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DISCLAIMER
This report has been reviewed by the Environmental Sciences Research
Laboratory, U.S. Environmental Protection Agency, and approved for publica-
tion. Approval does not signify that the contents necessarily reflect the
views and policies of the U.S. Environmental Protection Agency, nor does
mention of trade names or commercial products constitute endorsement or
recommendation for use.
ii
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ABSTRACT
Photolysis of nitrogen dioxide is the major reaction resulting in the
formation of ozone in the troposphere. Under ambient conditions, k , the
rate constant for the photodissociation of NO , is a function of solar
altitude and cloud cover and, therefore, is highly variable.
The objective of this study was to collect k , radiometric, and se-
lected meteorological data over periods of several days under a variety of
meteorological conditions. Data were collected during the spring and fall
of 1975. Eight days of data were collected between 21 April and 30 April.
The time resolution of these data was 10 minutes for 6 days and 5 minutes
for the remaining 2 days. Between 3 October and 31 October, 13 days of data
were collected with 1-minute time resolution. Data from this study are
needed to aid the modeling of tropospheric photochemical air quality and
smog chamber results.
This report was submitted in fulfillment of Task C of Contract No.
68-02-2258 by the Research Triangle Institute under the sponsorship of the
U.S. Environmental Protection Agency. This report covers a period from
June 30, 1975, to June 30, 1977, and work was completed as of July 31,
1977.
iii
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IV
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CONTENTS
Abstract iii
Figures vi
Tables vi
Acknowledgments vii
1. Introduction 1
Background 1
Objectives 1
2. Summary and Recommendations 2
3. Experimental 5
Description of the k1 Device 5
Radiometric Instruments 10
Temperature 12
Meteorological Observations 12
Measurement Program 13
Site Description 13
Data Acquisition 15
Procedure 15
4. Results 17
Data 17
Error Analysis 19
References 21
Appendixes 22
A. April 1975 k and Radiometric Data 23
B. April 1975 Local Climatological Data 41
C. October 1975 k and Radiometric Data 45
D. October 1975 Local Climatological Data 181
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FIGURES
Number Page
1 Flow diagram of 1-liter quartz globe CSTR for nitrogen
dioxide photolysis rate measurements 6
2 General layout of the data collection site in Research
Triangle Park, North Carolina 14
TABLES
1 Summary of Input Data 11
2 Characteristics of Radiometric Instruments 12
3 Summary of Measurement Program 13
4 Summary of Environmental Data 18
vi
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ACKNOWLEDGMENTS
This project was conducted by the Research Triangle Institute under
Task C of Contract Number 68-02-2258 for the U.S. Environmental Protection
Agency. The support of this agency is gratefully acknowledged as is the
advice and guidance of the EPA personnel who contributed to the project:
Dr. J. J. Bufalini who served as Project Officer, and Drs. Basil Dimitriades
and Ken Demerjian who initiated the project. The helpful and cooperative
discussions with Dr. Ken Demerjian, Dr. Jim Peterson, Mr. John Rudisill, and
Mr. Ken Schere are also appreciated.
Many people at the Research Triangle Institute contributed substan-
tially to this project. Mr. Cliff Decker was Laboratory Supervisor for the
project. Mr. Dennis Ewald, Mr. Dave Dayton, and Mr. Bob Murdoch conducted
the day-to-day measurements in the mobile laboratories. Mrs. Sandra Burt,
Mrs. Debbie Miles, and Mr. Jerry Smith were instrumental in transferring the
collected data into computer-compatible format.
We gratefully acknowledge these individuals for their efforts in bring-
ing this project to a successful conclusion.
VII
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SECTION 1
INTRODUCTION
BACKGROUND
The photolysis of nitrogen dioxide (N0?) is considered to be the pri-
mary stimulus to chemical change for photochemical air pollution systems.
It is the major, if not the only, reaction resulting in the tropospheric
formation of ozone. The rate constant for the photodissociation of N0_ is
usually represented as "ka for NO " or simply as "k". Continuous k data
are needed to aid the interpretation of photochemical air quality data and
as input for computer models of smog chamber results.
Under ambient conditions, k1 is not constant. It is a function of the
sun's position in the sky and thus is dependent on time of day, season of
year, and geographical location. Variable atmospheric conditions, such as
cloud cover and aerosol loading, influence ambient sunlight intensity and
thereby preclude the accurate prediction of k over the sunlit portion of
the day. Although continuous radiometric instrumentation is available for
determining both ultraviolet (UV) and total solar radiation (TSR), relation-
ships between measurements with these instruments and chemically meaningful
light intensity are not well established.
