August 1992 ISOPROPYL METHYLPHOSPHONIC ACID Health Advisory Office of Water U.S. Environmental Protection Agency Washington, DC 20460 ------- Isopropyl Methylphosphonic Acid (IMPA) Health Advisory Office of Water U.S. Environmental Protection Agency Washington, DC 20460 August 1992 ------- ------- Health Advisory on Isopropyl Methylphosphonic Acid (IMPA) Authors: Joyce Morrisey Donohue, Ph.D. Welford C. Roberts, Ph.D. Project Officer: Krishan Khanna, Ph.D. Office of Water U.S. Environmental Protection Agency Washington, DC 20460 August 1992 ------- PREFACE This report was prepared in accordance with the Memorandum of Understanding between the Department of the Army, Deputy for Environmental Safety and Occupational Health (OASA(ILSE)), and the U.S. Environmental Protection Agency (EPA), Office of Water (OW) , Office of Science and Technology, for the purpose of developing drinking water Health Advisories (HAs) for selected environmental contaminants, as requested by the Army. Health Advisories provide specific advice on the levels of contaminants in drinking water at which adverse health effects would not be anticipated and which include a margin of safety to protect the most sensitive members of the population. A Health Advisory provides health effects guidelines and analytical methods and recommends treatment techniques on a case-by-case basis. These advisories are normally prepared for one-day, ten-day, longer-term, and lifetime exposure periods where available toxicological data permit. These advisories do not condone the presence of contaminants in drinking water, nor are they legally enforceable standards. They are not issued as official regulations and they may or may not lead to the issuance of national standards or Maximum Contaminant Levels (MCLs). This report is the product of the Health Advisory Development process. Available toxicological data (as provided by the Army and as found in open literature sources) on the munitions chemicals Sarin, diisopropyl methylphosphonate (DIMP) and isopropyl methylphosphonic acid (IMPA) have been reviewed, and relevant findings are presented in this report in a manner that allows for evaluation of the data without continual reference to the primary documents. This report has been submitted for critical internal and external review by the EPA. I would like to thank the authors who provided the extensive technical knowledge required for the preparation of this report. I am grateful to the members of the EPA Toxicology Review Panel who took time to review this report and to provide their invaluable input, and I would like to thank Dr. Edward Ohanian, Chief, Human Risk Assessment Branch, and Ms. Margaret Stasikowski, Director, Health and Ecological Criteria Division, for providing me with the opportunity and encouragement to be a part of this project. The preparation of this Health Advisory was funded, in part, by Interagency Agreement (IAG) 85-PP5869 between the U.S. EPA and the U.S. Army Medical Research and Development Command (USAMRDC). This IAG was conducted with the technical support of the U.S. Army Biomedical Research and Development Laboratory (USABRDL), Dr. Howard T. Bausum, Project Manager. Krishan Khanna, Project Officer Office of Water ------- TABLE OF CONTENTS PAGE LIST OF TABLES iii LIST OF APPENDICES iii EXECUTIVE SUMMARY ES-I I. INTRODUCTION 1-1 II. GENERAL INFORMATION AND PROPERTIES II-1 III. OCCURRENCE III-l IV. ENVIRONMENTAL FATE IV-1 V. TOXICOKINETICS V-l A. Absorption V-l B. Distribution V-l C. Metabolism V-2 D. Excretion V-3 VI. HEALTH EFFECTS VI-1 A. Health Effects in Humans VI-1 1. Short-term Exposure VI-1 2. Longer-term Exposure VI-1 B. Health Effects in Animals VI-1 1. Short-term Exposure VI-1 a. Skin and Eye Irritation VI-2 b. Dermal Sensitization VI-2 2. Longer-term Exposure VI-4 3. Reproductive Effects VI-4 4. Developmental Effects VI-4 5. Mutagenicity VI-4 6. Carcinogenicity VI-5 VII. HEALTH ADVISORY DEVELOPMENT VII-1 A. Quantification of Toxicological Effects VII-1 1. One-day Health Advisory VII-1 2. Ten-day Health Advisory VII-2 3. Longer-term Health Advisory VII-2 4. Lifetime Health Advisory VII-3 B. Evaluation of Carcinogenic Potential VII-5 VIII. OTHER CRITERIA, GUIDANCE AND STANDARDS VIII-1 IX. ANALYTICAL METHODS IX-1 i ------- Table of Contents - continued PAGE X. TREATMENT TECHNOLOGIES X-l XI. CONCLUSIONS AND RECOMMENDATIONS XI-1 XII. REFERENCES XII-L ii ------- LIST OF TABLES PAGE II-l General Chemical and Physical Properties of Isopropyl Methylphosphonic Acid II-2 VI-1 Mortality in Rats and Mice Exposed to Acute Doses of IMPA VI-3 LIST OF APPENDICES Data Deficiencies/Problem Areas and Recommendations for Additional Data Base Development for IMPA Al-1 iii ------- EXECUTIVE SUMMARY Isopropyl methyl phosphonic acid (IMPA) is a degradation product of the nerve gas isopropyl methylphosphonofluoridate (GB or Sarin). Isopropyl methyl- phosphonic acid is a moderately strong acid (pKa - 2.38) which is most commonly found in the environment in its ionized state; it is nonvolatile and soluble in water. The resonance-stabilized IMPA ion is chemically stable with a hydrolytic half-life of 1,900 years at pH 1 and longer at higher pH values. Most bacterial species are not able to degrade IMPA; an exception is Pseudomonas testosteroni. a species that is able to convert IMPA to methane, isopropanol and phosphorous acid or phosphoric acid under anaerobic conditions. Some of the toxicokinetic and toxicological data that can be used in the evaluation of IMPA come from studies of Sarin and diisopropyl methyl- phosphonate (DIMP; a by-product produced during the manufacture of Sarin). Since these compounds degrade to produce IMPA in living systems, the data are applicable to IMPA. Although there have been no absorption studies of IMPA, the systemic toxicity that occurs following oral administration of this compound and the low concentration of IMPA in the feces when DIMP is administered orally, indicate that intestinal absorption does occur. After absorption, the IMPA is distributed in the plasma to the tissues. There appears to be little or no metabolic conversion of the IMPA to simpler compounds. The highest concentrations of IMPA are found in the kidney, lungs and brain. A portion of the IMPA in the brain becomes tissue-bound, particularly in the hypothalamus. Unbound IMPA is excreted in the urine. The oral LD50 values for rats and mice (5,500 to 7,700 mg/kg) are indicative of low acute toxicity. Rabbits did not show any signs of toxicity or irritation from IMPA (100 mg) applied to the eyes, but it was moderately irritating to the skin at a dose of 2.0 mg/kg. Dermal application of a 0.1% solution did not cause sensitization and IMPA was not mutagenic in the Ames assay at concentrations of 0.5 to 5,000 /ig/plate. Compound-related adverse effects did not develop in rats that were exposed to concentrations of 300 to 3,000 ppm (300-3,000 mg/L) IMPA in drinking water for 90 days. There are no data on the reproductive or developmental toxicity of IMPA and no information pertaining to its carcinogenic potential. Since there are no other appropriate data, all of the HA values for IMPA were derived from a 90-day study of rats exposed to concentrations of 0, 300, 1,000 or 3,000 ppm (0, 300, 1,000 or 3,000 mg/L, respectively) in drinking water, despite the lack of any effects in this study. The highest concentration tested (3,000 ppm) was determined to be the no-observable-adverse-effect-level (NOAEL), based on observations of body weight, clinical signs, hematological parameters, terminal blood chemistry values, and histopathology. (This concentration is equivalent to a dose of 399.1 mg/kg/day for females and 278.5 mg/kg/day for males.) The longer-term HA for a 10-kg child calculated from a NOAEL of 278.5 mg/kg/day is 30 mg/L. In the absence of available data to ES-1 ------- determine One-day and Ten-day HAs, the Longer-term HA for a 10-kg child is considered acceptable for these exposure durations. The Longer-term HA for an adult is 100 mg/L. The 90-day study in rats also serves as the basis for the Lifetime HA. The Reference Dose (RfD), derived from the 90-day NOAEL of 278.5 mg/kg/day, is 0.1 mg/kg/day (100 Mg/kg/day). The Drinking Water Equivalent Level (DWEL) derived from the RfD is 4 mg/L and the Lifetime HA is 0.7 mg/L (700 /ig/L), assuming that 20% of the total exposure to IMPA comes from drinking water. According to the EPA criteria for the classification of carcinogens, IMPA is placed in Group D: Not classifiable as to human carcinogenicity. This category is for chemicals with inadequate human and animal evidence of carcinogenicity and for chemicals for which no data are available. ES-2 ------- I. INTRODUCTION The Health Advisory (HA) Program, sponsored by the Office of Water (OW), provides information on the health effects, analytical methodology and treatment technology that would be useful in dealing with the contamination of drinking water. Health Advisories describe nonregulatory concentrations of drinking water contaminants at which adverse health effects would not be anticipated to occur over specific exposure durations. Health Advisories contain a margin of safety to protect sensitive members of the population. Health Advisories serve as informal technical guidance to assist Federal, State and local officials responsible for protecting public health when emergency spills or contamination situations occur. They are not to be construed as legally enforceable Federal standards. The HAs are subject to change as new information becomes available. Health Advisories are developed for one-day, ten-day, longer-term (approxi- mately 7 years, or 10 percent of an individual's lifetime) and lifetime exposures based on data describing noncarcinogenic end points of toxicity. For those substances that are known or probable human carcinogens, according to the Agency classification scheme (Group A or B), Lifetime HAs are not recommended. The chemical concentration values for Group A or B carcinogens are correlated with carcinogenic risk estimates by employing a cancer potency (unit risk) value together with assumptions for lifetime exposure and the consumption of drinking water. The cancer unit risk is usually derived from the linearized multistage model with 95 percent upper confidence limits. This provides a low-dose estimate of cancer risk to humans that is considered unlikely to pose a carcinogenic risk in excess of the stated values. Excess cancer risk estimates may also be calculated using the one-hit, Weibull, logit or probit models. There is no current understanding of the biological mechanisms involved in cancer to suggest that any one of these models is able to predict risk more accurately than another. Because each model is based on differing assumptions, the estimates that are derived can differ by several orders of magnitude. 