-------
TABLE 14. ATMOSPHERIC NITRATE DISTRIBUTION
Location Gaseous/Total
St. Louis, Mo. (1973) .95
West Covina, Calif. (1973) .98
Phoenix, Ariz. (1977) .50
Temple City, Calif. (1976) .75
Upland, Calif. (1976) .96
Rubidoux, Calif. (1976) .45
Beverly, Mass. (1978) .98
Remote troposphere ^.80
(above boundary layer)
56
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ANALYSIS OF AIRCRAFT DATA
Rationale
The aims of this study are to determine the rate of NO removal and the
7 x
nitrogen balance in an urban plume. In order to accomplish these goals it
is important that the urban plume not be subject to fresh emissions of NO
X
and tracer gases once it leaves the city. For this reason the Boston plume
was chosen for study.
Conceptually, as a polluted air parcel leaves the dense emission area
of the city and moves downwind, several things can happen to the nitrogen
oxides. First, NO and the other plume constituents will be diluted with
X
the surrounding air, the rate depending on the meteorological stability.
Secondly, NO can undergo transformations into reaction products. Finally,
NO (primarily NO-) can be removed by physical processes (dry deposition,
X ^
wet scavenging). We are concerned principally with the two latter processes,
the chemical and physical removal of NO from the plume, but the dilution
X
process so dominates the changes in concentration of NO within the plume
X •
that it must be carefully accounted for in order to derive information on the
slower processes. In the Boston study, we used three inert urban tracers,
carbon monoxide, acetylene and fluorocarbon-11, to track dilution of the
urban plume during downwind transport.
Referring to Figure 8 we note that the measured concentration (C ) of a
m
conserved species within the urban plume just as it leaves the city is equal
to the sum of the background concentration (C, ) and the urban input (C ).
For a plume transported over areas with minimal sources, the measured con-
centration of the species as the plume moves downwind is given by
C = C e"kt + C.
mo b
where the concentration due to the city is diluted at some rate governed by
k. As shown in Figure 8, at infinite dilution the measured concentration
will equal the background concentration.
We can now restate the above equation for a conservative tracer and for
the reactive species, NOX.
* Throughout this report NO is defined as NO + NO-,
X •£
57
-------
I Co
o
"c
4)
O
Time
FIGURE 8. TRACER CONCENTRATION WITHIN AN URBAN PLUME
58
-------
— kt
For Conservative Tracer: [Tracer] = [Tracer] e -f- [Tracer], I
mo b
For Reactive Species: [NO ] + [NO ] = [NO ] e"kt + [NO ] II
x m x xoss x o x D
Note that Equation II has a new term on the left side to account for removal
of NO , either chemically or physically, from the plume. It is this NO loss
X X
term which is the object of the analysis.
Since the tracers and NO are gases, they will dilute at the same rate,
-kt X
and the term e will be the same in both equations. We therefore rearrange
I and II, divide to remove the exponential term, and rearrange again to obtain
Equation III.
run l tTrac«*ln - tracer],, ([HO j . [HO j )
[N°x]loss - [Tracer] /[NO ] - ~ X m X b
O X O
All of the terms on the right side of Equation III are now measureable,
enabling us to determine NO loss. Operationally, the background concentra-
X
tion terms are determined by making aircraft measurements outside the plume,
the urban input ratio ([Tracer] /[NO ] ) is determined by making plume cross-
section measurements just at the downwind edge of the city (naturally back-
ground levels must.be subtracted to derive urban input terms), and the
[Tracer] and [NO ] terms are measured simultaneously during cross-sections
m x m
of the plume at successive downwind distances. Note that [NO ] , when
x m
determined by chemiluminescence, must be corrected for interferences due to
PAN and HN03<
If the first downwind measurement and successive downwind measurements
are made on the same general air parcel (i.e., a Lagrangian mode), the
calculation of NO loss is relatively straightforward. We will discuss such
X
flights as specific case studies shortly.
In a typical day's experiment, hourly meteorological data from several
eastern Massachusetts stations were obtained by telephone several times each
day and were used to manually construct working trajectories for Boston's polluted
morning air mass. These trajectories were used to define each day's flight
patterns. Data were collected during multiple traverses of the plume on
each of three or more daily flights in order to bracket the morning air
parcel, in this way, data on pollutant concentrations within the selected
air parcel were obtained from early morning to late afternoon.
At the conclusion of the field study, an important part of our data
interpretation efforts was the construction of surface level wind field grids
59
-------
from wind speed and direction data from 10 eastern Massachusetts stations.
The wind fields were used to compute forward trajectories to pinpoint the
position of the air parcel selected for study. The intended use of the
trajectories mandates a high resolution wind field grid. An air mass
trajectory computer code was modified at Battelle for this purpose. Hand
trajectories have also been drawn for selected times for comparison with the
computer-derived plots.
The aircraft data which will be used with the trajectories were
collected in such a way as to maximize the sensitivity of the experiment
for detection of transformation rates. Our earlier research on transfor-
mations in the Phoenix plume suggested that one way to improve the
experimental design would be to collect the integrated bag samples (for
PAN, C2-C5 hydrocarbons and CO) near the midpoint of the urban plume,
rather than integrating the collection across the entire plume. The
dilution of the sample which accompanies collection near the edges of the
plume results in lower measured concentrations of tracers and NO reaction
X
products. Subtraction of background values from the concentrations of the
pertinent species introduces considerable uncertainty, since two similar
numbers are being subtracted. Thus the overall accuracy and sensitivity
of the transformation analysis is impaired. Integrations across the plume
were required in previous studies because, even when trajectories were
constructed before each flight, it was never possible to predict exactly
where the highest plume concentrations would be found. Consequently a pre-
planned flight pattern was drawn with fixed sample collection coordinates.
Because of this, even when high plume concentrations were observed and
sampled during part of the collection period, the remainder of the
collection time diluted the samples.
To resolve this problem during the Boston study, we actually made
two complete passes through the Boston plume for each collection. On the
first pass, the concentrations of 0_, NO , and CNC were observed and noted
•J X
on recorders. On the return pass the bag samples were collected over the
5-10 miles of the plume where the concentrations were highest. Trajectories
were still prepared before each flight to indicate the position of the
particular air parcel we were tracking (usually the 7-8 a.m. emissions bulge)
The traverses were then preplanned to bracket the predicted position of the
60
-------
parcel. However, the collection locations and times were not prespecified
but were determined from observations during the "scouting" pass through the
plume.
In order to conserve flight time, background air measurements were
not made on every flight. The upwind concentrations of N0x and the three
tracers can be estimated from several flights for which upwind data were
collected. These upwind concentrations are given in Table 15. These
data, together with clean air results of other investigators has led to the
selection of the following values to represent clean air dilution around Boston:
NO * 0.002 ppm
X
CO * 0.17 ppm
C2H2 = 0.001 ppmC
F-ll - 129 ppt.
