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An assessment of the amounts of arsenical pesticides used historically in a geographical area
The Science of the Total Environment 218 Ž1998. 89]101
An assessment of the amounts of arsenical pesticides used historically in a geographical area E.A. Murphy a,U , M. Aucott b a Di¨ ision of Science and Research, Department of En¨ ironmental Protection, Trenton, NJ, USA Air Quality Management, New Jersey Department of En¨ ironmental Protection, Trenton, NJ, USA
b
Received 6 May 1997; accepted 8 June 1997
Abstract Using a methodology that utilizes existing accessible public information, estimates of the amounts of arsenical pesticides historically applied to cropland, turf and golf courses in New Jersey were made to the county level. Specifically, estimates of the amounts of lead arsenate and calcium arsenate pesticides are presented. In New Jersey it is estimated that 49 000 000 pounds Žlb. of lead arsenate and 18 000 000 lb of calcium arsenate were applied to soils in the state from 1900 to 1980. Of this, a cumulative total of approx. 15 000 000 lb of arsenic was applied during this time frame. It is important to assess the approximate quantities of arsenical pesticides in New Jersey because soils in the state have been shown to contain elevated levels of lead and arsenic. In order to target soil monitoring efforts, it is important to determine which counties are most likely to have received treatment. Furthermore, exposure assessments can be better evaluated when estimates of application for these pesticides are available. Q 1998 Published by Elsevier Science B.V. All rights reserved. Keywords: Arsenical pesticides; New Jersey; Soil monitoring
1. Introduction The issue of assessing the amounts of lead and calcium arsenates used in agriculture was first raised in New Jersey as a result of the discovery of arsenic- and lead-contaminated soils in residential developments located on former apple orchards in the central and southern part of the state. This report uses a procedure to approximately quantify the amount of lead arsenate and calcium U
Corresponding author.
arsenate pesticides applied in New Jersey from 1900 to 1980 on a county level. Such estimates can be made in other states where the same type of crops have been grown. 2. Methods 2.1. Crop recommendations from the US Department of Agriculture (USDA) and from the New Jersey Agriculture Experiment Station (NJAES) Crop recommendations published by the US Department of Agriculture ŽUSDA. and the New
0048-9697r98r$19.00 Q 1998 Published by Elsevier Science B.V. All rights reserved. PII S0048-9697Ž98.00180-6
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E.A. Murphy, M. Aucott r The Science of the Total En¨ ironment 218 (1998) 89]101
Jersey Agricultural Extension Service ŽNJAES. were consulted from their earliest versions through to the present to ascertain on which crops arsenical pesticides were recommended for the control of pests. Currently, farmers tend to follow these recommendations, so it is assumed that farmers followed them for the time periods of interest as well. 2.2. Census information The US Department of Commerce has kept a decennial Census of Agriculture since 1840 ŽUS Department of Commerce, 1910]1992.. The USDA uses this data and individual state data to compile its yearbooks on agricultural statistics ŽUSDA, 1936]1980.. These publications were consulted for the years 1900]1990 to assess the quantity and change of acres of various types of crops in New Jersey for which arsenical pesticides were recommended. The Census of Agriculture reports data on agricultural acreages on a national, state and county level. 2.3. Bureau of Mines and Agricultural Statistics information The US Department of the Interior has issued Bureau of Mines reports since the mid 1800s ŽUS Department of Commerce, 1917]1992.. These publications were also consulted from 1900 through the present to determine the quantity of white arsenic consumed in various industries nationally. Data after 1960 are not reported consistently due to confidentiality conflicts. These data are presented in Table 1. The Bureau of Mines did not always report the actual quantities of lead arsenate and calcium arsenate pesticides consumed nor did it always report the actual percentage of white arsenic used in the manufacture of these pesticides. To get this information, the US Department of Agriculture’s annual Agricultural Statistics ŽUSDA, 1936]1980. were consulted. Here, national records of lead arsenate and calcium arsenate consumption in the country were reported. Data are reported up to 1973 and are presented in Table 2.
Table 1 Total white arsenic consumption in the US Žfrom the Bureau of Mines. and approximate percent used in agriculture, 1900]1990 Year
Total white arsenic, US consumption Žlb.
Percent in agriculture Ž%.
Agricultural arsenic use Žlb.
1900 1902 1903 1904 1905 1906 1907 1909 1910 1911 1912 1913 1914 1915 1916 1917 1918 1919 1920 1921 1922 1923 1924 1925 1926 1927 1928 1929 1930 1931 1932 1933 1934 1935 1936 1937 1938 1939 1940 1941 1942 1943 1944 1945 1946 1947 1948 1949 1950
600 000 2 706 000 1 222 000 72 000 1 508 000 1 474 000 3 502 000 3 318 000 5 690 000 10 106 000 12 488 000 8 064 000 12 528 000 13 796 000 14 114 000 14 658 000 16 259 950 20 836 000 30 484 000 12 910 000 88 216 000 48 846 000 46 660 000 43 266 000 39 016 000 48 154 000 45 840 000 55 406 000 55 792 000 40 336 000 40 336 000 40 760 000 54 066 000 53 890 000 64 334 000 69 384 000 50 196 000 67 826 000 63 258 000 86 920 000 94 166 000 93 120 000 84 072 000 74 202 000 49 720 000 62 256 000 48 602 000 29 754 000 64 208 000
12U 12U 12U 12U 12U 12U 12U 12U 12U 12U 12U 12U 12U 12U 12U 12U 12 42U 42U 42U 42U 42U 42U 42U 42U 42U 42U 42U 42U 42U 71 69U 69 69 69U 69U 69U 70 62 73 73 69U 69U 69U 69U 69U 69U 69U 69U
72 000 324 720 146 640 8640 180 960 176 880 420 240 398 160 682 800 1 212 720 1 498 560 967 680 1 503 360 1 655 520 1 693 680 1 758 960 2 000 000 8 751 120 12 803 280 5 422 200 37 050 720 20 515 320 19 597 200 18 171 720 16 386 720 20 224 680 19 252 800 23 270 520 23 432 640 16 941 120 28 638 560 28 124 400 37 305 540 37 184 100 44 390 460 47 874 960 34 635 240 47 478 200 39 219 960 63 451 600 68 741 180 64 252 800 58 009 680 51 199 380 34 306 800 42 956 640 33 535 380 20 530 260 44 035 520
E.A. Murphy, M. Aucott r The Science of the Total En¨ ironment 218 (1998) 89]101 Table 1 Ž Continued. Year
Total white arsenic, US consumption Žlb.
Percent in agriculture Ž%.
Agricultural arsenic use Žlb.
1951 1952 1953 1954 1955 1956 1957 1958 1959 1960 1973 1974 1975 1982 1983 1984 1985 1986 1987
57 738 000 27 454 000 32 064 000 32 742 000 37 790 000 50 596 000 45 840 000 40 910 000 53 250 000 na 26 992 000 27 484 000 24 027 000 na 25 662 000 33 736 000 38 068 000 160 937 357 149
69U 69U 69U 69U 69U 69U 69U 69U 69U na 25U 25U 25U na 25U 25U 25 na na
39 392 220 18 432 260 22 124 160 22 591 980 26 075 100 34 911 240 31 629 600 28 227 900 36 742 500 na 6 748 000 6 871 000 6 006 750 6 415 500 8 434 000 9 517 000
An asterisk ŽU . represents an estimate from the nearest percentage. Pounds used in agriculture from 1900 to 1918 were calculated based on 12% because that is the percentage reported used in agriculture in 1918. From 1919 to 1931, 42% was used becasue it is the average of 12% and 71%, used in 1918 and 1932, respectively.
3. Results 3.1. Crops on which arsenical pesticides were recommended in New Jersey and the application rates The primary arsenical pesticides recommended in New Jersey for agricultural and turf use were the insecticides, lead arsenate Žacid: PbHAsO4 and basic: Pb 4 wPbOHxwAsO4 x 3 . and calcium arsenate ŽCa 3 wAsO4 x 2 . Žalthough sodium arsenites were used as herbicides on railroads, this use is not being discussed in this report.. The first step in the assessment was to determine those crops that may have received arsenic treatment as part of a pest control program. Arsenicals appeared in the earliest NJAES bulletins from 1888 ŽNJAES, 1888.. Indeed, the primary early agents recommended against crop pests in general in the US include Paris green Ža copper-based arsenical .
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and London purple Žan arsenical . as well as kerosene emulsion, carbolic acid, bisulfide of carbon, whale oil soap, pyrethrum, hot water, lime, Bordeaux mix Žcopper sulfate, lime and water., copper sulfates and acetate, and potassium sulfide ŽNJAES, 1888, 1892.. Lead andror calcium arsenate appears continuously in the NJAES and USDA recommendations for ornamental trees ŽNJAES, 1912., tree fruit, especially apples but also plums, peaches, pears and cherries ŽNJAES, Table 2 Lead arsenate Žacid and basic. and calcium arsenate consumption levels from the USDA’s Agricultural Statistics yearbooks Year
Lead arsenate, US consumption Žlb.
Calcium arsenate, US consumption Žlb.
1929 1931 1933 1935 1938 1939 1941 1942 1943 1944 1945 1946 1947 1948 1949 1953 1954 1955 1956 1957 1958 1959 1960† 1961 1962 1963 1964 1965 1966 1967 1968 1969 1970 1971 1972 1973
29 118 597 36 185 693 29 181 119 51 988 929
29 924 793 19 878 217 12 912 657 39 190 544 34 618 000
57 857 000 16 318 000 63 159 000 70 901 000 86 440 000 61 486 000 53 872 000 27 083 000 22 592 000 16 006 000 13 893 000 14 910 000 13 696 000 9 193 000 10 704 000 12 838 000 11 505 000 11 950 000 9 517 000 8 507 000 7 039 000 9 258 000 7 098 000 7 328 000 5 952 000 9 016 000 9 204 000 1 456 000 6 168 000 5 164 000 3 946 000
50 239 000 80 195 000 68 470 000 41 939 000 22 144 000 28 515 000 41 929 000 22 665 000 11 959 000 3 322 000 782 000 1 884 000 26 478 000 16 698 000 9 158 000 6 301 000 6 300 000 7 274 000 3 718 000 3 123 000 6 958 000 4 192 000 2 890 000 2 040 000 3 398 000 1 158 000 1 144 000 940 000
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E.A. Murphy, M. Aucott r The Science of the Total En¨ ironment 218 (1998) 89]101
1916, 1917a,b; Rutgers, 1943]1967; Childers, 1969., bush and vine berries like strawberries, grapes and raspberries ŽRutgers, 1943]1967., sweet potatoes ŽPoole, 1922; Daines, 1942 and 1948; Pepper, 1944; USDA, 1946 and 1951; USDA, 1951; Knott, 1957., white potatoes ŽMatin, 1923; Rutgers, 1943]1967; USDA, 1946 and 1951; USDA, 1951; Knott, 1957., a wide variety of vegetables ŽCroy, 1917; Beattie, 1924 and 1951; NJAES, 1941, 1943a,b, 1958; Pepper, 1942, 1944; Thompson, 1944; USDA, 1946 and 1951; USDA, 1951, 1959; Frear et al., 1956, 1966 and 1972. and turfrlawns ŽUSDA, 1940; Wolfe, 1948; Rockwell and Grayson, 1956; Lawfield, 1959; Musser, 1962; Madison, 1971; Schery, 1973. from the early 1900s through to the early 1960s. Lead arsenate was recommended broadly to control insect pests on a number of crops in New Jersey. NJAES bulletins recommended lead arsenates on apples and a variety of vegetables. In a comprehensive circular describing recommended materials and application rates ŽPepper, 1944. NJAES list the following applications for commercial vegetables: asparagus, tomato, potato, sweet potato, eggplant, pepper, cucumber, squash, melons, etc. carrots, celery, corn, spinach and beets in various formulations including sprays, dusts and baits. The only vegetable for which lead arsenate was not recommended was beans. Since arsenic is highly toxic to beans, this is not surprising. Lead arsenate use on apples is significant because it is included on the regular apple spray calendars ŽRutgers, 1943]1967.; that is, lead arsenate was recommended for the routine spraying of apples throughout the growing season. For the other crop uses, lead arsenate was recommended annually or when a certain pest was a problem. The use of lead arsenate on apples first appeared in a New Jersey apple spray calendar in 1917 ŽNJAES, 1917a,b. and was probably used even before this date. Lead arsenate was recommended on apples for the control of red-banded leaf roller, curculio, canker worms, green fruit worms, tent caterpillars and scab. Application recommendations ranged from 2 to 4 lb lead arsenate in 100 gallons of water to be sprayed three or more times in the growing season.