1-1 ------- II. GENERAL INFORMATION AND PROPERTIES Isopropyl methylphosphonic acid (IMPA) is a hydrolytic degradation product of the nerve gas isopropyl methylphosphonofluoridate (GB or Sarin) (Rosenblatt et al., 1975a). Sarin was used as a chemical warfare agent. Isopropyl methyl phosphonic acid can be prepared through the alkaline hydrolysis of diisopropyl methylphosphonate (DIMP) or the hydrolysis of isopropyl methylphosphonochloridate with cold aqueous acetone (Rosenblatt et al., 1975b). The pKg of the acid functional group is estimated to be about 2.38 (Bossle et al., 1983). The anionic form of the molecule will, accordingly, exist at neutral and alkaline pHs. Based on structure and chromatographic behavior with an acetic acid/n-butanol/water solvent mixture (Hoskin, 1956), IMPA is soluble in water and other polar solvents. Solubility in nonpolar solvents is predicted to be limited. Based on a boiling point of 97—98°C at 0.08 torr and its chemical structure, IMPA is expected to be relatively nonvolatile. Chemically, IMPA is extremely stable due to resonance stabilization of the alkyl-ester bond. Based on the rate of hydrolysis of IMPA in benzenesulfonic acid, IMPA has a half-life of 1,900 years at pH 1 (Rosenblatt et al., 1975b). At neutral and alkaline pHs the half-life of this compound is much longer. Hydrolysis of the ester bond, when it does occur, produces methylphosphonic acid (MPA) and isopropyl alcohol. II-l ------- TABLE II-1 General Chemical and Physical Properties of Isopropyl Methylphosphonic Acid CAS Number Synonyms Molecular Weight Chemical Formula Structure Physical State Boiling Point Melting Point Density Vapor Pressure Solubility Octanol/Water Partition Coefficient L°g K0W Taste Threshold (Water) Odor Threshold (Water) Conversion Factor (in air) 1832-54-8 6838-93-3 (Sodium salt) isopropyl methylphosphonate; methyl phosphonic acid, isopropyl ester; phosphonic acid, methyl, monoisopropyl ester; phosphonic acid, methyl, mono(l-methylethyl) ester 138.12 c4Hh03p < OH (CH3)2CHO' acid - liquid (oil) sodium salt - solid 97—98°C (0.08 torr) 123—125°C (0.2 torr) . .(a) 1.1091 (20"C) 1 ppm = 6 mg/m3 References: Beilstein Database, 1992; Rosenblatt et al., 1975b (a) No data II -2 ------- Ill. OCCURRENCE Isopropyl methylphosphonic acid was introduced into the environment as a degradation product of the nerve gas, Sarin. It is known to have contaminated groundwater at, and adjacent to, its site of production. Its very low volatility makes it an unlikely atmospheric contaminant. Isopropyl methyl- phosphonic acid is not known to occur naturally. Active production of Sarin was limited to the area of the Rocky Mountain Arsenal (RMA) adjacent to the northern city limits of Denver, Colorado. This area subsequently became a storage site for unused Sarin. Prior to 1956, effluents from the manufacture of Sarin entered five unlined surface ponds located on site at the RMA, with subsequent discharge into an asphalt-lined reservoir at the same facility. Seepage from these ponds has contributed to the contamination of the groundwater in the underlying aquifers (Robson, 1981; PMRMA, 1991a). Between 1973 and 1981, the RMA was involved in the detoxification of the previously-stored Sarin (Robson, 1981). Actual levels of IMPA in groundwater during the years of active Sarin produc- tion were not measured. However, a computer-simulation model based on groundwater movement and solute transport, as described by Robson (1981), has been used to estimate concentrations and movement of diisopropyl methyl- phosphonate (DIMP), a by-product of Sarin synthesis, in the groundwater. Since IMPA is formed from the degradation of DIMP, this same model can be used to estimate the subsurface movement of IMPA at Rocky Mountain Arsenal. Based on the Robson (1981) model, the movement of the groundwater through the alluvial aquifer resulted in one contaminated area or plume reaching the South Platte River, to the west of the arsenal, with the maximum rate of discharge occurring between 1958 and 1960. Based on the rate of plume movement, this particular contaminated area should have been essentially nonexistent by 1972, according to the Robson (1981) model. Two additional contaminated areas, to the south of the arsenal and to the north of the ponds and extending to the surrounding area, are postulated to be relatively stable due to low groundwater velocities. The northern plume has contaminated a creek, an adjacent lake and its canal tributary. The diisopropyl methylphosphonate has been detected in two samples from the lake (Robson, 1981). Rocky Mountain arsenal area wells sampled in 1989 and 1991 had IMPA concentrations ranging from less than 0.392 /ig/L to 26,236 /ig/L (PMRMA, 1991b). The initial chemical analysis for DIMP, undertaken in 1974, revealed its presence in the groundwater both at the arsenal and in the surrounding areas to the north and west. Levels as high as 44,000 ng/L were detected near one of the abandoned ponds (Robson, 1981), whereas wells at the arsenal contained levels ranging from below the detection limit to 1,420 Mg/L (1.42 ppm). In December 1974, analysis of off-post wells indicated concentrations of 75 ^g/L (75 ppb) DIMP (Rosenblatt et al., 1975a). Trace concentrations have been found in wells down-gradient from the ponds, generally north-northwest of the arsenal, and within one mile of municipal water wells (Robson, 1981). More recent measures of DIMP in groundwater at RMA ranged from 2.1 ng/L to 30,000 (ig/L in the first half of 1989, and from 0.445 //g/L to 37,200 ^g/L in the fall of 1989 (PMRMA, 1991a,b). Monitoring data from 1991 show that DIMP concentrations ranged from 0.43 ug/L to 21,000 Mg/L (PMRMA, 1991b). III-l ------- Computer-based predictions for distribution of DIMP indicate that without remedial action or additional input of the contaminant, a steady decrease in the concentration of DIMP in the groundwater in most of the area will occur as a result of discharge to the South Platte River and dilution by uncontaminated water, thereby posing no danger to municipal water supplies (Robson, 1981). Levels of DIMP in the surface water of the lake act to recharge the aquifer. Thus, the concentration of DIMP in the aquifer between the arsenal and the contaminated lake will remain constant. Similar predictions apply to IMPA since it will accompany DIMP in the environment. This estimate is based on the assumption that the migration rate of IMPA in the aquifer is the same as or is faster than the migration rate of DIMP. Differences between IMPA and DIMP migration in soils and groundwater may exist due to differences in chemical and physical properties. Diisopropyl methylphosphonate is nonionic whereas isopropyl methylphosphonic acid is an ionizable acid with a low pKg. The IMPA anion is expected to be more water soluble than DIMP and more likely to bind to cationic soil surfaces. Based on measured levels of DIMP in ground and surface waters 18 to 23 years after active disposal of the effluent at the RMA, and considering IMPA's low volatility, it appears likely that IMPA will remain in the water with little or no volatilization into the atmosphere. The chemical stability of IMPA will also contribute to its persistence in the environment. Ill - 2 ------- IV. ENVIRONMENTAL FATE The available data suggest that little abiotic degradation of IMPA occurs in the environment. Small amounts of the compound can be converted to methyl phosphonic acid (MPA) particularly at low pHs. The half-life of IMPA at pH 1, however, is 1,900 years and it is longer at higher pHs. Therefore, production of MPA from IMPA is minimal in sterile media (Rosenblatt et al., 1975b). Isopropyl methylphosphonic acid also appears to be stable to biotic degradation under most circumstances. Cook et al. (1978) isolated one strain of bacteria from sewage which appeared to metabolize IMPA, producing methane as a by-product of IMPA degradation (Daughton et al., 1979a). This bacterium was identified as a strain of Pseudomonas testosteroni. Thirteen other bacterial strains from sewage had no effect on IMPA (Cook et al., 1978). Detailed studies of the action of P. testosteroni on IMPA indicate that the bacteria will utilize IMPA as a phosphorus source when other phosphorus sources are limited (Daughton et al., 1979a). Under these conditions, the phosphorus-carbon bond of IMPA is cleaved, resulting in a stoichiometric release of methane under aerobic conditions. Some evidence exists that hydrolysis of the ester bond occurs, releasing isopropanol and phosphorous acid or phosphoric acid (Alexander et al., 1977). Daughton et al. (1979b) studied the effect of soil binding and alternate phosphate sources on IMPA metabolism by P. testosteroni. Isopropyl methylphosphonic acid did not bind to the soils (pH 3.9; 35% organic matter) and, therefore, remained available to the bacterial inoculum as a source of phosphorus. The