Monitoring of Environmental Chemicals · 2016. 12. 22. · Monitoring of Environmental Chemicals Georg Becher and Aif Bjerseth ABSTRACT The principles, purpose and methods for monitoring

Methods For Assessing the Effects of Mixtures of ChemicalsEdited by V. B. Vouk, G. C. Butler, A. C. Upton, D. V. Parke and S. C. Asher~ 1987 SCOPE

Monitoring of Environmental Chemicals

Georg Becherand Aif Bjerseth

ABSTRACT

The principles, purpose and methods for monitoring environmental chemicalshave been reviewed. In particular, the various monitoring techniques (i.e. processmonitoring, emission monitoring, ambient monitoring, exposure monitoring,and biological monitoring) are discussed. Relevant sampling and analyticaltechniques are summarized and applications are illustrated by discussion ofselected examples for both organic and inorganic pollutants. The use of indexchemicals and indicator organisms is also discussed. Finally, various concepts ofdata interpretation are discussed, including qualitative and quantitative aspects,as well as use of multimedia environmental goals.

1 DEFINITION AND PURPOSE OF MONITORING

Environmental monitoring may be defined as a series of measurements of definedvariables for a specified purpose according to a predetermined schedule in time.Monitoring schemes may differ greatly in their extent in space and time-from asmall area around an emission source, a continuous measurement to globalmonitoring programmes, and a frequency that seeks to define not more thanyear-to-year trends such as the carbon dioxide content of the atmosphere. Anymonitoring system is an expensive exercise and the costs rise sharply whenincreasing numbers of samples and increasing numbers of variables are beingmonitored. Thus, clear and concise problem definition and careful planning are aprerequisite for designing a monitoring scheme. Models describing the environ-mental system can provide useful guidance in designing a monitoring scheme andinterpreting the data. There are various reasons for establishing monitoringsystems; the main goals are: (a) to provide information about the substancesbeing emitted to the environment, their quantities and sources; (b) to determinethe distribution and transformation of chemicals in the environment; (c) todetermine changes in environmental conditions with time; (d) to provide a soundbasis for the development of standards, regulations, and other legal requirementsrelating to the protection of human health and the environment; (e) to determinehow well regulatory measures are being met; (1)to provide information about the

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226 Methods for Assessing the Effects of Mixtures of Chemicals

relationship between exposure to chemicals and biological effects; and (g) to testand refine models on transport and transformation of chemicals in theenvironment and on exposure estimation.

2 DIFFERENT KINDS OF MONITORING

A chemical pollutant may follow various routes from a source to the target, asindicated in Figure 1. Both point sources and non-point sources will giveemission of pollutants which again are transported and distributed in theenvironment. During this transport, transformation of the chemicals may takeplace. This leads to the ambient level of pollutants and ultimately to exposure ofboth human and other target organisms.

Measuring chemicals in the environment can be carried out at several pointsalong the pathway from the source to the target (Holdgate, 1979).These include:(a) process monitoring within an industrial process; (b) emission monitoring atthe point of emission to environment; (c) environmental monitoring at a networkof points in the environment; (d) exposure monitoring at the surface of the target;and (e) biological monitoring within a target.

Process monitoring may be advantageous in controlling discharges oremissions from a given plant. Control technologies might be applied beforehazardous chemicals are released to the environment. Most modern plants havesophisticated feedback systems to a central control unit which reacts to anymalfunction of any component including pollution control devices such aselectrostatic precipitators or bag-house filters.

The main objective of emission monitoring is to determine the output ofecologically active compounds related to specificprocesses or process parameters(Dorsey et aI., 1979).The source from which a pollutant enters the environmentmay be related to industry, energy conversions, agriculture, or domestic andmunicipal activities. The scale of input to the environment depends on severalfactors such as kind of process, size, and number of sources.

Because several different physical and chemical transformations of theemissions may take place in the environment before they reach the target, theinformation value of emission monitoring for the prediction of environmentalimpacts may be questioned. However, from the practical point of view emissionmonitoring offers some advantages. Major emission sources may be identifiedrapidly and may be ranked according to their individual hazards. Furthermore,monitoring of individual emissions is essential if standards and controls havebeen imposed on the discharges from a source.

