TOXICITY OF NEODOL<"> SURFACTANTS by Anna S. Mammons C. Donald Powers Science Applications International Corporation Oak Ridge, TN 37831 May 1987 Prepared for Office of Toxic Substances U.S. Environmental Protection Agency Washington, DC 20460 Task Officer Terry O'Bryan ------- TABLE OF CONTENTS 1.0 INTRODUCTION 1 2.0 DESCRIPTION OF NEODOlW PRODUCTS 2 2.1 NEODOL Alcohols 2 2.2 NEODOL Ethoxylates 2 2.3 NEODOL Sulfates 3 2.4 NEODOL Ethoxysulfates 4 3.0 EFFECTS ON NON-MAMMALIAN ORGANISMS 5 3.1 Acute Effects LCcn 5 3.1.1 Alcohols 5 3.1.2 Alcohol Ethoxylates 7 3.1.3 Alcohol Sulfates 7 3.1.4 Alcohol Ethoxysulfates 8 3.2 Sublethal Effects 9 3.2.1 Aquatic Animals 9 3.2.2 Plants 10 3.3 Chronic Effects 12 4.0 ENVIRONMENTAL FACTORS INFLUENCING AQUATIC TOXICITY 13 4.1 Water Hardness 13 4.2 Biodegradablllty 13 4.3 Exposure 14 5.0 MAMMALIAN TOXICITY 15 5.1 Acute Effects 15 5.2 Subchronic Effects 16 5.3 Chronic Effects 17 5.4 Carclnogenlcity 17 5.5 Mutagenldty 18 5.6 Teratogenlcity/Reproduction 18 5.7 Studies In Humans 19 11 ------- TABLE OF CONTENTS 5.8 Metabolism jg 6.0 CONCLUSIONS 20 6.1 Toxicity to Non-Mammalian Organisms 20 6.2 Mammalian Toxicity 21 6.3 1,4-Dioxane Contamination 25 7.0 REFERENCES 26 APPENDIX A - Acute Toxicity (LC50) of Alcohol Surfactants to Aquatic Animals 38 iii ------- LIST OF TABLES Table 1 General direction of toxicity and rate of bio- degradation of linear primary alcohols and deriva- tive surfactants in an aquatic environment as a function of alkyl or ethoxylate (EO) chain length ... 6 Table 2 Effects of NEODOl products in laboratory mammals .... 22 iv ------- TOXICITY OF NEODOL(R) SURFACTANTS 1.0 INTRODUCTION This report is the result of Work Assignment #3 of IAG #DW-89930405. Toxicity data from a voluntary submission (FYI-AX-0685-0410 Sequence A) by Shell Chemical Company to EPA's TSCA Existing Chemicals Program and two published reports by Arthur D. Little, Inc. ("Human Safety and Environmental Aspects of Major Surfactants," May, 1977; "Supplement," by Goyer et al. February, 1981) were reviewed to evaluate the toxicity and structure-activity relationships of NEODOlW chemicals for which data are available and to identify gaps in the toxicity database. TSCA 8(e) submission 8EHQ-0580-0326 Sequence C was also reviewed for its applicability to NEODOL toxicity. Today's dishwashing and laundry agents are superior to those of the past because they thoroughly clean man-made fibers, tolerate hard water, form little foam, and are readily biodegraded. These improvements are due largely to the extensive use of three classes of surfactants (NEODOL products) in cleaning formulations. Derived from primary alcohols, these compounds are classified according to the chemical group(s) attached to the alkyl chain: alkyl sulfates, if sulfated; alkyl or alcohol ethoxylates, if ethylene oxides are present; and alkyl or alcohol ethoxysulfates, if ethylene oxides are sulfated. In addition to the widespread use of NEODOL products as household cleaning agents (primarily the ethoxysulfates), they are extensively used in personal care products such as shampoos, bubble baths, and cosmetics, and also have many industrial applications. NEODOL ethoxylates are also used as analgesic.s and anesthetics. While recent product/consumption figures have not been provided, a review of the values reported by Arthur D. Little (1977, Goyer et al. 1981) indicates the considerable use of these surface-active agents. Comparing data from 1973 and 1978, annual use of ethoxylates in the United States increased from 188,000 tons to 238,000 tons during the five-year period. Similarly, the use of ethoxysulfates rose from 53,000 tons to 64,000 tons during those same years. As for alkyl sul fates, 90,000 tons were used ------- worldwide in 1976. Shell Chemical Company is the world's largest producer of linear primary alcohols and alcohol-based surfactants, exceeding 450 million pounds per year in the United States. In England and Japan certain NEODOL products are produced under the name DOBONOl(R). 2.0 DESCRIPTION OF NEODOl(R) PRODUCTS NEODOL products include: o NEODOL alcohols (ROH) o NEODOL ethoxylates [RO(CH2CH20)XH] o NEODOL sulfates (ROS03-Na+ or NH4+) o NEODOL ethoxysulfates [RO(CH2CH20)xS03-Na+ or NH4+] 2.1 NEODOL Alcohols Linear primary alcohols (ROH) included in NEODOL products consist essentially of two groups: chains of Cg to GU carbon atoms and chains of q2 to C15 carbon atoms. Nomenclature is based on the length of the alkyl chain. For example, NEODOL 91 indicates that this product is a mixture of mostly Cg to Cn alcohols; NEODOL 25 is a mixture of mostly C12 - Ci5 alcohols (Shell b, P. 1). 2.2 NEODOL Ethoxvlates NEODOL ethoxylates are mainly produced from the reaction of ethylene oxide (CH2CH20 or EO) with linear primary alcohols, although some branched- chain alcohols are used (Satkowski et al. 1967, as reported in Arthur D. Little, Inc. 1977, p. 240). Examples: Primary CH3-(CH2)X CH2-0-(CH2-CH2-0)yH ------- Secondary CH3-(CH2)z-CH-(CH2)ziCH3 0-(CH2-CH2-0)yH x - usually 05 to Cje y - usually £63 to E02Q z + zj - usually €5 to NEODOL 25-3 or Cj2-l5 ^03 indicates that the product is comprised mostly of Cj2 to Cj5 alcohols reacted with an average of 3 molecules of EO to form a 3-unit EO chain (Shell b, p. 2). 2.3 NEODOL Sul fates NEODOL sul fates (alcohol or alkyl sul fates or AS) are produced by sulfation of the parent alcohol with either sulfur trioxide or chlorosulfonic acid and subsequent neutralization of the product with an appropriate base as follows: S03 or NaOH R-OH ....... > R-OS03-H+ ...... > R-OS03'Na+ C1S03H (R usually averages between 12 and 18 carbons). To produce secondary AS, the parent alkene is reacted with sulfuric acid. H2S04 C-C-C-C-C-C-C-C=C ...... >C-C-C-C-C-C-C-C-C OS03-H+ A complex mixture of isomers can occur because the sulfate ester group can add at any position along the chain, except at the terminal carbon atoms (Higgins and Burns 1975; Kerfoot and Flammer 1975; Swisher 1970, p. 36; as reported in Arthur D. Little, Inc. 1977, p. 171). ------- NEODOL 91 -S Indicates that the alkyl chain is Cg to Cu carbons in length, and that the sulfated alcohol has been neutralized with NaOH to produce a sodium (S) salt of the sulfate. NEODOL 23-A specifies the ammonium (A) salt of the sulfate (Shell b, p. 1). AS are used in many specialty products such as shampoos, cosmetics, dentifrices, antacids, and depilatories (Gleason et al. 1969 as reported in Arthur D. Little, Inc. 1977, p. 170), and are extensively used in heavy duty laundry products (Kerfoot and Flammer 1975, as reported in Arthur D. Little, Inc. 1977, p. 170). 2.4 NEODOL Ethoxvsulfates Walker et al. (1973, as reported in Arthur D. Little, Inc. 1977, p. 346) described the following procedures for production of NEOOOL ethoxysulfates (EOS). "(1) ethoxylation of a fatty alcohol (prepared from either vegetable oil or petroleum hydrocarbons) / \ KOH R-OH + / CH2-CH2 > R-0-(CH2CH20)X H I \ / J catalyst \ 0 J x (usually x = 2-4) (2) sulfation of the product with either sulfur trioxide (S03) or chlorosulfonic acid (C1S03H), S03 R-0-(CH2CH20)X H > R-0-(CH2CH20)X S03 H (3) and neutralization to form either the sodium or ammonium salt OH- R-0-(CH2CH20)X S03 H > R-0-(CH2CH20)X S03'Na+(or NH4+)B EOS can be designated as, for example, NEODOL 25-3A or Ci2.15E03A, signifying a mixture of 12 to 15 carbon alcohols, an average of three mole- cules of EO to form a three-unit chain, sulfation of the ethoxylate, and neutralization to form the ammonium salt (Shell b, p. 1). ------- EOS, high foaming anionic surfactants, are principally used in light-duty dishwashing products and laundry detergent formations. They are also used in shampoos and other household specialty products (Arthur D. Little Inc 1977 p. 345). 3.0 EFFECTS ON NON-MAMMALIAN ORGANISMS 3 . 