TABLE 15. CONCENTRATIONS FROM SEVERAL
FLIGHTS UPWIND OF BOSTON
NOX, ppm
0.003
O'.OOA
0.002
0.004
0.002
0.004
CO , ppm
0.20 .
0.35
0.17
0.33
0.17
0.33
C2H2, ppmC
0.0019
0.0030
0.0009
0.0004
0.0009
0.0004
F-ll, ppt
147
165
144
129
144
129
An example of one day's flights is included in Figure 9a-c. Each
figure represents a continuous flight; there were three flights on August 18
at progressively farther downwind distances. The bag sample and filter sample
collection points are noted in the figures. Each solid line in the figures
represents two passes through the plume. There are two plume traverses per
flight, for a total of 4 passes through the plume. The purpose of the two
traverses is to bracket the predicted position of the air parcel and thereby
minimize errors introduced by the limited data base used to predict air
parcel positions. For the transformation analysis we have used the data from
61
-------
I
as
2
oo
!•»•
ON
B -
-------
ad
SI
«
63
-------
so
fB
so
z
t
2
-------
the traverse which lies closest to the actual air parcel position. This de-
termination was based on the more accurate trajectories discussed earlier.
Case Study No. 1: August 18, 1978
August 18, 1978, was a warm, sunny, clear day in eastern Massachusetts.
The maximum ozone recorded at Beverly airport was 0.089 ppm at 1600 EDT. PAN
also reached its maximum value of 5 ppb at this time. The nitric acid concen-
tration averaged 0.84 ppb over the 8-hour daylight sampling period. Winds were
a brisk 8-10 mph from the west and northwest during much of the day, making the
day well suited for a study of urban plume reactions east of Boston over the ocean.
Figure 10 shows the calculated ocean trajectory for the Boston plume* and
the positions of our aircraft bag collections. As shown by the flight maps
in Appendix B, full traverses of the plume were conducted; Figure 10 shows the
position of bag collections along a given traverse, rather than the entire
traverse. As an example, the ozone profile from the plume traverse along
which Sample 22-2 was collected is depicted in Figure 11. The ozone concentra-
tion profile across the plume is reminiscent of ozone plumes from New Yorkd^),
Phoenix^), and St. Louis(4). xhe plume character of the profile is obvious.
The interval over which Sample 22-2 was collected is noted on the 0 pro-
file. This collection interval is represented on the flight map (Figure 10),
as a solid line labeled 22-2.
Of all the plume traverses carried out on August 18, those shown in
Figure 10 yield the best match of time and position such that a Lagrangian frame-
work is approximated. Even so, there are mismatches of up to an hour, so we
were not monitoring exactly the same air parcel throughout the day. Assuming
that the tracer/NO emissions ratios averaged over all of Boston do not change
X
rapidly over the course of an hour, then exact time and position matches are not
critical. Since the greatest fraction of the CO, C9H7, and N0_ emitted
*— *— X
in the urban center during the morning hours is from automobiles (as judged by
the CO/NOx and C2H2/NOX ratios), it is unlikely that the emissions ratios
will change substantially during an hour.**
Using Sample 20-1 to derive the urban input ratios and employing the
background air concentrations of NOX and tracers discussed earlier,- we
* The plume width is not defined by the trajectory calculation; we have
approximated the plume width and given sides to the plume in this and
subsequent figures for clarity.
** Emissions from large point sources were generally not a factor, probably
because our 500-1000 foot flight altitude was below the plume height. A
case where a power plant was observed is discussed next.
65
-------
8-18-78
10 15 20
Statute Miles
25 30
FIGURE 10. AIR PARCEL TRAJECTORY AND
AIRCRAFT SAMPLE POSITIONS FOR
18 AUGUST, 1978
66
-------
CM c
12Z 0)
O)
-------
can calculate NO deficits for Samples 21-2, 22-1, and 22-2 using Equation
X
III. The deficits are shown for the three tracers in Table 16. The data
for these calculations was given earlier in Table 10.
TABLE 16. NOX DEFICITS FOR FLIGHTS 20-22
NOX Deficit (ppm)
Based On:
Sample No.
21-2
22-1
22-2
Reaction Time*
3.0 hours
6.4 hours
6.9 hours
CO
.030
.012
.012
C2H2 F-ll
.010 .016
.010 .010
.009 .018
* Based on sample 20-1 as T = 0.
Considering the inaccuracies inherent in the analytical methods
together with inaccuracies introduced by the correction for background con-
centrations of tracers, the deficits based on acetylene and CO should be
given the greatest credence, with the value based on C2H- being slightly
favored. The F-ll values are shown merely for comparison. In most cases
the F-ll results agree with the CO and C2H_ data, but they are not con-
sidered to be as reliable.*
The nitrogen balance for the three downwind samples is shown in
Table 17. The NO deficits based on CO and C?H9 have been averaged, except
X £ sL
for Sample 21-2, where the CO-derived value appeared unreasonable.
The sum of the measured reaction products, PAN, nitric acid and
particulate nitrate account for less than, about the same as, and more than
the calculated deficit, respectively for the three samples. Considering the
low concentrations involved, the sensitivities of the analytical methods
and the uncertainties in the deficit calculation, the agreement between the
NO deficit and the measured reaction product concentration is reasonable.
* F-ll is considered a less reliable tracer because its source is different
from NOX. The initial F-11/NOX ratios of different air parcels are likely
to show more variation than ratios of constituents from the same source.
Both F-ll and CO also suffer from high background concentrations relative
to the plume concentrations. This tends to introduce uncertainty into
the Equation III calculation. Due to its much lower background and better
measurement precision, Zfii is considered the m°re reliable tracer.
68
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TABLE 17. NITROGEN BALANCE IN THE BOSTON PLUME DURING
TRANSPORT — August 18, 1978
NOX Deficit, (PAN + HON02 + NO")
Sample No. Reaction Time, hrs. [0_], ppm ppm pptn
21-2 3.0 .068 .010 .005
22-1 6.4 .125 .011 .012
22-2 6.9 .129 .011 .015
69
-------
The processes which lower the NO concentration in the air parcel
X,
include dilution, conversion to products (e.g. PAN, HONC>2, NO^) and deposi-
tion. Dilution is taken into account by the use of inert tracers, so this
discussion can focus on transformation and deposition losses. Calculation
of a rate of NO removal is not straightforward due to the complexity of the
X
chemical processes involved and the interconversion of NO and NO-. An
average rate of loss can be calculated from the NO deficits and the
X
reaction times shown in Table 16. The rate varies from .0016 to .0033
ppm hr depending on the reaction time selected.