rate of degradation of IMPA was not affected by alternate phosphate sources in the environment in this study. Howells et al. (1973) examined the biotransformation of Sarin by wheat plants. Isopropyl methylphosphonic acid was produced in the plants from the uptake of Sarin from a hydroponic growth solution. There was no evidence that the IMPA was further degraded to MPA in the 5-week period following 24-hour exposure of the plants to Sarin. This study suggests that vascular plants lack the ability to metabolize IMPA. Wheat plants will also absorb Sarin from the vapor phase through leaf surfaces. The Sarin is then metabolized to IMPA (Howells et al., 1976). In this study, Sarin and IMPA were both detected in the exposed plants, but MPA was not detected. These data confirm the stability of IMPA in tissues of the wheat plant. IV-1 ------- V. TOXICOKINETICS Although there have been no absorption studies of IMPA, the systemic toxicity that occurs following oral administration of this compound and the low concentration of IMPA in the feces when DIMP is administered orally indicate that intestinal absorption does occur. After absorption, the IMPA is distributed in the plasma to the tissues. There appears to be little or no metabolic conversion of the IMPA to simpler compounds. The highest concentrations of IMPA are found in the kidney, lungs and brain. A portion of the IMPA in the brain becomes tissue-bound, particularly in the hypothalamus. Unbound IMPA is excreted in the urine. A. Absorption No data are available relating to the absorption of IMPA through the oral, dermal or respiratory routes of exposure. However, based on effects that occurred during oral LD5Q studies in rats and mice, it can be assumed that IMPA is absorbed from the gastrointestinal tract. B. Distribution No data are available describing the tissue distribution of IMPA following oral exposure. The tissue disposition of Sarin, however, has been evaluated following intravenous administration of a sublethal dose (80 A/g/kg) of tritium-labeled material to mice (Little et al., 1986). Since IMPA is the major degradation product of Sarin, Little et al. (1986) measured tissue levels of IMPA as well as the parent compound. These data, accordingly, provide information on the tissue distribution of IMPA, but they do not indicate whether the label entered the cell as Sarin or IMPA. Since Sarin is hydrolyzed to IMPA by a rat serum enzyme (Hoskin, 1956), it is postulated that at least a portion of the tissue label enters the cell as IMPA. Following intravenous administration of radiolabeled Sarin (80 ^g/kg, 70 ^Ci), groups of five IRC outbred male mice were sacrificed at 1, 5, 15 or 30 minutes and 1, 2,4, 8 or 24 hours. Blood was collected and tissues removed for assay. Samples of brain, liver, lung, heart and kidney tissue, diaphragm fat, and blood plasma were analyzed for Sarin, IMPA and MPA (Little et al., 1986). In all cases, the concentration of IMPA in the tissues was greater than the concentration of Sarin, suggesting a rapid metabolism of Sarin to IMPA (Little et al., 1986). Isopropyl methylphosphonic acid concentration was 20 times greater than the Sarin concentration in all tissues except the brain. A smaller concentration difference occurred in the brain, IMPA concentration being only 4 times greater than that of Sarin. Isopropyl methylphosphonic acid concentration in the lungs, heart, kidneys and plasma declined by about 50% in the first 30 minutes after administration and more slowly after that. At the end of 24 hours, free IMPA concentrations were highest in the lungs, plasma and kidney. These organs also contained the highest concentrations of bound IMPA. The high concentration of IMPA in the kidneys suggests that the kidneys play a major role in Sarin detoxification and excretion. Liver levels of free and bound IMPA were lower than the kidney levels at all time points. V-l ------- Residual bound IMPA in the brain exceeded the concentration of free IMPA in the early, as well as most of the late, time periods suggesting rapid binding of IMPA to brain proteins. After 24 hours, the levels of bound IMPA exceeded the free IMPA in all tissues. Additional studies have been conducted on the fate of Sarin in rat brain tissues. Following intravenous administration of 60 fig/kg of P32-Sarin, IMPA was bound to brain proteins (Fleisher et al., 1964). The administered dose was equivalent to 1.5 times the LD5Q for Sarin. In an attempt to study regional impacts of Sarin on the brain, Little et al. (1988) injected tritium-labeled Sarin into the tail vein of groups of five mice each. The animals were sacrificed at 10 minutes and at 6 or 24 hours after injection. The brains were removed and carefully divided into seven sections. Concentrations of Sarin, IMPA and MPA in each brain compartment were measured. Sarin and its degradation products, IMPA and MPA were present in the greatest concentration in the hypothalamus as compared to the cerebellum, medulla, midbrain, striatum and cortex regions of the brain. The level of IMPA in the hippocampus was also elevated compared to other brain areas. The concentration of free IMPA declined with time in all brain compartments whereas levels of bound IMPA increased in the period between 6 and 24 hours. C. Metabolism The biochemical stability of IMPA was studied by Hoskin (1956). Isopropyl methylphosphonic acid was administered by an intraperitoneal injection of 56 mg to a single adult male Wistar rat. This is equivalent to a dose of 140 mg/kg, based on a body weight of 400 g for an adult male rat. Paper chromatographic examination of urine collected over 48 hours indicated that IMPA was excreted intact. No MPA was excreted, suggesting either that there is little or no hydrolysis of the isopropyl-ester functional group or, if hydrolysis does occur, the MPA produced is retained by the body. Tissue retention of methyl phosphonic acid may well occur. In the Little et al. (1986) study of tissue distribution of tritium-labeled Sarin, all tissues except the kidney and plasma had relatively constant concentrations of nonextractable label during the 24-hour period after compound administration. The nonextractable radioactivity was presumed to be protein-bound MPA. Bound MPA was also identified in the brain 24 hours after compound administration (Little et al., 1988). However, conversion of Sarin to MPA has not been demonstrated. Hoskin (1956) also investigated the availability of the phosphate from IMPA to form hexose phosphonate esters in the presence of active phosphorylase enzymes. In vitro incubation of IMPA with phosphorylase, glycogen and adenylic acid, followed by chromatographic analysis of the reaction product, indicated that no hexose phosphonate esters were formed. When inorganic phosphate was added to the same reaction medium, both glucose-1-phosphate and glucose-6-phosphate were produced. V- 2 ------- D. Excretion Isopropyl methylphosphonic acid appears to be excreted without metabolic alteration. Hoskin (1956) found that 40% of the label from an intravenous dose of 56 mg of P32-labeled IMPA was excreted in the urine over the first 48 hours following injection. The only label-containing compound found in a chromatogram of the urine was the IMPA itself. There was no MPA excreted. Isopropyl methylphosphonic acid is also an excretory metabolite for Sarin and DIMP (Little et al., 1986; Ivie, 1980). Radioactive 14C-labeled DIMP was given to a 357 kg lactating Jersey cow following 5 days of oral dosing with 10 mg/kg DIMP in gelatin capsules (Ivie, 1980). On the sixth day, the cow was given radiolabeled compound. All excreta were collected. Analysis of the excreta indicated that DIMP was stoichiometrically converted to IMPA which was excreted primarily in the urine. Small amounts of IMPA and DIMP were also identified in the feces. After 96 hours, 84% of the label had been excreted in the urine and 7.4% in the feces. Milk samples collected from the cow contained 0.08% of the label. V- 3 ------- VI. HEALTH EFFECTS Isopropyl raethylphosphonic acid has a low degree of toxicity as demonstrated by the lack of effects in animals during acute and subchronic studies (Mecler and Dacre, 1982). Oral LD50 values for rats and mice demonstrated low acute toxicity. Rabbits did not show any signs of toxicity or irritation from IMPA applied to the eyes, but it was mildly irritating to the skin. Dermal application did not cause sensitization, and IMPA was not mutagenic in the Ames assay. Compound-related adverse effects did not develop in rats that were exposed to IMPA in drinking water for 90 days. A. Health Effects in Humans 1. Short-term Exposure No information was found in the available literature regarding adverse health effects associated with short-term exposure of humans to IMPA. 2. Longer-term Exposure No information was found in the available literature regarding adverse health effects associated with long-term exposure of humans to IMPA. B. Health Effects in Animals 1. Short-Term Exposure LD5Qs of IMPA have been evaluated in both the mouse and rat (Mecler, 1981). In each study, IMPA was administered by gavage as a single dose. The animals were observed for 14 days following treatment and weighed at 0, 7 and 14 days. Appearance, behavior and clinical signs were monitored daily. Male Charles River rats (56-67 days old, 5/sex/dose) were treated with doses of 4,640, 6,810, 10,000 or 14,700 mg/kg 99% pure IMPA as the sodium salt (Mecler, 1981). The females received doses of 3,160, 4,640, 6,810 or 10,000 mg/kg. The resulting mortality is summarized in Table VI-1. Loose stools were observed in several animals at all dose levels. Reduced motor activity and prostration were seen in some animals of both sexes at doses of 3,160 mg/kg or greater, while ataxia was observed in some animals at doses of 4,640 mg/kg or greater. The ataxia occurred in one female at