Environmental monitoring of pollutants at a network of sites in theenvironment is more difficult to design. The environment receives emissions froma large number of sources and not all the sources are recorded. The various flowsmix and dilute the emissions and in some cases the pollutants interact chemicallyto produce new pollutants. Some airborne pollutants settle on soil, are trapped

CHARACTERIZATION

PROCESS

CONSEQUENCE

Figure 1 Schematic pathways of pollutants. POM, polycyclic organic matter; PCB, polychlorinated biphenyls

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r I Distribution r

AMBIENTSOURCES EMISSIONS CONCENTRATIONS IMPACT

Fuel combustion t::{> Inorganic pollutantst::C> In air water soil Human health

Industrial (S02,NOx,heavy metals) Primary pollutants EcologicalDomestic, institutional Organic pollutants Transformation AgriculturalAgricultural (POM, PCB, pesticides) products Economic

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by the foliage of trees, or are washed down in rain. Aqueous pollutants may befiltered by water plants or bound chemically or physically to sediments.

To obtain a meaningful picture of what is happening demands carefulsampling. The system should be designed to meet several goals: (a) it shouldindicate where and when target exposure is likely to be above the desired levels,and (b) it should be related to emission monitoring through reliable models inorder to provide a measure of adequacy of emission controls.

Exposure monitoring at the surface of the target is an unambiguous point onthe pathway of a chemical which can reveal whether emission controls areproviding satisfactory protection. An example is the personal monitoring of aworker's exposure to hazardous chemicals in the workplace atmosphere. Withrespect to non-human biota, exposure monitoring is scarcely used.

In many cases only a part ofthe pollutant to which a target is exposed is actuallyabsorbed and very often the relationship between exposure and uptake is notknown. Thus, biological monitoring of a pollutant may be needed to measure theeffectivedose. This has been done, for example, for organochlorine pesticides, bymeasuring residue levels in animal and human tissues (Bj0rseth et al., 1977;Phillips, 1978).

With respect to non-human biota, emission monitoring, environmentalmonitoring, and biological monitoring are by far the most used measuringtechniques and will therefore be discussed in more detail.

It should be noted that monitoring (and characterization) of environmentalpollutants puts strong demands on the analytical techniques to be applied. Mostsamples encountered in environmental chemistry contain complex mixtures ofpollutants originating from anthropogenic sources which in nature are ratherunspecific. For instance, polycyclic aromatic hydrocarbons (PAHs) emitted fromall combustion processes and high-temperature reactions involving carbo-naceous materials frequently contain more than 100different compounds. Otherindustrial chemicals, such as polychlorinated biphenyls (PCBs), theoreticallycontain more than 200 compounds. For chlorinated paraffins, the number ofindividual compounds may be even higher. It is therefore apparent that theanalytical techniques used for monitoring must meet strong requirements withrespect to separation efficiency, sensitivity (low detection limits), precision andaccuracy. Unless such requirements are met, the possibility of drawing conclu-sions from the analytical (or monitoring) data is limited.

3 SAMPLING TECHNIQUES

Sampling is defined as the collection of small components from the respective(sub)compartments of the environment. The collection should be carried out insuch a manner that the sample represents, within measurable limits of error, theproportion of the quantity of the whole. Sampling is a critical step in themeasurement of environmental pollution (Grob and Kaiser, 1982; Josefsson,

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Monitoring of Environmental Chemicals 229

1982). In the absence of a reproducible and quantitative sampling procedure,sophisticated and sensitive analytical methods are of no value.

3.1 Emission Sampling

The measurement of emission components from different sources today hasbecome a routine technique in many laboratories around the world. However,different sampling techniques and work-up procedures are usually employed indifferent laboratories, limiting the possibility for a reliable, reproducible andcomparable emission data base. Therefore, several regulatory agencies havemade proposals or recommendations in order to harmonize methods forsampling and analysis. For instance, the United States EnvironmentalProtection Agency (USEP A) has proposed a standardized sampling and analysisprogramme that addresses, to the maximum extent possible, the sampling andidentification of all potential air, water, and terrestrial pollution problems(Lentzen et al., 1978).The approach is based on a multimedia sampling strategyorganized around five general types of sampling rather than around theanalytical procedures required. These five sample types are: (a) gases andvapours; (b) liquids/slurries; (c) solids; (d) particulates or aerosols; and (e)fugitive emissions.

Gas, liquid/slurry and solid samples are usually collected by grab samplingtechniques. Care has to be taken to insure that the sample is representative andmay therefore be composed of a time- or space-integrated series of smallersamples.

A special 'source assessment sampling system' (SASS) (Figure 2) has beendeveloped for the collection of particulate samples and volatile matter fromstationary sources (Blake, 1976). The SASS train includes cyclones separatingparticulate matter into three size fractions, a filter, a sorbent cartridge forcollecting volatile organic material, an aqueous condensate collector, and a seriesof impingers for volatile inorganic compounds.