OBJECTIVES
A device has been developed by Sickles and Jeffries1 to monitor k , the
rate constant for the photodissociation of N0?. The purpose of the task
described in the present document was to collect 21 days of ambient k data
using the technique of Sickles and Jeffries.1 Each day's measurements were
to be collected from sunup until sundown. In addition to the k data,
radiometric data and meteorological conditions were also to be recorded.
The scope of this task was limited to data collection; the analysis and
interpretation of the results are, therefore, deferred to future studies.
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SECTION 2
SUMMARY AND RECOMMENDATIONS
The objective of this study was to collect several days of ambient k ,
radiometric, and selected meteorological data under a variety of meteorolog-
ical conditions.
A total of 21 days of data was collected during spring and fall
measurement periods in 1975. Eight days of data were collected between 21
April and 30 April. The time resolution of this data was 10 min for 6 days
and 5 min for the remaining 2 days. Between 3 October and 31 October, 13
days of data were collected with 1-min time resolution.
The estimated precision of the k determinations in the present study
is +8 percent. This can be improved substantially by improving the preci-
sion of gas flow rate control. It is suggested that mass flow controllers
could satisfy this requirement. This approach should be considered in
future k measurement programs that employ the technique used in the present
study.
The data from this study are needed for two reasons:
1. To provide much-needed kinetic information to modelers of
polluted atmospheres and smog chambers.
2. To provide a data base for correlating ambient k measure-
ments with solar radiation data as determined by conventional
radiometric instrumentation.
It is recommended that the data compiled in this study be analyzed in de-
tail. Correlations of k and radiometer data should be made. Such analyses
would allow future and historical radiometric data to be applied directly in
airshed modeling.
The following recommended approach would involve statistical analyses
of data collected over different time scales.
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1. The data should be stratified into hourly and daily data sets.
Regressions should be compared for each hour of every measurement
day. These should also be compared with overall regressions for
each corresponding measurement day.
2. Day-to-day comparisons of k1 data should be made to examine the
effects of local weather conditions such as clear versus overcast
sky conditions. Other atmospheric factors that may change con-
siderably from day to day include ozone column, water vapor con-
centration, and haze or particulate loading. The influence of
these factors on ambient k data should be explored.
3. The data from the spring and fall measurement periods should be
compared. From this analysis, trends indicative of seasonal
behavior may become apparent. In addition, overall regressions
for the measurement period should be compiled.
In addition to analyzing and interpreting the data collected in the
present study, it is recommended that a more extensive measurement program
be undertaken. Such an effort would have two major goals: to develop an
extensive data base at a single ground station and to measure the dependence
of k on vertical altitude. The first phase of the program would require
collecting and archiving k , radiometer, and meteorological data at a single
ground station over at least a 1-yr period. This effort would establish a
sufficient data base for statistical analyses. Not only could the types of
statistical data analyses suggested previously be conducted, but additional
tests to isolate seasonal effects could be performed as well.
The second phase of the program would require mounting the k1 device on
an aircraft and collecting actinic flux data as determined by this chemical
actinometer at altitudes up to 10 km. Atmospheric aerosols contribute sig-
nificantly to the optical thickness of the atmosphere. This is particularly
evident near the earth's surface where these aerosols are highly concen-
trated. It has been suggested recently from model predictions that this
phenomena may be responsible for a marked increase in actinic flux with
altitude through the lowest few kilometers of the atmosphere.2 These pre-
dictions suggest that the actinic flux at 1 km may be 20 to 60 percent
larger than that at the surface of the earth. This should be verified by a
field program employing an airborne measurement platform.
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An alternate approach might employ ground stations located on a moun-
tain top and in a nearby valley. Although this approach may not address the
question at hand as specifically as the airborne program, it would be sim-
pler to implement.
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SECTION 3
EXPERIMENTAL
DESCRIPTION OF THE kj DEVICE
This subsection describes the operation of each of the two k devices
employed in this study. For more details concerning the theoretical devel-
opment of the technique, the original paper1 should be consulted.
Apparatus
A schematic of the k device and gas delivery system is presented in
Figure 1. A stream of approximately 37 ppm NO- in nitrogen was blended with
a nitrogen stream to yield a nominal concentration of 1.5 ppm. Commercially
prepared cylinders of N02 in nitrogen (Scott) and oxygen-free nitrogen
(Matheson) were used. The NO^-N^ delivery system consisted of the following
hardware: gas cylinders, dual-stage stainless steel diaphragm pressure
regulators, stainless steel precision needle valves, Teflon mixing tees, and
3.2-mm ID Teflon tubing. Forty-five-meter lengths of 2.5-cm ID black PVC
tubing were employed as light-shielded umbilical cords. Each cord contained
the 3.2-mm Teflon feed and effluent lines. The umbilical cord served to
connect its flask with the remainder of the gas delivery system and the NO
analyzer that were housed in a mobile laboratory. A nominal flow rate of
1 liter/min was maintained. This corresponds to a 20-s residence time from
the flask to the NO analyzer. Flow rate from the effluent line was meas-
ured periodically with a wet test meter.
