Ecological Research Series
Sulfur Content of Douglas-Fir
Foliage Near a Paper Mill
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55
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National Environmental Research Center
Office of Research and Development
U.S. Environmental Protection Agency
Corvallis, Oregon 97330
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EPA-660/3-74-018
August 1974
SULFUR CONTENT OF DOUGLAS-FIR
FOLIAGE NEAR A PAPER MILL
by
Hilman C. Ratsch
Plant Ecology Branch
National Ecological Research Laboratory
Corvallis, Oregon 97330
Roap/Task 21 ALR 03
Program Element 1AA006
NATIONAL ENVIRONMENTAL RESEARCH CENTER
OFFICE OF RESEARCH AND DEVELOPMENT
U.S. ENVIRONMENTAL PROTECTION AGENCY
CORVALLIS, OREGON 97330
For sale by the Superintendent of Documents, U.S. Government Printing Oulce
Washington, D.C. 20402 - Price 65 cents
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ABSTRACT
Douglas-fir needles were collected at eleven sites on the
south side of the Columbia River in the vicinity of the Wauna
Pulp and Paper Mill. The concentration of total sulfur in the
needles ranged from 0.1 -- 0.2 percent at eiciht locations
and 0.5 -- 1.0 percent at three hillside locations. Douglas-fir
needles with high sulfur contents at the three hillside locations
had no visible sulfur dioxide injury symptoms. The hinh sulfur
values in needles indicate sulfur dioxide is beinn absorbed
by the foliage and are on the borderline level of producina
visible injury.
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CONTENTS
Page
Abstract ii
Sections
I Introduction 1
II Methods and Materials 1
III Results 4
IV Conclusion 7
V References 8
VI Appendices 9
m
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INTRODUCTION
This study deals with Technical Assistance to the Northwest Region
of the Department of Environmental Quality, State of Oregon. The
Department has begun an evaluation of the feasibility of expanding the
Crown Zellerbach pulp and paper mill at Wauna, OR. In the evaluation,
S02 emissions were predicted to occur on a ridge and hillside
downwind from the mill at concentrations sufficient to cause plant
damage. The presence or absence of plant injury in this area may
provide insight into the validity of the dispersion model estimates.
The Wauna pulp and paper mill is located on the south side of the Columbia
River, approximately 25 miles east of Astoria at Wauna, Oregon. The
hillside impact areas are on the north facing slope of the Columbia
gorge approximately two to three miles southeast of the mill.
The objective of the study is to determine if 862 effluent has an
effect on vegetation on the hillside impact areas. An S0? effect
can be demonstrated by the observations of visible injury symptoms and/or
the presence of high sulfur content in foliage.
METHODS AND MATERIALS
On March 8, 1974, eleven sites in the vicinity of the mill were visited
to observe S02 injury and to collect samples of Douglas-fir foliage for
sulfur analysis, see fig. 1 and Table 1. Most of the samples were collected
either southwest or northeast of the mill. Three background samples were
collected, one over the ridge from the Columbia gorge at Gnat Creek Forest
Park and two on Fall Creek near Clatskanie.
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The Douglas-fir needles collected were separated into current year and
1 year-old needle samples and submitted to Laboratory Services
Branch (NERC) for total sulfur analysis.
Sulfur Analysis as a Diagnostic Technique
The visible effects of SOp on vegetation can be classified into
two categories: acute and chronic injury. Acute injury is severe
injury that is assoicated with high, short-term SOp concentrations,
while chronic injury is light to severe injury associated with long
term exposures and SOp concentrations sufficiently high to
produce cell disruption. Much of the damage attributed to SOp may
in fact be due to sulfuric acid and sulfates resulting from photochemical
oxidation of SOp.
In general, a large amount of sufate is found in leaves with chronic
symptoms, whereas leaves that are acutely injured show only a small
increase in sulfate content. However, large quantities of sulfate
may accumulate in leaf tissue without visible leaf injury.