Fugitive emissions are those air and water pollutants generated by a givenprocess that are transmitted into the ambient atmosphere or receiving waterbodies without first passing through some stack, duct, pipe or channel designedto direct or control their flow. They constitute an important fraction of the totalpollution problem. Airborne fugitive emissions are sampled using a high-volumesampler consisting of a cyclone separator and/or a glass fibre filter for particulatematter and a sorbent resin for volatile organic species (Lentzen et al., 1978).

3.2 Ambient Sampling

To obtain a representative sample of pollutants in the ambient environmentrequires considerable care in planning and implementation. This includessampling methods, sampling strategy, choice of sampling sites, etc. (Grab and


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Figure 2 Source assessment sampling train, schematic

Kaiser, 1982;Josefsson, 1982).The future use of the samples, i.e. for chemical,biological or other analyses, must also be taken into consideration.

In the case of slow-moving air or water a singlesample is unlikely to represent acorrect picture of the pollution level. Therefore, such samples should be taken byintegrated techniques which incorporate a preconcentration step. In this waylarge volumes are sampled.

An air sampler may consist of a cyclone separating ambient particles intoseveral size fractions and/or a glass fibre or membrane filter and a sorbentmodule to sample gaseous components. Commonly used adsorbents includeactivated alumina, silica gel, molecular sieves, charcoal, organic resins such asTenax GC and Amberlite XAD-2, and polyurethane foam. The use of adsorbentsfor vapour-phase collection may be of considerable importance. Recent studies(Cautreels and Van Cauwenberghe, 1978; Thrane and Mikalsen, 1981) ofsampling of PAHs have shown that the losses oflow molecular weight PAHs areup to 95 %for three-ring PAHs such as phenanthrene/anthracene when onlyfilters are used. At ambient summer temperatures even five-ringcompounds suchas benzo[a]pyrene may show considerable losses (Pupp et al., 1974). Table 1shows the particulate/vapour ratio for the main PAH components in ambient airsamples (Thrane and Mikalsen, 1981). Since the gases of interest have a wide


Table I Distribution (%) of selected PAHs on filter andpolyurethane foam plug in ambient air sample collected in Oslo,Norway

range of vapour pressures and breakthrough volumes, no single sorbent cansimultaneously collect all of them. Gaseous pollutants may also be concentratedby freezing out (Stenberg et al., 1983) at low temperatures (cryogenic tech-niques). Deep-freezing combined with adsorption may improve the trappingefficiency.

Adsorption sampling techniques have also been widely used for ambient watersamples. In the direct mode the water to be sampled is passed through a columnof porous organic polymers or similar sorbent where the components of interestare removed from the water stream (Dressler, 1979;Jolley, 1981). In the indirectmode (Figure 3), the water sample is stripped of its volatile components bybubbling an inert gas through the water sample (Beller and Lichtenberg, 1974).The gas stream is then passed through a column containing a suitable sorbent.The subsequent removal of sorbates is achieved by thermal desorption or bysolvent extraction.

3.3 Biological Sampling

Plants and animals known to accumulate residues of environmental chemicalsare particularly suitable for monitoring these substances in the environment andare concerned with such compounds as hydrocarbons, polychlorinated bi-phenyls (PCBs), radionuclides andheavymetals.Thebioticspeciesnormallyused

Compound Particles Gas phase

Naphthalene 0 100Biphenyl 0 100Fluorene 0 100Phenanthrene 4 96Anthracene 5 952-Methylanthracene 20 80Fluoranthene 48 52Pyrene 50 50Benzo[a]fluorene 65 35Benz[a]anthracene 97 3Chrysenejtriphenylene 34 6Benzo[e]pyrene 90 10Benzo[a]pyrene 80 20Perylene 100 0Indeno[ I ,2,3-cd]pyrene 100 0Benzo[ghi]perylene 100 0Coronen 100 0

From Thrane and Mikalsen (1981).

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Flow Meter

Sample

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Figure 3 Purge and trap device used to purge and concentratevolatile organic compounds from liquid samples

for these programmes are fish, mussels, oysters, and algae (Phillips, 1977, 1978).For air monitoring a common technique is to analyse mosses and lichens(Carlberg et aI., 1983; Thomas and Herrmann, 1980).

Major advantages of biotic sampling for monitoring pollutants are: (a) theaccumulation of chemicals present at low and often undetectable concentrationsin the environment; and (b) a time integration of the biologically availablequantity of the chemicals present.

