EPA-560/8-76-004 CONSIDERATIONS RELATING TO TOXIC SUBSTANCES IN THE APPLICATION OF MUNICIPAL SLUDGE TO CROPLAND AND PASTURELAND v A BACKGROUND SUMMARY PREPARED BY OFFICE OF Toxic SUBSTANCES ENVIRONMENTAL PROTECTION AGENCY WASHINGTON, D,C, 2f NOVEMBER 1976 ------- EPA-560/8-76-004 CONSIDERATIONS RELATING TO TOXIC SUBSTANCES IN THE APPLICATION OF MUNICIPAL SLUDGE TO CROPLAND AND PASTURELAND A Background Summary Prepared By Office of Toxic Substances Environmental Protection Agency Washington, D.C. 20460 November 1976 ------- TABLE OF CONTENTS Page Introduction 1 I. Municipal Sludge 2 II. Elements and Substances Found in Municipal Sludge 4 III. Plant Uptake of Chemical Substances from Municipal Sludge-Amended Soil 7 IV. Health Effects Aspects 13 Literature Cited 18 Appendix - Sludge Information Summary 23 LIST OF TABLES Table 1 - Trace Elements and Substances Found in Municipal Sludge 5 Table 2 - Factors Influencing Plant Uptake of Chemical Substances 8 Table 3 - Studies on Plant Uptake of Chemical Substances from SI udge-Amended Soi 1 9 Table 4 - Plant Uptake of Trace Elements from Other Substrates 12 ------- NOTICE This report has been reviewed by the Office of Toxic Substances, Environ- mental Protection Agency, and approved for publication. Approval does not signify that the contents necessarily reflect the views and policies of the Environmental Protection Agency. Mention of tradenames or commercial products is for purposes of clarity only and does not constitute endorse- ment or recommendation for use. This document is available to the public through the National Technical Information Service, Springfield, Virginia 22151. ------- INTRODUCTION Background information is presented pertinent to an assessment of the potential health hazards from toxic substances when disposing/utilizing municipal sludge on agricultural lands, particularly croplands and pasturelands where the products enter the human food chain. The report considers some of the toxic elements and synthetic organic chemical substances known to be present in municipal sludges. Only readily available information has been used. The report clearly does not represent an exhaustive review of the subject. Nevertheless, it is clear that applicable and available data on this subject are scarce adding to the uncertainties regarding the hazard potential associated with applying municipal sludge to cropland and pastureland. Potential difficulties which might be associated with bacterial and viral pathogens and radioactive substances present in municipal sludge are beyond the scope of the report. -1- ------- I. Municipal Sludge The volume of municipal sludge requiring disposal in the United States is estimated to be about 17,000 dry tons per day and is expected to increase over the next ten years, with the implementation of nation- wide secondary treatment, to be about 23,000 dry tons per day. Current disposal methodologies reported to the EPA Office of Water Programs Operations are presented in the Appendix. A review of that information has indicated that the quantity of sludge will increase by about 35% and that industrial users of municipal sewage treatment plants will increase by over 40% in the next 10 years. Industrial wastes are estimated to account for about 25% of municipal treatment plant influent nationally and may be near 100% in some localities. The toxic metal content of municipal sludge from various cities approaches the levels found in some industrial sludges. At present, it is estimated that 20% of the total municipal sludge produced is applied to croplands (see Appendix). Estimates of the amount of agricultural land area that would be used if all sludges were disposed/utilized for landspreading have been made. One estimate is that with a "typical" application rate of 20 tons/acre/year about 570 square miles would be required (Dean, 1973). This amounts to less than 1% per year of the total agricultural land areas of the United States. Other estimates of typical application rates range from 10 to 20 tons/acre/year but these vary considerably due to site-specific condi- tions. Some guidelines exist which limit applications based on fertil- 'izer rates of nitrogen. ] I The levels of trace elements and chemical substances found in munic- i ipal sludge can be highly variable even on a daily basis. The range of levels detected is quite wide, depending to a large degree on the type -2- ------- and quantity of industrial input to the municipal treatment plant (see p. 23). Considering purely domestic sludge to be free of trace element and chemical substance contaminants is not warranted. In sewer systems with no industrial connections there are inputs from hospitals, research laboratories, and dentist offices (mercury). Other sources of contaminants include motor oil additives; flow entrainment of lead, copper, cadmium, zinc, and antimony from water-carrying pipes; street runoff; detergents and laundry products; and consumer products, including