the 4,640 mg/kg level, three females at the 6,810 mg/kg level, and one male and one female at the 10,000 mg/kg level. In the necropsy studies, no gross organ or tissue abnormalities were observed in the animals that survived until sacrifice. The animals that succumbed to compound administration displayed red or mottled lungs and dark spots on the thymus. Among rats that died, red or mottled lungs occurred in some of the males at the 10,000 and 14,700 mg/kg levels and some females at the 6,810 mg/kg level, and one female at each of the 4,640 and 10,000 mg/kg levels. The thymus spots were seen in females at 6,810 and 10,000 mg/kg VI-1 ------- levels and in males at the 10,000 and 14,700 nig/kg levels. The stomach tissue was red and both the stomach and intestines were filled with fluid (Mecler, 1981) . All of the highest-dose test animals (5/sex) died in the study, while none of the lowest-dose animals died (Mecler, 1981). The LD50 value for the males was 7,650 mg/kg; for the females it was 6,070 mg/kg. Effects were seen at even the lowest dose administered, thus, the lowest-observable-adverse-effect-level (LOAEL) from this study is 3,160 mg/kg. Male and female 9-week-old Charles River mice (5/sex/group) were given doses of 3,160, 4,640, 6,810 or 10,000 mg/kg IMPA (Mecler, 1981). The observation parameters for this study paralleled those for the rat study discussed above with the resulting mortality summarized in Table VI-1. Soft liquid stools were observed in some animals at all dose levels except the 3,160 mg/kg females. Reduced motor activity and ataxia were seen in some animals at doses of 3,160 mg/kg or greater, in all male mice at the 6,810 mg/kg level, and all mice at the 10,000 mg/kg level that survived for 1 hour. Prostration occurred in one female at 6,810 mg/kg and in two males and one female at 10,000 mg/kg. Mottled or red lungs were observed in three females at the 10,000 mg/kg level who died during the study; fluid-filled stomach and intestines appeared in all mortalities. As described for rats, there were no mortalities in the low-dose group. All animals in the high-dose group died before the end of the observation period. Abnormal necropsy findings were not observed in any of the mice that survived for 14 days. The LD5Q dose for male mice was 5,620 mg/kg and for female mice it was 6,550 mg/kg. Since some effects were seen at all dose levels, the LOAEL is 3,160 mg/kg. a. Skin and Eve Irritation A single dose of 2.0 mg/kg IMPA (sodium salt) was applied with an occluded gauze pad to the prepared (hair removed) epidermis of six 16-week-old New Zealand white rabbits for a 24-hour period (Mecler, 1981). An average of 65% of the applied dose was absorbed as determined by pre- and post-dose weighing of the gauze pad. In three rabbits, the epidermal surface was abraded prior to compound administration, and the application site was observed daily for 14 days after testing. The animals were examined daily for gross signs of systemic toxicity. All animals were sacrificed at the end of the 14-day observation period. Erythema was seen in all animals during the 1- to 5-day period after treatment (Mecler, 1981). One animal had hair loss from the mid-dorsal cervical area; another rabbit had a swollen left leg with a discharge. No mortality or signs of systemic toxicity were noted in the rabbits and there were no visible abnormalities noted at necropsy. b. Dermal Sensitization In order to test for dermal sensitivity from IMPA, a 0.1% solution of the sodium salt was injected intradermally in nine female guinea pigs (Mecler, 1981). Ten 0.1 mL injections were given over a 3-week period; 2 weeks later, a 0.1 mL challenge injection was administered. Four guinea pigs were treated VI-2 ------- TABLE VI-1. Mortality in Rats and Mice Exposed to Acute Doses of IMPA(a) Male rats Female rats Male mice Female mice Mortality Dose (mg/kg) Number of Mortalities by Day of death 0(b) 1 2 3 4 5-14 Total Mortality 4,640 6,810 10,000 14,700 0/5(c) 1/5 5/5 5/5 3,160 4,640 6,810 10,000 0/5 1/5 3/5 5/5 3,760 4,640 6,810 10,000 0/5 1/5 4/5 5/5 3,160 4,640 6,810 10,000 0/5 1/5 2/5 5/5 (a) Isopropyl methylphosphonic acid, sodium salt; administered by gavage in distilled water (b) Day of death (c) Number dead/Total number in group VI-3 ------- with 2,4-dinitro-l-chlorobenzene as a positive control. There were no indications of erythema during the sensitization period. A very slight reaction to the challenge was noted during the 24 hours after injection. The response of the exposed animals to IMPA was not significant when compared to the response of the control animals exposed to 2,4-dinitro-1-chlorobenzene (Mecler, 1981) . Ocular irritation was studied by instilling 100 mg IMPA (sodium salt) into one eye each of 6 female New Zealand white rabbits (Mecler, 1981). The eyes of the treated rabbits were examined at intervals of 1, 24, 48, 72, 96 and 168 hours after treatment. No effects of exposure were noted in five of the tested rabbits. One rabbit exhibited congestion and swelling of the iris and redness of the conjunctiva at 24 hours. Isopropyl methylphosphonic acid was judged not to be an eye irritant. 2. Longer-term Exposure Concentrations of 0, 300, 1,000 or 3,000 ppm IMPA (sodium salt) in drinking water were given to groups of 20 male and 20 female Sprague-Dawley rats for a period of 90 days (Mecler, 1981). Based on body weight and fluid consumption data, the male rats were exposed to an average of 0, 25, 92.4 or 278.5 mg/kg/day; the female rats, to doses of 0, 34, 137.4 or 399.1 mg/kg/day. The animals were observed for gross signs of toxicity twice daily. Food and water intake and weight were noted on a weekly basis. Blood samples were analyzed for standard hematological parameters at 4, 8 and 12 weeks, but blood chemistry measurements were determined only at the end of the study. After 90 days the animals were sacrificed. All tissues for the control and 3,000 ppm groups were examined histologically and the weights of key body organs were determined. No statistically significant effects of exposure were noted in this study. There was a slight decrease in the body weight of the 3,000 ppm dose group when compared to the controls; however, the difference was not significant. The decrease in body weight was less than 10% for both the males and females. There is, accordingly, no LOAEL in this study. The NOAEL is based on observations in the 3,000 ppm group. Based on fluid intake and body weights, the NOAEL was 399.1 mg/kg/day for females and 278.5 mg/kg/day for males. 3. Reproductive Effects No information was found in the available literature regarding the repro- ductive effects of IMPA. 4. Developmental Effects No information was found in the available literature regarding the develop- mental effects of IMPA. 5. Mutagenicity Isopropyl methylphosphonic acid had negative mutagenicity results in five strains of Salmonella tvphimurium when tested according to the Ames protocol, VI -4 ------- both with and without microsomal activation (Mecler, 1981). Concentrations 0.5, 1.0, 10, 100, 500, 1,000, 2,500 and 5,000 /ig/plate were tested. There were signs of compound toxicity in some of the tested strains at doses of 2,500 jig/plate or greater. 6. Carcinogenicity No information was found in the available literature regarding the carcinogenic potential of IMPA. VI-5 ------- VII. HEALTH ADVISORY DEVELOPMENT A. Quantification of Toxicological Effects Health Advisories (HAs) are generally determined for one-day, ten-day, longer-term and lifetime exposures if adequate data are available that identify a sensitive noncarcinogenic end point of toxicity. The HAs for noncarcinogenic toxicants are derived using the following formula: HA - where: NOAEL or LOAEL = BW = UF ~ L/day = 1. One-dav Health Advisory There are no appropriate data for calculating a One-day Health Advisory. The available animal data include LD5Q studies for rats and mice as well as testing for dermal and ocular irritation and dermal sensitivity in animals. LD50 data cannot be used, however, for quantification of toxicological effects. Some adverse effects other than death were noted in the LD5Q studies. Both rats and mice experienced loose stools and reduced motor activity. Gross observations of the organs following death or sacrifice revealed some reddening and mottling of the lungs. Fluid was found in the stomach and intestines. The combined observations of fluid in the gastrointestinal (GI) tract and soft liquid stools suggest that body fluids may have been drawn to this body compartment due to the high osmolality of GI contents; thus, these effects are not related directly to the IMPA. The reddening of the lung surface and motor abnormalities, on the other hand, may be directly related to IMPA toxicity. The studies of Little et al. (1986, 1988) indicate that IMPA has an affinity for both lung and brain tissues and will bind to proteins in these tissues. No suitable information was found in the available literature for determining the One-day HA for IMPA. Accordingly, the Longer-term HA of 30 mg/L for a child (calculated below) is recommended for use as a conservative estimate for a one-day exposure. (NOAEL or LOAEL) x (BW) .. . . . _ (UF) x ( L/day) - _ »b/L (rounded to _ „g/L) No- or Lowest-Observed-Adverse-Effect Level in mg/kg bw/day. assumed body weight of a child (10 kg) or an adult (70 kg). uncertainty factor (10, 100, 1,000 or 10,000) in accordance with NAS/EPA guidelines. assumed daily water consumption of a child (1 L/day) or an adult (2 L/day). VII-1 ------- 2. Ten-dav Health Advisory No suitable information was found in the available literature for determining the Ten-day HA for IMPA. The Longer-term HA of 30 mg/L for a child (calcu- lated below) is recommended for use as a conservative estimate for a ten-day exposure. 