EPA-600/1-78-014 February 1978 Environmental Health Effects Research Series SCREENING METHODS FOR TOXIC SUBSTANCES Health Effects Research Laboratory Office of Research and Development U.S. Environmental Protection Agency Research Triangle Park, North Carolina 27711 ------- RESEARCH REPORTING SERIES Research reports of the Office of Research and Development, U.S. Environmental Protection Agency, have been grouped into nine series. These nine broad cate- gories were established to facilitate further development and application of en- vironmental technology. Elimination of traditional grouping was consciously planned to foster technology transfer and a maximum interface in related fields. The nine series are: 1. Environmental Health Effects Research 2. Environmental Protection Technology 3. Ecological Research 4. Environmental Monitoring 5. Socioeconomic Environmental Studies 6. Scientific and Technical Assessment Reports (STAR) 7. Interagency Energy-Environment Research and Development 8. "Special" Reports 9. Miscellaneous Reports This report has been assigned to the ENVIRONMENTAL HEALTH EFFECTS RE- SEARCH series. This series describes projects and studies relating to the toler- ances of man for unhealthful substances or conditions. This work is generally assessed from a medical viewpoint, including physiological or psychological studies. In addition to toxicology and other medical specialities, study areas in- clude biomedical instrumentation and health research techniques utilizing ani- mals — but always with intended application to human health measures. This document is available to the public through the National Technical Informa- tion Service, Springfield, Virginia 22161. ------- EPA-600/1-78-014 February 1978 SCREENING METHODS FOR TOXIC SUBSTANCES by Harish C. Sikka Syracuse Research Corporation Syracuse, New York 13210 Contract No. 68021786 Project Officer Larry L. Hall Environmental Toxicology Division Health Effects Research Laboratory Research Triangle Park, N.C. 27711 U.S. ENVIRONMENTAL PROTECTION AGENCY OFFICE OF RESEARCH AND DEVELOPMENT HEALTH EFFECTS RESEARCH LABORATORY RESEARCH TRIANGLE PARK, N.C. 27711 ------- DISCLAIMER This report has been reviewed by the Health Effects Research Laboratory, U.S. Environmental Protection Agency, and approved for publication. Approval does not signify that the contents necessarily reflect the views and policies of the U.S. Environmental Protection Agency, nor does mention of trade names or commercial products consitute endorsement or recommendation for use. ii ------- FOREWORD The many benefits of our modern, developing, industrial society are accompanied by certain hazards. Careful assessment of the relative risk of existing and new man-made environmental hazards is necessary for the estab- lishment of sound regulatory policy. These regulations serve to enhance the quality of our environment in order to promote the public health and welfare and the productive capacity of our Nation's population. The Health Effects Research Laboratory, Research Triangle Park, conducts a coordinated environmental health research program in toxicology, epidemiology, and clinical studies using human volunteer subjects. These studies address problems in air pollution, non-ionizing radiation, environ- mental carcinogenesis and the toxicology of pesticides as well as other chemical pollutants. The Laboratory develops and revises air quality criteria documents on pollutants for which national ambient air quality standards exist or are proposed, provides the data for registration of new pesticides or proposed suspension of those already in use, conducts research on hazardous and toxic materials, and is preparing the health basis for non-ionizing radiation standards. Direct support to the regulatory function of the Agency is provided in the form of expert testimony and preparation of affidavits as well as expert advice to the Administrator to assure the adequacy of health care and surveillance of persons having suffered imminent and substantial endangerment of their health. The objective of this project was to explore the feasibility of using fluorescent probes as a technique for detecting effects produced by the action of neurotoxic chemicals. This approach may ultimately provide a more sensitive test for adverse biological effects needed in the hazard evaluation of agricultural and other chemicals. John H. Knelson, M.D. Director, Health Effects Research Laboratory iii ------- ABSTRACT The present report deals