pesticides and organics, flushed into the sewer. -3- ------- II. Elements and Substances Found in Municipal Sludge Table 1 lists some of the trace elements and chemical substances found in municipal sludge which may deserve attention from a health effects standpoint. The range of concentrations (dry weight) observed is indicated. The amount of sludge-analysis data is limited and the use of different analytical methodologies complicates the evaluation of the available data. The wide ranges observed have been attributed to the variable quantity and character of industrial input to different municipal treatment plants. References 1, 9, 13, 21, 25, 26, 27, 32, 47, 53, and 61 were used as sources in compiling table 1. Commercial "bagged sludge" soil conditioners derived from municipal sludge, such as Milorganite, also deserve consideration. Milorganite has been analyzed and found to contain what were considered high cadmium and chromium levels. Recent analysis of a sample by EPA Region X found cadmium at 117 mg/kg and chromium at 6,042 mg/kg. Home and hobbyist use of municipal sludge such as Milorganite can result in intensive application to small plots of land. Use is not limited to ornamental plants, but it has been applied to vegetable gardens as well. Home-grown vegetables are not subject to FDA monitoring, nor are contaminants in them diluted in family use by the commercial food distribution system. In season, they can form a major portion of a family's diet. As table 1 indicates, municipal sludges also may contain persistent organic chemical contaminants such as PCBs and chlorinated pesticides. Data are scarce on other organics present in municipal sludge largely due to lack of research in this area, although the range of contaminants (over 100) reported for drinking water is indicative of the compounds which could be present in municipal sludge. Typical drinking water contaminants which might be present in municipal sludges include halogenated j (mostly chlorinated) hydrocarbons, long chain hydrocarbons, benzenes and j polynuclear aromatics. Other classes of organic chemicals which appear ! to have a high potential for sludge contamination due to their persistence j in environmental waters include chlorobenzenes, chlorophenols, chlorinated paraffins, and halogenated cyclodiene flame retardants (Braude e£. al_., 1975). -4- ------- Table 1. TRACE ELEMENTS AND SUBSTANCES FOUND ) Elements Aluminum (Al) Antimony (Sb) Arsenic (As) Boron (B) Barium (Ba) Beryllium (Be) Bismuth (B1) Bromine (Br Cadmium (Cd Calcium (Ca Cerium (Ce) Cesium (Cs) Chlorine (Cl) Chromium (Cr) Cobalt (Co) Copper (Cu) Dysprosium (Dy) Erbium (Er) Europium (Eu) Fluorine (F) Gadollmlum (Gd) Gallium (Ga) Germanium (Ge) Gold (Au) Hafnium (Hf) Holmlum (Ho) Indium (In) Iodine Irldlum (Ir) Iron (Fe) Lanthanum (La) Lead (Pb) Lutecium (Lu) Magnesium (Mg) Manganese (Mn) Mercury (Hg) Range of Concentration (ppm dry weight) In Municipal Sludge 8,100-51,200 2.6-44.4 3.0-50 4-1 ,430 272-1066 <4-<15 0.03-55.8 13.7-165 2-1,100 1760-116,400 12.4-272 0.45-2.9 500-17.800 22-30,000 2-800 84-17,000 0.7-19.8 0.2-4.5 0.7-12.2 2.2-738 1.1-22.7 0.9-54 1.1-10.5 0.21-7.00 1.3-10.7 0.07-0.67 0.07-3.7 1.0-17.1 0.04-0.46 1,000-144,000 5,1-380 80-26,000 0.04-0.34 2,000-14,035 32-8,800 0.1-89 IN MUNICIPAL SLUDGE Concentration Range (ppm) In Unamended Soil (dry) 10,000-300,000 2-10 0.1-40 2-100 100-3,000 0.1-40 -- 1-10 0.01-7 7,000-500,000 __ 0.3-25 5-3,000 1-40 2-100 -_ __ 30-300 __ __ __ __ __ ^^ __ __ _«. __ 7.000-550,000 1-5,000 2-200 »_ 600-6.000 100-4.000 0.01-0.3 Mean level (ppm) In dry Soil 71,000 6 6 10 500 6 5 0.06 13,700 50 6 100 100 8 20 200 30 1 38,000 30 10 5,000 850 0.03 ------- A) Elements TABLE 1. (CONT.) Range of Concentration (ppm dry weight) In Municipal Sludge art I B) Molybdenum (Mo) Neodymium (Nd) Nickel (Ni) Nitrogen (N) Osmium (Os) Palladium (Pd) Phosphorus (P) Platinum (Pt) Protractlnlum (Pr) Rhenium (Re) Rubidnium (Rb) Ruthenium (Ru) Samarium (Sm) Scandium (Sc) Selenium (Se) Silver (Ag) Sodium (Na) Strontium (Sr) / Sulfur (S) Tantalum (Ta) Tellurium (Te) Terbium (Tb) Thorium (Th) Thulllum (Tm) Tin (Sn) Titanium (T1) Tungsten (N) Uranium (U) Vanadium (V) Ytterbium (Yb) Yttrium (Y) Zinc (Zn) Zirconium (Zr) Organics Aldrin Chlordane ODD DDT Dieldrin fluorescent whitening agents PCBs 1.2-1000 0.6-8.6 12-8,000 16,000-66,000 0.06-3.18 0.5-16.2 8,000-40,000 0.05-0.74 1.1-119 0.03-0.98 4.3-94.6 0.21-7.05 1.0-14.2 0.5-7.1 1.7-8.7 ND-960 567-8,800 ND-2,230 9,000-11,000 0.11-1.45 0.07-1.52 0.27-4.83 3.1-16.8 0.06-3.31 40-700 1080-4580 0.9-99.6 0.8-6.4 ND-2100 0.29-1.30 0.8-10.1 72-50,000 4.8-319 ND-16 ND-32.2 ND-1.0 ND-1.1 0.8-2.2 12-50 ND-1700 Concentration Range (ppm) In Unamended Soil (dry) 0.2-5 10-1000 200-2500 20-600 10-25 0.01-2 0.01-5 750-7,500 50-1,000 30-900 0.1-12 2-200 1,000-10,000 0.9-9 20-500 25-250 10-300 60-2000 Mean level (ppm) in dry Soil 40 1000 650 100 7 0.2 0.1 6,300 300 700 10 5,000 1 100 50 50 300 ------- ;| III. Plant