TECHNICAL REPORTS

642

Mass balances on 10 polycyclic aromatic hydrocarbons (PAHs) in the New York–New Jersey Harbor (hereafter “the Harbor”) were constructed using monitoring data from the water column, sediment, and atmosphere. Inputs considered included tributaries, atmospheric deposition, wastewater treatment plant discharges, combined sewer overfl ows (CSOs), and stormwater runoff . Removal processes examined included tidal exchange between the Harbor and the coastal Bight and Long Island Sound, volatilization, and accumulation or burial of sediment-bound PAHs in the Harbor. Th e PAHs investigated were fl uorene, phenanthrene, fl uoranthene, pyrene, benz[a]anthracene, benzo[a]pyrene, perylene, benzo[ghi]perylene, indeno[1,2,3-cd]pyrene, and dibenz[a,h]anthracene. Th e results show inputs and outputs are fairly well balanced for most compounds, a fi nding that suggests aerobic biodegradation may not be a key loss process in this Harbor, as has been assumed in other systems. Th e main pathway for inputs of all PAHs is stormwater runoff . Atmospheric deposition is an important conveyor of PAHs with molecular weights ≤202 g mol−1. A principal objective of this report is to expose key data gaps, which include the need for comprehensive monitoring of both fl ow and PAH concentrations in stormwater and CSOs. An improved understanding of the key transmission routes of nonpoint source pollutants is essential for sustainable management of urban water resources.

Mass Balances on Selected Polycyclic Aromatic Hydrocarbons

in the New York–New Jersey Harbor

Lisa A. Rodenburg* Rutgers University

Sandra N. Valle, Marta A. Panero, and Gabriela R. Muñoz New York Academy of Sciences

Leslie M. Shor University of Connecticut

Polycyclic aromatic hydrocarbons (PAHs) are ubiqui-

tous organic compounds containing two to eight fused aro-

matic rings. Polycyclic aromatic hydrocarbon compounds can

be produced naturally via volcanoes and forest fi res; however,

PAHs in the urban environment are dominated by those aris-

ing from anthropogenic sources, which include various combus-

tion processes (burning of wood, coal, gasoline, diesel, natural

gas, municipal waste, etc.). In most cases, humans are exposed

to PAHs mainly by breathing contaminated ambient air, eating

grilled meat, and inhaling tobacco smoke. Th e U.S. Department

of Health and Human Services has determined that some PAHs

may reasonably be expected to be carcinogens. Some PAHs,

most notably benzo[a]pyrene, are known as probable human

carcinogens (Agency for Toxic Substances and Disease Registry,

1995). Benzo[a]pyrene is on the U.S. Environmental Protection

Agency (USEPA) list of 12 priority Persistent, Bioaccumulative,

and Toxic (PBT) chemicals currently being addressed under its

PBT initiative (http://www.epa.gov/pbt/ [verifi ed 13 Jan. 2010]).

Furthermore, PAHs are part of a group of 31 priority chemicals

that the USEPA has identifi ed for source reduction under the

National Partnership for Environmental Priorities.

Due to their ubiquitous presence and potential to cause

adverse human health eff ects, PAHs are a concern in all urban

watersheds. Historical contamination can have ongoing eff ects to

biota in urban watersheds (Cooper et al., 2009). Th e complex-

ity of such watersheds, however, makes the construction of eco-

system mass balances challenging. Most urban watersheds have

not been subjected to the kind of intense data-gathering eff orts

required to adequately characterize sources. Th e New York–New

Jersey Harbor (hereafter “the Harbor”) is likely an exception. Th e

Abbreviations: CARP, Contamination Assessment and Reduction Project; CSOs,

combined sewer overfl ows; IEC, Interstate Environmental Commission; MW, molecular

weight; NJADN, New Jersey Atmospheric Deposition Network; NJDEP, New Jersey

Department of Environmental Protection; NYSDEC, New York State Department of

Environmental Conservation; PAHs, polycyclic aromatic hydrocarbons; POC, particulate

organic carbon; REMAP, Regional Environmental Monitoring and Assessment Program.

L.A. Rodenburg, Dep. of Environmental Sciences, Rutgers Univ., 14 College Farm Rd.,

New Brunswick, NJ 08901; S.N. Valle, M.A. Panero, and G.R. Muñoz, New York Academy

of Sciences, 7 World Trade Center, 250 Greenwich St., 40th Floor, New York, NY 10007-

2157; M.A. Panero, current address: Robert F. Wagner Graduate School of Public Policy,

New York Univ., 295 Lafayette St., Ste. 2317, New York, NY 10012; G.R. Muñoz, current

address: New York-New Jersey Harbor Estuary Program, New England Interstate

Water Pollution Control Commission, 290 Broadway, 24th Floor, New York, NY 10007;

L.M. Shor, Dep. of Chemical, Materials and Biomolecular Engineering and Center for

Environmental Science and Engineering, Univ. of Connecticut, Storrs, CT 06269-3222.

Assigned to Associate Editor Steven Siciliano.

Copyright © 2010 by the American Society of Agronomy, Crop Science

Society of America, and Soil Science Society of America. All rights

reserved. No part of this periodical may be reproduced or transmitted

in any form or by any means, electronic or mechanical, including pho-

tocopying, recording, or any information storage and retrieval system,

without permission in writing from the publisher.

Published in J. Environ. Qual. 39:642–653 (2010).

doi:10.2134/jeq2009.0264

Published online 29 Jan. 2010.

Received 10 July 2009.

*Corresponding author, formerly Lisa A. Totten

(rodenburg@envsci.rutgers.edu).

© ASA, CSSA, SSSA

677 S. Segoe Rd., Madison, WI 53711 USA

TECHNICAL REPORTS: SURFACE WATER QUALITY

Rodenburg et al.: Mass Balances on 10 PAHs in the New York–New Jersey Harbor 643

Contamination Assessment and Reduction Project (CARP)

(Contamination Assessment and Reduction Project, 2007a

and 2007b) and other extensive monitoring eff orts have made

it possible to assess loadings and losses for this system. Such an

analysis can help scientists and policymakers establish targeted

programs to prevent primary emission or secondary transmis-

sion of contaminants—including PAHs—in urban water-

sheds. Previous attempts to assess PAH contamination in the

Harbor have been hampered by a lack of data on regional PAH

concentrations due to both a limited number of studies and

diffi culties associated with measuring PAHs in environmental

media. For example, Farley et al. (1999) used PAH concentra-

tion data from the Great Lakes region to estimate atmospheric

deposition to the Harbor.

