II. NJADN Results
II.A. Semi-Volatile Organic Compounds: Concentrations & Deposition
II.A1. Polychlorinated Biphenyls
Gas phase. A summary of the spatial variations in gas-phase PCB concentrations is presented in
Figure 6. Lab blank masses were not subtracted from gas-phase samples for this analysis due to
Gas-Phase PCB Concentration (pg m-3)
9000
8000
7000
6000
5000
4000
3000
2000
1000
0
CC XQ DB LS NB PL SH TK WC
Figure 6. Box and whisker plot of gas-phase PCB concentrations at all nine
NJADN sites. Upper dot, upper error bar, upper edge of box, lower edge of box,
lower error bar, and lower dot represent 95th, 90th, 75th, 25th, 10th and 5th percentile
concentrations, respectively. Within each box, mean and median concentrations are
shown by dashed and solid lines, respectively.
the low masses observed in lab blanks. Figure 6 demonstrates that gas-phase PCB
concentrations vary over more than 2 orders of magnitude from site to site in the state, with
highest concentrations typically occurring in the urbanized areas of Camden and Liberty Science
Center (Jersey City). Concentrations at each site appear to be log-normally distributed as well
(Figure 7). In great portions of the state, represented by 5 sites (PL, XQ, DB, WC, TK) which
18
encompass forested, coastal, and suburban environments, PCB concentrations are essentially
equal to concentrations observed at remote areas surrounding the Great Lakes (34). The similar
gas-phase PCB concentrations observed at sites surrounding the Great Lakes and in New Jersey
suggests this level of contamination represents a continental background and does not reflect any
Gas-Phase PCB Concentration (pg m-3)
10000
1000
100
10
CC XQ DB LS NB PL SH TK WC
Figure 7. Box and whisker plot of gas-phase PCB concentrations on a log scale at
all nine NJADN sites, demonstrating the log-normal distribution of concentrations.
influence of local PCB sources. Thus the influence of urban contamination appears to be highly
localized within New Jersey and does not extend spatially to these 5 "lesser-impacted" sites. For
example, the urban/industrial complex of New York City/Newark/Northern New Jersey emits
PCBs resulting in the high concentrations observed at Jersey City. The influence of these
emissions is felt but noticeably diluted at the nearby SH and NB sites, which are 30 and 40 km
away from JC, respectively. It should also be noted that the Hudson River Estuary emits PCBs
to the atmosphere year-round (21), and therefore likely contributes to the elevated gas-phase
concentrations observed at the three sites surrounding the estuary (JC, NB, and SH). The
19
urban/industrial area of Camden also emits PCBs resulting in gas-phase PCB concentrations
which comparable to measurements in urban Chicago, IL (6), and are among the highest ever
recorded. This local signal is, however, diluted to continental background at Washington's
Crossing and Pinelands, which are both about 45 km from Camden. The strong correlation
between urbanization and gas-phase PCB concentrations suggests that atmospheric PCBs in NJ
arise from highly localized, urban sources and are not transported from source regions out of
state.
The spatial pattern of concentrations observed near urban areas in NJ is similar to that
observed around Chicago, IL; and Baltimore, MD. In Baltimore (15), concentrations ranged
from 680-3,360 pg m-3 (similar to the range observed at JC), while 18 km away, the range
dropped to 210-740 pg m-3 (similar to SH) and thence to 20- 340 pg m-3 at a rural site 23 km
downwind of Baltimore (similar to the 5 “lesser-impacted” sites in the present study). In
Chicago (6), high concentrations of PCBs in the urban area (14200-270 pg m-3) are diluted to
780-230 pg m-3 at a rural site 125 km to the northwest. This site, South Haven, is thought to be
impacted by sources of PCBs other than the Chicago urban/industrial complex. Thus the range
of PCB concentrations measured there is slightly higher than the range observed at the 5 “lesserimpacted” sites in this study.
Gas-phase PCBs tend to be dominated by the lower Molecular Weight (MW) congeners,
due to their greater volatility. Tri- and tetrachlorinated congeners comprised about 50-65% of
the total measured PCBs at each site, with heavier homologue groups comprising decreasing
percentages with MW. The dichloro congeners comprised from 8 to 18% of the total measured,
despite the fact that the analytical methods quantified a single dichloro chromatographic peak
(consisting of PCBs 8 and 5). Had the analytical method employed allowed quantification of
more dichloro congeners, they likely would have comprised a larger portion of the total gasphase PCB burden.