Uptake of Chemical Substances from Municipal Sludge-Amended Soil .:i i A limited amount of data were located on the uptake of metals and ] other substances by plants from soil, especially the uptake of non- essential elements from sludge-amended soils. Many factors have been ...: recognized as having an effect on plant accumulation of toxic metals; ; however, few definitive studies have been conducted to allow a precise description of soil-piant relationships for all factors for any element or substance. t Knowledge of the chemical forms preferentially absorbed from the soil by plants is an important factor in estimating plant uptake. Considerable research is necessary to define plant-available forms. Any factor that affects the availability of elements in the soil also may affect plant accumulation. Table 2 is a partial .list of factors known to influence plant uptake. In addition, there are probably several unknown factors which contribute to the complexity of this problem. Table 3 lists some of the elements and types of plants for which uptake has been observed. An uptake of 50% or greater over controls was the criterion for inclusion on the list. The cited studies are not directly comparable with each other and do not adequately describe all aspects of uptake for any element. The elements and substances listed (except manganese) have been considered non-essential for plants. Excess concentrations of the essential elements also may accumulate in plant tissue from sludge and/or soil substrate. In some cases, excess nutrient may be toxic to the plant. When plant injury occurs due to toxicity, there is some protective value for those (animals and humans) who may choose not to consume damaged crops; however the accumulation of substances in crops without phytotoxicity raises some concern with respect to the human food chain. Even though some elements are essential nutrients for plants, their importance as potential toxic hazards when plant accumulation occurs should not be overlooked when additions of municipal sludge are made to soils used to grow crops in the human food chain. -7- ------- Table 2. Factors Influencing Plant Uptake of Chemical Substances Soil/Sludge Factors PH organic matter content cation exchange capacity phosphate (amounts) availability specific metal characteristics presence of competing ions soil distribution of metals soil variables - moisture, temperature, aeration (02)5 composition soil solubility status Plant Factors rooting depth plant age plant species and variety, tissue differences with species Other climatic (seasonal) effects -8- ------- TABLE 3. STUDIES ON PLANT UPTAKE OF CHEMICAL SUBSTANCES Element* or Substances arsenic cadmium chromium lead manganese mercury nickel PCBs FROM SLUDGE-AMENDED Plants in which Uptake has been observed ** fodder rape bush beans, corn barley wheat corn corn rye soybeans sorghum tomatoes (leaves) sudan grass alfalfa white clover (forage) tall fescue bermuda grass Swiss chard spinach, lettuce, curly cress fescue (forage) carrots, radishes, potatoes peas (vines, pods), tomatoes corn, lettuce barley corn, rye fescue (forage) fodder rape barl ey fodder rape fescue (forage) Swiss chard fescue (forage) corn, rye ' corn fodder rape barley corn, rye soybeans (grain, leaves) carrots, beets, leeks corn, bush beans grain, corn SOIL Type of Study*** F F X X,X,F,F X,F,X,X F.F.F X,X X,X . X X X X X X X F X F X X X X X,X F F X F F F F X X F X X F F F F literature Citation ( 2) (24) (38) (6,43,60) (6,4,13,15) (36,39,59) (13, 15) (6, 35) (45) ( 9) ( 9) ( 9) ( 7) ( 7) ( 7) (23) ( 6) ( 8) (18) (18) (18) (17) (13, 14) ( 8) ( 2) (17) ( 2) ( 8) (23) ( 8) (13) (15) ( 2) (17) (13) ( 4) (42) (24) ( 3) * without regard to oxidation state or compound **without regard to tissue ***Type of Study F= field study X = experimental/greenhouse -9- ------- Some specific element interactions have been observed to influence plant uptake. Due to the insolubility of lead phosphate (Pb-^PO^) lead uptake and accumulation by plants may be significantly mediated by phosphate levels in the substrate. Zinc and cadmium interactions also have been observed to influence plant uptake. Control of zinc:cadmium ratios to 100:1 or greater has been proposed by some investigators to protect against cadmium accumulation by plants (Chaney, 1973). The utilization/disposal of municipal sludge on croplands and pasturelands emphasizes the need for definitive data on plant uptake of synthetic organic chemicals. The Food and Drug Administration (FDA) has indicated that based on uptake studies, edible parts of plants contain some of the pesticides listed in table IB), but the levels are 5 to 20 percent of the levels in the soils used and that, in general, root crops take up more chlorinated organics from the soil than other types of crops. However, other studies have shown that chlordane, heptachlor and dieldrin are translocated from soil into soybeans and stored in the oil of the seed. Although the