1 Acute Effects Anionic surfactants are less acutely toxic to aquatic organisms than are nonionic surfactants. However, anionics cause more permanent damage to the gill structure of fish than do nonionics (Shell a, p. 4). Aquatic organisms are better able to recover after exposure to nonionic surfactants than after exposure to anionic surfactants. For example, 50% of the barnacle larvae exposed for 30 minutes to the LC50 concentration of a nonionic surfactant completely recovered within 20 minutes after removal to clean water. By contrast, barnacle larvae tested under similar conditions recovered no swimming ability within 48 hours after exposure to anionic surfactants ended (Wright 1976, as reported in Shell a, p. 16). Acute toxicities, expressed as LC50s, of NEODOL surfactants are compared in Appendix A for those aquatic organisms for which sufficient data are available. Chemicals are arranged in order of decreasing toxicity. Results are discussed in the following subsections. 3.1.1 Alcohols Alcohols are the NEODOL products least toxic to aquatic organisms Toxicity decreases with increases in the length of the carbon chain (Table 1) because water solubility eventually decreases so that the alcohol floats on the water surface (Shell a, p. 11). This is demonstrated by studies with rainbow trout (Salmp. gairdneri) showing an increase in 96 hour LC50 values from 6 to 10 mg/L for Dobanol 91 (Shell Internal Report TLGR. 0166.78, as reported in Shell a, p. 11) to a non-toxic response at saturation for Dobanol 45 (Shell Internal Report TLGR. 0162.78, as reported in Shell a, p. 11). ------- TABLE 1. General direction of toxicity and rate of biodegradation of linear primary alcohols and derivative surfactants in an aquatic environment as a function of alkyl or ethSiyfate (EO) chain" length Chain Lenatfi Alkyl EO Class (No. of carbon atoms) (No. of units) Alcohols | up Alkyl sul fates . up (AS) f 10 Alkyl ethoxylates I (EO) t or . I 19 1C 12 /o - 20 2 t Alkyl ethoxy- 16 sul fates (EOS) 16 t 1 6 2 6 2 ^^^^^^^^^^™B^^^^=a^^B1^^^^^^^^^^^«B™wa^^^^s^^B^«a^MB^^^^^^-^^^a5^ Rate of Toxicity Biodegradation I — t — A. . v Reports range from "no effect" to "very slight decrease" as complexity of the molecule increases. 1 1 1 T xLess toxic Same as for EO com- Ithan pounds. parent r t Key: | = increase I = decrease -no change NP = not prese = moderate or gradual decrease ------- 3.1.2 Alcohol Ethoxylates The toxicity of alcohol ethoxylates varies according to both the length of the alkyl chain and the number of EO units present. Generally, when the length of the alkyl chain remains the same, increases in the number of EO units decrease the toxicity (Table 1), as shown in Appendix A by the one-hour LC50 studies with goldfish (Carassius auratus) (Gloxhuber et al. 1968, as reported in Shell a, p. 14) and the 96-hour LC50 studies with rainbow trout (summarized by Shell a, p. 13, Figure 5) and Daohnia (U.S. Food and Drug Administration, as reported in Shell a, p. 15). Shell (a, p. 4) suggests that the toxicity is decreased because the molecule becomes less fat-soluble and, therefore, penetrates the gill membrane less readily. If, however, the number of EO units is unchanged and the length of the alkyl chain is increased, toxicity increases (Shell a, p. 13). Invertebrates (except Daohnia) are relatively tolerant to alcohol ethoxylates, with most LC50 values ranging from 500 to 5,000 mg/L (Shell a, p. 13) compared to bluegill sunfish (Laoomis macrochirus). with LC50 values ranging from 1.8 mg/L (C12-i5E03) to 11.0 mg/L (C12.i5E09, 98% linear pri- mary), and rainbow trout, with LC50 values ranging from 0.8 mg/L (C14.15E07) to 8-9 mg/L (C9.10E05) (Appendix A). Less active species are perhaps more tolerant to surfactants than the more active species because lower respiratory rates cause less surfactant to pass over their gills (Shell a, p. 4). 3.1.3 Alcohol Sulfates Alcohol sulfates do not appear to be as acutely toxic to aquatic organisms as are the ethoxylates. According to Kikuchi et al. (as reported in Goyer et al. 1981, p. 100), 24-hour LC50 values reported for Japanese killi- fish (Oryzias latipes) ranged from 0.78 mg/L for NaC16AS to 70 mg/L for NaC12aveAS- The variation was attributed to the difference in the length of the alkyl chain (Table I). However, close examination of the limited LC50 data presented in Appendix A does not clarify whether chain length affects toxicity. ------- 3.1.4 Alcohol Ethoxysulfates Sulfation of ethoxylates appears to reduce their toxicity by a factor of 21 to 23 compared to the parent products (Shell a 1985, p. 16). According to studies using fathead minnows (Pimeohales promelas). the most important factor influencing the toxicity of these surfactants is the number of EO units present rather than the number of carbon atoms present (Monsanto Co., un- published data, as reported in Arthur D. Little, Inc. 1977, p. 363). In- creasing the number of EO units when the number of carbon atoms was kept constant and less than 16 decreased toxicity (Table 1); however, when the number of carbon atoms was equal to or more than 16, increasing the number of EO units drastically increased toxicity (see Appendix A). The most toxic surfactant tested was CjsEOsS, producing a 24-hour LC$Q value of 0.8 mg/L. The peak toxicity at Cie changed very little with EO units decreasing to £03. The least toxic ethoxysulfate tested was CisE02S at an LC$Q of 80 mg/L. Contrary to Monsanto's results with minnows, Gafa (1974, as reported in Arthur D. Little* Inc. 1977, p. 363) found CjeEOa^S to be one of the least toxic surfactants to goldfish. Shell d (unpublished data, as reported in Goyer et al. 1981, p. 199) demonstrated substantial differences in 96-hour LC$Q values for rainbow trout when the numbers of carbon atoms were changed and the numbers of EO units were only slightly different. The LC50 for C^-isEOsS was 8.9 mg/L compared to an LC5Q of 400-450 mg/L for Cg.ioE02.5S. These results indicate that data are insufficient to generalize about the factors in- fluencing the toxicities of various alcohol ethoxysulfates. / The few data available for invertebrates suggest that they may be slightly less susceptible to EOS than are fish. LC$Q values (24-hour) ranged from 5 mg/L (C12E03S) to 37 mg/L (C12E03S, Ziegler or natural fatty alcohol- derived) in Daohnia (Lundahl et al. 1972, as reported in Arthur D. Little, Inc. 1977, p. 364). 8 ------- 3.2 Sublethal Effects 3.2.1 Aquatic Animals Surfactants have been shown to cause a variety of sublethal effects In aquatic organisms, such as changes In ventilation rates, Inhibition of larval development, and Immobilization. Alcohol ethoxylates and ethoxysulfates affect the ventilation rates of blueglll sunfish. For example, forty-eight hour tests by Makl (1979a, as reported In Goyer et al. 1981, p. 158} demon- strated that concentrations ranging from 0.26 mg/L to 1.2 mg/L of C^.sEO suppress ventilation rates In bluegills by 30 to 50% compared to controls. To a lesser extent, similar effects were also caused by C^^EO. However, 48 hours of exposure to 0.39 mg/L ^£03$ significantly increased the ventilation rate of bluegills (Maki 1979a, as reported in Goyer et al. 1981, p. 198). Larval development was inhibited in the Eastern oyster (Crassostrea viralnical after 48 hours exposure to a 0.11 mg/L concentration of Ci^EO (Maki 1979b, as reported in Goyer et al. 1981, p. 159), in the Pacific oyster (Crassostrea ojflas) after 48 hours exposure to a 0.84 mg/L (average) concentration of NaC^AS (Cardwell et al. 1977, as reported in Goyer et al. 1981, p. 104), and in the horse clam (Tresus cajjax) after 48 hours exposure to a 0.4 mg/L concentration of NaC^AS (Cardwell et al. 1978, as reported in Goyer et al. 1981, p. 104). Immobilization of barnacle nauplii occurred after 30 minutes exposure to 580 mg/L of a concentration of CjoEt^o (Wright 1976, as