United States Environmental Protection 1=1 m m Agency EPA/690/R-07/01 OF Final 8-13-2007 Provisional Peer Reviewed Toxicity Values for p,p '-Dichlorodiphenyldichloroethane (p,p '-DDD) (CASRN 72-54-8) Superfund Health Risk Technical Support Center National Center for Environmental Assessment Office of Research and Development U.S. Environmental Protection Agency Cincinnati, OH 45268 ------- Acronyms and Abbreviations bw body weight cc cubic centimeters CD Caesarean Delivered CERCLA Comprehensive Environmental Response, Compensation and Liability Act of 1980 CNS central nervous system cu.m cubic meter DWEL Drinking Water Equivalent Level FEL frank-effect level FIFRA Federal Insecticide, Fungicide, and Rodenticide Act g grams GI gastrointestinal HEC human equivalent concentration Hgb hemoglobin i.m. intramuscular i.p. intraperitoneal IRIS Integrated Risk Information System IUR inhalation unit risk i.v. intravenous kg kilogram L liter LEL lowest-effect level LOAEL lowest-observed-adverse-effect level LOAEL(ADJ) LOAEL adjusted to continuous exposure duration LOAEL(HEC) LOAEL adjusted for dosimetric differences across species to a human m meter MCL maximum contaminant level MCLG maximum contaminant level goal MF modifying factor mg milligram mg/kg milligrams per kilogram mg/L milligrams per liter MRL minimal risk level MTD maximum tolerated dose MTL median threshold limit NAAQS National Ambient Air Quality Standards NOAEL no-ob served-adverse-effect level NOAEL(ADJ) NOAEL adjusted to continuous exposure duration NOAEL(HEC) NOAEL adjusted for dosimetric differences across species to a human NOEL no-ob served-effect level OSF oral slope factor p-IUR provisional inhalation unit risk p-OSF provisional oral slope factor p-RfC provisional inhalation reference concentration p-RfD provisional oral reference dose 1 ------- PBPK physiologically based pharmacokinetic ppb parts per billion ppm parts per million PPRTV Provisional Peer Reviewed Toxicity Value RBC red blood cell(s) RCRA Resource Conservation and Recovery Act RDDR Regional deposited dose ratio (for the indicated lung region) REL relative exposure level RfC inhalation reference concentration RfD oral reference dose RGDR Regional gas dose ratio (for the indicated lung region) s.c. subcutaneous SCE sister chromatid exchange SDWA Safe Drinking Water Act sq.cm. square centimeters TSCA Toxic Substances Control Act UF uncertainty factor Hg microgram |j,mol micromoles voc volatile organic compound 11 ------- 8-13-2007 PROVISIONAL TOXICITY VALUES FOR p,p '-DICHLORODIPHENYLDICHLOROETHANE 1)I)I)) (CASRN 72-54-8) Background On December 5, 2003, the U.S. Environmental Protection Agency's (EPA's) Office of Superfund Remediation and Technology Innovation (OSRTI) revised its hierarchy of human health toxicity values for Superfund risk assessments, establishing the following three tiers as the new hierarchy: 1. EPA's Integrated Risk Information System (IRIS). 2. Provisional Peer-Reviewed Toxicity Values (PPRTV) used in EPA's Superfund Program. 3. Other (peer-reviewed) toxicity values, including: ~ Minimal Risk Levels produced by the Agency for Toxic Substances and Disease Registry (ATSDR), ~ California Environmental Protection Agency (CalEPA) values, and ~ EPA Health Effects Assessment Summary Table (HEAST) values. A PPRTV is defined as a toxicity value derived for use in the Superfund Program when such a value is not available in EPA's Integrated Risk Information System (IRIS). PPRTVs are developed according to a Standard Operating Procedure (SOP) and are derived after a review of the relevant scientific literature using the same methods, sources of data, and Agency guidance for value derivation generally used by the EPA IRIS Program. All provisional toxicity values receive internal review by two EPA scientists and external peer review by three independently selected scientific experts. PPRTVs differ from IRIS values in that PPRTVs do not receive the multi-program consensus review provided for IRIS values. This is because IRIS values are generally intended to be used in all EPA programs, while PPRTVs are developed specifically for the Superfund Program. Because new information becomes available and scientific methods improve over time, PPRTVs are reviewed on a five-year basis and updated into the active database. Once an IRIS value for a specific chemical becomes available for Agency review, the analogous PPRTV for that same chemical is retired. It should also be noted that some PPRTV manuscripts conclude that a PPRTV cannot be derived based on inadequate data. Disclaimers Users of this document should first check to see if any IRIS values exist for the chemical of concern before proceeding to use a PPRTV. If no IRIS value is available, staff in the regional Superfund and RCRA program offices are advised to carefully review the information provided in this document to ensure that the PPRTVs used are appropriate for the types of exposures and 1 ------- 8-13-2007 circumstances at the Superfund site or RCRA facility in question. PPRTVs are periodically updated; therefore, users should ensure that the values contained in the PPRTV are current at the time of use. It is important to remember that a provisional value alone tells very little about the adverse effects of a chemical or the quality of evidence on which the value is based. Therefore, users are strongly encouraged to read the