pesticides levels found were low, these data revealed that sludge can be a source of recycling of chemical contami- nants from sludge back into the food supply (Jelinek e_t al_., 1976). Table 4 reports plant uptake of certain elements (known to be in sewage sludge at variable concentrations) where sewage sludge was not part of the substrate employed in the experiment. These studies are listed because many of them were cited frequently in the past as indi- cating the potential for plant uptake of heavy metals from sludge- amended soils. Cunningham ejt al_. (1975) has urged caution in attempting to evaluate phytotoxicity or uptake from sludge-amended soils based on such studies. It should be recognized that surface contamination of the above ground portions of plants is also a potential problem in sludge applica- tion to croplands and pasturelands. Recent work by the United States Department of Agriculture for the FDA showed that dried grass contained -10- ------- about 5% by weight of sludge, when the grass had been mowed 80 days after it had been sprayed with the sludge. In this case about 30% of the applied sludge remained on the grass. It is noteworthy that the grass in this study was grown in the East; not an arid section of the country. This work indicated a potential for contamination by persist- ent synthetic organics such as organochlorine pesticides and PCBs as a resul^ of sludge application (Jelinek e£ al_., 1976). -11- ------- TABLE 4. PLANT UPTAKE OF TRACE ELEMENTS FROM OTHER SUBSTRATES* Element or Substance cadmi um lead nickel selenium Plants in which increased Uptake has been observed lettuce, radish, celery, green pepper, soybeens, wheat corn, turnips, beets, beans, tomatoes, cabbage, lettuce, green pepper, barley lettuce, broccoli, spinach, cauliflower, peas, oats, radish, carrots raddish, lettuce lettuce, oats corn, alfalfa tree seedlings (8 species) pasturage herbage (mixed clovers) wild oats corn oats, soybeens oats, barley, clover, turnip potatoes, beets, cabbage, kale oats, beans, peas, sunflowers tomatoes wheat, barley, cotton, peanut ryegrass, rice, sorghum grasses, clovers, garden vegetables alfalfa wheat, corn Literature Citation (25) (51) (32,33) (34) (33) (41) (54) (47) (53) ( 5) (56) (27) (12) (62) (40) (10) (55) *Specific metal additions to soils or hydroponic solutions. -12- ------- IV. Health Effects Aspects The chronic effects resulting from low-level dietary exposure to many of the trace elements and substances (found in sewage sludge) that make their way into the food chain are not known. A major health concern is that application of municipal sewage sludge to cropland and pastureland can result in plant uptake and accumulation of heavy metals and other toxic substances. Chronic exposure to the increased amounts of these materials in food could give rise to adverse health effects. Although FDA expressed concern (Jelinek e£al_., 1976) about the application of sludge to land used to grow crops in the human food chain, no quantitative guidance, except for PCBs, was given as to what levels of metals or other substances in sludge or plants would protect human health. In view of the uncertainties and real lack of data on this subject, a controversy has ensued as to whether such practices are "safe". Past presentations in the literature on this subject have not always clearly distinguished phytotoxicity from animal toxicity. It is recognized that toxic effects to crops can provide some protection for crop consumers (animal and human). However, accumulation of elements or toxic substances in crops without manifest phytotoxicity provides the opportunity for human exposure to potentially harmful substances. The reported levels in plant tissue are sometimes subject to misinterpretation. Care must be taken to distinguish between data on the edible and non- edible portions of the plant. However, even the "non-edible" portions may be used for animal feed so that a particular substance of concern may still enter the food chain. Also, non-harvested portions of the plant may remain in the soil where the elements accumulated could contribute to local increases in soil levels. -13- ------- Cadmium The most frequently cited concern, with a specific toxic chemical in sludge, is the potential for adverse chronic effects such as kidney disease (renal tubular dysfunction) from increased cadmium intake. The Joint Food and Agricultural Organization/ World Health Organization (FAO/WHO) Expert Committee on Food Additives proposed a tolerable weekly intake for cadmium of 400 to 500 micrograms (about 57-71 micrograms/day) (WHO, 1972). In comparison, the FDA estimates (based on their market basket surveys)the present daily cadmium intake (including drinking water) to be approximately 72 micrograms per day (Jelinek e_t a_l_., 1976). Even though only six percent of ingested cadmium has been shown to be accumulated by the body, most of the accumulation is by the kidney so that even at low concentrations