Fluorides in the Air

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Fluorides in the Air[HH_Newsletter] Fluorides in the Air

 

 

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Fluoride Action Network

Fluorides in the Air

 

 

 

 

 

 

Environment, Vol. 15, No. 3

 

p. 25-32.

 

Fluorides in the Air

 

by Michael J. Prival and Farley Fisher

 

 

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MICHAEL J. PRIVAL and-FARLEY FISHER were research associates at the Center

for Science in the Public Interest at the time this article was written.

 

 

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WHEN A RANCHER sold 54 acres of his Garrison, Montana, land to the Rocky

Mountain Phosphate Company it was a matter of civic pride. The new factory

promised jobs and tax revenues for the industry-hungry region. Four years later,

the Ponderosa pine and Douglas fir were turning brown, and the cattle on

Garrison's ranches were so crippled they could not stand up. It took six years

of vigorous and frustrating campaigning before the residents of Garrison

succeeded in forcing the Rocky Mountain Phosphate Company to close permanently

in January 1970.

 

The story of Garrison (1) is but one of many in which an industry and its

neighbors have fought long and bitter battles over the damage caused by

fluorides in the air. The federal government and many affected states have been

slow to enact regulations to control fluoride air pollution. They have taken

action only when public pressure has forced them to recognize an emergency, such

as in the case of Garrison, where the people had to struggle to shut down an

industry that threatened the very existence of their town. Unless more decisive

steps are taken to control fluoride pollution, other American communities that

successfully attract new industry may suffer as Garrison did.

 

Fluoride is released into the air in large quantities by aluminum

reduction plants, phosphate processors, steel mills, coal burning operations,

brick and tile manufacturers, and various less significant sources.(2)

 

It can cause adverse effects when ingested by domestic animals or absorbed

by plants. There are also reports that fluoride air pollution can adversely

effect human health, though these are less well documented than those concerning

sensitive animals and plants.

 

Fluorides are released into the air in both a gaseous state (as hydrogen

fluoride and silicon tetrafluoride) and in solid particles. The particles fall

on, and the gases are absorbed by, vegetation near the polluting industry. If

this vegetation includes forage crops which are fed to cattle, sheep, horses, or

pigs, serious problems may ensue, since these animals, particularly the cattle,

are vulnerable to fluoride. (3) In fact, according to the U.S. Department of

Agriculture, " Airborne fluorides have caused more worldwide damage to domestic

animals than any other air pollutant. " (4)

 

Ninety-six percent of the ingested fluoride that accumulates in the bodies

of animals is incorporated into the crystal structure of bone and tooth

mineral.(5) When fluoride is ingested with food or water, most of that which is

not deposited in the bones, teeth, and other calcified tissue is excreted in the

urine within hours of ingestion.(6) Thus it is not surprising that fluoride

mainly affects the bones and teeth.

 

Teeth are more markedly affected by ingested fluoride than are bones, but

their high sensitivity is limited to the period of their formation. Thus a cow

that has not been exposed to excessive fluoride before the age of two and

one-half to three years will not develop the severe dental lesions which would

occur in the same animal exposed at a younger age.(7) The developing tooth

exposed to small amounts of fluoride may experience color variations

( " mottling " ) that have little or no effect on the animal's ability to eat.

Higher levels of fluoride result in more serious dental abnormalities, ranging

from small, brittle, chalky areas on the tooth surface to pitting of enamel and

easily eroded teeth.(3) Even more serious effects, including severe pain and the

wearing down of the tooth right to the gum, can prevent the cattle from drinking

cold water or eating.

 

Localized or generalized enlargement of certain bones in the legs

(metacarpals and metatarsals) and the lower jaw (mandible) of cattle are common

symptoms of excessive fluoride ingestion.(8) As highly abnormal bone tissue

replaces normal bone, (9) overall enlargement occurs, and the normally smooth

bone surfaces take on a chalky, white, irregular appearance.(3) Hard ground can

cause fluorotic hoof (pedal) bones to fracture, resulting in severe lameness.(7)

Cattle with advanced fluorosis may also be crippled by mineralization of

ligaments, tendons, and the structures surrounding the joints.(10) Enlargement

of the joints themselves may also contribute to lameness. Fluoride-induced tooth

destruction, lameness, and stiff joints affect the animals ability to stand,

eat, and graze, and all tend to lower the milk yield of dairy cattle or the

weight of beef cattle.