entire PPRTV manuscript and understand the strengths and limitations of the derived provisional values. PPRTVs are developed by the EPA Office of Research and Development's National Center for Environmental Assessment, Superfund Health Risk Technical Support Center for OSRTI. Other EPA programs or external parties who may choose of their own initiative to use these PPRTVs are advised that Superfund resources will not generally be used to respond to challenges of PPRTVs used in a context outside of the Superfund Program. Questions Regarding PPRTVs Questions regarding the contents of the PPRTVs and their appropriate use (e.g., on chemicals not covered, or whether chemicals have pending IRIS toxicity values) may be directed to the EPA Office of Research and Development's National Center for Environmental Assessment, Superfund Health Risk Technical Support Center (513-569-7300), or OSRTI. INTRODUCTION No verified chronic reference dose (RfD) or reference concentration (RfC) forp,p '- dichlorodiphenyldichloroethane (p,p '-DDD) is available on the U.S. Environmental Protection Agency's (EPA) Integrated Risk Information System (IRIS) (U.S. EPA, 2007), Drinking Water Standards and Health Advisories list (U.S. EPA, 2006) or Health Effects Assessment Summary Tables (HEAST) (U.S. EPA, 1997). The U.S. EPA's Chemical Assessments and Related Activities (CARA) list (U.S. EPA, 1991, 1994) does not indicate any documents relating to the noncancer health effects ofp,p '-DDD. The Agency for Toxic Substances Disease and Registry (ATSDR, 2002) prepared a toxicological profile for dichlorodiphenyltrichloroethane (DDT), dichlorodiphenyldichloroethylene (DDE) and DDD. ATSDR did not develop any Minimal Risk Levels (MRLs) forp,p '-DDD, but no explanation was provided. The American Conference of Governmental Industrial Hygienist (ACGIH, 2006), Occupational Safety and Health Administration (OSHA, 2006) and National Institute for Occupational Safety and Health (NIOSH, 2006) have not adopted occupational exposure limits forp,p '-DDD. A NIOSH Special Occupational Hazard Review document, two International Agency for Research on Cancer monographs (IARC, 1974, 1991), the National Toxicology Program status report (NTP, 2006) and two World Health Organization documents (WHO, 1979, 1989) were consulted for relevant information. A cancer weight-of-evidence classification and an oral slope factor for p,p '-DDD are available on IRIS (U.S. EPA, 2007). The cancer assessment, verified in 1988, classifiesp,p '- DDD in category B2 (probable human carcinogen) under U.S. EPA (1986) Guidelines for Carcinogen Assessment, based on lung tumors in female mice, lung and liver tumors in male 2 ------- 8-13-2007 mice, and thyroid tumors in male rats after dietary exposure. IRIS (U.S. EPA, 2007) reports an oral slope factor of 0.24 per mg/kg-day, and drinking water unit risk of 6.9 E-6 per |ig/L, based on liver tumors in male mice exposed via the diet by Tomatis et al. (1974). The IRIS carcinogenicity assessment forp,p '-DDD is derived from the Hazard Assessment Report on DDT, DDD and DDE (U.S. EPA, 1980) and Carcinogen Assessment Group's Calculation of the Carcinogenicity of Dicofol (Kelthane), DDT, DDE, and DDD (TDE) (U.S. EPA, 1985a). IRIS does not report an inhalation unit risk forp,p '-DDD. p,p '-DDD is not included in the NTP's 11th Report on Carcinogens (NTP, 2005). IARC (1991) classifies DDT and associated compounds (includingp,p -DDD) in Group 2B (possibly carcinogenic to humans), citing inadequate evidence in humans, but sufficient evidence in animals for the carcinogenicity of DDT. The present document does not include a cancer assessment forp,p '-DDD, as one is available on IRIS. To identify toxicological information pertinent to the derivation of provisional toxicity values for p,p '-DDD, references from the 2002 ATSDR Toxicological Profile for DDT, DDE and DDD were screened for publications pertinent to the toxicity ofp,p '-DDD. Update searches were conducted in January, 2007 for literature dating from 2001 to 2007 using the following databases: MEDLINE, TOXLINE Special, and DART/ETIC (2001-2007); BIOSIS (2000-2007); TSCATS, CCRIS, GENETOX, HSDB, RTECS (not date limited); and Current Contents (previous 6 months). REVIEW OF PERTINENT DATA Human Studies Human studies of p,p '-DDD include one subchronic study with a human volunteer (Morgan and Roan, 1971), several studies of occupational exposure to technical grade DDT, which containsp,p '-DDD (Kolmodin et al., 1969; Laws et al., 1967, 1973; Morgan and Lin, 1978; Morgan et al., 1980; Ortelee, 1958; Poland et al., 1970; Wong et al., 1984), and several investigations of associations between reproductive effects andp,p '-DDD levels in biological fluids (Saxena et al., 1980, 1981, 1983; Pines et al., 1987; Dalvie et al., 2004; Pant et al., 2004; Perry et al., 2006). Due to the low number of study subjects, concurrent exposures to other chemicals, and difficulty in distinguishing between biological levels ofp,p '-DDD resulting from exposure and levels resulting from human metabolism of DDT or DDE, data from the available human studies were not considered useful for derivation of provisional toxicity values. In a study of the toxicokinetics of DDT and its metabolites (including p,p -DDD), an adult male volunteer ingested 5 mg/day ofp,p '-DDD for 81 days (Morgan and Roan, 1971). The pesticide was mixed with