reported in Goyer et al. 1981, p. 159). Daohnia were immobilized by concentrations of sulfates ranging from 42 mg/L for C^AS to 8200 mg/L for CsAS indicating a trend of increasing AS toxicity with increasing numbers of carbon atoms (Lundahl and Cabridenc 1978, as reported in Goyer et al. 1981, p. 97). Similarly, Wright (1976, as reported in Goyer et al. 1981, p. 97) found CjnAS to be approximately ten times as toxic as CsAS in barnacle larvae (Elininius modestus). However, Bode et al. (1978, as reported in Goyer et al. 1981, p. 101) found toxicity decreased with increasing chain length when budding Hvdra attenuata were exposed to CJQ, C^, C^, and C^AS. The decrease was attri- buted to reduced water solubility at the assay temperature of 20°C. ------- Most data indicate that increasing the length of the alkyl chain of alcohol sulfates tends to increase toxicity (Table 1). Insufficient data are available on sublethal effects to make such generalizations about ethoxylates. Another type of effect was detected in whitefish fCareaonus clupeaformisl by Hara and Thompson (1978, as reported in Goyer et al. 1981, p. 103). The olfactory bulbar electric response was suppressed with 0.1 mg/L Ci2aveAS, the lowest concentration at which sublethal effects were observed. The authors considered this an adverse effect because feeding and migrating behavior could be impaired by reduced olfactory sensitivity. Feather oils of ducks were dissolved after 30 minutes exposure to a solution of 19 mg/L C12AS in distilled water (Choules et al. 1978, as reported in Goyer et al. 1981, p. 110). Such an effect could obviously place water- fowl at increased risk of hypothermia in waters polluted with detergents. 3.2.2 Plants Surfactants are toxic to aquatic plants. Alcohol ethoxylates have been shown to inhibit the growth of algae. C^.^AEs was algistatic to populations of the diatom (Navicula seminuluml at concentrations of 5-10 mg/L and to the green algae (Selenastrum capricornutuml at concentrations of 50 mg/L. The same surfactant was algicidal to the diatom at 100 mg/L and to the green algae at 1000 mg/L (Payne and Hall 1979, as reported in Goyer et al. 1981, p. 156). The growth of 12 species of marine phytoplankton (chlorophyceae) was completely inhibited by MgC12aveAS at concentrations of 100 and 1000 mg/L. Nannochloris sp. and Stichococcus sp. were completely inhibited by this surfactant at 10 mg/L (Ukeles 1965, as reported in Arthur D. Little, Inc. 1977, p. 194). Rockstroh (1967, as reported in Arthur D. Little, Inc. 1977, p. 196) demonstrated the toxicity of Na-C12aveAS to ciliates fCvrtolophosisl. Exposures of 4 and 15 minutes to concentrations of 0.1 and 0.2 mg/ml caused autolysis of the cytoplasm, fissures in the mitochondrial membrane, and formation of a diffuse mitochondrial edema. 10 ------- An unusual relationship between toxicity of a coconut-alcohol-derived ethoxysulfate and a red tide dinoflagellate (Gvmnodinium breve) was reported by Kutt and Martin (1974, as reported in Goyer et al . 1981, p. 201). Mor- tality decreased with increasing concentrations of the surfactant (87% with 2.5 ug/L, 63% with 12.5 mg/L, and 44% with 50 ug/L). No explanation was given for these abnormal results. Surfactants also affect the growth and developmnt of higher plants. Aquatic duckweed (Lemna minor) was adversely affected by exposures to C^^AE. On the basis of frond count, the 7-day £650 was 21 mg/L and on the basis of root length, it was 1.9 mg/L (Bishop and Perry 1979, as reported in Goyer et al. 1981, p. 166). Of ten AE surfactants tested on rye and barley grasses by Valores and Letez (1978, as reported in Goyer et al . 1981, p. 166), n-pri-Ci2- 15AE3 and n-pri-Cj2-i5AE3 were the most toxic to both grasses. Barley growth was reduced 25% and 20%, respectively, and rye growth was reduced 50% and 80%, respectively. All surfactants tested inhibited growth in both grasses at concentrations of 100 mg/L. The least phytotoxic compounds were n-pri 15AE20» n-pri Cg.nAEe, and n- Grain yield was reduced in paddy rice plants watered with 50 mg/L AS. Water absorption by the roots was markedly inhibited, photosynthesis was inhibited, and considerable yellowing of the leaf blade also occurred (Taniyama and Nomura 1978, as reported in Goyer et al. 1981, p. 109). However, a stimulatory effect was demonstrated with corn seeds watered with 0.01, 0.1, or 1 g/L Cj2aveAS (Nadasy et al. 1972, as reported in Arthur D. Little, Inc. 1977, p. 197). Seeds weighed 97%, 130%, and 136% of controls, respectively. Similar increases also occurred in length and dry weight of the corn plants. Treatment of barley seeds (Hordeum vulaare L.) with 100% active NaCi2aveAS (10~3M) for 24 hours before germination resulted in significant growth inhibition as determined by shoot length (Antonielli and Lupatteli 1977, as reported in Goyer et al. 1981). 11 ------- 3.3 Chronic Effects Few data are available on the chronic effects of NEODOL products. Much of the data that are available are "no observed effect concentrations" (NOEC) for ethoxylates derived by Maki from studies with fathead minnows and Daohnia. For example, a chronic toxicity test emphasizing egg production and spawning rate in minnows resulted in a NOEC of 0.32 mg/L, the highest concentration tested for C12-5EO (Maki 1979c, as reported in Goyer et al. 1981, p. 160). For Daphnia, a similar NOEC, 0.27 mg/L, was obtained with a chronic exposure to C13.67E02.25S (Mak1 1979d, as reported in Goyer et al. 1981, p. 200). Growth was inhibited, however, in the fathead minnow after a one-year exposure to 0.22 mg/L concentration of Cj3.7E02.2sS (Maki, 1979d, as reported in Arthur D. Little, Inc. p. 200). Maki (1979a, as reported in Shell a, p. 18) demon- strated that chronic exposure to low levels of alcohol ethoxylates decrease respiratory rates in fathead minnows, whereas the rates are increased by exposures to ethoxysulfates. The mode of action is unknown. Other studies have shown that egg fertilization can be inhibited in crustaceans by exposure to surfactants. Grammo and Jorgensen (1975, as reported in Goyer et al. 1981, p. 160 and Shell a, p. 19) caused almost complete inhibition of egg fertilization by exposing mussels fMvtilus edulisl to 2 mg/L TAE10 (ethoxylated tallow alcohol) for five months. Some inhibition occurred at concentrations as low as 0.1 mg/L. Arthur D. Little, Inc. (1977) reviewed the results of a chronic toxicity test on clam (Mercenaria mercenaria) and oyster (Crassostrea virainical larvae. At 1 mg/L AS, ferti- lized egg development was significantly retarded compared to controls, while complete inhibition of development occurred at 2.5 mg/L. After a 10-day exposure to 5 mg/L, clam mortality was 68%; oyster mortality was 82% after 12 days exposure. More studies are needed before conclusions can be reached about the long- term toxicity of surfactants to aquatic systems. The limited data available indicate that, generally, concentrations exceeding 0.2 mg/L can cause adverse effects in aquatic organisms when exposures last for several months. 