in food, the concentration of cadmium in the kidney will gradually increase (Friberg e_t a]_., 1974). The Joint FAO/WHO Expert Committee on Food Additives recommended that cadmium levels in food should not be allowed to rise further. It is recognized that soil improvement with nutrient supplements is a source of cadmium entry into the food chain. The practice of applying municipal sludge to croplands has been shown to increase up to several fold the cadmium content of some crops. The Swedish National Board of Health and Welfare in 1973 established a regulation that limits the application of sludge on available land to one metric ton of dry matter per hectare annually (English equivalent 0.446 ton/acre), with the cadmium concentration limited to 15 milligrams per kilogram of dry matter (Stenstrom, 1974). By comparison, the typical U.S. rate of sludge application is high, 10- 20 dry/tons/acre with a range of 2-1,100 ppm cadmium in sludges analyzed. A recent review of cadmium as an environmental problem concluded that food intake is the major exposure route (EPA, 1975). The report indicated that the mechanisms involved in the transfer of cadmium into food chains are not adequately understood. It also pointed out that knowledge is insufficient regarding the cycling of cadmium in the environment. The document did not address land application of municipal sludge as a possible source/mechanism for entry of cadmium into the -14- ------- food chain although it did mention the use of super-phosphate fertilizers which can contain significant amounts of cadmium. Lead The World Health Organization has recommended a tolerable weekly intake for adult humans of 3 milligrams of lead (430 micrograms/day). Infants and children are considered a high-risk group. An HEW-appointed ad hoc committee of experts on pediatric lead toxicity has proposed a tolerable daily intake of lead of 300 micrograms per day for 1 to 3 year olds. No level has been proposed for infants, but it would probably be lower due to smaller body size and greater gastrointestinal absorption of lead (Jelinek, 1975). The potential exists for increased levels of lead in foods as a result of sludge application. Considering the often limited lead uptake by plants, especially under pH conditions greater than 5.5 and with the i presence of phosphate in the substrate, the margin of safety seems to be greater than that for cadmium. However, since lead accumulates in bones, liver, and kidneys, its ingestion via dietary intake cannot be ignored. ij Mercury : The Joint FAO/WHO Expert Committee on Food Additives established a ] provisional tolerable weekly intake of 0.3 mg of total mercury per | person, of which no more than 0.2 mg should be present as methyl/mercury (WHO, 1972). Little or no mercury has been found in plant produce. The principal source of mercury in the diet is fish (Mahaffey e_t al_., 1975). There is, however, a potential for mercury uptake by plants grown on sludge-amended soil since the presence of mercury in municipal sludge has been documented. The limited data available indicate little plant uptake of mercury; however, since mercury is a cumulative poison and biological methylation yields highly toxic alky! forms, the potential cannot be ignored. -15- ------- PCBs The recent discovery (April, 1976) of PCBs in the milk of a family cow in Bloomington, Indiana, illustrated one potential consequence of municipal sludge application to pastures when industrial discharge contaminates the sludge. This cow grazed on pasture to which 12 tons per acre of city sludge from the Winston-Thomas treatment plant had been applied in November 1975. Subsequent analysis of the sludge samples from that plant showed 105 ppm and 240 ppm PCBs (dry weight basis). The cow's milk contained 5 ppm PCBs (Arochlor 1016) on a fat basis, which is twice the FDA limit of 2.5 ppm (Jordan, 1976). Transfer of PCBs to the cow was probably related to grazing habits resulting in consumption of the contaminant rather than uptake by the pasturage. In this instance, the FDA limit did not provide direct control since the product was not shipped in interstate commerce. Other Substances of Concern The Food and Drug Administration has expressed concern about "heavy metals" in foods in the U.S. and is according highest priority to mer- cury, lead, cadmium, arsenic, selenium, and zinc in its program on toxic elements in foods. Specifically, it is suggested that new developments, such as widespread application of municipal sludge to land used for growing crops, should hot be initiated on such a substantial scale that a significant increase of cadmium in the diet would result (Jelinek, 1975). More recently, "In regards to methods of disposal of sludge, FDA prefers that the sludge be disposed of by means other than on productive land, if at all possible. If sludge is to be applied to productive land, we would prefer it be used to grow plants not in the human food chain, such as trees, ornamentals, grass