vegetable oil, emulsified with gum arabic and water and taken with meals (no further detail on dosing was provided). Assuming a reference body weight of 70 kg (U.S. EPA, 1988a), the intake ofp,p '-DDD was 0.071 mg/kg-day. Before, during and after the treatment period, the man was given a battery of hematological and clinical biochemical tests (frequency and nature of testing not reported). No abnormalities were detected. Serum and adipose levels of p,p '-DDD rose steadily during the exposure period, peaking at exposure termination at almost 80 ppb in serum and more than 4 ppm in adipose (based on visual 3 ------- 8-13-2007 examination of data presented graphically). After exposure was withdrawn, levels in both serum and adipose declined rapidly. Measurements taken 180 days after exposure termination showed no detectablep,p '-DDD in serum and levels reduced to almost 1 ppm in adipose. Although no adverse effects on hematological and clinical chemistry endpoints were observed, details of the test endpoints, frequency, and results were not reported, and other endpoints were not assessed; thus the administered dose cannot be considered a NOAEL. Furthermore, the study was conducted on only one volunteer, limiting the usefulness of the data. Several epidemiology studies of workers exposed to technical grade DDT were located (Kolmodin et al., 1969; Laws et al., 1967, 1973; Morgan and Lin, 1978; Morgan et al., 1980; Ortelee, 1958; Poland et al., 1970; Wong et al., 1984). Technical grade DDT consists of a mixture ofp,p -DDT (77.1%), o,p '-DDT (14.9%), p,p '-DDE (4.0%), p,p '-DDD (0.3%), o,p '- DDE (0.1%), o,p '-DDD (0.1%) and unidentified compounds (3.5%) (U.S. EPA, 1980). Exposure was primarily via the inhalation and dermal routes, but some oral exposure probably occurred as well. In most of the studies, workers were exposed to a variety of other compounds in addition to technical grade DDT. Because of the mixed exposures, these studies do not provide any useful information on health effects ofp,p '-DDD in humans. Measurements ofp,p '-DDD in biological fluids have been used to evaluate potential effects on female reproductive function. Saxena et al. (1980, 1981, 1983) studied the levels of organochlorine insecticides in maternal blood and placenta in cases of stillbirth, premature labor and delivery, spontaneous abortion, and normal full-term delivery among patients in India. The levels ofp,p '-DDD in maternal blood, placentas and cord blood of stillbirths were not significantly different from the levels in normal full-term deliveries (Saxena et al., 1983); however, there were few participants in this study (9 stillbirths and 27 full-term deliveries). Maternal blood and placental levels ofp,p '-DDD were significantly (p<0.001) higher in cases of preterm labor and spontaneous abortion when compared with full-term deliveries; levels ofp,p '- DDT, p,p '-DDE, lindane, and aldrin were also significantly higher (Saxena et al., 1980, 1981). However, due to the small numbers of study participants (<25 cases and <25 controls) and the confounding role of other pesticides, a causal relationship betweenp,p '-DDD and reproductive effects cannot be established from these data. As reported in an abstract, Perry et al. (2006) evaluated the association between serum levels of DDT and its metabolites (not specified) with urinary levels of progesterone and estrogen, and menstrual cycle characteristics in 287 newly- married women who were trying to conceive. Data were collected from each woman for 1 year or until conception. After adjustment for potential confounders, increased serump,p '-DDD levels were associated with decreased urinary levels of pregnanediol-3-glucuronide across all menstrual cycle days; however, the authors did not present statistical analysis of the results. No other associations withp,p '-DDD were reported in the abstract. In these studies (Saxena et al., 1980, 1981, 1983; Perry et al., 2006), it is not known whether thep,p '-DDD detected in the subjects was derived from direct exposure to p,p '-DDD or from metabolism of DDT or DDE. In addition, since the subjects in these studies also had detectable levels of other compounds (including DDT and its other metabolites), the degree to which the observed effects can be attributed top,p '-DDD is uncertain. Because there are indications thatp,p '-DDD may have antiandrogenic effects, several studies have examined the association between male reproductive function and p,p '-DDD in 4 ------- 8-13-2007 biological fluids. Pines et al. (1987) studied the possible associations between organochlorine insecticide exposures and reproductive function in men by comparing concentrations of these compounds in the serum of 29 infertile and 14 fertile men from the general Israeli population. Serum concentrations ofp,p '-DDD alone or in combination with p,p '-DDT and p,p '-DDE were statistically significantly (p<0.05) higher in infertile men than in fertile men. Correlations between semen characteristics (sperm count, motility, morphology) and the serum concentrations of these compounds, however, were not significant. Dalvie et al. (2004a) evaluated the effects of DDT and its metabolites on semen, fertility and sexual function in a cross-sectional study of 60 anti-malaria workers in South Africa. There were no statistically significant associations between serum levels ofp,p '-DDD and