figure 1). In risk evaluation, the assessed risk is evaluated by being contrasted to the positive outcome of a reduced risk, including for example economical values, lives saved or better quality of life, and an improved environment, which then serve as the basis for decision making. Risk reduction includes different measures aiming to reduce, prevent and control risks. This element has also been referred to as emission and exposure control (WHO 2004). The last part, risk monitoring, aims to follow-up the development of risks.
Uncertainty and variability Uncertainty and variability, both often referred to as uncertainties, are present in and affect every risk assessment and need, therefore, to be considered. Mathematical models are often used in risk assessment, and are associated with a varying degree of uncertainty, both in the choice of model and in parameters. Sources of uncertainty in empirical quantities can, for example, include measurement errors, systematic errors, natural variation, inherent randomness and subjective judgments (Granger Morgan et al. 1990, Regan et al. 2002a). There are also uncertainties in language and uncertainties due to disagreement between experts (Carey and Burgman 2008, Granger Morgan and Keith 1995). Risk assessment is inherently subjective as it includes both science and judgments (Slovic 1999).
Various taxonomies of uncertainties have been suggested (Cullen and Frey 1999, Granger Morgan et al. 1990, Rowe 1994). However, uncertainty that is due to a lack of knowledge is often separated from natural variation (variability) (Cullen and Frey 1999, Ferson and Ginzburg 1996, Hoffman and Hammonds 1994), as has also been recommended by the United Stated Environmental Protection Agency (US EPA 1995). In this thesis, uncertainty refers to the uncertainty that arises from a lack of knowledge and variability denotes natural variation.
Uncertainty that is due to incomplete information has, for example, been referred to as epistemic uncertainty, subjective uncertainty, lack-of-knowledge uncertainty, incertitude or ignorance (Cullen and Frey 1999, Ferson and Ginzburg 1996). This uncertainty can be reduced by further investigations.
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The other type of uncertainty is variability and it arises from natural heterogeneity or stochasticity. It cannot be reduced, which differentiates it from uncertainty that is due to lack of knowledge. However, it can be better described, and the uncertainty in our knowledge of variability is thereby reduced (Jager et al. 2001). Different terms used for variability include stochastic uncertainty and aleatory uncertainty (Cullen and Frey 1999, Paté-Cornell 1996).
The following section outlines various types of uncertainty and variability, beginning with uncertainty (Cullen and Frey 1999, ECHA 2008, US EPA 1992, US EPA 2001, WHO 2008):
� Model uncertainty exists since models are never exact representations
of reality, but rather simplifications. Sources of model uncertainty can be extrapolation, dependencies, assumptions and when a model is used out of its applicability domain. Further, the complexity of a model also contributes to uncertainty. Although model uncertainty may decrease with the increasing number of model variables, the estimation error will increase with the increasing number of variables in the model, since there is uncertainty in the parameters included in the model.
� Parameter uncertainty is uncertainty in different types of quantities. These can be both empirical quantities (measurable) and defined constants. Sources of this uncertainty can, for example, be measurement errors, the use of default data and sample uncertainty, that is to say the representativeness of the data set and uncertainty in the choice of statistical distributions.
� Scenario uncertainty is uncertainty in assumptions about different scenarios made in risk assessments; for example in the choice of exposure pathways or in the description of the source and release of a chemical. It arises from a lack of information on present conditions or future scenarios.
Natural variation, or variability, can be of various types; here interindividual, spatial and temporal variability are described (Cullen and Frey 1999, ECHA 2008):
� Interindividual variability is variation between individuals, such as
differences in physiological parameters, lifestyle and consumption rates. There is also variability within an individual: intraindividual variability. This type of variability can also be mentioned as inter- and intraspecies variability.
� Spatial variability is variation in space, for example differences in the distance between the source of the contamination and the exposed
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individuals. In air and water, the concentration of the contaminant can vary rapidly. Contaminations in soil also differ depending on geographical variation.
� Temporal variability is variation over time. For example, the pollutant concentration in ambient air can vary dramatically over time, depending on wind velocity and temperature, which can also be mentioned as variability in environmental characteristics. The breathing rate varies over a 24-hour period; food consumption varies depending on the season (home-grown vegetables) and so forth. How these factors are to be handled depends on, for example, the time aspect of the risk assessment; whether it is a short-term risk assessment (acute effects) or a long-term one.
There is also linguistic uncertainty in risk analysis (Carey and Burgman 2008), which means uncertainty in language that arises since natural language often is vague, ambiguous, context dependent, not specific enough or exhibits theoretical indeterminacies (Regan et al. 2002a).
Characterization of uncertainty and variability in risk assessments An appropriate treatment of variability and uncertainty in risk assessment is essential as a basis for decision making (Aven and Zio 2011). The various methods used in quantitative risk assessments as well as the flexibility in the different methods imply that the inputs in a quantitative risk assessment, and thus the characterization of variability and uncertainty, can take different shapes: point estimates, probability distributions, probability boxes (p-boxes), as well as fuzzy arithmetic including intervals (Darbra et al. 2008, Ferson 2002, Hammonds et al. 1994).
Deterministic risk assessment In a deterministic risk assessment, each input parameter is given by a point estimate. Variability and uncertainty can be taken into account when choosing the input; however, variability and uncertainty are not controlled or evaluated in the calculations. The traditional way of handling uncertainty and variability has been to incorporate safety factors or use conservative assumptions, which can lead to unrealistically high estimations which are neither transparent nor efficient when further testing or measures might be necessary (Jager et al. 2001). Conversely, it is also possible to underestimate the exposure for sensitive populations (Bonomo et al. 2000). Deterministic estimations cannot elucidate the number of individuals that might be exposed to a dose over a
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reference value or the probability of a certain exposure. Furthermore, deterministic estimations are given with a precision that does not reflect the uncertainty and variability that is inevitable in such assessments.
Probabilistic risk assessment Probabilistic risk assessment is an alternative to deterministic risk assessment. The interest in and attention given to probabilistic methods in the chemical and environmental field have increased during the past years (Bogen et al. 2009, Jager et al. 2001, Lester et al. 2007, Mekel and Fehr 2001, Öberg and Bergbäck 2005), although it has been used before in the nuclear field (US NRC 1975).
Probability is the likelihood of a certain outcome and is expressed as a number from 0 to 1, where 0 indicates that the outcome is impossible and 1 indicates that the outcome is sure to happen. Even though there is not one single definition of probability, the definition “the extent to which an event is likely to occur” is according to the ISO (the International Organization for Standardization)/IEC (the International Electrotechnical Commission) Guide 73. In order to make a probabilistic evaluation of risk, it is consequently necessary to account for uncertainty and variability. Thus, in probabilistic methods, variability and uncertainty are characterized to obtain a more transparent and better basis for decision making.