with the application of fluorescent probe technique to the detection of conformational changes in rat brain synaptosomes under the influence of certain neurotoxic chemicals, chlorophenothane (DDT) and diphenylhydantoin, which are expected to produce functional changes in nerve membranes. Pretreatment of the rats with (1) a single dose of DDT capable of producing neurological symptoms and (ii) repeated sub-lethal doses of DDT did not alter the fluorescence characteristics of the hydro- phobic probe 8-anilino-l-naphthalene sulfonic acid (ANS) bound to the synaptosomes. DDT treatment also showed no effect on native protein fluorescence of synaptosomes. Exposure of synaptosomes to diphenylhydantoin in vitro did not induce conformational changes as measured by ANS and intrinsic fluorescence. iv ------- CONTENTS Disclaimer ii Foreword iii Abstract iv I ' '; 1. INTRODUCTION . . . 1 General 1 Objectives 2 2. CONCLUSIONS 3 3. MATERIALS AND METHODS A 4. EXPERIMENTAL PROCEDURES 7 5. RESULTS 9 References 16 ------- SECTION 1 INTRODUCTION GENERAL A large number of industrial and agricultural chemicals including pesticides, detergents, solvents, plastics, chemical Intermediates, and plasticizers may be introduced into the environment as effluents from manufacturing plants, or during their use and disposal. Among the major concerns associated with the presence of these chemicals in the environment is their potential toxicity to man. From a toxicological standpoint, the nervous system is one of the more sensitive sites of action of various environmental contaminants. At present, a toxicological evaluation of neurotoxic chemicals usually consists of measuring a given organism's behavioral response, neurophysio- logical activity and examining pathological changes in the nervous system. These methods are suitable for detecting neurotoxic disorders resulting from acute or chronic toxicity, but may not be able to detect subtle effects or a minimal degree of damage resulting from low-level exposure to these chemicals. Evidence has been presented which shows that subclinical nerve damage was detected in workers exposed to lead who showed no clinical neurological symptoms. » Therefore, reliable, sensitive techniques are needed to detect early damage resulting from a variety of neurotoxic substances. ------- Although various neurotoxic substances like DDT, nicotine, pyrethroids, tetrodotoxin and methylmercury act via different mechanisms, an effect upon the nerve membrane as a whole is implicated with all of them.3'4 It is generally believed that these chemicals interact specifically or non- specifically with components of the nerve membrane, thereby leading to possible changes in membrane function. Such changes may account for the neurophysiological effects of these chemicals. It is conceivable that such alterations may be preceded by changes in the conformation or structural organization of the nerve membrane. The conformational changes could there- fore be used as an indicator of neurotoxicity. In recent years, fluorescent probes have been employed for detecting structural or conformational changes in membranes and other biological structures.8'9'10'11'12'13 The high sensitivity of fluorescent probes to their microenvironment permits one to detect relatively low levels of alteration which cannot be discerned by biochemical or physiopathological methods. The objective of this investigation was to explore the feasibility of using fluorescent probes as a sensitive technique for detecting effects produced by the action of neurotoxic chemicals. OBJECTIVES 1. To examine if selected neurotoxic chemicals induce conformational changes in nerve cells or their components in vivo, using fluorescent probes. 2. To establish the usefulness of fluorescent probes as a tool for predicting neurotoxicological hazards. ------- SECTION 2 CONCLUSIONS The present investigation was undertaken to determine whether DDT, a neurotoxic pesticide, produces conformational changes in nerve membranes and if these changes can be detected by fluorescent probes. It has been shown that DDT alters ion permeability in nerve membranes.5 Hilton et al.3 and Hilton and O'Brien14 have postulated that the mechanism by which DDT alters nerve membrane permeability involves modification of the membrane structure. It may be postulated that DDT, on account of its high lipid solubility, may expand cellular membranes leading to an alteration in their structure as has been reported for certain nonspecific