Nitrogen Oxides Analyzer
Two Bendix Model 8101-B Oxides of Nitrogen Analyzers were employed in
the study. A separate instrument was used to monitor the NO and NO,, concen-
trations from the effluent lines of each of the two k devices. The prin-
ciple of operation employs the chemiluminescent gas-phase reaction between
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hv
Quartz Globe
Volume -1 Liter
To Second
Device
Teflon
Mixing
Needle Tee
Valves
To Second
Device
Needle
Valves
0-Ringsģ
X.
Plug*
Ģ
5 ppm NOo
;
s
s
1*1
-
s
s
&
*
~1000 cc/min
3.2 mm ID
Teflon Tubing
-1000 cc/min
"150 cc/min
l
NO
X
Analyzer
Waste
Figure 1. Flow diagram of 1-liter quartz globe CSTR for nitrogen
dioxide photolysis rate measurement.
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NO and 0-. Two modes of operation are required to determine both [NO] and
[NO ]. Nitric oxide concentration is determined first using the reaction
between NO and 0_. The determination of [N02], however, requires catalytic
reduction of NO to NO prior to the reaction of NO with ozone. After re-
duction of NO to NO, the signal from the total NO in the sample is taken to
be the NO concentration. Electronic subtraction of the original NO signal
X
from the NO signal gives the NO- concentration. In the normal "NO-NO -NO '
X ^ X 2.
mode, the instrument operates on a 1-min cycle: N0Ģ and NO concentrations
^ A
are updated at the end of the first 30-s interval and the NO concentration
is updated at the end of the second 30-s interval. Continued exposure to
high concentrations of NO- such as that from the k device causes the per-
formance of the reducing catalyst to deteriorate. The instrument was,
therefore, operated primarily in the "NO only" mode. Brief operation in the
"NO-NO -NO " mode once every 3 to 6 h verified the constancy of the NO
X ^ X
concentration from the k device and thus allowed determination of the NO.
concentration at any time by a mass balance calculation. The analyzer was
operated on a range of 0 to 2 ppm with a minimum detectable concentration of
0.005 ppm.
A mixture of NO- in nitrogen was fed to a spherical quartz continuous
stirred tank reactor (CSTR) of volume, V, where light of the appropriate
wavelengths caused the NO to photodissociate. The measured flow rate (Q)
and NO and NO concentration levels in both the CSTR feed and effluent
streams may then be transformed by Equation 1 to a k value. Equation 1
applies for constant temperature conditions only.
A [NO ] r [NO] + A [NO ]
k =
1 .2T[N00] |x 1 2 [N02]
-.
J
where
A[NO ] = decrease in [N00] due to reaction = [NO,] - [NO-]
^- -i- *~ O Ŗ.
[NO-] = concentration of N02 in the feed stream
[NO-] = concentration of NO- in the effluent stream
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[NO] = concentration of NO in the feed stream
[NO] = concentration of NO in the effluent stream
T = residence time in the reactor = V/Q
(Note that if flow rate is measured at laboratory
temperature (298°K) and the reactor is at a dif-
ferent temperature (T°K) , then the temperature
correction factor (298/T) must be applied to cor-
rect the residence time)
V = flask volume
Q = flow rate
R = ratio k1 [M]/k" for the following two reactions:
0 + NO + M --* NO + M
k' = 1.0 x 10 cm molec sec
NO + 0
k" = 9.1 x 10 cm molec sec
Both k' and k" are reported to be independent of
temperature.3 The temperature dependency of the
19
third body concentration ([M] = [N ] = 2.463 x 10
-3
molec cm at 298°K) may be incorporated into the
following expression for the dimensionless ratio, R.. ;
RI = 80.664/T
Note that at 298°K, RX = 0.27.
ratio k"'[M]/k"
0 + NO + M*-N02 + M
,iii in i/v-33 940/T 6 . -2 -1
k = 4.2 x 10 e cm molec sec
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The temperature dependency of both the third body
concentration and k"' may be incorporated into the
following expression for the dimensionless ratio,
R2' = 3.3879 940/T
K2 T e
Note that at 298°K, RŖ = 0.27.
A mass balance on nitrogen oxides (NO ) for the CSTR may be written.
[NO]Q + [N02]Q = [NO] + [N02] = [NO ] = constant
This expression may be combined with Equation 1 to arrive at Equation 2.
Equations 1 and 2 apply only for constant temperature conditions.
