Environ. Sci. Technol. 1996, 30, 3525-3533
Global HCH Usage with 1° × 1° Longitude/Latitude Resolution Y I - F A N L I , * ,† A N N M C M I L L A N , † A N D M. TREVOR SCHOLTZ‡ Atmospheric Environment Service, Environment Canada, 4905 Dufferin Street, Downsview, Ontario, M3H 5T4 Canada, and ORTECH, 2395 Speakman Drive, Mississauga, Ontario, L5K 1B3 Canada
The global usage of technical HCH and lindane in 1980 and 1990 are presented. The total global usage for technical HCH was estimated to be 40 000 t in 1980 and 29 000 t in 1990, and for lindane it was 5900 t in 1980 and 4000 t in 1990. Based on these data, the global usage of both R-HCH and γ-HCH were calculated. The total usage of R-HCH was around 28 000 t in 1980 and 20 400 t in 1990, while the total usage of γ-HCH was around 11 900 t in 1980 and 8400 t in 1990. The ratio of γ-HCH to R-HCH was 0.43 in 1980 and 0.41 in 1990. The usage data on countries are then mapped to a grid system with 1° × 1° longitude/latitude resolution to be useful for modeling. It is suggested that banning usage of technical HCH by a number of countries, such as China in the early 1980s and the former Soviet Union in the beginning of 1990s, may contribute to the decline of the atmospheric concentrations of both R-HCH and γ-HCH in 19921993. While many countries banned use of technical HCH in 1980s, lindane was still used by many countries around world in 1990.
Introduction Hexachlorocyclohexane (HCH, also called benzene hexachloride) is an organochlorine insecticide used throughout the world and is available in two formulations: technical HCH (a mixture of different isomers) and technical lindane (almost pure γ-HCH). Although only γ-HCH possesses insecticidal properties, all isomers are acutely and chronically toxic (1). Also β-HCH and γ-HCH were reported to have reproductive and endocrine-disrupting effects (2, 3). The usage of HCH and other organochlorine insecticides contributes to an increased agricultural yield, the protection of livestock, and the elimination of vector-transmitted disease. However, the global contamination caused by indiscriminate usage of HCH and other pesticides over the past four decades has been found to be ubiquitous and persistent in various environmental media and biota (49). These contaminants have spread all over the world, even to remote areas like the North Pole, through long* Corresponding author e-mail address:
[email protected]. † Environment Canada. ‡ ORTECH.
S0013-936X(96)00312-4 CCC: $12.00
1996 American Chemical Society
range atmospheric transport, rivers, and ocean currents. HCH (R- and γ-isomers) was the major organochlorine insecticide detected in Arctic air and seawater (10-14). In Canadian Arctic snow, total HCH concentrations far exceed all other organochlorine compounds combined (15). As a result, the Arctic seas and nearby oceans serve as one of the significant sinks for toxic and bioaccumulative contaminants and become a new source of HCH to the global environment (16). Evidence has shown that over 8400 t of HCH residues is present in the surface seawater of the North Pole region. About 400 t of it are going southward to the Atlantic Ocean every year through water currents (15). All this indicates that the indiscriminate use of HCH and other pesticides over the past four decades poses a great ecological risk. The impact of the contaminants on ecosystems and humans is of great concern among the scientific, regulatory, and policy communities. The atmospheric modeling community has been working very hard to understand the occurrence and pathways of the contaminants. They try to differentiate between contributions from past use and from present sources and to predict how these inputs and concentrations in the various environmental compartments may change in the future. These models require information on usage of the pollutants as a basis for estimating emissions. The model results will vary significantly depending on the available usage data and how this usage data is processed into input for models. Since 1993, staff at the Canadian Global Emissions Interpretation Centre (CGEIC), Atmospheric Environment Services, Environment Canada have been working on collecting data on pesticides (17, 18). Information on registration status, trends in regional use/emissions, and mode and time of applications have been collected on a global basis. Our purpose is to compile information and create a computerized database of historical, present, and predicted global usage or sale of the highly toxic, persistent pesticides, such as aldrin, dieldrin, endrin, HCH, lindane, DDT, chlordane, endosulfane, heptachlor, and toxaphene. In this paper, we only deal with technical HCH and lindane. We assembled the usage data of these two species for more than 100 countries for the years 1980 and 1990. For those countries for which data in 1980 and 1990 are missing, the nearest year’s data were used as a replacement. Sources of usage information were United Nations’ reports, government reports, scientific publications, or other sources. Neither spatial nor temporal interpolation were made. In the near future, usage data will be translated into estimates of emissions. While there are widely accepted techniques for creating emissions inventories of stationary point sources, mobile sources, and some area sources, presently there are no accepted techniques to quantify the air-soil and air-water exchanges of pesticides and other chemicals. CGEIC is, therefore, working on the development and application of a pesticide emissions model (19).