Lead arsenate continued to be an important pesticide in the apple spray schedules through 1964 when it was recommended to be applied at a rate of 3 lb per 100 gallons. By 1967 ŽRutgers, 1943]1967. the synthetic organic pesticides Žprimarily DDT. started to appear much more frequently than lead arsenate though lead arsenate continued to be included. In fact, it was reported that the synthetic organic pesticides were more effective against common insects, and in the years following World War II, the use of arsenicbased pesticides declined rapidly with the ready availability of more economical and more effective synthetic organic insecticides like dieldrin and DDT. 3.2. Arsenic consumption in agriculture nationally Consumption of arsenic in the US has historically been primarily for the preparation of insecticides and herbicides. Other uses include the manufacturing of glass and in the preparation of drugs Žespecially early in the 20th century.. Paris green Ža copper arsenic compound. was first adopted as a means of combating the Colorado potato beetle. It is proposed that Paris green was first used against the potato beetle in the Western US in 1865 ŽFrear, 1942.. By 1868, its use had been fairly well established. Between 1880 and 1900, Paris green was probably the most commonly used insecticide, with London purple Žan arsenic compound. a close second ŽFrear, 1942.. By the 1930s, other uses of arsenic were growing, such as its use in ‘medicinal preparations, in lead alloys for bullets and shot, in pyrotechnic and boiler compositions, as a depilatory agent, in the manufacture of paint pigments, opal glass and enamels, in textile dying and calico printing, as a bronzing agent or decolorizing agent for glass, and for vermin poisons and sheep dips’ ŽUS Department of Commerce, 1917]1992.. Calcium arsenate found extensive use in the south between 1920 and 1950 where it was used for boll-weevil control in cotton fields, but was used as a general insecticide on a variety of vegetable crops and on white potatoes throughout the US.
E.A. Murphy, M. Aucott r The Science of the Total En¨ ironment 218 (1998) 89]101
Lead arsenates were used primarily in sprays and dusts for protection against insects attacking fruits and vegetables. The US Department of Agriculture’s annual Agricultural Statistics ŽUSDA, 1936]1980. lists consumption of arsenic in agriculture and separates lead arsenate consumption from calcium arsenate consumption. The data are presented in Table 2. The Bureau of Mines also presents information on arsenic consumption but does not always distinguish between lead arsenate and calcium arsenate Žsee Table 1.. The difference is important because calcium arsenate was used primarily against grasshoppers in the south and against the boll-weevil in the southeast, while lead arsenate was used more uniformly throughout the country. Therefore New Jersey’s consumption of calcium arsenate is more difficult to calculate than lead arsenate; the actual quantities of calcium arsenate used for purposes other than grasshopper and boll-weevil control are not clearly delineated. It is reported in the Bureau of Mines for some years that ‘most’ of the total US calcium arsenate consumption was used for boll-weevil or grasshopper control in the south and midwest. No actual amounts or percentages of calcium arsenate used for this purpose are presented. It was not until the 1920s that calcium arsenate was found to be highly effective against the boll-weevil, and its use in this capacity continued until around 1950. In order to account for calcium arsenate used exclusively for boll-weevil and grasshopper control, it is assumed that 50% of the US consumption of calcium arsenate occurred for this use between 1920 and 1950 and that the remaining 50% was available for other uses on vegetables and white potatoes throughout the country. For calcium arsenate data before 1920 and after 1950, the actual amounts reported in the Bureau of Mines or Agricultural Statistics are used. The data presented in this report represent these modifications of the available US consumption of calcium arsenate for 1920]1950. The Bureau of Mines reports the total quantities of white arsenic consumed in the US and the amounts consumed by dominant categories of users. On average, 69% the nation’s total con-
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sumption of white arsenic was used to produce insecticides like lead arsenate and calcium arsenate during the country’s peak agricultural years. There were other arsenical insecticides produced but these two were the dominant forms. Herbicidal arsenicals Ži.e. sodium arsenite . consumed approx. 14]20% of the total consumption of white arsenic. In general, most of the arsenic consumed in the US went into pesticide production with a small percentage going into other industries like glass manufacturing. USDA Agricultural Statistics report specifically the quantities of lead arsenate and calcium arsenate Žnot just the arsenic used in their production. consumed in agriculture Žincluding use on golf courses and turf.. These differences in reporting are significant given the actual amount of arsenic contained in lead arsenate and calcium arsenate pesticides. Based on atomic masses, calcium arsenate was approx. 38% arsenic while acid and basic lead arsenates were 22% and 15%, respectively Ž18.5% average.. Because calcium arsenate contains more arsenic, by weight, than lead arsenate, its application in some areas may be important. It is therefore vital to know whether quantities being reported represent arsenic or lead or calcium arsenate. Peak use of both lead and calcium arsenate occurred from approx. 1930 to the late 1940s Žapprox. 60 000 000 lb of each., with some decline during the war years. By 1960, consumption of these pesticides was less than a quarter of what it was during the peak years Žto approx. 10 000 000 lb of each.. This decline, which continued through the 1970s, was probably due to the ready access of the more effective substitute synthetic organic pesticides. 3.3. Acres of arsenic-treated land in New Jersey The Census of Agriculture reports acreage of land devoted to specific crops for the country, for states and for counties. Acres of land in the US and in New Jersey that were potentially treated with arsenical pesticides were tabulated to the county level. In order to allocate arsenic ‘loads’ to New
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E.A. Murphy, M. Aucott r The Science of the Total En¨ ironment 218 (1998) 89]101
Jersey agricultural land, it is necessary to know the proportion of arsenic-treated land in New Jersey in relation to the US. ‘Arsenic-treated’ land is defined as land that probably received lead arsenate or calcium arsenate insecticide treatment based on the crop recommendations for the period. Because the Bureau of Mines and Agricultural Statistics report arsenic consumption on a national basis only, the amount of arsenic used by any particular state must be apportioned based on the state’s percent contribution of arsenictreated acres of land. Table 3 shows the average annual acreage of land by decade where arsenical insecticides may have been used nationally and statewide. Using this information, it is possible to calculate the percentage of arsenic-treated land that was in New Jersey. For instance, for the years 1900]1910, 2.2% of the nation’s lead arsenate-treated land and 3.4% of the nation’s calcium arsenate-treated land was in New Jersey. Therefore 2.2% of the lead arsenate and 3.4% of the calcium arsenate used nationally in agriculture can be apportioned to New Jersey. It was difficult retrieving information on the acreage of land devoted to sod and turf production since the Census of Agriculture does not include them. Some data are available for golf courses from various publications and the remainder is calculated based on existing data. From the 1920s and 1960s, a rather consistent 2]3% of the nation’s golf courses were in New Jersey. By the 1970s, this had fallen to 1.5%. Thomas Ž1927. wrote that a golf course, at a minimum, should have approx. 120 acres with up to 80 acres for fairways and greens. Using 80 acres as the minimum standard acreage potentially treated with pesticide ŽThomas, 1927. an approximate acreage can be calculated for New Jersey courses. In the early 1930s, there were approx. 158 courses in New Jersey Žof the 5700 in the country. totaling 12 640 acres of land; in the early 1950s, there were 126 courses in New Jersey Žof the 5350 in the country. totaling 10 080 acres of land. By 1994, there were 249 golf courses in New Jersey using approx. 19 920 acres of land in the state. Once the percentage of arsenic-treated land in New Jersey is calculated, that percentage is multi-
plied by the corresponding national arsenic consumption value. Data showing the statewide arsenic consumption in New Jersey are presented in Table 4. 3.4. Arsenic consumption in agriculture in counties in New Jersey The Census of Agriculture provides data on a county basis for states. Therefore it is possible to calculate, roughly, the amount of arsenic that may have been applied to New Jersey on a county basis using the same procedure as that used for the statewide calculation. Estimates of the amount of lead arsenate and calcium arsenate that may have been used per county in New Jersey were generated by multiplying the total amount used in the state by the percentage of arsenic-treated cropland in the county. For instance, the average annual amount of lead arsenate used in New Jersey in 1921]1930 Ž902 676 lb. was multiplied by 0.037, which is the proportion of arsenic-treated land in Atlantic county, to get 33 399 lb of lead arsenate applied to land annually in Atlantic County in the years 1921]1930. To further quantify the amount of actual arsenic applied in the form of lead arsenate, the amount of lead arsenate was multiplied by 0.185, which is the average amount of arsenic in acid or basic lead arsenate, and the amount of calcium arsenate was multiplied by 0.38, which is the amount of arsenic in this pesticide. To follow the above example for Atlantic County, 33 399 lb was multiplied by 0.185 to get 6179 lb of arsenic applied in the form of lead arsenate in Atlantic county annually from 1921 to 1930. Cumulative data are presented for all of New Jersey’s 21 counties from 1900 to 1980 in Fig. 1. From 1900 to 1980, approx. 15 000 000 lb of white arsenic was applied in New Jersey in the form of lead and calcium arsenate. The top five counties in New Jersey for total cumulative totals of white arsenic applied cumulatively are Burlington, Cumberland, Gloucester, Monmouth and Salem. It is interesting to note that in 1990 and 1994, 94 and 80 lb, respectively, of arsenic in the form of the organic arsenicals DSMA and MSMA were
Table 3 Percent contribution of New Jersey to US crops and golf courses on which arsenical pesticides were recommended for use Apples wPbAs recommendedx Žacres.
White potatoes wCaAs recommendedx Žacres.
Sweet potatoes wPbAs recommendedx Žacres.
Golf courses wPbAs or CaAs recommendedx Žacres.
Average annual number of acres treated with arsenical pesticides Žall.
1 011 374 86 227 1 475 274 94 996 2 814 132 130 449 3 415 069 148 841 4 120 006 159 988 3 615 378 136 229 3 333 772 113 235 3 457 252 79 556 3 462 714 66 575
4 824 771 34 964 3 366 761 43 578 2 825 564 48 278 1 907 968 34 289 1 292 911 21 989 675 833 13 941 524 039 10 855 577 967 8875 590 541 6130
3 668 855 72 991 3 251 703 82 533 2 927 434 49 582 3 113 658 51 161 2 025 406 52 546 1 205 652 20 290 1 173 918 16 869 1 395 150 7602 738 954 5929
641 525 22 504 803 662 15 427 558 508 12 294 831 668 15 201 532 845 15 109 239 756 15 094 112 128 7401 85 545 2356 95 240 2102
48 880 480 80 000 800 456 000 12 640 441 600 11 360 441 600 11 360 427 200 11 840 793 600 12 760 793 600 18 640 1 160 000 17 120
10 195 405 217 166 8 977 400 237 334 9 581 638 253 243 9 709 963 260 852 8 412 768 260 992 6 163 819 197 394 5 939 418 161 120 6 309 513 117 028 6 047 449 97 855
Percentage of As-treated acres in New Jersey All
PbAs
CaAs
2.1
2.2
3.4
2.6
2.7
3.4
2.6
3.1
3.7
2.7
3.2
3.1
3.1
3.3
3.0
3.2
3.6
3.4
2.7
3.0
3.2
1.8
2.2
2.7
1.6 1.7 Ž1.5 golf only.
