Monitoring fluoride pollution in Flathead National Forest and Glacier National Park

Historic, Archive Document

Do not assume content reflects current
scientific knowledge, policies, or practices.

««w

MONITORING FLUORIDE

in Flathead NaXuntaCfWiT and
Glacier National Park

FEB 24 1973

POLLUTICR'"*

AD-33 Bookplate
(i-*3)

NATIONAL

LIBRARY

The Anaconda Aluminum Company reduction works at Columbia Falls,
Montana, is shown in the top photo. Note fluoride-killed trees
in foreground. The lower-left photo shows top dieback and
brooming in a Douglas-fir caused by fluorides from the Anaconda
Company plant. Biologist Don Berg is sampling forest vegetation
for fluoride analyses in the lower-right photo.

$fS/0

J10NIT0RING .-FLUORIDE -POLLUTION
^IN JXATHEAD NATIONAL FOREST

and glacier Rational park

>- by

Clinton E. Carlson-^

1/

SUMMARY

During August 1971, we conducted a study to monitor fluoride
pollution in Flathead National Forest and Glacier National Park,
near Columbia Falls, Montana. The study was done as a followup to
our 1970 fluoride study (Carlson and Dewey 1971) of pollution caused
by fluoride emissions from the Anaconda Aluminum Company at Columbia
Falls. During the 1970 study fluoride emissions by the company were
reduced from 7,500 to 2,500 pounds per day.

Fifteen plots, 20 percent of the 77 permanent radial plots established
in 1970, were resampled in 1971. Chemical analysis of vegetation
indicated average plot fluoride concentration was from 4 percent less
in Glacier National Park to 77 percent less close to the aluminum
plant when compared to 1970 data. Injury indexes dropped an average
of 45.8 percent.

Analysis of conifer, shrub, and forb stem tissues indicated fluorides
are accumulated by stem tissue. However, the exact location of
accumulation was not determined.

Isopols, illustrated in the 1970 study, were recomputed based on the
1971 monitoring data. The total area polluted was 59 square miles
(34,560 acres) less than in 1970, and injury was found on 84 square
miles (53,920 acres) less than in 1970.

Analysis of insect tissue in 1971 indicated insects are still
accumulating excessive fluorides. Even though the Anaconda Company
reduced fluoride emissions at the aluminum plant in 1970, above¬
normal fluorides are still accumulating in vegetation up to 12 miles
distant in Glacier National Park. This represents an area of 179,200
acres. Fluoride injury to vegetation was found on 15,200 acres,
indicating the fluoride pollution problem at Columbia Falls has not
been alleviated.

1/ Plant pathologist, U.S. Forest Service, Missoula, Montana.

INTRODUCTION

During 1970 the U.S. Forest Service intensively studied fluoride
pollution in and adjacent to Flathead National Forest, near
Columbia Falls, Montana (Carlson and Dewey 1971). Abnormally high
concentrations of fluorides were found in vegetation on 214,000
acres of public and private lands. The Anaconda Aluminum Company
at Columbia Falls was found to be the source of the airborne
fluorides. Visible fluoride injury to plants, including tree
mortality, branch dieback of trees and shrubs, and chlorosis and
necrosis of foliage, was found on 69,120 acres.

Insects, including pollinators, foliage feeders, and predators,
had abnormally high quantities of fluorides.

The Environmental Protection Agency (EPA) also studied fluorides
in 1970 at Columbia Falls (personal communication; report not
yet published) . Their extensive meteorological data confirmed
the Forest Service data on fluoride distribution in the area.

EPA also found considerable fluoride- induced injury to indigenous
vegetation throughout the area.

Dr. Clarence Gordon, University of Montana, contracted by EPA to
study fluorides in Glacier National Park in 1970, found basically
the same distribution of fluorides as did the Forest Service
(Gordon 1972). Also, he found fluoride-caused injury to vegetation
over the same area. Gordon’s studies included fauna of the area;
he correlated high fluoride concentrations in animal teeth and
bones with the high fluorides in plant tissue.

Concurrent with these three independent studies, the Anaconda
Company began reducing fluoride emissions at the aluminum plant.
Early in 1970 the plant was emitting 7,500 pounds of fluorides
per day; by September emissions had been reduced to 5,000 pounds
per day; and by summer of 1971, emissions were down to 2,500
pounds per day. U The reductions were attained by installing
Venturi scrubbers and limiting aluminum production.

Reductions in fluoride emissions implied that subsequent accumula¬
tions of fluorides by vegetation may have been reduced, and that
resultant injury may also have been lessened. Therefore, we felt
it necessary in 1971 to monitor for possible continuing accumula¬
tion and effects of fluorides on vegetation as a followup to the
1970 study. Specifically the objectives of this study were:

2 J Reported by Anaconda Aluminum Company in various issues
of Hungry Horse News, Columbia Falls, Montana, from 1970 to 1971.