Usage Data Based on Countries Table 1 gives the annual usage of technical HCH and lindane in 1980 and 1990 for some major consuming countries. The total global usage of technical HCH was estimated to
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TABLE 1
TABLE 2
Annual Technical HCH and Lindane Usage (t/yr) in 1980 and 1990 for Some Consuming Countriesa
Annual r-HCH and γ-HCH Usage (t/yr) in 1980 and 1990 for Some Consuming Countriesa
technical HCH in
r-HCH in
lindane in
γ-HCH in
country
1980
1990
1980
1990
country
1980
1990
1980
1990
Algeria Argentina Australia Belgium Brazil Canada China Egypt Former USSR France Germany Honduras India Italy Mexico Myanmar Niger Pakistan Poland South Korea Spain Sri Lanka Turkey Ukraine United Kingdom United States
NA 60 NA NA NA 0 14497 NA 1674 NA 120 NA 21570 25.5 150 1.7 511.2 91.4 2 120 NA 59.7 897.7 NA NA 0
66.8 6 NA 0 NA 0 0 0 0 0 120 NA 28400 4.5 261.5 NA NA 3.1 NA NA NA NA NA 240 NA 0
NA 183 55.8 22 80 286 0 201 NA 1171.8 211.4 4.4 141 1576.1 35 725.1 12 2.5 144.8 NA 139 NA 73.1 NA 86.5 268
4 0.6 NA 66 NA 284.5 100 0 NA 1863.3 76 137.1 NA 599.1 15 6 396.5 NA NA NA 95.7 NA NA 0 76.8 114.4
Algeria Argentina Australia Belgium Brazil Canada China Egypt Former USSR France Germany Honduras India Italy Mexico Myanmar Niger Pakistan Poland South Korea Spain Sri Lanka Turkey Ukraine United Kingdom United States
NA 42 NA NA NA 0 10147.9 NA 1171.8 NA 84 NA 15099 17.9 105 1.2 357.8 64 1.4 84 NA 41.8 628.4 NA NA 0
46.8 0 NA 0 NA 0 0 0 NA 0 84 NA 19880 3.2 183.0 NA NA 2.2 NA 0 0 NA NA 168 0 0
NA 192 55.8 22 80 286 2174.6 201 251.1 1171.75 229.4 4.4 3376.5 1579.9 57.5 725.4 88.7 16.2 145.1 18 139 9 207.8 NA 86.5 268
14.0 0.6 NA 66 NA 284.5 100 0 NA 1863.3 94 137.1 4260 599.8 54.2 6 396.5 0.5 NA 0 95.8 NA NA 36 76.8 114.4
a This information has been taken from several sources (20-32). NA, not available. 0, we use zero data here as long as we have information showing that the country banned use of technical HCH or lindane. However, technical HCH or lindane may still have been allowed for special applications; use of old stock may have been permissible or illegal use may have occurred after the ban (20, 24, 40).