3. Longer-term Health Advisory The study by Mecler (1981) has been selected to serve as the basis for the Longer-term HA since there are no other appropriate data. This is a 90-day subchronic study of Charles River rats given concentrations of 0, 300, 1,000 or 3,000 ppm IMPA in drinking water. The animals were observed for gross signs of toxicity twice daily. Food and water intake and weight were recorded weekly. Blood samples were analyzed for hematological parameters at 4, 8 and 12 weeks. Blood chemistry measurements were all within the norms for the species. There was a slight (<10%) decrease in the body weight of the 3,000 ppm dose group when compared to the controls. Thus, the 3,000 ppm dose is the NOAEL for this study. Based on water intake and body weight records, the 3,000 ppm concentration is equivalent to a dose of 399.1 mg/kg for the females and 278.5 mg/kg for the males. This study is the only multi-dose data available on IMPA; therefore, it is used to provide a conservative HA estimate for both a child and an adult. The 278.5 mg/kg/day dose for the males is used as the NOAEL in the HA calculation. The Longer-term HA for the 10-kg child is calculated as follows: 27.5 mg/L (: 30.0 mg/L or 30,000 Mg/L) t - u* (278.5 mg/kg/day) (10 kg) Longer-term HA = (100) (1 L/day) = (rounded to where: 278.5 mg/kg/day = NOAEL, based on absence of an effect in male rats exposed to IMPA via drinking water for 90 days. 10 kg = assumed weight of child. 100 = uncertainty factor; this uncertainty factor was chosen in accordance with NAS/EPA guidelines in which a NOAEL from an animal study is employed. 1 L/day = assumed water consumption by a 10-kg child. The Longer-term HA for the 70-kg adult is calculated as follows: Longer-term HA - (278^ ) (70 kg) _ (100) <2 L/day) 1Q() ^ ^ ^ ^ VII - 2 ------- where: 278.5 mg/kg/day = NOAEL, based on absence of an effect in male rats exposed to IMPA via drinking water for 90 days. 70 kg = assumed weight of adult. 100 = uncertainty factor; this uncertainty factor was chosen in accordance with NAS/EPA guidelines in which a NOAEL from an animal study is employed. 2 L/day = assumed water consumption by a 70-kg adult. 4. Lifetime Health Advisory The Lifetime HA represents that portion of an individual's total exposure that is attributed to drinking water and is considered protective of noncarcino- genic adverse health effects over a lifetime exposure. The Lifetime HA is derived in a three-step process. Step 1 determines the Reference Dose (RfD), formerly called the Acceptable Daily Intake (ADI). The RfD is an estimate of a daily exposure to the human population that is likely to be without appre- ciable risk of deleterious effects over a lifetime, and is derived from the NOAEL (or LOAEL), identified from a chronic (or subchronic) study, divided by an uncertainty factor(s). From the RfD, a Drinking Water Equivalent Level (DWEL) can be determined (Step 2). A DWEL is a medium-specific (i.e., drinking water) lifetime exposure level, assuming 100% exposure from that medium, at which adverse, noncarcinogenic health effects would not be expected to occur. The DWEL is derived from the multiplication of the RfD by the assumed body weight of an adult and divided by the assumed daily water consumption of an adult. The Lifetime HA is determined in Step 3 by factoring in other sources of exposure, the relative source contribution (RSC). The RSC from drinking water is based on actual exposure data or, if data are not available, a value of 20% is assumed. If the contaminant is classified as a known, probable or possible carcinogen, according to the Agency's classification scheme of carcinogenic potential (U.S. EPA, 1986), then caution must be exercised in making a decision on how to deal with possible lifetime exposure to this substance. For human (A) or probable human (B) carcinogens, a Lifetime HA is not recommended. For possible human carcinogens (C), an additional 10-fold safety factor is used to calculate the Lifetime HA. The risk manager must balance this assessment of carcinogenic potential and the quality of the data against the likelihood of occurrence and significance of health effects related to noncarcinogenic end points of toxicity. To assist the risk manager in this process, drinking water concentrations associated with estimated excess lifetime cancer risks over the range of 1 in 10,000 to 1 in 1,000,000 for the 70-kg adult drinking 2 L of water/day are provided in the Evaluation of Carcinogenic Potential section. The study by Mecler (1981) has been selected to serve as the basis for the Reference Dose because it is the only candidate study for this calculation. An additional uncertainty factor of 10 is used because the study is a 90-day VII- 3 ------- study. An additional uncertainty factor of 3 is used because of the lack of data on reproductive toxicity and teratogenicity and because of the lack of a study in a second species. However, because IMPA is a metabolite of DIMP (Little et al., 1986; Ivie, 1980; Hart, 1980), the DIMP data base can be used to provide additional data on IMPA. In studies on DIMP conducted in rats, mice, dogs, mink, quail and ducks, for periods ranging from 90 days to 26 weeks, and also in a three-generation reproduction study, DIMP was found to be nontoxic to all species (U.S. EPA, 1989). The EPA concluded that no significant adverse effect was observed in any species. Because DIMP is rapidly and almost completely metabolized to IMPA, it is reasonable to assume that the DIMP administered to mammals in these studies was metabolized to IMPA; therefore, the absence of significant effects from DIMP supports the observation of the absence of effects from IMPA in the Mecler study. Using the Mecler (1981) study, the Lifetime HA is derived as follows: Step 1. Determination of the Reference Dose (RfD) RfD = (278-^mg/kg/day) _ 0 093 mg/kg/day (rounded to 0.1 mg/kg/day or 100 Mg/kg/day) where: 278.5 mg/kg/day = NOAEL, based on absence of an effect in rats exposed to IMPA via drinking water for 90 days. 3,000 = IAW NAS/EPA uncertainty factor. This uncertainty factor includes a factor of 10 for interspecies variation, a factor of 10 for intraspecies variation, and a factor of 10 for use of a less - than-lifetime study. An additional factor of 3 is applied for the lack of reproductive and developmental toxicity studies and lack of a study in a second species. Step 2. Determination of the Drinking Water Equivalent Level (DWEL) 3.5 mg/L (rounded 4 mg/L or 4,000 Mg/L) DUEL - "-1 k8> - 3.5 ng/L (rounded to where: 0.1 mg/kg/day = RfD 70 kg = assumed weight of adult. 2 L/day = assumed water consumption by 70-kg adult. Step 3. Determination of the Lifetime HA Lifetime HA = (3.5 mg/L) (20%) = 0.7 mg/L (700 Mg/L) VII -4 ------- where: 3.5 mg/L = Lifetime HA at 100% contribution from ingestion of drinking water. 20% ¦= Relative source contribution (RSC); percentage of daily exposure contributed by ingestion of drinking water. B. Evaluation of Carcinogenic Potential Applying the criteria described in EPA's guidelines for assessment of carcino- genic risk (U.S. EPA, 1986), IMPA is classified in Group D: Not classifiable as to human carcinogenicity. This category is for agents with inadequate human and animal evidence of carcinogenicity and for those with no available data. VII - 5 ------- VIII. OTHER CRITERIA. GUIDANCE AND STANDARDS In 1984, the U.S. Army Medical Bioengineering Research and Development Laboratory (USAMBRDL) recommended water concentrations for IMPA of 16.75 mg/L for ambient water quality and 16.80 mg/L for drinking water as an interim criteria for the protection of human health (Dacre, 1984). No other guidance or standards were available in the published literature. VIII-1 ------- IX. ANALYTICAL METHODS Analytical techniques that are appropriate for the identification and quantification of IMPA utilize some form of ion exchange or liquid chromatography. Chromatographic procedures are sometimes combined with mass spectrometry or some other suitable technique to facilitate the identification of the specific phosphonic acid present. The techniques discussed in the following paragraphs apply to several methylphosphonic acids including isopropyl methylphosphonic acid. Schiff et al. (1977) developed a method using a Dionex Model 14 Ion Chromato- graph for the separation and analysis of phosphonic acids. Both 3 x 150 mm and 3 x 500 mm column sizes were used. Columns were connected in series. Eluents were varied depending on the specific phosphonic acid to be eluted. A 0.005 M borate eluent and flow rate of 138 mL/hr with a 650 mm total column length provided effective separation of isopropyl methylphosphonic acid from other phosphonates and competing inorganic anions. A detection limit of 0.1 mg/L was achieved. The most effective separation of methyl phosphonic acid in the presence of chloride ion was achieved with 0.01 M sodium hydroxide, a flow rate of 322 mL/hr and a 500 mm column length (Schiff et al., 1977). The detection limit under these conditions was 1.26 mg/L. Alternatively, methyl phosphonic acid separation could be achieved on a 650 mm column with a bicarbonate/ carbonate eluent (0.0024 M/0.0018 M) and a flow rate of 138 mL/hr. Although the separation from chloride achieved was not as effective as that with the sodium hydroxide, the detection limit of 0.1 mg/L for methyl phosphonic acid was superior. The major difficulty encountered in separating the alkyl phosphonic acids from a medium that contains several members of this class of compounds using the ion exchange chromatography method, is the similarity in the charges of the anions. The various alkyl phosphonic acids have very similar pK0s and, therefore, similar net ionic charges. Detection of the individual phosphonic acids in the eluent is also difficult since, lacking a chromophore, the individual compounds cannot be detected using a UV or fluorescent detector (Bossle et al., 1983). Esterification