-2-

1. Determine current fluoride concentrations in vegetation
in the 1970 study area.

2. Determine current vegetational injury attributable to
fluorides .

3. Evaluate current fluoride concentrations in insects.
MATERIALS AND METHODS

Selection of Study Plots

Fifteen of the 77 study plots established in 1970 were selected

: evaluation.

They were:

R2-P21/

R5-P4

R5-P6

R3-P3

R5-P5

R8-P5

R3-P4

R6-P3

Columbia Mountain

R4-P2

R6-P4

special plot
R4-P6

R5-P3

R7-P3

R5-P9

Control data was obtained by sampling control plot No. 3.

The plots were arbitrarily selected on the basis of 1970 fluoride
distribution in the area. We believed it would be desirable to
sample plots on the west face of Teakettle Mountain where
fluorides were high, plots on the east side where fluorides were
moderate, and plots in Glacier National Park where fluorides were
low. The 15 plots listed above satisfied these conditions.

Collection of Vegetation

All collections were made in late August of 1971 to correspond
with the second sampling of 1970. Two pounds of foliage were
collected from each of two conifer species, one or two shrub
species, one forb, and one grass species on each plot. Conifer
branches were cut to include 3 years’ foliage from each tree
sampled. Tree species were not held constant from plot to plot.
Basically, species were the same as those collected in 1970. Each
sample was placed in a clean plastic bag and brought to the
Forest Service laboratory in Missoula for observation and analysis.

3/ R * radius; P = plot.

-3-

Laboratory Analysis

Specific ion chemical analysis

We were in need of a simple, fast, accurate, and relatively cheap
method of fluoride analysis for our work. The cost of contracting
analyses to WARF—' was prohibitive in 1971. Also, studies at
Boyce Thompson Institute (Jacobson and McCune 1969), indicated
the colorimetric method used by WARF produced highly variable
results between different laboratories. The specific ion method
(Durst 1969) showed promise of meeting our criteria. Therefore,
we used a Beckman research potentiometer and Orion fluoride and
reference electrodes to do the chemical analyses.

To test the method, we obtained 110 samples analyzed by WARF in
1970 for available fluoride. These samples were analyzed with
our specific ion equipment.

We also exchanged a small number of samples with Dr. Clarence
Gordon. Mr. Phil Tourangeau, Dr. Gordon's laboratory director,
analyzed these samples on an Orion specific ion apparatus.

During our analyses, we checked repeatability of the method by
twice analyzing 56 of the samples collected in 1971.

Foliar analysis

Conifer foliage was sorted by year of origin: 1969, 1970, or 1971.
Injury index (I. I.), an estimate of the proportion of tissue
thought killed by fluorides for foliage of a given year, was
measured separately for each year's foliage (Carlson and Dewey
1971). Foliage of each year was then dried, ground, and analyzed
chemically for available^/ fluoride. The method is outlined in
Appendix I.

Current (1971) foliage of shrubs, herbs, and grasses was chemically
analyzed for available fluoride, but injury index was not measured.

4/ Wisconsin Alumni Research Foundation, Madison, Wisconsin.

5/ All samples collected in 1971 were chemically analyzed in
the Forest Service laboratory in Missoula, Montana, using the
specific ion method. Samples were not washed; thus fluoride deter¬
minations reflected particulate and gaseous states, or "available"
fluoride.

-4-

Stem analysis

Because analyses of bark beetles in 1970 indicated fluorides
may be translocated in the woody tissue of trees, we decided
to analyze stem tissue in 1971. Conifer, shrub, and forb stems
were sorted by year of wood — 1969, 1970, and 1971 — and chemically
analyzed for available fluoride.

Histological analysis

Needles from 30 different conifer samples showing visible
fluoride necrosis were prepared for histological analysis and
examined as in the 1970 study (Carlson and Dewey 1971) .

Collection and Analysis of Insects

Nine insect samples, all from within one-half mile of the aluminum
plant, were collected in mid-August 1971. There were pollinators,
including mixed Hymenoptera, wood nymph butterflies ( Ceroyonis sp.),
skipper butterflies ( Evynnis sp.), and mixed Syrphildae; predators,
including robberflies (mixed Asilidae) and dragonflies (mixed
Anisoptera) ; and foliage feeders, including Arctridae larvae and
Notodontidae larvae. Each was chemically analyzed, unwashed, for
available fluoride using the same procedure as used for vegetation.
At least 5 grams fresh weight were required for each species. If
less than 5 grams was collected, the sample was combined with
another sample from the same family.