be 40 000 t for 1980 and 29 000 t for 1990. The total global usage of lindane was 5900 t for 1980 and 4000 t for 1990. The above estimates do not include the amounts of pesticides that have been placed in storage or disposed of as waste. Since the usage information for many countries, including Australia, Brazil, and most countries in Africa, is not available, these figures may not give a complete technical HCH and lindane usage pattern. We are still trying to fill these gaps. According to data available in our database, in 1980, the annual consumption of technical HCH in two Asian countries, India and China, accounts for more than 84% of the total technical HCH consumption in the world. In 1990, although increased in India, the usage of technical HCH decreased dramatically among other countries. We can also see that the leading lindane consuming countries include developing countries as well as developed countries. In 1990, France, Italy, Niger, Canada, Honduras, the United States, and China were among the leading lindane consuming countries with annual usage more than 100 t. Generally, technical HCH contains the isomers in the following percentages (1): R, 55-80%; β, 5-14%; γ, 8-15%; δ, 2-16%; and , 3-5%. Technical lindane contains more than 90% of γ-HCH (33), but lindane used in many countries is almost pure γ-HCH. We converted technical HCH and lindane usage to R-HCH and γ-HCH usage by assuming that technical HCH contains 70% R-HCH and 15% γ-HCH and that technical lindane contains 100% γ-HCH. The results are shown in Table 2. The total global usage of R-HCH was estimated to be around 28 000 t in 1980 and
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a The data were calculated from the usage data in Table 1. Footnotes are the same as in Table 1.
20 400 t in 1990, and the total global usage of γ-HCH was around 11 900 t in 1980 and 8400 t in 1990. The ratio of γ-HCH to R-HCH was 0.43 in 1980 and 0.41 in 1990. In 1980, India and China were the top two leading R-HCH and γ-HCH consuming countries in the world. In 1990, however, India alone is the main source of R-HCH, and the top γ-HCH consuming countries were India and France, with annual usage more than 1000 t. Figure 1 presents trends in usage of R-HCH and γ-HCH for India, China, and the United States from 1948 to 1995. This figure shows that the United States used R-HCH around the1950s. The highest usage was around 4100 t per year. The usage of γ-HCH decreased from 5460 t in 1950 to 270 t in1970. The usage of R-HCH in India increased constantly before 1970, reaching 23 700 t in 1970, and stayed around 18 000 t a year from 1988 to 1992. The usage of γ-HCH in India reached 5100 t in 1970 and stayed around 4000 t a year from 1988 to 1992. The usage of R-HCH in China increased until 1980, reaching 10 000 t a year and stopped in 1983. The usage of γ-HCH in China increased constantly before 1980, reaching 2100 t a year, and decreased dramatically since then. China has been using around 500 t of γ-HCH a year since 1995.
Usage Data Based on Grid It can be very deceiving if the total annual amount of HCH used in a country is distributed over the whole country rather than attributed to a specific region. For example, the usage of lindane in the United States was primarily concentrated in the southern part, with no usage in Alaska (34). The major pesticide use areas in the former Soviet Union include the Russian and Ukraine Republics and the Republics of Middle Asia (25). Thus, it will be very useful
FIGURE 2. Relationship between the grid system and the political units.
distribution of usage data of HCH based on country among cultivated land with 1° × 1° longitude/latitude resolution. The methodology of doing this is as follows. Figure 2 shows the relationship between the grid system and the political units. The grid cell i is shared by two different political units, j and j′ (they can be countries or special regions). Ci is the cultivation intensity for grid i. There are five intensity classes that were located in each grid cell: 0%, 20%, 50%, 75%, and 100%, respectively (36). Rij in Figure 2 is the percentage of the overlaid area between the cell i and the unit j to the total area of the unit j. Consider the grid cell i, which contains Rij (percent) of total area of political unit j. The cultivation intensity of this cell is Ci. If the total usage of the pesticide in the political unit is Vj, then the usage in grid cell i by political unit j is given by
Vij ) FIGURE 1. Trends in usage of (a) r-HCH (calculated from technical HCH) and (b) γ-HCH (calculated from technical HCH and lindane) for India, China, and the United States.