The NO loss rate is expected to be faster or slower depending
on whether N02 or NO is the predominant oxide present. Little NO loss
is expected while NO is undergoing oxidation to NO., however, once the
interconversion is largely complete, several chemical and physical
processes will compete to remove NO.. For these reasons, the rate of NO
2 x
removal from a transported air mass is expected to be highly variable,
with an induction period likely during the initial stages of reaction as
NO is converted to N0~. In this and subsequent case studies, NO removal
/ x
kinetics will be determined by plotting the plume data in the integrated
form of the first order rate equation and using the slope to calculate a
removal rate constant (also referred to as the removal "rate" in reciprocal
hours by common usage in the field of atmospheric chemistry) .
The first order rate equation used to describe these experiments is
13
In - = kt
(N0x)t
where (NO ) is the expected concentration of NO , or the concentration
x e x.
which should be present in the air parcel at time t after dilution is
taken into account, and (NO ) is the actual amount of NO (i.e. NO + NO-)
x t x £
measured at time t. (NO ) is determined from the first term on the right
x e
side of Equation III, after correction for the background levels of tracer
and NOX in the dilution air.
For Flights 20-22 on August 18, 1978, the first order plot is
shown in Figure 12. The data conform reasonably well to the first
order form. The slope of the line yields a pseudo-first order rate
70
-------
345
Reaction Time, hours
FIGURE 12. FIRST ORDER PLOT FOR FLIGHTS 20-22,
AUGUST 18, 1978
71
-------
constant of 0.24 hr . Additional case studies will be presented shortly
in an attempt to verify both the first order fit and the removal rate.
We expect the major portion of NO removal to occur via transformation
X
to reaction products (i.e. PAN, HNO~, NCL). The rate of transformation
has been estimated above by the use of inert tracers to account for dilution.
It is also possible to calculate a conversion rate based on the change in
the distribution ratio, F , with time as the air gareel reacts during
transport. F , defined as PAN + HON02 + N03 can fee us£d
a NO + N02 + PAN + HON02 + N0§
calculate exactly the rate of conversion to products if the sum of the
measured oxidized nitrogen compounds (the denominator of F ) is conserved.
n
Since deposition processes are known to remove some of these compounds,
F can only provide an estimate of the conversion rate. We expect that
deposition losses will lower the apparent F , leading to a conversion
rate estimate which is a lower limit. However, the effect of deposition
losses on F should not be great (since the compounds most likely to be
deposited appear in both the numerator and denominator), and we therefore
expect the conversion rate estimated by F to be a reasonable approximation
of the true conversion rate. A semilog plot of F versus reaction time
for Flights 20-22 is shown in Figure 13. The slope of the line yields a
ent
-1
pseudo-first order conversion rate of 0,23 hr , in excellent agreement
with the overall NO loss rate calculated above of 0.24 hr
X
Case Study No. 2: August 23. 1978
August 23 was a cool, clear, sunny day in eastern Massachusetts.
Winds had shifted from easterly on the previous day to a steady westerly
flow. At the Beverly Airport, gaseous and aerosol pollutant concentrations
were generally low with the exception of 0,, which reached .106 ppm.
Some curvature might be expected during the early portion of the
reaction as NO is converted to N02, with little net loss of NOX.
To avoid this difficulty, our measurements were initiated after this
process was largely complete.
72
-------
NO + NOs + PAN + HNO3
FIGURE 13. SEMILOG PLOT OF Fn VS REACTION TIME
FOR FLIGHTS 20-22 ON AUGUST 18, 1978
73
-------
Four multiple-traverse flights were carried out on 23 August in an
attempt to define the rate of NO removal from the Boston plume under
2C
transport conditions. The flights were conducted over a 9 hour period
from 0900 to 1800 EDT. Unfortunately the chromatographic system for PAN
determination was not operating well during this portion of the study and
the PAN data are not reliable as a consequence. While it will not be
possible to derive nitrogen balances from these flights, the NO removal
A>
rate can be estimated from the tracer and NO data. These data may be
X
found in Table 10.
The trajectory of the morning Boston air mass is depicted in Figure 14
together with the appropriate sample positions from the flights. For the
most part the time and position matches of the air parcel location and the
aircraft sample positions are quite good. Two exceptions are Samples
29-5 and 32-3. Sample 29-5 matches very well in time; that is, it was
collected at 0955 EDT at the downwind distance where the 0800 EDT air
parcel should have been located, but the sample position in Figure 14
appears to be outside the plume to the north. However, the plume width
dimensions are drawn only for visual clarity. From the traverse data
it is clear that Sample 29-5 was actually within the plume. Sample
32-3 was collected at 1800 EDT at the 1600-1630 EDT position of the air
parcel. These times are considered to be too dissimilar for use in the
rate computations. All of the other samples shown in Figure 14 match
the air parcel position and time quite well.
August 23 was an especially good day for measurements of the type
needed here because a low inversion which formed before dawn trapped
pollutants very close to the surface. The resulting high concentrations
permitted very precise measurements. Samples 29-5, 30-1 and 30-2 all were
collected within 150 feet of the ocean surface. On the later Flights, 31
and 32, samples were obtained at altitudes of 300-500 feet.
74
-------
hJ
O.
H
(*.
U
os oo
M r-.
< 01
i— I
Q
Z •
< m
CM
><
PS H
O V5
H 3
U U
Ed en
U 2
OS O
OS 01
M O
< ft.
PS
O
75
-------
Using the high pollutant concentrations measured at 1000 EDT (Sample
29-5) to define the urban emissions ratios, the background concentration data
discussed earlier, and Equation III, one can calculate NO deficits for
X
various transport times for the 23 August Boston plume. These deficits are
listed together with reaction time in Table 18. Once again, the F-ll
.results are considered to be inferior to the CO and C^H^ data because F-ll
arises from a completely different source than NO and because of the large
X
background air correction. It is clear from the negative values in Table 18
that the NO deficits based on F-ll are completely unreliable, at least for
X
this flight. The results derived from CO and £2*12 are reasonably consistent.
The NO deficits are plotted along with ozone concentration and C-H./
C.H- ratio in Figure 15. The CO and C-H based deficits have been
averaged for this plot, except for Sample 32-2 where only the CO-based
value was used. The plot of NO deficit suggests the possibility of an
X
induction time during which NO removal is minimal. It seems likely that
* X
this induction period may be the time required to convert NO to N02- This
explanation is consistent with the build-up in 0 from .028 to .063 ppm
during the first 1-1/2 hours of reaction. After the induction period, a
rapid loss of NO is observed. After about 5 hours of reaction there is
r x
no evidence for further loss of NO , suggesting that most of the original
X
urban NO has been removed by chemical or physical processes. It is
X
noteworthy that ozone reaches its maximum concentration at 5 hours and
declines thereafter. If nearly all of the NO were consumed at this time,
X
0_ accumulation would be expected to cease and the NO deficit would
3 x
remain constant, as observed after 5 hours of reaction. The validity of this
explanation is uncertain, since the C^H./C^H,, ratio indicates that at least
some reactions which consume hydrocarbons continue after 5 hours. It may
be that nearly all of the NO has been converted to products and/or
X
deposited on the surface by the fifth hour, thereby terminating further
reaction, but without valid PAN results this can not be proven. As the
data now stand, 40-50 percent of the urban NO appears to have been lost
X
after 5 hours of reactions. This is a lower limit because we are unable
to correct the NO data for PAN interference.
x
76
-------
TABLE 18 . REACTION TIMES AND NOX DEFICITS FOR
FLIGHTS ON 23 AUGUST, 1978
Sample No.