Probabilistic risk assessments can be performed in various ways, for instance using interval calculations, Monte Carlo analysis or probability bounds analysis (PBA) (Ferson 2002, Hammonds et al. 1994, US EPA 1997b). But probabilistic approaches require more work, quality assurance and awareness of limitations. However, one procedure does not exclude the other; point estimates can be used initially, and thereafter complemented by probabilistic methods in cases where risks cannot be fully excluded.
Interval calculation is a simple method to evaluate variability and uncertainty and it is similar to the point estimate but complemented with a second value. It can be a minimum and maximum value or a best estimate and a reasonable maximum exposure (RME).
Describing inputs as parametric or empirical distributions is a common approach in probabilistic risk assessment. An empirical distribution is based on data, while a parametric has a functional form and is defined by a few parameters (Cullen and Frey 1999). Moments are used to describe the shape of a probability distribution and thereby also the variability. The first, second, third and fourth moments are mean, variance, skewness and kurtosis, respectively. Kurtosis is the peakedness of a distribution. Skewness describes the asymmetry of a distribution; thus, a symmetric distribution has a skewness of zero.
In a Monte Carlo simulation, probability distributions are used to characterize variability and values are randomly selected from these distributions in a large number of iterations (US EPA 1997b). Monte Carlo
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analyses can be performed one-dimensionally with only single distributions. The distributions can also be complemented with estimations of uncertainty and is thereby two-dimensional, and variability and uncertainty are then propagated separately (WHO 2008). A separation of variability and uncertainty is important since it will increase the accountability and transparency of a risk assessment (US EPA 1997b).
While probability theory has been accepted as a suitable tool to describe variability, there have been discussions on the proper way to describe uncertainty; other methods such as interval analyses and fuzzy logic have been suggested (Aven 2010, Darbra et al. 2008, Ferson and Ginzburg 1996). Thus, probability distributions are an optimal way to describe variability when much information is available. But it is usually not possible to give an exact description of variability in the form of a distribution. The choice of a distribution is associated with uncertainty and this step is therefore of great importance and should be documented (Burmaster and Anderson 1994, Haas 1997, US EPA 1997b, US EPA 2001). In cases where the precise distribution or the parameters used to define a distribution cannot be given, probability boxes (p-boxes) may serve as an alternative since the exact distribution does not need to be specified.
In a probability bounds analysis (PBA), probability boxes are defined by combining probability theory with interval arithmetic, describing variability and uncertainty, respectively (Tucker and Ferson 2003). Specific distribution does not need to be chosen although it is possible. P-boxes do not represent a single distribution, but rather a class of distributions (Tucker and Ferson 2003). P-boxes can be defined using different inputs depending on the information available; for example distributions or a variety of different statistical parameters, such as mean, standard deviation (SD) and percentiles. This information on variability can be combined with uncertainty intervals such as confidence intervals. A wide variety of statistics can be used in different combinations to define the p-boxes. A further description and examples of p-boxes are given in the method section as well as in the appendix.
Aims of the included papers in a risk-analysis context The research in this thesis is focused on different parts of the risk analysis process and the overall goal is to provide information that aims to facilitate the performance of transparent, comparable and trustworthy risk analyses.
In paper I, the aim was to investigate varying catalyzing potency of different metals in the formation process of chlorinated aromatic compounds during heating of fly ash. Chlorinated aromatic compounds are toxic,
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persistent and unwanted by-products and a description of these emissions is useful information in a hazard identification and characterization.
The main aim of paper II was to provide data on Swedish exposure factors (physiological parameters, time use factors and food consumption) including measures of variability and uncertainty. Exposure factors data that are well-described will facilitate the performance of risk assessments and contribute to more transparent and comparable risk assessments. The statistics provided in paper II can be used in deterministic risk assessments as well as in probabilistic ones, as shown in paper III and IV where PBA was used as a probabilistic approach.
In paper III, the exposure to a number of metals and polycyclic aromatic hydrocarbons (PAHs) at a public bathing place was assessed. Previous measurements in sediments from the deeper parts of the lake showed contamination levels of concern (Sternbeck et al. 2003), and the aim was therefore to investigate whether recreational activities such as swimming may cause any significant adverse health effects.
PAHs are persistent and metals are not biodegradable; both of them have the potential to be toxic for future generations as well. The aim of paper IV was to exemplify how future climate changes may affect cadmium exposure for 4-year-old children at a highly contaminated iron and steel works site in southeast Sweden. Of the 39 model variables six were assessed to be sensitive to a change in climate, and thus changed in two different climate change scenarios and compared to a present scenario.
While papers I to IV mainly concern risk assessment, paper V is about risk management. These processes are equally important since the information about the risk needs to be managed in order to lead to improvement and thereby good health and environment. A questionnaire was sent to employees at all the Swedish County Administrative Boards (Länsstyrelsen) working with contaminated land. The aim was to investigate if the employees’ gender, age and experience affect their reviewing of risk assessments and their perception of knowledge gained from the research programme Sustainable Remediation. The funding source of the contaminated land project was also considered: projects financed by the government or by a legally responsible operator.
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METHODS
Catalytic effects of metal oxides Chlorinated aromatic compounds, such as dibenzo-p-dioxins (PCDD) and dibenzofurans (PCDF) are toxic, persistent and unwanted by-products of the combustion process. To investigate the variability in catalytic effects of different metal oxides on the formation and degradation of chlorinated aromatic compounds, fly ash was mixed in glass tubes with metal oxides in various combinations (paper I). The fly ash originated from an electrostatic precipitator at a biofuel incinerator, where the fuels consisted of household and industrial wastes (paper and textiles). The content of fly ash had been investigated previously, and it includes a wide variety of different elements and chlorinated aromatics (Öberg et al. 2007b). The glass tubes were sealed with permeable polyurethane foam plugs and heated. The test tubes with fly ash and foam plugs were thereafter analysed at an accredited laboratory as a composite sample. The samples were analysed for chlorinated benzenes, polychlorinated dibenzo-p-dioxins (PCDD) and dibenzofurans (PCDF).
Factorial experiment The catalytic effects of metal oxides (magnesium, yttrium, titanium, vanadium, niobium, chromium, molybdenum, tungsten, manganese, iron, cobalt, nickel, copper, zinc and tin) were statistically evaluated by a factorial experiment. The aim with an experimental design like this is to analyse each factor separately, without confounding with the other factors.
Fifteen factors (the metal oxides) were investigated initially by a resolution III fractional factorial, including 16 runs and two replicates. This experiment was not enough for separating main effects from two-factor interactions, since the number of significant factors was too high. The resolution III experiments were therefore complemented by a fold-over, giving a resolution IV fractional factorial, with a total of 32 runs and four replicates. The main effects were thereby separated from the two-factor interactions. These two experimental batches were performed with a time interval of six weeks. As control two replicates without any metal oxides were included in each batch.