This can be explained by the mechanism in which plants are injured by
SOp. Acute injury does not occur if the rate of SOp absorption does
not exceed the capacity of the plant to oxidize the sulfite to sulfate
ions. Under long term SOp stress, sulfates thus formed may accumulate with
the subsequent development of chronic injury symptoms. It is also
feasible that sulfates may accumulate without reaching the critical
level necessary to produce injury symptoms. Under natural conditions,
sulfur analysis can reflect the magnitude of pollution to which
vegetation has been exposed.
The exterior symptoms of acute or chronic injury caused by SO,, emissions,
in the form of necrosis chlorosis, and alterations in the physical
appearance of the plants, are not sufficiently specific in themselves
to allow the definite identification of SOp effects. However, injury
resulting from chronic SOp exposure can usually be confirmed by the
presence of a high sulfur content in leaves.
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Normal Sulfur Content
Katz and McCallum collected Douglas-fir foliage from many points
in Washington and British Columbia and found the normal average
sulfur content increased from .082 percent in current year needles to
2
0.149 percent in three-year-old needles. In another source they
state that the normal sulfur content of Douglas-fir leaves varied
from 0.10 percent to a little over 0.20 percent.
They found that the sulfur content in some cases varied little from
year to year while in others there was a definite increase in the older
leaves. They assumed that where sufficient sulfur was available in
the soil, the sulfur content of the needles increased with age, while
at other low soil sulfur locations it remained constant.
Sulfur Accumulation
In 1930 and 1931, Douglas-fir needles were collected south of Trail,
B.C., in the Columbia River Valley in the "Smoke Zone" of a large
smelter and analyzed for sulfur. The sulfur content of the needles
exposed to S02 was substantially higher than normal and decreased
with increasing distance from the source. A three or four-fold
increase over the average normal sulfur content occurred in some needles,
although there were no symptoms of either acute or chronic injury.
2
In experimental plots Katz found that sulfates accumulated in plant
tissue were not toxic to leaves even in amounts three-five times greater
than the original sulfur content.
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Apparently, conifer needles can accumulate sulfur by absorption of sulfur
dioxide at low concentrations over a long period without suffering
visible injury. However, a heavy dose exposure over a short period
may produce significant damage with only a slight increase in sulfur
content.
If the normal sulfur content of Douglas-fir needles varies from
0.1 to 0.2 percent, the needles can conceivably accumulate sulfur in
a range from 0.6-1.0 percent sulfur without resulting in any visible
injury. This level of sulfur content indicates a high degree of
pollution and is on the borderline of producing chronic injury symptoms,
RESULTS
On-Site Conditions
Severe injury symptoms on Douglas-fir were observed at the Bradley
State Park location. Two trees on the slope below the parking lot
had needle tip burn on the current year, one year and two year-old needles.
The most severe tip burn occurred on the two year-old needles where
50-75 percent of the needle was brown and necrotic. Several branches
on these two trees had considerable needle loss. Needle loss was most
severe on the one and two year-old stems. The current needles had
a chlorotic mottle type of injury.
On the basis of visible symptoms, the injury observed may be the
result of S0? exposures, winter dessication or insect injury. Injury
symptoms on Douglas-fir were also observed at locations No. 2 and 4,
but were not specific as to cause.
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Histological Examination
Needle tissue showing visible injury from Bradley State Park was
examined histologically. Freehand cross sections were cut from
needle tissue and mounted on slides in glycerin and water and examined
under the microscope. The injury in Douglas-fir needles consisted
of the collapse and pigmentation of the mesophyll in the upper part
of the needle with occasional collapse and pigmentation of mesophyll
below the vascular bundle, see Fig. 2. In most injured sections the
guard cells of the stomata on the lower needle surface were pigmented
and occasionally the epidermal and resin canal cells were also pigmented.
The microscopic injury symptoms observed on the Douglas-fir needle
tissue point strongly to SO^ and salt injury. In view of the somewhat
elevated sulfur content of the needles, SCL is highly suspect as the
cause of injury at Bradley State Park.