RESULTS AND DISCUSSION

Specific ion method

Comparative analysis of our results to those of WARF is detailed
in Appendix II. Linear regression analysis of the paired data
gave a correlation coefficient of 0.98. Slope of the regression
line was significant at the 99 percent level. This showed our
method gave results comparable to those found by WARF in 1970.
Samples checked by the University of Montana were also in close
agreement with our determinations.

Data on repeatability is given in Appendix III. The average
difference was 5.31 p.p.m. + 1.99 p.p.m. at the 95 percent level.
Again, this variation was well within the limits we were willing
to accept. Thus, we accepted the specific ion method as a reliable
way to determine fluoride concentration in biological material.

This indicated results obtained in 1971 by the specific ion method
could be directly comparable to those of 1970.

-5-

Foliar analyses

Results of foliar analyses are listed in Appendix IV. The table
is designed to compare 1971 data to 1970 data and, for the plots
sampled in 1971, includes:

1. 1970 second sampling: average fluoride value and injury
indexes by vegetation class.

2. 1971 average fluoride values and injury indexes. (Grand
average here does not include 3-year-old tissue.)

3.

between

Difference (+ or -) in fluoride concentration and I. I.
1970 and 1971 data, using 1970 as base year.

4. Percent difference of (3).

5. One-year change, from 1970 to 1971, in average fluoride
concentration for conifer tissue originating in 1969 and 1970.

6. Total 1970 values, total 1971 values, total differences,
average differences, and average percent difference, using 1970 as
base year. These are averages of average plot values.

Control data

Control vegetation had basically the same amount of fluoride as in
1970. Only the herbaceous plants, at 11.2 p.p.m., exceeded the
1970 established control concentration of 10 p.p.m. The grand
average was 8.91 p.p.m., up 0.57 p.p.m. from 1970. Therefore, we
accepted 10 p.p.m. as the normal background or control level of
fluoride in foliar tissue.

Needles of 1969 origin increased 2.44 p.p.m. from 1970 to 1971.
Needles of 1970 origin increased 3.28 p.p.m.

Injury index remained the same at 0.0. The conservative value of
0.006 is still accepted as control I. I.

Radial data

Vegetation from all plots sampled in 1971 contained above-normal
fluoride condentrations . A maximum of 24 times the normal comple¬
ment of fluoride was found at R4-P2 and a minimum of 1.6 times the
control value was found at R4-P6 in Glacier National Park.

Injury index ranged from 21 times control at R3-P3 near the aluminum
plant to control levels in Glacier Park. The data indicates visible
fluoride injury to vegetation occurred up to 6 air miles from the
aluminum plant in 1971.

-6-

We felt the most important way to look at the data was to
evaluate the change in fluoride accumulation and I. I. from

1970 to 1971. This was done by comparing current and 1-year-
old conifer tissue and current shrub, forb, and grass tissue
collected in 1971 with the same types and ages of tissue col¬
lected in the same plots in 1970. By averaging all plots by
vegetational type, we found:

1. Average fluoride in 1971 shrubs was 95.1 p.p.m. lower,
down 45.6 percent from 1970.

2. Average fluoride in 1-year-old conifer needles was

63.3 p.p.m. lower, down 45.1 percent from 1970.

3. Average fluoride in current conifer needles was 10.1
p.p.m. lower, down 28.6 percent from 1970.

4. Average fluoride in current herbaceous foliage was

59.4 p.p.m. lower, down 41.5 percent from 1970.

5. Average fluoride in current grass foliage was 46.8
p.p.m. lower, down 38.7 percent from 1970.

Considering all data, not stratifying by vegetational type or
plot, the average fluoride in 1971 was down 76.1 p.p.m. (49.3
percent) from 1970. Injury index dropped 0.036 (45.8 percent)
from 1970.

We also looked at the 1-year change in fluoride concentration
of conifer needles. A 1969 needle sampled in 1970 had a given
amount of fluoride; how much additional fluoride did that needle
accumulate from 1970 to 1971? Obviously it was not possible to
sample the same needle because of the destructive nature of the
sampling. Therefore, in 1971 we compared different needles but
from the same tree sampled in 1970.

Overall, the data indicates that needles originating in 1969
accumulated, on the average, an additional 3.01 p.p.m. fluoride;
while those originating in 1970 accumulated an additional 41.53
p.p.m. This is compared with control data which showed 1969
needles increased 2.44 p.p.m. and 1970 needles 3.28 p.p.m.

Stem analyses

Results of stem analyses are in Appendix V.

Control data. — The range in control tissue was 5.8 p.p.m. in

1971 herbaceous tissue to 11.3 in 1970 conifer tissue. The grand
average was 8.4 p.p.m. We accepted 10 p.p.m. as a reasonable
control concentration.

-7-

Radial data. — Based on vegetation type, the fluoride concentration
averaged 11.57p.p.m. in 1970 shrubs to 19.74 p.p.m. in 1970 conifers.
On a plot basis, regardless of vegetation type, the range was from
29.5 p.p.m. at R4-P2 near the company to 9.6 p.p.m. at R5-P9 in
Glacier National Park.