on rights of way, etc. Finally, it if is_ to be used for growing crops in the human food chain, we prefer that it be applied to the land itself, rather than sprayed on the grow- ing crops," (Jelinek e_t al_., 1976). -16- ------- A recently published study involving feeding a vegetable (Swiss chard) grown on sludge-amended soil to guinea pigs has indicated that other chemical elements may deserve some attention. Analysis for 41 elements showed elevated concentrations of some elements in certain animal tissues. Accumulations were noted for antimony in adrenals, cadmium in kidneys, manganese in liver, and tin in kidney, muscle, and spleen. The animals did not reveal any observed toxicological effects after 28 days on a 45% Swiss chard diet (subsequent to a week of graduated introduction to the 45% amount). This study involved only a small number of animals for a short period of time and must be treated with caution in drawing inferences. The authors concluded that the preliminary data developed are inconclusive, but emphasized the need for conducting similar replicated feeding studies over a long term and with a greater number of animals. A similar study is being conducted under EPA and FDA sponsorship with cattle grazing on pasture to which sludge has been applied. The results will be available within several months (FDA, 1976). -17- ------- LITERATURE CITED (1) Allaway, W.H., "Agronomic Controls Over the Environmental Cycling of Trace Elements", Advance Agron, 20: 235-275 (1968). (2) Andersson, A. and Nilsson, K.O., "Enrichment of Trace Elements from Sewage Sludge Fertilizer in Soils and Plant", AMBIO, ]_: 176-179 (1972). (3) Background to the Regulation of Polychlorinated Biphenyls (PCB) in Canada, A report of the Task Force on PCB, to the Environmental Contaminants Committee of Environment Canada and Health & Welfare Canada, Technical Report 76-1, (April, 1976). (4) Bauer, W.J. and Sheaffer, J.R., Sludge, Soils, Water, and Plants, Soil Enrichment Materials Corp., December 1973. (5) Baumhardt G.R. and Welch L.F., "Lead Uptake and Corn Growth with. Soil Applied Lead", J. Environ. Quality, !_: 92-94 (1972). (6) Bingham, F.T., Page, A.L., Mahler, R.J., and Ganje, T.J., "Growth and Cadmium Accumulation of Plants Grown on a Soil Treated with a Cadmium-Enriched Sewage Sludge, J. Environ. Qua!., £: 207-11 (1975). (7) Bingham, F.T. et_al_., "Yield and Cadmium Accumulation of Forage Species in Relation to Cadmium Content of Sludge-Amended Soil", J. Environ. Qua!., 5: 57-60 (1976). (8) Boswell, F.C., "Municipal Sewage Sludge and Selected Element Applications to Soil: Effect on Soil and Fescue", J. Environ. Qua!., 4: 267-272 (1975). (9) Bowen, H.J.M., Trace Elements in Biochemistry, Academic Press, New York, 1966. (10) Bradford, G.R. ejt ^1_., "Trace Element Concentrations of Sewage Treatment Plant Effluents and Sludges: Their Interactions with Soils and Uptake by Plants", J. Environ. Qua!.. 4_: 123-127 (1975). (11) Braude, G.L., Jelinek, C.F., and Corneliussen, P., FDA's Overview of the Potential Health Hazards Associated with the Land Application of Municipal Wastewater Sludges," in Proceedings of the 1975 National Conference on Municipal Sludge Management and Disposal (1975). (12) Carter D.L., Brown M.J., and Robbins C.W., "Selenium Concentrations in Alfalfa from Several Sources Applied to Low Selenium, Alkaline Soil", Soil Science Society of America Proc.. 33_: 715-718 (1969). (13) Chaney, R.L., "Crop and Food Chain Effects of Toxic Elements in Sludges and Effluents", in Recycling Municipal Sludges and Efflu- ents on Land, Proceedings of Joint Conference, (July 9-13, 1973). -18- ------- (14) Crooke, W.M., "Effect of Heavy-Metal Toxicity on the Cation Ex- change Capacity of Plant Roots", Soil Sci., 86.: 231-240 (1958). (15) Cunningham, J.D., Keeney, O.K., and Ryan, J.A., "Yield and Metal Composition of Corn and Rye Grown on Sewage Sludge-Amended Soil", J. Environ. Qua!., 4: 448-454 (1975). (16) Cunningham, J.D., Keeney, D.R., and Ryan, J.A., "Phytotoxicity and Uptake of Metals Added to Soils as Inorganic Salts or in Sewage Sludge", J. Environ. Qua!., 4: 460-462 (1975). (17) Cunningham, J.D., Ryan, J.A., and Keeney, D.R., "Phytotoxicity in and Metal Uptake from Soil Treated with Metal-Amended Sewage Sludge", J. Environ. Qua!., 4: 455-460 (1975). (18) Dean, R.B., "Disposal and Reuse of Sludge and Sewage: What are the Options", in Proceedings of Conference on Land Disposal of Munici- pal Effluents and Sludges, Rutgers University, N.J. (March, 1973). (-19) Dowdy, R.H., and Larson, W.E., "Metal Uptake by Barley Seedlings Grown on Soils Amended with Sewage Sludge", J. Environ. Qua!., 4_: 229-233 (1975). (20) Dowdy, R.H. and Larson, W.E., "The Availability of Sludge-Borne Metals to Various Vegetable Crops", J. Environ. Qua!., 4_: 278-282 . (1975). (21) EPA, Review of PCB Levels in the Environment, EPA-560/7-76-001, (January, 1976). (22) EPA, Scientific and Technical Assessment Report on Cadmium, EPA- 