Th e goal of this work has been to estimate loads and losses

of 10 PAH compounds from various transmission routes to

the Harbor to identify the key loading pathways and thereby

to inform policies designed to stem or lessen these loadings.

Th e focus of this investigation is on loads because they are

better characterized and can be calculated with less uncertainty

than losses. Rough estimates of losses are also presented. To

the extent that the Harbor is typical of urban watersheds in

the United States, the results should increase our understand-

ing of the types of processes that are important for the cycling

of PAHs in urbanized estuaries. To our knowledge, this report

represents the fi rst attempt to construct a mass balance on

PAHs in the Harbor based entirely on data collected in the

Harbor region.

Materials and Methods

Study Area and System BoundariesTh e New York–New Jersey Harbor drainage system covers an

area of 42,128 km2 (16,456 mi2). Th e water surface encom-

passes about 932 km2 (Adams et al., 1998; Adams and Benyi,

2003). For ease of discussion, the Harbor is divided into subar-

eas (Table 1 and Fig. 1).

To better characterize regional-scale loading and loss pro-

cesses in this large Harbor system, we defi ned unambiguous

system boundaries, and neglected both movements of PAHs

within the system and recirculation across system boundaries.

Only net infl ows or outfl ows across system boundaries were

considered. In this study, the New York–New Jersey Harbor

system boundaries were defi ned as the heads of tide of all trib-

utaries and the line connecting Sandy Hook with Rockaway

Point on Long Island, which separates the Harbor from the

Table 1. Total water surface area of the New York–New Jersey Harbor (including subbasins) used to calculate loads and losses of polycyclic aromatic hydrocarbons (Adams et al., 1998; Adams and Benyi, 2003).

Subbasin Area % of area

km2 %

Lower Harbor 318 34

Upper Harbor 104 11

Jamaica Bay 47 5.0

Newark Bay 32 3.4

Battery to Newburgh Bridge 431 46

Total water surface area 932 100

Fig. 1. Map of the New York–New Jersey Harbor and its watershed (shaded area). NJADN, New Jersey Atmospheric Deposition Network.

644 Journal of Environmental Quality • Volume 39 • March–April 2010

New York Bight (Fig. 1). Th e East River, which is not a true

river but a channel connecting Long Island Sound to the

Upper Harbor, is another boundary. Although there is sub-

stantial dynamic recycling between bottom sediment and sus-

pended sediment in a typical estuary, net sediment movement

is governed by nontidal gravitational forces (Grabemann and

Krause, 1989). Th erefore, to unambiguously identify key input

and output sources to the Harbor, we focused our mass bal-

ance on the Harbor water column itself, and defi ned the inter-

face between the water column and the sediment as another

system boundary. As a result, bottom sediments are external

to this Harbor system, and loss processes occurring in bottom

sediment such as PAH biodegradation and dredging were not

considered. Although accumulation of sediment-bound PAHs

in the bottom sediments of the Harbor removes them from

the water column, it does not remove them from the Harbor

ecosystem itself and therefore is not truly a loss process.

Polycyclic Aromatic Hydrocarbons Loading

and Loss PathwaysPathways of PAHs to the Harbor considered in this paper

include tributaries, atmospheric deposition via wet and dry

particle deposition and gross gas absorption, wastewater treat-

ment plant discharges, CSOs, and stormwater runoff . Th e

tributaries considered are the Hudson, Wallkill, and Mohawk

rivers in New York, and the Hackensack, Passaic, Raritan,

Elizabeth, and Rahway rivers in New Jersey.

Direct petrogenic-related inputs, including oil spills and

creosote, have been identifi ed as important sources of PAHs in

other studies, especially in localized regions directly adjacent

to sites of major oil spills or wood treatment facilities (Iannuzi

et al., 1995; Katz, 1998; Brenner et al., 2002; Walker et al.,

2005). Reported oil spills directly in the Harbor were deter-

mined not to be a major source of PAHs, and we know of no

currently operating wood treatment facilities in the immediate

vicinity of the Harbor. Ongoing emissions from individual oil

spills and leaching from creosote-treated wood pilings in the

Harbor area were considered in a previously published report

related to this study (Valle et al., 2007). Leaching of PAHs from

creosote-treated wood may be an important individual emis-

sion source of PAHs in the watershed as a whole. However, it is

diffi cult to estimate the magnitude of this input due to the lack

of long-term leaching studies and the diffi culty in determin-

ing the number of marine pilings in the Harbor. Nevertheless,

emission estimates of creosote to the Harbor directly (i.e., via

creosote-treated marine pilings) were estimated and are likely to

be minor for most PAHs relative to other input sources (Valle

et al., 2007). Other processes, such as groundwater discharges

to the Harbor from leaking underground storage tanks, erosion

of PAH-laden soils within the Harbor area (for example, super-

fund sites associated with creosote production, wood-treatment,

or manufactured gas production), or unidentifi ed point sources

could represent important loadings of PAHs to the Harbor, but

the data necessary to evaluate their importance are unavailable.

Losses considered include tidal exchange with the Bight and

Long Island Sound and volatilization. Sedimentation (accu-

mulation or storage in sediments) is also calculated, although

as noted above this is not a true loss process. Aerobic degra-

dation of PAHs in the water column is a potential loss pro-

cess that is not included because the parameters necessary to

accurately estimate it are lacking. Th ere is no clear consensus

in the literature on the importance of biodegradation in estu-

aries. Th e water quality model for the Harbor developed by

HydroQual does not consider degradation of PAHs at all due

to the absence of strong evidence indicating that such degrada-

tion is occurring (HydroQual, 2007).

Modeling Loads and LossesFlows of PAHs in surface water, including inputs from the

New York tributaries, wastewater treatment plants, CSOs,

stormwater, and outfl ows from tidal exchange, were quantifi ed

as mass fl ow rates:

aq diss part( )M C C Q= + [1]

where Maq

is the mass fl ow rate (in or out) via the aqueous

phase (kg yr−1), Cdiss

is the PAH concentration in the dissolved

phase (kg m−3), Cpart

is the PAH concentration in the particle

phase, and Q is the annual volumetric fl ow rate (m3 yr−1).

