Table 1

Sample Locations in the Vicinity

of the Wauna Pulp Mill

Approximate Age Sample
Location Description Elevation of Needle Number
1 on hillside between Westport and 300 ft. current 11001
Taylorsville, solitary Doug-fir with
broken top along logging road 1 year old 002
2 on hillside between Westport and 500 ft. current 003
Taylorville above location #1,
smal] Doug-fir 1 year old 004
3 on top of ridge (next to power line) 640 ft. current 005
between Westport and Taylorville.
Large Doug-fir on outer perimeter of 1 year old 006
a group of trees
4 on low hillside just south of 200 ft. current 007
Taylorville, medium size Doug-fir
in line of sight of plume 1 year old 008
5 Bradley State Park 640 ft. current 009
on steep slope below parking lot 1 year old 010
6 Bradley State Park 640 ft. current 011
on steep slope below parking lot 1 year old 012
7 Gnat Creek Forest Park, large 240 ft. current 013
Doug-fir in heavy fir-hemlock
stand upstream from park 1 year old 014
8 Lost lake residential area south 400 ft. current 015
of Westport, solitary Doug-fir
along road near dead end 1 year old 016
9 EPA Westport Substation, large 240 ft. current 017
Doug-fir next to power line 1 year old 018
10 Fall Creek Road, large Doug-fir 550 ft. current 019
adajacent to road 1 year old 020.
WV on logging road off Fall Creek Road 700 ft. current. 021
small Douglas-fir in hemlock stand 1 year old 022



CONTENTS

Abstract

Sections

I Introduction

II Methods and Materials
Ill Results

IV Conclusion

Vv References

VI Appendices

Page

ii

o oN


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


Histological Examiniation

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 mesophyl]
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 S05 and salt injury. In view of the somewhat
elevated sulfur content of the needles, SO, 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.


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 SO, on vegetation can be classified into

two categories: acute and chronic injury. Acute injury is severe

injury that is assoicated with high, short-term S0, concentrations,
while chronic injury is light to severe injury associated with long

term exposures and S05 concentrations sufficiently high to

produce cell disruption. Much of the damage attributed to SO, may

jin fact be due to sulfuric acid and sulfates resulting from photochemical
oxidation of S0,.

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

S0,. Acute injury does not occur if the rate of S0, absorption does

not exceed the capacity of the plant to oxidize the sulfite to sulfate
jons. Under long term SO, 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 S05 effects. However, injury
resulting from chronic SO, exposure can usually be confirmed by the
presence of a high sulfur content in leaves.

2


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,
S05 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 SO) effluent has an

effect on vegetation on the hillside impact areas. An SO, 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 SO, 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.


BIBLIOGRAPHIC DATA. 1. Report No.
SHEET EPA-660/3-74-018

3. Recipient's Accession No.

4, Title and Subtitle

Sulfur Content of Douglas-fir Foliase Near a Paper Mill

5. Report Date

Auaust_1974
6.

7, Author(s)

Hilman C. Ratsch

8. Performing Organization Rept.
jo.

200 SW 35th St.
Corvallis, OR 97330

9. Performing Organization Name and Address

National Ecological Research Laboratory
Environmental Protection Agency

10. Project/Task/Work Unit No.
PE JAA006__ 21. ALR 03

11. Contract/Grant No.

same

12 Sponsoring Organization Name and Address

13. Type of Report & Period
Covered

Final Report

14.

15. Supplementary Notes

16, Abstracts

visible injury.

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.
of total sulfur in the needles ranged from 0.1 -- 0.2 percent at eight locations
and 0.5 -- 1.0 percent at three hillside locations.
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 producina

Doualas-fir needles with

The concentration

sulfur

17. Key Words and Document Analysis.

Douglas-fir needles
pulp and paper mills
sulfur accumulation

air pollution

17b. Identifiers /Open-Ended Terms

17c. COSATI Field/Group

17a. Descriptors

sulfur analysis of Douglas-fir needles

18. Availability Statement

19.. Security Class (This

21 No. of Pages

Repost) 16
UNCLASSIFIED
20. Security Class (This 22. Price

Page
“SINCLASSIFIED

FORM NTIS-35 (REV. 2-72)

USCOMM-DC 14952-P72


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 SO, 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.