sperm count, density or morphology; self-reported problems with sexual function; prevalence of genital abnormalities on physical examination; or number of pregnancies fathered. In a companion study, Dalvie et al. (2004b) reported that levels of estradiol and testosterone were significantly (p<0.05) increased with higher serum levels of p,p '-DDD. Pant et al. (2004) compared levels ofp,p '-DDD and other chlorinated pesticides in the semen of 45 fertile and 45 infertile men in India. Levels ofp,p -DDD, p,p '-DDE, total DDT and various isomers of hexachlorocyclohexane (HCH) were significantly (p<0.05) higher in the semen of infertile than fertile men. Semen levels of p,p '-DDD were 78% higher in infertile men. Correlation analysis showed that p,p '-DDD levels in semen of infertile men were significantly correlated with higher levels of fructose (a marker for seminal vesicle secretion). Infertile men had higher levels of fructose than fertile men and the authors suggested that the higher fructose was indicative of underutilization of fructose due to biochemical defects. As with other studies using biological levels of p,p '-DDD as a measure of exposure, it is not possible to associate any of the observed effects on male reproductive function with exposure to p,p '-DDD. In summary, the available human studies do not provide conclusive evidence for an association between p,p '-DDD exposure and reproductive or hormonal effects. In all of these studies, the participants had measurable levels of other chlorinated compounds, including DDE and DDT. Further, whenp,p '-DDD levels in biological fluids are used as a surrogate for exposure, it is not possible to determine whether the levels result from direct exposure top,p '- DDD or from metabolism of DDT and/or DDE. As a consequence, none of the human studies is suitable for use in deriving provisional toxicity values. Animal Studies Oral Exposure Subchronic Exposure — In preparation for a chronic cancer bioassay, NCI (1978) conducted a range-finding dietary toxicity study of DDD in Osborne-Mendel rats and B6C3F1 mice. Technical grade DDD (60%p,p '-DDD) in corn oil was mixed with feed and administered ad libitum to groups of 5 male and 5 female rats per concentration for 6 weeks, followed by a 2- week observation period. The test material contained 19 impurities contributing 40% of the total dose; none of the impurities were identified. The major analytical peak comprising 60% of the test material was assumed to bep,p '-DDD. Diets containing 0, 562, 1000, 1780, 3160 or 5620 ppm technical grade DDD were fed to rats (corresponding top,p '-DDD doses of 0, 29, 52, 93, 5 ------- 8-13-2007 166 or 295 mg/kg-day in males, and 0, 32, 57, 101, 179 or 319 mg/kg-day in females1 after adjustment for 60% purity). Only mortality and body weight changes were evaluated; no animals were necropsied. No deaths were observed in rats exposed top,p '-DDD concentrations up to 3160 ppm; no information was reported on mortality at 5620 ppm (NCI, 1978). Mean body weights were reduced in male rats exposed to 1780 ppm (9% lower than controls) and 3160 ppm (10% lower), and in female rats exposed to 1000 ppm (39% lower) and 1780 ppm (4% lower); neither statistical analysis nor raw data were presented. No data on body weight changes at other doses were reported. This study did not provide sufficient information to establish effect levels. Groups of 5 male and 5 female mice were exposed to dietary p,p '-DDD for 6 weeks, followed by a 2-week observation period (NCI, 1978); test material and study protocol were as described above for rats (NCI, 1978). Mice received diets containing 0, 251, 398, 631, 1000 or 1590 ppm (0, 27, 43, 68, 108 or 172 mg/kg-day p,p '-DDD in males, and 0, 29, 47, 74, 117 or 186 mg/kg-day p,p '-DDD in females2 after adjustment for 60% purity). Mortality was observed in male mice of all but the 631 ppm exposure group (data and details not reported); no deaths occurred among control males (NCI, 1978). Mortality was also observed in female mice exposed to 1000 and 1590 ppm but not in other groups (data not reported). p,p '-DDD did not affect body weights in the exposed mice; mean body weight gain in male and female mice exposed to concentrations up to 631 ppm exceeded weight gain in controls (details not reported). This study did not provide sufficient information to establish effect levels. Baneijee et al. (1996) evaluated the effects of dietary p,p '-DDD exposure on humoral and cell-mediated immune response in Wistar rats. Groups of 8-12 male rats were given either the control diet or a diet containing 200 ppmp,p '-DDD (99% pure) for 6 weeks (equivalent to about 18 mg/kg-day3), during which general condition, food consumption and body weights were recorded weekly. Half of each group was immunized by subcutaneous administration of 3 mg ovalbumin three weeks before the end of the exposure period; the other half was left unstimulated. At the end of the exposure period, rats were sacrificed and blood samples collected. The liver, spleen and thymus from each animal were removed and weighed. The humoral immune response was quantified by measuring immunoglobulin levels (IgM and IgG), estimating the albumin/globulin ratio and measuring the ovalbumin antibody titer by ELISA. Cell-mediated response was assessed in vivo, by quantifying the delayed type hypersensitivity reaction (measuring footpad thickness after ovalbumin challenge) and in vitro by measuring leukocyte and macrophage migration inhibition. The latter tests assess whether chemical exposure results in suppression of lymphokine production. Exposure top,p '-DDD had no effect on mortality, food intake, body weight, or relative liver or thymus weights, but significantly (p<0.05) reduced relative spleen weight by 14%; absolute spleen weights were not reported (Banerjee et al., 1996). With regard to humoral 1 Based on reference values for food consumption and body weight (U.S. EPA, 1988a); doses given are for pure p,p '-DDD after adjustment for 60% purity. 