([NO] - [NO] )
(2)
- r -,
°_ i + R + R [NOJ
2x([NO ] - [NO]) r + Kl + K2 [NO ] - [NO]
X Lģ X J
Equation 3 may be derived for variable temperature conditions by substitut-
ing the temperature-dependent expressions for R and R and the temperature-
corrected expression for t into Equation 2. Equation 3 is the formula used
in this study to calculate k .
([NO] [NO]J , , 8Q.664 3.3879 940/T [N0]
' rpi "T" _ G r---. ^
Q
k =
l 2T([NO ] - [NO])
x
298
- [NO]
"I
J
Calculations
Raw nitrogen oxides concentration data for both the spring and the fall
measurement periods were corrected by applying the appropriate span and zero
correction factors. The other input data that are required for the calcu-
lation of k were assumed to be constant for each measurement day: flask
volume, initial NO concentration, volumetric flow rate, and total NO con-
centration. The flask volume is constant. The [NO] was generally small:
between 0.00 and 0.02 ppm. Mean values of Q and [NO ] were determined for
A
each measurement day. Relative percent variations (%RV), i.e., percentage
of the average constituting the range, were also calculated for Q and [NO ].
The required input data (V, [NO] , Q, and [NO ]) for each measurement day
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are presented in Table 1 along with %RV for Q and [NO ]. Relative vari-
ations were generally less than 7 percent.
For both measurement periods, ambient air temperature data were assumed
to be representative of flask effluent conditions and were employed in the
k computing formula, Equation 3. In the event, of missing temperature data,
default temperatures interpolated from the 3-h data collected at the Raleigh
Durham Airport (RDU)4 were employed.
RADIOMETRIC INSTRUMENTS
Radiometric instruments were provided by the EPA Division of Meteorol-
ogy. These instruments were positioned on an 8-m-tall wooden platform.
Data from four radiometers were collected during both the spring and fall
measurement periods. The operating characteristics of these four instru-
ments are summarized in Table 2. The following paragraphs provide a brief
description of each instrument. A more complete description of each instru-
ment is presented by Coulson.5
The Eppley Precision Spectral Pyranometer is used to measure total
solar radiation and can also be used with various Schott optical filters to
measure ultraviolet radiation and solar radiation in selected spectral
bands. The sensing element is a thermopile of copper electroplated on
constantan wire over one-half of each turn of a wire-wound thermopile.
In this study two such devices were employed: one with a 295-nm filter
(TSR) and one with a 395-nm filter (395). Total solar radiation was deter-
mined by the first device using a clear WG7 Schott filter. The second
device employed a Schott GG 395 filter for the determination of light inten-
sity at wavelengths longer than 395 nm. Although the difference between the
TSR and 395 outputs was not calculated in the present study, this value
should correspond closely to that of the ultraviolet sensor.
The Eppley Ultraviolet Radiometer (UV) is designed to measure global
flux in the near ultraviolet region (295-385 nm). The sensing element for
this device is a Weston selenium barrier-layer photoelectric cell.
The Eppley Normal Incidence Pyrheliometer (NIP) is used to measure di-
rect solar radiation. The sensing element is a fast response wire-wound
plated (copper-constantan) multifunction thermopile with a 9-mm-diameter
10
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TABLE 1. SUMMARY OF INPUT DATA
Lunar
date
4-21-75
4-22-75
4-23-75
4-25-75
4-27-75
4-28-75
4-29-75
4-30-75
10-10-75
10-12-75
10-14-75
10-16-75
10-20-75
10-22-75
10-23-75
10-24-75
10-27-75
10-28-75
10-29-75
10-30-75
10-31-75
Julian
date
111
112
113
115
117
118
119
120
283
285
287
289
293
295
296
297
300
301
302
303
304
va
(cm3)
1174
1174
1174
1174
1174
1174
1174
1174
1185
1185
1185
1185
1185
1185
1185
1185
1185
1185
1185
1185
1185
[N0]o
ppm
0.012
0.014
0.010
0.011
0.005
0.011
0.011
0.015
0.004
0.000
0.000
0.002
0.000
0.002
0.000
0.002
0.006
0.020
0.004
0.012
0.015
(cm3 min )
886
887
902
897
900
915
898
922
1005
1026
1027
1053
1094
1117
1131
1129
1126
1122
1104
1116
1105
%RVC
2.9
2.3
0.6
1.2
0.3
0.7
1.3
3.2
1.6
5.7
2.7
3.1
6.3
3.3
7.1
3.6
3.2
3.0
5.5
3.0
3.9
[NO ]d
X
1.707
1.646
1.490
1.586
1.520
1.474
1.233
1.228
1.064
1.032
1.033
1.024
0.969
0.898
0.914
0.969
0.885
0.874
0.887
0.952
0.869
%RVe
1.3
2.6
1.1
1.2
3.0
2.0
0.3
7.2
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
Volume of flask.