Loadings of PAHs from the New Jersey tributaries were

not computed according to Eq. [1] because the concentration

information available at the head of tide of the New Jersey

tributaries was not background-corrected. Instead, loads were

generated by the U.S. Geological Survey (USGS) and are

described in detail elsewhere (Bonin and Wilson, 2007). In

brief, particle-phase PAH concentrations were normalized to

particulate organic carbon (POC), and these concentrations

were multiplied by the POC loads. Th e POC loads were con-

structed using rating curves that describe the concentration of

POC as a function of river fl ow. Th ese loads do not include an

estimate of uncertainty.

Input pathways of atmospheric PAHs include gas absorp-

tion of gaseous PAHs and wet and dry deposition of particle-

associated PAHs. Loadings to the Harbor from the atmosphere

from these processes combined, Matm-in

(kg yr−1) were com-

puted as follows

gatm-in g p p r r

H

( )K

CM v C v C v A= + + [2]

where Cg and C

p are the concentrations of PAHs in the atmo-

sphere in the gaseous phase and associated with atmospheric

particles, respectively (kg m−3), and Cr is the concentration of

PAHs in rain (kg m−3). Th ese concentrations were multiplied

by deposition velocity vg, v

p, or v

r (m yr−1), for the gaseous,

particle-associated, and rain phases, respectively. Th e PAH

concentrations in the gas phase were converted to aqueous con-

centrations using KH, the temperature-corrected Henry’s Law

constant, as described elsewhere (Gigliotti et al., 2002). Th e

resulting fl uxes were converted to a mass fl ow rate by multiply-

ing by the Harbor area, A (m2).

Th e loss of PAHs from the Harbor due to volatilization

(Matm-out

) was calculated by

atm-out diss gM C v A= [3]

where Cdiss

is dissolved concentration of PAHs (kg m−3).

Rodenburg et al.: Mass Balances on 10 PAHs in the New York–New Jersey Harbor 645

Mass outfl ows of PAHs via net sediment settling were com-

puted by

s sM C SA= [4]

where Cs is the concentration of PAHs in sediment (kg m−3),

and S is the net sedimentation rate (m of sediment yr−1).

Estimating UncertaintyAlthough more complete than any previous mass balance study

for PAHs in the Harbor, our study is limited by a lack of detailed

environmental monitoring data. For example, particle-phase

PAH concentrations in each tributary were measured by the

CARP in just eight to 14 grab samples from 1998 to 2001. Th e

paucity of data made it challenging to characterize uncertainty

in loading and losses estimates. Furthermore, although it is

well known that in most river systems the majority of sediment

load (and associated PAHs) moves during a few extreme events,

limitations in the available data made it impossible to recon-

struct hydrographs for all tributaries and integrate loads from

paired fl ow and concentration data, as has been recommended

(Webb et al., 2000). In fact, for the CARP data set, there was

no signifi cant correlation between particle-phase PAH concen-

trations and tributary fl ow rate or POC concentrations for the

New York tributaries. Although sediment total organic carbon

(TOC) content and PAH concentration are widely known to

be highly correlated, Ouyang et al. (2006) similarly found no

correlation either in space or time in two Florida rivers because

major TOC and PAH inputs to the systems were widely segre-

gated. Th ese researchers stress the importance of better charac-

terization of pollutant input sources to understand eff ects on

sediment systems (Ouyang et al., 2006).

Our approach for estimating infl ows and outfl ows and

characterizing their uncertainty was to multiply each available

concentration by each available annual volumetric fl ow rate or

average transport velocity (i.e., deposition velocity, or settling

velocity) and to report the 25th, 50th, and 75th percentile loads

of the resulting matrix along with its mean. For water-based

input and output pathways, where PAH concentrations were

available separately for aqueous and particle-bound phases, the

mean, median, 25th, and 75th percentile loads were calculated

separately for each phase and then summed. Our approach is

to rely directly on the full scope of all available data to char-

acterize variability in loadings estimates. Th e major drawback

of our unweighted full factorial approach may be a tendency

to skew loads low because uncommon extreme events are less

likely to have been sampled, yet may comprise a dispropor-

tionately large proportion of total infl ows. For similar reasons,

our approach may also tend to underestimate variability. Our

approach was also not able to account for autocorrelation in

parameters, for example between PAH aqueous concentrations

and tributary volumetric fl ow rate.

Uncertainty could not be propagated and calculated ana-

lytically. Concentration data are often distributed log normally,

while volumetric fl ow rates tend to be distributed normally.

Th ere is no accepted analytical procedure for propagating error

for the product of a log-normally distributed parameter with

a normally distributed parameter, even assuming enough data

were available to identify the parameter distributions accurately.

Other authors have used a numerical Monte Carlo

approach to compute loads and estimate uncertainty (Venier

and Hites, 2008; Schenker et al., 2009). In Monte Carlo simu-

lations, individual data sets are fi t to distributions, then the

distributions are sampled repeatedly in evaluating the loading

model, and summary statistics for thousands of computations

are reported directly. Th is approach was not warranted in the

present work because of the diffi culty of uniquely identifying

parameter distributions from sparse data sets.

Th e uncertainty in all input and output pathways could not

be estimated using the metrics of the full factorial matrix. Since

the publicly available New Jersey CARP surface water PAH

concentration data did not include information on blanks nec-

essary to perform background correction, we judged it was pref-

erable to use the results from a separate USGS analysis, wherein

USGS used the CARP data to calculate tributary loads (Bonin

and Wilson, 2007). In calculating these loads, USGS used a

diff erent procedure in which particle-phase PAH concentra-

tions were normalized to POC. Th e USGS did not include an

estimate of uncertainty in these loads. Also, volumetric fl ow

rate information for several input and output pathways were

so sparse that a single best estimate value was used instead and

multiplied by an average concentration, as described below.

Pathways where a single best estimate of annual volumetric

fl ow rate was used include infl ows from CSOs and outfl ows

from tidal exchange and sedimentation. Because uncertainly

on losses was so poorly characterized in general, loss estimates

should be considered as rough estimates only, and are provided

here primarily for comparison purposes.