30-1
30-2
31-1
31-2
31-3
32-2
Reaction Time,
hrs.
1.6
2.2
4.6
5.2
5.2
8.0
^ NOX Deficit Based on:
CO C?H? F-ll
(ppm) (ppm) (ppm)
-.002
.011
.016
.016
.013
.012
.003
.012
.012
.013
.010
.005
-.015
-.012
-.002
-.004
-
.006
*Using 29-5 as T = 0.
77
-------
234567
Reaction Time, hours
10
FIGURE 15. NOX DEFICIT, 03 AND C2H4/C2H2 VS REACTION
TIME FOR FLIGHTS 29-32, AUGUST 23, 1978
78
-------
The pertinent data from Flights 29-32 (Table 10) were converted to a
form suitable for graphical analysis, as described earlier on page 70.
The results have been plotted in a first order form in Figure 16. Most
of the data points fall along a straight line passing through zero. The
slope of this line yields a rate constant of 0.15 hr~ .
Loss rates on the order of .15 hr during strong photochemical
activity in an urban plume are consistent with previous studies in Los
Angeles, model estimates, and recent smog chamber data. Other
flights during this investigation also confirm that the rate can be this high
under appropriate conditions. Before turning to another such flight however,
there is a special feature of Flights 29-32 which must be mentioned.
During the flights of 23 August, several of the urban plume traverses
detected the plume from the Salem power plant. This plant is located about
5 km south of Beverly Airport, and its plume is expected to parallel the
Boston urban plume on this day.
Figure 17 shows the positions of traverses from Flights 29, 30, and 31.
*
On each of these traverses we observed both the urban plume from Boston and
the Salem power plant plume. The power plant plume was observed at 10, 25,
and 79 km downwind (east) of the plant at 1003, 1140, and 1510 EOT, respec-
tively. The concentrations of NOX, 03 and condensation nuclei recorded during
the complete traverses are also shown in Figure 17 and are keyed to the
appropriate traverse. In all three cases, both the urban and the power
station plume appear in the data. For Flight 29, the urban plume is clearly
observed in the NO plot. The location of Sample 29-5 collection is noted.
Just north of the polluted urban air, a sharp spke in the NO and condensation
X
nuclei (CN) levels and a concurrent reduction in 0- indicate the presence of
the power station plume. A similar situation is observed along the traverse
from Flight 30. Just north of the urban plume (Sample 30-1), a NO and CN
X
spike and an 0. decrease mark the plume from the Salem plant. The NO and 0_
•J X J
indicators are not as dramatic as they might be because the plane's altitude
was not eKactly matched with that of the plume. The plane was sampling at
150 feet above the ocean's surface and apparently just skimmed the underside
of the plume.
79
-------
FIGURE 16. FIRST ORDER PLOT FOR FLIGHTS 29-32,
AUGUST 23, 1978
80
-------
0 5 10 15 20 Zi 30
StutuU Miles
FIGURE 17. TRAVERSE POSITIONS AND CONTINUOUS DATA RECORDS FOR
FLIGHTS 29-31, AUGUST 23, 1978
81
-------
The traverse for Flight 31 also showed both the urban and power station
plumes. The width of the power plant plume has increased greatly as observed
from the NO and 0- signals from the 10, 25, and 79 km traverses. Under the
X j
conditions of these flights no 0_ bulges were observed; in fact there was
still an 0- deficit of ^40 ppb even after 79 km of transport. The increase
in 0, concentration in the urban plume stands out clearly from traverse to
traverse. There is some indication from the final traverse of an increase in
0- at the edges of the power plant plume, although the data are insufficient
to discuss plume fringe versus core in any detail.
The reactions and fate of nitrogen oxides in power plant plumes are at
least as uncertain as their urban plume analogs. The subject of NO reactions
X
in the plumes from electric generating plants has been treated in other
reports ' , but is still far from understood. Any information pertaining to
this subject is therefore of interest. Fortunately, the Salem plume was
sampled directly during Flight 31 at a point 79 km from the stack. This
sample (31-4) yields some interesting insights into the composition and
reactions in transported power plant plumes.
The features of the power plant plume sample can best be illuminated by
comparing it with the urban plume sample, No. 31-3, taken 20 miles to the
south. The bag and integrated flight data from Table 10 are reproduced in
Table 19. The differences between the two samples are few, as expected
from the fact that both plumes are largely diluted after 79 km of transport.
The power plant plume contains about twice as much NO as its urban
X
counterpart, and shows suppression of 0-, as mentioned earlier. Perhaps the
most significant feature is a 50 percent higher concentration of nitric acid
in the reacted power plant exhaust. The absolute PAN values are uncertain,
but based on relative peak heights there was more PAN in the power plant plume
than in the urban plume. Because of the unreliable PAN data it is not
possible to present PAN and HONO distributions and ratios in the two
plumes. This is unfortunate since such information would be very valuable.
Nevertheless, the higher concentrations of HONO and PAN are intriguing.
These findings are consistent with current smog chamber studies of
NO reactions in power plant plumes.
82
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TABLE 19. RESULTS FOR SAMPLES 31-3 AND 31-4
o3, PPb
NOX, ppb
HON02, ppb
CO, ppm
F-ll, ppt
ethane, ppbC
ethylene, ppbC
acetylene, ppbC
isobutane, ppbC
n-butane, ppbC
isopentane, ppbC
n-penetane, ppbC
Urban Plume
31-3
137
10.7
4.0
.62
-
3.6
2.7
8.0
5.7
11.8
11.7
5.3
Power Plant Plume
31-4
117
19.4
6.0
.61
242
3.9
4.9
7.8
5.0
11.0
14.6
5.8
83
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Case Study No. 3: August 30, 1978
Cool, clear sunny weather prevailed over eastern Massachusetts on
August 30, 1978. Winds were from the west and northwest during the day.
Since Beverly Airport is northeast of Boston, it was unaffected by Boston's
emissions and the pollutant levels remained relatively low throughout the
day. Maximum hourly 0- was .076 ppm, accompanied by 5 ppb of PAN. Twenty-
four hour averaged nitric acid was .64 ppb, compared to a particulate
nitrate concentration corresponding to .02 ppb. As on other days, gaseous
nitrate (PAN + MONO.) dominates the total atmospheric nitrate burden.
Weather and air quality data for 30 August have been summarized in Table 5.