2 Based on reference values for food consumption and body weight (U.S. EPA, 1988a); doses given are for pure p,p '-DDD after adjustment for 60% purity. 3 Based on reference values for food consumption and body weight (U.S. EPA, 1988a). 6 ------- 8-13-2007 immune responses, treatment with p,p '-DDD had no effect on the serum albumin/globulin ratio, but significantly (p<0.05) reduced the levels of IgG, IgM and the titer of anti-ovalbumin antibody in serum by 15, 24 and 35%, respectively, compared to controls. Treatment withp,p '- DDD significantly reduced cell-mediated immune responses; delayed type hypersensitivity reactions (increase in footpad thickness) and tests of inhibition of migration of leucocytes and macrophages were suppressed by 24%, 24% and 25% (respectively) compared to controls. In this study, the only dose tested (18 mg/kg-day) is a minimal LOAEL for evidence of immunosuppression and potential effects on spleen weight in rats; no NOAEL can be identified from these data. The LOAEL is considered minimal because the impact of the observed changes on immune function is not certain. Chronic Exposure — Tomatis et al. (1974) evaluated the carcinogenicity ofp,p '-DDD (and p,p '-DDE separately) in CF-1 mice treated via the diet for a lifetime. The authors administeredp,p '-DDD in the diet (250 ppm) to 60 male and 60 female mice (6-7 weeks old) for up to 123 weeks; 101 male and 97 female mice were maintained on a control diet. The test compound was 99% pure and was dissolved in acetone prior to being mixed with powdered food and converted to pellets. It is not clear whether the control diet contained acetone. A dietary concentration of 250 ppm corresponds to an estimated p,p '-DDD dose of about 43 mg/kg-day (for both males and females) based on reference values for food consumption and body weight of mice (U.S. EPA, 1988a). Groups of four animals (sex not specified) were sacrificed either between weeks 65 and 74 of treatment or between weeks 94 and 118 of treatment for analysis of p,p '-DDD levels in the liver and interscapular fat (and sometimes in liver tumors and kidney; details not provided). All animals dying spontaneously or killed humanely were necropsied; remaining animals were sacrificed at 130 weeks of age. Histopathology evaluation was restricted to the lungs, heart, thymus, liver, kidneys, spleen, brain and any organs with gross abnormalities. Survival was not affected by p,p '-DDD (Tomatis et al., 1974). Survival to 90 weeks was 76 and 72% in treated males and females, compared with 67 and 73% in control males and females, respectively. There were no clinical signs of toxicity among mice treated with p,p '- DDD. The authors reported neither a statistical comparison of body weights nor raw data; however, based on visual evaluation of body weight curves (covering the period from the 3rd through 14th month of age), body weights of the treated males were depressed by more than 10% relative to controls over the entire period of observation; body weights of treated females were unaffected by treatment. The only other possible effect was a 5-fold increase in the incidence of myocardial necrosis in males, although the overall incidence was small (3/59 in treated animals vs. 1/98 in controls). No statistical analysis was presented by the authors. A post-hoc Fisher's Exact test was performed on the response data with a p-value of 0.15. Although not statistically significant by standard definitions, the 5-fold increase is still suggestive of an effect. The only dose ofp,p '-DDD tested, 43 mg/kg-day, is a LOAEL for body weight depression and suggestive of myocardial necrosis in male mice in this study. The authors noted that the incidence of lung tumors was increased over controls in p,p '- DDD-exposed mice of both sexes; in addition, the incidence of hepatomas was increased in male mice (Tomatis et al., 1974). This study was used in the derivation of the oral slope factor for p,p '-DDD (U.S. EPA, 2007). 