 

Economic loss due to the crippling of animals by fluoride has been

reported in widely scattered areas of the US The crippling of cattle in

Garrison, Montana, was but one of many similar cases. The Cominco American

Phosphate Company moved out of Douglas Creek, Montana, after being successfully

sued for $250,000 in 1968.(11) Phosphate processing operations in Florida have

affected both cattle and horses, (12) and crippling of cows has recently

destroyed dairy operations near the Ormet Aluminum plant in Hannibal, Ohio.

There have been complaints of damaged cattle teeth in the Massena, New

York-Cornwall, Ontario area, where both the Reynolds Metals and Alcoa aluminum

plants emit fluoride.(13) A farmer in Ferndale, Washington, recently won an

$83,060 judgment against the Intalco Aluminum Company.(14) US Steel paid $4

million to cattle ranchers around its steel mill near Provo, Utah, before

spending $9 million on fluoride-control devices.(15) The number of out-of-court

settlements of claims of fluoride damage to animals and vegetation is impossible

to determine, though it certainly exceeds the number of court-ordered payments.

 

Effects on Plants

 

When the Anaconda Company opened its aluminum reduction plant in Columbia

Falls, Montana, in 1955, company officials insisted that damage to animals and

vegetation from fluoride emissions would be negligible. By 1969, following

several expansions of the plant, dead and dying trees were observed over the

entire west face of Teakettle Mountain, which stands between the reduction plant

and Glacier National Park.(16) Trees on 2,000 acres of US Forest Service land

have been destroyed (17) and fluoride has damaged lodgepole, white, and

Ponderosa pines, and Douglas firs in Glacier National Park, eight miles from the

plant.(16) As the data accumulate, the destruction of these unique national

resources continues unabated. There are also documented reports of damage to

trees and crops from fluoride emissions in Oregon, Washington, Idaho, and New

York.(18)

 

Airborne fluoride can damage either the foliage or the fruit of a wide

range of plants, and the amount of fluoride necessary for this depends on the

species involved. The most characteristic type of lesion is " tip burn, " in which

the tips and edges of leaves turn brown in a characteristic pattern. The dead

tissue may separate from the rest of the leaf and fall off, (19) decreasing the

rate at which the whole plant grows. In the case of ornamental plants, of

course, tip burn adversely affects the aesthetic and economic value of the

plant, regardless of its effects on overall growth. For example, airborne

fluorides from the intensive phosphate processing done in central Florida have

damaged a major local gladiolus industry.

 

Plants with foliage particularly susceptible to fluoride damage include:

apricots, grapes, plums, corn, sorghum, Jerusalem cherry, gladiolus, iris, St.

John's wort, tulips, Douglas fir, western larch, and many species of pine.(20)

Many other plants, including citrus trees, have suffered significant leaf damage

from fluoride pollution but are not quite as sensitive as the above species.

 

In some plants it is the fruit which is effected by fluoride, while the

leaves may be either sensitive or resistant. Peaches, for example, get soft

suture disease or " suture red spot, " in which the region of the peach along the

seam near the tip ripens before the rest of the fruit. Thus, if the peach is

picked and eaten when the rest of the fruit is ripe, this region is already

over-ripe and soft, and often the fruit is split under the skin.(19) Fluoride

causes " snub nose " or " shrivel tip " in cherries. The tip ripens and shrivels

prematurely.(19) Fluoride from aluminum manufacture has been found to cause

similar damage to apricots and pears growing near the Rhone River in

Switzerland.(21) Economic loss to farmers, not to mention the loss of pleasure

to consumers, can easily result from such crop damage.

 

Occupational Exposure

 

The effects of airborne fluorides on human beings were studied in great

detail by Kaj Roholm, who reported in 1937 on the effects upon Danish workers of

inhaling and swallowing large quantities of dust from fluoride-rich cryolite

rock.(22) He discovered that fluoride intake and accumulation result in changes

in bone structure, detected in the early stages as an increase in the density of

bones to X rays. Such irreversible skeletal changes have now been studied in

great detail and are part of the well characterized condition known as " skeletal

fluorosis. "

 

Roholm also discovered many nonskeletal symptoms among the cryolite

workers, including gastrointestinal complaints, loss of appetite, shortness of

breath, localized rheumatic pains, and susceptibility to colds. It is hard to

distinguish which of the symptoms recorded by Roholm resulted from fluoride

exposure and which were due to other working conditions and the physical nature

of the inhaled dusts. Most American and Western European investigators now

maintain that the only effect of occupational fluoride intake is skeletal

fluorosis, which is harmful only in the advanced stages.