1.9
The Census of Agriculture supplied acres of apples only for certain years Ž1937, 1978, 1982 and 1992.. To get the acres of apples, the total number of trees was divided by the known number of acres to get the average number of trees per acres for those years. These estimates were used to calculate the acres from the number of trees. For years 1940]1970, an average of the 1937 and 1978 estimate was used to calculate the number of acres. From Golf Architecture, the value of 80 acres of treated greens was offered as a typical golf course constructed in the 1930]1960s. To get acres of golf courses, the number of golf courses was multiplied by 80 to get the number of acres of green that would typically be treated with pesticide.
E.A. Murphy, M. Aucott r The Science of the Total En¨ ironment 218 (1998) 89]101
US 1900]1910 NJ 1900]1910 US 1911]1920 NJ 1911]1920 US 1921]1930 NJ 1921]1930 US 1931]1940 NJ 1931]1940 US 1941]1950 NJ 1941]1950 US 1951]1960 NJ 1951]1960 US 1961]1970 NJ 1961]1970 US 1971]1980 NJ 1971]1980 US 1981]1990 NJ 1981]1990
Vegetables ŽPbAs or CaAs recommendedx Žacres.
95
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E.A. Murphy, M. Aucott r The Science of the Total En¨ ironment 218 (1998) 89]101
Table 4 Average annual consumption of lead and calcium arsenate insecticides in New Jersey from 1900 to 1980 Year
US PbAs consumption
NJ contribution of PbAs-treated crops Ž%.
PbAs used in New Jersey agriculture and golf courses Žlb.
US CaAs consumption
New Jersey contribution of CaAstreated crops Ž%.
CaAs used in New Jersey agriculture and golf courses Žlb.
1900]1910 1911]1920 1921]1930 1931]1940 1941]1950 1951]1960 1961]1970 1971]1980 1981]1990
724 036a 9 147 265a 29 118 597 43 803 185 46 429 000 12 336 000 7 437 000 5 093 000 No datac
2.2 2.7 3.1 3.2 3.3 3.6 3.0 2.2 1.7
15 929 246 976 902 676 1 401 702 1 532 157 444 096 223 110 112 046 No data
291 188 3 678 791 14 962 397b 1 332 427b 20 447 500b 8 865 000 3 589 000 940 000 No data
3.4 3.4 3.7 3.1 3.0 3.4 3.2 2.7 1.9
9900 125 079 553 609 41 305 613 425 301 410 114 848 25 380 No datac
a
These values calculated using Bureau of Mines total arsenic consumption data: approx. 12]42%, on average, of the total arsenic was used to produce arsenical insecticides, so 12]42% of the arsenic consumption was halved to estimate the amounts of arsenic used to manufacture these two dominant insecticides. Since acid and basic lead arsenate is, on average, 18.5% arsenic and calcium arsenate is 46% arsenic, the arsenic values were divided by 0.18 and 0.46, respectively, to determine the lead and calcium arsenate estimates. All subsequent data are from USDA Agricultural Statistics yearbooks. b Reflects 50% deduction of the total consumption to account for boll-weevil and grasshopper use in the South and Midwest. c Data after 1972 was not released by either Bureau of Mines nor Agricultural Statistics due to reasons of confidentiality to producers.
Table 5 Cumulative total arsenic applied in the form of lead arsenate Žacidrbasic. and calcium arsenate in New Jersey 1900]1980 using values calculated from national consumption data and crop recommendations Years National consumption data method 1900]1910 1911]1920 1921]1930 1931]1940 1941]1950 1951]1960 1961]1970 1971]1980 80-Year total Crop recommendations method 1900]1950
Arsenic Žlb.
PbAs Žlb.
67 090 932 210 3 773 660 2 750 110 5 165 500 1 966 940 849 180 303 730 15 808 420
159 290 2 469 760 9 026 760 14 017 020 15 321 570 4 440 960 2 231 100 1 120 460 48 786 920
8 880 000] 37 000 000
48 000 000] 200 000 000 Žapples.
CaAs Žlb.
99 000 1 250 790 5 536 080 413 050 6 134 250 3 014 100 1 148 480 253 800 17 849 550
1900]1960
10 855 350] 108 553 500
33 666 000] 33 660 000
1921]1950
4 644 000] 69 660 000
14 400 000] 216 000 000 Žgolf.
Total
66 179 350] 215 213 500
48 000 000] 200 000 000
48 066 000] 249 666 000
E.A. Murphy, M. Aucott r The Science of the Total En¨ ironment 218 (1998) 89]101
Fig. 1. Total pounds of arsenic applied cumulatively in New Jersey counties, 1900]1980.
applied to golf courses according to unpublished data collected by the NJDEP Pesticide Control Program. 3.5. Rates of arsenic application recommended by the USDA and the NJAES Estimates of quantities of lead arsenate and calcium arsenate applied in New Jersey have been presented on a county-wide basis in Fig. 1. To test how accurate these estimates are, another method of calculating rates was applied. Recommended rates of arsenic application in the USDA and NJAES bulletins and circulars were used to calculate the possible maximum number of pounds of arsenicals recommended per acre per year on given crops, assuming that every acre of land used to grow these crops used the recommended amounts. Application rates in the apple spray calendars were 2]4 lb of lead arsenate mixed in 100 gallons of water and sprayed 3]5 times in a growing season with 400]500 gallons being used per acre. Therefore approx. 24]100 lb of lead arsenate could have been sprayed on apple orchards in a growing season, using these maximum recommendation rates. Actual application rates of lead arsenate to apple orchards have been reported by
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Stevens et al. Ž1970. in four states. The rates range from 4]100 lbracre in the 1950s to 3]23 in the 1960s and 0]26 in the late 1960s. These reported rates correspond with the recommended rates in the apple spray calendars. To determine the annual application on apples, the total number of acres of land used to grow apples in New Jersey from 1900 to 1950 Ž40 000 acres. was multiplied by the application rate of 24]100 lbracre. Approximately 960 000]4 000 000 lb of lead arsenate could have been sprayed on apples annually using the crop recommendations. Lead and calcium arsenates were recommended at relatively high rates when used as insecticides on white potatoes, cabbage and related crops, melons and cucumbers. USDA bulletins from the 1920s through the early 1950s ŽBeattie, 1924 and 1951; Thompson, 1944; USDA, 1946 and 1951. call for calcium arsenate to control the Colorado potato beetle on potatoes, cabbage worms on cabbage and related crops, and the striped and spotted cucumber beetle on melons and cucumbers. These bulletins direct the application of the chemical as either a dust or a spray. The dust formulation was one pound of calcium arsenate to 2]3 lb of hydrated lime, with application rates of 15]30 lb of the dust per acre. For cucumbers, a less concentrated dust was recommended Ž1 lb calcium arsenate to 9 lb gypsum., but it was suggested that the dust be applied up to 10 times per season when striped or spotted cucumber beetles were prevalent. Spray recommendations were for 2]3 lb calcium arsenate to 50 gallons of water, with 75]125 gallons to be used per acre. Based on these bulletins, the overall recommended application of lead or calcium arsenate was 3]30 lbracre. Approximately 187 000 acres of land were used on average to grow vegetables and potatoes in New Jersey from 1900 to 1960, so approx. 561 000]5 610 000 lb per year could have been applied. Arsenates of lead were recommended for the control of earthworms, grubs and ants in turf and lawn fields as described in various USDA and NJAES bulletins ŽUSDA, 1940; Wolfe, 1948. and other publications ŽRockwell and Grayson, 1956; Lawfield, 1959; Musser, 1962; Madison, 1971; Schery, 1973.. On average, 40]600 lb of lead or
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E.A. Murphy, M. Aucott r The Science of the Total En¨ ironment 218 (1998) 89]101
calcium arsenate was recommended. This means that approx. 480 000 to just over 7 000 000 lb per year could have been applied to the 12 000 acres of golf courses that existed in the state from 1920 to 1950. Cumulative totals of lead and calcium arsenate and the corresponding arsenic that could have been applied in New Jersey using the crop recommendations method are presented in Table 5. Data are presented using the method described in this report, which calculates the estimates based on national consumption data, and using crop recommendations for the period. It is evident here that the method relying on national consumption data results in lower estimates than those generated using the crop recommendations. This is actually to be expected since the crop recommendations are simply that } recommendations. It is unlikely that every acre of every vegetable, fruit and golf course in the state consistently received the maximum application of pesticide. The actual amount of pesticide used probably falls somewhere between the two estimates and is probably closer to those reached using national consumption rates. 4. Discussion It is possible to estimate the amounts of a particular pesticide applied in agriculture on a statewide and county-wide basis. Heavy metals like arsenic applied in the past may persist indefinitely in the environment. In fact, elevated levels of lead and arsenic have been found in former orchard soils in New Jersey ŽFields et al., 1993. and elsewhere in the US ŽStevens et al., 1970.. Cumulative totals of lead arsenate or calcium arsenate insecticides applied to New Jersey crop land and golf courses from 1900 to 1980 using consumption values are approx. 49 000 000 lb of lead arsenate and 18 000 000 lb of calcium arsenate. Of this, approx. 15 000 000 lb was in the form of arsenic. Using crop recommendations, the cumulative arsenic total was 66 000 000]215 000 000 lb. While a certain percentage of applied arsenicals may volatilize ŽWoolson, 1977; Woolson and Isensee, 1981. and an even smaller percentage is taken up by plants ŽKabata-Pendias and Pendias,
1992; Domir et al., 1967; Woolson et al., 1971a,b, 1973; Woolson, 1975; Pyles and Woolson, 1982; Merwin et al., 1994., the rest either remains in soil ŽStevens et al., 1970; Woolson et al., 1971a,b; Woolson, 1975, 1977; Aten et al., 1980; Woolson and Isensee, 1981; Wauchope and McDowell, 1984; Kabata-Pendias and Pendias, 1992; Merwin et al., 1994; Redondo et al., 1994; Sanok et al., 1995. or leaches to subsoil ŽWood, 1985; Schimmack and Bunzl, 1986; Woolson et al., 1973; Davenport and Peryea, 1991; Elfving et al., 1994; Peryea and Creger, 1994; Yin et al., 1996.. Some investigators have measured not only total arsenic present in soils but water-soluble fractions as well. It is the water-soluble fraction that may be available Ži. to leach to subsoils or ground water and Žii. to be taken up by crops. Although arsenic is not considered to be highly mobile, its downward migration has been shown to be greater in a sandy soil than in a clay loam ŽElfving et al., 1994.. Scientists have been measuring total arsenic and have guessed at its water solubility since the early part of this century. As reported in the New Jersey Agricultural Experiment Station Bulletin 419 from 1925, Haywood and McDonnell ŽNJAES, 1925. have demonstrated that lead arsenate is much more soluble in tap water than in distilled water in agricultural spraying experiments. Stewart ŽNJAES, 1925. also found that 10 times as much lead arsenate was dissolved in tap water as in distilled water and attributed the dissolution to the presence of chloride and calcium and magnesium in the water. The arsenic formed salts chiefly of chlorides and bicarbonates in the tap water. Any increase of carbonate, bicarbonate, or potassium ions is accompanied by an increase in the dissolution of the arsenate; waters with high chloride also had an increased solution effect on lead arsenate. In the Stewart study, it was found that nitrates and sulfates increased the solubility of lead arsenate only slightly, while neutral chlorides increased solubility significantly. Since lead arsenate was often recommended to be applied with lime-sulphur, this practice may have prevented any increase in the solubility of the arsenic caused by the presence of chlorides in the spray water. However, in cases where liming did not accompany the appli-