7 ------- 8-13-2007 NCI (1978) conducted a carcinogenicity bioassay of p,p '-DDD in Osborne-Mendel rats and B6C3F1 mice. Technical grade DDD (60% p,p '-DDD) in corn oil was mixed with feed at varying concentrations and administered ad libitum. The test material contained 19 impurities, contributing 40% of the total dose; none of the impurities were identified. Nominal concentrations, durations of exposure at these concentrations, and weighted average concentration and dose estimates are given in Table 1. As the table indicates, the exposure concentration was increased once in rats and twice in mice, as the animals tolerated the exposures well. Rats were observed for 34 or 35 weeks after exposure termination and prior to sacrifice. Mice were observed for 13 to 15 weeks after the 78-week exposure period and prior to sacrifice. Weighted average exposure concentrations shown in Table 1 are averaged over the 78- week exposure period and do not take into account the post-exposure observation period. Weighted average dose estimates shown in the table are doses ofp,p '-DDD after adjustment for purity. Body weight and food consumption measurements, clinical observations and palpations for masses were conducted weekly for 10 weeks and monthly thereafter; mortality checks were performed daily (NCI, 1978). Necropsy was performed on all animals, but organ weights were not recorded. Histopathologic examination was initially limited to control animals, animals with visible tumors and at least 10 males and females with no gross pathological findings from each group. Later in the study, the protocol was altered to include tissues from other animals; however, the authors did not indicate how the other animals were selected, how many were included or when the protocol change was initiated. Nearly 30 tissues were subjected to microscopic examination. The authors noted that tissues were not examined from some animals that died early and that some animals were missing, cannibalized or in an advanced state of autolysis, precluding histopathologic examination. Incidence of lesions was reported using the number of animals for which that specific tissue was examined as the number at risk, except where lesions were observed grossly or could appear at multiple sites (e.g., lymphoma), in which cases the number of animals necropsied was used. The authors reported that, beginning during week 30 and continuing through termination of the exposure period, treated rats exhibited a slightly greater incidence of clinical signs of toxicity (hunched appearance and urine staining; data not reported) (NCI, 1978). Prior to 30 weeks and during the recovery period, there was no treatment-related effect on the incidence of clinical signs (data not reported), according to the authors. p,p '-DDD treatment did not significantly affect probability of survival in either sex. There were clear treatment-related reductions in body weight, but the authors did not present statistical comparisons of group mean body weights or raw data. Based on graphical presentation of the data, the greatest differences from control weights occurred between weeks 60 and 75, when the mean body weights were about 10%) and 20% lower than controls in low- and high-dose males (respectively) and about 20% and 30% lower in low- and high-dose females. Treatment withp,p '-DDD had no significant effect on the incidence of nonneoplastic lesions in rats in any tissue examined. A NOAEL cannot be determined from this study. The low dose (39 mg/kg-day in females) is a LOAEL for depression of body weight gain and clinical signs of toxicity. The LOAEL is for the mixture. A LOAEL forp,p '-DDD cannot be established from this study. 8 ------- 8-13-2007 Table 1. Group Sizes, Dietary Concentrations and Dose Estimates for NCI (1978) Cancer Bioassay forp,p'-DDD Group Group Size Nominal Concentration (mg/kg) Duration at this Concentration (weeks) Untreated Duration (weeks) Weighted Average Concentration Technical grade DDDa (mg/kg) Weighted Average Daily Dose />,/>-DDDb (after adjustment for purity) (mg/kg-day) Male Rats Control 20 0 111 0 Low Dose 50 1400 1750 0 23 55 34 1647 69 High Dose 50 2800 3500 0 23 55 35 3294 138 Female Rats Control 20 0 111 0 Low Dose 50 850 0 78 35 850 39 High Dose 50 1700 0 78 35 1700 79 Male Mice Control 20 0 90 0 Low Dose 50 315 375 425 0 5 11 62 13 411 42 High Dose 50 630 750 850 0 5 11 62 14 822 85 Female Mice Control 20 0 90 0 Low Dose 50 315 375 425 0 5 11 62 14 411 43 High Dose 50 630 750 850 0 5 11 62 15 822 85 " Calculated by the authors as the sum of concentration x time averaged over 78 weeks. b Calculated using weighted average concentration and reference values for body weight and food consumption from U.S. EPA (1988a); doses adjusted for 60% purity. Source: NCI, 1978. 9 ------- 8-13-2007 The authors reported treatment-related increases in the incidence of thyroid follicular-cell neoplasms in rats treated withp,p '-DDD (NCI, 1978). No other treatment-related effects on neoplasm frequency were observed. This study was evaluated as part of the IRIS cancer assessment, but was not used in deriving the oral slope factor. In mice, p,p '-DDD treatment had no significant effect on probability of survival in either sex. Clinical signs occurred with the same frequency in treated and control animals. Exposure to p,p '-DDD had no effect on male body weight throughout the treatment period, but dose- related depression of body weight was observed in female mice after week 30. The authors did not present statistical comparisons of group mean body weights or raw data. Based on graphical presentation of the data, the body weight reduction peaked at about 14% in the high-dose group between weeks 60 and 75; in the low-dose group, body weight decrements appeared to be less than 10% throughout the study. Treatment did not significantly increase the incidence of neoplastic or nonneoplastic lesions in any tissue in either sex. The low dose of 42 mg/kg-day p,p '-DDD is a NOAEL and the high dose of 85 mg/kg-day p,p '-DDD is a LOAEL for body weight depression in female mice. Inhalation Exposure There are no data on the effects in laboratory animals ofp,p '-DDD exposure