12 ------- 4.0 ENVIRONMENTAL FACTORS INFLUENCING AQUATIC TOXICITY 4.1 Water Hardness Water hardness appears to play a role in the toxicity of at least the alcohol sulfates. WUh an Increase In water hardness, the toxicity (and uptake) of AS increases (Arthur D. Little, Inc. 1977, p. 165; Goyer et al. 1981, p. 85 and 106). The effect of water hardness on ethoxylate and ethoxy- sulfate toxicity is less certain, however. Studies by Maki and Bishop (1979) and Maki et al. (1979) using Daohnia and Cj^EOy suggest a slight decrease in EO toxicity with increased water hardness (as reported in Goyer et al. 1981, p. 161). However, no such trends were apparent in similar studies by Procter and Gamble Company (unpublished data, as reported in Goyer et al. 1981). No intra-species, water hardness data were available for EOS. 4.2 Biodearadabilitv It is generally agreed in all reports reviewed (Shell a and b; Arthur D. Little, Inc. 1977, Goyer et al. 1981) that" the linear primary alcohol-based surfactants do not persist in laboratory or field tests. Even slightly branched or secondary structures are easily degraded, albeit at a somewhat slower rate (Table 1). Concentrations of EO as high as 1000 mg/L in shake flask tests simulating spills, were 70 to 80% degraded in three days (Kravetz et al. 1979, as reported in Shell a, p. 5). Goyer et al. (1981, p. 143) suggests, however, that a study using an atmosphere containing 70% oxygen to enable "complete surfactant oxidation to C02n may not be indicative of degradation rates occurring in the same time period under natural conditions. Ethoxysulfates added to activated sludge were completely metabolized to carbon dioxide and water within five to ten days (Mlura et al. 1979 and Itoh et al. 1979, as reported in Goyer et al. 1981, p. 195). Numerous other studies using sludge or river, estuarine or ocean waters have demonstrated the rapid breakdown of these compounds. Degradation of ethoxylates has been shown to be generally faster in saltwater than in freshwater, and faster in freshwater at high temperatures than at lower temperatures (Schoberl and Mann, 1976, as reported in Goyer et al. 1981, p. 142). The degradation rate of ethoxylates 13 ------- is also influenced by the length of the EO chain; increased length of the chain caused degradation to be slower, especially in freshwater at low temperature. Ethoxylates having 100 EO units/mole of alcohol biodegrade considerably slower (20% ultimate biodegradation in 21 days) than those having up to 30 EO units/mole of alcohol (90% or more in 21 days) (Kravetz et al. 1979, as reported in Shell p. 5; Goyer et al. 1981, p. 144). Shell claims to market only products having a maximum of 13 EO units/mole (NEODOL 45-13). Biodegradation was essentially complete 10 days after DOBONOL 45-7, simulating a spill condition, was added to an activated sludge medium (Cook 1979, as reported in Shell a, p. 5). Degradation results In a rapid loss of toxicity of surfactants to aquatic organisms. Products resulting from EO biodegradation were much less toxic to rainbow trout and goldfish than were the parent compounds (Reiff 1976 and Kurata et al. 1977, as reported in Goyer et al. 1981, p. 153). Maki et al. (1979, as reported in Goyer et al. 1981, pp. 151 and 152) concluded that initial concentrations of 3 mg/L or less of C14.5 E07 in stream water effluent was non-toxic to fathead minnows within 24 hours. • At 10 mg/L, toxicity was observed for five days in stream water and for two to three days in secondary effluent. NEODOL-type surfactants are readily utilized as a carbon (energy) source by bacteria present in activated sludge and natural waters (Shell a p 5). 4.3 Exposure By comparing an organism's sensitivity to a chemical with the concentra- tion of that chemical likely to be present in the environment, one can often predict with reasonable accuracy the potential threat posed by the chemical to the organism. Modeling techniques have been used to estimate surfactant concentrations in 20 estuarine locations (Maki 1979b, as reported in Goyer et al. 1981, pp. 163 and 164). Estimated maximum EO concentrations ranged from 0.2 ug/L in Penobscot Bay, Maine to 19.8 ug/L in the Hudson River; the geometric mean for all estuaries was 3.2 ug/L. It should be noted that these values are probably high because the model was provided with an elevated 14 ------- estimate of inflow from sewage treatment plants. Further, degradation was not factored in. Comparing these estimated concentrations with the acute sensitivities of test species, it appears unlikely that, short of a direct spill, concentra- tions of surfactants acutely dangerous to aquatic organisms will be attained in the environment. 5.0 MAMMALIAN TOXICITY 5.1 Acute Effects All LDso data reviewed indicate that, at their worst, NEODOL surfactants are moderately toxic (0.5 to 5 g/kg) when rated according to Gosselin et al . (1976, as reported in Shell b, p. 10). LDsgs for all types of surfactants generally exceed 1.0 g/kg. Alcohols appear to be the least toxic (oral 1050$ >5 g/kg), becoming more so with either sulfation or ethoxylation. Sulfation, however, decreases the toxicity of alcohol ethoxylates (Shell b, pp. 9-11). Acute oral toxicity studies with rats indicate that the degree of ethoxylation has some influence on toxicity. For example, NEODOL 91-2.5 produced LDsgs ranging from 2.7 to 10 g/kg (Shell Internal Reports HSE-78- 0156, TLGR.124.79, and TLGR. 088.80, as reported in Shell b, p. 11), whereas NEODOL 91-8 was more toxic, exhibiting LDsgs of 1.0 or 2.7 g/kg (Shell Internal Reports TLGR. 088. 80 and TLGR. 0024. 76, as reported in Shell b, p. 4). The length of the alkyl chain does not appear to influence the acute toxicity of alcohol ethoxylates (Shell b, Table V, p. 12). Skin and eye irritation tests with rabbits have demonstrated that NEODOL surfactants, except the alcohols, are generally severe irritants at high or undiluted concentrations (Shell b, pp. 17 and 20). Shell b (p. 21), however, reports that when directions are followed, actual use concentrations for NEODOL products are <0.04%. At 0.1% dilutions, NEODOL products tested ranged from non-irritating for alcohols and alcohol sul fates to non-irritating to mildly irritating for alcohol ethoxylates (Shell b, p. 21). 15 ------- Most NEODOL products produced negative results in skin sensitization tests (Shell b, p. 25, Table XIV). Most exceptions showed some, weak or moderate, sensitivity in one type of test but none in other tests. By contrast, NEODOL 25-3 was found to be a very weak sensitizer in the Maximiza- tion Test (Shell b, p. 25). Results of repeated-insult patch tests of NEODOL products in human volunteers agree with most observations in animal studies that NEODOL products are not skin sensitizers (Shell b, pp. 25 and 27). 5.2 Subchronic Effects Available data indicate that effects of subchronic exposures to surfac- tants mainly involve changes in organ and body weights. Studies exposing rats for 16 weeks to a diet containing C12 sulfate (4% of the total diet) resulted in reduced body weights (Arthur D. Little, Inc. 1977 and 1981 and Fitzhugh and Nelson 1948, as reported in Shell b, p. 29). Compared to controls, ethoxy- lates (C13E06 and C14E07) produced elevated.liver weights in rats exposed to concentrations equivalent to 1% of the total diet (Brown and Benke 1977, Arthur D. Little, Inc. 1977, and Goyer et al. 1981, as reported in Shell b, p! 29). Lower body weight was also observed with exposure .to C13E06. Other subchronic feeding studies exposing rats to sulfates and ethoxysulfates produced no major biological effects at concentrations up to 0.1% of the diet for 13 weeks (Shell Internal Report R(T)-12-66 and Walker et al. 1967, as reported in Shell b, p. 29). Increases in serum urea or protein concentra- tions and increases in some organ weights occurred at concentrations of 0.5% of the diet. Because histopathology was normal, these effects were considered minor. Another type of effect observed was slight inhibition of the progression of cholesterol-induced atherosclerosis in rabbits (Kivak et al. 1975 as reported in Goyer et al. 1981). The mechanism of action is not known, although a reduction in accumulation of cholesterol esters in aortic tissue was suggested as a possibility (Morin et al. 1974, as reported in Goyer et al 1981). 