E.A. Murphy, M. Aucott r The Science of the Total En¨ ironment 218 (1998) 89]101
cation of an arsenical, the possibility of mobility exists. Clearly, scientists were concerned with available arsenic from the standpoint of phytotoxicity. Later, scientists like Woolson et al. Ž1971a. determined that the form of arsenic ŽFe-, Al- or Ca-As. was more important than total arsenic present in soil. Soils with extremely high reactive Al levels were less phytotoxic even after heavy applications of arsenic than soils with low reactive Al contents, presumably because the arsenic was tightly bound to the aluminum. Subsequent studies ŽWoolson et al., 1973. confirmed this. In the latter study, the percentage of water-soluble arsenic increased as the application rate increased but was higher in the soil having a higher pH with low extractable Fe, Al and Ca. Al-As remained at 40]50% of total arsenic applied, indicating that aluminum may act as a reservoir for arsenic. Both Fe and Al may form relatively insoluble arsenic compounds. At comparable soil arsenic levels, the addition of P increased the arsenic content of the plant significantly. In an experiment with Dunkirk fine sand Ža New York orchard soil. containing 625 ppm arsenic from normal pesticidal applications of lead arsenate, the amount of arsenic removed by KH 2 PO4 leaching was a function of the amount of leachate used. Initially, arsenic was leached rapidly from the soil Ž77% of the total arsenic present was leached from the soil. then decreased over time. Southern New Jersey soils are generally high in aluminum and iron with low pH, indicating that leaching, if it did occur, probably was not significant enough to pose a ground water problem. In the north, however, conditions are such that perhaps leaching was more severe. It is possible that some of the arsenic applied to New Jersey agricultural crops was mobile, or that it volatilized. Most commercial lead arsenates contained some small percentage of soluble arsenic. The New Jersey Experiment Station analyzed common pesticides on an annual basis. In 1925 the amount of soluble arsenic found in the water solutions after an extraction of 24 h varied from 1.02 to 2.35% with an average of 1.60% ŽNJAES, 1925.. In the 1928 evaluations, the solu-
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ble arsenic ranged from 0.07 to 1.69% in lead arsenates Žsoluble arsenic in Paris Green were ordinarily higher: 1.01]3.26%.. While these percentages are low, given the rather large amounts of arsenic applied to soils, there is the possibility of some leaching to subsurface soils or to shallow ground water. The major repository, however, of this soil-applied arsenic is probably the soil and subsoil itself. References Aten CF, Bourke JB, Martini JH, Walton JC. Arsenic and lead in an orchard environment. Bull Environ Contam Toxicol 1980;24:105]115. Beattie JH. Watermelons, USDA Farmers’ Bulletin 1394, Washington, DC, 1924 and 1951. Childers NF. Modern fruit science. New Brunswick, New Jersey: Rutgers University Press, 1969. Croy MS. Putnam’s vegetable book. G.P. Putnam’s Sons, New York: The Knickerbocker Press, 1917. Daines RH. Scurf, black rot, and stem rot of sweet potatoes. New Jersey Agricultural Experiment Station, Rutgers University, New Brunswick, New Jersey, Circulars 437 and 514, 1942, 1948. Davenport JR, Peryea FJ. Phosphate fertilizers influence leaching of lead and arsenic in a soil contaminated with lead arsenate. Water Air Soil Pollut 1991;57r58:101]110. Domir SC, Woolson EA, Kearney PC, Isensee AR. Translocation and metabolic fate of monosodium methanearsonic acid in wheat. J Agric Food Chem 1967;24:1214]1217. Elfving DC, Wilson KR, Ebel JG, Manzell KL, Gutenmann WH, Lisk DJ. Migration of lead and arsenic in old orchard soils in the Georgian Bay region of Ontario. Chemosphere 1994;29:407]413. Fields TW, McNevin TF, Harkob RA, Hunter JV. A summary of selected soil constituents and contaminants at background locations in New Jersey. Trenton, NJ: NJDEP, 1993. Frear DEH. Chemistry of insecticides and fungicides, chap. II: the arsenicals. New York: Van Nostrand Co., Inc., 1942. Frear DEH, Friedman S, DeMartino T. Pesticide handbook } Entoma. State College, Pennsylvania: College Science Publishers, 1956, 1966 and 1972. Kabata-Pendias A, Pendias H. Trace elements in soils and plants. 2nd ed. Ann Arbor, MI: CRC Press, 1992. Knott JE. Handbook for vegetable growers. NY: John Wiley and Sons, 1957. Lawfield WN. Lawns and sportsgreens. London: W.H. and L. Collingridge, Limited, 1959. Madison JH. Practical turfgrass management. NY, Van Nostrand Reinhold and Co., 1971. Matin WH. Potato diseases in New Jersey and their control.
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New Jersey Agricultural Experiment Station, Circular 146, Rutgers Univ., New Brunswick, New Jersey, 1923a. Merwin I, Pryune PT, Ebel JG, Manzell KL, Lisk DJ. Persistence, phytotoxicity and management of arsenic, lead and mercury residues in old orchard soils of New York State. Chemosphere 1994;29:1361]1367. Musser HW. Turf management. NY: McGraw-Hill Book Co., Inc., 1962. New Jersey Agricultural Experiment Station. Rutgers University, New Brunswick, New Jersey, Circular 50, 1888. New Jersey Agricultural Experiment Station. Rutgers University, New Brunswick, New Jersey, Circular 86, 1892. New Jersey Agricultural Experiment Station. Rutgers University, New Brunswick, New Jersey, Circular 15, 1912. New Jersey Agricultural Experiment Station. Rutgers University, New Brunswick, New Jersey, Circular 44, 1916. New Jersey Agricultural Experiment Station. Rutgers University, New Brunswick, New Jersey, Circular 80, 1917a. New Jersey Agricultural Experiment Station. Rutgers University, New Brunswick, New Jersey, Circular 81, 1917b. New Jersey Agricultural Experiment Station. Rutgers University, New Brunswick, Bulletin 419, 1925. New Jersey Agricultural Experiment Station. The answer to your tomato problem. Rutgers University, New Brunswick, New Jersey, Circular 414, 1941. New Jersey Agricultural Experiment Station. Farm science goes to war. Rutgers University, New Brunswick, New Jersey, 1943a. New Jersey Agricultural Experiment Service. Vegetable crop notes. Rutgers Univ, New Brunswick, New Jersey, 1943b. New Jersey Agricultural Experiment Station. Pesticides, economic poisons inspection series 71. New Jersey Agricultural Experiment Station, Rutgers University, New Brunswick, New Jersey, 1958. Pepper BB. Controlling insects in the home vegetable garden. New Jersey Agricultural Experiment Station, Rutgers University, New Brunswick, New Jersey, Circular 443, 1942. Pepper BB. Vegetable insects and their control on commercial plantings. New Jersey Agricultural Experiment Station, Rutgers University, New Brunswick, New Jersey, Circular 476, 1944. Peryea FJ, Creger TL. Vertical distribution of lead and arsenic in soils contaminated with lead arsenate pesticide residues. Water Air Soil Pollut 1994;78:297]306. Poole RF. Sweet potato diseases in New Jersey. New Jersey Agricultural Experiment Station, Circular 141, Rutgers Univ., New Brunswick, New Jersey, 1922. Pyles RA, Woolson EA. Quantitation and characterization of arsenic compounds in vegetables grown in arsenic acid treated soil. J Agric Food Chem 1982;30:866]870. Redondo MJ, Ruiz MJ, Boluda R, Font G. Persistence of pesticide residues in orchard soil. Sci Total Environ 1994;156:199]205. Rockwell FF, Grayson EC. The complete book of lawns. NY: The American Garden Guild and Doubleday and Co., Inc., 1956.
Rutgers Extension Service Spraying Recommendations for Apples, Peaches, Potatoes, Strawberries, Grapes and other small berries. Spray Calendars 1-95A, Rutgers University, New Brunswick, New Jersey, 1943]1967. Sanok WJ, Ebel JG, Manzell KL, Gutemnann WH, Lisk DJ. Residues of arsenic and lead in potato soils on Long Island. Chemosphere 1995;30:803]806. Schery RW. A perfect lawn, the easy way. NY: Macmillan Publishing Co., Inc., 1973. Schimmack W, Burzl K. Migration of solutes in a cultivated soil: effect of ploughing. Geoderma 1986;38:155]163. Stevens LJ, Collier CW, Woodhain DW. Pesticides in soil: monitoring pesticides in soils from areas of regular, limited and no pesticide use. Pest Monit J 1970;4:145]166. Thomas GC. Golf architecture in America. New York: The Times-Mirror Press, 1927. Thompson RC. Cauliflower and broccoli varieties and culture, Farmers Bulletin No. 1957. Washington, DC: USDA, 1944. US Department of Agriculture. Agricultural statistics, 1936, 1939, 1940, 1945, 1950, 1955, 1960, 1965, 1970, 1975, 1980. US Dept. of Agriculture. Planting and care of lawns, Farmers’ Bulletin No. 1677. Washington, DC, 1940. US Department of Agriculture. Vegetable gardeners’ handbook on insects and diseases, Miscellaneous Publication 605. Washington, DC, 1946 and 1951. US Department of Agriculture. Miscellaneous publication No. 605: Vegetable gardeners’ handbook on insects and diseases. Washington, DC: USDA, 1951. US Department of Agriculture. Insects and diseases of vegetables in the home garden. Home and Garden Bulletin No. 46, Washington DC, 1959. US Department of Commerce., Bureau of the Census, Census of ŽAGRICULTURE., 1910, 1925, 1930, 1945, 1950, 1955, 1960, 1965, 1970, 1975, 1980, 1982, 1992. US Department of Commerce. Bureau of Mines, Minerals Resources of the United States. Part 1. Metals, AKA Minerals Yearbook. Washington, DC, 1917]1992. Wauchope RD, McDowell LL. Adsorption of phosphate, arsenate, methanearsonate, and cacodylate by lake and stream sediments: comparisons with soils. J Environ Qual 1984;13:499]504. Wolfe DE. Killing turf weeds with chemicals, new jersey agricultural experiment station, Circular 513. Rutgers Univ., New Brunswick, New Jersey, 1948. Wood JM. EfFects of acidification on the mobility of metals and metalloids: an overview. Environ Health Perspect 1985;63:115]119. Woolson EA. Arsenical pesticides, ACS symposium series 7. American Chemical Society, Washington, DC, 1975. Woolson EA. Generation of alkylarsines from soils. Weed Sci 1977;25:412]416. Woolson EA, Isensee AR. Soil residue accumulation from three applied arsenic sources. Weed Sci 1981;29:17]21. Woolson EA, Axley JH, Kearney PC. The chemistry and phytotoxicity of arsenic in soils: I. contaminated field soils. Soil Sci Soc Am Proc 1971a;35:938]943.
E.A. Murphy, M. Aucott r The Science of the Total En¨ ironment 218 (1998) 89]101 Woolson EA, Axley JH, Kearney PC. Correlation between available soil arsenic, estimated by six methods, and response of corn. Soil Sci Soc Am Proc 1971b;35:101]105. Woolson EA, Axley JH, Kearney PC. The chemistry and phytotoxicity of arsenic in soils: II. Effects of time and phosphorus. Soil Sci Soc Am Proc 1973;37:254]259.