Detailed ground monitoring results may be found in Appendix A.
The trajectory of the 0800 EDT Boston air mass was computed using
wind records. The air mass trajectory is depicted in Figure 18, along
with the positions of selected samples from three monitoring flights
conducted during the period from 0830 EDT to 1500 EDT. The gas phase
data from these flights is reported in Table 10; the aerosol results
are presented in Table 11. The particulate nitrate levels were very
low (<0.3yg/m-3) during all flights and showed no tendency to increase with
reaction time. The sulfate concentration varied from 4.0 to 7.2 pg/m3,
3
consistent with the 7.4 ug/m observed outside the urban plume at Beverly
Airport. The changes in SO* followed no consistent pattern.
The time and position matches for the samples shown in Figure 18 were
quite good. The greatest discrepancy involved sample 39-1, which missed the
computed air parcel position by ^45 minutes. Considering all the other
uncertainties and imponderables, even this match is acceptable. All the
others were nearly exact.
84
-------
FRAMINGHAM
0 5 10 15 20 25 30
Statute Miles
FIGURE 18. AIR PARCEL TRAJECTORY AND AIRCRAFT SAMPLE
POSITIONS FOR FLIGHTS 37-39, AUGUST 30, 1978
85
-------
Sample 37-4 was a good clean background sample and was used in deriving
the general background values used throughout the study. Sample 37-2,
collected 200 feet above the surface of the Bay at 0856 EDT will serve
to define the urban ratios of CO/NO , C,H,/NO and F-ll/NO . This sample was
X fc i X X
collected as close to the urban center as Logan Airport's air traffic would
permit.
Using the background concentrations, the urban ratios from Sample 37-2,
and Equation III, we have calculated the NO deficits for the Boston plume
X
on August 30. The deficits are shown along with reaction time in Table 20 .
TABLE 20. NOX DEFICITS FOR FLIGHTS 37-39,
AUGUST 30, 1978
Sample No.
38-1
39-1
39-3
Reaction Time,*
Hrs.
2.3
i
5.1
5.6
NOX Deficit (ppm) Based On:
CO
.008
.013
.016
C2H2 F-ll
.007 -.003
.008 -.001
.012 .001
*Based on Flight 37-2 as T = 0
86
-------
The deficits derived from CO and C-H measurements are in reasonable
agreement and suggest a continuous loss of NO over the 5.6 hour reaction
X
interval studied. The results based on F-ll are once again unreasonable and
are not included in the subsequent discussion. The NO deficit obtained by
X
averaging the CO and C-H- results is plotted in Figure 19 against reaction
time. A line has been drawn through the data, the slope of the line indicating
an average NOX loss of 2.5 ppb per hour. This is in good agreement with the
results of the other case studies. Since the NO concentration averaged .022
X
ppm over the 5.6 hour period, the data from Flights 37-39 suggest an average
NO removal rate of 0.11 hr . This rate can be checked using the data at
A
5.6 hours from Sample 39-3. For this sample, the averaged tracer results
estimated that .025 ppm of NO should have been observed. Since 56 percent
X
(.014 out of .025 ppm) of the NO has been lost in 5.6 hours, the average loss
-1 ' x
rate was 0.1 hr . The first order plot of the NO results from these
X
flights are shown in Figure 20. The data fit the first order form
almost exactly. The slope of the line suggests a first order removal
rate constant of 0.14 hr
Three other data sets are plotted in Figure 19 . The ozone concentrations
for the urban plume samples are graphed against reaction time. Ozone increases
continuously over the 5.6 hour reaction time at a rate of .012 ppm per hour.
Ozone appears to be increasing linearly even after 5.6 hours of reaction,
indicating that the air parcel still contains NO . The CJi /C.H ratio shown
in Figure 19 also demonstrates that the reaction is proceeding even after 5
hours. In fact, the slope of the C9H./C7EL line indicates that ethylene may
" *f ^ *m •»
be removed at about the same relative rate as NO , that is ^0.1 hr
x
Also shown in Figure 19 is a plot of the oxidized nitrogen distribution
function,. F . The F data show that with an exception, the reaction products
n n
PAN and HONO- make up a continuously increasing fraction of the oxidized
nitrogen burden. The linear increase in F is in agreement with the NO
n x
deficit data in demonstrating that conversion of NO to reaction products
X
continues unabated for at least 5 hours. As described earlier, particulate
nitrate production in the urban plume was so low as to be undetectable.
87
-------
I 23456
Reaction Time, hours
FIGURE 19. SELECTED VARIABLES VS REACTION TIME
FOR FLIGHTS 37-39, AUGUST 30, 1978
88
-------
1.0
0.9
0.8
0.7
_0.6
§ 0.5
•£ 0.4
0.3
0.2
O.I
0
345
Reaction Time , hours
FIGURE 20. FIRST ORDER PLOT FOR FLIGHT 37-39,
AUGUST 30, 1978
89
-------
A nitrogen balance can be determined for the 30 August Boston plume by
comparing the sum of the measured nitrogen species (i.e., NO, N0_, PAN, and
HONO«) with the concentration of oxidized nitrogen which should be present in
some form. This latter estimate is derived from the tracer results and is
simply the first term on the right side of Equation III. To this prediction
of the amount of urban NO present must be added the NO background concentra-
X X
tion. This comparison is- made for the three downwind flight cross-section in
Figure 21. The equivalence line which would indicate a perfect nitrogen
balance is also plotted on. the figure. Two of the points lie on the line,
with the third somewhat below. The data in Figure 21 demonstrate that the
nitrogen balance is excellent for two of the plume traverses. About 75
percent of the expected nitrogen is accounted for in the remaining sample.
Within the limits of uncertainty of these experiments we believe that an
adequate nitrogen balance exists and that the combined concentrations of
PAN and HONO? reasonably account for the missing NO , with some small losses
& X
due to deposition accounting for any missing NO .
X
Ratios of pollutant concentrations are frequently useful as predictors
and in some cases serve to elucidate underlying chemical processes. The
(n\ (2) (18)
ratio 0 /PAN has been discussed by Lonneman , Spicer and Jorgen et al
During peak periods of photochemical activity in urban areas this ratio
frequently lies in the range 5-15. Using urban plume Sample 39-1 from
30 August, we find an 0,/PAN ratio of 11. This sample was selected over
39-3 because the reaction product data seem more reliable judging by the
excellent nitrogen mass balance.
Ozone/HONCL ratios in polluted atmospheres have been observed in the
range 15-30 during peak smog periods. The ratio of ozone to nitric acid for
Sample 39-1 was slightly outside this range at 36. PAN/HONO. ratios have
(15 19) (2 20)
been reported for smog chamber experiments ' and urban studies '
This ratio is dependent on the type and reactivity of the hydrocarbon
precursors, the extent of reaction, availability of surface for reaction/
depletion, relative humidity, NMHC/NO ratio, and perhaps other factors.