Histological analyses

Histological analysis of necrotic conifer needles indicated micro¬
scopically the same disease syndrome occurred in 1971 and in 1970.
Expanded parenchyma and occluded resin canals were common, causing
crushing and collapse of adjacent cells.

Insect analyses

Comparative results between 1970 and 1971 are given in Appendix VI.

No controls were analyzed in 1971, so data was compared to 1970
controls .

Accumulations were similar to those found in 1970. All were
greater than accumulations in the control samples. Pollinators
contained the most fluoride, ranging from 81.3 p.p.m. in Erynnis sp.
to 585.0 in mixed Hymenoptera. Predators, i.e., Asilidae, dragon¬
flies, and damselflies, accumulated from 21.7 to 82.9 p.p.m., and
foliage feeders had from 168 to 255 p.p.m. fluoride.

As mentioned earlier, the Anaconda Company reported it had reduced
fluoride emissions at its Columbia Falls, Montana, plant from
7,500 pounds per day in 1970 to 2,500 pounds per day in 1971.

This is a 67 percent reduction. Our data indicated an average
reduction of fluoride in plant tissue of about 50 percent and an
average I. I. reduction of about 46 percent. However, this does
not imply the pollution problem is solved.

In our 1971 report (Carlson and Dewey 1971), we presented an isopol
map depicting lines of equal average plant tissue fluoride concen¬
tration. This map is shown in Figure 1. In Appendix III-A of
that report we listed calculated acreages within isopols. The
1971 data was used to recompute and adjust the isopols. The isopol
map constructed from this data is shown in Figure 2.

The fluoride grand averages, listed in the 1971 report, were
grouped and adjusted downward by the following factors, based on
data collected in 1971:

1.

2.

3.

Plots 1, 2, and 3 reduced 33.8 percent.
Plots 4 and 5 reduced 42.7 percent.

Plots 6 through 10 reduced 14.3 percent.

-8-

-9-

-10-

Isopols for 1971 were then developed by the same procedure used
for 1970 data, using the adjusted 1970 data.

Table 1 shows the area polluted by fluorides as estimated from the
new isopol map. The total area polluted (area within the 10
isopol) was 280 square miles (179,200 acres), down 54 square miles
(34,560 acres) from 1970. The area sustaining most of the fluoride-
induced injury to vegetation (within the 30 isopol) was 23.75
square miles or 15,200 acres. This is down 84.25 square miles or
53,920 acres. The data indicate a critical air pollution problem
still exists in the Columbia Falls area.

Table 1. — Area polluted by fluorides

Isopol _ All lands _ Glacier National Park

Square miles

Acres

Square miles

; Acres

10

280.00

179,200

100.0

64,000

15

140.00

89,600

20.0

12,480

20

62.00

39,680

1.5

960

30

23.75

15,200

60

12.00

7,680

100

5.25

3,360

300

1.50

960

600

.75

480

The area

polluted by greater

than 10 p.p.i

m. in Glacier

National

Park was

100 square miles, down 12 square

miles (7,680

acres) from

1970. The 30 and 60 isopols did not extend into the Park as in
1970. The 20 p.p.m. isopol included 1.5 square miles (960 acres)
and the 15 isopol included 20 square miles (12,480 acres).

Although the I. I. grand averages in Glacier National Park indicate
no injury was found, in R4-P6 fluoride markings were found on 1970
ponderosa pine needles, but were not severe enough to bring the
I. I. up to 0.006 or greater.

CONCLUSIONS

In our 1971 report, we indicated that significant reductions in
emissions likely would not eliminate fluoride accumulation by
vegetation at distant plots, including those in Glacier Park.
Current data support that hypothesis. Fluorides in plots R4-P6
and R5-P6 were reduced only 8.0 percent and 4.3 percent, respec¬
tively. Vegetation there still is accumulating considerable
fluorides, indicated by the 16.1 p.p.m. and 30.3 p.p.m. plot
averages computed in this report. It is not unreasonable to
hypothesize that even if the aluminum plant reduced fluoride
emissions to the State of Montana standard of 864 pounds per day,
fluorides will continue to be accumulated by vegetation in Glacier
Park.

-11-

Stem analyses showed definitely that excessive fluorides do occur
either on or within the woody tissue. The exact distribution
could be determined by analyzing separately the outer and inner
bark and xylem. However, the presence of fluorides either on or
in the tissue presents a potential hazard to wildlife browsing
on that tissue. Bark beetles may be accumulating these fluorides
if they (fluorides) are carried within the vascular system of the
tree.

It is not known what effect fluorides are having on insect popula¬
tions in the study area. We believe that fluorides are being
accumulated by insects and passed along the food chain in the area.