via inhalation. Other Studies Adrenal Effects — Cueto and Brown (1958) fractionated technical grade DDD and tested the fractions and isolates, delivered in gelatin capsules, for adrenocorticolytic activity in male dogs (breed not specified). A single dog received 80 mg/kg-day of purified p,p '-DDD for 29 days and another the same dose for 80 days; a third dog was treated with 200 mg/kg-day for 30 days and a fourth dog was left untreated for 100 days as a control. The endpoints examined included general appearance, periodic tests of adrenal activity and, after necropsy, examination of adrenal histopathology. No other organ system was evaluated. Treatment with p,p '-DDD at either dose level had no effect on the physical state of the dogs. In tests of adrenal activity administered after 4 and 20 days of treatment, the dog treated with 200 mg/kg-day of p,p '-DDD and the control dog exhibited the same effects in response to an injection of adrenocorticotropic hormone: there were similar decreases in the eosinophil count and similar increases in the plasma level of 17-hydroxycorticosteroids. At termination, no treated dogs showed evidence of adrenal histopathology. In a similar study, Powers et al. (1974) fed technical grade DDD (characterized by the authors as 90%p,p '-DDD and 5-8% o,p '-DDD, other impurities unspecified) dissolved in corn oil and administered in gelatin capsules to mixed groups of mongrel and purebred beagle dogs. The dogs were given doses of either 100 or 200 mg/kg for varying time periods up to 30 days. Control groups (mongrels and beagles) of various sizes were maintained. Upon sacrifice, the adrenal glands were weighed (in some cases) and/or examined with light and electron microscopy. The authors reported histopathology findings in the adrenals of treated dogs, including degenerative vacuolation, especially in the inner cortex, mitochondrial swelling, 10 ------- 8-13-2007 cellular necrosis and dilatation of smooth endoplasmic reticulum. Because the test material in this study included o,p '-DDD and potentially other contaminants, it is not possible to determine whether any of the adrenal affects are attributable to p,p '-DDD exposure. Mechanistic — A number of studies have investigated the hormonal activities of DDT and related compounds. When Gellert et al. (1972) injected groups of 11 or 12 mature ovariectomized Sprague-Dawley rats with 0.1 or 10 mg/day ofp,p '-DDD in DMSO for 7 days, there was no effect on uterine weight, uterine histology, cytology of vaginal smears or serum levels of luteinizing hormone or follicle stimulating hormone. In castrated male Brl Han: WIST Jcl (GALAS) rats treated with 8, 40 or 200 mg/kg-day p,p '-DDD via gavage for 10 days, either with or without testosterone propionate, treatment with 200 mg/kg p,p '-DDD and testosterone propionate resulted in significant decreases in seminal vesicle and bulbocavernosus/levator ani muscles, indicating antiandrogenic activity (Yamasaki et al., 2004). In in vitro assays, p,p '-DDD did not competitively inhibit binding of 17P-estradiol to the estrogen receptor, but competitively inhibited binding of a synthetic androgen (R1881) to the rat androgen receptor (Kelce et al., 1995). In in vitro assays using yeast reporter gene systems, p,p '-DDT was unable to activate expression of the estrogen receptor gene or the androgen receptor gene at concentrations below 10"4 M (Gaido et al., 1997). Using an in vitro human hepatoma cell reporter gene system, Maness et al. (1998) found that p,p '-DDD did not stimulate expression of the human androgen receptor (hAR) gene, but did inhibit androgen-dependent expression of the hAR gene. p,p '-DDD gave positive results in an androgen receptor binding assay (Yamasaki et al., 2004). The results of these experiments suggest that p,p '-DDD has antiandrogenic activity, but no estrogenic activity. Limited evidence suggests thatp,p '-DDD binds to lung tissues and can be cytotoxic to lung cells. When Lund et al. (1989) intravenously injected radiolabeledp,p '-DDD into mice, autoradiography of solvent-extracted, whole-body sections revealed specific covalent binding in the alveoli of the lung, in the lateral nasal gland and the salivary glands. The results of the in vivo study suggest that pulmonary binding of p,p '-DDD can occur after intravenous exposure. An in vitro experiment in the same paper demonstrated that p,p '-DDD irreversibly bound to protein following incubation with S-9 fractions from murine lung or liver. The authors concluded that covalent binding of p,p '-DDD in the lung was the result of in situ bioactivation. In an in vitro study, Nichols et al. (1992) incubated lung cells isolated from rabbits withp,p DDD, with or without 1-aminobenzotriazole (1-ABT - a suicide substrate inhibitor of cytochrome P-450 monooxygenases). Cytotoxicity ofp,p '-DDD to Clara cells especially and to alveolar type II cells and alveolar macrophages to a lesser degree, was dependent on the presence of functional cytochrome P-450. Subsequently, Nichols et al. (1995) evaluated potential mechanisms for bioactivation of p,p '-DDD in cultured Clara cells of rabbits and a transformed human bronchial epithelial cell line (BEAS-2B). Both cell types were vulnerable to p,p '-DDD- mediated cytotoxicity and were protected by co-incubation with 1-ABT, the inhibitor to cytochrome P-450. In another experiment, Nichols et