X
For Sample 39-1 the PAN/HONO- ratio was about 3.
90
-------
-§.
Q.
40
of 35
03
30
en
§ 25
o»
2
20
•Q
2
en
o
(U
6
3
tn
15
10
• Equivalence line
for perfect n-balance
0 5 10 15 20 25 30 35 40
Expected Nitrogen Concentration, ppb
FIGURE 21. SUM OF THE MEASURED NITROGEN COMPOUNDS
VS PREDICTED TOTAL NITROGEN
91
-------
Earlier in the flight, Sample 38-1 provided the following ratios:
0,/PAN = 10
03/HON02 = 18
PAN/HON02 - 2
Discussion of secondary pollutant ratios will be continued in a later
case study.
Case Study No. 4; August 14, 1978
August 14, 1978, was a hot, humid, hazy day in the Boston area. Ground
station data from Beverly Airport are not available due to breakdown of the
primary and backup data acquisition systems in the mobile lab. The gas
chromatographic system for PAN also was performing poorly so the PAN data
are considered suspect. Nevertheless, the meteorological conditions were
well suited to a study of NO decay in Boston's plume, and three flights
X
were conducted with this goal. Westerly winds prevailed during the day,
carrying the polluted urban air eastward over the ocean. The trajectory for
the 1100 EOT Boston air is pictured in Figure 22. During the first flight
sequence (Flight 11) Boston's emissions were trapped beneath a very low
surface inversion. Safety considerations precluded sampling at such low
altitudes; heavy traffic from low flying fish-spotting planes was the root
of the problem. Later in the afternoon, two flights were completed which
matched well with the air parcel time and position. The pertinent samples
are 12-1 and 13-2, obtained at 1316 EOT and 1632 EOT, respectively.
Undoubtedly a good deal of the NO emitted earlier in the morning has
X
reacted by 1316 EDT. Consequently, this discussion will deal with the later
stages of reaction. Of primary interest is the average rate of NO depletion
&
between 1316 and 1632 EDT (Samples 12-1 and 13-2, respectively).
92
-------
11-3
FRAMINGHAM
8-14-78
GLOUCESTER
WEYMOUTH
0 5 10 15 20 25 30
Statute Miles
FIGURE 22. AIR PARCEL TRAJECTORY AND AIRCRAFT
SAMPLE POSITIONS FOR 14 AUGUST, 1978
93
-------
Using the general background concentrations and the measurements from
Sample 12-1 as input data for Equation III, the NO deficits shown in
X
Table 21 have been calculated. All three tracers are in reasonable
TABLE 21.
NOX DEFICITS FOR
FLIGHTS 12 AND 13,
AUGUST 14, 1978
„ ... ™. NOV Deficit Based On:
Reaction Time, x
Sample No.
13-2
hours CO C2&2
3.3 .006 ppm .002 ppm
F-ll
.005 ppm
agreement; the average NO deficit is .004 ppm whether the F-ll results
X
are included or not. Since Equation III predicts that .008 ppm of NO
X
should have been present, it can be concluded that 50 percent of the
NO present in the air at 1316 EOT has been lost after an additional 3.3
hours of reaction. Using the first-order rate equation, we calculate
a pseudo-first order rate constant for NO removal of 0.20 hr for the
X
3.3 hour interval. The C E,/CJ12 ratio decreased from .43 to .17 over the
same 3.3 hour reaction interval. As reported earlier, the average rate of
ethylene removal appears similar to the NO decay rate. By comparison,
X
the ratios of less reactive hydrocarbons like propane, isobutane and n-butane
to acetylene changed very little over the 3.3 hour reaction period.
An example of the ozone and nitric acid profile of Boston's plume is
included as Figure 23. The figure was constructed from the continuous
instantaneous 0, and HONO data recorded during the plume traverse in which
Sample 12-1 was collected. The traverse was flown about 30 km downwind of
Boston shortly after 1300 EDT. The plume character of the ozone profile is
clear. Ozone concentrations on the fringe of the plume were 85-95 ppb. In
94
-------
Boston Plume Traverse, 30 km
13:30 8-14-78
IDU
160
140
"§: 120
^100
80
60,
^
A
>/"
/
w
L_ *
r
•^x*
k
A S
VJ
A
A^
\^.^l '
, /S
V
'V
1
\
4
/Xy'
-iu -y
-8 a.
6~
cv
-4 O
_ v "3—
-n y
Distance Through Plume, mites
FIGURE 23. OZONE AND HON02 DURING URBAN
PLUME TRAVERSE
95
-------
the center of the plume 0. exceeded .160 ppm. The nitric acid profile also
displays a definite plume character, tracking 0_ reasonably well. Nitric
acid was generally below 2 ppb outside the center of the urban plume, but
averaged about 4 ppb near the plume center. The 0,/HONO- ratio was
Summary of Case Studies
In previous sections we have described four case studies in which NO
X
reactions were followed in a Lagrangian fashion in Boston's urban plume. All
four experiments were conducted by instrumented aircraft on days when the
urban plume was transported eastward over the ocean. This strategy was
employed to eliminate fresh emissions into the air parcel during transport;
such fresh emissions would greatly complicate the interpretation of the
reaction rate data. The case studies were conducted on August 14, 18, 23
and 30, 1978. Inert tracers of opportunity (CO, C-H , F-ll) were used to
account for air mass dilution, and the resulting data were plotted using the
form of the first order rate equation. Once NO is largely converted to N0?,
further chemical reaction and physical scavenging processes can remove NO
A
from the air. Data for the four case study experiments yielded reasonable
straight line fits to the first-order equation. A tabulation summarizing
the results of the four case studies is included as Table 22. The peak
TABLE 22. SUMMARY OF RATE DATA FOR
CASE STUDY EXPERIMENTS
Date
August 15,
August 18,
August 23,
August 30,
1978
1978
1978
1978
Reaction
Interval (hrs)
3
7
7.5
5.5
Maximum
Transport Distance
Observed (km)
83
122
142
95
Rate Constant
for NOX
Removal (hr'-'-)
0.20
0.24
0.15
0.14
96
-------
ozone concentrations in the plume during these four days ranged from 90
to 140 ppb. The pseudo-first order rate constants ranged from 0.14 to 0.24
for the four experiments, and averaged 0.18 hr . For one case study, the
conversion ratio, F , was used to calculate a rate of NO conversion to
n x
products of 0.23 hr .
The NO removal rates for the four case studies indicate lifetimes
X
(1/k) of from 4.2 to 7.1 hours, with an average of from 4.2 to 7.1 hours,
with an average of 5.5 hours. We believe these values represent the first
accurate determination of NO removal rate and lifetime in urban air.
x
The data are applicable to sunny, moderately polluted urban air. These
results should be validated and extended by further studies under similar
as well as different environmental conditions.