of the alkyl methylphosphonic acids with para-bromophenacyl bromide (PBPB) has been proposed by Bossle et al. (1983) as a method for the separation and quantification of alkyl phosphonates. After adding the chromophore to the molecule, the modified methylphosphonic acids are separated by high pressure liquid chromatography (HPLC). Using this technique, Bossle et al. (1983) were able to separate ethyl, isopropyl, and phenacetyl methylphosphonic acid and quantify the concentrations of these phosphonic acids. The detection limits achieved with the ethyl, isopropyl, and phenacetyl methylphosphonic acids were 43, 59 and 62 ng, respectively. According to the Bossle et al. (1983) approach, the alkyl methylphosphonic acids were first esterified with PBPB, 18-crown-6 catalyst, and potassium bicarbonate in dry acetonitrile. The reaction product was sealed in a WISP sample vial and applied to a 30 x 0.4 cm I.D. Bondapak C18 column for reverse IX-1 ------- phase HPLC. Clear separation of the three alkyl methylphosphonic acids was achieved. There was also a clear separation of the methylphosphonic acids from excess PBPB reagent. Retention times for the methylphosphonic acids were propor- tional to the size and lipophilicity of the alkyl side chains. Wils and Hulst (1988) evaluated a different approach for the separation of organophosphonic acids. Ion pairs of the phosphonic acids with ammonium acetate or one of three tetraalkylammonium salts (methyl, ethyl, n-butyl) were established. These ion pairs were then separated by liquid chromatography (LC) on a Sep-Pac C18 column using methanol/water as an eluent. The column was connected to a thermospray (TSP) interphase prior to analysis of the eluent by a mass spectrometer with a TSP ion source. Although this approach showed potential as an analytical technique for a wide variety of phosphonic acids, a number of procedural difficulties were encountered. The experimental conditions which favored effective separation of the short chain alkyl phosphonates were not as effective for the longer chain alkyl derivatives and vice versa. The method was not useful for separation and identification of the diprotic methylphosphonic acid (MPA) which is formed when isopropyl methylphosphonic acid degrades. The creation of an ion pair between an alkyl methylphosphonic acid and an ammonium compound is the first step in an additional analytical method which can be used for isopropyl methylphosphonic acid and other alkyl phosphonic acids (Tornes and Johnson, 1989). Samples of alkyl methylphosphonic acids (10-100 mL) were separated on a column containing 100 mg of an aminopropyl ion exchanger. The column was eluted with 300 pL of 0.1 M trimethylphenylammonium hydroxide (TMPAH) in methanol. The eluent from the column was injected into a Packard Model 438 gas chromatograph coupled to an LKB 2091 mass spectrometer. The injector port temperature was set at 300°C so that the alkyl methyl- phosphonate would react with the TMPAH. In this reaction the acid functional group was methylated, producing a volatile ester. The Tornes and Johnson (1989) method was developed specifically for the identification of the alkyl methylphosphonic acids produced during the degradation of the nerve agents Sarin and Soman. The TMPAH modification approach for identifying isopropyl methylphosphonic acid from Sarin was evaluated by Tornes and Johnson (1989) under field conditions. Sarin (1 mg) was first added to 5 mL samples of water or 10 g samples of sand, soil or grass. All samples were held for 1 to 4 weeks under the ambient temperature and humidity conditions. Prior to analysis, the sand, soil and grass samples were extracted by shaking with 50 mL water for 1 minute and filtered to obtain the supernatant. The dissolved, unreacted (nonionic) Sarin was separated from isopropyl methylphosphonic acid by passing the supernatant through a C18 column prior to use of the aminopropyl ion exchange column. Sarin was identified in all the 1- and 2-week samples and in the 4-week water sample. Isopropyl methyl- phosphonic acid was quantitatively identified in all samples except the 4-week soil sample. The Tornes and Johnson (1989) method can be used in the field as a method for verifying Sarin use, even several weeks after the initial release of the nerve gas into the environment. Based on their field studies, the authors suggested that reversing the arrangement of the C18 and ion exchange IX-2 ------- columns so that the C18 column follows rather than precedes the ion exchange column may improve the recovery of the degradation products from parent nerve gas. There can be some retention of the degradation products by the C18 column. IX-3 ------- X. TREATMENT TECHNOLOGIES Mill and Gould (1979) reported that hydrogen peroxide (H202) combined with oxygen and ultraviolet light degrades IMPA in aqueous solution. At pH 9, a 1 M solution of IMPA as its sodium salt was combined with 3.0 M hydrogen peroxide and 2.11 mmol of oxygen and irradiated with 300 nm light for 2 hours at 25°C. At the end of 2 hours, irradiation was terminated for analysis of intermediary oxidation products and then resumed with the addition of 3.0 M hydrogen peroxide for another 2-hour period of irradiation. The reaction cycle was then repeated with additional 3.0 M peroxide for a final 2-hour irradiation period. Analysis of the final solution after three 2-hour treatments with 3 M hydrogen peroxide, oxygen and irradiation indicated that IMPA had been converted to acetic acid (0.13 M), carbon dioxide (0.36 mmol), and phosphoric acid (Mill and Gould, 1979). A small amount (0.07 mmol) of methyl phosphonate was also detected. In the initial steps of the reaction, the isopropyl functional group was converted to acetone and acetic acid while the methylphosphonate group remained intact. Oxidation of the methylphosphonate continued during the second and third oxidation periods. Further oxidation of the acetone reduced it to carbon dioxide and acetic acid. Some carbon monoxide was formed as a transient intermediate. These data indicate that IMPA can be degraded by oxidation using peroxide and oxygen as oxidizing agents under ultraviolet light. Elevated temperatures are not needed for the reaction. Oxidation of isopropyl methylphosphonic acid to acetic acid, carbon dioxide and phosphoric acid requires vigorous conditions of oxidation (9 M H202/1 M IMPA; 6-hour irradiation). Less vigorous oxidation (3 M H202/1 M IMPA; 2-hour irradiation) resulted in minimal oxidation of the carbon-phosphorus bond, producing methyl phosphonic acid as a product of the reaction. The isopropyl moiety of isopropyl methylphosphonic acid was oxidized to acetone and acetic acid. Accordingly, oxidation of water containing isopropyl methylphosphonic acid using oxygen, hydrogen peroxide, and ultraviolet light is a potential treatment option. Careful control of reaction conditions is important if carbon dioxide and acetic acid are the desired end products and the use of expensive oxidant is minimized. The solutions which were irradiated in the study of Mill and Gould (1979) were initially at pH 9. The influence of pH on the reaction was not determined. However, the use of other pH solutions could influence the rate of reaction. Data reported by Schiff et al. (1977) on the oxidation of DIMP by ozone and ultraviolet light indicate that DIMP is first converted to IMPA which is then oxidized to acetate, formate, and MPA. Only small amounts of MPA were converted to free phosphate ion. A 3-hour reaction time was employed; the other reaction conditions were not specified. These results, however, are in general agreement with those of Mill and Gould (1979) and indicate that oxidation of the carbon-phosphorus bond in MPA is difficult to achieve. No additional information has been located in the literature on the use of specific treatment technologies for the removal of IMPA from potable water. X-l ------- Since this compound is not volatile, it would not be amenable to aeration. Based on the low pK of the acid functional group, it should be amenable to removal by ion exchange chromatography. Ion exchange processes are used as analytical methods for IMPA (Bossle et al., 1979; Schiff et al., 1977). Competition from other negative ions including the inorganic chloride and fluoride ions can interfere with the ion exchange process (Bossle et al. , 1979). X- 2 ------- XI. CONCLUSIONS AND RECOMMENDATIONS Based on the available animal toxicity data, the HA for one-day, ten-day, and longer-term exposures for a child is 30 mg/L. The Longer-term HA for the adult is 100 mg/L and the Lifetime HA is 0.7 mg/L (700 Mg/L). These values are considered protective against toxic effects for the most sensitive members of the population. Currently, data are insufficient to assess the carcinogenic risk for IMPA. Isopropyl methylphosphonic acid is classified in Group D: Not classifiable as to human carcinogenicity. A companion report, "Data Deficiencies/Problem Areas and Recommendations for Additional Data Base Development for Isopropyl Methylphosphonic Acid" (Appendix 1), summarizes the scope of existing data reviewed for this Health Advisory. Recommendations are made for additional studies to assess the lifetime toxicity, reproductive, teratological and carcinogenic risk, if any, of isopropyl methylphosphonic acid. XI-1 ------- XII. REFERENCES Alexander, M., A.M. Cook and C.G. Daughton (Cornell University). 1977. Induction of microbial metabolism of organophosphorus compounds. Contractor Report ARCSL-CR-78013. Aberdeen Proving Ground, MD: U.S. Army Armament Research and Development Command, Chemical Systems Laboratory. Beilstein Database. 1979. Data record for isopropyl methylphosphonic acid. Scientific and Technical Information Network, Handbook of Organic Chemistry. New York, NY. May 11, 1992. Bossle, P.C., J.J. Martin, E.W. Sarver and H.Z. Sommer. 