Mean value of flow rate over measurement day.
"Relative percent variation for Q, i.e., [(range x 100) -r mean].
Mean value of [NO ] over measurement day.
X
rģ
"Relative percent variation for [NO ]; ND = not determined.
X
11
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TABLE 2. CHARACTERISTICS OF RADIO-METRIC INSTRUMENTS
Designation
Manufacturer
Model
Operating principle
Range , W m
Sensitivity,
mV/(W m"2)
Response time, s
TSR
Eppley
Precision
Spectral
Pyranometer
Thermopile
0-2800
9
1
395
Eppley
Precision
Spectral
Pyranometer
Thermopile
0-2800
9
1
UV
Eppley
Ultraviolet
Radiometer
Photoelectric
cell
0-70
150
ID'3
NIP
Eppley
Normal
Incidence
Pyrheliometer
Thermopile
0-2800
8
1
1 Langley = 1 cal cm
700 W m
-2
receiver coated with Parsons optical black lacquer. The instrument was
attached to an electrically driven equatorial mount for solar tracking.
TEMPERATURE
An ambient air temperature monitoring instrument was provided by EPA.
Air temperature was determined by a thermistor located in a Gill Aspirated
Temperature-Radiation Shield. Measurement errors are within +0.05° C.
Ambient air temperature data are reported for both the spring and the fall
measurement periods.
METEOROLOGICAL OBSERVATIONS
The meteorological conditions for the measurement days are charac-
terized by such data as cloud cover, visibility, temperature, and relative
humidity. These and additional environmental data are collected by the
National Weather Service at RDU.4 The measurement site for the present
study is located within 8 km of RDU. Meteorological conditions at RDU are
considered to be generally representative of those existing at the measure-
ment site and therefore are reported in this study.
12
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MEASUREMENT PROGRAM
Data were collected during the spring (April) and again during the fall
(October) of 1975. The types of measurements that were conducted during each
period are summarized in Table 3.
SITE DESCRIPTION
Data were collected near a building on Davis Drive in Research Triangle
Park, North Carolina, which houses part of the EPA Division of Meteorology.
The general layout of the site is illustrated in Figure 2.
Two instruments were employed in this study to measure k . One of these
devices designated as "Flask A" or the "Platform Flask" was normally located
on an 8-m-tall wooden platform that also supported a battery of radiometric
TABLE 3. SUMMARY OF MEASUREMENT PROGRAM
NO, N02, N0x (Flask A)C
NO, NO NO (Flask B)
^_ X
TSR
395
uv
NIP
Ambient temperature
Meteorological conditions
Spring 19753
V
d
V
V
V
V
"V
d
Fall 1975b
d
V
J
V
V
V
V
^
Measurement period April 21-30, 1975; note that time resolution was
usually once per 10 minutes.
Measurement period October 3-31, 1975; note that time resolution was
once per minute.
For k determinations.
Data from this instrument were invalidated due to NO instrument drift
x
and anomalous behavior.
Meteorological conditions were reported for each measurement period by the
U.S. Weather Service at the Raleigh-Durham Airport.4
13
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DAVIS DRIVE
EPA
Building
(5 m Tall)
60
40 m
Flask A
8m Tall
Platform
Umbilical
Cord
^-Ģ Flask B
8 m r~l-
< >l h<2Qm
\
Mobile
Laboratory
55m
Parking
Lot
= N
Trees
(12 m Tall)
Figure 2. General layout of the data collection site in
Research Triangle Park, North Carolina.
14
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sensors. This flask was positioned at the center of a flat, 1.5 m x 1.5 m
square surface that had been painted with optical black paint. This config-
uration was chosen to limit the view angle of the k sensor to the skyward
hemisphere by blocking reflected light from the earth's surface.
The second of these devices, designated as "Flask B" or the "Tower
Flask" was suspended by a 2.5-cm-diameter pipe over a grassy area. The view
angle of this flask was essentially 360°. The nearest obstruction was
approximately 20 m from the device.
DATA ACQUISITION
During the spring measurement period, the nitrogen oxides concen-
trations determined by instruments housed in a mobile laboratory were re-
corded on strip charts (see Figure 2). Subsequently, these records were
manually reduced into the form of 1-min average values at 10-min intervals
for each measurement day. This 10-min NO data set was then computerized.
Instantaneous radiometric and ambient air temperature data were ac-
quired at 1-min intervals by a Digitem automatic data acquisition system.
This data system was maintained by the EPA Division of Meteorology for the
purpose of archiving local environmental data. The 1-min radiometric and
temperature data were computerized and then machine-sorted. Data collected
at the same time as the NO data were retained. The NO data and the cor-
x x
responding radiometric and temperature data were then merged into a single
computerized raw data set for the spring period.
