Original Article
Mercury Exposure from Interior Latex Paint
N Engl J Med 1990; 323:1096-1101October 18, 1990
- Abstract
- Abstract
Background.
Many paint companies have used phenylmercuric acetate as a preservative to prolong the shelf life of interior latex paint. In August 1989, acrodynia, a form of mercury poisoning, occurred in a child exposed to paint fumes in a home recently painted with a brand containing 4.7 mmol of mercury per liter (at that time the Environmental Protection Agency's recommended limit was 1.5 mmol or less per liter).
Methods.
To determine whether the recent use of that brand of paint containing phenylmercuric acetate was associated with elevated indoor-air and urinary mercury concentrations, we studied 74 "exposed" persons living in 19 homes recently painted with the brand and 28 "unexposed" persons living in 10 homes not recently painted with paint containing mercury.
Results.
The paint samples from the homes of exposed persons contained a median of 3.8 mmol of mercury per liter, and air samples from the homes had a median mercury content of 10.0 nmol per cubic meter (range, <0.5 to 49.9). No mercury was detected in paint or air samples from the homes of unexposed persons. The median urinary mercury concentration was higher in the exposed persons (4.7 nmol of mercury per millimole of creatinine; range, 1.4 to 66.5) than in the unexposed persons (1.1 nmol per millimole; range, 0.02 to 3.9; P<0.001). Urinary mercury concentrations within the range that we found in exposed persons have been associated with symptomatic mercury poisoning.
Conclusions.
We found that potentially hazardous exposure to mercury had occurred among persons whose homes were painted with a brand of paint containing mercury at concentrations approximately 2 1/2 times the Environmental Protection Agency's recommended limit. (N Engl J Med 1990; 323:1096–101.)
Media in This Article
Figure 1
Adjusted Urinary Mercury Concentrations in Persons Exposed to Paint Containing Mercury and Those Not Exposed.Table 1
Characteristics of Persons Exposed to Paint Containing Mercury and of Those Not Exposed.*Article Activity
- Article
MERCURY, in both its organic and inorganic forms, can be toxic to humans. Exposure to organic mercury during the late 1950s in Minamata, Japan, caused 41 deaths and at least 30 cases of infantile cerebral palsy.1 In the 1940s, inorganic mercury added to teething powders caused numerous cases of acrodynia, a form of childhood mercury poisoning.2 Despite its known toxicity, mercury is still used in many household products, such as latex (water-based) paint. Because of their fungicidal and bactericidal properties, mercury compounds have often been added to latex paint to prolong shelf life. Up to now, approximately one third of all interior latex paint in the United States has contained mercury.3 , 4
In August 1989, the symptoms of acrodynia developed in a four-year-old boy in Michigan 10 days after the inside of his home was painted with 64 liters (17 gallons) of interior latex paint containing phenylmercuric acetate. Leg cramps, a generalized rash, pruritus, sweating, tachycardia, an intermittent low-grade fever, marked personality change, erythema and desquamation of the hands, feet, and nose, weakness of the pelvic and pectoral girdles, and lower-extremity nerve dysfunction developed sequentially. A 24-hour urine sample contained 324 nmol of mercury per liter (reference value, <100). All four other family members had increased urinary mercury excretion. The only substantial source of mercury exposure common to them all was the paint applied to their home. Three samples from one unopened paint can remaining in their home contained an average of 4.7 mmol of mercury per liter. (The Environmental Protection Agency's recommended limit was 1.5 mmol per liter. The recommendation was based on fungicidal and bactericidal efficacy.5 6 7)
To determine whether mercury exposure had occurred among other persons whose homes had recently been painted with that brand of interior latex paint, we conducted a study in November 1989.