lipid-soluble drugs.6 In the present study, using brain synaptosomes as a model system, we have demonstrated that any structural or conformational changes produced by DDT can not be detected by fluorescent probe technique suggesting that the technique is not a sensitive indicator of DDT-induced toxicity. This evaluation of the fluorescent probes is based on the assumption that the pesticide at the concentrations tested did induce changes in the structure of the synaptosomes. ------- SECTION 3 MATERIALS AND METHODS Preparation of Brain Subcellular Fractions Brain synaptosomes were prepared from male Sprague-Dawley rats fed ad_ libitum and weighing 200-250g. The animals were sacrificed by decapita- tion, the brain was excised and placed in cold (4°C) homogenizing medium. ' - Rat brain synaptosomes were prepared according to the method of Gray and Whittaker. ** The brain tissue was disrupted by homogenization in 0.32 M sucrose. The crude mitochondrial fraction was separated from the cell debris, red blood cells, nuclei and soluble fraction by means of differ- ential centrifugation. Synaptosomes, free mitochondria, and myelin were then separated by means of density-gradient centrifugation. The scheme for the isolation of various subcellular fractions is outlined in Figures 1 and 2. The protein content of synaptosomes was determined according to the method of Lowry et^ al. Fluorescence .Measurements Fluorescence measurements were made with an Aminco-Keirs spectro- photofluorometer (American Instruments Company) using an X-Y recorder. The light source was a Xenon lamp. Measurements were made at 25°C in a temper- ature-controlled cell holder connected to a circulating water bath. Aliquots of synaptosomal preparations were resuspended in 0.32 M sucrose ------- in 15 mM Trls-HCl buffer (pH 7.4) before making fluorescence measurements. The final synaptosome concentration was approximately 75 wg/ml unless indicated otherwise. An aliquot of ANS (8-anilino-l-naphthalene sulfonic acid) stock solution was then added to give a final probe concentration of 3.2 X 10 M, unless indicated otherwise. The fluorescence measurements were carried out at wavelengths corresponding to excitation and emission maxima determined by analysis of the spectrum of ANS bound to the synaptosomes. ANS was obtained from Eastman Kodak and was recrystallized twice from boiling water before use. Brain homogenate -Pi (nuclei and cell debris) -P2 ~A (ravelin fragments) -B (nerve-ending particles) _C (mitochondria) —P3 (microsomes) —Pi+ (ribosomes: post-microsomal fraction) Figure 1. Nomenclature used in describing subcellular fractions. ------- Homogenate of brain tissue 10% (w/v) in 0.32 M sucrose centrifuged at lOOOg for 10 minutes I Precipitate V Washed twice by resuspension in 0.32 M sucrose and re-centrifuging as above f Separated in a density gradient to give three fractions Layer between 0.32 and 0.8 M sucrose centrifuged at 105g for 60 min. Layer between 0.8 and 1.2 M sucrose diluted with equal vols. of water, centrifuged at 105g for 60 min. Washings added to supernatant -> Supernatant centrifuged at 17000g for 55 min. \/ Supernatant centrifuged at 105g for 60 min. Pellet below 1.2 M sucrose Supernatant centrifuged at 10bg for 120 min. 1 * Final supernatant (discarded) B Figure 2. Scheme summarizing preparation of subcellular fractions. 6 ------- SECTION 4 EXPERIMENTAL PROCEDURES Method of Tissue or Cell Treatment Since absorption, distribution, excretion, and metabolism of a chemical determine its toxicity to the animal, it is desirable to expose the animal to the test chemical in vivo followed by in vitro testing to determine if the chemical produces any effect. The rats were exposed to the toxic substance, following which suitable tissues were removed and examined for possible conformational changes. Selection of Cell and/or Cell Components Examined for Possible Conformational Changes The techniques for measuring conformational changes using fluorescent probes, reproducibly and without complicated instrumentation requires that the biological material be in suspension. This precludes the use of brain slices or axons. In the present studies, which were designed to examine an overall effect of a given chemical on cell structure, it was desirable to use an isolated intact cell system in order to detect the possible conformational changes occurring in the whole nerve cell as well as its components. However, since techniques for the preparation of intact nerve cells are not