During the fall measurement period, all the raw data (nitrogen oxides
concentration, radiometric, and temperature data) were acquired by the EPA
data system at 1-min intervals over each measurement day. Backup strip
chart records were also maintained for nitrogen oxides concentrations and
radiometric data. The 1-min data were subsequently computerized into a raw
data set for the fall period.
PROCEDURE
Zero and span settings of the NO analyzers were adjusted prior to dawn
A
or on the evening before a measurement day. Calibrations for NO and NO
A
were established by dilution of a certified cylinder of NO in nitrogen.
Calibration for NO- was performed by using the NO. produced from the gas-
15
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phase titration of known NO concentrations with CL from a calibrated ozone
3
generator.
Nitrogen and NO flow rates to each flask were adjusted to the nominal
target values prior to dawn. Initial concentrations of NO, N02, and NO
were recorded, and the effluent flow rates were determined with a wet test
meter. To prevent deterioration of the NO -reducing catalyst, the NO
4u "
analyzers were operated primarily in the "NO only" mode. Both radiometric
and NO concentration data were acquired either on strip charts or by an
automatic data acquisition system. The instruments then remained essen-
tially unattended for 3- to 6-h intervals. Between these intervals, flow
rates were measured and the NO analyzers were operated in the "NO-NO -NO "
mode. These periodic determinations were performed to assess the vari-
ability of the flow rates and the NO concentrations from each flask.
During the early morning hours, dew appeared on the surface of the
flasks. The flask surfaces were manually wiped during this period. Time
records of the flow checks and condensate removal activities were main-
tained, and data for these periods were invalidated and removed from the
final data set.
During the spring measurement period, the position of Flask A was not
fixed from day to day; whereas Flask B remained in a fixed location during
both measurement periods (see Figure 2). On 21 April and throughout the
morning of 22 April, both flasks were suspended at a height of approximately
3 m above a grassy area. At 1310 EST on 22 April, Flask A was repositioned
at approximately 2 cm above the grassy area. Flask A remained at this
location until it was moved to the 8-m wooden platform at 1450 EST on 24
April. Flask A remained on the platform for the remainder of the spring
measurement period and throughout the fall measurement period.
Flask B remained in a more or less fixed location during both measure-
ment periods (see Figure 2). From 21 April through 28 April, it was sus-
pended at a height of approximately 3 m above a grassy area. The height was
increased to approximately 8 m at 1645 EST on the afternoon of 28 April.
Data were collected on 29 April, 30 April, and throughout the fall measure-
ment period with Flask B at 8 m above a grassy field.
16
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SECTION 4
RESULTS
DATA
Eight days of k data were collected using Flask A during the spring
measurement period, and 13 days of data were collected using Flask B during
the fall period. The environmental conditions that existed on each day of
the measurement program are summarized in Table 4. The measurement day is
identified in the first column. The percent of possible minutes of direct
sunshine (%SS) and the percent of sky cover (%SC) are listed in the next two
columns.4 Total atmospheric ozone concentration determined at Wallops
Island, Virginia, and at Nashville, Tennessee,6 are listed in the next two
columns. Selected meteorological observations at RDU4 such as daily maximum
temperature, daily minimum temperature, daily mean dew point temperatures,
and comments on the prevailing meteorological conditions complete the table.
The [NO] and k data for Flask A and temperature and solar radiation
data are compiled in Appendix A for each day of the spring measurement
period. Note that these data are tabulated at 10-min intervals for each
measurement day except 4-23-75 and 4-27-75, and 5-min data are provided for
these days. Local climatological data for April 1975 are presented in
Appendix B.
Data for the fall measurement period are tabulated at 1-min intervals
in Appendix C. The values presented in this appendix are [NO] and k data
for Flask B and temperature and solar radiation data. Local climatological
data for October 1975 are presented in Appendix D.
The tabulated [NO] and temperature data may be used with the input data
listed in Table 1 to verify the k.. values in Appendixes A and C. As noted
in a previous section, Equation 3 is the formula used to calculate the k
data that are tabulated in Appendixes A and C.