Data analysis The data analysis was conducted by linear multiple linear regression (MLR), analysis of variance (ANOVA) and partial least squares regression (PLSR).
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The software programs Design-Expert v6.0 (Stat-Ease Inc.) and Unscrambler v9.1 (CAMO software A/S) were used for the data analysis.
Multiple linear regression (MLR) is an approach to analyse one response variable, and it was used to fit linear polynomial models to the data. The statistical significance of these models was assessed with an ANOVA.
Partial least squares regression (PLSR) is a multivariate approach, meaning that several variables for each observation can be analysed simultaneously. In this case correlations between different congeners of chlorinated benzenes, PCDD and PCDF were analysed.
Variability and uncertainty in exposure factors Information on relevant non-chemical specific exposure factors was compiled and evaluated in paper II. With the help of literature searches and direct contact with researchers and other external information contributors, information about exposure factors, such as body weight, time use, food consumption, was collected from official statistics, technical reports and the scientific literature. Primary data were obtained from external studies (Becker and Pearson 2002, Berg et al. 2009, Boldeman et al. 2004, Boldemann et al. 2006, Boström 2006, Pettersson and Rasmussen 1999, Sepp et al. 2002, Västernorrland County Council n.d.) and were used for further statistical evaluations with the kind permission of the data owner. The statistical evaluations included characterizations of interindividual variability as well as uncertainty. Interindividual variability was described by arithmetic mean, standard deviation (SD), skewness, kurtosis and multiple percentiles. The calculated percentiles were 1, 5, 10, 25, 50 (median), 75, 90, 95 and 99; however, the 1st and 99th percentiles were not always calculated depending on sample size. Calculations were made with SPSS 15.0 for Windows (SPSS Inc., Chicago, IL).
All the above-mentioned measurements of interindividual variability are more or less uncertain. To describe uncertainty, 95% confidence intervals (CI) were estimated with bootstrapping. The Excel add-in module Crystal Ball v7.2.2 (Decisioneering Inc., Denver, CO) was used with 10 000 bootstrap replications for the calculations.
Bootstrapping Bootstrapping, or “resampling of data with replacement”, is a technique used for statistical inference, such as estimating confidence intervals, to assess the accuracy of different parameters (Efron and Tibshirani 1993). The term refers to the idiomatic expression “to pull oneself up by one’s bootstraps”, in this case meaning that only primary data are used for the statistical analyses, i.e. the
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resampling is non-parametric (empirical distributions are used). Therefore, no underlying assumption about distribution of data is needed, unlike many other statistical analyses. This is an advantage since assumptions about underlying distribution are uncertain (Binkowitz and Wartenberg 2001, Sander et al. 2006). Furthermore, bootstrapping can provide confidence intervals where analytical mathematical solutions are missing (Frey and Burmaster 1999).
But the primary data limits the bootstrap analysis and thus this analysis only addresses the uncertainty that comes from the error due to a finite sample size. Other sources of uncertainty, such as analytical error, biased sampling designs, bias in self-reporting or differences between the population in the survey and the population of concern in a risk assessment are not considered. Some of these sources of uncertainty are discussed in paper II.
Bootstrapping was used to generate confidence intervals (95%) for all parameters that describe interindividual variability: mean, SD, skewness, kurtosis and multiple percentiles.
Bootstrapping works as follows (Efron and Tibshirani 1993):
� Values from the dataset are randomly selected. Each sample is replaced after selection and the random selection continues until as many values have been selected and replaced as there are values in the data set. If a dataset contains 841 values (as in the case for girls’ body weight and skin surface area in table 1 under Results and discussion), 841 values are randomly selected and replaced. This means that some values might be selected several times and others not at all.
� Parameters (mean, SD, skewness, kurtosis and multiple percentiles) are calculated in the new dataset.
� This process is repeated a large number of times, in this case 10 000 so-called bootstrap replications. These 10 000 replications each contain 841 values drawn from the original primary data set. This will generate 10 000 different estimations of each parameter, from which confidence intervals can be calculated from the percentiles. The 95th percentile is then given by the 2.5th and 97.5th percentile.
Since confidence intervals for high and low percentiles were calculated,
10 000 replications were chosen. A large number of bootstrap replications are then needed to provide a stable estimate since empirical data are fewer in the tails of the distribution.
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Exposure assessments Deterministic and probabilistic risk assessments have been performed both in papers III and IV. Paper III concerns exposure to metal- and PAH-contaminated sediments at a public bathing place, and paper IV concerns exposures of cadmium at a highly polluted iron and steel works site and the possible impacts of uncertainty due to climate changes.
Exposure to contaminated sediments at a public bathing place The exposure to contaminants in sediment and lake water during recreational activities, such as swimming and playing in water at a public bathing place was assessed at Lake Trekanten, Stockholm, Sweden. Best estimates (average) and reasonable maximum exposures (RME) (95th percentile) were assessed for a number of metals and PAHs, which were complemented by a probabilistic assessment performed by probability bounds analysis (PBA).
A multiple pathway model, which in this case is a mathematical description of the exposure process, was used for the exposure assessment. The exposure pathways considered were oral intake of contaminants from lake water, oral intake of contaminants from sediment and dermal uptake of contaminants from sediment. The exposure model conforms to the US EPA multiple pathway model for Superfund risk assessments (US EPA 1989).
Oral intake of contaminants from lake water while bathing, mg/kg-day (Iw) is determined by chemical concentration in water, mg/L (CW), amount of water swallowed, L/h (CR), exposure time, i.e. time spent in water, h/day (ET), exposure frequency, i.e. days spent at the site, days/year (EF), exposure duration, years (ED), body weight, kg (BW) and the period over which exposure is averaged, days (AT):
ATBW
EDEFETCRCWIw
×
××××= (Eq. 1)
Oral intake of contaminants from sediment, mg/kg-day (Is) is determined by chemical concentration in sediment, mg/kg (CS), ingestion rate, i.e. intake of sediment from the contaminated source, mg/day (IR), exposure frequency, days/year (EF), exposure duration, years (ED), body weight, kg (BW) and the period over which exposure is averaged, days (AT). A conversion factor of 10-6 kg/mg is also included:
ATBW
EDEFCFIRCSIs
×
××××= (Eq. 2)
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Dermal uptake of contaminants from sediment, mg/kg-day (Idu) is determined by chemical concentration in sediment, mg/kg (CS), skin surface area available for contact, cm2/day (SA), sediment-to-skin adherence factor, mg/cm2 (AF), absorption factor, no unit (ABS), exposure frequency, days/year (EF), exposure duration, years (ED), body weight, kg (BW) and the period over which exposure is averaged, days (AT). A conversion factor of 10-6 kg/mg is included:
ATBW
EDEFABSAFSACFCSIdu
×
××××××= (Eq. 3)
When calculating with imprecise figures, such as intervals or probability boxes, repeated parameters can result in greater uncertainty than necessary (Ferson 2002). To avoid repetition of exposure factors in the probabilistic calculation, the exposure pathways (Eq. 1-3) were reorganized and summarized as follows:
ABS))))AF(SA(IRCF(CSET)CR((CWATBW
EDEFItot ××+××+×××
×
×=
(Eq. 4)
To estimate the contaminant uptake as accurately as possible, the exposure factors in equations 1-4 should be characterized. Behaviour (exposure time and exposure frequency) was investigated on site at the bathing place (Lindström 2006). Sediment and water samples were collected at the bathing site (Peltola 2006, Peltola 2007).