 

Investigators in certain other countries have reported both skeletal and

non-skeletal effects of industrial exposure to fluorides. A recent report from

the Soviet Union on the health of cryolite workers resembles Roholm's in that a

whole array of symptoms were found, including inflammation of the upper

respiratory passages, gastrointestinal disorders, and bone pain.(23). According

to one report, workers in a Japanese aluminum factory may have suffered lung

damage due to inhalation of fluorides.(24)

 

Few studies have been published on the effects of airborne fluorides on

the health of American workers. In one such study, workers exposed to fluorides

in a Tennessee Valley Authority (TVA) phosphate plant showed some signs of

skeletal fluorosis.(25) They also had significantly more respiratory disease

than their unexposed co-workers. Workers exposed to fluoride in Alcoa's

relatively " clean " Massena, New York, aluminum plant also had some increase in

the rate of upper respiratory infections, although the difference in this study

was not statistically significant.(26)

 

An increased rate of respiratory symptoms might be due to the highly

irritating-acid hydrogen fluoride gas in the air of the workplaces of these

factories. Neither of the published American studies have reported the large

array of nonskeletal effects described by Roholm in Denmark.

 

The fluoride-exposed workers at a TVA phosphate fertilizer plant had,

however, in addition to bone changes and respiratory symptoms, a higher rate of

kidney abnormalities, as shown by the excretion of albumin in the urine.(25)

People with skeletal fluorosis in India (27) and in Aden (28) also had

alterations in kidney function, indicated by urea clearance tests or by

excretion of albumin. While excretion of albumin is not always a sign of kidney

disease, it may indicate that high levels of fluoride exposure have the

potential to cause some kidney damage. A fluoride-exposed industrial worker,

especially if he has a preexisting kidney condition, may be in danger from

excessive fluoride ingestion.

 

A firm determination of the potential for low and moderate levels of

airborne fluorides to effect the respiratory, gastrointestinal, and other

non-skeletal systems is very important. American industries, such as steel and

aluminum manufacturers and phosphate processors, in which workers are subjected

to varying doses of fluorides, have accumulated a great deal of information on

the health of these workers. Only one American company, Alcoa, has chosen to

release any of this information to the public.(26) If more of these industrial

studies were published in the open literature, the relationship between airborne

fluorides and various skeletal and nonskeletal conditions could be better

evaluated.

 

The American Conference of Governmental Industrial Hygienists has set a

" threshold limit value " of 3 parts per million (ppm) for hydrogen fluoride gas

in industrial workplaces.(29) The threshold limit value is supposed to be the

concentration of gas that nearly all workers can inhale for eight hours a day,

five days a week, with no adverse effects. The threshold limit value for

fluoride-containing dusts is 2.5 milligrams fluoride per cubic meter, which is

very close to the threshold limit value for hydrogen fluoride gas, with regard

to fluoride concentration.

 

These threshold limit values appear to be set to protect employers from

costly compensation suits rather than to ensure that the exposed workers have

real health protection. For example, 2.5 milligrams fluoride per cubic meter

could easily induce detectable, irreversible skeletal changes in workers. Drs.

H. C. Hodge and F. A Smith of the University of Rochester state that daily

fluoride intake should be kept below 5 to 8 milligrams per day to avoid the

possibility of increased X-ray density of bones.(30) Thus at the accepted limit

of 2.5 milligrams fluoride per cubic meter, in eight hours a man might inhale

eight to ten cubic meters of air containing a total of 20 to 25 milligrams of

fluoride. Hodge and Smith justify the existing standard by assuming that a man's

lungs will only absorb 25 percent of the fluoride inhaled. There is, however, no

evidence to support this low estimated absorption value. The absorption of

gaseous hydrogen fluoride has been reported to be close to 100 percent, (31) and

solid fluorides can be absorbed with about the same high efficiency as gaseous

fluorides. (32) Thus, to ensure that daily intake is kept below 7 or 8

milligrams per day, the air concentration would have to average below about 0.8

milligram per cubic meter, not just below the 2.S milligrams now accepted.