In conclusion, it has been determined:

1. Chemical analysis of vegetation in the Columbia Falls area
indicates the Anaconda Company aluminum plant likely has reduced
its fluoride emissions.

2. The reduction was not enough to prevent vegetation as far
away as Glacier Park, up to 12 miles from the Anaconda Aluminum
Company plant, from accumulating above-normal amounts of fluoride.

3. Injury to vegetation can still be observed over an extensive
area of 15,000 acres.

4. Insects continue to accumulate fluorides.

ACKNOWLEDGEMENTS

I express my appreciation to Mrs. Carma Gilligan for her careful
and accurate work in preparing tissues for chemical and histologi¬
cal analysis. Also, a special word of thanks is due Jerald E. Dewey,
entomologist in the Northern Region heardquarters, Division of State
and Private Forestry, for making the field collections of insects.

Mention of trade names and commercial products in this publication
is for information only. No endorsement of the U.S. Department of
Agriculture is implied.

-12-

LITERATURE CITED

Carlson, C. E. , and J. E. Dewey, 1971. Environmental pollution
by fluorides in Flathead National Forest and Glacier National
Park. USDA, Forest Service, Missoula, MT, 57 pp.

Durst, R. A., 1969. Ion selective electrodes. National Bureau
of Standards special publication 314, 474 pp.

Gordon, C. C., 1972. 1970 Glacier National Park study. Univer¬

sity of Montana, Missoula, MT.

Jacobson, J. S., and D. C. McCune, 1969. Inter laboratory study
of analytical technique for fluorine in vegetation. Jour, of
the ADAC , 52: 5.

-13-

APPENDIX I

CHEMICAL ANALYSIS OF PLANT AND INSECT TISSUE^/

Determination of fluoride content in vegetation and insect tissue
was done exactly the same. The following procedure was used:

1. Field samples were dried for 2 days at 100° F. in a
forced-draft oven.

2. Dried samples were ground in a Wiley mill to pass a
40-mesh screen.

3. 0.5000 gram of dried tissue was weighed into a nickle
crucible. 0.0500 gram of low-fluorine calcium oxide was then
added .

4. Sample and CaO were slurried with distilled water.

5. Slurry was dried and charred under infrared oven.

6. Charred material was ashed for 16 hours at 600° C. in
a muffle furnace.

7. After ashing, crucibles were allowed to cool in a
dessicator .

8. Ashed samples were moistened with distilled water, then

3 ml. of 30 percent perchloric acid were added to dissolve the ash.

9. Dissolved ash was then brought to 100 ml. volume by
adding TISAR^/ diluted 50 percent by distilled water.

10. Fluoride activity was determined using a Beckman research
pH meter and Orion fluoride and reference electrodes.

1/ From Dr. C. C. Gordon, University of Montana.

2/ Trade name of Orion’s product which adjusts pH and total
ionic strength of sample solution.

-14-

pai

1

2

3

4

5

6

7

8

9

10

11

12

13

14

15

16

17

18

19

20

21

22

23

24

25

26

27

28

29

30

31

32

33

34

35

36

37

38

APPENDIX II

COMPARATIVE FLUORIDE ANALYSES WITH WARF-i/

WARF

Our

Data

WARF

Our

result

result

pair

result

result

306.0

147.0

39

19.5

31.0

600.0

455.0

40

97.5

113.0

469.0

329.0

41

23.0

26.4

825.0

294.0

42

78.5

79.0

2,750.0

1,440.0

43

10.0

20.8

10.5

25.6

44

21.0

26.2

1,288.0

595.0

45

31.5

27.6

113.0

127.9

46

32.0

38.6

198.0

120.0

47

11.5

33.6

37.5

44.4

48

104.0

87.2

11.5

65.0

49

115.0

118.0

3.0

42.0

50

1,425.0

830-0

21.0

70.8

51

32.5

40.8

99.0

132.0

52

385.0

172.0

38.5

79.0

53

293.0

224-0

13.5

34.0

54

12.5

10-0

19 .0

29.6

55

29.0

35.6

12.0

39.6

56

22.0

29.8

31 .0

112.0

57

30.5

30.4

91.5

136.0

58

32.5

29.6

23.0

52.0

59

30.5

39.6

29 .0

47.4

60

12.5

34.O

113.0

112.0

61

44.5

45.8

139 .0

162.0

62

16.0

28.4

15 .0

73.0

63

33.0

30.5

16 .0

28.0

64

9.0

26.4

275 .0

236.0

65

508.0

256-0

14 .0

23.6

66

73.0

75.0

198 .0

124.0

67

750.0

352.0

200 .0

164.0

68

16.5

28.0

45 .0

54.0

69

28.5

23.6

59.5

64.4

70

27.0

40.8

63.5

50.0

71

76.0

52.4

178 .0

114.5

72

10.0

16.4

8.0

27.8

73

325.0

290.0

14.5

23.6

74

168.0

152.0

295.0

264.0

75

55.0

65.6

293.0

250.0

76

8.0

22.4

P.p.m. fluoride, dry weight basis.