Other exposure factors data were compiled from various sources. Body weight and skin surface area are according to paper II. Accidental water ingestion while swimming was investigated by the US EPA in a pilot study and a full field sampling study (Dufour et al. 2006, Evans et al. 2006). Primary data from the full field sampling study (Evans et al. 2006) were used to characterize variability and uncertainty with the same approach as in paper II.
Children’s intake of sediments was estimated according to the Exposure Factors Handbook and the Child-Specific Exposure Factors Handbook (US EPA 1997a, US EPA 2002). A conservative estimate of the mean value was chosen as a best estimate since it is reasonable that the exposure to sand is higher at a sandy bathing place. A sediment-to-skin adherence factor for children was estimated by combining sediment-to-skin adherence data (Shoaf et al. 2005) with the information on the percentage of skin surface area per body part (US EPA 1985).
The Risk Assessment Guidance for Superfund Volume I: Human Health Evaluation Manual (Part E, Supplemental Guidance for Dermal Risk
18
Assessment) recommends that, due to a lack of further information, the same absorption factor as for soil is used for sediment (US EPA 2004). In the same report, an absorption factor of 13% has been recommended specifically for PAHs, based on a study by Wester et al. (1990). This value is likely an overestimation for the exposure scenario at Lake Trekanten, since the contact time was 24 hours in the survey. A number of additional studies also indicate that 13% for PAHs is an overestimate (Abdel-Rahman et al. 2002, Kao 1989, Roy and Singh 2001, Sartorelli et al. 2001, Yang et al. 1989). Further, the absorption has been shown to decrease when the contaminants are mixed with the soil for a longer period of time (Abdel-Rahman et al. 2002, Roy and Singh 2001). For these reasons, half the value was used as the best estimate.
Climate change – an uncertainty factor in risk analysis The exposure assessment in paper IV considers climate change by comparing a present-day exposure scenario with two possible scenarios in which climate-sensitive variables were altered. The investigated site was Kallinge Bruk, a heavily contaminated former iron and steel works site in southeastern Sweden (Sander and Öberg 2006).
In the two climate change scenario the climate-sensitive variables were changed in an order of 5-10% and 15-20% respectively. The variables that were assessed, by a literature review, as climate-sensitive were soil moisture, groundwater recharge, hydraulic conductivity, soil-water distribution coefficient (Kd) and bioconcentration factor for root respective stem. A further explanation with motivation for the choice of climate sensitive variables is given in paper IV.
A similar multiple pathway model to that used in paper III was also applied for this exposure assessment. The model used in this case was developed by the Swedish Environmental Protection Agency for use in contaminated land risk assessments (Swedish EPA 2009). The exposure pathways considered were oral intake of contaminants from ground water and vegetables, as well as direct soil contact (inhalation of dust, ingestion of soil and dermal contact). Inhalation of volatile compounds is considered in the original model but was not included in this assessment as Cd is not volatile. The exposure model and input variables are thoroughly described in paper IV with its appendix and the exposure assessment is therefore not further exemplified and described here.
Probability bounds analysis (PBA) The probabilistic approach applied in paper III and IV was probability bounds analysis (PBA) using the software program RAMAS Risk Calc v4.0 (Applied Biomathematics, Setauket, NY) (Ferson 2002). The method was originally developed in the 1980s (Frank et al. 1987, Williamson and Downs 1990) and
19
the approach has thereafter been applied in different context in the environmental and technical field (Karanki et al. 2009, Kriegler and Held 2005, Regan et al. 2002b), including assessment of contaminated land (Regan et al. 2002c).
In a PBA, variability and uncertainty are propagated separately by letting the input variables be described by probability boxes (p-boxes) and the result is thus also presented as p-boxes. P-boxes (examples are shown in figure 2 and the appendix) are delimited by two cumulative distribution functions. Variability is then represented by the probability distributions and uncertainty by interval bounds (the horizontal distance between the two distribution functions).
0 10 20 30 400
0.5
1
BW1
BW3
BW2
Figure 2. P-boxes, describing body weight (kg) of girls (age 4), delimited by different parameters
but using the same data from table 1. The data originates from paper II. The y-axis shows
cumulative probability from 0 to 1.
Parametric distributions, for example normal or log-normal, with or without uncertainty bounds on the parameters that specify the distribution can be used to define p-boxes. Figure 2 shows three different p-boxes. The
P-boxes are delimited by: min, max and uncertainty intervals of mean and SD
min, max and uncertainty intervals of mean, SD and multiple percentiles normal distribution specified with uncertainty intervals of mean and SD
20
narrowest is defined with a normal distribution specified with uncertainty intervals (95% confidence intervals) of the mean and standard deviation (SD).
However, assumptions about a specific distribution are uncertain, as previously highlighted (Binkowitz and Wartenberg 2001, Filipsson et al. 2008, Sander et al. 2006). But p-boxes can also be constructed using available information without making any further assumptions about distributions.
In paper II, interindividual variability was described by the different statistical parameters mean, standard deviation (SD), skewness, kurtosis and multiple percentiles. Confidence intervals (95%) were used as estimates of uncertainty of the parameters, which can be used to define p-boxes as in papers III and IV. Figure 2 also shows a p-box defined by minimum, maximum and uncertainty intervals of the mean, SD and multiple percentiles. If little information about the input variable is known, the p-box can be delimited by less information. This means that available data can be fully applied (Ferson 2002).
A wider p-box delimited by minimum, maximum and uncertainty intervals of the mean and SD is also shown in figure 2. Less information will generate a wider p-box along the horizontal axis. PBA thus consider the uncertainty in the selection of input distributions (Ferson 2002, Ferson and Ginzburg 1996), since a certain p-box encloses all possible distributions that are in agreement with the specified constraints. The bounds will be tighter if more data is specified and the p-box will then gradually move closer to the true distribution. In the exposure assessments in paper III and IV, one parametric distribution, the lognormal, was only used to define the p-box in the case of cadmium soil concentration in paper IV as more data were available.