currently available, we used nerve cell synaptosomes (presynaptic nerve-ending), as the test system because this fraction represents a well-characterized and functionally important part of the ------- neuron. There Is evidence to show that synaptosomes retain most of the metabolic and membrane properties of the nerve ending in situ. As Whittaker has pointed out, synaptosomes can be regarded as miniature, non-nucleated neurons, or even as model cells. Type of Fluorescent Probe Used Both intrinsic and extrinsic fluorescent probes were used in these studies to detect any possible conformational changes. In these studies, a fluorochrome, 8-anilino-l-naphthalene sulfonic acid (ANS) was used as an extrinsic probe since it has been most commonly used in detecting conforma- tional changes in membranes. Anesthetics and certain drugs which are known to act on the cell membrane have been found to cause a change in the ANS fluorescence in the presence of microsomal, erythrocyte and mitochondrial membranes.18'19'20'21'22 Spero et al.7reported that tetrodotoxin, a neurotoxin, reduced the ANS fluorescence increase in guinea pig brain synaptosomes. Fluorescence parameters including (i) fluorescence intensity, (ii) fluorescence spectra, and (iii) energy transfer from intrinsic membrane chromophores to ANS were measured to determine if any conformational changes in the test system had occurred. ------- SECTION 5 RESULTS Interaction of ANS with Rat Brain Synaptosomes Addition of synaptosomes to a dilute solution of ANS resulted in a marked enhancement of the fluorescence measured at 490 nm, using light of 390 nm wavelength for excitation. The enhancement of ANS fluorescence due to synaptosomes was accompanied by a shift of the emission maximum from 520 to 490 nm wavelength. Since ANS does not fluoresce in aqueous solution, the appearance of fluorescence on addition of synaptosomes indicates an interaction of the dye molecules with synaptosomes. An enhancement of ANS fluorescence and a shift of the maximum emission to shorter wavelengths is characteristic of a change in ANS environment from one of high to low dielectric constant. On the basis of the above observations, it is reason- able to assume that ANS is bound to hydrophobic phase when this compound interacts with synaptosomes. Figure 3 indicates a titration of 6 x 10 M ANS with brain synapto- somes (390 nm excitation, 490 nm measurement). Figure 4 illustrates the titration of 75 yg/ml of synaptosomal protein/ml with ANS. Effect of an Acute Dose of DDT on Synaptosome Fluorescence In these experiments the effect of DDT was studied following adminis- tration of a single dose which produced overt neurological symptoms in the animals. Sprague-Dawley rats (250-300g) were fasted overnight before being ------- c 8 I 2 o 3 75 100 125 Protein (/jg/ml) 175 200 Figure 3. Tltration of ANS (6 x 10~ M) with brain synaptosomes 10 ------- c 5 § 50 75 100 ANS(/LiM) 125 150 175 Figure A. Titration of brain synaptosomes (75 yg protein/ml) with ANS 11 ------- given high purity UDT in corn oil by oral intubation at a rate of 150 mg/kg body weight. Control animals were given corn oil. The treated animals showed tremors within 4 hours. They were then sacrificed by decapitation, the brain was excised and the synaptosomes were prepared as described earlier. Aliquots of synaptosomal preparation were resuspended in 0.32 M sucrose in 15 mM Tris-HCl buffer (pH 7.4). The final membrane concentration was approximately 75 yg of protein/ml. An aliquot of ANS stock solution was _c then added to give a final probe concentration of 3.2 x 10 M and fluor- escence measurements were performed in an Aminco-Keirs spectrofluorometer. The excitation and emission wavelengths were 390 and 490 nm, respectively. The emission spectrum of membrane-bound ANS was also measured. Fluorescence Intensity and Spectra The results showed that the fluorescence intensity and spectra of the ANS bound to synaptosomes from control and DDT-treated rats did not differ. DDT treatment also caused no change in the fluorescence intensity of ANS bound to brain mitochondria. These findings represent the results of three separate experiments. Effect of Energy Transfer from Intrinsic Membrane Chromophores to ANS The excitation spectrum of ANS overlaps the emission spectrum of tryptophan and tyroslne. One might expect a measurable transfer of excita- tion energy from membrane tryptophane and tyrosine to ANS molecules inserted in close proximity to these amino acids. Therefore, in