-15-

APPENDIX II

COMPARATIVE FLUORIDE ANALYSES WITH WARP!/ (con.

Data

WARF

Our

pair

result

result

77

75.0

78.0

78

135.0

112.0

79

14.0

20.4

80

30.5

33.4

81

11.5

39.0

82

10.0

16.4

83

52.5

55.6

84

39.0

62.4

85

25.5

70.0

86

18.5

50.4

87

1,375.0

780.0

88

218.0

152.0

89

190.0

188.0

90

37.0

31.6

91

60.0

69.0

92

130.0

158.0

93

32.5

41.0

94

26.5

52.0

95

6.3

30.2

96

72.5

66. 0

97

319.0

134.0

98

8.5

58.2

99

25.5

35.8

100

35.0

44.4

101

15.5

12.4

102

27.5

41.5

103

32.0

51.8

104

96.5

78.4

105

5.5

14.0

106

28.5

34.2

107

16.5

34.0

108

16-0

24.6

109

7.5

10.1

110

293-0

264.0

F ratio for slope =

2685.97

Correlation (r) =

0.98

1/ P.p .m. fluoride, dry weight basis.

-16-

41

12

4

6

13

54

93

84

74

115

128

144

153

151

168

182

199

223

202

232

251

265

252

264

272

318

292

348

362

37 7

378

386

394

388

APPENDIX III

REPEATABILITY OF SPECIFIC ION FLUORIDE ANALYSES^

Check

crucible

Original

Check

Percent

number

analysis

analysis

Difference

difference

57

20.0

20.0

0.0

0.0

56

126.0

136.4

10.4

8.3

55

16.4

15.2

1.2

7.3

53

28.4

22.4

6.0

21.1

52

47.6

39.8

7.8

16.4

51

61.8

74.2

12.4

20.0

92

74.2

66.4

7.8

10.5

98

48.6

48.0

0.6

1.2

99

210.0

214.0

4.0

1.9

104

10.8

13.4

2.6

24.0

122

23.6

27.8

4.2

17.8

143

72.2

71.4

0.8

1.1

154

15.2

14.9

0.3

2.0

161

9.4

11.6

2.2

23.4

170

15.2

18.0

2.8

18.4

178

12.8

15.2

2.4

18.7

187

63.0

60.8

2.2

3.5

203

23.2

22.6

0.6

2.6

229

14.0

12.6

1.4

10.0

230

19.0

18.4

0.6

3.2

244

10.2

14.1

3.9

38.2

263

46.0

46.4

0.4

0.9

274

8.6

8.6

0.0

0.0

285

72.2

87.0

14.8

20.5

297

71.0

64.0

7.0

9.9

309

64.2

51.0

13.2

20.6

322

124.0

152-0

28.0

22.6

352

240.0

284.0

44.0

18.3

350

30.4

18.8

11.6

38.2

365

9.6

8.2

1.4

14.6

382

21.0

21.6

0.6

2.9

384

43.0

49.0

6.0

14.0

400

23.6

27.0

3.4

14.4

415

14.6

5.0

9.6

61.9

424

9.4

16.2

6.8

72.3

4 34

21.6

35.8

14.2

65.7

P.p.m. fluoride, dry weight basis.

-17-

APPENDIX III

REPEATABILITY OF SPECIFIC ION FLUORIDE ANALYSES

1/

(con. )

Crucible

number

Check

Crucible

number

Original

analysis

Check

analysis

Difference

Percent

difference

437

450

5.8

6.6

0.8

13.8

440

451

13.8

18.2

4.8

34.8

4 38

452

12.0

17.0

5.0

41.7

2

30.8

29.2

1.6

5.6

5

20.0

19.0

1.0

5.0

7

49.2

47.8

1.4

2.8

9

20.8

21.8

1.0

4.8

10

21.5

16.0

5.5

34.4

11

292.0

306.0

14.0

4.6

14

10.4

11.6

1.2

10.3

15

10.1

10.4

0.3

2.9

16

100.4

102.4

2.0

2.0

17

11.8

14.4

2.6

18.0

18

19.6

24.4

4.8

19.7

19

16.4

21.2

4.8

22.6

20

64.2

62.6

1.6

2.6

21

17.2

17.8

0.6

3.4

22

32.6

38.4

5.8

15. 1

24

27.2

24.2

3.0

12.4

31

16.8

17.0

0.2

1.2

TOTAL

297.2

884.1

AVERAGE

5.31

15.8

S x =

.9932

t 56 =
.05

2.00

Confidence interval

at 95 percent level = 5.31 + 1.9864

1/ P.p.m. fluoride, dry weight basis.