The Philadelphia Urban Plume: August 24. 1978
Simultaneously with the Boston Plume Study, EPA sponsored a program on
oxidant transport in the Philadelphia area. The Philadelphia investigation
was aimed at evaluating methodology for quantifying ozone transport into and
out of an urban area. To assist EPA and their contractors in this effort, we
participated in a one day collaborative experiment during which we made air-
craft measurements to help define the extent of Philadelphia's ozone plume
and concentrations of pollutants therein. This experiment is included as a
case study because it obtained for perhaps the first time simultaneous ver-
tical profiles of nitric acid, 0^, NOX and condensation nuclei in a trans-
ported urban plume.
97
-------
The experiment was conducted on 24 August, a hot hazy day throughout
the northeast U.S. The flights on 24 August were designed to provide a
cross-section of the Philadelphia urban plume approximately 30 km downwind
of the city at two different times. Weather was poor on departure from
the Boston area, with heavy haze and low visibility prevailing throughout
the flight. As shown in Figure 24, three vertical profiles as well as
horizontal data at 1000' AGL were obtained downwind of the city in the late
morning. After refueling, a second cross-sectional pattern was attempted,
but had to be aborted after two vertical patterns due to IFR conditions and
thunderstorms. The horizontal data and spiral locations from this second
flight are shown in Figure 25. Vertical data on altitude, temperature, ozone
concentration, NO concentration and particle concentration are presented in
X
Tables 23 and 24for Flight 33 and 34, respectively. The data represent one
minute averages of the various measurements. The first set of profiles were
obtained between 1140-1300 EDT, while Flight 34 profiles were taken between
1430-1530 EDT.
The horizontal data from Flight 33 (Figure 24) show high ozone
concentrations pervading an area from Philadelphia to western Connecticut.
With westerly winds, the ozone concentration downwind of Philadelphia
reached 150 ppb during the late morning flight and nearly 200 ppb during
afternoon monitoring. These levels are consistent with earlier studies of
urban plumes in the northeast. ^
A strong inversion at about 5000 feet MSL served to control the pollutant
levels on 24 August. The temperature inversion does not show up very clearly
in some of the vertical profile data in Tables 23 and 24 due to the data
averaging. There is a clear drop in 0», CN and in most cases NO at this
j x
altitude in all the spirals conducted on 24 August, indicating the presence
of the inversion. In all cases, high concentrations of 0., were observed
beneath the inversion. Ozone levels above the inversion were in the 40-60
ppb range characteristic of the relatively unpolluted troposphere during
midafternoons. The concentration of nitrogen oxides above the inversion
layer was near the limit of detection of the chemiluminescence monitor
used in these flights. The concentration of condensation nuclei increased
significantly between the morning and afternoon profiles, both within and
98
-------
PHILADELPHIA ,
FIGURE 24. OZONE CONCENTRATIONS (ppb) AT
1000'AGL DURING FLIGHT 33,
24 AUGUST, 1978
25 50
Scale, mites
-H
75
99
-------
ALBANY /
/
FIGURE 25. OZONE CONCENTRATIONS (ppb) AT
1000'AGL DURING FLIGHT 34,
24 AUGUST, 1978
25 50
Scale, miles
75
100
-------
TABLE 23. RESULTS OF VERTICAL PROFILES FROM FLIGHT 33, 24 AUGUST, 1978
Time Altitude Temperature 03 NOX CNC
(EDT) (Feet MSL) (°C) (ppm) (ppm) (10* particles/cc)
Spiral 1
1142 1,470 24.3 .109 .006 4.2
1143 1,540 24.1 .109 .008 3.2
1144 1,730 23.3 .105 ,009 2.9
1145 1,890 22.7 .111 .008 3.9
1146 1,980 22.7 .112 .007 4.4
1147 2,310 22.1 .122 .005 4.1
1148 2,700 21.1 .124 .005 2.9
1149 2,880 20.7 .122 .005 2.1
1150 3,030 20.7 .120 .005 1.1
1151 3,380 19.9 .115 . .004 1.2
1152 3,800 18.9 .109 .003
1153 4,030 18.1 .117 .005 0.9
1154 4,700 - 17.6 .065 .003
1155 5,230 17.1 .045 .001
1156 5,600 16.0 .049 .002
1157 6,090 14.3 .047 .002 -
1158 6,510 13.1 .044 .001
1159 6,870 11.9 .046 .002
1200 7,110 11.2 .045 .002 ' -
Spiral 2
1222 1,350 25.9 .155 .014 4.3
1223 1,580 25.1 .151 .019 3.2
1224 1,930 23.7 .155 .019 4.6
1225 2,390 22.2 .149 .018 4.3
1226 2,940 20.5 .137 .014 3.3
1227 3,140 20.1 .108 .006 4.4
1228 3,600 18.7 .089 .004
1229 4,110 17.3 .107 .003 1.1
1230 4,570 16.6 .075 .002 .2
1231 5,010 17.3 .037 . .004 .02
1232 5,340 16.9 .053 .002 .4
1233 5,800 15.3 .057 .002 .3
1234 6,120 14.3 .049 .002 .3
1235 6,560 12.7 .046 .001 .5
1236 6,870 11.9 .044 .001 .2
1237 7,050 - .046 .001 .01
101
-------
TABLE 23. (Continued)
Time Altitude Temperature 03 NOX . CNC
(EDT) (Feet MSL) (°C) (ppm) (ppm) 10 particles/cc)
Spiral 3
1246 1,600 26.1 .117 .006 3.8
1247 1,770 25.2 .111 .005 4.7
1248 2,400 22.4 .108 .006 3.3
1249 2,740 21.7 .105 .006 3.7
1250 3,250 19.6 .109 .006 2.0
1251 3,690 18.9 .087 .003 0.8
1252 4,040 17.7 .095 .004 0.6
1253 4,630 17.4 ' .078 .002 0.1
1254 5,190 17.2 .046 .002 0.6
1255 5,590 16.1 .053 .002 0.6
1256 6,160 14.2 .048 .002 0.5
1257 6,660 12.8 .050 .003 0.3
1258 6,930 11.8 .047 .002 0.1
102
-------
TABLE 24. RESULTS OF VERTICAL PROFILES FROM FLIGHT 34, 24 AUGUST, 1978
Time
(EDT)
1432
1433
1434
1435
1436
1437
1438
1439
1440
1441
1442
1443
1444
1445
1446
1447
1448
1449
1512
1513
1514
1515
1516
1517
1518
1519
1520
1521
1522
1523
1524
1525
1526
1527
1528
Altitude
(Feet MSL)
1,460
1,660
2,000
2,370
2,800
3,120
3,470
3,780
4,130
4,550
4,970
5,290
5,570
5,750
6,150
6,460
6,810
7,180
1,200
1,410
1,680
2,090
2,470
2,850
3,240
3,550
3,970
. 4,500
4,880
5,300
5,650
6,010
6.410
6,730
7,120
Temperature
°C
Spiral
27.0
25.8
24.7
23.2
21.9
20.9
19.4
18.3
17.2
16.5
18.4
17.3
16.5
16.3
14.9
13.5
12.8
11.7
Spiral
27.8
27.1
26.5
24.9
23.7
22.4
20.9
19.7
18.6
17.5
18.8
18.3
17.5
16.3*
15.0
14.4
14.2
03
(ppm)
1
.152
.148
.146
.148
.147
.144
.154
.149
.145
.117
.040
.054
.052
.050
.049
.053
.049
.045
2
.179
.178
.177
.173
.178
.171
.171
.170
.159
.122
.042
.049
.061
.066
.065
.064
.050
NOX
(ppm)
.005
.005
.006
.006
.006
.006
.007
.006
.007
.007
.001
.001
<.001
.001
.003
.001
.003
.001
.013
.012
.013
.013
.012
.014
.011
.011
.012
.009
.002
.001
.002
.003
.002
.001
.002
CNC
(104 particles/cc)
7.8
9.0
9.3
10.5
9.2
8.7
9.1
8.9
8.6
9.0
4.5
4.4
4.8
3.9
3.9
3.8
3.5
3.6
10.6
11.0
11 '.3
11.5
11.2
10.3
11.4
11.6
11.5
11.2
9.7
6.1
8.1
10.4
8.2
8.7
8.3
103
-------
above the inversion. However, the instrument performance was not entirely
satisfactory during the morning flight, and these data are included with
a caveat.