the presence of ANS, excitation of protein fluorescence by 280 nm light produces energy transfer from tryptophan emission to bound ANS resulting in ANS fluorescence with an 12 ------- emission peak at about 490 nm. It has been shown that energy transfer is sensitive to even a small perturbation in membrane conformation. To determine if DDT treatment had an effect on energy transfer, DDT- exposed or control membrane suspensions (protein content 75 pg/ml) were placed in cuvettes and the intrinsic protein fluorescence peak (340 nm) was read following excitation with 280 nm light. ANS was then added to the cuvette and the emission was recorded following excitation at 280 nm. Treat- ment with DDT did not cause a change in ANS emission resulting from excita- tion at 280 nm, suggesting that the pesticide does not affect the transfer of tryptophan emission energy to ANS. Effect of DDT on Calcium-dependent Enhancement in Fluorescence The action of DDT on synaptosome-bound ANS fluorescence was further evaluated by examining the effect of the pesticide on a calcium-dependent 2+ increase in ANS fluorescence. Divalent cations including Ca cause an increase in the red cell membrane-bound ANS.20'23 It is likely that if DDT induces any conformational changes in synaptosomes, such changes may 2+ 2+ modify the ANS-fluorescence in response to Ca . We observed that Ca enhanced the fluorescence intensity of synaptosome-bound ANS by about 60%. 2+ When synaptosomes from DDT-treated rats were incubated with Ca , no change in fluorescence intensity or quantum yield was observed as compared to 2+ untreated synaptosomes also incubated with Ca Effect of DDT on Synaptosomal Protein (Intrinsic)Fluorescence The intrinsic chromophores of the proteins in the membrane originate e\ 1, from the amino acids, tyrosine and tryptophan. A change in fluorescence intensity or a shift in the position of the peak of intrinsic fluorescence 13 ------- can be used as a measure of conformational changes resulting from treatment with membrane perturbants. The intrinsic fluorescence technique has been used to study the interaction of anesthetics and hormones with erythrocyte n c Of membranes and proteins.^ ' For measurement of intrinsic protein fluorescence, the fluorescence emission was scanned from 300-400 nm following excitation with 280 nm light. The peak height, which was usually at 340 nm in control synaptosomes was recorded. Our results showed that treatment with DDT did not alter the intensity or emission spectrum of the native protein fluorescence. Effect of Repeated Doses of DDT on Synaptosomes Fluorescence The above studies showed that a single dose of DDT which produced overt neurological symptoms in rats, did not induce conformational changes in brain synaptosomes. Additional studies were undertaken to examine whether or not administration of repeated sublethal doses of the pesticide to rats over an extended period induced conformational changes in brain synaptosomes. In these studies, two groups of rats (200-250 gm) were given DDT at two different dosage levels daily for eight consecutive days. One group of animals was administered the pesticide daily in corn oil by oral intuba- tion at a rate of 25 mg/kg body weight. These experiments were repeated with the second group using a dose of 50 mg/kg. Control animals were given corn oil. None of the animals in either of the treated groups showed obvious symptoms of toxicity at the end of the treatment period. They were then sacrificed by decapitation, the brain was excised and the synaptosomes were prepared according to the method of Gray and Whittaker. The effect of DDT on synaptosomes as measured by extrinsic and intrinsic fluorescence was determined as described in single-dose studies. 14 ------- The results showed that like the single dose of DDT, administration of repeated doses of the pesticide at the. levels used in the study did not induce any conformational changes in brain synaptosomes as measured by ANS fluorescence (intensity, emission spectrum and energy transfer). DDT treatment also did not alter the intensity or emission spectrum of intrinsic fluorescence. Effect of Diphenylhydantoic on Synaptosomal Membranes Exposed to the Drug in vitro Diphenylhydantoic (dilantiir^v is an Important drug used to protect SO epileptic patients against seizure. It has been suggested that Dilantin^ interacts with plasma membranes and exerts a stabilizing effect on all excitable cell membranes.27*28 It was therefore of interest