However, biological variables such as lipid content, age, and sexual condition,and environmental conditions such as temperature, season, and salinity of watermay affect the reproducibility and accuracy of the determination of pollutionconditions in a given location. Furthermore, species which move over con-siderable distances (such as pelagic species) may 110tprovide relevant infor-mation about the pollutants in the sampling area.

4 ANALYSIS METHODOLOGY

4.1 Direct Methods

There are two approaches for continuously measuring environmental pollutants.In the first approach a sample is continuously extracted from a source or theenvironment, conditioned, if necessary, and transported to an appropriatedetector. Examples are the continuous determination of emission and ambientlevels of gaseous pollutants such as sulphur dioxide, ozone and nitrogen oxides(Leh and Lak, 1974)and the use of ion-selective electrodes in flow-through cellsfor continuous measurement of various ions in waste water effluents (Cammann,1977). More recently, methods for in.situ monitoring of pollutants have been


developed. These measurements avoid any extraction of the sample by utilizingthe effluent stream or the ambient compartment itself as an analysis chamber.Commercial in situ monitors have been developed for in-stack measurements ofcertain gaseous pollutants such as sulphur dioxide and nitrogen oxides(Homolya, 1974). Tunable diode lasers have been used for the detection ofambient air pollutants such as ethylene and formaldehyde (Hinkley and Kelley,1971). Recently, Pitts (1983) applied a long-path differential optical absorptiontechnique to the ambient measurement of gaseous nitrous and nitric acid at thesub-ppb level. Other pollutants such as formaldehyde, formic acid, nitrogendioxide, sulphur dioxide and ozone can also be measured at the same ambientlevel (Platt et aI., 1980).

4.2 Sum Parameters

Group parameters such as total chromatographable organics, total organiccarbon, total organic halogen, and others, are often used to screen emissionsamples for unknown pollution potential, monitor changes in environmentalpollution or determine the efficacy of pollution control technologies.

Dissolved organic carbon is one of the key parameters in water analysis andmay give good information for comparison (Leithe, 1973).Total organic halogenhas been used for the quantification of non-volatile organic halogen compoundsin drinking water, waste water and biological samples (Bj0rseth et aI., 1981;Glaze and Peyton, 1978;Glaze et aI., 1977).Total chromatographable organics,as determined by gas chromatography (GC) with flame ionization detection, hasbeen proposed for environmental source assessment as a semiquantitativeestimate of organiccompounds in emissionsamples(Lentzenet al., 1978).

Perchlorination of the complex mixture of PCBs to form decachlorobiphenylhas been proposed for quantitating the total amount of PCBs in environmentalsamples (Hutzinger et aI., 1972; Stratton et aI., 1979).

4.3 Index Chemicals

The determination of index chemicals may often be sufficient to characterize asource, measure changes in pollution levels or indicate the presence of aparticular class of pollutants. Usually specific, low-cost analysis techniques areemployed in the measurement of index chemicals. Sulphur dioxide is often used asa key component for air pollution in larger environmental pollution monitoringprogrammes (OECD, 1977).

Benzo[a]pyrene has been used as an indicator for the presence of the largegroup ofP AHs and the most extensive information is available on the occurrenceof this potential human carcinogen (Perera, 1981). However, it has beendoubted that a valid carcinogenic risk estimate may be obtained from monitoringthis compound alone (Holmbergand Ahlborg, 1983).

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Further examples of index chemicals are hepta- and octachlorostyrenes. Thereis no commercial synthesis of these compounds. Nevertheless, they have beenobserved in environmental and biological samples from different countries(Kuehl et aJ., 1976;Ofstad et ai., 1978).They may be formed as unexpected by-products of high-temperature reactions involving carbon and chlorine of whichthe production of magnesium is an example (Becher et ai., 1981; Lunde andBj0rseth, 1977).

4.4 Detailed Characterization

4.4.1 Prefractionation Techniques

Various separation and concentration techniques are employed to isolatecompounds and compound classes from complex environmental samples.Extraction, especially solvent extraction, is widely used. Examples are theextraction oflipid-soluble chlorinated hydrocarbons from fish with a mixture ofhydrocarbon solvent and isopropanol (Ofstad et ai., 1978, 1981)or the selectiveextraction of PAHs from cyclohexane solutions by dimethylformamide-water9: I (Bj0rseth, 1977; Grimmer and Bohnke, 1972). A further example is thespecific extraction of trace metals from aqueous solutions with organic solventsusing chelating agents (Leyden and Wegscheider, 1981).Gas-liquid extraction isincreasingly applied for volatile pollutants in water samples by using the purge-and-trap technique (Dreisch and Munson, 1983).