Methods
We studied 19 "exposed" families who lived in homes painted with the same brand of latex paint (manufactured by the Mercury Paint Company and containing phenylmercuric acetate) used in the ill child's home. The index family was not included in this group. The 19 homes were painted between June 1 and October 28, 1989, and had either 11 or more liters (3 gallons) of paint applied or three or more rooms painted. The families were recruited from a list of more than 100 persons who called the Michigan Department of Public Health after a press release announced that some interior latex paint produced by that manufacturer contained more than the recommended limit of mercury. Persons on the list were called until 19 families meeting the above criteria had been identified. "Unexposed" families were the families of employees of the Oakland County Health Department in Michigan or their acquaintances who lived in homes that either had not been painted in the previous 18 months or had been painted with paint that did not contain mercury additives. Since 13 of the 19 exposed families included a child ≤10 years of age, we selected only unexposed families with at least one child ≤10 years of age for comparison. All the study families lived in the northern and western suburbs of Detroit.
An interviewer obtained written informed consent for each family member and administered a questionnaire to an adult in each family. Specific information was gathered about possible sources of mercury exposure for all family members and about the painting history and other characteristics of the home. Samples of remaining liquid paint, indoor air, vacuum-cleaner-bag dust, and first morning urine were collected to analyze their total mercury content. Liquid paint samples were obtained from all paint cans that remained in the homes of the unexposed families and from paint cans used between June 1 and October 28, 1989, in the homes of the exposed families; the samples were digested with nitric and sulfuric acid before analysis for mercury. Samples of indoor air were collected in Hopcalite tubes with a personal air-sampling pump (Gilian) that operated for 12 hours at a flow rate of 0.5 liter per minute. Vacuum-cleaner-dust samples were sifted through a 60-mesh sieve, and the resulting dust was analyzed.
Samples of liquid paint, vacuum-cleaner dust, and urine were analyzed by cold-vapor atomic absorption. The limit of mercury detection was ≤10 nmol per liter for the paint, ≤10 nmol per kilogram for the dust, and 0.5 to 1.0 nmol per liter for the urine.8 , 9 Atomic absorption spectrophotometry was used to analyze samples of indoor air. The limit of mercury detection was 0.5 nmol per tube and ≤0.5 nmol per cubic meter.10 11 12 Because of pump failure, the limit was ≤3.5 nmol per cubic meter in the homes of two unexposed families.
We have reported the results of the urinary mercury determinations both unadjusted (nanomoles per liter of urine) and adjusted for the creatinine concentration of the urine (nanomoles per millimole of creatinine). The molecular weight of mercury is 201, and that of creatinine is 113. One nanomole of mercury per millimole of creatinine thus equals 201 μg of mercury per 113 g of creatinine, which is 1.77 μg of mercury per gram of creatinine. Unadjusted values were reported in much of the early literature and in the only comprehensive study of expected background concentrations of urinary mercury.13 Concentrations adjusted for creatinine have been used to reduce the variability of results in spot urine samples.14
Approximately three weeks after the initial urine samples were collected, a second sample of first morning urine was obtained from selected exposed persons: all 15 children ≤10 years of age with an initial urinary mercury concentration ≥50 nmol per liter or 5.6 nmol per millimole of creatinine; all 10 people over 10 years old with initial urinary mercury concentrations ≥100 nmol per liter or 11.3 nmol per millimole of creatinine; and 14 people arbitrarily chosen from families with a person meeting one of these criteria.
We performed multiple linear-regression analyses to identify factors that contributed significantly to the concentrations of mercury in the air in the 19 exposed homes and to identify factors that contributed significantly to the variance in the adjusted urinary mercury concentrations among the 65 exposed people who provided first morning urine samples.15 We included all factors in the initial regression model that were found to be significantly associated (P≤0.05) with the variable of interest on univariate analysis, as well as any other factors we thought important.
Because the urinary mercury concentrations were not normally distributed, the Wilcoxon signed-rank-sum test was used to test the significance of differences between the exposed and unexposed groups. The Kruskal—Wallis test was used when more than two groups were compared. Correlations were measured by the Spearman correlation coefficient.
