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OCR for page 184
Fluorine
Fluanne (F), chemically bound as fluoride, is found in both igneous and
sedimentary rock add constitutes about 0.06 0.09 percent of the upper
layers of the earths crust. Fluorine rarely occurs free in nature but
combines chemically to form fluorides that are mdely, but variably,
distributed in the environment. An association between high-fluor~de
intakes and dental defects was first demonstrated in rats in 1925
(McCollum e' al., 192S). By 1931, chronic endemic fluorosis in man and
livestock was identified in several parts of the world (Churchill, 1931;
Srn1th et al., 1931; Velu, 1931~. F-luonde-beanng fumes and dusts from
industrial plants processing fluande-conta~n~ng raw matenals, such as
bauxite or phosphate rock, were found to constitute a health hazard to
man and animals living nearby (Roholm, 1937; Agate et al., 1949~. The
use of unprocessed rock phosphates as mineral supplements subjected
livestock to a further fluoride hazard. However, in the late 1930's it was
discovered that fluoride had significant anticarieogen~c properties, and
subsequent research has explored both the toxic and essential character
of this element. Excellent reviews are available (National Research
Council, 1971, 19741.
ESSENTIALITY
Whether fluorine is considered essential depends up-on the criteria
used. No one has yet produced an environment so low in this element
184
OCR for page 185
Fluorine
185
that animal survival has been vitally threatened. However, fluorine was
identified as a constant constituent of bones and teeth as early as lX05,
and trace quantities are beneficial in development of caries-resistance
and may be beneficial in inhibiting excessive dem~neralization of bone
in the aged.
McClendon and Gershon-Cohen (1953) fed weanling rats for 66 days
upon materials grown hydroponically in water said to be "fluorine-
free.'' The rats weighed 51 g and had 10 carious molars per animal
compared to fluoride-supplemented rats that weighed 128 g and had 0.5
canous molars per animal. No data on fluorine concentration in diets or
tissues were presented. Maurer and Day (1957) purified dietary in-
gredients and produced a diet that contained about 0.007 ppm fluoride
on which four generations of rats were raised without evidence of
impaired general health, dental health, or weight gain as compared to
rats raised on the same diet plus 2 ppm of fluoride in their drinking
water. Doberanz et al. (1963) fed a diet containing less than 0.005 ppm
fluoride (prepared from hydroponically grown soybeans and sorghum
grain) and found no difference in general health or growth rate between
rats fed this diet and rats fed the same diet plus 2 ppm of fluoride in their
drinking water. A similar study (Weber, 1966) failed to find that fluoride
was essential for mice raised through three generations. However,
Messer et al. (1972a, 1973) have reported that fertility is impaired in
female mice on a diet containing 0.1~.3 ppm fluoride, and anemia in
infant mice produced by low-fluor~de females is more severe than when
supplemental fluoride is provided (Messeret al., 1972b). Tao and Suttie
(1976) used the same low-fluande diet fed to mice by Messer et al.
(1973), found no impairment of reproduction, and suggested that the
apparent essentiality of fluoride proposed by Messer and associates
was due to a pharmacological effect of fluoride in improving iron utili-
zation in mice fed a diet marginally sufficient in iron. Schwarz and
MiIne (1972), working in a fiItered-air environment, reported a favor-
able growth response when small increments (1-2 ppm) of fluoride were
added to a low-fluonde diet for rats.
METABOLISM
Absorption of fluoride is presumed to be largely a passive process
(National Research Council, 1974), although some researchers
(Stookey et al., 1964; Parkins et al., 1966; Parkins, 1971) have
suggested active transport on the basis of in vitro studies with invested
rat intestine. Sites of absorption include the stomach in man (Carlson
OCR for page 186
OCR for page 187
Fluorine
187
ppm, respectively. F]uonde crosses the placental balkier of cows, and
fluoride levels in the bones of the offspring are correlated with the
fluoride concentration of maternal blood (National Research Council,
19741. However, bone fluoride concentrations of calves born to cows
consuming as much as 108 ppm fluoride (from sodium fluoride) were
low (Hobbs and Merriman, 1962), and it appeared that neither placental
fluoride transfer nor milk fluoride concentrations were sufficient to
adversely affect the health of these calves.
SOURCES
The primary fluorine-containing minerals are fluorspar (CaF2), cryolite
(Na~AlF6), and fluorapatite [CalOF2(PO4)6]. Natural deposits of cryo-
lite are currently of little economic importance, and cryolite for indus-
tr~al purposes is synthesized in chemical plants. F~luorspar and fluor-
apa?dte deposits are widespread, and a 500 square-mile area at Bartow,
Florida, contains deposits of phosphate rock that is chiefly fluorapatite.