The profiles of individual PCB congener concentrations between sites were compared to
assess whether sites are affected by similar source types. The DB site consistently demonstrated
the lowest correlation coefficients (R2 = 0.64 – 0.74) in comparison with the other 8 sites,
suggesting that DB may be affected by a different source of PCBs than the other 8 sites, which is
not surprising considering the geographical separation of this site from the rest of the state. The
next most dissimilar site was CC; its correlation coefficients were the lowest in comparison to 6
20
out of the 7 remaining sites. This may reflect the strong source which must be located near the
CC sampling site and generates the extremely high gas-phase PCB concentrations observed
there. The other 7 sites displayed correlation coefficients ranging from 0.79-0.98, suggesting
that PCBs in the rest of the state arise from a single dominant source type or process.
The temperature dependence of atmospheric PCB concentrations is well documented (3440). Such temperature dependence can indicate the distance of the monitoring site from the
source of PCBs, with steeper slopes (a) resulting from fitting the data to a Clausius-Clapeyrontype expression resulting from proximate sources (36, 38):
ln P 
a
b
T
where P is the partial pressure of the PCBs (in Pa, assuming an average molecular weight of
285 g mol-1), a and b are fitting parameters, and T is temperature (K).
The high R2 values
resulting from these regressions for the NJADN sites (Table 6) demonstrate that temperature is a
highly significant predictor of gas-phase PCB concentrations throughout New Jersey. Although
small differences in the slopes of these plots are evident, they are not statistically significant (as
suggested by the 95% confidence limits). Thus it is not possible to discern any information
about the proximity of each sampling location to possible sources from the results of these
regressions. The slopes presented in Table 6 are similar to those reported by Hillery et al. (34) at
remote sites surrounding the Great Lakes.
Table 6. Results of regressions of ln P (partial pressure in Pa) vs. 1/T (T in K) at NJADN sites.
Site
XQ
CC
DB
JC
NB
PL
SH
TK
WC
Slope
4277
6356
4414
5391
4649
5630
4396
4389
4419
95% CL
 2166
 1311
 1436
 1172
 1076
 873
 941
 1636
 1858
R2
0.42
0.65
0.53
0.56
0.40
0.78
0.52
0.42
0.37
p-value
0.000455
3.93E-13
4.11E-07
2.05E-13
7.55E-14
3.81E-17
2.56E-14
2.91E-06
2.28E-05
N
25
52
36
68
112
49
81
43
41
21
Previous analysis via the equation below of data from 1997-1999 reveal no significant
correlation between wind direction (wd) and gas-phase PCB concentrations (Cgas) at JC, NB,
and SH (41).
ln C gas  a0  a1 / T  a2 ln( 1 / u )  a3 sin (wd )  a4 cos( wd )
In this equation, ax values are fitting parameters and u is wind speed in m s-1. Similar analysis of
all data gathered at CC through May 2001 also demonstrated no significant link between
measured PCB concentrations and wind direction, suggesting that these impacted sites are all
affected by multiple localized sources of PCBs surrounding the sampling site. At JC, NB, and
SH, wind speed was not a significant predictor of PCB concentrations. At CC, however, wind
speed was a significant variable (p = 0.006), suggesting that a doubling of wind speed dilutes
atmospheric PCBs by about 40% from the average concentration measured at CC.
Gas-phase concentrations of PCBs drive the gross gas absorption component of total
atmospheric deposition. Thus gross gas absorption is greatest at CC and JC (Table 7). Wind
speed is also a critical parameter in the calculation of gas absorption, and the influence of wind
speed is evident in that the gas absorption flux is higher at SH than at NB, despite higher gasphase PCB concentrations at NB. For the same reason, fluxes are higher at TK and WC than at
NB. It must be noted that the wind speeds were measured at a variety of land-based sites. Wind
speeds over open waters such as Raritan Bay and Delaware Bay are likely to be higher than those
measured over land, and the corresponding gas absorption fluxes are therefore likely to be
higher. If the wind speed is assumed to be constant at 5 m/s, the gross gas absorption fluxes are
a direct function of gas-phase PCB concentration, and are therefore highest at the urbanized and
impacted sites and lowest at the 5 “lesser-impacted” sites (Table 7).
The homologue profile of the gas absorption fluxes is dominated by the low MW
congeners to an even greater extent that the gas-phase concentrations, with congeners containing
2-4 chlorines contributing 60-95% of the overall gas absorption flux at all sites.
Table 7 reveals no clear seasonal trend in gas absorption fluxes. This lack of seasonality
arises in part because low T during the winter has two effects which partially negate each other:
Henry’s law constants decrease with decreasing T (29, 30), resulting in an increased tendency
toward gas absorption, and gas-phase PCB concentrations are also lower during the cold winter
months, with lower concentrations available for gas absorption.