Chromatography has proved to be a very useful tool for the isolation ofcompound classes. Liquid chromatography is by far the most used technique andis applied in several modes (Table 2). Recently, normal-phase high-performanceliquid chromatography (HPLC) has been introduced to fractionate organicsolvent extracts of ambient air particles and of various emissions fromcombustion processes (Ramdahl and Becher, 1982; Ramdahl et aJ., 1982;Schuetzle et ai., 1981).

Table 2 Separation modes in liquid chromatography

Mode Packing Separation mechanism

Liquid -liquid Liquid coated onsolid supportActive solid(silica, alumina, etc.)Surface-reacted(chemically bonded organic)Ion-exchange resinOrganic gels or bondedphase

Partition

Liquid -solid Adsorption

Bonded phase Partition/adsorption

Ion exchangeSize exclusion

Ion exchangeExclusion of largemolecules from pores


4.4.2 Predetermined Analysis

Detailed predetermined chemical analysis is widely used in the analysis ofenvironmental pollutants. It is aimed at the determination of specificcompoundsusually contained in a priority pollutant list. This list of compounds affects theselection of method because sample processing and measurement techniquesmay be optimized for the particular pollutants. Detailed chemical and instru-mental procedures may be designed to isolate these pollutants from the samplematrix and known interferences, concentrate them and measure their concentra-tions with general or selective detectors.

Nevertheless, the final fraction obtained after clean-up and preseparationprocedures may still contain a large number of isomers or compounds of similarchemical nature. For example, several hundred different PAHs have beenidentified in airborne particles, workplace atmospheres or cigarette smokecondensate (Bj0rseth and Eklund, 1979; Lee et aI., 1976; Snook et aI., 1976).Similarly PCBs in environmental samples consist of up to 100 closely relatedcompounds with varying numbers of chlorine atoms (Ballschmiter and Zell,1980; Jensen and Sundstrom, 1974).

There are two important facts concerning quantitative determination of theindividual components in environmental samples. First, the biological activity ofa particular compound within a class is highly dependent upon compoundstructure. Second, if an extensive characterization of compound classes is basedon analyses of individual components rather than of unresolved mixtures, we canimprove our ability to describe the sources and fates of these chemicals in theenvironment.

The methods used for the quantitative determination of individual compoundsin environmental samples usually include some type of chromatographicseparation and a spectroscopic or other means of detection. The methods whichseem to have the highest potential in terms of separation efficiencyand sensitivityfor a wide range of compounds are HPLC and Gc.

Capillary GC has proved to be extremely useful in characterizing multicom-ponent mixtures (Becher et aI., 1981; Grob and Grob, 1969; Jennings, 1980).Capillary GC exhibits excellent reproducibility, high sensitivity and goodresolution power and is routinely applied to the analyses of mixtures of volatilesubstances or substances which can be converted to volatile derivatives (Groband Kaiser, 1982). In predetermined analysis of environmental samples identifi-cation of a GC peak is usually made on the basis of relative retention times (Heeget al., 1979;Vassilaros et aI., 1982).Additional information for identification aswell as increased sensitivity may be obtained by the use of selective detectors(Ettre, 1978).Table 3summarizes some of the more commonly used selectiveGCdetectors.

HPLC is especially useful for the separation of non-volatile or thermallyunstablecompounds.Afurtheradvantageisthe highflexibilityofthe system,e.g.

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Table 3 Major GC selectivedetectors

DetectorCommonsymbol

Minimumdetection limit

(g)

Electron-capture detectorFlame photometric detectorThermionic detectorElectrolytic conductivity detector (Hall)Mass spectrometric detector

ECDFPDNPDHECDMS

10-12-10-1310-1°-10-1110-12-10-1310-11-10-1310-11-10-12

the selectivitycan be altered by varying solute-mobile phase interactions. Recentadvances in column and instrument technology have resulted in high efficiencyand sensitivity. Separations may be based on adsorption, partition, ion exchangeor size exclusion. Examples are the analysis of inorganic ions by ion-exchangechromatography (Sawicki et aI., 1978) or the analysis of polar pesticides bynormal- and reversed-phase HPLC (Lawrence and Turton, 1978). Spectroscopicdetectors, such as ultraviolet, infrared and fluorescence detectors, otTer highselectivity and sensitivity and may be used for peak identification by scanningover the spectral range.