1983. High- performance liquid chromatography analysis of alkyl methylphosphonic acids by derivatization. J. Chromatogr. 267:209-212. Cook, A.M., C.G. Daughton and M. Alexander. 1978. Phosphonate utilization by bacteria. J. Bacteriol. 133(1):85-89. Dacre, J.C. 1984. Recommended interim criteria for three environmental polluting compounds of Rocky Mountain Arsenal. Technical Report 8302. Frederick, MD: U.S. Army Medical Bioengineering Research and Development Laboratory, Ft. Detrick. Available from NTIS, Alexandria, VA. Order No. ADA 154826. Daughton, C.G., A.M. Cook and M. Alexander. 1979a. Biodegradation of phosphonate toxicants yields methane or ethane on cleavage of the C-P bond. FEMS Microbiology Letters 5:91-93. Daughton, C.G., A.M. Cook and M. Alexander. 1979b. Phosphate and soil binding: Factors limiting bacterial degradation of ionic phosphorus- containing pesticide metabolites. Appl. Environ. Microbiol. 37(3):605-609. Fleisher, J.H., L.W. Harris, D.M. Murray and L.M. Braswell. 1964. Dealkyl- ation as a mechanism for aging of rat-brain cholinesterase in vivo following poisoning with GD or GB. Technical Report CRDLR 3243. Edgewood Arsenal, MD: U.S. Army Edgewood Arsenal, Chemical Research and Development Laboratories. Hart, E.R. 1980. Mammalian toxicology study of DIMP and DCPD. (Phase 2). Kensington, MD: Litton Bionetics, Inc. Available from NTIS, Alexandria, VA. Order No. AD-A058-323. Hoskin, F.C.G. 1956. Some observations concerning the biochemical inertness of methyl phosphonic and isopropyl methylphosphonic acids. Can. J. Biochem. Physiol. 34:743-746. Howells, D.J., J.L. Hambrook, D. Utley and J. Inoodage. 1973. Degradation of phosphonates II: The influence of the 0-alkyl group on the breakdown of some 0-alkyl methylphosphonofluoridates in wheat plants. Pestic. Sci. 4:239-245. Howells, D.J., J.L. Hambrook and E.A. Allenby. 1976. Uptake of some volatile alkyl methylphosphonofluoridates from the vapor phase by wheat plants. Pestic. Sci. 7:349-354. XII-1 ------- Ivie, G.W. 1980. Fate of diisopropyl methylphosphonate (DIMP) in a lactating cow. Bull. Environ. Contam. Toxicol. 24:40-48. Little, P.J., M.L. Reynolds, E.R. Bowman and B.R. Martin. 1986. Tissue disposition of [3H]Sarin and its metabolites in mice. Toxicol. Appl. Pharmacol. 83:412-419. Little, P.J., J.A. Scimeca and B.R. Martin. 1988. Distribution of [3H] diisopropylfluorophosphate, [3H]Soman, [3H]Sarin, and their metabolites in mouse brain. Drug Metab. Dispos. 16(4):515-520. Mecler, F.J. and J.C. Dacre. 1982. Toxicological assessment of isopropyl methylphosphonic acid. The Toxicologist 2(1):35. Mecler, F.J. 1981. Mammalian toxicological evaluation of DIMP and DCPD (Phase 3-IMPA). Final Report. Litton Bionetics, Inc., Contract No. DAMD 17-77-C-7003. Frederick, MD: U.S. Army Medical Research and Development Command, Ft. Detrick. Mill, T. and C.W. Gould. 1979. Free-radical oxidation of organic phosphonic acid salts in water using hydrogen peroxide, oxygen and ultraviolet light. Environ. Sci. Technol. 13(2):205-208. PMRMA. 1991a. Program Manager for Rocky Mountain Arsenal. Contract No. DAAA 15-87-0095. Annual groundwater report for 1990. Final report. Version 1.1. Commerce City, CO: U.S. Army Program Manager for Rocky Mountain Arsenal. PMRMA. 1991b. Program Manager for Rocky Mountain Arsenal. Comprehensive monitoring program. Army complex disposal trenches reevaluation report (first year), August 1991. Contract No. DAAA 15-88-D-0022. Commerce City, CO: U.S. Army Program Manager for Rocky Mountain Arsenal. Robson, S.G. 1981. Computer simulation of movement of DIMP-contaminated groundwater near the Rocky Mountain Arsenal, Colorado. Permeability and groundwater contaminant transport. ASTM Special Technical Publication No. 746, pp. 209-220. Rosenblatt, D.H., T.A. Miller, J.C. Dacre, I. Muul and D.R. Cogley. 1975a. Problem definition studies on potential environmental pollutants I: Toxi- cology and ecological hazards of 16 substances at Rocky Mountain Arsenal. Technical Report 7508. Frederick, MD: U.S. Army Medical Bioengineering Research and Development Laboratory, Fort Detrick. Available from NTIS, Alexandria, VA. Order No. ADB039661L. Rosenblatt, D.H., I. Muul, T.A. Miller, D.R. Cogley and J.C. Dacre. 1975b. Problem definition studies on potential environmental pollutants II: Physical, chemical, toxicological and biological properties of 16 substances. Technical Report 7509. Frederick, MD: U.S. Army Medical Bioengineering Research and Development Laboratory, Fort Detrick. Available from NTIS, Alexandria, VA. Order No. ADA030428. XII - 2 ------- Schiff, L.J., S.G. Pleva and E.W. Sarver. 1977. Analysis of phosphonic acids by ion chromatography. Mulik, J.D. and E. Sawicki, eds. Ion chromatographic analyses of environmental pollutants. Ann Arbor, MI: Ann Arbor Science Publishers, Inc., pp. 329-344. Tornes, J.A. and B.A. Johnson. 1989. Gas chromatographic determination of methylphosphonic acids by methylation with trimethylphenylammonium hydroxide. J. Chromatogr. 467:129-138. U.S. EPA. 1986. U.S. Environmental Protection Agency. Guidelines for carcinogen risk assessment. Fed. Reg. 51(185):33992-34003. September 24. U.S. EPA. 1989. U.S. Environmental Protection Agency. Health advisory on diisopropyl methylphosphonic acid (DIMP). Washington, DC: U.S. EPA, Office of Water. Available from NTIS, Alexandria, VA. Order No. P1390273517. Wils, E.R.J, and A.G. Hulst. 1988. Determination of organophosphorus acids by thermospray liquid chromatography-mass spectrometry. J. Chromatogr. 454:261-272. XII - 3 ------- APPENDIX I Data Deficiencies/Problem Areas and Recommendations for Additional Data Base Development for Isopropyl Methylphosphonic Acid ------- r INTRODUCTION The U.S. Environmental Protection Agency, Office of Water (U.S. EPA/OW), in conjunction with the Department of the Army (DA), has reviewed the available data on isopropyl methylphosphonic acid (IMPA) for the purpose of developing a Health Advisory (HA) for this compound. The Health Advisory is designed to provide data that are useful in selecting options for dealing with the contamination of drinking water. The Health Advisory includes "state-of-the- art" information on environmental fate, health effects, analytical methodology and treatment options associated with IMPA. OBJECTIVES The objective of this appendix is to provide an evaluation of the data deficiencies and/or problem areas encountered in the review process for IMPA, and to make recommendations for additional data base development. An indepen- dent analysis of the current status of IMPA technology, as it relates to IMPA's possible presence in drinking water, is presented. This appendix also includes a summary of the background information used in the development of the HA. For greater detail on the toxicology of IMPA, the Health Advisory on IMPA should be consulted. BACKGROUND Isopropyl methylphosphonic acid is a strong acid which is formed during degradation of the nerve gas, isopropyl methylphosphonofluoridate (Sarin). Isopropyl methylphosphonic acid is soluble in water and is present in groundwater in the vicinity of the site of Sarin production near Denver, Colorado (Rosenblatt et al., 1975a). Isopropyl methylphosphonic acid is a chemically stable molecule. In the chemical decomposition of IMPA, hydrolysis of the ester bond produces methylphosphonic acid (MPA) and isopropyl alcohol. The rate of abiotic IMPA hydrolysis is slow, resulting in environmental persistence (Rosenblatt et al., 1975b). One strain of bacterium found in sewage, Pseudomonas testosteroni. is able to aerobically degrade IMPA, releasing methane, isopropyl alcohol, and phosphoric acid or phosphorous (Alexander et al., 1977). Isopropyl methylphosphonic acid found in either ground or surface waters is expected to have a relatively long half-life (1,900 years). Isopropyl methylphosphonic acid is nonvolatile due to the polarity of the nonionized molecule and its ionic state under most pH conditions. Therefore, IMPA is not found as an atmospheric contaminant even in situations where it occurs free in the environment. Most of the data on the pharmacokinetics of IMPA are the result of studies of the tissue distribution of Sarin. Sarin appears to be rapidly degraded to IMPA by a serum enzyme (Hoskin, 1956). Subsequent de-esterification of IMPA to produce MPA is minimal. Thus, IMPA is the principal metabolite of Sarin. Distribution studies of tritium-labeled Sarin indicate that IMPA concentrates in the kidney, lungs, liver and brain (Little et al., 1986). A portion of the IMPA in all tissues becomes bound to cellular proteins. The concentration of the bound IMPA increases with time (Little et al., 1986). Isopropyl Al -1 ------- methylphosphonic acid appears to be excreted without metabolic alteration. In studies of the pharmacokinetics of P32-labeled IMPA, Hoskin (1956) found that IMPA was the only labeled material that could be identified in the urine. Data on the toxicity of IMPA are limited. Oral exposure data are available from LDj0 studies in the mouse and rat and from a subchronic study in the rat. The dermal and ocular toxicity and the dermal sensitizing effects of IMPA have also been tested. There are no studies of the reproductive, teratogenic or carcinogenic properties of this compound. All of the available data have been produced from studies in animals; there are no data available which apply to human exposures. The LD50 values for IMPA in male mice and rats are 5,620 mg/kg and 7,650 mg/kg, respectively (Mecler, 1981). The values for female mice and rats are 6,550 mg/kg and 6,070 mg/kg, respectively. In each of these LD50 studies, the compound was administered orally as a single dose (ranging from 3,160 mg/kg to 114,700 mg/kg). The animals were observed for a period of 14 days following dosing; during this period both the mice and rats demonstrated reduced motor activity and ataxia even at