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Yin Y, Li Y, Allen HE, Huang CP. Adsorptionrdesorption and transport of mercury and arsenic in New Jersey soils. MDEP-DSR Final Report, Trenton, NJ, 1996.
An assessment of the amounts of arsenical pesticides used historically in a geographical area E.A. Murphy a,U , M. Aucott b a Di¨ ision of Science and Research, Department of En¨ ironmental Protection, Trenton, NJ, USA Air Quality Management, New Jersey Department of En¨ ironmental Protection, Trenton, NJ, USA
b
Received 6 May 1997; accepted 8 June 1997
Abstract Using a methodology that utilizes existing accessible public information, estimates of the amounts of arsenical pesticides historically applied to cropland, turf and golf courses in New Jersey were made to the county level. Specifically, estimates of the amounts of lead arsenate and calcium arsenate pesticides are presented. In New Jersey it is estimated that 49 000 000 pounds Žlb. of lead arsenate and 18 000 000 lb of calcium arsenate were applied to soils in the state from 1900 to 1980. Of this, a cumulative total of approx. 15 000 000 lb of arsenic was applied during this time frame. It is important to assess the approximate quantities of arsenical pesticides in New Jersey because soils in the state have been shown to contain elevated levels of lead and arsenic. In order to target soil monitoring efforts, it is important to determine which counties are most likely to have received treatment. Furthermore, exposure assessments can be better evaluated when estimates of application for these pesticides are available. Q 1998 Published by Elsevier Science B.V. All rights reserved. Keywords: Arsenical pesticides; New Jersey; Soil monitoring
1. Introduction The issue of assessing the amounts of lead and calcium arsenates used in agriculture was first raised in New Jersey as a result of the discovery of arsenic- and lead-contaminated soils in residential developments located on former apple orchards in the central and southern part of the state. This report uses a procedure to approximately quantify the amount of lead arsenate and calcium U
Corresponding author.
arsenate pesticides applied in New Jersey from 1900 to 1980 on a county level. Such estimates can be made in other states where the same type of crops have been grown. 2. Methods 2.1. Crop recommendations from the US Department of Agriculture (USDA) and from the New Jersey Agriculture Experiment Station (NJAES) Crop recommendations published by the US Department of Agriculture ŽUSDA. and the New
0048-9697r98r$19.00 Q 1998 Published by Elsevier Science B.V. All rights reserved. PII S0048-9697Ž98.00180-6
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Jersey Agricultural Extension Service ŽNJAES. were consulted from their earliest versions through to the present to ascertain on which crops arsenical pesticides were recommended for the control of pests. Currently, farmers tend to follow these recommendations, so it is assumed that farmers followed them for the time periods of interest as well. 2.2. Census information The US Department of Commerce has kept a decennial Census of Agriculture since 1840 ŽUS Department of Commerce, 1910]1992.. The USDA uses this data and individual state data to compile its yearbooks on agricultural statistics ŽUSDA, 1936]1980.. These publications were consulted for the years 1900]1990 to assess the quantity and change of acres of various types of crops in New Jersey for which arsenical pesticides were recommended. The Census of Agriculture reports data on agricultural acreages on a national, state and county level. 2.3. Bureau of Mines and Agricultural Statistics information The US Department of the Interior has issued Bureau of Mines reports since the mid 1800s ŽUS Department of Commerce, 1917]1992.. These publications were also consulted from 1900 through the present to determine the quantity of white arsenic consumed in various industries nationally. Data after 1960 are not reported consistently due to confidentiality conflicts. These data are presented in Table 1. The Bureau of Mines did not always report the actual quantities of lead arsenate and calcium arsenate pesticides consumed nor did it always report the actual percentage of white arsenic used in the manufacture of these pesticides. To get this information, the US Department of Agriculture’s annual Agricultural Statistics ŽUSDA, 1936]1980. were consulted. Here, national records of lead arsenate and calcium arsenate consumption in the country were reported. Data are reported up to 1973 and are presented in Table 2.
Table 1 Total white arsenic consumption in the US Žfrom the Bureau of Mines. and approximate percent used in agriculture, 1900]1990 Year
Total white arsenic, US consumption Žlb.
Percent in agriculture Ž%.
Agricultural arsenic use Žlb.
1900 1902 1903 1904 1905 1906 1907 1909 1910 1911 1912 1913 1914 1915 1916 1917 1918 1919 1920 1921 1922 1923 1924 1925 1926 1927 1928 1929 1930 1931 1932 1933 1934 1935 1936 1937 1938 1939 1940 1941 1942 1943 1944 1945 1946 1947 1948 1949 1950
600 000 2 706 000 1 222 000 72 000 1 508 000 1 474 000 3 502 000 3 318 000 5 690 000 10 106 000 12 488 000 8 064 000 12 528 000 13 796 000 14 114 000 14 658 000 16 259 950 20 836 000 30 484 000 12 910 000 88 216 000 48 846 000 46 660 000 43 266 000 39 016 000 48 154 000 45 840 000 55 406 000 55 792 000 40 336 000 40 336 000 40 760 000 54 066 000 53 890 000 64 334 000 69 384 000 50 196 000 67 826 000 63 258 000 86 920 000 94 166 000 93 120 000 84 072 000 74 202 000 49 720 000 62 256 000 48 602 000 29 754 000 64 208 000
12U 12U 12U 12U 12U 12U 12U 12U 12U 12U 12U 12U 12U 12U 12U 12U 12 42U 42U 42U 42U 42U 42U 42U 42U 42U 42U 42U 42U 42U 71 69U 69 69 69U 69U 69U 70 62 73 73 69U 69U 69U 69U 69U 69U 69U 69U
72 000 324 720 146 640 8640 180 960 176 880 420 240 398 160 682 800 1 212 720 1 498 560 967 680 1 503 360 1 655 520 1 693 680 1 758 960 2 000 000 8 751 120 12 803 280 5 422 200 37 050 720 20 515 320 19 597 200 18 171 720 16 386 720 20 224 680 19 252 800 23 270 520 23 432 640 16 941 120 28 638 560 28 124 400 37 305 540 37 184 100 44 390 460 47 874 960 34 635 240 47 478 200 39 219 960 63 451 600 68 741 180 64 252 800 58 009 680 51 199 380 34 306 800 42 956 640 33 535 380 20 530 260 44 035 520
E.A. Murphy, M. Aucott r The Science of the Total En¨ ironment 218 (1998) 89]101 Table 1 Ž Continued. Year
Total white arsenic, US consumption Žlb.
Percent in agriculture Ž%.
Agricultural arsenic use Žlb.
1951 1952 1953 1954 1955 1956 1957 1958 1959 1960 1973 1974 1975 1982 1983 1984 1985 1986 1987
57 738 000 27 454 000 32 064 000 32 742 000 37 790 000 50 596 000 45 840 000 40 910 000 53 250 000 na 26 992 000 27 484 000 24 027 000 na 25 662 000 33 736 000 38 068 000 160 937 357 149
69U 69U 69U 69U 69U 69U 69U 69U 69U na 25U 25U 25U na 25U 25U 25 na na
39 392 220 18 432 260 22 124 160 22 591 980 26 075 100 34 911 240 31 629 600 28 227 900 36 742 500 na 6 748 000 6 871 000 6 006 750 6 415 500 8 434 000 9 517 000
An asterisk ŽU . represents an estimate from the nearest percentage. Pounds used in agriculture from 1900 to 1918 were calculated based on 12% because that is the percentage reported used in agriculture in 1918. From 1919 to 1931, 42% was used becasue it is the average of 12% and 71%, used in 1918 and 1932, respectively.
3. Results 3.1. Crops on which arsenical pesticides were recommended in New Jersey and the application rates The primary arsenical pesticides recommended in New Jersey for agricultural and turf use were the insecticides, lead arsenate Žacid: PbHAsO4 and basic: Pb 4 wPbOHxwAsO4 x 3 . and calcium arsenate ŽCa 3 wAsO4 x 2 . Žalthough sodium arsenites were used as herbicides on railroads, this use is not being discussed in this report.. The first step in the assessment was to determine those crops that may have received arsenic treatment as part of a pest control program. Arsenicals appeared in the earliest NJAES bulletins from 1888 ŽNJAES, 1888.. Indeed, the primary early agents recommended against crop pests in general in the US include Paris green Ža copper-based arsenical .
91
and London purple Žan arsenical . as well as kerosene emulsion, carbolic acid, bisulfide of carbon, whale oil soap, pyrethrum, hot water, lime, Bordeaux mix Žcopper sulfate, lime and water., copper sulfates and acetate, and potassium sulfide ŽNJAES, 1888, 1892.. Lead andror calcium arsenate appears continuously in the NJAES and USDA recommendations for ornamental trees ŽNJAES, 1912., tree fruit, especially apples but also plums, peaches, pears and cherries ŽNJAES, Table 2 Lead arsenate Žacid and basic. and calcium arsenate consumption levels from the USDA’s Agricultural Statistics yearbooks Year
Lead arsenate, US consumption Žlb.
Calcium arsenate, US consumption Žlb.
1929 1931 1933 1935 1938 1939 1941 1942 1943 1944 1945 1946 1947 1948 1949 1953 1954 1955 1956 1957 1958 1959 1960† 1961 1962 1963 1964 1965 1966 1967 1968 1969 1970 1971 1972 1973
29 118 597 36 185 693 29 181 119 51 988 929
29 924 793 19 878 217 12 912 657 39 190 544 34 618 000
57 857 000 16 318 000 63 159 000 70 901 000 86 440 000 61 486 000 53 872 000 27 083 000 22 592 000 16 006 000 13 893 000 14 910 000 13 696 000 9 193 000 10 704 000 12 838 000 11 505 000 11 950 000 9 517 000 8 507 000 7 039 000 9 258 000 7 098 000 7 328 000 5 952 000 9 016 000 9 204 000 1 456 000 6 168 000 5 164 000 3 946 000
50 239 000 80 195 000 68 470 000 41 939 000 22 144 000 28 515 000 41 929 000 22 665 000 11 959 000 3 322 000 782 000 1 884 000 26 478 000 16 698 000 9 158 000 6 301 000 6 300 000 7 274 000 3 718 000 3 123 000 6 958 000 4 192 000 2 890 000 2 040 000 3 398 000 1 158 000 1 144 000 940 000
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1916, 1917a,b; Rutgers, 1943]1967; Childers, 1969., bush and vine berries like strawberries, grapes and raspberries ŽRutgers, 1943]1967., sweet potatoes ŽPoole, 1922; Daines, 1942 and 1948; Pepper, 1944; USDA, 1946 and 1951; USDA, 1951; Knott, 1957., white potatoes ŽMatin, 1923; Rutgers, 1943]1967; USDA, 1946 and 1951; USDA, 1951; Knott, 1957., a wide variety of vegetables ŽCroy, 1917; Beattie, 1924 and 1951; NJAES, 1941, 1943a,b, 1958; Pepper, 1942, 1944; Thompson, 1944; USDA, 1946 and 1951; USDA, 1951, 1959; Frear et al., 1956, 1966 and 1972. and turfrlawns ŽUSDA, 1940; Wolfe, 1948; Rockwell and Grayson, 1956; Lawfield, 1959; Musser, 1962; Madison, 1971; Schery, 1973. from the early 1900s through to the early 1960s. Lead arsenate was recommended broadly to control insect pests on a number of crops in New Jersey. NJAES bulletins recommended lead arsenates on apples and a variety of vegetables. In a comprehensive circular describing recommended materials and application rates ŽPepper, 1944. NJAES list the following applications for commercial vegetables: asparagus, tomato, potato, sweet potato, eggplant, pepper, cucumber, squash, melons, etc. carrots, celery, corn, spinach and beets in various formulations including sprays, dusts and baits. The only vegetable for which lead arsenate was not recommended was beans. Since arsenic is highly toxic to beans, this is not surprising. Lead arsenate use on apples is significant because it is included on the regular apple spray calendars ŽRutgers, 1943]1967.; that is, lead arsenate was recommended for the routine spraying of apples throughout the growing season. For the other crop uses, lead arsenate was recommended annually or when a certain pest was a problem. The use of lead arsenate on apples first appeared in a New Jersey apple spray calendar in 1917 ŽNJAES, 1917a,b. and was probably used even before this date. Lead arsenate was recommended on apples for the control of red-banded leaf roller, curculio, canker worms, green fruit worms, tent caterpillars and scab. Application recommendations ranged from 2 to 4 lb lead arsenate in 100 gallons of water to be sprayed three or more times in the growing season.