4.4.3 Unconditional Analysis

The unconditional approach to the analysis of compounds in environmentalsamples is not guided by a predetermined list of compounds to be measured. Theidea of this approach is rather to identify the broad spectrum of whatever ispresent in a sample as major or minor components. Sample preparation isdesigned to be as simple as possible to preclude losses of significant componentsand to minimize the possibility of sample contamination. The idea is to divide thesample into classesof compounds and to apply general-purpose chromatographicmethods for the separation of individual compounds in each group (Kveseth,1981).

For the unconditional analysis approach a spectroscopic detector is preferred.Spectroscopic detectors are defined as devices that continuously measure spectraof energy absorptions, ion abundances, etc., of the various components as theyelute from a chromatographic system, e.g. mass spectrometric, ultraviolet andinfrared detectors. The spectra are of sufficient quality to permit identificationwithout prior knowledge of which compounds are present.

Spark-source mass spectroscopy (MS) and inductively coupled plasma-atomic emission spectroscopy have been used for the general survey ofenvironmental samples for trace inorganic toxic substances (Aberchrombie andCruz, 1979; Briden and Lewis, 1981).


Computerized capillary GCfMS has become the most powerful tool in thedetection of organic pollutants in all media (Budde and Eichelberger, 1979).Well-known examples include analyses of organic compounds in drinking water (Lin etal., 1981), industrial waste water (Bj0rseth et al., 1981; Hites et al., 1979) andairborne particulate matter (Karasek et al., 1978).

On-line LCfMS is a promising technique for the identification of non-volatileor thermally unstable components in environmental samples (McFadden, 1980).However, instrumental difficulties are still severe and comparatively few researchpapers on LCfMS have appeared (Arpino, 1982).

4.4.4 Simultaneous Use of Sum Parameters and High-resolution Techniques

Combining data obtained from detailed analyses with the determination of groupparameters such as total organic halogen and total organic carbon have beenshown to give valuable information about the fraction of individual identifiedpollutants in a sample.

It is now generally accepted that only approximately 10- 20 %of the totalorganic matter present in both raw and drinking water is amenable to analysis byGCfMS (Crathorne and Watts, 1982;Gloor et al., 1981).Therefore, great efforthas been concentrated on the development of techniques which provideinformation on the bulk of non-volatile organic matter in water (Glaze et al.,1980; Watts et al., 1982).

The combined application of total organic halogen determination andcapillary GC with electron-capture detection to environmental samples has beenreported in several instances, e.g. human adipose tissue (Bj0rseth et al., 1977),marine and freshwater organisms (Bj0rseth et al., 1981; Ofstad et aI., 1978),freshwater and seawater (Lunde et al., 1975),and industrial effluents (Bj0rseth etal., 1981;Glaze and Peyton, 1978).Table 4 indicates that in some cases a majorpercentage of chlorinated hydrocarbons present in biological material isidentified by GCfMS. On the other hand, in water samples which result frombleaching and disinfection processes, using chlorine, generally only a small part

Table 4 Comparison of results from determination of organic chlorinecompounds by sum parameter and detailed analysis

SamplePercentage of extractable organic

chlorine accounted for by GC

Human adipose tissueFish (fillet or whole)Sulphite bleaching effluent

85 (SD = 15)a68 (SD = 21)b18c

a Bjerseth et al. (1977).

b Ofstad et at. (1978).

c Bjerseth et al. (1981).


of the chlorinated organic compounds present is amenable to GCjMS analysis(Bj0rseth et al., 1984).

4.5 Indicator Organisms

The fact that some organisms may be indicators of their physical and chemicalenvironment has long been used for monitoring environmental pollution. In apolluted environment some organisms will die, some will thrive and some willapparently tolerate a certain degree of pollution. This will find expression in thediversity of species present or in stimulation or inhibition of physiologicalfunctions.

In the context of this paper we wish to restrict the term indicator organisms tothose which tolerate a given ecological stress and accumulate pollutants from air,water or food, i.e. the organism acts as an indicator by means of its pollutantcontent. Accumulation may occur through uptake in the indicator organism (e.g.fish,mussels), or by mere adsorption on the surface of the indicator organism (e.g.vegetables). The major advantages of the use of biological indicators are theirdirect measurement of the biological availability of pollutants and their timeintegration of the ambient pollution conditions at the site of collection. The valueofthe selected organism will also strongly depend on its position in the food chainand the bioaccumulation and biomagnification factors.

4.5.1 Aquatic Organisms

Aquatic organisms have been widely used to monitor aquatic pollutants such astrace metals (Phillips, 1977), chlorinated hydrocarbons (Phillips, 1978), andPAHs (Dunn, 1983; Neff, 1979).