if we can distribute the usage data based on country among some areas, say, cultivated land, instead of the whole country. The usage data, based on region, will be of only limited usefulness unless these data are assigned to proper use areas. The best global climate models today have a typical spatial resolution of about 3° latitude by 3° longitude (35). The area covered by each grid cell is about 300 km × 300 km. However, with increasing computing power, the scientists working on global climate and chemical dispersion models hope to improve the spatial resolution to 1° latitude × 1° longitude. Thus, each data point will represent a region of about 100 km × 100 km. Models on this scale can begin to simulate major topographical features that can influence pollutant transport. Our practice here is to map the HCH usage on a 1° × 1° longitude/latitude grid horizontal placed over the Earth Sphere. In order to distribute the HCH and lindane usage data in a 1° × 1° longitude/latitude grid system, we compiled a 1° × 1° longitude/latitude data set of countries and regions of the world. Our data set on political units consists of 17 660 grid cells and 223 countries and regions, which shows what political unit the cell belongs to and how much percent of the overlaid area between the cell and the unit compares with the total area of the unit. By using our global data set on political units and the NASA/GISS global distribution of cultivation intensity data set (36), we mapped the global
CiRij
∑C R
Vj
i ij
i
This methodology has been applied to usage data assembled by country in order to generate usage on a 1° × 1° longitude/latitude grid. To use this method, we assume that the cultivated land is evenly distributed over the grid cell, the pesticide HCH is only used in the cultivated area, and the amount of HCH used in the cultivated land is proportional to the cultivation intensities. For those countries that are not included in the cultivation intensity data set, like Omen, Cyprus, Suriname, and Kuwait, the usage data were distributed over whole country. Gridded global R-HCH usage with 1° × 1° longitude/ latitude resolution is shown in Figure 3. In 1980, the main areas using R-HCH were in India and eastern China. The south and northeastern part of India have the highest usage densities of R-HCH, reaching 100-135 t per grid cell. In 1990, India had almost the same usage pattern as that in 1980, although the usage of R-HCH was almost phased out in other areas. Figure 4 gives the usage patterns of γ-HCH in 1980 and 1990, which were quite similar in Europe, North America, and South Asia.
Results and Discussion Some monitoring data from several measurement programs support the usage data well. The monitoring data of HCH in air and water from eastern and southern Asia between 1989 and 1991 (41, 42) showed that many areas in India had very high levels of HCH in both air and water. In Calcutta, concentrations of HCH reached as high as 11 000
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FIGURE 3. Gridded global r-HCH usage (calculated from technical HCH) in (a) 1980 and (b) 1990 with 1° × 1° longitude/latitude resolution.
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FIGURE 4. Gridded global γ-HCH usage (calculated from technical HCH and lindane) in (a) 1980 and (b) 1990 with 1° × 1° longitude/latitude resolution.
ng/m3 in air and 200 ng/L in water. This is not surprising since a large amount of technical HCH was used in India during that time. Mean atmospheric concentrations of R-HCH and γ-HCH from the samples, which were collected at Resolute Bay, Canada, in August-September, 1992, were 2-3 times lower than summer Arctic levels in the 1980s (43). The measurements made between 1979 and 1993 from stations in the Canadian and Norwegian Arctic and from stations in the Bering and Chukchi Seas indicate that atmospheric concentrations of R-HCH in 1992-1993 were 2-4-fold lower than values in the mid-1980s. The atmospheric concentrations of γ-HCH also declined in the same period (16, 44). This may be because of banning usage of technical HCH by a number of countries, such as China in the early 1980s and the former Soviet Union in the beginning of 1990s. The reported information on HCH in this paper should be viewed with caution, since data on present and historical use of HCH (other persistent organochlorines as well) are difficult to obtain and uncertain. Many countries do not keep records on pesticides, while in other countries such information is confidential. Commercial data bases are costly to access. Therefore, to improve this data base and knowledge of usage of pesticides in general, international cooperation is required. The present work is a first attempt to distribute HCH usage based on countries over a grid system with 1° × 1° longitude/latitude resolution. In the near future, the gridded usage data presented here will be used in our pesticide emissions model (19) to produce atmospheric emissions for global environmental pathways models (4547).
Acknowledgments The authors would like to dedicate this paper to the memory of the late Dr. Eva Voldner, who started this work and had made great contributions until she died in 1994. The authors gratefully acknowledge the invaluable contribution from Dr. G. Shkolenok, IRPTC/UNEP, who arranged the contracted studies for the People’s Republic of China, the former Soviet Union, and GDR; from Dr. R. Biermann, Battelle Europe; Drs. T. Bidleman, L. Barrie, and D. Gregor, Ms. T. Shapiro, and Ms. C. Spencer, Environment Canada. This research is a contribution of the Global Emissions Inventory Activities (GEIA), a component of the International Global Atmospheric Chemistry (IGAC) core project of the International Geosphere-Biosphere Program (IGBP).
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Received for review April 8, 1996. Revised manuscript received July 14, 1996. Accepted July 17, 1996.X ES960312V X
Abstract published in Advance ACS Abstracts, October 1, 1996.
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