Polycyclic Aromatic Hydrocarbons ConsideredMass balances were constructed for fl uorene, phenanthrene, fl u-

oranthene, pyrene, benz[a]anthracene, benzo[a]pyrene, perylene,

benzo[ghi]perylene, indeno[1,2,3-cd]pyrene, and dibenz[a,h]

anthracene. Th ese compounds were chosen because they repre-

sent a wide range of molecular weights, which are closely related

to the physical properties of the compounds. In addition, these

PAHs were measured in all three of the key data sets (i.e., CARP,

New Jersey Atmospheric Deposition Network [NJADN], and

Regional Environmental Monitoring and Assessment Program

[REMAP]). Furthermore, these compounds (except for per-

ylene) are included in the 16 priority PAHs designated by the

USEPA. Compounds with molecular weight (MW) <202 g

mol−1, including fl uorene, phenanthrene, fl uoranthene, and

pyrene, are referred to here as low-MW PAHs, while the remain-

ing compounds are grouped into the high-MW PAH category.

Data Sources—Polycyclic Aromatic

Hydrocarbon ConcentrationsConcentration information for 22 PAHs in surface waters, sewer

overfl ows, wastewater treatment plant effl uent, and stormwater is

available from the CARP. Information on regional atmospheric

concentrations of 27 PAHs is available from the NJADN. Finally,

Harbor sediment concentrations for 17 PAHs are available from

the REMAP. Th is project is made possible by the availability of

high-quality monitoring data for a wide range of PAHs in the

water, air, and sediment of the Harbor region.

646 Journal of Environmental Quality • Volume 39 • March–April 2010

Th e CARP is a collaborative eff ort among several federal,

state, and nongovernmental partners that involved environ-

mental data collection by the New York State Department

of Environmental Conservation (NYSDEC), the New Jersey

Department of Environmental Protection (NJDEP), and the

USGS. Th e NYSDEC CARP samples were collected during

1998 to 2001 and the NJDEP CARP data were collected

during 2000 to 2002. Th e CARP measured PAHs by isotope

dilution gas chromatography with high-resolution mass spec-

trometry. Details of the methodology are available in a vari-

ety of reports through two Web sites: http://www.state.nj.us/

dep/dsr/njtrwp/ (verifi ed 13 Jan. 2010) and http://www.dec.

ny.gov/chemical/23839.html (verifi ed 13 Jan. 2010), and the

raw CARP data are available by request (http://www.carpweb.

org [verifi ed 14 Jan. 2010]).

Th e CARP data were used to construct PAH loads from

tributaries, wastewater treatment plants, CSOs, and storm-

water outfl ows, and to calculate losses from the Harbor due

to volatilization and tidal exchange. Th e CARP generally pro-

vided PAH concentration data as both aqueous and particle-

bound phases, except for tributary samples.

Information on blank concentrations was not available for

the NJDEP CARP data, so the NYSDEC CARP data were

used where possible. Th e sole exception was data from storm-

water outfalls. New Jersey CARP data from stormwater outfalls

were used in the mass balance because PAH concentrations in

the stormwater samples were generally high enough that blank

correction was not necessary.

Th e PAH inputs from New York tributaries were calculated

using particle-phase concentrations at the head of tide (i.e., the

farthest point upstream where a river is aff ected by tidal fl uctua-

tions). Dissolved-phase PAHs were not measured in these tribu-

taries. Th e dissolved-phase load was therefore estimated using

all dissolved-phase measurements from CARP samples collected

from other areas of the Harbor. About 90 of these were available,

but many PAHs were below detection limit in the majority of

these samples. One-half the detection limit was therefore used as

the concentration in these samples. Th is represents a reasonable

compromise between discarding below-detection-limit data,

which would result in a load estimate that is biased high, and

substituting zero for below-detection-limit data, which would

result in a load estimate that is biased low. Because the dissolved-

phase load is estimated using data collected in other areas of the

Harbor, it is less accurate than the particle-phase load and may

be biased high, because other areas of the Harbor tend to be

more contaminated that the northern tributaries, which lie well

outside the New York City metropolitan area.

Volatilization losses were based on dissolved PAH concen-

trations from the locations within the Harbor that represent

the largest portion of the total surface area: the Hudson River,

Jamaica Bay, and the Lower Bay. Tidal exchange terms were

calculated using PAH concentrations measured in Raritan Bay,

New York Bight, Long Island Sound, and Hudson River below

the Harlem River in both dissolved and particle-bound forms.

Th e NJADN measured atmospheric concentrations of 27

PAHs at several sites in New Jersey every 12th day for a period of

4 yr starting in 1997 (Gigliotti et al., 2005). Polycyclic aromatic

hydrocarbons in the gaseous, particle-associated, and aqueous

(precipitation) phases were measured by isotope dilution gas

chromatography with low-resolution mass spectrometry via

methods detailed elsewhere (Gigliotti et al., 2005). Th e NJADN

included two sites within the Harbor watershed at Sandy Hook

and Jersey City. In general, atmospheric concentrations of

PAHs are higher by about a factor of 4 at Jersey City than at the

more remote Sandy Hook (Gigliotti et al., 2005). Yan (2003)

reports PAH concentrations in the atmosphere at a location

in the middle of Raritan Bay that were generally higher than

those measured at Sandy Hook and lower than those measured

at Jersey City. Th us, the PAH concentrations measured at Jersey

City and Sandy Hook are assumed to be representative of con-

centrations throughout the Harbor, and both data sets were used

to characterize atmospheric PAH concentrations for this study.

Sedimentation losses were estimated using data from

REMAP, which includes measurements of 17 PAHs in sedi-

ment samples collected during 1993–1994 and 1998 at 28

locations in each of four subbasins of the Harbor (Adams et al.,

1998; Adams and Benyi, 2003). Th e four subbasins included in

the REMAP were the Upper Harbor, Lower Harbor, Newark

Bay, and Jamaica Bay. REMAP data from the Upper Harbor

were used for the Battery to Newburgh Bridge area. Th e 1998

REMAP data set (Adams and Benyi, 2003) is the most recent

available and was used for all but dibenz[a,h]anthracene.

Th is PAH was not included in the 1998 REMAP study, so

the 1993–1994 sediment concentrations were used instead

(Adams et al., 1998).

Although data for all 10 PAHs were available in all data

sets, CARP and REMAP measured dibenz[a,h]anthracene,

while NJADN measured dibenz[a,h+a,c]anthracene. Use of

the combined compound data from NJADN may overestimate

loadings from atmospheric processes to the Harbor; however,

atmospheric inputs for dibenz[a,h]anthracene are small com-

pared with overall loadings so this issue is unlikely to impact

the overall mass balance for this compound.