Sulfur Analysis
The results of the analysis for total sulfur on the collected Douglas-
fir needles are shown in Table 2. The sulfur content of the background
samples (0.10 - .21 percent sulfur) at locations No. 7, 10, 11 agrees
with published sulfur values for "normal" Douglas-fir needles (0.1 -
0.2 percent sulfur). The hillside samples at locations 1, 2 and 3 from
the suspected worst impacted area had sulfur contents of 0.49 - 1.05
percent. This indicates a high sulfur enrichment and in many cases
was associated with visible injury symptoms.
At location No. 4 on the border of the worst impacted area and at locations
No. 8 and 9 in the second impact area, the sulfur contents appear to be
normal.
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At Bradley State Park (locations No. 5 and 6) the sulfur contents
are somewhat elevated and the current needles have as high or
higher sulfur values than the one year-old needles.
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CONCLUSION
Sulfur accumulation in Douglas-fir foliage is indicative of sulfur
dioxide exposures and absorption. Whether leaf damage occurs depends
not only on the amount of sulfur accumulated, but on the adsorption
rate of sulfur dioxide as well as on the specific type and environment-
conditioned plant resistance. At the hillside locations 1, 2 and
3 the sulfur content of foliage was several times normal, although there
was no characteristic visible injury. At Bradley State Park (locations
5 and 6) the sulfur content of foliage was only slightly above
normal, although sulfur dioxide injury symptoms were evident.
The sulfur content of Douglas-fir needles at locations 1, 2 and 3
indicate sulfur dioxide is being absorbed by foliage and is responsbile
for the sulfur enrichment of the needles. The sulfur values are on
the borderline level of producing visible injury.
The needle sulfur contents at locations 4, 8 and 9 are at a normal
level and do not appear to be in the sulfur dioxide impact area. Based
on visible injury symptoms and histological examination, the injury
at Bradley State Park is probably due to sulfur dioxide.
Doug! as-fir is intermediate in its sensitivity to sulfur dioxide
(see Table 3) for concentrations that produce injury after short
term exposures. Plants that fall in the sensitive category of
susceptibility that may be observed in the future are as follows:
alder, paper birch, Sitka mountain ash, Douglas maple, bitter cherry,
chokecherry, blueberry elder, willow, aspen, alfalfa, sweet clover,
larch and white pine.
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REFERENCES
1. Katz, Morris and A. W. McCallum. "Effect of Sulphur Dioxide on
Vegetation," Ottawa. National Research Council of Canada, 1939.
Chapter IV, pp. 104-30.
2. Katz, Morris and A. W. McCallum. The Sulphur content of Douglas-
fir and yellow pine in northern Stevens county, Washington, in
1935. Trail Smelter Question, Documents Series B, Appendix BB 5, 1936.
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Table 1
Sample Locations in the Vicinity
of the Wauna Pulp Mill
Location
1
2
3
4
5
6
7
8
9
10
11
Approximate
Description Elevation
on hillside between Westport and 300 ft.
Taylorsville, solitary Doug-fir with
broken top along logging road
on hillside between Westport and 500 ft.
Taylorville above location #1,
small Doug-fir
on top of ridge (next to power line) 640 ft.
between Westport and Taylorville.
Large Doug-fir on outer perimeter of
a group of trees
on low hillside just south of 200 ft.
Taylorville, medium size Doug-fir
in line of sight of plume
Bradley State Park 640 ft.
on steep slope below parking lot
Bradley State Park 640 ft.
on steep slope below parking lot
Gnat Creek Forest Park, large 240 ft.
Doug-fir in heavy fir-hemlock
stand upstream from park
Lost lake residential area south 400 ft.
of Westport, solitary Doug-fir
along road near dead end
EPA Westport Substation, large 240 ft.