Ecological Research Series

Sulfur Content of Douglas-Fir
Foliage Near a Paper Mill

ED ST,
: yy 7s

SZ

"AL por?

Qnoulaiyy
NV AGENCY

2
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%

National Environmental Research Center
Office of Research and Development

U.S. Environmental Protection Agency
Corvallis, Oregon 97330


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.

Douglas-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.


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.


Normal Sulfur Content

Katz and McCal1um! 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
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 S05 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.

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.


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 eiaht locations
and 0.5 -- 1.0 percent at three hillside locations. Doualas-fir
needles with high sulfur contents at the three hillside locations
had no visible sulfur dioxide injury symptoms. The hich sulfur
values in needles indicate sulfur dioxide is beina absorbed
by the foliage and are on the borderline level of producina
visible injury.

Vi


Table 2
Total Sulfur Content of Douglas-fir
Needles in the Vicinity of the Wauna Pulp and Paper Mill

Age Sample Percent Total Sulfur
Location of Needle Number (dry weight)
1 current 11001 1.05
1 year old 002 1.01
2 current 003 +98
1 year old 004 1.01
3 current 005 62
1 year old 006 49
4 current 007 VW
1 year old 008 21
5 current 009 +22
1 year old 010 17
6 current 011 23
1 year old 012 24
7 current 013 -10
1 year old 014 15
8 current 015 14
1 year old 016 14
9 current O17 14
1 year old 018 15
10 current 019 14
1 year old 020 «15
i current 021 18
1 year old 022 21

10


a

o7
Bradley Park

On

Fig. 1. Douglas-fir foliage collection
sites in the vicinity of the Wauna pulp
and paper mill.

Scale of Miles



EPA-660/3-74-018
August 1974

SULFUR CONTENT OF DOUGLAS-FIR
FOLIAGE NEAR A PAPER MILL

by
Hilman C. Ratsch
Plant Ecoloay Branch
National Ecological Research Laboratory
Corvallis, Oregon 97330

Roap/Task 21 ALR 0:
Program Element TAAOGG

NATIONAL ENVIRONMENTAL RESEARCH CENTER

OFFICE OF RESEARCH AND DEVELOPMENT
U.S. ENVIRONMENTAL PROTECTION AGENCY
CORVALLIS, OREGON 97330

For sale by the Superintendent of Docurnents, U.S. Government Printing Office
Washington, D.C. 20402 - Price 65 cents


RESEARCH REPORTING SERIES

Research reports of the Office of Research .and
Monitoring, Environmental Protection Agency, have
been grouped into five series. These five broad
categories were. established to facilitate further
development and application of environmental
technology. Elimination of traditional grouping
was consciously planned to foster technology
transfer and a maximum interface in related
fields. The five series are:

1. Environmental Health Effects Research
2. Environmental Protection Technology
3. Ecological Research

4. Environmental Monitoring

5. Socioeconomic Environmental Studies

This report has been assigned to the ECOLOGICAL
RESEARCH series. This series describes research
on the effects of pollution on humans, plant and
animal species, and materials. Problems are
assessed for their long- and short-term
influences. Investigations include formaticn,
transport, and pathway studies to determine the
fate of pollutants and their effects. This work
provides the technical basis for setting standards
to minimize undesirable changes in living
organisms in the aquatic, terrestrial and
atmospheric environments.

EPA REVIEW NOTICE

The Office of Research and Development has reviewed this
report and approved its publication. Mention of trade names
or commercial products does not constitute endorsement or
recommendation for use.


REFERENCES

Katz, Morris and A. W. McCallum. “Effect of Sulphur Dioxide on
Vegetation," Ottawa. National Research Council of Canada, 1939.
Chapter IV, pp. 104-30.

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.


Table 3
Sulfur Dioxide Concentrations that will Produce
Threshold Injury to Intermediate Susceptible Plants
For Short-Term Exposures.

Time

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)

il