Results
The exposed group consisted of 74 people in 19 households, and the unexposed group of 28 people in 10 households (Table 1Table 1
Characteristics of Persons Exposed to Paint Containing Mercury and of Those Not Exposed.*). One unexposed person was excluded from analysis because she had collected paint samples from exposed homes. The median age was 24 years (range, <1 to 72) in the exposed group and 30 years (range, 3 to 48) in the unexposed group. The exposed families had an average of 3.9 persons and the unexposed families an average of 2.8 persons. Seventeen of the exposed persons (23 percent) had participated in the painting of their homes. The homes of the exposed persons had been painted a median of 22 days before the study. Six of the homes of unexposed persons (60 percent) were painted more than three years before the study.Paint samples were obtained from all the homes of the exposed families, and each home contained at least one can of paint that contained ≥1.5 mmol of mercury per liter. The median mercury content of the paint in the 29 cans sampled from the exposed households was 3.8 mmol per liter. Paint in 26 cans (90 percent) contained more than 1.5 mmol of mercury per liter. Paint samples were obtained from the homes of six of the unexposed families (60 percent); no mercury was detected in any of these samples.
Air samples were obtained from the homes of all the exposed families (exposed households) and from the homes of 9 of the 10 unexposed families (unexposed households). The concentrations of mercury in the air were significantly higher in the exposed households than the unexposed households (P<0.001). The median air concentration in the exposed households was 10.0 nmol of mercury per cubic meter (range, <0.5 to 49.9). No mercury was detected in the air samples from the unexposed households. Among the exposed households, the mercury concentrations in the air were significantly higher in the homes that had had more rooms painted, had been painted more recently, had windows open for fewer hours a day at the time the questionnaire was administered, and were newer. The model r2 was 0.72 (Table 2Table 2
Factors Contributing to Mercury Concentrations in the Air on Multiple Linear-Regression Analysis.*).Sixty-five persons in the exposed group (88 percent) and 28 persons in the unexposed group (100 percent) provided samples of first morning urine for analysis. Samples were not obtained from two exposed adults who were traveling on business, nor from seven exposed children five years of age or younger who were unable or unwilling to provide samples. Urinary mercury concentrations, both adjusted and unadjusted, were significantly higher among the exposed persons than among the unexposed persons (P<0.001) (Fig. 1Figure 1
Adjusted Urinary Mercury Concentrations in Persons Exposed to Paint Containing Mercury and Those Not Exposed.). The median adjusted urinary mercury concentration was 4.7 nmol per millimole of creatinine in the 65 exposed persons (range, 1.4 to 66.5) and 1.1 nmol per millimole of creatinine in the 28 unexposed persons (range, 0.02 to 3.9) (Table 3Table 3
Median Urinary Mercury Concentrations in Persons Exposed to Paint Containing Mercury and in Those Not Exposed, According to Age.*). Fourteen exposed persons (22 percent) had urinary mercury concentrations ≥100 nmol per liter, and 45 exposed persons (69 percent) had concentrations ≥50 nmol per liter. Only one unexposed person (4 percent) had a concentration ≥50 nmol per liter.Among the exposed persons, there was a poor correlation between urinary mercury concentrations and the concentration of mercury in the air in the home (r = 0.17). The urinary mercury concentrations were higher, however, among exposed persons who were younger, applied the paint themselves, spent more hours in the home, and lived in homes painted less recently. The model r2 was 0.29.
A second urine sample was obtained from 39 exposed persons. The median mercury concentrations in the two samples were similar (7.7 and 8.6 nmol per millimole of creatinine, respectively; r = 0.76).
Samples of vacuum-cleaner-bag dust were obtained from seven exposed households (37 percent) and three unexposed households (30 percent). The dust samples from the exposed households had a higher mercury content (median, 188.4 nmol per kilogram; range, 26.4 to 267.7) than those from the unexposed households (median, 16.9; range, 9.5 to 64.8; P = 0.05).
Discussion
We found that homes recently painted with one brand of interior latex paint containing mercury had significantly higher mercury concentrations in indoor air than homes not recently painted with a paint containing mercury. People living in the recently painted homes had significantly higher urinary mercury concentrations than those living in the homes not recently painted with paint containing mercury.