to determine if the drug induces conformational changes in synaptosomal membranes as measured by intrinsic and ANS fluorescence. fa In these studies, the in vitro effect of Dilantiir^ on the fluorescence of ANS bound to synaptosomes isolated from untreated rats was examined. The synaptosomes were incubated with the sodium salt of diphenylhydantoin (10~ to 10" M) for fifteen minutes. An aliquot of ANS solution was then _c added to give a final probe concentration of 5 x 10 M and fluorescence (S) measurements were made as described above. We observed that the Dilantin^ -4 up to a concentration of 10 M did not cause any change in the fluorescence •* intensity or spectrum of ANS. The chemicals also showed no effect on intrinsic fluorescence. 15 ------- REFERENCES 1. Catton MJ, Harrison MJG, Fullerton PM, et al: Br Med J 2:80, 1970 2. Seppalainen AM, Hernberg S: Br J Ind Med 29:243, 1972 3. Hilton BD, Bratkowski TA, Yaraada M, et al: Pestic Biochem Physiol 3:14, 1973 4. Hilton BD, O'Brien RD: Pestic Biochem Physiol 3:206, 1973 5. Narahashi T: Bull WHO 44:337, 1971 6. Segall HJ, Wood JM: Nature 248:456, 1972 7. Spero, L, Siemens AJ, Toulis, GA: Mol Pharmacol 9:330, 1973 8. Azzi A: Methods Enzymol 32:234, 1974 9. Brand L, Gohlke JR: Anna Rev Biochem 41:843, 1972 10. Chignell CF: Methods in Pharmacology Edited by CF Chignell. 1972, 2: pp 33 11. Radda GK: Current Topics in Bioenergetics. Edited by DR Sanadi. 1971, 4pp81 12. Radda GK, Vanderkooi J: Biochim Biophys Acta 265:509, 1972 13. Seeman P: Pharmacol Rev 24:583, 1972 14. Gray EG, Whittaker VP: J Anat 96:79, 1962 15. Lowry OH, Rosebrough NJ, Farr AL, et al: J Biol Chem 193:265, 1951 16. Whittaker VP, Barker LA: Methods in Neurochemistry. Edited by R Fried. 1972, 2ppl 17. Narahashi T, Hess HG: J Gen Physiol 51:177, 1968 18. Azzi A, Chance B, Radda GK, et al: Proc Nat Acad Sci 62:612, 1969 19. Chance B, Azzi A, Mela L, et al: FEES Lett 3:10, 1969 20. Feinstein MB, Spero L, Felsenfield: FEBS Lett 6:245, 1971 16 ------- 21. Freedmuu KB, Kadda CK: FEBS Lett 5:150, 1969 22. Vanderkooi J, Martonosi A: Arch Bloc hem Biophys 133:153, 1969 23. Rubaclava B, Munoz 1), Gltler C: Biochemistry 8:2742, 1969 24. Teale FWJ, Weber G: Biochm J 65:476, 1956 25. Sonnenberg M: Proc Natl Acad Sci USA 68:1051, 1971 26. Spero L: Proc. Canad Fed Biol Sco 14:32, 1971 27. O'Donnell JM, Kovacs T, Szabo B: Pflugers Arch 358:275, 1975 28. Wilensky AJ, Lowden JA: Can J Physiol Pharmacol 50:346, 1972 17 ------- TECHNICAL REPORT DATA (Please read Instructions on the rcrcrse before c 1. REPORT NO. EPA-6QO/1-78-QU 2. 3. RECIPIENT'S ACCESSION-NO. 4. TITLE AND SUBTITLE SCREENING METHODS FOR TOXIC SUBSTANCES 5. REPORT DATE February 1978 6. PERFORMING ORGANIZATION CODE 7. AUTHOR(S) Harish C. Sikka 8. PERFORMING ORGANIZATION REPORT NO. 9. PERFORMING ORGANIZATION NAME AND ADDRESS Syracuse Research Corporation Syracuse, New York 13210 10. PROGRAM ELEMENT NO. 1LA629 11. CONTRACT/GRANT NO. 68-02-1786 12. SPONSORING AGENCY NAME AND ADDRESS Health Effects Research Laboratory Office of Research and Development U.S. Environmental Protection Agency Research Triangle Park. N.C. 27711 13. TYPE OF REPORT AND PERIOD COVERED RTP.NC 14. SPONSORING AGENCY CODE EPA 600/11 15. SUPPLEMENTARY NOTES 16. ABSTRACT The present report deals with the application of fluorescent probe technique to the detection of conformational changes in rat brain synaptosomes under the influence of certain neurotoxic chemicals, chlorophenothane (DDT) and diphenylhydantoin, which are expected to produce functional changes in nerve membranes. Pretreatment of the rats with (i) a single dose of DDT capable of producing neurological symptoms and (ii) repeated sub-lethal doses of DDT did not alter the fluorescence characteristics of the hydrophobic probe 8-anilino-l- naphthalene sulfonic acid (ANS) bound to the synaptosomes. DDT treatment also showed no effect on native protein fluorescence of synaptosomes. Exposure of synaptosomes to diphenylhydantoint in vitro did not induce conformational changes as measured by ANS and intrinsic fluorescence. 17. KEY WORDS AND DOCUMENT ANALYSIS DESCRIPTORS b.IDENTIFIERS/OPEN ENDED TERMS c. COSATI Field/Group toxicity fluorescent penetration tests sieve analysis neurochemistry brain laboratory animals toxic substances screening tests 06 A, T 14C 18. DISTRIBUTION STATEMENT RELEASE TO PUBLIC 19. SECURITY CLASS (ThisReport} UNCLASSIFIED 21. NO. OF PAGES 23 20. SECURITY CLASS (Thispage) UNCLASSIFIED 22. PRICE EPA Form 2220-1 (9-73) 18 ------- |