Both freshwater and marine fish have been extensively used for monitoringchlorinated hydrocarbons. Examples include discharges from the pulp and paperindustry (Bj0rseth et al., 1981) and electrochemical industries (Ofstad et al.,1978). Due to their high lipophilicity and their resistence to degradation, thesecompounds tend to accumulate in the lipid phase offish. Bioaccumulation factorsare usually several orders of magnitude for compounds such as hexachloro-benzene, DDT or PCBs (Phillips, 1978). These compounds can thus bemonitored even though their concentrations in the environment are too low to bedetected by traditional means. One must, however, be aware of the fact that therelative proportions of compounds in mixtures that are concentrated in biotamay not be the same as they occur in the media.

Molluscs such as mussels and oysters are well known for their rapid uptake ofmetals and hydrocarbons (Phillips, 1977). Very high values of PAHs weredetected in tissue from mussels in a fjord contaminated with waste effluents froma ferro alloy smelter (Bj0rseth et al., 1979) (Figure 4). A steep gradient of totalPAH concentration was observed away from the source. Comparison with


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Figure4 A real variation of PARs in horsemussel(Modiolusmodiolus)in Saudafjord,Norway. From Bj~rseth et al. (1979). Reproduced by permission of Elsevier SciencePublishers

concentration in the sediments from the same area indicated substantialbioaccumulation.

'Active' monitoring by transplanting mussels from unpolluted areas to theregions to be studied has been proposed for trace elements such as mercury andzinc (Hueck, 1976).However, transplantation may result in a significant changeof accumulation rate, as demonstrated for PAHs (Kveseth et al., 1982).Changesin biological activity under the influence of the sudden pollution load may affectthe accumulation rate of pollutants.

4.5.2 Terrestrial Plants

The use of terrestrial plants as indicator organisms for air pollutants has beenstudied by several authors (Buckley, 1982;Carlberg et al., 1983; Kveseth et al.,1981; Thomas and Herrmann, 1980).

Plant foliage has been shown to accumulate the vapour of PCBs and may beused for airborne PCB monitoring (Buckley, 1982). Moss and lichen sampleshave been used to monitor the atmospheric deposition of both organic andinorganic trace substances (Carlberg et al., 1983;Thomas and Herrmann, 1980).The use of moss and lichen as bioindicators is based on their large surface areaand the fact that pollutants enter the plant to a large extent through the air.

PAH levels in leafy vegetables such as lettuce and kale have been studied in

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detail in a Nordic research programme (Kveseth et al., 1981). The observedconcentrations of individual PAHs correlated well with local PAH sources.

5 INTERPRETATION

5.1 Qualitative Aspects: Source Identification

The identification and relative distribution of chemical pollutants in environ-mental samples may provide a basis for the characterization of the sources.

The presence of specific polycyclic organic matter has been used as anindication of the emitting source. The appearance of benzo[b]naphtho[2,1-d]thiophene seems to be typical for coal combustion while a relatively largeconcentration of cyclopenta[cdJpyrene is characteristic for automobile traffic(Grimmer, 1980).Recently, Ramdahl et ai. (1984)demonstrated that l-methyl-7-isopropylphenanthrene (retene) and methyldehydroabietate may qualitatively beused as tracers for wood combustion.

A more sophisticated method to distinguish between PAH sources is the use ofthe 'parent PAH profile', i.e. the distribution pattern of a given number of keyPAH compounds in the sample. The method has been applied to a number ofemission samples from high-temperature industrial processes (Bj0rseth, 1980).PAH profiles have also been used by Grimmer (1983) in studies of PAHs inambient air.

A more sophisticated method to distinguish between profiles has beendeveloped by Gether and Seip (1979). It comprises an interactive graphictechnique and a 'one-way splitting algorithm' and takes full advantage of all dataaccumulated in a multicomponent analysis. The method has been successfullyapplied to various data sets connected to air pollution (Gether and Seip, 1979)and to the PAH content in kale related to possible sources (Kveseth et ai., 1981).

5.2 Quantitative Aspects: Emission Factors

A given process with a fixed set of process parameters may produce a specificandinvariable amount of pollutants. This amount can be correlated with the processparameters whereby an emission factor for the process can be established.

Emission factors have been determined for a great number of air and waterpollutants based on emission measurements, material balance studies, etc.(Dutch Ministry of Health and Environmental Protection, 1980;USEPA, 1977).

Emission factors of anthropogenic sources for PAHs have been discussed indetail by Ramdahl et ai. (1983). In this study residential combustion of wood wasfound to be a significant source for PAHs in Norway besides aluminium smeltersand gasoline automobiles. Although many emission factors are based on arelatively small number of measurements, they may give a good estimate of theseverity of a source and form a basis for control technology programmes.