A case of acrodynia prompted this study; however, this was not the first case of the disease associated with paint containing mercury. Acrodynia developed in a five-year-old boy with a urinary mercury concentration of 449 nmol per liter associated with paint containing 997 nmol of mercury per liter.16 Acrodynia has been reported in people with urinary mercury concentrations of 249 nmol per liter,14 a value comparable to the concentrations found among exposed children in our study. The long-term health effects associated with increased urinary mercury concentrations and the potential consequences to a child or fetus have not been well studied. In rats, however, maternal inhalation of mercury vapor results in the accumulation of mercury in the fetus.17 Occupational exposure to mercury has been linked to increased lymphocyte aneuploidy and chromosomal aberrations.18
Occupational studies have found increasing abnormalities with increasing urinary mercury concentrations. Tremor, decreased short-term memory, and delays in motor- and sensory-nerve conduction have been documented.19 20 21 22 23 24 25 26 27 28 29 30 31 32 Exposure to mercury was also the probable cause of neuromyasthenia (headache, weakness, unsteady gait, tremor, and psychological depression) in 59 workers after the application of paint containing mercury and the initial use of a boiler for heat.33
In this study, the median concentration of mercury in indoor air in exposed households (10 nmol per cubic meter) exceeded the acceptable residential concentration of 2.5 nmol per cubic meter suggested by the Agency for Toxic Substances and Disease Registry34 and was more than 600 times higher than the average concentration of mercury in outdoor air in the Detroit area (0.015 nmol per cubic meter) (Warner PO, Wayne County Health Department: personal communication). The measurements of mercury in the air in exposed households were taken an average of one month after painting had been completed and were probably higher during and immediately after painting. Investigators have measured 997 nmol of mercury per cubic meter during the application of paint indoors.35 After 30 minutes, the application of paint containing 997 nmol of mercury per liter resulted in a concentration of 847 nmol per cubic meter in the air.17 Since the National Institute for Occupational Safety and Health recommends no more than 249 nmol per cubic meter (a 10-hour time-weighted average) in a work setting, painters may be at risk of excessive exposure to mercury.36
Mercury is released from surfaces coated with a paint containing mercury after the paint has dried. Mercury concentrations measured in the air in seven buildings ranged from 8.0 nmol per cubic meter 7 days after painting to 0.35 nmol per cubic meter after 33 months.37 In another study, two hours after the application of paint containing 234 nmol of mercury per liter, a concentration of 18.9 nmol per cubic meter was detected in a room; after eight days, 6.5 nmol per cubic meter remained. Opening all windows and doors decreased the concentration to 1.5 nmol per cubic meter; however, if the doors and windows were then closed, the concentration of mercury in the air returned to the earlier (unventilated) value within three hours.38 The investigators concluded that mercury would be emitted at a rate of 499 nmol per day for 7 1/2 years. The vaporization of mercury from paint containing mercury compounds may be due to the presence of inorganic metallic mercury, which can be formed during the manufacture of the compounds or during light-catalyzed decomposition of the compounds.39 , 40
Humans readily absorb both inorganic and organic mercury vapor after inhalation. In the body, phenyl-mercuric acetate is rapidly broken down to form inorganic mercury. Inorganic mercury accumulates in the kidney, enters the brain and the fetus, and is excreted in the urine.14 Little information is available about urinary mercury levels, particularly in children. In 1961 the World Health Organization (WHO) measured urinary mercury concentrations in 1107 adults in 15 countries and found that 95 percent had concentrations below 100 nmol per liter and 89 percent had concentrations below 50 nmol per liter.13 On the basis of these results, a urinary mercury concentration of less than 100 nmol per liter is considered the background value for adults. A background urinary mercury concentration has not been established for children. The distribution of the urinary mercury values for unexposed persons in our study paralleled the WHO values. Among the exposed persons, however, 78 percent had concentrations below 100 nmol per liter, and only 31 percent had concentrations below 50 nmol per liter.