This is a major center for the production of phosphate fertilizers and
calcium phosphates for animal feeds, although a number of other im-
portant phosphate deposits are found in the United States (U.S.
Department of the Interior, 19701.
Soils may contain fluoride in several different minerals. The fluoride
content tends to increase with depth, and the usual range in the United
States is 2~500 ppm (average, 190 ppm) from ~8 cm deep and 2~1,620
ppm (average, 292 ppm) from ~30 cm deep (Robinson and Edgington,
1946~. Some soils, unusually high in fluoride, have been found in Idaho
(3,870 ppm) and in Tennessee (8,300 ppm).
Surface water in lakes and rivers generally contains less fluoride than
water from springs or wells, unless that surface water is contaminated
by dust from mining and processing of high-fluorine phosphate rock.
The fluoride content of wed water vanes regionally, dependent on its
omega. Much of the northeastern United States has water with nature
fluoride concentrations ranging from 0.02 to 0.1 ppm. Farther west and
south, concentrations tend to be above 0.2 ppm, but seldom over 1
ppm. In endemic fluorosis areas, deep well water may percolate
through fluorapatite and frequently contains 3-5 ppm fluonde, and
sometimes 1~15 ppm (Harvey, 1952; Cholak, 1959~.
Active volcanoes and fumaroles, and certain industrial processes,
may contribute significantly to local concentrations of fluoride. The
latter furnish fluoride in one of three principal forms: hydrofluoric acid,
silicon tetrafluoride, or fluende-contain~ng particulate matter. Direct
OCR for page 188
188 MINERAL TOLERANCE OF DOMESTIC ANIMALS
inhalation of fluoride does not contribute significantly to fluoride accu-
mulation in animals. However, these emissions may contaminate
plants, soil, and water. Gaseous fluoride may be absorbed and income
rated into plant tissues. Particulate fluorides may accumulate on plant
surfaces and be ingested as the plants are eaten. Rain may wash off
some of the particles, and the particles are usually quite inert, with
toxicity related largely to solubility.
Forages and grains are seldom a major factor in chronic fluorosis in
animals or man, unless contaminated by fluor~de-beanng- dusts, fumes,
or water. Most plants have a limited capacity to absorb fluoride from
the soil. The tea plant and camellia are exceptions, and fluoride concen-
trations of 100 ppm or more have been reported (Underwood, 1977~.
Pasture plants have been shown to range from 2 to 16 ppm on a dry
basis. Cereals and cereal by-products usually contain 1-3 ppm.
Animal by-products containing bone may contribute significant
quantities of fluoride to animal diets, depending upon the amount of
by-product used (and bone contained) and the dietary history of the
animals from which the by-products were derived. Bone ash normally
contains less than 1,500 ppm of fluoride and would contribute only
minor amounts. However, cattle grazing fluoride-contaminated pas-
tures can have bone ash containing over 10,000 ppm fluoride, or 5.5
parts of fluoride for each 100 parts of phosphorus.
Normally, the primary sources of dietary fluorides are the phos-
phorus supplements. These vary greatly in fluoride content, depending
on origin and manufacturing processes. The majority of U.S. feed phos-
phates originate from rock phosphate deposits with fluoride levels of
2-5 percent (average, 3.5 percent) (VanWazer, 1961~. When processed
sufficiently to qualify as defluonnated, feed-grade phosphates must
contain no more than 1 part of fluorine to 100 parts phosphorus (AAFCO,
19771. Processed low-fluoride, feed phosphates include mono-, di-, and
tricalcium phosphates, mono- and diammonium phosphates, mono- and
disodium phosphates, ammonium and sodium polyphosphates, feed-
grade phosphoric acid, and defluorinated phosphate. Unprocessed feed
phosphates, supplying substantial amounts of fluorine, include soft
rock phosphate, ground rock phosphate, and ground low-fluoride rock
phosphate. More dangerous sources of fluoride, when incorporated
in animal diets, are undefluorinated, fertilizer-grade phosphates.
Analyses of the above phosphates are presented in Table 17.
OCR for page 189
Fluorine
TOXICOSIS
LOW LEVELS
189
The precise dietary concentration at which fluoride ingestion becomes
hannfill is difficult to define. No single value Is appropriate because
low-level toxicosis depends upon duration of ingestion, solubility of the
fluoride source, general nutritional status, species of animal, age when
ingested, and toxicity-modifying components of the diet.