Risk management of contaminated land
The questionnaire A questionnaire was sent to employees working with contaminated land at all Swedish County Administrative Boards (CAB), a government authority in each of the 21 Swedish counties. The aim was to investigate if the personal factors gender, age and experience affect the reviewing of risk assessments. The funding source of the contaminated land project was also considered by asking the same questions for projects financed by governmental grants and by the legally responsible operator, respectively. Further, the questionnaire included questions and statements about perception and the application of knowledge gained from the research programme Sustainable Remediation, which involved around 50 projects during the period 2003-2009 (Svensson et al. 2009). All questions and statements are given in paper V. The respondents rated answers from 1 to 5, where 1 is “do not agree at all” and 5 is “totally
21
agree”, with some exceptions where the answer had to be given as text, numbers or yes/no.
Data analysis The respondents’ answers with respect to their gender, age and experience were analysed with two multivariate methods, principal component analysis (PCA) and partial least squares regression (PLSR). Both PCA and PLSR are based on linear transformations to a limited number of orthogonal factors. In PCA the covariance between the original variables are maximized (Jackson 1991). Patterns in the whole data set can thereby be identified initially. This analysis showed that gender was the most important factor and the correlation between respondents’ gender and their answers was therefore analyzed with a discriminant analysis using PLSR. In PLSR the covariance between a linear combination of the independent predictor variables and a linear combination of the dependent response variables are maximized (Martens and Næs 1989). Jack-knifing was used to assess the statistical significance (Westad and Martens 2000). The lengths of employment and working experience were log-transformed. Gender, job description and yes/no questions were coded into dummy variables. The variables were standardized to zero mean and unit variance before the data analysis. The analysis was performed using the software program Unscrambler v9.1 (CAMO Process, Oslo, Norway). Additional t-tests, with significance level of α=0.05, were performed using PASW Statistics 18 (SPSS Inc., Chicago, IL, USA).
22
RESULTS AND DISCUSSION
Catalytic effects of metal oxides The catalytic activity of copper in the formation process of chlorinated aromatic compounds has been shown in several studies (Hatanaka et al. 2003, Takayuki et al. 2007, Taylor and Lenoir 2001, Öberg and Öhrström 2003). Other metals also seem to affect the catalytic formation or degradation (Öberg et al. 2007a, Öberg et al. 2007b).
In line with previous studies, copper showed a positive catalytic effect on the formation of chlorinated aromatic compounds in paper I. A weak positive effect could also be observed for zinc. Conversely, chromium, cobalt and vanadium showed catalytic effects for degradation of chlorinated aromatic compounds. A weak negative effect was observed for iron. The other metals did not yield any significant effects.
These results found contribute to the understanding of formation and degradation of chlorinated aromatic compounds in thermal processes (combustion, metal industries, etc.) and can provide valuable information for use in risk assessment involving these compounds. The information can also lead to improved risk management strategies to reduce the emissions. The statistical experiment design was a useful approach to screen the effects of 15 metals at the same time and thereby identify and characterize hazards.
Variability and uncertainty in exposure factors Variability has been presented previously in a number of secondary sources (ECETOC 2001, US EPA 1997a, US EPA 2008, US EPA 2009, Vuori et al. 2006), but information about uncertainty is mostly lacking. In paper II, data on Swedish exposure factors including variability and uncertainty are presented under the following categories:
� Physiological parameters (body weight and skin surface area). � Time use (time outdoors during stay in preschools). � Intake of food and water (vegetables, fruit and berries and tap water). The data analyses showed that there is a major interindividual variability
inherent in these exposure factors, which must be considered in risk assessments. However, there is not only variability between individuals within the same gender and age group, but also between different age groups and
23
between females and males. The exposure factor parameters are also uncertain and here these uncertainties are represented by 95% confidence intervals. The statistics provided can be used as point estimates, as well as in probabilistic assessment, as exemplified in paper III and IV.
As example of the data, table 1 shows girls’ body weight and total skin surface area. Additional statistics are given in paper II and in a more extensive report in Swedish (Filipsson et al. 2008). Table 1. Girls’ (age 4)1 body weight and total skin surface area calculated using data from the database Epibarn (Västernorrland County Council n.d.).
Body weight (kg) Total skin
surface area (m2)
N 841 841
Mean 18.2 (18.0-18.4)
0.75 (0.74-0.75)
SD 2.8 (2.5-3.0)
0.07 (0.06-0.07)
Skewness 1.5 (0.8-2.1)
0.98 (0.49-1.49)
Kurtosis 8.7 (4.1-13.4)
6.19 (3.53-9.34)
Percentiles
1 12.8 (12.3-13.8)
0.61 (0.59-0.63)
5 14.6 (14.3-14.8)
0.65 (0.64-0.66)
10 15.2 (15.0-15.4)
0.67 (0.66-0.67)
25 16.4 (16.2-16.6)
0.70 (0.70-0.71)
50 17.8 (17.6-18.0)
0.74 (0.73-0.74)
75 19.6 (19.2-19.8)
0.78 (0.77-0.79)
90 21.6 (21.0-22.0)
0.83 (0.82-0.84)
95 23.4 (22.6-24.2)
0.87 (0.85-0.89)
99 27.1 (24.8-28.2)
0.94 (0.91-0.97)
1 Mean age was 4.1 years. Most children were aged between 4.0 and 4.9: only 7% were aged 3 years and only 1.5% 5 or 6 years.
There is still a need for more supporting data, both on uncertainty and variability. Data must be collected, evaluated and made available for risk
Variability
Confidence interval (95%) within brackets representing uncertainty
24
assessors. There is a lack of information for some factors, in particular the consumption of home-grown vegetables, tap-water consumption (from private wells) and time-use patterns. Several factors were not evaluated in this study, such as chemical specific exposure factors. Dependencies between exposure factors were not investigated, but should preferably be characterized. There is also an ongoing need for collection and evaluation of exposure factors data since new studies are published constantly. During the data compilation presented in paper II, new surveys without published results were found, for example on time spent outdoors1 and time spent by children in day care centers2. Furthermore, some surveys recur over time, for example Health on Equal Terms was performed in 2010 for the seventh time (FHI 2010). Body weight, which has increased over time (Berg et al. 2005, Portier et al. 2007, Rasmussen et al. 1999), is included in this survey. Other factors, such as food consumption, also change over time (Becker and Pearson 2002), which motivates a re-evaluation with time.
Exposure assessments The results from the exposure assessments performed in papers III and IV are presented and discussed below under the headings “Exposure to contaminated sediments at a public bathing place” and “Climate change – an uncertainty factor in risk analysis”, respectively.
Exposure to contaminated sediments at a public bathing place PAHs are a group of ubiquitous environmental contaminants which include more than 100 substances that humans are exposed to, most often as mixtures rather than individual compounds (Ramesh et al. 2004). The exposure assessment for PAHs for children aged 1 to 6 years are shown below. Other exposure durations have been evaluated and are presented in paper III. The assessment is also presented in a more extensive report in Swedish (Filipsson and Öberg 2008).