A better representation of the data from these flights is obtained by
plotting instantaneous data points against altitude. Such a plot for
spiral No. 1 of Flight 34 is presented in Figure 26. The temperature
structure of the atmosphere as well as pollutant concentration behavior
becomes much clearer when the unaveraged data are employed.
The inversion is pictured quite clearly in the temperature profile in
Figure 26. The concentrations of 0,, NO , HONO, and CN all drop significantly
J X £•
above the inversion. The nitric acid concentration averages approximately
6 ppb in the polluted layer and drops to about 2 ppb above the inversion.
The concentration above the inversion is somewhat uncertain due to the
instrumental detection limit. The 0,/HONCL ratio within the polluted layer
below 5000 feet averages about 25. This is within the range we have observed
for this ratio in other urban areas and is similar to the ratio reported
earlier for the transported Boston plume for 30 August.
The data from these two flights are being interpreted by others as part
of the analysis of the Philadelphia study data base. The data have been
reported briefly here because of their relevance to the issue of atmospheric
nitrates.
104
-------
DOWNWIND PHILADELPHIA, 8-24-78
WOO
ALTITUOC,
fT(MSl)
20«0
Y
>
^••MLM*WMBM*MMMMIIHHB*»J VlMBM^BMMWWHtaM^B^^ WnHMMMUMMMM^J
15 19 23 27 03(9 30 70 110
TEMPERATURE. «C M ^ * 1M "° NO* PfB * J ' ' CMC.
OZONE. PFB HONO»PP« PARVCC(I10»)
FIGURE 26. VERTICAL PROFILES DOWNWIND OF PHILADELPHIA
105
-------
REFERENCES
1. Breeding, R. J., Klonis, H. B., Lodge, J. P., Jr., Pate, J. B.,
Sheesley, D. C., Englert, T. R. and Sears, D. R., Atmos. Environ.,
10, 181 (1976).
2. Spicer, C. W., "The Fate of Nitrogen Oxides in the Atmosphere", in .
Adv. Environ Sci. and Tech., V. 7, Pitts, J. N. and Metcalf, R. L.,
ed., John Wiley (1977).
3. Calvert, J. G., Environ. Sci. and Tech., 10, 256 (1976).
4. Spicer, C. W., Joseph, D. W., Sticksel, P. R., Sverdrup, G. M. and
Ward, G. F., "Reactions and Transport of Nitrogen Oxides and Ozone
in the Atmosphere", Battelle-Columbus draft report to EPA, Contract
No. 68-02-2439 (June, 1979).
5. Spicer, C. W., Joseph, D. W. and Ward, G. F., "Investigations of
Nitrogen Oxides Within the Plume of an Isolated City", Battelle-
Columbus report to CRC (CAPA-9-77) July, 1978.
6. Joseph, D. W. and Spicer, C. W., Anal. Chem., 50, 1400 (1978).
7. Spicer, C. W., in "Current Methods to Measure Atmospheric Nitric
Acid and Nitrate Artifacts", EPA-600/2-79-051 (1979).
8. Stephens, E. R., "Absorptivities for infrared Determination of
Peroxyacyl Nitrates", Anal. Chem., 36., 928 (1964).
9. Lonneman, W. A., Bufalini, J. J. and Seila, R. L., Environ. Sci. and
Tech., 10, 374 (1976).
10. Spicer, C. W. and Schumacher, P. M., Atm. Environ., 11, 873 (1977).
11. Spicer, C. W. and Schumacher, P. M., Atmos. Environ., 13, 543 (1979).
12. Liljestrand, H. M. and Morgan, J. J., Environ. Sci. and Tech., 12,
1271 (1978).
13. Galvin, P. J., Samson, P. J., Coffey, P. E., and Romano, D., Environ.
Sci. and Tech.. 12 580 (1978).
106
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14. Spicer, G. W., Joseph, D. W., Sticksel, P. R. and Ward, G. F.,
Environ. Sci and Tech.. 13, 975 (1979).
15. Spicer, C. W., "The Distribution, Fate and Reaction Rate of NOX in
the Atmosphere", paper presented at "Symposium on Implications of a
Low NO Vehicle Emission Standard", Reston, Va., May, 1979.
Jt
16. Easter, R. C., Busness, K. M., Hales, J. M., Lee, R. N., Arbuthnot,
D. A., Miller, D. F., Sverdrup, G. M., Spicer, C. W. and Howes, J. E.,
"Plume Conversion Rates in the SURE Region", Battelle Draft Final
Report to EPRI, Research Project 860-1 (1978).
17. Hegg, D., Hobbs, P. V., Radke, L. F. and Harrison, H., Atmos.
Environ.. 11, 521 (1977).
18. Jorgen, R. T., Meyer, R. A. and Hughes, R. A., Preprint 78-50.1
from 71st APCA Meeting, Houston, Tx. (1978).
19. Spicer, C. W. and Miller, D. F., J. Air Poll. Control Assoc.. 26_,
45 (1976).
20. Spicer, C. W., "Photochemical Atmospheric Pollutants Derived From
Nitrogen Oxides", Atm. Environ., 11, 1089 (1977).
107
-------
APPENDIX A
GROUND LEVEL DATA FROM BEVERLY AIRPORT
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APPENDIX B
FLIGHT MAPS FOR BOSTON PLUME STUDY
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