Lead arsenate continued to be an important pesticide in the apple spray schedules through 1964 when it was recommended to be applied at a rate of 3 lb per 100 gallons. By 1967 ŽRutgers, 1943]1967. the synthetic organic pesticides Žprimarily DDT. started to appear much more frequently than lead arsenate though lead arsenate continued to be included. In fact, it was reported that the synthetic organic pesticides were more effective against common insects, and in the years following World War II, the use of arsenicbased pesticides declined rapidly with the ready availability of more economical and more effective synthetic organic insecticides like dieldrin and DDT. 3.2. Arsenic consumption in agriculture nationally Consumption of arsenic in the US has historically been primarily for the preparation of insecticides and herbicides. Other uses include the manufacturing of glass and in the preparation of drugs Žespecially early in the 20th century.. Paris green Ža copper arsenic compound. was first adopted as a means of combating the Colorado potato beetle. It is proposed that Paris green was first used against the potato beetle in the Western US in 1865 ŽFrear, 1942.. By 1868, its use had been fairly well established. Between 1880 and 1900, Paris green was probably the most commonly used insecticide, with London purple Žan arsenic compound. a close second ŽFrear, 1942.. By the 1930s, other uses of arsenic were growing, such as its use in ‘medicinal preparations, in lead alloys for bullets and shot, in pyrotechnic and boiler compositions, as a depilatory agent, in the manufacture of paint pigments, opal glass and enamels, in textile dying and calico printing, as a bronzing agent or decolorizing agent for glass, and for vermin poisons and sheep dips’ ŽUS Department of Commerce, 1917]1992.. Calcium arsenate found extensive use in the south between 1920 and 1950 where it was used for boll-weevil control in cotton fields, but was used as a general insecticide on a variety of vegetable crops and on white potatoes throughout the US.
E.A. Murphy, M. Aucott r The Science of the Total En¨ ironment 218 (1998) 89]101
Lead arsenates were used primarily in sprays and dusts for protection against insects attacking fruits and vegetables. The US Department of Agriculture’s annual Agricultural Statistics ŽUSDA, 1936]1980. lists consumption of arsenic in agriculture and separates lead arsenate consumption from calcium arsenate consumption. The data are presented in Table 2. The Bureau of Mines also presents information on arsenic consumption but does not always distinguish between lead arsenate and calcium arsenate Žsee Table 1.. The difference is important because calcium arsenate was used primarily against grasshoppers in the south and against the boll-weevil in the southeast, while lead arsenate was used more uniformly throughout the country. Therefore New Jersey’s consumption of calcium arsenate is more difficult to calculate than lead arsenate; the actual quantities of calcium arsenate used for purposes other than grasshopper and boll-weevil control are not clearly delineated. It is reported in the Bureau of Mines for some years that ‘most’ of the total US calcium arsenate consumption was used for boll-weevil or grasshopper control in the south and midwest. No actual amounts or percentages of calcium arsenate used for this purpose are presented. It was not until the 1920s that calcium arsenate was found to be highly effective against the boll-weevil, and its use in this capacity continued until around 1950. In order to account for calcium arsenate used exclusively for boll-weevil and grasshopper control, it is assumed that 50% of the US consumption of calcium arsenate occurred for this use between 1920 and 1950 and that the remaining 50% was available for other uses on vegetables and white potatoes throughout the country. For calcium arsenate data before 1920 and after 1950, the actual amounts reported in the Bureau of Mines or Agricultural Statistics are used. The data presented in this report represent these modifications of the available US consumption of calcium arsenate for 1920]1950. The Bureau of Mines reports the total quantities of white arsenic consumed in the US and the amounts consumed by dominant categories of users. On average, 69% the nation’s total con-
93
sumption of white arsenic was used to produce insecticides like lead arsenate and calcium arsenate during the country’s peak agricultural years. There were other arsenical insecticides produced but these two were the dominant forms. Herbicidal arsenicals Ži.e. sodium arsenite . consumed approx. 14]20% of the total consumption of white arsenic. In general, most of the arsenic consumed in the US went into pesticide production with a small percentage going into other industries like glass manufacturing. USDA Agricultural Statistics report specifically the quantities of lead arsenate and calcium arsenate Žnot just the arsenic used in their production. consumed in agriculture Žincluding use on golf courses and turf.. These differences in reporting are significant given the actual amount of arsenic contained in lead arsenate and calcium arsenate pesticides. Based on atomic masses, calcium arsenate was approx. 38% arsenic while acid and basic lead arsenates were 22% and 15%, respectively Ž18.5% average.. Because calcium arsenate contains more arsenic, by weight, than lead arsenate, its application in some areas may be important. It is therefore vital to know whether quantities being reported represent arsenic or lead or calcium arsenate. Peak use of both lead and calcium arsenate occurred from approx. 1930 to the late 1940s Žapprox. 60 000 000 lb of each., with some decline during the war years. By 1960, consumption of these pesticides was less than a quarter of what it was during the peak years Žto approx. 10 000 000 lb of each.. This decline, which continued through the 1970s, was probably due to the ready access of the more effective substitute synthetic organic pesticides. 3.3. Acres of arsenic-treated land in New Jersey The Census of Agriculture reports acreage of land devoted to specific crops for the country, for states and for counties. Acres of land in the US and in New Jersey that were potentially treated with arsenical pesticides were tabulated to the county level. In order to allocate arsenic ‘loads’ to New
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E.A. Murphy, M. Aucott r The Science of the Total En¨ ironment 218 (1998) 89]101
Jersey agricultural land, it is necessary to know the proportion of arsenic-treated land in New Jersey in relation to the US. ‘Arsenic-treated’ land is defined as land that probably received lead arsenate or calcium arsenate insecticide treatment based on the crop recommendations for the period. Because the Bureau of Mines and Agricultural Statistics report arsenic consumption on a national basis only, the amount of arsenic used by any particular state must be apportioned based on the state’s percent contribution of arsenictreated acres of land. Table 3 shows the average annual acreage of land by decade where arsenical insecticides may have been used nationally and statewide. Using this information, it is possible to calculate the percentage of arsenic-treated land that was in New Jersey. For instance, for the years 1900]1910, 2.2% of the nation’s lead arsenate-treated land and 3.4% of the nation’s calcium arsenate-treated land was in New Jersey. Therefore 2.2% of the lead arsenate and 3.4% of the calcium arsenate used nationally in agriculture can be apportioned to New Jersey. It was difficult retrieving information on the acreage of land devoted to sod and turf production since the Census of Agriculture does not include them. Some data are available for golf courses from various publications and the remainder is calculated based on existing data. From the 1920s and 1960s, a rather consistent 2]3% of the nation’s golf courses were in New Jersey. By the 1970s, this had fallen to 1.5%. Thomas Ž1927. wrote that a golf course, at a minimum, should have approx. 120 acres with up to 80 acres for fairways and greens. Using 80 acres as the minimum standard acreage potentially treated with pesticide ŽThomas, 1927. an approximate acreage can be calculated for New Jersey courses. In the early 1930s, there were approx. 158 courses in New Jersey Žof the 5700 in the country. totaling 12 640 acres of land; in the early 1950s, there were 126 courses in New Jersey Žof the 5350 in the country. totaling 10 080 acres of land. By 1994, there were 249 golf courses in New Jersey using approx. 19 920 acres of land in the state. Once the percentage of arsenic-treated land in New Jersey is calculated, that percentage is multi-
plied by the corresponding national arsenic consumption value. Data showing the statewide arsenic consumption in New Jersey are presented in Table 4. 3.4. Arsenic consumption in agriculture in counties in New Jersey The Census of Agriculture provides data on a county basis for states. Therefore it is possible to calculate, roughly, the amount of arsenic that may have been applied to New Jersey on a county basis using the same procedure as that used for the statewide calculation. Estimates of the amount of lead arsenate and calcium arsenate that may have been used per county in New Jersey were generated by multiplying the total amount used in the state by the percentage of arsenic-treated cropland in the county. For instance, the average annual amount of lead arsenate used in New Jersey in 1921]1930 Ž902 676 lb. was multiplied by 0.037, which is the proportion of arsenic-treated land in Atlantic county, to get 33 399 lb of lead arsenate applied to land annually in Atlantic County in the years 1921]1930. To further quantify the amount of actual arsenic applied in the form of lead arsenate, the amount of lead arsenate was multiplied by 0.185, which is the average amount of arsenic in acid or basic lead arsenate, and the amount of calcium arsenate was multiplied by 0.38, which is the amount of arsenic in this pesticide. To follow the above example for Atlantic County, 33 399 lb was multiplied by 0.185 to get 6179 lb of arsenic applied in the form of lead arsenate in Atlantic county annually from 1921 to 1930. Cumulative data are presented for all of New Jersey’s 21 counties from 1900 to 1980 in Fig. 1. From 1900 to 1980, approx. 15 000 000 lb of white arsenic was applied in New Jersey in the form of lead and calcium arsenate. The top five counties in New Jersey for total cumulative totals of white arsenic applied cumulatively are Burlington, Cumberland, Gloucester, Monmouth and Salem. It is interesting to note that in 1990 and 1994, 94 and 80 lb, respectively, of arsenic in the form of the organic arsenicals DSMA and MSMA were
Table 3 Percent contribution of New Jersey to US crops and golf courses on which arsenical pesticides were recommended for use Apples wPbAs recommendedx Žacres.
White potatoes wCaAs recommendedx Žacres.
Sweet potatoes wPbAs recommendedx Žacres.
Golf courses wPbAs or CaAs recommendedx Žacres.
Average annual number of acres treated with arsenical pesticides Žall.
1 011 374 86 227 1 475 274 94 996 2 814 132 130 449 3 415 069 148 841 4 120 006 159 988 3 615 378 136 229 3 333 772 113 235 3 457 252 79 556 3 462 714 66 575
4 824 771 34 964 3 366 761 43 578 2 825 564 48 278 1 907 968 34 289 1 292 911 21 989 675 833 13 941 524 039 10 855 577 967 8875 590 541 6130
3 668 855 72 991 3 251 703 82 533 2 927 434 49 582 3 113 658 51 161 2 025 406 52 546 1 205 652 20 290 1 173 918 16 869 1 395 150 7602 738 954 5929
641 525 22 504 803 662 15 427 558 508 12 294 831 668 15 201 532 845 15 109 239 756 15 094 112 128 7401 85 545 2356 95 240 2102
48 880 480 80 000 800 456 000 12 640 441 600 11 360 441 600 11 360 427 200 11 840 793 600 12 760 793 600 18 640 1 160 000 17 120
10 195 405 217 166 8 977 400 237 334 9 581 638 253 243 9 709 963 260 852 8 412 768 260 992 6 163 819 197 394 5 939 418 161 120 6 309 513 117 028 6 047 449 97 855
Percentage of As-treated acres in New Jersey All
PbAs
CaAs
2.1
2.2
3.4
2.6
2.7
3.4
2.6
3.1
3.7
2.7
3.2
3.1
3.1
3.3
3.0
3.2
3.6
3.4
2.7
3.0
3.2
1.8
2.2
2.7
1.6 1.7 Ž1.5 golf only.