In our study, urinary mercury concentrations correlated poorly with the levels of mercury in the air. Urinary concentrations may not adequately reflect the current concentration in the air because of the long half-life of mercury in the body (40 to 60 days) and because mercury may be eliminated by unmeasured routes, such as sweat.14 , 41 Also, individual exposure to mercury may vary with the time spent in painted rooms, the depth and frequency of inhalation, the degree of ventilation in the room, and the likely decrease in mercury vapors over time. We found that exposed children had the highest urinary mercury concentrations. Young children may be at increased risk, since vapors containing mercury are heavier than indoor air and settle toward the floor.42
More mercury was detected in the dust samples from vacuum-cleaner bags in the exposed households than in those from the unexposed households. Because we did not determine when the bags had last been emptied or changed, the collection time our findings represent is unknown. The source of mercury in the unexposed households may have been dust from paint containing mercury released from deteriorating surfaces (as is the case with leaded paint) or soil containing mercury that was brought into the home (the mercury content of soil in the United States ranges from 0.05 to 22.9 nmol per kilogram).43 Children may be more exposed to soil and dust particles containing mercury than adults, since children are more apt to have contact with these particles on the floor and to put hands, feet, and objects in their mouths.
We believe the significantly higher urinary mercury concentrations we found in the exposed persons in our study were attributable to the vaporization of mercury from paint. None of the other sources of mercury exposure we evaluated accounted for the differences. We were not, however, able to evaluate the contribution of such household sources of mercury as adhesives, acoustical plates, or joint cement.
Our study showed that significant exposure to mercury occurred in persons exposed to Mercury Paint Company paint that contained a median concentration of mercury 2 1/2 times the previously recommended limit. However, because this was purely a recommended, not a legally enforceable limit, it is probable that many other paint manufacturers have exceeded it. Other kinds of paint preservatives besides mercury are available. On June 29, 1990, the Environmental Protection Agency therefore announced that compounds containing mercury could no longer be lawfully added to interior latex paint after August 20, 1990. The decision represented a voluntary end to this use of mercury and was made jointly with the National Paint and Coatings Association and the manufacturers of the mercury compounds. Interior latex paint containing mercury that was manufactured before August 20, 1990, may still be sold. Thus, proper ventilation during painting must be ensured.
We are indebted to the families who agreed to participate in this study, as well as to the following persons who gave us valuable assistance: Regine Aronow, M.D., director, and the staff of the Poison Control Center, Children's Hospital, Detroit; Ms. Terri Dibble and Mr. Jerry Wright, Oakland County Health Department; Mr. Bruce Davis, Wayne County Health Department; Ms. Louise Fabinsky, Region V, Agency for Toxic Substances and Disease Registry; Benjamin Johnson, M.D., Michael O'Keefe, and James Bedford, Ph.D., Michigan Department of Public Health; Charles P. Cubbage, Ph.D., Michigan Department of Agriculture; and Sue Binder, M.D., Edmond Maes, Ph.D., Jeff Sacks, M.D., Mark McClanahan, Ph.D., John Liddle, Ph.D., and Henry Falk, M.D., all from the Center for Environmental Health and Injury Control of the Centers for Disease Control.
The use of trade names is for identification and does not constitute endorsement by the Public Health Service or the Department of Health and Human Services.
Source Information
From the Division of Environmental Hazards and Health Effects (M.M.A., R.A.E., R.G.P., E.M.K.) and the Division of Environmental Health Laboratory Sciences (D.C.P.), Center for Environmental Health and Injury Control, Centers for Disease Control, Atlanta; the Environmental Response Branch, Environmental Protection Agency, Edison, N.J. (P.R.C.); the University of California at San Diego School of Medicine, San Diego (D.S.C.); and the Center for Environmental Health Sciences, Michigan Department of Public Health, Lansing (J.L.H.). Address reprint requests to Dr. Etzel at Mail Stop F28, Centers for Disease Control, 1600 Clifton Rd., Atlanta, GA 30306.
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