-18-

APPENDIX IV

nil

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-19-

1/ All values are p.p.m. fluoride.

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CO

<3"

r-H

CM

so

r-H

m

CO

sO

<3*

i-H

CM

un

o

•<r

CM

1 — 1

d

CO

+

+

i-H

r-H

i

1

i

l

r“H

CM

+

+

rH

O

<!

O

#

m

o

i-H

44

o

r-H

44

O

r-H

44

o

»H

44

H

CM|

sO

44

S'?

CO

r-'.

44

S'?

<3-

r»

44

CO

44

Ph

OS

Os

•H

Ph

OS

os

•H

P-1

OS

OS

•H

d4

Os

OS

•H

1

i-H

i-H

Q

1

i—H

r-H

Q

1

i-H

i-H

Q

1

i-H

r-H

Q

m

sO

sO

r-»

Pi

oi

Pi

Pi

-21-

SUMMARY OF 1971 DATA- (con.

Ml

o

00

4)

■H

‘H

O

r^-

o

o

ON

00

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■u

5-1

r-~

•

•

.

•

c

00

cO

O

O'

CO

r^

o

CTv

cO

cO

5-i

• — 1

+

+

r-H

+

J3

5-i

•U

05

+

o

05

C

G

>

a>

CO

.

cO

o

i n

5-i

G

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G

o

4-1

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i— — i

o

uo

<r

•rH

a

40

•

•

«

•

T— 1

•

O'

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r-H

r-H

5-i

pH

+

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r-H

1

U-i

><

+

+

If)

O)

mh

•H

c

o

o

•JC

00

•H

XI

C

g

5-1

o

cm aj
>-!

O

140

140

O

co

o

o

O'

O'

O'

O

O'

o

•

o

o

o

MD

CM

co

o

o

o

o

pH

O

r-H

o

M

o

o

o

r-H

o

r-H

MO

o

o

o

o

o

o

o

•

•

•

•

•

•

•

•

•

•

•

•

•

•

•

1 — 1

o

+

i

U0

o

+

o

1

o

00

o

1

pH

05

M

o

140

140

r-H

r^-

O

o

M0

M0

o

o

G

c

o

o

00

r-H

40

o

o

O

O

pH

o

r-H

o

5-1

o

o

o

o

o

O

o

O

o

o

o

o

o

a)

•

•

•

•

•

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•

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+

1

CM

o

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00

o

1

r-H

05

OC

G

r-H

CO

CO

M0

CO

<f

U0

pH

o

O'

CM

uo

5-i

•

05

140

00

vD

00

r— H

MO

40

r-H

00

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00

00

o

>

CM

r-H

1

CO

CM

CM

+

+

r-H

r-H

1

1

CM

pH

1

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G

1

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140

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00

o

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pH

U)

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O'

in

CM

r-H

CM

o

pH

5-i

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1

CO

r-H

r-H

CM

pH

- - 1

U0

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i

1

1

U)

UO

00

UO

140

CM

o

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00

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o

m

00

rQ

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r—H

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co

UO

CM

M0

CO

uO

oo

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UO

CM

CO

co

o

05

CO

« — 1

t-H

CM

00

r-H

CM

r-H

00

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CM

i

pH

eg

i

1

+

r-H

+

+

1

■U

G

0)

140

00

in

CO

oo

U0

*<r

CO

O'

pH

CM

UO

o

<r o co uo

H H | (M

I

N O' CN

LO O' <f O'
i — I i— 1 -(- CM

cm oo O' mo

O' r-~ r-H uo

l — •
l

oo m> O

oo oo O' in
CM ■ — I I CO

I

O'

CM

oo oi m h
co cm ■— i <r

I i

CM

a-'

h o o m

i— I r— I '£>

M0

CM

<r ■— i cm o'

oo -i o o

o- -<r o o

CM CM I

CO

CM

<u

X)

B
a .
a.
g
G

W

JO

UO

oo

o

o

UO

pH

<1-

CO

o

40

3

•

•

•

•

•

5-4

CO

U0

CO

CM

00

<1*

O'

o

00

o

-C

CO

CM

i

CM

CO

pH

r-H

40

CM

<r

CO

i

1

1

i

i

•

4-1

•

•

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o

» — l

4-1

a

O

r-H

4-1

o

pH

4-1

O

r-H

UH

U0

4-4

4-1

S'? 40

4H

O'

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64?

P-i

O'

O'

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•

O'

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Oh

O'

O'

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Cu

O'

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1

pH

r— H

a

i-H

r—H

pH

o

1

pH

pH

Q

1

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pH

Q

oo

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Pi

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Pi

pi

cn
05
0
i — I

G

>

-22-

2/ Conifers only.