 

Calculating Total Intake

 

The calculation of Hodge and Smith given above corresponds to a situation

in which either particulate fluoride or hydrogen fluoride gas are present at the

accepted threshold limit value concentration. If both are present

simultaneously, then the amount of fluoride intake would be approximately

doubled. Furthermore, the gas silicon tetrafluoride (SiF4), a major airborne

form of fluoride in industry, is not taken into account by any occupational

health standards. It too can contribute to total fluoride intake in factories.

Thus, the threshold limit value for fluorides should not be restricted to

particulates alone but should include all airborne forms of fluoride

simultaneously.

 

We have still, however, neglected the fact that people ingest fluoride

from many sources, including food and water. If the drinking water used by a

worker is artificially fluoridated, his daily fluoride intake from food and

water alone could easily exceed 3 or even 4 milligrams per day, especially if

his job were physically demanding, resulting in high fluid consumption. In a

region with naturally high-fluoride water, his intake might be still higher. If

he eats vegetables that are grown in the vicinity of the industry, he may

increase his fluoride intake even more, since local vegetation is likely to have

been subjected to fluoride air pollution. High-fluoride dusts which settle on

food eaten inside the factory can also be a significant source of ingested

fluoride. (33)

 

It has been claimed by some that fluoride-induced, irreversible structural

changes in bone which result in increased density to X-rays may weaken the bone,

make it more brittle, or help induce or aggravate such conditions as

osteoarthritis. In the absence of good experimental data concerning the

relationships between bone fluoride content, mechanical properties, and

osteoarthritis, it is only prudent to conclude that industrial workers should

not be subjected to fluoride levels that result in detectable increases in bone

density to X rays.

 

In order to ensure, with a small margin of safety, that the bones of the

workers will not undergo detectable fluoride-induced changes, fluoride intake

from the air at the workplace would have to be below 2 milligrams per day. The

air itself thus would have to average below about 0.25 milligram (2SO

micrograms) per cubic meter in total fluoride. This is equal to one-tenth of the

currently accepted industrial standard for particulate fluorides alone.

 

In addition to its contribution to total fluoride intake, hydrogen

fluoride has other effects. The accepted threshold limit value of 3 PPM for

hydrogen fluoride gas is supposed to protect workers from damage to lungs, eyes,

and other sensitive tissue. When hydrogen fluoride comes in contact with water

(as on the surface of moist tissue) it forms an extremely strong and reactive

acid called hydrofluoric acid. In an experiment in the Soviet Union, hydrogen

fluoride concentrations as low as 0.036 PPM caused the subjects' eyes to become

more sensitive to light.(34) This concentration is less than one-eightieth of

the accepted threshold limit value supposed to protect the health of

fluoride-exposed workers in the US

 

In other experiments, performed in the U. S.,(13) gaseous hydrogen

fluoride concentrations averaging 3.5 PPM caused irritation and peeling of the

skin as well as nose, and eye irritation. These experiments involved exposure

for six hours a day and lasted only a few weeks. Workmen exposed to similar

concentrations for eight or more hours a day over many years might be expected

to suffer far more serious damage. But the accepted threshold limit value for

hydrogen fluoride (3 PPM) is very close to the average concentrations (3.5 PPM)

which caused these symptoms in a very short-term experiment.

 

Industrial fluoride pollution has been reported to have effects on the

health of people living near polluting industries. Early in December 1930,

thousands of people became sick and 60 died when a heavy mist settled into the

Meuse Valley in Belgium. The official investigation of the incident concluded

that sulfur dioxide and sulfuric acid mists were probably chiefly responsible

for 3 the effects, Others, including Roholm, (35) believed that fluorides were

the real culprits. A similar dispute over the possible role of fluorides grew

out of the deaths of 20 people in Donora and Webster, Pennsylvania, during an

air pollution episode in 1948.(36) Since no reliable measurements were made of

the pollutant concentrations in either case, it is certainly impossible now to

make any firm judgments, but the possibility that hydrogen fluoride mists

contributed to the acute respiratory distress which resulted in the deaths

certainly cannot be ruled out. Fatalities from high-level, acute hydrogen

fluoride exposures have certainly taken place in industry.(33)

 

The question of possible effects of chronic exposure is, however, more

relevant to the levels of fluorides usually found in the air surrounding

polluting industries. Here, again, the available information is not conclusive

in implicating fluorides, since fluorides are often accompanied by other

airborne pollutants. For example, an aluminum smelter in Bratislava,

Czechoslovakia, and aluminum and phosphate manufacturers in the Soviet Union

emit large quantities of fluorides into the air. Pollution from these industries

have been implicated in high rates of bronchitis, pneumonia, tuberculosis, and

other upper respiratory infections in the surrounding areas.(37) The other air

pollutants, including sulfur dioxide, " tar products, " and particulates released

by these plants, make it impossible to attribute the health effects observed to

fluorides alone. The possible role of hydrogen fluoride certainly cannot,

however, be discounted completely.