16 ------- 5.3 Chronic Effects The few data available on the chronic effects of surfactants do not demonstrate any alarming effects. One or two year studies using 1.0% alcohol sulfate (Goyer et al. 1981, p. 118) or 0.5% alcohol ethoxysulfate (Arthur D. Little, Inc. 1977, p. 377), respectively, in the diets of rats have produced no adverse effects. However, 1% alcohol ethoxylate, C^-is £05.5, added to the diets of rats for two years resulted in reduced body weight, elevated organ to body weight ratios for liver, kidney, brain, and heart in females and for liver in males and increased incidence of focal myocarditis, a common spontaneous lesion found in aging populations of rats (Procter and Gamble, unpublished data, as reported in Goyer et al. 1981, p. 174). Food consumption was also reduced in groups having reduced body weights, and was attributed to poor palatability of the diet. Reduced body weights and increased organ to body weight ratios also occurred in females at the 0.5% treatment level. A second feeding study using as much as 1.0% Ci4_15 EO; in the diets of rats for two years resulted in reduced body weight gains for females and males, and in decreased absolute organ weights for liver, kidney, heart, and thyroid/ parathyroid glands in females and for brain and adrenals in males in the 1% treatment groups. Gross incidences of focal myocarditis increased with increasing treatment levels for all groups of rats at 12 months, but severity of lesions was not treatment-related (Proctor and Gamble, unpublished data, as reported in Goyer et al. 1981, p. 175). Eighteen months exposure to repeated dermal applications of up to 5.0% C^-iaEOe^ produced no notable results in ICR Swiss mice (Procter and Gamble Company, unpublished data, as reported in Goyer et al. 1981, p. 176). 5.4 Carcinoaenicitv No evidence for carcinogenic potential of NEODOL products has emerged from the limited data available from long-term oral or dermal studies exposing rats or mice to C12_i3 E06<5 or C14.15 E07 (Proctor and Gamble Company, unpublished data, as reported in Goyer et al. 1981, pp. 174-176); C^S (Goyer et al. 1981, p. 119); or C12E03S (Tusing et al. 1962, as reported in Arthur D. Little, Inc. 1977, p. 378). 17 ------- 5.5 Mutaqenicltv Mutagenicity has not been demonstrated for any NEODOL product tested with in vitro or jn vivo mammalian systems or in bacterial or yeast systems. The following NEODOL products have been tested for mutagenicity: C12ave AS (Hope 1977, as reported in Goyer et al. 1981, p. 120); n-pri-C12_13E03 (Shell Toxicology Laboratory unpublished data, as reported in Goyer et al. 1981, p. 177); CJ2-15EOS (Hope 1977, as reported in Goyer et al. 1981, p. 209); C12_ 13E02.5S (53:43) (Inoue et al. 1980, as reported in Goyer et al. 1981, p. 210); and n-pri-C12-i5E03S (Shell Research Limited, unpublished data, as reported in Goyer et al. 1981, p. 210). 5.6 Teratooeni ci tv/Reproducti on Few teratogenesis/reproduction studies have been performed with NEODOL products; no teratogenesis studies have been performed with AES administered alone. However, formulations containing AES administered orally to mice, rats, or rabbits have produced no teratogenie effects (limori et al. 1973, Iseki 1972, Nolan et al. 1975, and Palmer et al. 1975 as reported in Arthur D. Little, Inc. 1977, p. 379). Results from testing the following chemicals have shown no cause for concern: C14.15 E07 and C12E06 (Proctor and Gamble unpublished data, as reported in Arthur D. Little, Inc. 1977, p. 322) and C12E03S (Tusing et al. 1962, as reported in Arthur D. Little, Inc. 1977, p. 378). An alcohol sulfate whose chain length was not identified has also been tested .(Nomura et al. 1980, as reported in Goyer et al. 1981, p. 119). Dermal applications of 10 to 20% concentrations of the alcohol sulfate to pregnant mice on days 1 to 10 of gestation interfered with embryonic development at the cleavage stage. Applications of 2% on days 1 through 17 also reduced the number of pregnancies, but the number of animals compared was too small to be statistically significant. Dermal applications of 10% alcohol sulfate twice a day prior to implantation (days 0 to 3) resulted in an elevated incidence of deformed embryos, compared to controls (29.1% vs 4.9 of 0 in controls) (Nomura 18 ------- et al. 1980, as reported in Goyer et al. 1981, p. 120). Dermal application of the alcohol sulfate during late pregnancy did not interfere with gestation. More tests, especially with AES products, are necessary before conclu- sions can be reached about the teratogenic potential or reproductive effects of surfactants. 5.7 Studies in Humans Studies using human volunteers have demonstrated the skin irritation properties of NEODOL products (Shell b, p. 27). In most cases, 1% dilutions caused very slight to mild Irritation with repeated exposures. Alcohol ethoxylates appear to be the least irritating, with only non-to-mild irrita- tions caused by repeated exposures to dilutions up to 25%. Use of certain alcohol ethoxylates as analgesics and anesthetics have caused no adverse reactions in humans (Goyer et al. 1981, p. 130). 5.8 Metabolism Alcohol sulfates, short-chain ethoxylates, and ethoxysulfates (Goyer et al. 1981, pp. 121, 178, and 211, respectively) are readily absorbed when administered orally to rats, and are primarily excreted in urine. Increasing the alkyl chain length of an ethoxylate decreases its excretion in urine and feces, and increases the amount in expired air (Goyer et al. 1981, p. 178). Increasing the length of the EO unit of an ethoxysul fate causes it to be poorly absorbed and excreted primarily unchanged in the feces (Arthur D. Little, Inc. 1977, p. 381). Cutaneous absorption of alcohol ethoxylates (about 50%) is somewhat slower than absorption after oral administration (>75%) (Drotmann 1977 and 1980, as reported in Shell b, p. 33). Dermal absorption of similar alcohol ethoxylates is greater than dermal absorption of alcohol sulfates or ethoxy- sul fates (Black and Howes 1979, as reported in Shell b, p. 33). Maximum absorption of alcohol sulfates on human callus occurred with a chain length of 12 carbons (Dominguez et al. 1977, as reported in Goyer et al. 1981, p. 123). 19 ------- After application of 100 mg of an alcohol ethoxylate (C12E06) to human skin, most (81% average) was recovered from swabbing the skin after 144 hours (Drotman 1980, as reported in Goyer et al. 1981, p. 180). 6.0 CONCLUSIONS 6.1 Toxicitv to Non-Mammalian Organisms Certain structure-activity relationships have been delineated for the alcohol-derived surfactants in aquatic systems (see Table 1). As the number of carbon atoms in the alkyl chain of straight-chain alcohols increases, the toxicity of the alcohol decreases. When the (EO) chain length of alkyl ethoxylates remains the same, an increase in the alkyl chain length increases toxicity. Conversely, when the alkyl chain remains the same, an increase in the EO chain length decreases toxicity (as opposed to the response of labora- tory rodents). The sulfation of the end EO group reduces the acute toxicity of these compounds by a factor of more than 20 compared to the parent ethoxy- late compound. Alcohol sulfates also appear to be less acutely toxic to aquatic organisms than are the alcohol ethoxylates. Although anionic surfac- tants are less acutely toxic than nonionic surfactants, fish have a greater ability to recover after exposure to nonionic surfactants than to anionic surfactants. Surfactants have been shown to cause a variety of sublethal effects in aquatic organisms, such as changes in ventilation rates, inhibition of larval development and immobilization. The limited data available on the chronic effects of surfactants (mainly the ethoxylates) indicate that growth inhibition and altered respiratory rates in crustaceans can be caused by long-term exposures. In general, exposure for several months to concentrations exceeding 0.2 mg/L can cause adverse effects in aquatic animals. Surfactants have been shown to inhibit the growth and development of aquatic microflora and higher plants such as barley and rye. 20 ------- Due to dissolution