Diagnosis of fluoride toxicosis is also difficult, because there may be
an extended interval of time between ingestion of elevated levels and
the appearance of toxic signs (Shupe, 1970~. Dietary history, clinical
evidence, radiography, chemical analyses, necropsy findings, and
histopathology are all important. The degree of dental fluorosis and
osteofluorosis, evidence of intermittent lameness, and the concen-
tration of fluoride in diet, urine, and bone are of particular diagnostic
importance.
If excessive fluoride is ingested during tooth development, fluorotic
lesions may be expected (Roholm, 1937~. The period during which
developing teeth in cattle are sensitive to excess fluoride is from
approximately 6 months to 3 years of age. Teeth that have erupted are
not influenced adversely by subsequent fluoride ingestion (Garlick,
1955), and cattle that are more than 3 years old will not develop typical
dental lesions. Dental fluorosis is usually diagnosed by examining the
· —
Incisors.
The degree of dental fluorosis that develops under experimental con-
ditions has been correlated with the amount and duration of fluoride
ingestion and the animal's age. Gross fluorotic lesions of the incisor
enamel begin with slight mottling (white, chalky patches or striations)
aIld progress to definite mottling, hypoplasia, and hypocalcif~cation.
The following scoring system for classification of dental fluorosis has
been proposed (National Research Council, 1974~:
Score
Description
o
Normal. Smooth, translucent, glossy white enamel; tooth has nor-
mal shape.
Questionable Effect. Slight deviation from normal but cause not
determinable; may have enamel flecks but is not mottled.
Slight Effect. Slight mottling of enamel, best observed as horizontal
striations with transmitted light; may be slightly stained but no
increase in normal rate of wear.
OCR for page 190
190 MINERAL TOLERANCE OF DOMESTIC ANIMALS
Score Descnption
4
Moderate Effect. Definite mottling; large areas of chalky enamel
or generalized mottling of entire tooth; tooth may have slightly
increased rate of wear and may be stained.
Marked Elect. Definite mottling, hypoplasia, and hyppcalcifica-
tion; may have pitting of enamel; with use, tooth will have increased
rate of wear and may be stained.
Severe Effect. Definite mottling, hypoplasia, and hypocalcification;
with use, tooth will have excessive rate of wear, and may have
eroded or pitted enamel. Tooth may be stained or discolored.
The amount of fluoride stored in bone may increase over time with
no apparent change in bone structure or function. However, if excess
fluoride ingestion is sufficiently high, and over a sufficiently long period
of time, morphological abnormalities will develop. In livestock, clini-
cally palpable (bilateral) lesions usually develop first on the medial
surface of the proximal third of the metatarsals. Subsequent lesions are
seen on the mandible, metaca~pals, and ribs. The osteofluorotic
lesions tend to be more severe in those bones, and parts of bones, that
are subject to the greatest physical stress. Radiographic evidence of
osteoporosis, osteosclerosis, osteomalacia, hyperostosis, and osteo-
phytosis, or any combination of these lesions, has been described
(Johnson, 1965; Shupe and Alther, 1966; Shupe, 1969~. Grossly,
severely affected bones appear chalky white, are larger in diameter and
heavier than normal, and have a roughened, irregular periosteal sur-
face. In cattle poisoned by industrial fluoride emissions, Krook and
Maylin (1979) contended that the primary target of fluoride was the
resorbing osteocyte. Morphological signs of osteolysis were absent,
and the failure of resorption caused osteopetrosis with retention of
lamellar bone in the cortices.
Animal movement may be impaired by intermittent periods of stiff-
ness and lameness, associated in advanced cases with calcification of
periarticular structures and tendon insertions. In animals with marked
periosteal hyperostosis, spurring and bridging of the joints may lead to
rigidity of the spine and limbs.
Anorexia, unthriftiness, dry hair, and thick, nonpliable skin have
been noted in fluorotic animals (Roholm, 1937; Shupe et al., 1963a).
Primary adverse effects on reproduction and lactogenesis have not
been demonstrated, although milk production may decrease on high-
fluoride intakes secondary to dental and skeletal damage and conse-
quent reductions in feed and water intake (Stoddard et al., 19631. Suttie
OCR for page 191
Fluorine . 191
et al. (1957b) have demonstrated that cows first exposed to fluoride at
4 months of age can consume 40 50 ppm of fluoride in their diet for two
or three lactations without measurable effect on milk production. Milk
production was reduced in the fourth and subsequent lactations. Higher
dietary fluoride levels (93 ppm) affected milk production In the second
lactation slightly and definitely reduced milk yield in subsequent lacta-
tions (Stoddard et al., 19631. Irrespective of level or duration of fluoride
intake, clinical signs of toxicosis will normally precede impaired milk
production. No characteristic, unequivocal histologic or functional
changes in blood or soft tissues have been correlated with fluoride
intakes sufficient to induce chronic fluorosis of bones and teeth.