Data Sources—Volumetric Flow Rates: TributariesAverage annual volumetric fl ow rates for the New York trib-

utaries for the years 1980 to 2007 were taken from USGS

reports and are available online (http://wdr.water.usgs.gov/

[verifi ed 13 Jan. 2010]). New Jersey tributary fl ow information

was not needed because loads of PAHs from the New Jersey

tributaries were taken directly from Bonin and Wilson (Bonin

and Wilson, 2007).

Data Sources—Volumetric Flow Rates:

Wastewater Treatment PlantsTh e Harbor receives about 94 m3 s−1 in effl uent from about 70

wastewater treatment plants according to annual reports published

by the Interstate Environmental Commission (IEC) (http://www.

iec-nynjct.org/publications.htm [verifi ed 21 Jan. 2010]). In com-

parison, fl ow of the Hudson River past Manhattan is about 430

m3 s−1 for most of the year (Farley et al., 1999). For the CARP, the

NYSDEC sampled 18 wastewater treatment plants in New York.

Th ese 18 plants discharge about 85% of the total wastewater fl ow

to the Harbor. Total volumetric fl ow rates through all plants in

the area are reported annually and are available online for 2000 to

2007 (http://www.iec-nynjct.org/publications.htm [verifi ed 21

Jan. 2010]). Th ese IEC reports include fl ow data for between 68

Rodenburg et al.: Mass Balances on 10 PAHs in the New York–New Jersey Harbor 647

and 75 plants (depending on the year). Th e total fl ows for each

year through all plants were multiplied by the effl uent concentra-

tions from the CARP data set.

Data Sources—Volumetric Flow Rates:

Combined Sewer Overfl owsCalculating CSO loads was challenging due to lack of informa-

tion on CSO fl ows. Th e most comprehensive monitoring of

CSOs performed in the area occurred during the 1980s as part

of a CSO facilities planning study. Th e results of this monitor-

ing resulted in a reported fl ow of about 12 m3 s−1 for the 1987–

1988 water-year (HydroQual, 1991). Th is reported fl ow did not

include an estimate of uncertainty. Since this time, there has not

been a comprehensive program to monitor CSO fl ows in the

Harbor region, although some cities and collection systems have

performed intermittent monitoring of CSO fl ows. Th erefore,

current CSO fl ow rates were calculated in two ways. Th e fi rst

used data from the Jamaica Bay Watershed Protection Plan. Th is

plan lists a CSO fl ow to Jamaica Bay of 2355 million gallons

yr−1 (0.28 m3 s−1), which represents 2.6% of the total wastewater

treatment plant effl uent fl ow into Jamaica Bay. Assuming that

this percentage is representative of the Harbor as a whole, the

total CSO fl ow into the Harbor would be 2.6 m3 s−1, or about

22% of the 1987–1988 fl ow. Th is seems reasonable because there

have been extensive eff orts to increase CSO capture and therefore

decrease CSO fl ows since the 1980s (http://www.iec-nynjct.org/

publications.htm [verifi ed 21 Jan. 2010]). Th e second approach

to estimating CSO fl ow is based on fl ow statistics reported by the

IEC. Th e IEC reports that 12% of total wastewater treatment

plant fl ow is in the form of CSOs, and that New York City’s cur-

rent capture rate for CSOs is 69%. Multiplying these percent-

ages suggests that 3.7% of the total wastewater treatment plant

effl uent fl ow is untreated CSO inputs into the Harbor. Th is is in

fairly good agreement with the 2.6% estimate given above. Both

of these estimates of fl ow are obviously highly uncertain. We have

used the higher 3.7% number, coincidentally corresponding to

3.7 m3 s−1, to estimate CSO loads. Th e New York CARP data

set contains four to fi ve CSO samples, so both the fl ow and the

concentration are highly uncertain. Because of the high degree

of uncertainty, we have elected to present the best estimate CSO

loads without error bars.

Data Sources—Volumetric Flow Rates: StormwaterEstimates of stormwater fl ows to the Harbor for six water-years

were kindly provided by Robin Miller of HydroQual (personal

communication, 2004). Th e HydroQual estimates are based

on the detailed hydrodynamic model of the Hudson River and

its estuary, developed over the last 25 yr. Th e area of the estuary

in the HydroQual model is essentially the same as the Harbor

in the present study except that in the HydroQual model, the

estuary begins at Piermont Marsh (Piermont, NY) as opposed

to Troy, NY. Stormwater fl ows were calculated based on the rain

that actually fell and the ground cover type in the drainage area

on an hourly basis for October to September in six water-years:

1988–1989, 1994–1995, 1998–1999, 1999–2000, 2000–

2001, and 2001–2002. Th e estimated stormwater fl ows range

from 462 to 1062 million m3 yr−1 and average 710 million m3

yr−1. For comparison, the fl ow of stormwater into the Harbor

has been estimated by the USEPA (TAMS Consultants, Inc.

and Gradient Corporation, 1995) to be about 900 million m3

yr−1 (converted from approximately 1000 ft3 s−1).

Data Sources—Volumetric Flow Rates: Tidal ExchangeVolumetric fl ow rates reported by Rosenthal and Perron-

Cashman (2002) were used to estimate mass fl ows from tidal

exchange into and out of Raritan Bay and the New York–New

Jersey Bight. Th ese authors report the fl ow of water from the

Harbor to the Bight to be 1971 m3 s−1, and the fl ow of ocean

water into the Harbor to be 726 m3 s−1. Caplow (2004) reports

tidal exchange fl ows in the East River which are 630 m3 s−1

from the Long Island Sound to the Harbor, and 430 m3 s−1

from the Harbor to the Sound. Although the net fl ow is into

the Harbor, the higher contaminant concentration in the

Harbor results in net export for most contaminants, including

all PAHs investigated here.

Data Sources—Air–Water Exchange Mass

Transfer Coeffi cientsTh e air–water exchange mass transfer coeffi cient, v

g (also

referred to as the gaseous deposition velocity or the volatiliza-

tion velocity) is typically based on tracer studies for exchange

of tracer gasses such as SF6 and CO

2 as a function of wind

speed. Th e resulting vg is a function of wind speed as well as

the physicochemical properties of the compound. Using this

methodology, described in detail by Gigliotti et al. (2002), this

study used 100 values of vg calculated for PAHs using 100 wind

speed values designed to replicate the typical wind speed distri-

bution observed in the region at Newark Liberty International

Airport in Newark, NJ.