Deterministic exposure assessment
The contaminant intakes for recreational users of Lake Trekanten were estimated using the exposure model (equations 1-4), the measured chemical
1 Adonix (Adult onset asthma and nitric oxide) at Occupational and Environmental Medicine, the Sahlgrenska Academy, University of Gothenburg, Sweden. Publication is in preparation (personal communication, Kristina Wass, January 24, 2011). 2 Daghemsmiljöns betydelse för astma och allergiska besvär hos barn at SP Technical Research Institute of Sweden. Publication is in preparation (personal communication, Thorbjörn Gustavsson, January 14, 2011).
25
concentrations in sediment and water, and the estimated exposure factors shown in table 2 for the deterministic assessment and in the appendix for the probabilistic assessment. Both best estimates and reasonable maximum exposures were calculated using point estimates. Since some PAHs are genotoxic and carcinogenic, the calculations are averaged over a lifetime (80 years), which means that the exposure is averaged over 29 200 days (365 days × 80 years). The toxic equivalency factors suggested by Nisbet and LaGoy were adopted, and the chemical concentrations of individuals PAHs were recalculated to benzo[a]pyrene equivalents (BaP equivalents). With this procedure individual PAHs were multiplied with weighting factors and summarized (Nisbet and LaGoy 1992). Table 2. Parameters used in the deterministic exposure calculation for PAHs in the case of 4-year-old children.
Parameter Definition Best estimate
RME
ABS Absorption factor (no unit) 0.65 0.13
AF Sediment-to-skin adherence factor (mg/cm2) 0.70 1.17
BW Body weight (kg) 18.2 14.6
CR Contact rate (water swallowed while swimming) (L/h) 0.054 0.16
CS Chemical concentration in sediment (mg/kg) 0.018 0.074
CW Chemical concentration in water (mg/L) 1.0E-5 1.5E-5
EF Exposure frequency (days/year) 32 70
ET Exposure time, i.e. time spent in water (h/day) 1 4
IR Intake of sediment from the contaminated source (mg/day) 200 400
SA Skin surface area available for contact (cm2/day) 7500 6500
The RME daily intake is calculated as follows (Eq. 1-3):
day-mg/kg 7-1.1E 8-7.2E 8-2.9E 9-9.5E
292006.14
67013.017.16500000001.0074.0
292006.14
670000001.0400074.0
292006.14
670416.0000015.0
IIII duswtot
=++
=
×
××××××
+
×
××××+
×
××××
=++=
26
This calculation shows that the most important exposure pathway for BaP equivalents is skin absorption. However, skin absorption is likely a highly uncertain pathway since several studies indicate that the absorption factor of 13% is overestimated (Abdel-Rahman et al. 2002, Kao 1989, Roy and Singh 2001, Sartorelli et al. 2001, Yang et al. 1989). By replacing the exposure factors by best estimates (table 2), a best estimate of the exposure can be calculated.
This calculation does not consider differences in bioavailability by oral intake. These differences increase the overall uncertainty in the intake estimates. However, sufficient data were not available to characterize this additional uncertainty.
Depending on the characteristics of some contaminants, the estimated daily intake can be averaged over a year rather than a life-time, which is further explained in paper III. In practice it means that exposure duration (ED) can be eliminated and the period over which exposure is averaged (AT) can be set to 365 days, since when ED is X years, depending on the assumed exposure scenario, AT will be X × 365 days and the number of years is therefore not relevant.
Probabilistic exposure assessment
As an example, an exposure assessment is shown for someone living in the vicinity between 1 and 6 years of age. Equation 4 was used for the probability bounds analysis (PBA). Information about how the probability boxes were entered into Risk Calc is given in the appendix. The result of the probability bounds analysis can be viewed both numerically and graphically as p-boxes. Uncertainty intervals in median and 95th percentile average lifetime daily intake of BaP equivalents are shown in table 3, and the corresponding p-boxes in figures 3 and 4.
There are often correlations between exposure factors. Dependencies could not be excluded for some factors in this PBA, which results in wider uncertainty intervals. Partial dependencies were assumed between some factors: body weight and the intake estimates, sediment intake and skin surface area, and sediment-to-skin adherence factor and absorption factor. Table 3. Uncertainty intervals in daily intakes of BaP equivalents during age 1 to 6 years on a lifetime basis, assuming independence or partial dependencies between exposure factors (mg/kg-day).
Median 95th percentile
Independence [1.1E-11, 1.9E-08] [1.5E-10, 1.8E-07]
Partial dependencies [3.0E-12, 7.2E-08] [2.1E-11, 5.6E-07]
27
0 1e-06 2e-06 3e-060
0.5
1
Intake1_6_independence
Figure 3. P-box. Intakes of BaP equivalents during age 1 to 6 years on a lifetime basis (mg/kg-
day), assuming independence of exposure factors. The y-axis shows cumulative probability from 0
to 1.
0 1e-06 2e-06 3e-060
0.5
1
Intake1_6_dependence
Figure 4. P-box. Intake of BaP equivalents during age 1 to 6 years on a lifetime basis (mg/kg-
day), assuming partial dependencies between exposure factors. The y-axis shows cumulative
probability from 0 to 1.
28
The best estimate and RME assessed deterministically are found within
the interval of the probabilistic uncertainty interval for the median and 95th percentile respectively. The upper uncertainty bound of the 95th percentile is higher and more conservative than the point estimate for the RME.
Risk characterization
The estimated lifetime exposure for BaP equivalents was compared to a risk-based daily intake of 8.3E-7 mg/kg-dag, which corresponds to a lifetime cancer risk of 1E-6 (Swedish EPA 2009). The estimated BaP-equivalents exposure during age 1 to 6 years was thus lower than the risk-based daily intake in both the deterministic and the probabilistic estimations. As shown in paper III, the risk-based daily intake was only slightly exceeded in some cases when longer exposure duration was assumed, together with assumptions about partial dependencies between some exposure factors. The overall conclusion of the risk assessment is that exposure to toxic substances while bathing in Lake Trekanten does not lead to any significant negative health effects in the population.
This assessment is valid for the current levels measured and changes in conditions were not considered. Consumption of fish and crayfish from the lake could also be a possible exposure pathway but was not considered in this assessment.
Climate change – an uncertainty factor in risk analysis The exposure assessment in paper IV concerns cadmium (Cd), which is a toxic metal that occurs in our environment, both naturally and anthropogenically (Järup and Åkesson 2009). Metals are not biodegradable and thus have the potential to be toxic for future generations as well. At the same time, human activities affect the global climate (Houghton 2005). A change in climate will likely also alter different input variables in an exposure model.
In this exposure scenario, the exposure pathways were somewhat different from the scenario at Lake Trekanten. But the principle and approach are similar. The exposure pathways considered were ingestion of contaminated soil, groundwater and vegetables grown on the site, as well as dermal uptake and inhalation of dust. The assessment considers exposure to Cd for a 4-year old child and the objective was to compare present conditions with two possible climate change scenarios, referred to as scenario I and II, at a highly contaminated iron and steel works site in southeastern Sweden.