600/6-75-003, (March 1975). (23) FDA, personal communication, Dr. George Braude, April, 1976. (24) Friberg, L. et al., Cadmiurn in the Environment, CRC Press, Cleve- land, Ohio, 2nd edition (1974). (25) Furr, A.K. et al., "Study of Guinea Pigs Fed Swiss Chard Grown on Municipal Sludge-Amended Soil", Archives of Env. Health, 31: 87-91 (1976). (26) Furr, A.K. et_al_., "Multielement and Chlorinated Hydrocarbon Analysis of Municipal Sewage Sludges of American Cities," Environ. Sci. and Tech.. j_0: 683-687 (1976). (27) Giordano, P.M., Mortvedt, J.J., and Mays, D.A., "Effect of Munic- ipal Wastes on Crop Yields and Uptake of Heavy Metals", J. Environ. Qua!.. 4: 394-399 (1975). (28) Haghiri, F., "Cadmium Uptake by Plants", J. Environ. Qua!., 2_: 93-96 (1973). -19- ------- (29) Hinesly.T.D. and Sosewitz, M. "Digested Sludge Disposal on Cropland", J_._ Water Pollution Control Federation, 41_: 822 (1969). (30) Hunter, J. and Vergano, 0., "Nickel Toxicity in Plants", Ann. Appl. Biol., 39_: 279-284 (1952). (31) IARC (1973), IARC Monographs on the Evaluation of Carcinogenic Risk of Chemicals to Man, Vol. 2, p. 100, IARC, Lyon. (32) Jelinek, C.F., Braude, G.L., and Read, R.B., "Management of Sludge Use on Land, FDA Considerations", Presented at the Associ- ation of Metropolitan Sewerage Agencies Conference on Sludge Management, Houston, Texas, April 13, (1976). (33) Jelinek, C.F., Mahaffey, K.R., and Corneliussen, P.E., "Estab- lishment of Regulatory Levels for Heavy Metals in Foods in the U.S.", delivered at the Intl. Conf. on Heavy Metals in the Env., Toronto, Ontario (Oct. 31, 1975). (34) John, M.K., "Cadmium Uptake by Eight Food Crops as Influenced by Various Soil Levels of Cadmium", Environ. Pollut.', 4_: 7-15 (1973). (35) John, M.K., Chuah, H.H., and Van Laerhoven, C.J., "Cadmium Con- tamination of Soil and Its Uptake by Oats", Env. Sci. and Tech., 6_: 555-7 (1972). (36) John, M.K. and Van Laerhoven, C.J., "Lead Uptake by Lettuce and Oats as Affected by Lime, Nitrogen, and Sources of Lead", J. Environ., Qua!., 1: 169-71 (1972). (37) John, M.K., Van Laerhoven, C.J., and Chuah, H.H., "Factors Affect- ing Plant Uptake and Phytoxicity of Cadmium Added to Soils", Env. Sci. and Tech., 6.: 1005-09 (1972). (38) Jones, R.L., Hinesly, T.D., and Ziegler, E.L., "Cadmium Content of Soybeans Grown in Sewage-Sludge Amended Soil", J. Environ. Qua!., 2: 351-53 (1973). (39) Jones, R.L. et al., "Cadmium and Zinc Contents of Corn Leaf and Grain Produced" by Sludge-Amended Soil", J. Environ. Qua!., 4: 509- 514 (1975). (40) Jordan, D., "PCBs Discovered in Family Cow's Milk", Bloomington . Herald Telephone (Indiana), (4/20/76). (41) Kirkham, M.B., "Uptake of Cadmium and Zinc from Sludge by Barley Grown Under Four Different Sludge Irrigation Regimes", J. Environ. Qua!.. 4: 423-26 (1975). (42) Kirkham, M.B., "Trace Elements in Corn Grown on a Long-Term Sludge Disposal Site", Environ. Sci. and Tech.. 8; 765-68 (1976). -20- ------- (43) Kubota, J. Allaway, W.H., Carter, D.L., Gary, E.E., and Lazar, V.A., "Selenium in Crops in the United States in Relation to Selenium-Responsive Diseases of Animals", J. Agr. Food Chetn., 15: 448-53 (1967). (44) Lagerwerf, J.V., Armiger, W.H., and Specht, A.W., "Uptake of Lead by Alfalfa and Corn from Soil and Air", Soil Sci.. 115: 455-60 (1973). (45) LeRiche, H.H., "Metal Contamination of Soil in the Woburn Market Garden Experiment Resulting from the Application of Sewage Sludge", J. Agric. Sci., 7]_: 205-208 (1968). (46) Linnman, L. et_al_., "Cadmium Uptake by Wheat from Sewage Sludge Used as a Plant Nutrient Source", Arch. Environ. Health, 27; 45-47 (1974). (47) Lisk, D.J., "Trace Metals in Soils, Plants and Animals", Advance Agron, 24: 267-325 (1972). (48) Lu, Po-Yung e_t aj_., "Model Ecosystem Studies of Lead and Cadmium and of Urban Sewage Sludge Containing These Elements", J. Environ. Qua!.. 4: 505-509 (1975). (49) Mahaffey, K.R., Corneliussen, P.E., Jelinek, C.F., and Fiorino, J.A., (1975) "Heavy Metal Exposure from Foods", Environ. Health Perspec.. 12.: 63-69. (50) Mitchell, R.L. and Reith, "The Lead Content of Pasture Herbage", J. Sci. and Food Agric., 1_7_: 435-440 (1966). « (51) NAS Medical and Biological Effects of Environmental Pol- lutants, Chromium, NAS, Washington, D.C. (1974). (52) NAS Medical and Biological Effects of Environmental Pol- lutants. Nickel. NAS. Washington. D.C. (1975). (53) Page, A.L., Fate and Effects of Trace Elements in Sewage Sludge When Applied to Agricultural Lands. A Literature Review Study, EPA-670/2-74-005 (NTIS No. PB-231171) (1974). (54) Page, A.L., Bingham, F.T., and Nelson, C., "Cadmium Absorption and Growth of Various Plant Species as Influenced by Solution Cadmium Concentration", J. Environ. Qua!., 1_: 288-291 (1972). (55) Papers from Proceedings of the National Conference on Municipal Sludge Management, (June 11-13. 