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5.3 Multimedia EnvironmentalGoals

In order to provide a comprehensive environmental hazard assessment theUSEPA has developed a methodology to facilitate quantitative evaluation andcomparison of streams and processes with respect to their potential environ-mental impacts (Kingsbury et aI., 1980). This methodology prescribes asystematic approach to the interpretation of data obtained in environmentalassessment projects. Multimedia environmental goals (MEGs) provide themechanism by which levels of pollutants or their transformation products (inambient air, water or land, or in discharges conveyed to ambient media) arerelated to their environmental effects.

The MEG system has been used for environmental assessment of dischargestreams to air and water from various industrial sources in a local area (Gangwalet aI., 1981;Kveseth, 1983).Kveseth (1983)has evaluated various techniques forheat production through stack gas emissions using the MEG system. Thetechniques studied include burning of whole wood, wood chips and peat, wasteincineration and oil combustion. The calculations show that burning of wholewood is least desirable in larger-scale energy production, whereas burning of peatand wood chips in larger plants represents the most preferable technique. Thehazard from the smoke gas emissions from burning whole wood is mainlyassociated with PAH emission, while in the other techniques the hazard isassociated with more complex emissions of various trace metals and inorganicvolatiles such as nitrogen oxides, sulphur dioxide and hydrogen chloride.

6 ENVIRONMENTAL MONITORING-FUTURE APPROACHES

In this paper we have described methods for survey, surveillance, and monitoringof environmental chemicals as a part of the contribution of analytical chemistryto ecotoxicology. It should, however, be stressed that monitoring data can rarelybe generalized unless one knows the significant interrelationships and theinteractions between the parts of an ecological system, i.e. relevant pathways ofpollutants, exchange processes, transport, and biological and chemical trans-formations. Similarly, it is usually very difficult to assess organisms underlaboratory conditions. In order to fully utilize the chemical data available, thereis a need to develop and apply general concepts on the environmental behaviourand fate of pollutants and to use these concepts as an aid to procuring relevantanalytical results. By evaluating the strength of natural and anthropogenicemission sources and by identifying the relevant pathways, interactions and unitprocesses that govern the behaviour and fate of chemicals in a given naturalsystem, we can improve our ability to understand and predict the future fluxes,distribution and effect of pollutants on ecological systems and on human health.

In a recent paper, Stumm et al. (1983) presented a plea for more concepts andlessmonitoringand testing.Theywereconcerned that the present preference for,


and over-emphasis on, monitoring programmes over flexible basic and ex-ploratory research may hinder rather than aid our understanding of nature andof its changing processes. The systematic monitoring of a compartment of theenvironment is an extremely involved, expensive, and time-consuming enter-prise. Because of a lack of understanding for the mutual interactions betweenpollutants and the environment, much of the effort in the past has by necessitybeen devoted to measuring which pollutants are present rather than tocharacterizing the dynamic processes that determine the fate and residence time ofthe pollutants. By using different models, concepts for assessing and predictingthe environmental behaviour of pollutants could be established (Figure 5). Acompound-specific data set aids in establishing the pollution potential ofindividual substances and permits one to forecast the manner in which thecompounds are distributed in the environment, how fast they may be degradedchemically or biologically, and thus to predict their fate and approximateresidence time. Such predictive assessment models may be complemented bylaboratory studies in which individual processes can be investigated undercontrolled conditions and by field studies which are necessary in order todetermine system parameters and to measure the spatial and temporal distri-bution of pollutants.

Information orstructure anddynamics ofecosystems

PollutantsCompound-specific porameters(vapour pressuresolubility etc.)

(Field studies)

natural and loranthropogenic input( sources, quantities+ ecological information)

markercompounds

field data reaction constantsand parameters

11

1_- 1

111 J

uPrediction of theenvironmental behaviourof a pollutant in a givennatura! system

Figure 5 General approach for the prediction of environmental behaviour ofpollutants. From Stumm et al. (1983). Reproduced by permission of VCHVerlagsgesellschaft


Analytical chemistry may contribute significantly to the solution of ecotoxic-ological problems. Relevant analytical data combined with chemodynamicconcepts permit, on the basis of physical/chemical generalizations and with thehelp of compound-specific data, the estimation of the fate, distribution, potentialfor bioaccumulation in the food chain, and approximate residence time ofpollutants in the environment, and therefore prediction of the relative riskassociated with different pollutants.

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