1.9
The Census of Agriculture supplied acres of apples only for certain years Ž1937, 1978, 1982 and 1992.. To get the acres of apples, the total number of trees was divided by the known number of acres to get the average number of trees per acres for those years. These estimates were used to calculate the acres from the number of trees. For years 1940]1970, an average of the 1937 and 1978 estimate was used to calculate the number of acres. From Golf Architecture, the value of 80 acres of treated greens was offered as a typical golf course constructed in the 1930]1960s. To get acres of golf courses, the number of golf courses was multiplied by 80 to get the number of acres of green that would typically be treated with pesticide.
E.A. Murphy, M. Aucott r The Science of the Total En¨ ironment 218 (1998) 89]101
US 1900]1910 NJ 1900]1910 US 1911]1920 NJ 1911]1920 US 1921]1930 NJ 1921]1930 US 1931]1940 NJ 1931]1940 US 1941]1950 NJ 1941]1950 US 1951]1960 NJ 1951]1960 US 1961]1970 NJ 1961]1970 US 1971]1980 NJ 1971]1980 US 1981]1990 NJ 1981]1990
Vegetables ŽPbAs or CaAs recommendedx Žacres.
95
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E.A. Murphy, M. Aucott r The Science of the Total En¨ ironment 218 (1998) 89]101
Table 4 Average annual consumption of lead and calcium arsenate insecticides in New Jersey from 1900 to 1980 Year
US PbAs consumption
NJ contribution of PbAs-treated crops Ž%.
PbAs used in New Jersey agriculture and golf courses Žlb.
US CaAs consumption
New Jersey contribution of CaAstreated crops Ž%.
CaAs used in New Jersey agriculture and golf courses Žlb.
1900]1910 1911]1920 1921]1930 1931]1940 1941]1950 1951]1960 1961]1970 1971]1980 1981]1990
724 036a 9 147 265a 29 118 597 43 803 185 46 429 000 12 336 000 7 437 000 5 093 000 No datac
2.2 2.7 3.1 3.2 3.3 3.6 3.0 2.2 1.7
15 929 246 976 902 676 1 401 702 1 532 157 444 096 223 110 112 046 No data
291 188 3 678 791 14 962 397b 1 332 427b 20 447 500b 8 865 000 3 589 000 940 000 No data
3.4 3.4 3.7 3.1 3.0 3.4 3.2 2.7 1.9
9900 125 079 553 609 41 305 613 425 301 410 114 848 25 380 No datac
a
These values calculated using Bureau of Mines total arsenic consumption data: approx. 12]42%, on average, of the total arsenic was used to produce arsenical insecticides, so 12]42% of the arsenic consumption was halved to estimate the amounts of arsenic used to manufacture these two dominant insecticides. Since acid and basic lead arsenate is, on average, 18.5% arsenic and calcium arsenate is 46% arsenic, the arsenic values were divided by 0.18 and 0.46, respectively, to determine the lead and calcium arsenate estimates. All subsequent data are from USDA Agricultural Statistics yearbooks. b Reflects 50% deduction of the total consumption to account for boll-weevil and grasshopper use in the South and Midwest. c Data after 1972 was not released by either Bureau of Mines nor Agricultural Statistics due to reasons of confidentiality to producers.
Table 5 Cumulative total arsenic applied in the form of lead arsenate Žacidrbasic. and calcium arsenate in New Jersey 1900]1980 using values calculated from national consumption data and crop recommendations Years National consumption data method 1900]1910 1911]1920 1921]1930 1931]1940 1941]1950 1951]1960 1961]1970 1971]1980 80-Year total Crop recommendations method 1900]1950
Arsenic Žlb.
PbAs Žlb.
67 090 932 210 3 773 660 2 750 110 5 165 500 1 966 940 849 180 303 730 15 808 420
159 290 2 469 760 9 026 760 14 017 020 15 321 570 4 440 960 2 231 100 1 120 460 48 786 920
8 880 000] 37 000 000
48 000 000] 200 000 000 Žapples.
CaAs Žlb.
99 000 1 250 790 5 536 080 413 050 6 134 250 3 014 100 1 148 480 253 800 17 849 550
1900]1960
10 855 350] 108 553 500
33 666 000] 33 660 000
1921]1950
4 644 000] 69 660 000
14 400 000] 216 000 000 Žgolf.
Total
66 179 350] 215 213 500
48 000 000] 200 000 000
48 066 000] 249 666 000
E.A. Murphy, M. Aucott r The Science of the Total En¨ ironment 218 (1998) 89]101
Fig. 1. Total pounds of arsenic applied cumulatively in New Jersey counties, 1900]1980.
applied to golf courses according to unpublished data collected by the NJDEP Pesticide Control Program. 3.5. Rates of arsenic application recommended by the USDA and the NJAES Estimates of quantities of lead arsenate and calcium arsenate applied in New Jersey have been presented on a county-wide basis in Fig. 1. To test how accurate these estimates are, another method of calculating rates was applied. Recommended rates of arsenic application in the USDA and NJAES bulletins and circulars were used to calculate the possible maximum number of pounds of arsenicals recommended per acre per year on given crops, assuming that every acre of land used to grow these crops used the recommended amounts. Application rates in the apple spray calendars were 2]4 lb of lead arsenate mixed in 100 gallons of water and sprayed 3]5 times in a growing season with 400]500 gallons being used per acre. Therefore approx. 24]100 lb of lead arsenate could have been sprayed on apple orchards in a growing season, using these maximum recommendation rates. Actual application rates of lead arsenate to apple orchards have been reported by
97
Stevens et al. Ž1970. in four states. The rates range from 4]100 lbracre in the 1950s to 3]23 in the 1960s and 0]26 in the late 1960s. These reported rates correspond with the recommended rates in the apple spray calendars. To determine the annual application on apples, the total number of acres of land used to grow apples in New Jersey from 1900 to 1950 Ž40 000 acres. was multiplied by the application rate of 24]100 lbracre. Approximately 960 000]4 000 000 lb of lead arsenate could have been sprayed on apples annually using the crop recommendations. Lead and calcium arsenates were recommended at relatively high rates when used as insecticides on white potatoes, cabbage and related crops, melons and cucumbers. USDA bulletins from the 1920s through the early 1950s ŽBeattie, 1924 and 1951; Thompson, 1944; USDA, 1946 and 1951. call for calcium arsenate to control the Colorado potato beetle on potatoes, cabbage worms on cabbage and related crops, and the striped and spotted cucumber beetle on melons and cucumbers. These bulletins direct the application of the chemical as either a dust or a spray. The dust formulation was one pound of calcium arsenate to 2]3 lb of hydrated lime, with application rates of 15]30 lb of the dust per acre. For cucumbers, a less concentrated dust was recommended Ž1 lb calcium arsenate to 9 lb gypsum., but it was suggested that the dust be applied up to 10 times per season when striped or spotted cucumber beetles were prevalent. Spray recommendations were for 2]3 lb calcium arsenate to 50 gallons of water, with 75]125 gallons to be used per acre. Based on these bulletins, the overall recommended application of lead or calcium arsenate was 3]30 lbracre. Approximately 187 000 acres of land were used on average to grow vegetables and potatoes in New Jersey from 1900 to 1960, so approx. 561 000]5 610 000 lb per year could have been applied. Arsenates of lead were recommended for the control of earthworms, grubs and ants in turf and lawn fields as described in various USDA and NJAES bulletins ŽUSDA, 1940; Wolfe, 1948. and other publications ŽRockwell and Grayson, 1956; Lawfield, 1959; Musser, 1962; Madison, 1971; Schery, 1973.. On average, 40]600 lb of lead or
98
E.A. Murphy, M. Aucott r The Science of the Total En¨ ironment 218 (1998) 89]101
calcium arsenate was recommended. This means that approx. 480 000 to just over 7 000 000 lb per year could have been applied to the 12 000 acres of golf courses that existed in the state from 1920 to 1950. Cumulative totals of lead and calcium arsenate and the corresponding arsenic that could have been applied in New Jersey using the crop recommendations method are presented in Table 5. Data are presented using the method described in this report, which calculates the estimates based on national consumption data, and using crop recommendations for the period. It is evident here that the method relying on national consumption data results in lower estimates than those generated using the crop recommendations. This is actually to be expected since the crop recommendations are simply that } recommendations. It is unlikely that every acre of every vegetable, fruit and golf course in the state consistently received the maximum application of pesticide. The actual amount of pesticide used probably falls somewhere between the two estimates and is probably closer to those reached using national consumption rates. 4. Discussion It is possible to estimate the amounts of a particular pesticide applied in agriculture on a statewide and county-wide basis. Heavy metals like arsenic applied in the past may persist indefinitely in the environment. In fact, elevated levels of lead and arsenic have been found in former orchard soils in New Jersey ŽFields et al., 1993. and elsewhere in the US ŽStevens et al., 1970.. Cumulative totals of lead arsenate or calcium arsenate insecticides applied to New Jersey crop land and golf courses from 1900 to 1980 using consumption values are approx. 49 000 000 lb of lead arsenate and 18 000 000 lb of calcium arsenate. Of this, approx. 15 000 000 lb was in the form of arsenic. Using crop recommendations, the cumulative arsenic total was 66 000 000]215 000 000 lb. While a certain percentage of applied arsenicals may volatilize ŽWoolson, 1977; Woolson and Isensee, 1981. and an even smaller percentage is taken up by plants ŽKabata-Pendias and Pendias,
1992; Domir et al., 1967; Woolson et al., 1971a,b, 1973; Woolson, 1975; Pyles and Woolson, 1982; Merwin et al., 1994., the rest either remains in soil ŽStevens et al., 1970; Woolson et al., 1971a,b; Woolson, 1975, 1977; Aten et al., 1980; Woolson and Isensee, 1981; Wauchope and McDowell, 1984; Kabata-Pendias and Pendias, 1992; Merwin et al., 1994; Redondo et al., 1994; Sanok et al., 1995. or leaches to subsoil ŽWood, 1985; Schimmack and Bunzl, 1986; Woolson et al., 1973; Davenport and Peryea, 1991; Elfving et al., 1994; Peryea and Creger, 1994; Yin et al., 1996.. Some investigators have measured not only total arsenic present in soils but water-soluble fractions as well. It is the water-soluble fraction that may be available Ži. to leach to subsoils or ground water and Žii. to be taken up by crops. Although arsenic is not considered to be highly mobile, its downward migration has been shown to be greater in a sandy soil than in a clay loam ŽElfving et al., 1994.. Scientists have been measuring total arsenic and have guessed at its water solubility since the early part of this century. As reported in the New Jersey Agricultural Experiment Station Bulletin 419 from 1925, Haywood and McDonnell ŽNJAES, 1925. have demonstrated that lead arsenate is much more soluble in tap water than in distilled water in agricultural spraying experiments. Stewart ŽNJAES, 1925. also found that 10 times as much lead arsenate was dissolved in tap water as in distilled water and attributed the dissolution to the presence of chloride and calcium and magnesium in the water. The arsenic formed salts chiefly of chlorides and bicarbonates in the tap water. Any increase of carbonate, bicarbonate, or potassium ions is accompanied by an increase in the dissolution of the arsenate; waters with high chloride also had an increased solution effect on lead arsenate. In the Stewart study, it was found that nitrates and sulfates increased the solubility of lead arsenate only slightly, while neutral chlorides increased solubility significantly. Since lead arsenate was often recommended to be applied with lime-sulphur, this practice may have prevented any increase in the solubility of the arsenic caused by the presence of chlorides in the spray water. However, in cases where liming did not accompany the appli-