22
Table 7. PCB gross gas absorption flux (ng m-2 d-1) at the NJADN sites.
Summer Fall Winter Spring
avg. WS
Annual
Annual
m/s
(WS = 5 m/s)
CC
262
253
141
196
208
4.0
273
XQ
2.7
2.0
4.2
3.3
3.1
1.4
18
DB
0.92
0.78
3.1
3.6
2.0
1.1
16
JC
139
112
88
115
112
4.9
105
NB
8.5
6.2
13
12
9.8
1.8
51
PL
4.4
4.3
4.3
7.8
5.2
2.6
12
SH
42
50
47
48
47
5.4
37
TK
7.5
21
12.8
19
13
5.0
16
WC
13
19
16
15
16
4.0
20
Although these studies did not calculate gross gas absorption fluxes, the gas-phase
concentrations observed in the Chicago, IL (6) and Baltimore, MD (15) areas suggest that
deposition of PCBs to Lake Michigan and the Chesapeake Bay are likely to be similar in
magnitude and spatial variation to the fluxes presented here. In Chicago gas-phase PCB
concentrations are similar to those measured at CC, suggesting that the gas absorption fluxes
would be similar at the two sites, although in both cases it must be remembered that both the
concentration and the flux are highly localized and do not extend more than a few tens of km
from the urban source. Similarly, gross gas absorption fluxes in the Chesapeake near Baltimore
are likely to be similar to those calculated for JC because the gas-phase PCB concentrations are
similar at the two locations. Again, both the high concentrations and fluxes are likely to exert
themselves over a limited spatial range, dropping to background levels a few tens of km
downwind.
Particle phase
As with the gas-phase PCB results, lab blank masses were not subtracted from particlephase PCB samples due to low masses encountered in lab blanks. Typically, less than 10% of
the total atmospheric PCB burden is found in the particle phase. This percentage is higher
23
during colder sampling periods due to the decrease in vapor pressure of PCB congeners at lower
temperatures increasing sorption onto airborne particles. The percentage is also higher, of
course, for the higher MW PCBs. For the octa- and nonachloro congeners, for example, perhaps
50% of their total atmospheric concentrations is in the particle phase during the warmer months,
while essentially 100% is sorbed to particles in the winter. The homologue profile of particlephase PCBs is therefore somewhat different than the gas-phase profile. Dichloro congeners
typically comprise less than 1% of PCBs in the particle phase, while homologues containing 3,
4, 5, or 6 chlorines each comprise about 20% of the total. PCBs containing 7, 8, and 9 chlorines
make up about 10%, 5%, and 2% of the total particle PCB burden, respectively.
PCBs in the particle phase generally followed the same spatial trends as the gas phase
with CC and JC exhibiting the highest concentrations and several sites (XQ, DB, PL, SH, TK,
WC) displaying concentrations that rarely exceed 40 pg m-3 (Figure 8). Particle-phase PCB
concentrations at NB exceed this level in about 10% of samples. These results are similar to
observations at sites surrounding the Great Lakes (42), where particle-phase PCB
concentrations in remote regions are usually less the 40 pg m-3, but concentrations in Chicago
frequently exceed 100 pg m-3. Particle-phase concentrations of PCBs of less than 40 pg m-3
thus appear to represent continental background. The spatial distribution of particle-phase PCBs
observed in New Jersey demonstrates that, like gas-phase PCBs, particle-phase PCBs in this
region arise from sources that are highly localized in urban areas. Dilution of the particle-phase
PCB signal appears to occur more rapidly than dilution of the gas phase, with particle-phase
concentrations approaching regional background even at NB and SH.
By the algorithm chosen to calculate dry deposition fluxes, higher particle-phase PCB
concentrations translate directly into higher dry deposition fluxes (Table 8). At most sites, the
highest dry depositional flux occurs in winter, probably due to increased sorption of PCBs to
particle surfaces at lower temperatures. Gross gas absorption exceeds dry deposition in most
cases. At DB and NB, dry deposition is equal to or greater than gas absorption, due to the low
wind speeds experienced at these sites which lead to low gas absorption fluxes. The calculated
dry deposition fluxes are similar to those estimated for the Lake Michigan (42), which average
3.3 ng m-2 d-1 in remote regions and 15 ng m-2 d-1 in Chicago, assuming a deposition
velocity of 0.2 cm s-1 (versus 0.5 cm s-1 in the present study). Hillery et al. (4) estimate PCB
24
dry deposition fluxes to Lakes Superior, Michigan, and Erie to be about 2 ng m-2 d-1 based on
particle-phase measurements at remote locations and a deposition velocity of 0.2 cm s-1.