Dry deposition velocities (vp) were taken from the literature.

Here, we use all available values of vp included in fi ve published

papers (Sheu et al., 1996; Franz et al., 1998; Odabasi et al.,

1999; Vardar et al., 2002; Shannigrahi et al., 2005). Th ese 81

values were log-normally distributed and ranged from 0.006 to

2.04 cm s−1 with a geometric mean of 0.3 cm s−1. For comput-

ing wet deposition loads, the total annual rain depths for the

region (vr) for all years between 1980 and 2007 were used. Th ese

depths averaged 1.24 m yr−1 and are available online from the

New Jersey state climatologist (http://climate.rutgers.edu/state-

clim_v1/norms/monthly/precip.html [verifi ed 13 Jan. 2010]).

Data Sources—Sedimentation RateHere we assume a net sediment accumulation rate of 2.5 mm

yr−1, based on the study of Woodruff et al. (2001). As a net

accumulation rate, this parameter accounts for the combined

eff ects of deposition and resuspension. Multiplying this accu-

mulation rate by the Harbor sediment surface area of 932 km2

(equal to the water surface area), and a solids concentration of

500 g L−1 (Farley et al., 1999), the net amount of solids settled

each year is 1.2 × 109 kg yr−1.

Results

Loads—TributariesDetailed information on PAH loadings to the Harbor are given

in Fig. 2 and 3 and Table 2 by pathway and compound. Tributary

648 Journal of Environmental Quality • Volume 39 • March–April 2010

inputs are presented individually for particle-bound PAHs for

each of the three New York tributaries, and as combined inputs

in the dissolved phase from the Hudson, Wallkill, and Mohawk

rivers. Inputs of PAHs from all the New Jersey tributaries are given

as a composite estimate for particle-bound plus dissolved PAHs.

In general, the tributaries contribute about 10 to 15% to

total PAH loadings to the Harbor. Th e New York tributaries

contribute between 7 and 25% of all PAH inputs by compound,

while inputs from the New Jersey tributaries contribute between

0.5 and 16%. No trends by compound are apparent. In general,

the Mohawk River contributed the greatest fraction to total par-

ticle-bound PAH loads among the New York tributaries with the

Hudson River at Troy contributing second most and the Wallkill

River the least. For example, the median load of particle-bound

benzo[a]pyrene from tributary infl ows was 27, 18, and 10 kg

yr−1 via Mohawk, Hudson, and Wallkill rivers, respectively. Th is

is somewhat at odds with their total average discharge: 7 × 1012

L yr−1 for the Hudson, 5 × 1012 L yr−1 for the Mohawk, and 1 ×

1012 L yr−1 for the Wallkill.

It was not possible to assess the uncertainty of the loadings via

the New Jersey tributaries, as previously explained. However, for

particle-bound PAHs from the three New York tributaries, the

Fig. 2. Calculated loads of polycyclic aromatic hydrocarbons to the New York–New Jersey Harbor. Top of box, midline of box, and bottom of box repre-sent the 25th, 50th, and 75th percentile calculated loads. Circles represent mean and/or best estimate loads. Atm Dep, atmo-spheric deposition; CSOs, combined sewer overfl ows; MW, molecular weight; tribs, tributaries.

Rodenburg et al.: Mass Balances on 10 PAHs in the New York–New Jersey Harbor 649

25th percentile of inputs is about 25% of the median, and the

75th percentile load is about three times the median.

Loads—Wastewater Effl uentsLoads from wastewater treatment plant effl uents were typically

<5% of total loads for most PAHs. Th ere is no clear trend by

compound, with the three-ring PAH fl uorene and the fi ve-ring

PAH dibenz[a,h]anthracene having the largest fraction of load-

ings from wastewater (7.6 and 18.5% of the median loading

value, respectively), and benzo[a]pyrene with the smallest frac-

tion of loadings from wastewater (1.4%).

Loads—Combined Sewer Overfl owsCombined sewer overfl ows contribute about 5% of total

Harbor PAH loadings. However, these estimates are very

uncertain because there is such limited information on CSO

fl ow rates in the region.

Loads—StormwaterFor many of the PAHs investigated, stormwater runoff is the

most important input pathway to the Harbor. Stormwater runoff

contributes between 17 and 46% of total loads for diff erent PAH

compounds, with the higher MW PAHs contributing a slightly

greater proportion to total inputs to the Harbor. Recovery of par-

ticulate matter from urban pavement runoff is high, in one study

exceeding 90% per event (Sansalone and Kim, 2008), so it is not

surprising that the high-MW PAHs, which tend to be particle

bound, are prevalent in stormwater. However, the magnitude of

the stormwater load is highly uncertain. Th e fl ow of runoff into

the Harbor is expected to exhibit signifi cant temporal variabil-

ity, as changes in precipitation rate and ground permeability will

change the amount of rainfall that percolates through the soil or

evaporates vs. the amount that runs off into the Harbor. Although

the annual average stormwater fl ow rate has been characterized

fairly well, the concentration of PAHs in stormwater runoff is not

well understood. Th e stormwater load-

ings described here are based on just

two measurements of PAHs in storm-

water outfl ows in New York, and 16

measurements in New Jersey.

Loads—Atmospheric DepositionAtmospheric deposition seems to be

an important route for the delivery of

low-MW PAHs to the Harbor. For

example, atmospheric inputs contrib-

ute 44% of total loads for the three-ring

compound phenanthrene, but only

about 2% of inputs of perylene, benzo[a]

pyrene, and dibenz[a,h]anthracene.

Losses

Tidal Exchange

Tidal exchange is responsible for

about 30% of PAH outfl ows from the

Harbor. About two-thirds of the tidal

exchange losses occur to the New York

Bight, with the remainder occurring to

the Long Island Sound. Tidal exchange

is slightly more important as a loss process for the heaviest PAHs,

including dibenz[a,h]anthracene and indeno[1,2,3-cd]pyrene,

but this process’s contribution to losses of low-MW PAHs such

as phenanthrene and fl uoranthene is less signifi cant. However,

the magnitude of tidal exchange is highly uncertain because the

average annual tidal exchange fl ow rates are so poorly character-

ized for the Harbor.