E.A. Murphy, M. Aucott r The Science of the Total En¨ ironment 218 (1998) 89]101
cation of an arsenical, the possibility of mobility exists. Clearly, scientists were concerned with available arsenic from the standpoint of phytotoxicity. Later, scientists like Woolson et al. Ž1971a. determined that the form of arsenic ŽFe-, Al- or Ca-As. was more important than total arsenic present in soil. Soils with extremely high reactive Al levels were less phytotoxic even after heavy applications of arsenic than soils with low reactive Al contents, presumably because the arsenic was tightly bound to the aluminum. Subsequent studies ŽWoolson et al., 1973. confirmed this. In the latter study, the percentage of water-soluble arsenic increased as the application rate increased but was higher in the soil having a higher pH with low extractable Fe, Al and Ca. Al-As remained at 40]50% of total arsenic applied, indicating that aluminum may act as a reservoir for arsenic. Both Fe and Al may form relatively insoluble arsenic compounds. At comparable soil arsenic levels, the addition of P increased the arsenic content of the plant significantly. In an experiment with Dunkirk fine sand Ža New York orchard soil. containing 625 ppm arsenic from normal pesticidal applications of lead arsenate, the amount of arsenic removed by KH 2 PO4 leaching was a function of the amount of leachate used. Initially, arsenic was leached rapidly from the soil Ž77% of the total arsenic present was leached from the soil. then decreased over time. Southern New Jersey soils are generally high in aluminum and iron with low pH, indicating that leaching, if it did occur, probably was not significant enough to pose a ground water problem. In the north, however, conditions are such that perhaps leaching was more severe. It is possible that some of the arsenic applied to New Jersey agricultural crops was mobile, or that it volatilized. Most commercial lead arsenates contained some small percentage of soluble arsenic. The New Jersey Experiment Station analyzed common pesticides on an annual basis. In 1925 the amount of soluble arsenic found in the water solutions after an extraction of 24 h varied from 1.02 to 2.35% with an average of 1.60% ŽNJAES, 1925.. In the 1928 evaluations, the solu-
99
ble arsenic ranged from 0.07 to 1.69% in lead arsenates Žsoluble arsenic in Paris Green were ordinarily higher: 1.01]3.26%.. While these percentages are low, given the rather large amounts of arsenic applied to soils, there is the possibility of some leaching to subsurface soils or to shallow ground water. The major repository, however, of this soil-applied arsenic is probably the soil and subsoil itself. References Aten CF, Bourke JB, Martini JH, Walton JC. Arsenic and lead in an orchard environment. Bull Environ Contam Toxicol 1980;24:105]115. Beattie JH. Watermelons, USDA Farmers’ Bulletin 1394, Washington, DC, 1924 and 1951. Childers NF. Modern fruit science. New Brunswick, New Jersey: Rutgers University Press, 1969. Croy MS. Putnam’s vegetable book. G.P. Putnam’s Sons, New York: The Knickerbocker Press, 1917. Daines RH. Scurf, black rot, and stem rot of sweet potatoes. New Jersey Agricultural Experiment Station, Rutgers University, New Brunswick, New Jersey, Circulars 437 and 514, 1942, 1948. Davenport JR, Peryea FJ. Phosphate fertilizers influence leaching of lead and arsenic in a soil contaminated with lead arsenate. Water Air Soil Pollut 1991;57r58:101]110. Domir SC, Woolson EA, Kearney PC, Isensee AR. Translocation and metabolic fate of monosodium methanearsonic acid in wheat. J Agric Food Chem 1967;24:1214]1217. Elfving DC, Wilson KR, Ebel JG, Manzell KL, Gutenmann WH, Lisk DJ. Migration of lead and arsenic in old orchard soils in the Georgian Bay region of Ontario. Chemosphere 1994;29:407]413. Fields TW, McNevin TF, Harkob RA, Hunter JV. A summary of selected soil constituents and contaminants at background locations in New Jersey. Trenton, NJ: NJDEP, 1993. Frear DEH. Chemistry of insecticides and fungicides, chap. II: the arsenicals. New York: Van Nostrand Co., Inc., 1942. Frear DEH, Friedman S, DeMartino T. Pesticide handbook } Entoma. State College, Pennsylvania: College Science Publishers, 1956, 1966 and 1972. Kabata-Pendias A, Pendias H. Trace elements in soils and plants. 2nd ed. Ann Arbor, MI: CRC Press, 1992. Knott JE. Handbook for vegetable growers. NY: John Wiley and Sons, 1957. Lawfield WN. Lawns and sportsgreens. London: W.H. and L. Collingridge, Limited, 1959. Madison JH. Practical turfgrass management. NY, Van Nostrand Reinhold and Co., 1971. Matin WH. Potato diseases in New Jersey and their control.
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New Jersey Agricultural Experiment Station, Circular 146, Rutgers Univ., New Brunswick, New Jersey, 1923a. Merwin I, Pryune PT, Ebel JG, Manzell KL, Lisk DJ. Persistence, phytotoxicity and management of arsenic, lead and mercury residues in old orchard soils of New York State. Chemosphere 1994;29:1361]1367. Musser HW. Turf management. NY: McGraw-Hill Book Co., Inc., 1962. New Jersey Agricultural Experiment Station. Rutgers University, New Brunswick, New Jersey, Circular 50, 1888. New Jersey Agricultural Experiment Station. Rutgers University, New Brunswick, New Jersey, Circular 86, 1892. New Jersey Agricultural Experiment Station. Rutgers University, New Brunswick, New Jersey, Circular 15, 1912. New Jersey Agricultural Experiment Station. Rutgers University, New Brunswick, New Jersey, Circular 44, 1916. New Jersey Agricultural Experiment Station. Rutgers University, New Brunswick, New Jersey, Circular 80, 1917a. New Jersey Agricultural Experiment Station. Rutgers University, New Brunswick, New Jersey, Circular 81, 1917b. New Jersey Agricultural Experiment Station. Rutgers University, New Brunswick, Bulletin 419, 1925. New Jersey Agricultural Experiment Station. The answer to your tomato problem. Rutgers University, New Brunswick, New Jersey, Circular 414, 1941. New Jersey Agricultural Experiment Station. Farm science goes to war. Rutgers University, New Brunswick, New Jersey, 1943a. New Jersey Agricultural Experiment Service. Vegetable crop notes. Rutgers Univ, New Brunswick, New Jersey, 1943b. New Jersey Agricultural Experiment Station. Pesticides, economic poisons inspection series 71. New Jersey Agricultural Experiment Station, Rutgers University, New Brunswick, New Jersey, 1958. Pepper BB. Controlling insects in the home vegetable garden. New Jersey Agricultural Experiment Station, Rutgers University, New Brunswick, New Jersey, Circular 443, 1942. Pepper BB. Vegetable insects and their control on commercial plantings. New Jersey Agricultural Experiment Station, Rutgers University, New Brunswick, New Jersey, Circular 476, 1944. Peryea FJ, Creger TL. Vertical distribution of lead and arsenic in soils contaminated with lead arsenate pesticide residues. Water Air Soil Pollut 1994;78:297]306. Poole RF. Sweet potato diseases in New Jersey. New Jersey Agricultural Experiment Station, Circular 141, Rutgers Univ., New Brunswick, New Jersey, 1922. Pyles RA, Woolson EA. Quantitation and characterization of arsenic compounds in vegetables grown in arsenic acid treated soil. J Agric Food Chem 1982;30:866]870. Redondo MJ, Ruiz MJ, Boluda R, Font G. Persistence of pesticide residues in orchard soil. Sci Total Environ 1994;156:199]205. Rockwell FF, Grayson EC. The complete book of lawns. NY: The American Garden Guild and Doubleday and Co., Inc., 1956.
Rutgers Extension Service Spraying Recommendations for Apples, Peaches, Potatoes, Strawberries, Grapes and other small berries. Spray Calendars 1-95A, Rutgers University, New Brunswick, New Jersey, 1943]1967. Sanok WJ, Ebel JG, Manzell KL, Gutemnann WH, Lisk DJ. Residues of arsenic and lead in potato soils on Long Island. Chemosphere 1995;30:803]806. Schery RW. A perfect lawn, the easy way. NY: Macmillan Publishing Co., Inc., 1973. Schimmack W, Burzl K. Migration of solutes in a cultivated soil: effect of ploughing. Geoderma 1986;38:155]163. Stevens LJ, Collier CW, Woodhain DW. Pesticides in soil: monitoring pesticides in soils from areas of regular, limited and no pesticide use. Pest Monit J 1970;4:145]166. Thomas GC. Golf architecture in America. New York: The Times-Mirror Press, 1927. Thompson RC. Cauliflower and broccoli varieties and culture, Farmers Bulletin No. 1957. Washington, DC: USDA, 1944. US Department of Agriculture. Agricultural statistics, 1936, 1939, 1940, 1945, 1950, 1955, 1960, 1965, 1970, 1975, 1980. US Dept. of Agriculture. Planting and care of lawns, Farmers’ Bulletin No. 1677. Washington, DC, 1940. US Department of Agriculture. Vegetable gardeners’ handbook on insects and diseases, Miscellaneous Publication 605. Washington, DC, 1946 and 1951. US Department of Agriculture. Miscellaneous publication No. 605: Vegetable gardeners’ handbook on insects and diseases. Washington, DC: USDA, 1951. US Department of Agriculture. Insects and diseases of vegetables in the home garden. Home and Garden Bulletin No. 46, Washington DC, 1959. US Department of Commerce., Bureau of the Census, Census of ŽAGRICULTURE., 1910, 1925, 1930, 1945, 1950, 1955, 1960, 1965, 1970, 1975, 1980, 1982, 1992. US Department of Commerce. Bureau of Mines, Minerals Resources of the United States. Part 1. Metals, AKA Minerals Yearbook. Washington, DC, 1917]1992. Wauchope RD, McDowell LL. Adsorption of phosphate, arsenate, methanearsonate, and cacodylate by lake and stream sediments: comparisons with soils. J Environ Qual 1984;13:499]504. Wolfe DE. Killing turf weeds with chemicals, new jersey agricultural experiment station, Circular 513. Rutgers Univ., New Brunswick, New Jersey, 1948. Wood JM. EfFects of acidification on the mobility of metals and metalloids: an overview. Environ Health Perspect 1985;63:115]119. Woolson EA. Arsenical pesticides, ACS symposium series 7. American Chemical Society, Washington, DC, 1975. Woolson EA. Generation of alkylarsines from soils. Weed Sci 1977;25:412]416. Woolson EA, Isensee AR. Soil residue accumulation from three applied arsenic sources. Weed Sci 1981;29:17]21. Woolson EA, Axley JH, Kearney PC. The chemistry and phytotoxicity of arsenic in soils: I. contaminated field soils. Soil Sci Soc Am Proc 1971a;35:938]943.
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Yin Y, Li Y, Allen HE, Huang CP. Adsorptionrdesorption and transport of mercury and arsenic in New Jersey soils. MDEP-DSR Final Report, Trenton, NJ, 1996.