17
-------
TABLE 4. SUMMARY OF ENVIRONMENTAL DATA
Lunar
Date
4-21-75
4-22-75
4-23-75
4-25-75
4-27-75
4-28-75
4-29-75
4-30-75
10-10-75
10-12-75
10-14-75
10-16-75
10-20-75
10-22-75
10-23-75
10-24-75
10-27-75
10-28-75
10-29-75
10-30-75
10-31-75
Julian
Date
111
112
113
115
117
118
119
120
283
285
287
289
293
295
296
297
300
301
302
303
304
%ssa
100
98
78
63
94
3
30
0
46
100
93
75
96
99
100
42
51
46
4
85
97
%scb
0
10
80
100
50
100
100
100
80
0
10
70
20
0
0
70
70
80
100
20
40
°3C
382
380
355
337
392
363
293
306
292
282
291
295
296
287
272
254
269
306
291
°3d
364
349
341
341
342
295
291
285
293
294
292
282
266
260
309
298
290
T e
max
19
23
26
28
23
18
22
15
24
23
30
28
19
27
27
23
23
23
23
16
13
T . f
mm
3
2
11
16
9
12
12
12
14
10
12
17
4
8
7
9
12
13
11
4
0
rn 8
DP
-1
3
11
17
5
13
14
12
14
11
14
17
4
8
8
13
9
13
12
3
-3
Comments
Clear
Clear
Partly cloudy
Partly cloudy
Partly cloudy
Rain, fog
Fog, haze
Fog, drizzle, haze
Fog, haze
Clear
Ground fog, clear
Ground fog, haze
Ground fog, clear
Ground fog, clear
Ground fog, clear
Ground fog, haze
Partly cloudy
Fog, haze
Ground fog, haze
Partly cloudy
Partly cloudy
%SS = percent of possible minutes of direct sunshine.4
%SC = percent of sky cover.4
Ozone column in 10 STP cm measured at Wallops Island, Virginia.6
Ozone column measured at Nashville, Tennessee.6
T = maximum daily temperature, °C.4
Ŗ max 3 *
T . = minimum daily temperature, °C.4
Tnp = daily mean dew point temperature, °C.4
18
-------
Two points should be considered prior to extensive data analysis and
interpretation.
1. The spring [NO ] data were reduced manually from strip chart
records. The subjective nature of this procedure may introduce
some inconsistencies on comparison of the spring data with the
more objective, machine-acquired fall data.
2. The nominal response time of the k.. device was over a minute.
Radiometric instruments have response times of approximately 1 s.
This difference in response times should be considered if precise
comparisons are to be made between k and radiometric data.
ERROR ANALYSIS
Several factors can introduce errors into the determination of k by
the technique employed in this study. These factors include errors in rate
constant ratios, nonideal mixing, temperature variation, rapidly changing
light intensity, reaction in the effluent line, and measurement error. A
complete discussion of sources of error including an error propagation
analysis for Equation 1 has been presented by Sickles and Jeffries.1 With
the exception of measurement error, the previously listed factors are
thought to be of minor importance in determining the precision of the k..
measurement.
Under the assumption of constant temperature and fixed values of R and
R , errors enter into Equation 2 in the measurement of residence time and
nitrogen oxides concentrations. The residence time is subject to variations
in flow rate. Nitrogen oxides concentrations themselves may vary with
variations in flow rate from the gas delivery system. The concentratons
indicated by the NO instrument are subject to instrumental span and zero
drift and to deterioration of the NO converter. The relative percent
variations presented in Table 1 suggest that +2 percent is a reasonable
estimate of 95 percent error limits for t, [NO] , [NO], and [NO ].
An error propagation analysis similar to that presented by Sickles and
Jeffries1 was performed using the +2 percent estimates noted above. Based
on this analysis, estimated 95 percent confidence limits on the precision of
k determinations in this study are +8.8 percent for a k1 of 0.50 min and
-1
+5.7 percent for a k of 0.10 min . It is suggested that these limits can
19
-------
be improved by at least a factor of two by modifying the technique to insure
more nearly constant flow rates from the N~ and N0_ cylinders. Mass flow
controllers could satisfy this requirement while simultaneously providing
continuous records of flow rates for mass balance verification purposes.
20
-------
REFERENCES
1. Sickles, J. E., II, and H. E. Jeffries. 1975. Development and Operation
of a Device for the Continuous Measurement of k for Nitrogen Dioxide.
Publication No. 396. Department of Environmental Sciences and Engineering,
University of North Carolina, Chapel Hill, North Carolina.
2. Peterson, J. T. 1976. Calculated Actinic Fluxes (290-700 nm) for Air
Pollution Photochemistry Applications. EPA 600/4-76-025, Environmental
Protection Agency.
3. Hampson, R. F., Jr., and D. Garvin, eds. 1975. Chemical Kinetics and
Photochemical Data for Modeling Atmospheric Chemistry. NBS Technical
Note 866.
4. Local Climatological Data: National Weather Service Forecast Office,
Raleigh-Durham Airport. U.S. Department of Commerce, National Climatic
Center, Asheville, North Carolina.
5. Coulson, K. L. 1975. Solar and Terrestrial Radiation Methods and Measure-
ments. Academic Press, New York.
6. Ozone Data for the World. 1975. Atmospheric Environment Service Publica-
tion, 16. Downsview, Ontario, Canada.