Volatilization

Not surprisingly, volatilization is a strong function of molecular

weight. Evaporative losses from the surface of the Harbor back

to the atmosphere contribute only about 10% or less to total

losses of the high-MW PAHs, but this loss pathway contrib-

utes about 30% or more for the low-MW PAHs. Volatilization

losses are fairly well characterized because there are high-qual-

ity monitoring data of aqueous-phase PAH concentrations in

the Harbor, as well as reasonable estimates of the water–air

exchange velocity based on tracer studies.

Sedimentation

Losses of high-MW PAHs from the Harbor are dominated

by sedimentation, which may account for about half of total

losses. However, sedimentation rates are not very well under-

stood. Th is study uses a single annual net settling velocity to

characterize loss due to sedimentation. Clearly, sedimentation

in a large estuary is an extremely complex process, with sedi-

mentation rates varying widely across the Harbor, and biotur-

bation, scour, and storm events contributing a great deal of

temporal variability to sedimentation processes as well.

Discussion

Polycyclic Aromatic Hydrocarbon Annual BudgetTables 2 and 3 present the annual budget for PAHs in the

Harbor. Figure 4 presents a comparison of loads and losses.

Fig. 3. Calculated loads of polycyclic aromatic hydrocarbons (PAHs) to the New York–New Jersey Harbor by PAH (in order of increasing molecular weight) and loading pathway. Loads presented are 50th percentile loads (where available) and best estimate (mean) loads for combined sewer over-fl ows (CSOs) and New Jersey tributaries (Tribs). Abbreviations for PAHs are given in Table 2. Atm Dep, atmospheric deposition; WPCP, water pollution control plant.

650 Journal of Environmental Quality • Volume 39 • March–April 2010

Table 2. Calculated loads of polycyclic aromatic hydrocarbons (PAHs) to the New York–New Jersey Harbor in kg yr−1.†

PAH PercentileHudson Wallkill Mohawk NY tribs Wastewater Stormwater Atm

dep

NJ tribs CSOsSum‡

Particle Particle Particle Dissolved Total Total Total Total

Benz[a]anthracene 50th 19 5.4 24 24 19 238 17 494

BaA 25th 3.4 1.7 3.2 12 9.1 69 4.3

MW 228 75th 51 33 45 66 38 540 71

Mean 30 21 36 86 55 404 107 117 30 886

n 11 14 10 45 107 18 371 4

Benzo[a]pyrene 50th 18 9.7 27 28 11 332 18 662

BaP 25th 9.2 3.2 4.8 13 5.8 82 5.1

MW 252 75th 61 38 49 65 20 673 71

Mean 34 22 36 63 19 524 99 180 38 1015

n 11 14 10 30 82 18 322 4

Benzo[ghi]perylene 50th 12 5.0 25 28 15 372 37 708

BghiP 25th 2.9 2.1 2.6 12 5.7 90 9.8

MW 276 75th 39 21 57 85 24 635 154

Mean 22 14 39 88 62 472 192 183 30 1101

n 11 14 10 53 106 18 316 4

Dibenz[a,h]anthracene 50th 2.0 0.94 2.5 21 18 66 4.8 148

DahA 25th 0 0.40 0.53 9.4 1.9 15 1.3

MW 278 75th 9.1 6.1 4.5 64 36 135 19

Mean 11 7.5 5.8 80 5.8 98 26 25 7.4 267

n 8.0 14 10 14 53 18 313 4

Fluoranthene 50th 30 9.7 73 130 53 744 333 1812

Fl 25th 0 2.9 6.0 42 24 283 143

MW 202 75th 84 54 132 237 110 1599 824

Mean 51 32 92 221 292 1113 736 365 76 2978

n 8.0 14 10 72 112 18 419 4

Fluorene 50th 2.6 1.4 5.9 46 57 126 122 382

F 25th 0.80 0.52 1.0 17 20 66 44

MW 166 75th 5.6 6.1 12 163 152 299 289

Mean 6.3 6.9 8.4 183 597 634 246 8.0 13 1703

n 11 14 10 48 110 18 418 4

Indeno[1,2,3-cd]pyrene 50th 30 14 73 23 11 296 44 688

IP 25th 0 4.5 6.0 9.4 3.8 84 12

MW 276 75th 84 61 132 76 23 551 173

Mean 51 48 92 85 83 433 257 174 25 1248

n 8.0 14 10 39 93 18 313 4

Perylene 50th 9.4 4.0 4.8 25 6.9 94 5.2 216

Pery 25th 3.1 1.6 1.9 11 4.2 21 1.5

MW 252 75th 32 20 22 50 12 183 20

Mean 26 13 14 65 74 147 31 56 11 436

n 11 14 10 21 64 18 313 4

Phenanthrene 50th 25 6.5 51 32 52 453 866 1738

Phen 25th 4.2 2.0 4.1 13 22 225 371

MW 178 75th 46 23 86 166 143 938 1909

Mean 32 23 64 180 505 1751 1471 192 61 4279

n 11 14 10 61 116 18 419 4

Pyrene 50th 27 12 45 179 130 813 218 1788

Pyr 25th 7.1 4.9 5.3 70 80 251 83

MW 202 75th 78 38 115 305 191 1455 600

Mean 49 40 81 258 519 1158 546 294 69 3014

n 11 14 10 74 119 18 419 4

† Atm dep, atmospheric deposition; CSOs, combined sewer overfl ows; MW, molecular weight; tribs, tributaries.

‡ Sums were computed as follows: the 50th percentile sum includes the 50th percentile loads where available, plus the mean loads for CSOs and New

Jersey tributaries. The mean sum load is the sum of the mean loads for all processes.

Rodenburg et al.: Mass Balances on 10 PAHs in the New York–New Jersey Harbor 651

For all but perylene, the median estimated loads are within a

factor of 2 of the estimated losses. For fl uorene and perylene,

the estimated losses are greater than the 75th percentile load

estimates. Th ere is some evidence that perylene is produced

naturally in the sediments of the Harbor (Venkatesan, 1988),

which could represent an additional input of perylene not

Table 3. Calculated losses of polycyclic aromatic hydrocarbons (PAHs) from the New York–New Jersey Harbor in kg yr−1.