It was assessed that six of the 39 model variables could possibly change with a changing climate. As example, the climate sensitive variables and the expected change in scenario II are shown in table 4. It is uncertain how future
29
climate change will affect these variables, but an estimation of the change was made using a literature search presented in paper IV.
Table 4. Model variables estimated to likely change with a change in climate and the parameters at present scenario compared to the expected change in climate change scenario II. Climate sensitive variables
Defining parameters in PBA
Present scenario
Expected change in climate scenario
Soil moisture, dm3/dm3 min max mode
0.05 0.50 0.30
0.04 (-20%) 0.40 (-20%) 0.24 (-20%)
Groundwater recharge, m/yr
interval [0.2;0.4] [0.17;0.34] (-15%, -15%)
Hydraulic conductivity, m/s
min max mode
6.0E-6 2.0E-5 1.3E-5
4.8E-6 (-20%) 2.4E-5 (+20%) 1.3E-5 (±0%)
Soil-water distribution coefficient (Kd), dm3/kg
min max mode
576 1440 1080
461 (-20%) 1728 (+20%) 1080 (±0%)
Bioconcentration factor root, (mg/kg)/(mg/kg)
mean stddev
0.35 0.33
0.42 (+20%) 0.40 (+20%)
Bioconcentration factor stem, (mg/kg)/(mg/kg)
mean stddev
0.85 0.61
1.02 (+20%) 0.73 (+20%)
The total exposure for the present condition was compared to the exposure
after a change in climate sensitive variables. Even though only six of model variables were estimated to be affected by a change in climate, a clear effect was seen on the exposure scenario. An increase in the uncertainty interval could be seen in general in the PBA, that is to say the p-box representing the total exposure got wider both in the lower and upper end along the horizontal x-axis. The comparison of the scenarios shown in table 4 for the 95th percentile showed that the lower bound of the uncertainty interval decreased with 11% while the upper bound increased with 18%. The Kd value was the variable with the strongest influence on the result
As already mentioned, risk assessment includes subjective judgments, as does risk management. Thus, this comparison is not an exact truth. However, it shows that a considerable uncertainty is associated with exposure assessment accounting for possible future climate change. Exposure levels that are close to the toxicological reference value (TRV) under present conditions may in the future exceed the TRV, and thus may also have implications for the risk management process which often needs to rely on precaution.
30
Risk management of contaminated land Risk management is the decision making process where the risk assessment is evaluated in a social, economic and technical perspective (WHO 2004). If necessary, the risk is also reduced and monitored.
Contaminated land risk management is difficult; as pointed out in papers II to IV, uncertainty and variability are present in the risk assessment process and need to be characterized and considered. At the same time, the costs involved in remediation as well as the consequences if no actions are taken may be high.
Uncertainty and variability do not only affect the risk assessment process, but also risk communication and risk management. For example, as already mentioned, there might be uncertainty in language which could be vague or ambiguous (Regan et al. 2002a). Furthermore, hazards and risks are perceived and evaluated differently by different individuals (Byrnes et al. 1999, Davidson and Freudenburg 1996, Gutteling and Wiegman 1993, Slovic 1999, Slovic et al. 1997, Steger and Witt 1989).
Of the questionnaire that was sent to employees at the Swedish County Administrative Boards (CAB) working with contaminated land, 56 questionnaires were returned, which was about 80% of the survey population. However, the response rate varied depending on the part of the questionnaire. The questionnaire revealed that there are significant differences in the reviewing of contaminated land risk assessments depending on the employees’ gender, age and work experience where gender was the most important.
A larger number of women were of the opinion that there were not sufficient guidance documents compared to men. Women agreed to lesser degree that there is enough time to review risk assessments. Women reported that they did not ask the consultants to complement a risk assessment before a decision was taken as often as men do. These differences may indicate a lower degree of confidence by women.
Not surprisingly, employees with less experience were also more likely to indicate that there were not sufficient guidance documents compared to their more experienced colleagues. Similarly, younger employees agreed to a greater extent that their assessments mainly depended on guidance documents, templates or similar, as compared to the older colleagues.
In total, gender was the most significant factor in the reviewing of risk assessments. Gender also affected the perception of knowledge. Compared to women, men estimated themselves to be more informed about the results from the research project Sustainable Remediation. The level of actual knowledge was, however, not measured. Consequently, the knowledge reported here reflects perceived confidence and is not necessarily the same as actual knowledge. In prior research, women had perceived themselves to be less knowledgeable, but at the same time exhibited a higher level of knowledge (McCright 2010).
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The risk assessments can be financed by different sources; governmental grants or operators that are legally obligated to do so. There are most likely greater monetary resources available in projects financed by governmental grants, compared to when a legally responsible operator is the financier. This may also explain why respondents found risk assessments financed by grants to be of higher quality and why these risk assessments carried greater weight in decisions compared to risk assessments financed by a legally responsible operator. The employees estimated that they had more time to review a risk assessment financed by grants and that they co-operated with the companies that performed the risk assessment to a greater extent as compared to when the risk assessments were financed by a legally responsible operator.
The process leading to the remediation of contaminated land, including risk assessment, risk communication and risk management, inevitable involves uncertainties and judgments. These differences affect the risk management process and may therefore also influence the outcome of a contaminated land project.
32
CONCLUSIONS
The focus of this thesis is environmental risk analysis, and the uncertainty and variability in this process, as investigated and reported in five different papers.
The experiments in paper I showed that the catalytic effects of metal oxides on the formation process of chlorinated aromatic compounds during heating of fly ash vary. The results corroborate previous investigations; copper showed a positive catalytic effect on the formation of chlorinated aromatic compounds. In addition, chromium, cobalt and vanadium decreased the formation. Knowledge of the catalytic effects of various metals may facilitate the choice and design of combustion processes in order to decrease emissions, but it also provides valuable information in the risk assessment process, especially in hazard assessment.
Exposure factors of importance in exposure assessments, such as physiological parameters, time use factors and consumption rates, were compiled and evaluated in paper II. Variability and uncertainty in exposure factors are of major importance and need to be considered in exposure assessments. Variability was described by mean, SD, skewness, kurtosis and multiple percentiles, while uncertainty was characterized by 95% confidence interval of these parameters. Exposure factors change over time and there is a lack of data for some exposure factors. New surveys are continuously published and there is therefore an ongoing need to review and evaluate exposure factors data. The compilation and evaluation of exposure factors data enhance the accessibility of information and thus facilitate the performance of transparent and comparable risk assessments.