21
-------
APPENDIX A
APRIL 1975 k AND RADIOMETRIC DATA
23
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APPENDIX B
APRIL 1975 LOCAL CLIMATOLOGICAL DATA
41
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42
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OBSERVRTIONS RT 3-HOUR INTERVRLS
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!j NOTES
s* CEIL INC CQLUHN-
22 UNL -notcn-M uiii"i'io
10
5 NCBTMtH COLUMN-
16 'OHNttUO
'* Q SOLIflLL
10 " " 1N
flH R IN SHOMEHS
7 S 5 OH
6 ^P 5 OH PŖn.E f5
* 1C I E Cģ*b'fU S
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IP 1 E PELLF'S
H H lL
3 f f C
6 P f E 00
5 OF C 3U 0 FOC
fl BS 8 OH NO 5NOH
s E"
1 1
,, WIND COLUMNS-
e
J6 01 EC ION5 flu? fwgsr f H0n
8 LH EO IN TENS 0(= 5EGBEES
FR M TRut SOUTH; ] f . 09
^ CflfSCRLM
;j 5u!M*'n!7"Ŗ?D!?o!!Ģi
13 TO M- r-. PER HQUģ
10
10
0
0
9
2
3
5
0
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8
5
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4
9
Ģ!CĢOHL1. HICROHCHE. 0ģ Kģ*E* COPIES OF THf 0*]QJNflL ģFCO*05. (WOuIIJES 13 '0
flVfllLBB HIT OHO C0513 SNOLKD flt HOQUESStO '0Ģ D1KECTQH. NflMONflL CUfHlIC CFNTEK.
'EDEKfli BUILDING. Ģsncv!Ltf. NOKTH CHRQLINR zBBoi
Stfll ION. RAIf tGH N i 1( HO 1 MONTH) 76 04
43
-------
APPENDIX C
OCTOBER 1975 ]a AND RADIOMETRIC DATA
45
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179
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APPENDIX D
OCTOBER 1975 LOCAL CLIMATOLOGICAL DATA
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OBSERVRTIONS RT 3-HOUR INTERVRLS
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183
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TECHNICAL REPORT DAI ^
(Please read Instructions on the reverse before completing)
1 REPORT NO.
EPA-600/7-78-053
3. RECIPIENT'S ACCESSION"NO.
4. TITLE AND SUBTITLE
NITROGEN DIOXIDE PHOTOLYTIC, RADIOMETRIC, AND
METEROLOGICAL FIELD DATA
5. REPORT DATE
March 1978
6. PERFORMING ORGANIZATION CODE
7 AUTHOR(S)
J.E. Sickles, II, L.A. Ripperton, W.C. Eaton, and
R.S. Wright
8. PERFORMING ORGANIZATION REPORT NO.
9. PERFORMING ORGANIZATION NAME AND ADDRESS
Research Triangle Institute
Research Triangle Park, North Carolina 27709
10. PROGRAM ELEMENT NO.
INE625 EA-03 (FY-77)
11. CONTRACT/GRANT NO.
Contract No. 68-02-2258
12. SPONSORING AGENCY NAME AND ADDRESS
Environmental Sciences Research Laboratory - RTP, NC
Office of Research and Development
U.S. Environmental Protection Agency
Research Triangle Park, North Carolina 27711
13. TYPE OF REPORT AND PERIOD COVERED
Final
14. SPONSORING AGENCY CODE
EPA/600/09
15. SUPPLEMENTARY NOTES
16. ABSTRACT
Photolysis of nitrogen dioxide is a major reaction resulting in the formation
of ozone in the troposphere. The rate constant, k-^, for the photodissociation of
N02 is, under ambient conditions, a function of latitude, solar zenith angle, and
cloud cover; therefore, ki_ is highly variable.
Nitrogen dioxide photolysis data for calculating k-^, and radiometric and
selected meteorological data, all under a variety of meteorological conditions,
were collected during the spring and fall, 1975. Data from this study can be used
to aid the modeling of tropospheric photochemical air quality and smog chamber
results.
17.
KEY WORDS AND DOCUMENT ANALYSIS
DESCRIPTORS
*Air pollution
*Nitrogen dioxide
*Photolysis
*Reaction kinetics
*Radiometry
*Meteorological data
Field tests
b.IDENTIFIERS/OPEN ENDED TERMS
c. COSATI Field/Group
13B
07B
07E
07D
14B
04B
18. DISTRIBUTION STATEMENT
RELEASE TO PUBLIC
19. SECURITY CLASS (This Report)
UNCLASSIFIED
21. NO. OF PAGES
20. SECURITY CLASS (Thispage)
UNCLASSIFIED
.122-
22. PRICE
EPA Form 2220-1 (9-73)
184
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