the lowest doses. Loose stools also were seen in all animals. Postmortem examinations of the treated animals revealed reddening of the lungs in both the mice and rats. In addition, there were dark spots on the thymus in the rats. Fluid was found in the stomach and intestines of the treated animals. A single dose of 20 mg/kg sodium isopropyl methylphosphonic acid, applied to either the intact or abraded dermal tissue of New Zealand white rabbits, caused erythema in all exposed animals (Mecler, 1981). Studies of the ability of IMPA to act as a sensitizing agent in female guinea pigs were negative (Mecler, 1981). In tests of ocular irritation, only one of five tested rabbits exhibited a response to 100 mg of IMPA instilled into the eyes (Mecler, 1981). When IMPA was administered orally to Sprague-Dawley rats for a period of 90 days, a nonsignificant decrease in the body weights of the high-dose animals was the only noted effect of exposure (Mecler, 1981). Doses of 0, 300, 1,000 or 3,000 ppm were administered in drinking water. Food and fluid consumption, body weight, hematological and blood chemistry parameters were measured as indices of toxicity. The observed decrease in the weights of the high-dose animals was less than 10% for both sexes. Thus, based on magnitude of change and significance criteria, the observed weight loss cannot be regarded as an adverse effect. The animals were sacrificed at the end of the study and the tissues were examined histologically; key organ weights also were recorded. No tissue abnormalities were noted and the organ:body weight ratios were not affected by exposure to IMPA. The 3,000 ppm dose is, accordingly, a NOAEL. Based on body weight data and fluid consumption records, this 3,000 ppm exposure is equivalent to a dose of 399.1 mg/kg for the females and 278.5 mg/kg for the males. Al-2 ------- There have been no animal studies that focus on determining the carcino- genicity of IMPA. The mutagenic potential of this compound has been evaluated through the Ames assay (Mecler, 1981). The results of exposing five strains of S. tvphimurium to concentrations of 0.5 to 5,000 Mg/plate indicate that IMPA is not mutagenic. Doses of 2,500 and 5,000 /zg/plate were toxic to some of the S. tvphimurium strains. Based on the existing data, the HA value for one-day, ten-day, or longer-term exposures for the 10-kg child is 30 mg/L. The longer-term exposure HA value for the 70-kg adult was 100 mg/L. In the absence of a lifetime study, subchronic data were used to calculate a lifetime HA in order to provide a conservative estimate of a no-effect- human-exposure level. Additional safety factors were used in calculating the lifetime HA value to accommodate the less-than-chronic exposure duration of the subchronic study, the lack of reproductive and teratogenicity data for IMPA, and the fact that there is only one study of multiple-dose exposures to IMPA. The resultant HA value is 0.7 mg/L (700 /zg/L) . There are several methods available for identifying and quantifying the concentration of IMPA in solution (Bossle et al., 1983; Schiff et al., 1977; Tornes and Johnson, 1989; Wils and Hulst, 1988). Each of the available methods uses either ion exchange or reverse phase liquid chromatography as the initial separation technique. Prior modification of IMPA with a chromophore or a detectable ion pair can be used to simplify the identification of this compound after separation. Both mass spectrometry and gas chromatography are useful as identification techniques. Although no studies on ion exchange as a treatment technique were identified in the literature, this method has the potential to be useful for the removal of IMPA from contaminated water based on the data provided in the analytical studies by Schiff et al. (1977). Oxidation with either ozone or hydrogen peroxide under ultraviolet light has been tested under laboratory conditions as a treatment technique for IMPA-contaminated water (Mill and Gould, 1979; Schiff et al., 1977). However, reaction conditions must be carefully controlled to allow for the complete decomposition of the IMPA to phosphate, carbon dioxide and acetic acid. Methyl phosphonic acid and acetone are produced as intermediates in the oxidation process and will be present in the treated water under conditions where oxidation is incomplete. The decompo- sition of the MPA under laboratory conditions requires the maintenance of an oxidative environment for several hours. It is the most stable intermediate in the oxidation reaction. DISCUSSION The pharmacokinetic data from intravenous administration of Sarin provide considerable information concerning the distribution and excretion of IMPA in the body. A study of the tissue distribution of IMPA when exposure occurs through the oral route, would demonstrate the effect of route on the toxicokinetics of the compound. A more detailed evaluation of the types of interactions that influence the protein binding properties of IMPA and identification of target proteins would be useful in evaluating the potential Al-3 ------- for this compound to produce functional impairment of either cellular transport or metabolism following long-term exposure. The occurrence of tissue protein binding suggests that a long-term chronic study of 1MPA should be done. Either the LD50 data or a repeated subchronic study using higher doses than those in the existing study should be used for selecting the doses for a chronic study. The selection of parameters to be monitored should be based on data from the protein binding studies. For example, the protein binding data might suggest that specific enzymes be evaluated in the toxicity screening. The fact that IMPA bonds to the brain tissue and the impact of this compound on motor activity in the LD5Q studies suggest that neurological toxicity end points should be evaluated in a chronic study. The protein binding characteristics of IMPA also suggest that this compound might have an impact on reproductive processes. At minimum, a two-generation oral exposure study that includes teratogenic end points should be conducted. CONCLUSIONS/RECOMMENDATIONS Based on the preceding discussion, the following conclusions/recommendations can be made: • The HA values that have been calculated are conservative estimates for humans. No studies or effects in humans were found in the available literature; the data are limited to acute and subchronic exposure studies in animals. Uncertainty factors were used in the calculations because there are no studies of sufficient duration that identify specific health effects resulting from exposures to IMPA and there are no data on the effects of this compound on the reproductive processes. • The protein binding properties of IMPA should be studied to delineate the mechanism of protein binding and target proteins. Information on target proteins should be used to select the end points that will be monitored during classical exposure studies. • A chronic study of oral exposures to IMPA should be conducted and should include tumorigenic end points in the evaluation criteria. Neurological and enzymatic end points also should be considered for monitoring in addition to the routine indices of chronic toxicity. A battery of genotoxicity tests should be conducted prior to a cancer assay. • A two-generation reproductive study that incorporates teratogenicity end points is recommended to evaluate the impact of IMPA on reproductive performance. No other studies of adverse health effects from exposure to IMPA, relative to potable water, are recommended at this time. Al-4 ------- REFERENCES Alexander, M., A.M. Cook and C.C. Daughton (Cornell University). 1977. Induction of microbial metabolism of organophosphorus compounds. Report No. ARCSL-CR-78013. Aberdeen Proving Ground, MD: U.S. Army Armament Research and Development Command, Chemical Systems Laboratory. Bossle, P.C., J.J. Martin, E.W. Sarver and H.Z. Sommer. 1983. High- performance liquid chromatography analysis of alkyl methylphosphonic acids by derivatization. J. Chromatogr. 267:209-212. Hoskin, F.C.C. 1956. Some observations concerning the biochemical inertness of methyl phosphonic and isopropyl methylphosphonic acids. Can. J. Biochem. Physiol. 34:743-746. Little, P.J., M.L. Reynolds, E.R. Bowman and B.R. Martin. 1986. Tissue disposition of [3H]diisopropylfluorophosphate, [3H]Soman, [3H]Sarin and their metabolites in mouse brain. Drug Metab. Dispos. 16(4):515-520. Mecler, F.J. 1981. Mammalian toxicological evaluation of DIMP and DCPD (Phase 3-IMPA). Final Report. Litton Bionetics, Inc., Contract No. DAMD 17-77-C-7003. Frederick, MD: U.S. Army Medical Research and Development Command, Ft. Detrick. Mill, T. and C.W. Gould. 1979. Free-radical oxidation of organic phosphonic acid salts in water using hydrogen peroxide, oxygen and ultraviolet light. Environ. Sci. Technol. 13(2):205-208. Rosenblatt, D.H., T.A. Miller, J.C. Dacre, I. Muul and D.R. Cogley. 1975a. Problem definition studies on potential environmental pollutants I: Toxicology and ecological hazards of 16 substances at Rocky Mountain Arsenal. Technical Report 7508. Frederick, MD: U. S. Army Medical Bioengineering Research and Development Laboratory, Fort Detrick. Available from NTIS, Alexandria, VA. Order No. ADB039661L. Schiff, L.J., S.C. Pleva and E.W. Sarver. 1977. Analysis of phosphonic acids by ion chromatography. Mulik, J.D. and E. Sawicki, eds. Ion chromatographic analyses of environmental pollutants. Ann Arbor, MI: Ann Arbor Science Publishers, Inc., pp. 329-344. Tornes, J.A. and B.A. Johnson. 1989. Gas chromatographic determination of methylphosphonic acids by methylation with trimethylphenylammonium hydroxide. J. Chromatogr. 467:129-138. Wils, E.R.J, and A.C. Hulst. 1988. Determination of organophosphorus acids by thermospray liquid chromatography-mass spectrometry. J. Chromatogr. 454:261-272. Al-5 ------- |