The exposure factor parameters from paper II were used in exposure assessments in papers III and IV. Uncertainty and variability in the two exposure assessments were described by probability boxes in a probability bounds analysis. An advantage with this method is that no assumptions about specific distribution are needed. Probability boxes were instead constructed from available data. In this way, a great deal of data is not necessary but the available data can be fully applied. It is also an advantage that variability and uncertainty can be described separately. Probability bounds analysis is a rapid and flexible approach for risk assessment and provides a useful alternative to Monte Carlo simulations.
The risk assessment in paper III concludes that even though elevated levels of contaminants had previously been found in the sediment in the deeper part of the lake, bathing was not considered to cause any harm.
The exposure assessment in paper IV accounted for possible changes due to a change in climate. Both an increase and decrease in exposure were seen
33
after altering the six variables that were assessed to be sensitive to a change in climate. This means that exposure levels that are close to the toxicological reference value (TRV) at present condition may in the future exceed the TRV, and thereby also have implications for the risk management process which often needs to rely on precaution. However, large uncertainties are associated with exposure assessments accounting for possible future climate change.
In paper V, it was concluded that the gender, age and work experience of the employees, as well as the funding source of the risk assessment, have an impact on the reviewing of risk assessments, with gender being the most significant factor. Gender also affected the perception of knowledge; however, this perceived knowledge does not necessarily correspond to actual knowledge. These differences can affect the risk management process and may thus also have implications for the outcome of a contaminated land project.
In the papers presented in this thesis different aspects of uncertainty and variability have been highlighted and demonstrated. This is a continuously ongoing work in progress as the risk analysis process is iterative and conditions change. Exposure factors also change with time and are in continuous need of being updated. Knowledge on how to treat uncertainty and variability in the risk analysis process is essential in order to create transparent and reliable risk assessments that can gain regulatory acceptance.
34
ACKNOWLEDGEMENTS
I thank my supervisor Tomas Öberg and co-supervisor Bo Bergbäck for their guidance, support and belief in me. To my co-authors – Anna Augustsson, Bo Bergbäck, Marianne Lindström, Lill Ljunggren, Pasi Peltola and Tomas Öberg – it has been a pleasure working with you.
During this time I have received invaluable information from many people. I would particularly like to gratefully acknowledge those who kindly gave advice and permission to use primary data from their surveys:
� Otis Evans and Alfred P. Dufour (US EPA) for data on water
ingestion while swimming. � Gunnel Boström and the survey Health on Equal Terms (Swedish
National Institute of Public Health), Elisabeth Strandhagen and the Intergene survey (University of Gothenburg), and Anna Bostedt and Kicki Wickberg and the Epibarn database (Västernorrland County Council) for body weight and height data.
� Cecilia Boldemann (Stockholm County Council and Karolinska institute) for data on time spent outdoors by children.
� Wulf Becker and Riksmaten 1997-98 (Swedish National Food Administration) and Hanna Sepp (Uppsala University) for food consumption data.
� Rolf Pettersson (Central Hospital, Skövde) for data on children’s tap water intake.
I would like to acknowledge the external funding sources. The exposure
factors survey was funded by the Swedish Environmental Protection Agency (Naturvårdsverket) and the Sustainable Remediation (Hållbar Sanering) research program. The risk assessment of Lake Trekanten was funded by the City of Stockholm and the District Administration of Liljeholmen.
For lots of fun and pleasant discussions, I would like to thank my colleagues at the School of Natural Sciences, Linnaeus University. In particular I would like to thank Stina Alriksson, Ullrika Sahlin and Ymke Mulder for comments on the manuscript. My greatest thanks and love go to David, my family, relatives and friends for always being there and for your endless support.
35
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APPENDIX
In this appendix, the inscriptions in RAMAS Risk Calc 4.0 Software (Ferson 2002) are shown for the exposure assessment example shown for paper III. Probability boxes (p-boxes) are presented as they appear in Risk Calc. All figures show cumulative probability from 0 to 1 on the y-axis and the exposure factor unit on the x-axis.
Exposure model
When exposure factors are assumed to be independent, the inscription of equation 4 (paper III) in Risk Calc looks as follows: Intake1_6_indep=((EF|*|6)|/|(BW|*|AT))|*|((CW|*|CR|*|ET)|+|((CS|*|CF)|*|(IR|+|(SA|*|AF|*|ABS)))) The same procedure except that some exposure factors are assumed to be dependent on each other (independency assumptions are removed by removing “|”): Intake1_6_dep=((EF|*|6)|/|(BW|*|AT))*((CW|*|CR|*|ET)|+|((CS|*|CF)|*|(IR+(SA|*|AF*ABS))))
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Exposure factors
In cases where multiple percentiles are available the p-boxes were delimited by minimum and maximum values, and uncertainty intervals around the mean, SD and percentiles. This was the case for body weight (BW), skin surface area (SA) and water intake while swimming (CR). Here, the body weight of 4-year-old children is shown as an example. The uncertainty intervals of mean, SD and multiple percentiles are found in table 1. The inscriptions in Risk Calc can be made as follows and the output as a p-box is shown in figure A:
BW=imp(imp(minmaxpercentile(10,30,95%,[22.6,24.2]),minmaxpercentile(10,30,99%,[24.8,28.2])),imp(imp(imp(posmeanstddev([18,18.4],[2.5,3]),minmaxpercentile(10,30,1%,[12.3,13.8])),imp(minmaxpercentile(10,30,5%,[14.3,14.8]),minmaxpercentile(10,30,10%,[15.0,15.4]))),imp(imp(minmaxpercentile(10,30,25%,[16.2,16.6]),minmaxpercentile(10,30,50%,[17.6,18.0])),imp(minmaxpercentile(10,30,75%,[19.2,19.8]),minmaxpercentile(10,30,90%,[21.0,22.0])))))
0 10 20 30 400
0.5
1
BW
Figure A. P-box. Body weight (kg) of girls aged 4 years.
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Information on other exposure factors was somewhat more limited. Contaminant concentrations in water (CW) and sediment (CS) were described by minimum, mean and SD. PAH (as BaP equivalents) concentration in sediment is shown as an example:
CW=minmeanstddev(6.98E-06, 1.02E-05, 3.46E-06)
0 1e-05 2e-05 3e-05 4e-05 5e-05 6e-050
0.5
1
CW
Figure B. P-box. BaP-equivalent concentration in water (mg/L).
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Minimum, maximum and mean values, without uncertainty intervals, were used for exposure time (ET), exposure frequency (EF) and intake of sediment (IR), while the uncertainty interval of the mean was used for adherence factor (AF): AF=minmaxmean(0.1,2,[0.36,1.17])
0 1 2 30
0.5
1
AF
Figure C. P-box. Sediment-to-skin adherence factor (mg/cm2).
Conversion factor (CF) and period over which exposure is averaged (AT) were entered as point estimates. For absorption factor (ABS), minimum and maximum values were used without uncertainty intervals.