1974). (56) Rains, D.W., "Lead Accumulation by Wild Oats (Avena fatua) in a Contaminated Area", Nature, 233: 210-11 (1971). (57) Rolfe, G.L., "Lead Uptake by Selected Tree Seedlings", J. Environ. Qua!.. 2: 153-157 (1973). -21- ------- (58) Rosenfield, I. and Beath, O.A., Selenium: Geobotany Biochemistry, Toxicity, Nutrition, Academic Press, NY (1964). (59) Roth, J.A., Wallihan, E.G., and Sharpless, R.G., "Uptake by Oats and Soybeans of Copper and Nickel Added to a Peat Soil", Soil Sci., 112: 338-42 (1971). (60) Sabey, B.R. and Hart, W.E., "Land Application of Sewage Sludge: I. Effect on Growth and Chemical Composition of Plants", J. Environ. Qua!., 4: 252-56 (1975). j (61) Shipp, R.F. and Baker, D.E., "Pennsylvania's Sewage Sludge Research ] and Extension Program", Compost Sci., 16(2) (March-April 1975). ! (62) Siddle, R.C., Hook, J.E., and Kardos, L.T., "Heavy Metals Applica- J tion and Plant Uptake in a Land Disposal System for Waste Water, 1 J. Environ. Qua!.. 5: 97-102 (1976). i " ~* """ '*- * ^~ : (63) Stenstrom, T., "Cadmium Availability to Wheat: A Study with Radio- ! active Tracers Under Field Conditions", AMBIO, 3_: 87-90 (1974). i 1 (64) WHO, "Evaluation of Certain Food Additives and the Contaminants i Mercury, Lead, and Cadmium", Sixteenth Report of the Joint FAQ/WHO 1 " Expert Committee on Food Additives, WHO Tech. Rept. Series No. 505, j Geneva (1972). i i (65) Wiltshire, G.H., "Effect of Nitrogen Source on Translocation of Nickel in Some Crop Plants and Weeds", Kirkia. 8.(2): 103-123 (1972). -22- ------- APPENDIX SLUDGE INFORMATION SUMMARY* 1. Quantities of sludge (estimated) dry tons/day Domestic Industrial users of municipal plants Total municipal sludge Current 10,000 7,000 17,000 2. Current disposition of sludge Method % Total Sludge Landfill 25% Ocean dump 15% Incineration 35% Land application 25% Croplands (20%) Others ( 5%) Secondary Treatment (next 10 years) 13,000 10,000 23,000 Reliability of Estimate Good Good Good Good Poor Poor *Derived from background information to the Technical Bulletin on Municipal Sludge Management: Environmental Factors, Fed. Reg. 41, 108: 22532-22543, (June 3, 1976). -23- ------- 3. 1972 Land Spreading Survey (Liquid Sludge Only) EPA Regions 2, 3, 4, 5, and 9 Mailed 1909, Responded 745 (39%) 4. Region 2 (NJ.NY 3 (DE..MD VA.WV) 4 (AL.FL KY,MS, SC.TN) 5 (IL.IN MN,OH, 9 (CA.HI Total Size MGD* 1-10 10-100 Greater Currently Use ) 6% , PA 27% ,GA, NC, 18% WI)' 36% ,NV) 14% 25% Currently Use 27% 15% than 100 7% Will Use 6% 5% 12% 9% 6% 8% Will Use 8% . 9% 13% Do Not Use 88% 68% 70% 55% 80% 67% Do Not Use 65% 76% 80% Total Costs for Various Sludge Methods Includes operating and construction costs 1 MGD Land Application 127-168 Landfill 171-208 Incineration 250-320 1 Ocean Dumping 376-417 $/Dry Ton 10 MGD 53-71 77-116 11-174 93-134 100 MGD 57-84 63-98 79-120 56-93 MGD = million gallons/day ------- : TECHNICAL REPORT DATA (Please read Instructions on the reverse before completing) 1. REPORT NO. EPA 560/8/76/004 4. TITLE AND SUBTITLE Considerations Relatinc Application of Muni ci pi Pastureland (A Backgroi 2. 3. RECIF 5. REPO ] to Toxic Suhstanrps in t^p il Sludge to Cropland and 6-PERF jnd Summary) 7. AUTHOR(S) 8. PERF Frank D. Kover EPA-Office of Toxic Substances 9. PERFORMING ORGANIZATION NAME M U.S. Environmental Pro1 Office of Toxic Substar 401 "M" Street, S.W. Washington, D.C. 2046C JD ADDRESS 10. PRO :ection Agency ?| lUeb 11. CON ) 12. SPONSORING AGENCY NAME AND ADDRESS 13. TYP Fl 14. SPO 15. SUPPLEMENTARY NOTES 'lENT'S ACCESSION-NO. RT DATE jvember 1976 ORMING ORGANIZATION CODE ORMING ORGANIZATION REPORT NO. GRAM ELEMENT NO. _A328 TRACT/GRANT NO. = OF REPORT AND PERIOD COVERED nal NSORING AGENCY CODE 16. ABSTRACT This report presents background information pertinent to an assessment of the potential health hazards from toxic substances when disposing/utilizing municipal sludge on agricultural lands, particularly croplands and pasturelands where products enter the human food chain. 17. a. DESCRIPTORS municipal sludge soi 1 amendment trace elements heavy metals PCBs cadmium 18. DISTRIBUTION STATEMENT Document is available to th the National Technical Info Springfield, Virginia 2215 KEY WORDS AND DOCUMENT ANALYSIS b.lDENTIFIERS/OPEN ENDE plant uptake food chain 19. SECURITY CLASS (This I e public through unclassified rmatlon Service 20. SECURITY CLASS (TMs i | unclassified - D TERMS c. COSATI Field/Group 02/A.D 06/F,H,I,T 07/B,C leport) 21. NO. OF PAGES >age) 22. PRICE EPA Form 2220-1 (9-73) ------- INSTRUCTIONS 1. REPORT NUMBER Insert the EPA report number as it appears on the cover of the publication. 2. LEAVE BLANK 3. RECIPIENTS ACCESSION NUMBER Reserved for use by each report recipient. 4. TITLE AND SUBTITLE Title should indicate clearly and briefly the subject coverage of the report, and be displayed prominently. Set subtitle, if used, in smaller type or otherwise subordinate it to main title. When a report is prepared in more than one volume, repeat the primary title, add volume number and include subtitle for the specific title. 5. 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