350
300
250
200
150
100
50
0
CC XQ DB LS NB PL SH TK WC
Figure 8. Summary of particle-phase PCB concentrations at NJADN sites.
Precipitation phase:
A detailed analysis of VWM precipitation concentrations and wet deposition of PCBs has
been conducted by VanRy et al. (43), and will be summarized here. For this analysis, lab blank
masses were subtracted from sample masses, due to relatively high masses of PCBs observed in
XAD blanks. VWM concentrations of PCBs at the seven sites at which precipitation was
collected varied over two orders of magnitude. The spatial variations in concentrations mirrored
those of the gas-phase, with highest concentrations occurring at CC and JC, followed by NB and
SH. The 3 “lesser-impacted” sites display the lowest VWM concentrations of all (rain samples
were not collected at DB and WC, the two other “lesser-impacted” sites). These results are
25
Table 8. PCB dry deposition fluxes (ng m-2 d-1)
Summer Fall Winter
Spring
Annual
CC
50
36
86
43
53
XQ
1.3
2.1
2.9
2.3
2.1
DB
5.3
6.4
8.3
5.2
6.5
JC
16
20
30
27
23
NB
13
6.1
10
7.5
9.4
PL
1.7
1.4
3.9
2.6
2.4
SH
4.8
4.3
7.1
4.7
5.1
TK
1.4
2.1
3.4
3.6
2.9
WC
1.7
3.4
4.9
4.3
3.8
were not collected at DB and WC, the two other “lesser-impacted” sites). These results are
similar to those of Offenberg and Baker (2), who observed that VWM concentrations of PCBs
in precipitation collected in Chicago, over Lake Michigan near Chicago, and at a remote site 125
km away (South Haven) were 29.3, 5.8, and 0.1 ng L-1, respectively.
Wet depositional flux is a function of both the VWM concentration and the precipitation
flux, but because precipitation fluxes are largely constant across the state, the wet depositional
fluxes follow the same spatial trend as the VWM concentrations. This spatial trend once again
suggests that highly localized, urban sources of PCBs exert an influence over atmospheric
concentrations and deposition fluxes over a distance of a few tens of km. Hillery et al. (4)
calculated wet deposition fluxes of PCBs to the Great Lakes from observations at remote sites;
the resulting averages ranged from 4 to 9 ng m-2 d-1, slightly higher than the fluxes calculated for
the 3 “lesser-impacted” sites in New Jersey. Offenberg and Baker (2) calculated wet deposition
fluxes on an event basis, but by applying a 30-year average precipitation flux for Chicago of 85
cm y-1, their VWM concentrations may be converted to fluxes of 68, 14, 0.2 ng m-2 d-1 at
Chicago, over Lake Michigan near Chicago, and at South Haven. Their results thus display a
similar spatial pattern driven by urbanization, again suggesting that concentrations and fluxes of
PCBs are diluted to background levels a few tens of km from the source.
At all sites except CC, the homologue distribution of PCBs in precipitation is similar to
that of the particle phase, with dichloro congeners typically comprising less than 4% of PCBs,
26
while tri- through hexachloro congeners comprise about 70-80% of the total. PCBs containing 7,
8, and 9 chlorines make up about 8%, 8%, and 1% of the total PCB burden, respectively. At CC,
Table 9. VWM concentrations and wet depositional fluxes of PCBs at NJADN sites.
Summer
Fall
Winter
Spring Annual
VWM concentrations (ng/L)
7.8
25
14
13
0.58
0.56
0.45
0.52
CC
XQ
6.0
0.53
JC
2.2
1.8
4.1
6.7
3.9
NB
1.1
0.63
1.9
1.6
1.3
PL
0.22
0.32
0.28
0.94
0.38
SH
0.99
0.52
0.70
0.75
0.80
TK
0.28
1.5
0.32
0.25
0.35
Fluxes (ng/m2/d)
CC
22
31
77
40
44
XQ
1.5
0.85
0.79
1.2
1.1
JC
6.6
4.6
12
18
11
NB
3.0
1.4
5.0
3.9
3.3
PL
0.97
1.0
0.83
2.2
1.2
SH
3.0
1.2
1.5
2.0
2.1
TK
1.6
0.87
0.64
0.47
0.85
high MW congeners (octa- and nonachloros) make up a much larger proportion of the total
(45%). This homologue profile highlights the efficient scavenging of particle by rain and
suggests that most of the PCBs detected in rain are in the particle phase.
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