PAH Percentile Volatilization SedimentationTidal exchange

Sum†Bight East River

Benz[a]anthracene 50th 57 809

25th 20

75th 155

Mean 161 568 102 82 913

n 15

Benzo[a]pyrene 50th 25 563

25th 11

75th 51

Mean 57 353 102 82 594

n 7

Benzo[ghi]perylene 50th 16 519

25th 8

75th 50

Mean 39 353 103 47 542

n 22

Dibenz[a,h]anthracene 50th 15 215

25th 7

75th 33

Mean 35 93 99 8 235

n 15

Fluoranthene 50th 263 1357

25th 85

75th 727

Mean 483 867 134 94 1577

n 15

Fluorene 50th 278 994

25th 123

75th 942

Mean 1079 206 439 70 1794

n 19

Indeno[1,2,3-cd]pyrene 50th 11 730

25th 5

75th 39

Mean 31 340 208 171 749

n 14

Perylene 50th 25 542

25th 11

75th 59

Mean 55 389 104 24 572

n 9

Phenanthrene 50th 138 1028

25th 71

75th 491

Mean 406 733 107 49 1296

n 28

Pyrene 50th 338 1885

25th 112

75th 782

Mean 511 895 238 414 2059

n 33

† Sums were computed as follows: the 50th percentile sum includes the 50th percentile volatilization loss and the means for the other losses. The mean

sum loss is the sum of the mean losses for all processes.

652 Journal of Environmental Quality • Volume 39 • March–April 2010

included in the mass balance. Th is could

therefore lead to losses exceeding inputs to

the system for this compound.

A system at steady state is one in which

inputs equal outputs and there is no long-

term change in PAH concentrations in the

waters of the Harbor. A mass balance that

is not closed suggests one of two things: (i)

sources or sinks (or both) are inaccurate or

(ii) the system is not at steady state. Do we

have any reason to believe that the Harbor’s

waters are at steady state with respect to

PAH contamination? Yan et al. (2006)

measured ΣPAH (ΣPAH = the 16 USEPA-

listed priority PAHs) in sediment cores

from several locations in the Harbor and

concluded that ΣPAH levels dropped sub-

stantially from the 1950s to the 1970s in

all areas of the Harbor. However, the trends

from 1970 to 1990 (when the cores were

collected) were not as clear. Some cores

(Passaic River) showed an increase in ΣPAH

concentrations, while others (Raritan Bay)

showed a decrease. A comparison of the

1993–1994 and 1998 REMAP data sets (Adams et al., 1998;

Adams and Benyi, 2003) shows that in the Raritan Bay, of the

16 PAHs for which enough data was available to determine

the trends, nine PAHs showed a decrease from 1993–1994

to 1998, while seven PAHs increased in concentration. Th e

trend for the sum of all 16 PAHs was a decline of 13%, which

is probably not signifi cant given the uncertainties involved.

Th us, it is likely that PAHs in the Harbor are near steady state

and the mass balances should be roughly closed.

Th e agreement between loadings and losses presented in this

study to within a factor of 2 for most PAHs suggests a Harbor

near steady state with regard to PAH contamination. Our

model includes several infl ow and outfl ow pathways, but does

not include biodegradation. As noted above, there is no clear

consensus in the literature on the importance of biodegrada-

tion in estuaries. While the water quality model for the Harbor

developed by HydroQual does not consider degradation of

PAHs at all (HydroQual, 2007), Greenfi eld and Davis (2005)

found biodegradation rate constants taken from the literature

caused their mass balance model of PAHs in San Francisco Bay

to indicate biodegradation is the most important loss process

for PAHs in sediments. However, these authors also note that

estimates of biodegradation are highly uncertain. Our results

do not directly contrast those of Greenfi eld and Davis because

we consider sediment to be outside the system boundary, so

biodegradation in the sediment would not have any impact on

our mass balance assessment. However, our results may suggest

biodegradation in the water column is not a very important

loss process for the PAHs considered in this study.

Data GapsTh is analysis has identifi ed several data gaps that should be

addressed to better understand PAH cycling in the Harbor.

Th e CARP has greatly reduced the uncertainty associated

with most of the loads by increasing the amount of data on

concentrations of PAHs in various sources. Additional char-

acterization of PAH concentrations in stormwater and CSOs

is needed. Additional information on CSO volumetric fl ow

rates is also needed to reduce the uncertainty in estimating

CSO loads.

Although atmospheric deposition is relatively well charac-

terized in the Harbor region, the lack of data on atmospheric

concentrations of low-MW PAHs such as naphthalene and

acenaphthene is problematic. Since this analysis suggests that

atmospheric deposition is an important source of low-MW

PAHs to the system, atmospheric measurements of these

low-MW species should be performed.

ConclusionsTh e PAH mass balances presented in this study suggest that

stormwater runoff is the most important transmission pathway

for all PAHs to the Harbor, contributing about half the total

load. Mass balances on polychlorinated biphenyls and polychlo-

rinated dibenzo-p-dioxins and -furans in the New York–New

Jersey Harbor suggest that stormwater runoff is a major source

for these pollutants as well (Totten, 2005; Fennell, 2006).

Additional stormwater sampling to confi rm the importance of

stormwater inputs to Harbor loadings is needed. Despite the

uncertainty associated with the loads presented here, the results

support implementation of enhanced stormwater management

plans as a means to prevent chronic nonpoint source inputs of

PAHs and other organics to the Harbor.

Atmospheric deposition is also an important input path-

way, comprising about 25% of total loads for low-MW PAHs.

Controls on the atmospheric emissions of low-MW PAHs

such as fl uorene and phenanthrene will be necessary to achieve

signifi cant reductions in their ambient water concentrations.

Possible sources of PAHs to the atmosphere as well as stormwa-

ter are explored in a separate report (Valle et al., 2007).

Fig. 4. Median estimated loads and losses of polycyclic aromatic hydrocarbons (PAHs) (in order of increasing molecular weight) in the New York–New Jersey Harbor. Error bars represent the 25th and 75th percentiles for the distribution. Abbreviations for PAHs are given in Table 2.

Rodenburg et al.: Mass Balances on 10 PAHs in the New York–New Jersey Harbor 653

AcknowledgmentsTh anks to the New York Academy of Sciences for their support of this

work. Th anks also to Simon Litten of New York State Department of

Environmental Conservation (NYCDEC) and Joel Pecchioli from the

New Jersey Department of Environmental Protection (NJDEP) for

providing data and discussions.

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