HIGH LEVELS
Acute fluoride toxicosis is relatively rare and has usually resulted from
accidental ingestion of compounds such as sodium fluosilicate, used as
a rodenticide, or sodium fluoride, used as an ascaricide in swine. The
rapidity with which toxic signs appear depends on the amount of
fluoride ingested (Cass, 19611. Toxic signs include high-fluoride content
of blood and urine, restlessness, stiffness, anorexia, reduced milk
production, excessive salivation, nausea, vomiting, urinary and fecal
incontinence, clonic convulsions, necrosis of gastrointestinal mucosa,
weakness, severe depression, and cardiac failure. Death sometimes
occurs within 12-14 hours (Krug, 1927~.
FACTORS INFLUENCING TOXICITY
The seventy of fluoride toxicosis is influenced by the form in which the
fluoride occurs, the nutritional status of animals consuming the fluoride
source, variations in fluande intake, and the presence of other dietary
components.
In genera, the toxicity of fluoride compounds that are most water-
soluble is greater than that of compounds with lesser water solubility.
Based on skeletal storage of fluoride by rats, Hobbs et al. (1954) con-
cluded that the toxicity of fluande compounds could be ranked in order
from high to low as follows: potassium and sodium fluosilicate, po-
tassium and sodium fluoride, rock phosphate, natural and synthetic
cryolite, calcium and magnesium fluosilicates, and calcium fluoride.
Hobbs and Memman (1962) found that fluoride in rock phosphate was
considerably less toxic to beef heifers than that in sodium fluoride.
Ammerman et al. (1964) observed that fluoride storage in the bones of
steers was least from calcium fluoride, intermediate from soft phos-
OCR for page 192
OCR for page 193
Fluorine 193
findings have been reported by Greenwood et al. (1964) and AUcroft et
al. (196S). Free choice accessed aluminum sulfate in a muneral mixture
offered to cattle gazing. a fluor'&e-coneaminated pasture was not.e~ec-
tive in reducing bone fluoride deposition, perhaps because continuous
intake of aluminum sulfate was inadequate (Merr~man and Hobbs,
19621. It has been shown that aluminum compounds may adversely
affect dietary phosphorus retention (Street, 1942; Hobbs et; at., 1954;
Alsmeyer et at., 1963; Storer and Nelson, 1968), and if they are used
to alleviate fluonde toxicosis, increased levels of phosphorus may have
to be fed. Aluminum chIonde and aluminum acetate also appear to be
effective in reducing fluorosis, but aluminum oxide produces Only slight
alleviation (Sharpless, 1936; Hobbs et al., 1954~. It should be noted,
however, that the effectiveness of soluble aluminum salts may be
dependent on feeding these compounds simultaneously with fluonde
ingestion. Dietary aluminum compounds were ineffective in promoting
depletion of fluonde previously deposited in the skeleton of the rat.
TISSUE LEVELS
Plasma fluonde concentrations are maintained within narrow limits by
regulatory mechanisms involving skeletal and renal tissues. Elevated
intakes of fluoride u ill result in increased concentrations of fluonde in
both urine and bone.
Unne fluande levels are roughly correlated with dietary intake,
although the duration of fluonde ingestion, sampling time, and total
urinary output will introduce vanation. Expression of urinary fluoride
concentration on a common specific gravity basis will somewhat reduce
the effect of variation in total urinary output. Shupe et al. (1963a) have
suggested that relating fluonde to creations levels in the urine may
even be more helpful. These workers found that by determining the
concentration of fluoride in the urine and by combining this information
with knowledge of the length of time fluoride had been ingested, the
concentration of fluonde in ingested tiry matter-could be estimated.
However, urinary fluonde concentration alone was an inadequate cr'-
tenon for a definitive diagnosis of fluorosis in cattle.