Doug-fir next to power line
Fall Creek Road, large Doug-fir 550 ft.
adajacent to road
on logging road off Fall Creek Road 700 ft.
small Douglas-fir in hemlock stand
Age
of Needle
current
1 year old
current
1 year old
current
1 year old
current
1 year old
current
1 year old
current
1 year old
current
1 year old
current
1 year old
current
1 year old
current^
1 year old
current
1 year old
Sample
Number
11001
002
003
004
005
006
007
008
009
010
on
012
013
014
015
016
017
018
019
020 .
021
022
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Table 2
Total Sulfur Content of Douglas-fir
Needles in the Vicinity of the Wauna Pulp and Paper Mill
Location
1
2
3
4
5
6
7
8
9
10
11
Age
of Needle
current
1 year old
current
1 year old
current
1 year old
current
1 year old
current
1 year old
current
1 year old
current
1 year old
current
1 year old
current
1 year old
current
1 year old
current
1 year old
Sample
Number
11001
002
003
004
005
006
007
008
009
010
on
012
013
014
015
016
017
018
019
020
021
022
Percent Total Sulfur
(dry weight)
1.05
1.01
.98
1.01
.62
.49
.11
.21
.22
.17
.23
.24
.10
.15
.14
.14
.14
.15
.14
.15
.18
.21
10
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Table 3
Sulfur Dioxide Concentrations that will Produce
Threshold Injury to Intermediate Susceptible Plants
For Short-Term Exposures.
Time 2
Hours ug/m (ppm)
0.5 9170-31,440 (3.5-12)
1.0 6550-26,200 (2.5-10)
2.0 3930-19,650 (1.5-7.5)
4.0 1310-13,100 (0.5-5)
8.0 524-6,550 (0.2-2.5)
11
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• 7
Fig. 1. Douglas-fir foliage collection
sites in the vicinity of the Wauna pulp
and paper mill.
I
Scale of Miles
10
II
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Epidermis
Vascular bundle
Mesophyll
Resin Canal
Endodermis
Transfusion tissue
Fig. 2. Diagram illustrating, in cross section, the tissue showing
collapse and pigmentation in a Douglas Fir needle.
13
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BIBLIOGRAPHIC DATA
SHEET
1. Report No.
EPA-660/3-74-018
3. Recipient's Accession No.
4. Title and Subtitle
Sulfur Content of Douglas-fir Foliage Near a Paper Mill
5. Report Date
Auoust 1974
6.
7. Author(s)
Hilman C. Ratsch
8. Performing Organization Rept.
No.
9. Performing Organization Name and Address
National Ecological Research Laboratory
Environmental Protection Agency
200 SW 35th St.
Corvallis. OR 97330
10. Project/Task/Work Unit No.
PE 1AA006 21 ALE 03
11. Contract/Grant No.
12. Sponsoring Organization Name and Address
same
13. Type of Report & Period
Covered
Final Report
14.
15. Supplementary Notes
16. Abstracts
Douglas-fir needles were collected at eleven sites on the south side of the
Columbia River in the vicinity of the Hauna Pulp and Paper Mill. The concentration
of total sulfur in the needles ranged from 0.1 — 0.2 percent at eiqht locations
and 0.5 -- 1.0 percent at three hillside locations. Doucilas-fir needles with
high sulfur contents at the three hillside locations had no visible sulfur dioxide
injury symptoms. The high sulfur values in needles indicate sulfur dioxide is
being absorbed by the foliage and are on the borderline level of producinc
visible injury.
17. Key Words and Document Analysis. 17o. Descriptors
sulfur
Douglas-fir needles
pulp and paper mills
sulfur accumulation
air pollution
17b. Identifiers/Open-Ended Terms
sulfur analysis of Douglas-fir needles
17c. COSATI Field/Group
18. Availability Statement
19.. Security Class (This
Report)
UNCLASSIFIED
20. Security Class (This
Page
UNCLASSIFIED
21. No. of Pages
16
22. Price
FORM NTIS-35 (REV. 3-72)
USCOMM-DC 14952-P72
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