of the waterproofing oils on their feathers, waterfowl may be at increased risk of hyperthermia if exposed to surfactants. NEODOLs and the other alcohol-based surfactants do not persist in aquatic environments, and are readily biodegraded to apparently non-toxic inter- mediates, then to carbon dioxide and water. Short of a direct spill, concen- trations of surfactants reaching waterways would be substantially lower than those that are acutely toxic to aquatic organisms. Effects of repetitive exposures to surfactants have not been adequately studied. Additional toxicity tests should focus on the effects of continuous exposure of early life stages of test organisms to low concentrations of surfactant, a situation such as might exist near a sewage outfall or drainage/ overflow conduit. The effects of 1,4-dioxane contamination of ethoxysulfates on aquatic organisms cannot be determined from available data. 6.2 Mammalian Toxicitv In general, NEODOL products exhibit a low order of toxicity to mammals in toxicity tests (see Table 2). At worst, acute toxicity can only be labeled moderate, except in the cases of skin or eye irritations which are often severe for undiluted derivitized NEODOL products. However, dilutions of 0.1% are generally non-irritating, and according to Shell, use concentrations are only <0.04%. NEODOL alcohols, which are the least acutely toxic to mammalian systems, become more toxic with either sulfation or ethoxylation. Sulfation of an ethoxylate, however, decreases toxicity. Length of the alkyl chain does not appear to play a significant role in acute toxicity of alcohol ethoxylates. Subchronic and chronic dietary tests resulted in reduced body weights and increased organ to body weight ratios for some organs. There was no evidence of carcinogenicity or mutagenicity for any NEODOL product tested. 21 ------- TABLE 2. Effects of NEODOl(R) products In laboratory mammals Alcohol Sulfates Alcohol Ethoxylates Alcohol Ethoxysulfates ro ro Acute LOcn (g/kg) Skin irrita- tion (rabbits) Eye irritation (rabbits) Subchronic Oral or dermal, rats, or rabbits, >1; commercial use dilutions between 5 and 15. 0.1% dilution, non- irritating; >10% dilution, severe. Undiluted, severe to extreme. 4% given in diet for 16 weeks reduced body weight of rats; cumulative skin irritation; daily inges- tion of 250 mg/kg for two months slightly inhibited progression of choles- terol-induced athero- sclerosis in rabbits. Oral, rats, 0.87 to >10; dermal, rats or rabbits, >2; inhalation (4 hrs. exposure) rats, between 1.5 and 3 mg/L. 0.1%, non-irritating to mild; >10%, mild to severe. >10%, practically non- irritating to extreme; 0.1% non-irritating. 1% given in diet for 13 weeks reduced body weight, increased liver weight of rats. Oral, rats, 1.7 to 5; dermal, rabbits, 4.7 to 12.9. 0.1%, non-irritating to minimal; undiluted, mild to severe. Undiluted, severe; 0.1% non-irritating. 0.5% given in diet for 13 weeks increased kidney, liver, and heart weights in female and kidney weights in male rats; repeated skin (guinea pigs and rabbits) exposure to 10% dilutions, severe irritation; 1% no reac- tion. ------- TABLE 2. Effects of NEODOlW products In laboratory mammals (Continued) Alcohol Sulfates Alcohol Ethoxylates Alcohol Ethoxysulfates Chronic Carcinogenic ro Mutagenic 1% in diet, rats, one year, no adverse effects. No evidence from long-term feeding studies in rats or skin-painting tests in mice. No effects on chromosomes of rat bone marrow cells from 90 day diet of maximum tolerated dose (1.13% active ingredient). 1% in diet, rats, two years, reduced body weight, elevated organ to body weight ratios, increased incidence of focal myocarditis. 5% dermal application to mice for 1.5 years, no notable results. No evidence from long-term feeding tests in rats or from long-term percu- taneous administration to mice. No evidence from in vitro and host-mediated mutagen- icity tests. 0.5% in diet, rats, two years, no adverse effects. No evidence from two-year feeding (0.5%), drinking water (0.1%), or skin- painting (5.0%) studies. No effects on choromosomes of rat bone marrow cells from 90 day diet of maximum tolerated dose (1.13% active ingredient). No evidence from hamster embryo cell culture or yeast or bacteria studies. ------- TABLE 2. Effects of NEODOlW products In laboratory mammals (Continued) Teratogenic/ Reproductive Alcohol Sulfates No evidence from ingestion of up to 300 mg/kg during gestation. Daily skin application of 20% to pregnant mice on days 1 to 10 interfered with embryonic development; 10% 2 times/day, pregnant mice, days 0 to 3, elevated incidence of deformed embryos. Doses severely toxic to dams reduced litter size and caused fetal loss in mice but not in rats or rabbits. Alcohol Ethoxylates No evidence from feeding (up to 0.5%) studies in rats or rabbits. Alcohol Ethoxysulfates No data on AES admini- stered alone. No evidence from oral administration of formulations containing AES to mice, rats, or rabbits. No adverse reproductive effects from 0.1% in the diets of rats for two generations. ------- Data are generally lacking on teratogenic/reproductive effects. Data available from a limited number of feeding studies indicate no teratogenicity for any of the NEODOL products tested. However, repeated dermal exposure of mice to high concentrations of an alcohol sulfate during early gestation interrupted cleavage of eggs and retarded fetal development. Further studies should be performed to clarify the teratogenic potential and/or reproductive effects of NEODOL products. Animal studies show that, in general, NEODOL products administered orally are readily absorbed, metabolized, and primarily excreted in the urine. Cutaneous exposure, the usual route of exposure to most surfactants, results in slower absorption of alcohol ethoxylates. 6.3 1.4-Dioxane Contamination There is concern because 1,4-dioxane is a contaminant of some NEODOL products. Shell (May 7, 1980 memorandum to G.T. Youngblood) claims that 1,4- dioxane (OCH2CH20CH2CH2) is present only in their EOS products, and postulates that it is formed during sulfation of the EO and that the presence of a polyoxyethylene chain and a highly acidic agent, such as sulfur trioxide, are required. The typical potential exposure for an adult female is estimated to be 1.65 x 10'8g/kg/d from hair shampoo and 7.56 x 10"10 g/kg/d from light duty liquid (Shell c 1980, Appendix B-3). Worst case estimates are 1.12 x 10" 7g/kg/d for shampoo and 6.68 x 10~9g/kg/d for light duty liquids. It is impossible to determine from the data provided whether dioxane contributes to the observed EOS toxicity. However, dioxane contamination does not alter the significance of the toxicity of NEODOL products, for it appears that it is often the dioxane-contaminated products (EOS) to which environ- mental species are exposed. It would be useful to compare the toxicities of contaminated samples with purified samples. 25 ------- 7.0 REFERENCES Abram F.S.H., et al. 1977. (Shell Laboratories Amsterdam). The biodegrad- ability of two primary alcohol ethoxylate non-ionic surfactants under practi- cal conditions, and the toxicity of the biodegradation products to rainbow trout. 4th Yugoslav Symposium on Surface Active Substances. Dubrovnik (Yugoslavia). October, 1977. (As reported in Shell a). Antonielli M., Lupatteli M. 1977. Un test orzo per misurare Tazione biologica di detergenti e.detersivi. [A barley test for measuring the biological action of detergents and detersives]. Agrochemica 21:15-22 (as reported in Goyer et al. 1981). Arthur D. Little, Inc. 1977. Report to the Soap and Detergent Association. Human safety and environmental aspects of major surfactants. National Technical Information Service. PB-301-193. Springfield, VA. 546 pp. Arthur D. Little, Inc. 1978. 