APPENDIX IV

Ml

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A)

•H

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0)

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5-1

G

00

CO

O

ON

cd

G

5h

t-H

JZ

g

■u

(D

o

cd

C

3

>

CD

10

•

CO

O

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5h

c

•H

kO

G

o

■U

ON

■H

a

v£>

1 - <

•

ON

5-i

* — 1

Ci-i

>-i

o

m

00

m

o

r— I

CN

-d

CO

m

o

co

<1-

00

vO

m o

JZ

•

00

M0

rH

r-H

in o

00 M

r^

o

o o

•H

•

•

•

•

• •

re

M

rH

l

r-H

1 CO

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1

0)

oo

00

i— H

vO o

.

cO

o

O

o

f-H

CO o

M

M

i— H

IT)

vO

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•

CD

•

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M

>

rH

1

i m

cO

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ON

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cd

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ON

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lO ON

c

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0)

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o

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>

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r— 1

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on

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1 cd

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co m

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vO

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t-H

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ON

00

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l l

CJ

t-H

t-H

CD

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<1

in

u

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1 CO

m

cm <d

o

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r-

CM

CO

o

O

o

o

O O

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co

t— H

o

i— 4 VO

3

,

•

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50

o

t-H

ON

<1*

in m

-C

CM

CO

00

H

on <t

CO

ON

CO

m

l i

CM

t-H

r-H

a)

14H

•

t)0

• >4H

i-l O

i — 1

MH

< — i

H

cd

<4H *H

cd t--.

cfl

4H

cd

54

<4H Q

■U ON

+->

*H

4-1

on

CD

•H

O • — I

O

O

o

t-H

>

Q

H

E-h

E-h

23

APPENDIX V

SUMMARY OF STEM ANALYSES'

1/

Shrubs Conifers

Year

of tissue

Year

of tissue

Herbs

Grand

Plot

1969

1970

1971

1969

1970

1971

1969

average

Control

7.8

9.5

6.9

9.3

11.3

5.9

5.8

8.4

R2-P2

11.6

19.8

12.8

25.5

25. 7

24.7

23.8

22.0

R3-P3

10.2

10.4

12.0

24.2

22.7

27.3

16.4

19.7

R3-P4

7.2

7.6

10.8

10.6

16.8

15.8

11.6

13.4

R4-P2

16.6

15.1

37.6

35.0

37.4

41.1

22.6

29.9

R5-P3

19.8

15.2

20.0

19.3

35.5

35.4

— —

26.2

R5-P4

9.4

13.0

19.8

16.6

12.8

17.6

10.8

14.7

R5-P5

11.4

8.4

7.8

13.6

14.6

14.2

11.6

12.2

R5-P6

11.8

9.8

15.1

11.3

10.1

11.2

_

11.3

R6-P3

15.2

22.8

16.2

20.4

21.0

17.7

21.0

19.3

R6-P4

14.0

11.6

16.6

21.5

14.6

25.5

14.0

18.9

R7-P3

17.0

20.2

29.8

20.2

19.0

18.3

10.2

19.2

R8-P5

14.8

12.6

9.8

13.2

14.2

10.4

11.2

12.4

Col. Mt.

11.3

9.0

9.8

28.4

21.5

13.8

17.2

15.0

R5-P9

8.5

7.6

6.4

8.4

13.9

7.4

10.4

9.2

R4-P6

10.6

6.8

14.8

17.8

8. 7

10.4

11.6

11.1

Veg. type

average

12.69

11.57

16.85

19.46

19.74

19.39

14.80

17.10

1/

All values are

p . p .m.

fluoride ,

dry weight bas

is .

-24-

APPENDIX VI

FLUORIDE ACCUMULATIONS BY INSECTS^

Date P.p.m.

collected fluoride

Pollinators

Bumblebees

8/12/70

406.

Mixed Hymenoptera

8/16/71

585.0

Wood nymph butterfly -

Ceroyonis sp .

8/12/70

58.0

Wood nymph butterfly -

Ceroyonis sp.

8/16/71

144.0

Skipper butterfly -

Erynnis sp.

8/12/70

146.0

Skipper butterfly -

Erynnis sp .

8/16/71

81.3

Mixed Syraphildae

8/16/71

140.0

Mixed Syraphildae

None collected

in 1970

Predators

Robberflies - mixed Asilidae

8/16/71

82.9

Robberflies - mixed Asilidae

None collected

in 1970

Dragonflies - mixed Anisoptera

8/16/71

24.8

Damselflies - Argia sp.

6/1/70

21.7

Foliage Feeders

Arctiidae (larvae)

8/16/71

255.0

Notodontidae (larvae)

8/16/71

168.0

1 / P.p.m. fluoride, dry weight basis. Where possible, 1970
results are given for comparative purposes.

-25-

*

*