 

Of the many claims of damage to health from fluoride air pollution which

have been made, only one has been upheld in US courts. In a highly controversial

decision in 1955, a family was awarded $38,823 for various health effects

attributed to emissions from the Reynolds Metals aluminum plant in Troutdale,

Oregon.(38) The merits of the case are still disputed by those familiar with it.

 

Most areas of the US do not have significant fluoride air pollution

problems. In a 1966-1967 national survey, over 7,700, 24-hour air samples taken

at numerous locations across the US were analyzed for total water soluble

fluorides. Ninety-seven percent of the nonurban and 87 percent of the urban

samples had less than 0.04 parts per billion (ppb) fluoride (the lower limit of

detection). Only 13 (0.2 percent) of the urban samples contained more than 0.8

ppb fluoride, the highest of these being 1.5 ppb. The highest concentration

found in a non-urban location was 0. 13 ppb.(39)

 

The fluoride concentration in the air in Bratislava, Czechoslovakia, which

contains an aluminum smelter as discussed above, often averages well over 100

ppb. By contrast, the airborne fluoride levels at the center of the most

concentrated cluster of fluoride-emitting industries in the US, the phosphate

processing plants of Polk County, Florida, rarely exceed 10 ppb and average less

than 2 ppb, (40) because these industries are strictly regulated by the state.

Residents of other states, with less vigorous enforcement programs, may be

subjected to higher fluoride levels, even though the emitting sources may be

much smaller. At the fluoride concentrations which exist in Polk County, it

would be quite impossible for a person to inhale enough air to result in a

fluoride intake of even 0.1 milligram per day. In contrast, for example,

artificial fluoridation of public water supplies results in an average total

fluoride intake of 2 to 5 milligrams per day.(41)

 

Outside the Factory

 

Those who live around fluoride-emitting industries inhale fluorides

directly and eat them in food contaminated by the polluted air. In terms of

quantity, the inhaled fluoride is usually far less than the total eaten

fluoride. For example, a person who ate one-half pound of heavily contaminated

food every day might add 1 milligram to his or her daily intake of fluoride. It

is improbable, however, that anyone would habitually consume this much highly

contaminated food over long periods of time, and thus it is unlikely that

fluoride contamination of food from industrial pollution would have a direct

adverse effect on the health of most people. In such cases, though, in which

people are exposed to fluoride at work or live in areas with excessively

fluoridated water, food contamination must be considered as part of total

environmental exposure, and then it might well be significant in terms of

health.

 

In one report, for example, fluoride emissions from a Soviet

superphosphate Plant were correlated with both dental fluorosis (mottling of

teeth) and a low rate of tooth decay among nearby children.(42) Other studies

have concluded that emissions from aluminum smelters in Kitakata, Japan, and

from a brickyard in Graz, Austria, resulted in increased fluoride levels in the

urine of local residents.(43) The fluoride emissions in Kitakata are also

reported to have slightly affected the rate of skeletal development of nearby

children.(44) It is probable that the high level of fluoride found in the

typical Japanese diet (in tea, rice, and seafood (45) would make the average

Japanese person more susceptible to adverse effects of increased fluoride intake

than the average American would be. But the fact that some Americans have very

atypical diets (for Americans) must be taken into account when the effects of

fluoride air pollution on human health are considered.

 

The concentration of airborne fluorides inside a polluting factory may be

on the order of 100 to 1,000 times that found outside the factory. The threshold

limit value for hydrogen fluoride in industrial situations has been set at 3 PPM

(3,000 ppb), though even this inadequate limit may be exceeded in real

industrial situations. By contrast, as mentioned before, the air fluoride levels

in many polluted areas of the US rarely exceed 10 ppb if emissions are

controlled.

 

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