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Procter and Gamble Company, unpublished data (as reported in Goyer et al 1981). 32 ------- Reiff B. 1976. The effect of biodegradation of three nonionic surfactants on their toxicity to rainbow trout. 7th International Congress on Surface Active Substances. Moscow, USSR. September 12-18. (As reported in Shell a and Goyer et al. W81). Reiff B., Lloyd R., How M.J., Brown D., Alabaster J.S. 1979. The acute toxicity of eleven detergents to fish: Results of an inter!aboratory exer- cise. Water Res 13:207-210. (As reported in Shell a and in Goyer et al. 1981). Rockstroth T. 1967. Uber die Wirkung von Detergent!en auf die Morphologic einer Ziliatenzelle. Acta. Biol. Med. German. 19(1):161-184. (As reported in Arthur D. Little, Inc. 1977). Satkowski W.B., Huang S.K., Liss R.L. 1967. Polyoxyethylene alcohols. Chapter 4. In. Nonionic surfactants. Surfactant Science Series, vol. 1. Schick M.J., ed. New York, NY: Marcell Dekker, Inc. (As reported in Arthur D. Little, Inc. 1977). Schoberl P., Mann H. 1976. Temperature—Eisfluss auf des biologischen abbau nicht-ionischer tenside in see-und susswasser. [The influence of temperature on the degradation of nonionic tensides in sea-and freshwater]. Arch Fisch Wiss 27(2):149-158. (As reported in Goyer et al. 1981). Shell a. Shell Chemical Company (FYI-AX-0685-0410 Sequence A). Aquatic safety of NEODOL(R) products. 37 pp. Shell b. Shell Chemical Company (FYI-AX-0685-0410 Sequence A). Human safety of NEODOL(R) products. 40 pp. Shell c. Shell Chemical Company. 1980. (8EHQ-0580-0326 Sequence C). 1,4 Dioxane in alcohol ethoxysulfate products. 90 pp. Shell d. Shell Chemical Company, unpublished data (as reported in Goyer et al. 1981). 33 ------- Shell Chemical Company. 1980. Interoffice Memorandum from J.J. Coyle to G.T. Youngblood. Shell Internal Report. EC01 Program. Summer 1973-Spring 1974. (As reported in Shell a). Shell Internal Report. 1971. Toxicity of surfactants to fishes. (As reported in Shell a). Shell Internal Report EMGR.0138.71. Dispersants for dealing with oil spill- ages. Development of a low toxicity product. Part 1. (As reported in Shell a). Shell Internal Report EMGR.0150.71. Dispersants for dealing with oil spill- ages. Development of a low toxicity product. Part III. (As reported in Shell a). Shell Internal Report EMGR.0162.71. Dispersants for dealing with oil spill- ages. Development of a low toxicity product. Part III. (As reported in Shell a). Shell Internal Report HSE-78-0156. Rat acute oral toxicity NEODOL 91-2.5 (as reported in Shell b). Shell Internal Report R(T)-12-66. The comparative toxicity of some biode- gradable detergent materials (as reported in Shell b). Shell Internal Report TLGR.0052.77. The acute toxicity of Dobanol 25 to rainbow trout. (As reported in Shell a). Shell Internal Report TLGR.0064.77. The acute toxicity of Dobanol 45-18 to rainbow trout (as reported in Shell a). Shell Internal Report TLGR.0066.77. The acute toxicity of Dobanol 91-5 to rainbow trout. (As reported in Shell a). 34 ------- Shell Internal Report TLGR.0079.068. The acute toxicity of Dobanol 91-2.5 to rainbow trout. (As reported in Shell a). Shell Internal Report TLGR.0088.80. Toxicology of detergents: The acute toxicity of Dobanol ethoxylates: 91-2.5, 91-5, 91-6, 91-8 (as reported in Shell b). Shell Internal Report TLGR.0124.79. Toxicology of detergent intermediates: acute mammalian toxicity, skin and eye irritancy and skin sensitizing poten- tial of Dobanol 91-2.5 (as reported in Shell b). Shell Internal Report TLGR.0161.78. The acute toxicity of Dobanol 23 to rainbow trout. (As reported in Shell a). Shell Internal Report. TLGR.0162.78. .The acute toxicity of Dobanol 45 to rainbow trout (as reported in Shell a). Shell Internal Report TLGR.0166.78. The acute toxicity of Dobanol 91 to rainbow trout. (As reported in Shell a). Shell Research Limited, unpublished data (as reported in Goyer et al. 1981). Shell Toxicology Laboratory, unpublished data (as reported in Goyer et al. 1981). Swisher R.D. 1970. Surfactant Biodegradation. Surfactant Science Series, vol. 3. New York, NY: Marcel Dekker, Inc. (As reported in Arthur D. Little, Inc. 1977). Taniyama T., Nomura T. 1978. Effects of various synthetic detergents on photosynthesis, dry matter, and grain production in rice plants. Mi Daigaku Kankyo kaguku Kenkyu kiyo. 3:93-104. (As reported in Goyer et al. 1981). Tusing, T.W., Paynter, O.E., Opdyke, D.L., Snyder, F.H. 1962. Toxicologic studies on sodium lauryl sulphate, sodium lauryl ethoxysulphate and corre- 35 ------- spending surfactants derived from synthetic alcohols. Fd Cosmet Toxicol 5:763-769 (as reported in Arthur D. Little, Inc. 1977). Ukeles R. 1965. Inhibition of unicellular algae by synthetic surface-active agents. J. Phycol. 1:102-110. (As reported in Arthur D. Little, Inc. 1977). Unilever Research Laboratories, unpublished data. (As reported in Arthur D. Little, Inc. 1977). U.S. Department of the Interior. Letter to Shell Development Co. Subject: Toxicity data for selected Neodol products. September, 1968. (As reported in Shell a). i U.S. Food and Drug Administration/Master File (MFJ-122 Shell Drug Master File on NEODOL alcohols and ethoxylates (as reported in Shell a). Valoras N., Letez J. 1978. Screening of Neodal chemicals for potential use in erosion control. Report of the University of California, Riverside, to Shell Chemical Co., Houston, Texas, Manuscript. (As reported in Goyer et al 1981). Walker A.P., Ashforth, 6.K., Davies, R.E., Newman, E.A. and Ritz, H.L. 1973. Some characteristics of the sensitizer in alkyl ethoxy sulphate. Acta Dermatovener 53:141-44 (as reported in Arthur D. Little, Inc. 1977). Walker A.I.T., Brown V.K.H., Ferrigan L.W., Pickering R.G., Williams D.A. 1967. Toxicity of sodium lauryl sulfate, sodium lauryl ethoxysulfate, and corresponding surfactants derived from synthetic alcohols. Food Cosmet Toxicol 5:763-769. (As reported in Shell b). Wright A. 1976. The use of recovery as a criterion for toxicity. Bull Environ Contam Toxicol 15(6):747-749. (As reported in Goyer et al. 1981). 36 ------- APPENDIX A. Acute toxlclty of alcohol surfactants to aquatic animals Exposure (hours) Surfactant LC50 (mg/L) Reference Daphnia maqna 24 C12_13E06.5 CO C12-15E09 C14E08 C12-14E07.4 C12-14E06.3 (39%) C12-14E011 NaC12-14AS NaC^aveAS (Ziegler derivative) C12-14E03S (Ammonium salt) C12-14E03S (Sodium salt) 0.57 1.1 1.71 2.0 2.3 2.5 3.3 5.0 5.1 6.3 13.5 16.3 18.9 Shell Internal Report 1974. ECO 1 Program Arthur D. Little, Inc. 1978 Shell Internal Report 1974. ECO 1 Program Arthur 0. Little, Inc. 1978 Arthur D. Little, Inc. 1978 Arthur 0. Little, Inc. 1978 Shell Internal Report 1974. ECO 1 Program Lundahl et al. 1972 Arthur D. Little, Inc. 1978 Arthur D. Little, Inc. 1978 Lundahl et al. 1972 Continental Oil Co., unpublished data Continental Oil Co., unpublished data ------- APPENDIX A. Acute toxldty (LC50) of alcohol surfactants to aquatic animals (continued) Exposure (hours) Surfactant LC5o (mg/L) Reference to 00 Daohnia maana 24 Cn.16E03S 48 96 C14.15E07 C12-14E02.2S (Natural alcohol derived) Ci2E03S (Ziegler derived) C14E03 C14E02 C14E04 C14EOg Blueaill sunflsh (Leooomis macrochirusl 24 19.6 (average) 0.36 (average) 21 37 0.73 0.83 1.53 1.76 4.17 10.07 0.3 1.8 Unilever Research Laboratories, unpub- lished data Goyer et al. 1981 Lundahl et al. 1972 Lundahl et al. 1972 U.S. Food and Drug Administration U.S. Food and Drug Administration U.S. Food and Drug Administration U.S. Food and Drug Administration U.S. Food and Drug Administration U.S. Food and Drug Administration Procter and Gamble Company, unpublished data U.S. Dept. of Interior 1968 ------- APPENDIX A. Acute toxlclty (LC50) of alcohol surfactants to aquatic animals (continued) Exposure (hours) Surfactant LC50 (mg/L) Reference Blueaill sunfish (Leooomis macrochirus) C12-15E09 CO vo C12-13E°6.5 Ci4E03S C12-15E09 (75% linear primary) C14-18E09 1.87 2.4 (average) 1.9 <2.1; <2.4 2.45; 2.36 4.3 <5.7; <7.5 7.1 8.0 10 Shell Internal Report 1974. ECO 1 Program U.S. Dept. of Interior. 