In several long-term experiments with beef and dairy cattle, the
skeletal retention of fluoride was approximately proportional to the
concentration of fluoride (from sodium fluoride) in the diet. In these
studies, relatively constant dietary fluonde concentrations were fed
throughout the entire experimental period. When dietary fluonde
concentrations vary widely over a study period, skeletal fluoride con-
OCR for page 194
194 MINERAL TOLERANCE OF DOMESTIC ANIMALS
centration may relate well to total fluoride intake, but correlations with
dietary fluoride concentrations at a single time may be poor (Suttie en
al., 1972~. In either case, there Will be a decreasing rate of skeletal
fluoride uptake with time (Shupe e' al., 1963b). Skeletal fluoride con-
centrations may be determined in the living animal by obtaining bi-
opsies of ribs or coccygeal vertebrae (Burns and Allcroft, 1962;
Purvance and Transtrum, 1967~. Cancellous bones such as the frontal,
ribs, vertebrae, and ilium have a higher fluoride concentration than the
more compact metacarpals and metatarsals (Suttie and Phillips, 1959;
Shupe et al., 1963b), although correlations may be established between
the fluoride levels in these different types of bone (Suttie, 19671. The
diaphyseal portion of the metaca~pals and metatarsals has a lower
fluoride concentration than the metaphyseal portion (Shupe et al.,
1963a; Ammerman et at., 1964~.
MAXIMUM TOLERABLE LEVELS
The following recommended maximum tolerable levels take into con-
sideration the adverse biological and economic ejects of excessive
intakes of fluonde, plus the practical reality that many useful phos-
phorus supplements for livestock contain significant concentrations of
fluoride. While small intakes of fluoride may be beneficial, or even
essential, prolonged intakes of dry diet fluoride concentrations above
these maximum tolerable levels may result in reduced performance.
These levels are based on tolerances to sodium fluoride or other fluo-
r'&es of similar toxicity (fluonde in certain phosphorus sources appears
to be less toxic) and assume that the diet is essentially the sole source
of fluoride. When water also contains appreciable fluoride (3 ppm or
more), these dietary levels should be proportionately reduced.
Excessive exposure during tooth development in cattle may result in
exaggerated tooth wear, impaired mastication, and sensitivity to cold
drinking water. Thus, maximum levels for young cattle are set at 40
ppm. Minor morphological lesions may be seen in cattle teeth when
dietary fluoride during tooth development exceeds 20 ppm, but a re-
lationship between these lesions and animal performance has not been
established. Mature dairy cattle tend to consume more feed in relation
to body weight than mature beef cattle, so maximum dietary fluoride
levels are set at 40 ppm for the former and at 50 ppm for the latter.
Lifetime fluoride exposure for finishing cattle is less than for breeding
cattle, so the maximum tolerable level for this productive class is set at
100 ppm. Maximum tolerable levels for other species are based on
OCR for page 216
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Fluorine
REFERENCES
221
Agate, J. N., G. H. Bell, G. F. Boddie, R. G. Bowler, M. Buckell, E. A. Cheeseman, T.
H. Douglas, H. A. Druett, J. Garrad, J. Hunter, K. Perry, J. D. Richardson, and J. B.
Weir. 1949. Med. Res. Counc. (Gr. Brit.) Memo. No. 22.
Allcroft, R., K. N. Burns, and C. N. Hebert. 1965. Fluorosis in cattle. II. Development
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Alsmeyer, W. L., B. G. Harmon, D. E. Becker, A. H. Jensen, and H. W. Norton. 1963.
Effects of dietary Al and Fe in phosphorus utilization. J. Anim. Sci. 22:11 16.
Ammerman, C. B., L. R. Arrington, R. L. Shirley, and G. K. Davis. 1964. Comparative
effects of fluorine from soft phosphate, calcium fluoride and sodium fluoride on steers.
J. Anim. Sci. 23:409.
Anderson, J. O., J. S. Hurst, D. C. Strong, H. M. Nielsen, D. A. Greenwood, W.
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Armstrong, W. D., and L. Singer. 1970. Distribution in body fluids and soft tissues, pp.
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Association of American Feed Control Officials (AFRO). 1977. Official Publication of He
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Boddie, G. F. 1957. Fluorine alleviators. II. Trials involving rats. Vet. Rec. 69:483.
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Bunce, G. E., Y. Chiemchaisri, and P. H. Phillips. 19~62. The mineral requirements of the
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ficiency syndrome. J. Nutr. 76:23.
Burns, K. N., and R. Allcroft. 1962. The use of tail bone biopsy for studying skeletal
deposition of fluorine in cattle. Res. Vet. Sci. 3:215.
Carlson, C. H., W. D. Armstrong, and L. Singer. 1960a. Distribution and excretion of
radiofluoride in the human. Proc. Soc. Exp. Biol. Med. 104:20S.
Carlson, C. H., W. D. Armstrong, L. Singer, and L. B. Hinshaw. 1960b. Renal excretion
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226 MINERAL TOLERANCE OF DOMESllC ANIMALS
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@
Representative terms from entire chapter:
milk production