al. (1995) found that cytotoxicity was reduced when human BEAS-2B cells, rabbit Clara cells, or rabbit pulmonary microsomes were incubated withp,p '-DDD that had a deuterium substitution at the C-l position. The results indicated that the cytotoxicity ofp,p '-DDD may be caused by its oxidation at C-l mediated by cytochrome P-450 in the lung. 11 ------- 8-13-2007 DERIVATION OF PROVISIONAL SUBCHRONIC AND CHRONIC ORAL RfD VALUES FOR 1) I) I) None of the human studies of p,p '-DDD are suitable for derivation of provisional oral RfD values. The database includes several epidemiological studies of workers exposed to technical grade DDT (a mixture that includes a small percentage ofp,p -DDD), as well as studies evaluating the potential association between biological measurements ofp,p '-DDD and reproductive or hormonal effects. It is not possible to clearly attribute any effects reported in these studies to direct exposure top,p '-DDD due to the confounding effects of concomitant exposure to other organochlorine compounds (especially DDT and its other metabolites), and because it is not possible to determine whetherp,p '-DDD measured in biological tissues resulted from exposure to p,p '-DDD or from metabolism of DDT or DDE to p,p '-DDD in the human body. There are no suitable long-term general toxicity animal studies for derivation of a provisional RfD. The Tomatis et al. (1974) study is designed primarily as a carcinogenicity bioassay, with very sparse detail on noncancer effects. Furthermore, the LOAEL of 43 mg/kg- day is very high compared to closely-related compounds. Chronic LOAELs for related compounds are 0.25 mg/kg-day ip,p'~DDT; U.S. EPA, 1985b), 4.0 mg/kg-day (Cueto and Brown, 1958) and 12 mg/kg-day (NCI, 1978), with the latter two being FELs (mortality). Given the low LOAELs and FELs for closely related compounds, the potential is high that a well- designed p,p '-DDT chronic study would produce a much lower LOAEL. As a result, the Tomatis study is judged to be inadequate for assessment of long-term noncancer toxicity. Studies suitable for use in deriving provisional RfD values include a chronic study in mice (Tomatis et al., 1974) and a 6-week immunotoxicity study in rats (Banerjee et al., 1996). Summaries of these studies and comparisons with the LOAEL values from the chronic NCI (1978) study are shown in Table 2. The usefulness of data from the NCI (1978) subchronic and chronic feeding studies for p-RfD derivation is compromised by the low purity of the technical grade DDD tested. Only 60% of the product was p,p '-DDD and at least 19 impurities (unspecified) were present in the remaining 40%. The chronic data are further compromised by the substantial adjustments in administered dietary level during the study and by the long post- treatment observation period, during which recovery from or reversal of effects could have occurred. The two studies in dogs (Cueto and Brown, 1958; Powers et al., 1974) are not suitable for p-RfD derivation due to the small number of animals used, limited endpoints evaluated and, in some cases, post-treatment observation periods allowing for reversal of effects. The only remaining study, Banerjee et al. (1996), is a 6-week immunotxicity study that does not cover the required general toxicity endpoints. Although the study was adequate for its purpose and establishes the lowest LOAEL forp,p '-DDD, by itself, it does not qualify as the basis for either a subchronic or chronic p-RfD. The oral noncancer database is inadequate for derivation of p-RfDs. Neither of the two studies available for p-RfD derivation included more than one dose level, precluding benchmark dose modeling of the effects. 12 ------- 8-13-2007 Table 2. Summary of Available Oral Noncancer Dose-Response Information Suitable for p-RfD Derivation and Comparison with LOAELs from NCI (1978) Chronic Studies Species Sex Dose (mg/kg-day) Exposure Duration NOAEL (mg/kg-day) LOAEL (mg/kg-day) Responses Comments Reference Rats M 0, 18 mg/kg- day 6 weeks NA 18 Immunosuppression (reduced humoral and cell- mediated immunity) and decreased relative spleen weight. Minimal LOAEL. Endpoints included clinical signs, body weight, selected organ weights, and immunotoxicity parameters. Baneijee et al., 1996 Mice M,F 0, 43 mg/kg- day 123 weeks NA 43 Body weight depression in males. Endpoints included survival, clinical signs, body weight, and histopathology of selected organs. Tomatis, 1974 Rats M,F 0, 69, 138 mg/kg-day (M) or 0,39, 79 mg/kg- day (F) 78 weeks, followed by 34-35 weeks observation NA 39 Depression of body weight gain and clinical signs of toxicity in females. Test article only 60% pure. Prolonged observation period may have allowed for recovery from toxic effects. Not suitable for p-RfD derivation. NCI, 1978 Mice M,F 0, 42, 85 mg/kg-day (M) or 0, 43, 85 mg/kg-day (F) 78 weeks, followed by 13-15 weeks observation 42 85 Depression of body weight gain in females. Test article only 60% pure. Prolonged observation period may have allowed for recovery from toxic effects. Not suitable for p-RfD derivation. NCI, 1978 13 ------- 8-13-2007 DERIVATION OF PROVISIONAL SUBCHRONIC AND CHRONIC INHALATION p-RfC VALUES FOR1) I) I) No studies specifically investigating the effects of inhaled p,p '-DDD in humans or animals were located. Thus, provisional RfCs were not derived forp,p '-DDD. 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