1968 Procter and Gamble Co., unpublished data Procter and Gamble Co., unpublished data Shell Internal Report. 1974. ECO 1 Program Procter and Gamble Co., unpublished data Procter and Gamble Co., unpublished data Procter and Gamble Co., unpublished data Cook Research Laboratories 1966 Cook Research Laboratories 1966 ------- APPENDIX A. Acute toxldty (LC50) of alcohol surfactants to aquatic animals (continued) Exposure (hours) Blued ill 24 Surfactant sunflsh (Leopomls macrochlrus) C17.9E°1.9S C12-15E09 (98% linear primary) C19.6E01.1S Ci3E03S C12-15E03A Cl2-15E03S C12E03S C12E03S C12E02.iS C8E03S LC50 (mg/L) 10.8 11.0 15 24 32 32 37 73 87 >250 Reference Procter and Gamble Co., unpublished data Cook Research Laboratories 1966 Procter and Gamble Co., unpublished data Procter and Gamble Co., unpublished data Shell Internal Report 1971 Shell Internal Report 1971 Procter and Gamble Co., unpublished data Procter and Gamble Co., unpublished data Procter and Gamble Co., unpublished data Procter and Gamble Co., unpublished data ------- APPENDIX A. Acute toxlclty (1X50) of alcohol surfactants to aquatic animals (continued) Exposure (hours) Surfactant Blueaill sunfish (Leopomis macrochirus) C10E02tlS 96 NH4C15AS, branched NH4C12.i4AS NH4C15AS NaC12AS NaC12AS NH4C15AS NH^nAS, branched NH4Ci3AS, branched NH4C12AS "50 375 2 3 3 4 4 5 16 18 20 .13 .2 .39 .5 .83 .19 .5 .4 .3 («ng/L) (1 (2. (2 .37-3. 8-3.7) .59-4. 3D 43) Procter data Procter data Procter data Procter data Reference and Gamble and and and Bishop and (4 (3 (13 (15 (16 .06-5. .97-6. .1-21. .2-22. .0-25. 75) 77) 0) 2) 7) Procter data Procter data Procter data Procter data Procter and and and and and Gamble Gamble Gamble Perry Gamble Gamble Gamble Gamble Gamble Co., Co., Co., Co., 1979 Co., Co., Co., Co., Co., unpublished unpubl ished unpublished unpubl unpubl unpubl unpubl ished ished ished ished unpublished unpubl ished data ------- APPENDIX A. Acute toxlclty (LC50) of alcohol surfactants to aquatic animals (continued) Exposure (hours) Surfactant ro Blueaill sgnfi^ (LeoDomis macrochirus) NH4C16AS NH4CHAS C16-18AS NaCjAS Rainbow trout (Salmo qalrdneri) 96 C14_15E07 C12-15E°9 C12-14E°10.5 C12.i5E03 C12-13E°2 C14-15E°11 LC50 (mg/L) Reference 21.7 (16.7-28.1) Procter and Gamble Co., unpublished data 26.0 (19.0-35.4) Procter and Gamble Co., unpublished data. 76.0 (50-116) Procter and Gamble Co., unpublished data. 1000 0.8 0.9 1.2 1.8 and 0.8 1.3 and 1.7 1 - 2 1.8 - 2.5 Procter and Gamble Co., unpublished data. Abram et al. 1977 Reiff 1976 U.S. Dept. of Interior. 1968 Reiff et al. 1979 Shell Internal Report, TLGR 113.78 Shell Internal Report, TLGR 0115.78 Reiff 1976 ------- APPENDIX A. Acute toxldty of alcohol surfactants to aquatic animals (continued) Exposure (hours) Surfactant LC50 (mg/L) Reference Rainbow trout I Sal mo oairdneri) C14-15E011 96 C12-i3 C14-15E018 C9-10E02.5 Cg-io C9-10E05 C12-15 C9-10E02.5S Fathead, minnow fPimeohales oromelasl 24 C16E06S C16E04S 1.1 2.7 4 - 10 5 - 6.3 5 - 7 6 - 10 8 - 9 8.9 (7.3-10.3) 28 (23-35) 45 400 - 450 0.8 0.9 Abram et al. 1977 Arthur 0. Little, Inc. 1978 Shell Internal Report, TLGR 0161.78 Shell Internal Report, TLGR 0064.77 Shell Internal Report, TLGR 79.068 Shell Internal Report, TLGR 0166.78 Shell Internal Report, TLGR 0066.77 Shell Chemical Co., unpublished data Shell Chemical Co., unpublished data Shell Internal Report, TLGR 0052.77 Shell Chemical Co., unpublished data Monsanto Co., unpublished data Monsanto Co., unpublished data ------- APPENDIX A. Acute toxlclty (LC50) of alcohol surfactants to aquatic animals (continued) Exposure (hours) Surfactant Reference Fathead minnow (Plmeohales promelas) Ci6E02S C12E02S C14E02S 24 C12_14E06.3 C12-14E°7.4 Ci8E06S C14E04S C14E06S Ci8E04S CnE04S C18E02S Goldfish (Carasslus auratus) 6 C12.14E08 C15E03.2S» branched 1.0 1.5 1.8 1.8 1.8 2.1 4.0 9.3 15 17 80 1.8 3.7 Monsanto Monsanto Monsanto Arthur D Arthur D, Monsanto Monsanto Monsanto Monsanto Monsanto Monsanto Co., unpublished data Co., unpublished data Co., unpublished data . Little, Inc. 1978 . Little, Inc. 1978 Co., unpublished data Co., unpublished data Co., unpublished data Co., unpublished data Co., unpublished data Co., unpublished data Reiff et al. 1979 Gafa 1974 ------- APPENDIX A. Acute toxlclty (LC50) of alcohol surfactants to aquatic animals (continued) Exposure (hours) Surfactant LC50 (mg/L) Reference U1 Goldfish fCarassius auratus) C12-14E010.5 nC14AS (92.4% AI) C12E04 C14E03S nC14AS (94.3% AI) C14AS (94% AI, branched) nC12-15AS (95.8% AI) C12-15AS Cn.15AS C14E03S (5% branched) C13E05 nC12-16AS (94-3 nC13AS (94.8% AI) C16E03.4S 4.3 5.0 5.2 6.0 6.3 7.8 7.8 7.8 8.1 8.1 8.5 12.0 18.3 41.0 Reiff et al. 1979 Gafa 1974 Marchetti 1964 Gafa 1974 Gafa 1974 Gafa 1974 Gafa 1974 Gafa and Lattanzi 1974 Gafa and Lattanzi 1974 Gafa 1974 Shell Internal Report, TLGR 79.068 Gafa 1974 Gafa 1974 Gafa 1974 ------- APPENDIX A. Acute toxlclty (LC50) of alcohol surfactants to aquatic animals (continued) o» Exposure (hours) Surfactant Goldfish I Carassius auratus) C14AS (98% AI, branched) Cl2E02.eS nC12AS (93% AI) C12E02.6S (5* branched) nC16AS (95.3% AI) 1 C12E02 C12E04 Ci2E06 C12E08 C12E010 C12E012 C12E014 Cl2«>i6 C12E018 «-C50 (mg/L) 49.1 55.0 60.0 66.5 >300 2 4 5 7 10 20 30 40 100 Reference Gafa 1974 Gafa 1974 Gafa 1974 Gafa 1974 Gafa 1974 Gloxhuber et al. Gloxhuber et al. Gloxhuber et al. Gloxhuber et al. Gloxhuber et al. Gloxhuber et al. Gloxhuber et al. Gloxhuber et al. Gloxhuber et al. 1968 1968 1968 1968 1968 1968 1968 1968 1968 ------- APPENDIX A. Acute toxlclty (LC50) of alcohol surfactants to aquatic animals (continued) Exposure (hours) ^^^^^^•^^•••M Goldfish 48 Surfactant LC50 (mg/L) fCarasslus auratus) . C12-15E09 (oxo-9™) 1.4 Cl2-15E<>9 (LA-9™) 1.9 C12-14E07 3.3 C12-14E09 5.1 C12-14E012 12.0 Reference Kurata et al. 1977 Kurata et al. 1977 Kurata et al. 1977 Kurata et al . 1977 Kurata et al. 1977 Hermit crab 48 C12-15E03 (30%, kerosene 85 solution) C12E01 (30%, Isopropanol «1000 solution) C12E03 (30%, Isopropanol <1000 solution) C12E09 (30%, Isopropanol «1000 solution) C14-15E03 (30%, Isopropanol <1000 Shell Internal Report, U.S. Dept. of Interior Shell Internal Report, Shell Internal Report, Shell Internal Reoort. EMGR 0150.71 1968 EMGR 0162.71 EMGR 0162.71 EMGR 0162.71 solution) ------- APPENDIX A. Acute toxlclty (1.650) of alcohol surfactants to aquatic animals (continued) Exposure (hours) Surfactant LC50 (mg/L) Reference Hermit crab 00 Brown shrimp 48 (30%, kerosene solution) C14E03 (30*» isopropanol solution) C16E09 (30*» isopropanol solution) C14EOg (30% ?) (30%, isopropanol solution) C14-15E01 (30%» isopropanol solution) C16-18E06 (30%» isopropanol solution) Cl6-18E09 (30%, isopropanol solution) C14-15E03 (30%t kerosene solution) <2000 1500 2000 2500 3500 3000-6000 4000 4000 50 Shell Internal Report, EMGR 0162.71 Shell Internal Report, EMGR 0162.71 Shell Internal Report, EMGR 0162.71 Shell Internal Report, EMGR 0162.71 Shell Internal Report, EMGR 0162.71 Shell Internal Report, EMGR 0162.71 Shell Internal Report, EMGR 0162.71 Shell Internal Report, EMGR 0162.71 Shell Internal Report, EMGR 0162.71 ------- APPENDIX A. Acute toxldty (LC50) of alcohol surfactants to aquatic animals (continued) Exposure (hours) Surfactant Brown shrimp • C12-15E03 (30%, kerosene solution) C12-15E03 (30%. Isopropanol solution) C14-15E03 (30%, Isopropanol solution) C14-15E01 (30%, Isopropanol solution) C12-15E09 (30%, Isopropanol solution) LC50 (mg/L) 20-30 200 200 500 >3300 Reference Shell Internal Report, EMGR 0150.71 Shell Internal Report, EMGR 0162.71 Shell Internal Report, EMGR 0162.71 Shell Internal Report, EMGR 0162.71 Shell Internal Report, EMGR 0138.71 ------- |