| ||||||||||||||||||||||||||||||||
|
|
|||||||||||||||||||||||||||||||
Below are the first 10 and last 10 pages of uncorrected machine-read text (when available) of this chapter, followed by the top 30 algorithmically extracted key phrases from the chapter as a whole.
Intended to provide our own search engines and external engines with highly rich, chapter-representative searchable text on the opening pages of each chapter.
Because it is UNCORRECTED material, please consider the following text as a useful but insufficient proxy for the authoritative book pages.
Do not use for reproduction, copying, pasting, or reading; exclusively for search engines.
OCR for page 233
Oil in the Sea III: Inputs, Fates, and Effects
I
Estimating Land-based Sources of Oil in the Sea
Because of the scarcity of available data for estimating land-based loads of oil to the sea from individual sources (i.e., municipal wastewaters, nonrefinery industrial discharge, refinery discharges, urban runoff, river discharges, and ocean dumping), loading estimates presented in this analysis were based on loading from all land-based sources per unit of urban land area. These calculations assumed that most of the contributions of petroleum hydrocarbons to the sea from land-based sources were from urban areas. This approach accounted for loading from all of the sources in the United States and Canada, with the exception of Gulf coast loadings from coastal refineries, which was calculated separately. The overall calculations of hydrocarbon loadings from all land-based sources for the United States and Canada were then extrapolated to other regions of the world to form a world estimate.
METHODOLOGY AND SOURCES OF THE DATA
A review of the U. S. Environmental Protection Agency’s STORET data base revealed oil and grease data for only nine major rivers in the United States, and several of these consisted of very few observations. Even fewer rivers (i.e., Brazos, Delaware, and Trinity) had hydrocarbon data. The dominance of oil and grease data measured using either the Soxhlet extraction method (tot-sxlt) or liquid-liquid extraction (freon-gr) methods in the available STORET data led to the use of measured oil and grease concentrations as the basis for estimates presented in this analysis.
Quantified estimates of oil and grease and petroleum hydrocarbon loadings were made for the United States and Canada. These estimates were made using unit loadings per urban land area. The annual loadings were calculated according to the coastal zones defined in this study, and the overall loadings for the United States and Canada were extrapolated to the world.
For the calculations in the United States and Canada, the land-based sources were divided into two categories: inland basins and coastal basins. It was assumed that inland basins discharged into one of the following major river basins that outlet to the sea along the coast of the United States and Canada (coastal basins were assumed to discharge directly to the sea):
Alabama-Tombigbee
Altamaha
Apalachicola
Brazos
Colorado (Texas)
Columbia
Copper (Arkansas)
Delaware
Hudson
James
Mississippi
Neuse
Potomac
Rio Grande
Roanoke
Sabine
Sacramento
St. Lawrence
Santee
San Joaquin
Saskatchewan
Savannah
Susitna
Susquehanna
Trinity
Yukon
OCR for page 234
Oil in the Sea III: Inputs, Fates, and Effects
Calculations for the Inland Rivers of the United States and Canada
The following methodology was used to estimate the loading of oil and grease to the sea from inland river basins in the United States and Canada:
The location of the mouth of each river was determined on a map. These locations were then expanded into regions of interest (generally defined by the latitude and longitude of the lowest U.S. Geological Survey (USGS) gauging station and a radius around that point; see Table I-1) for which water quality data were requested from STORET. Searches were made for all surface water quality data collected within these regions.
Data for the following parameter codes were then requested from STORET if they were included in the data summaries for the regions:
Parameter code 00550: oil-grse tot-sxlt (mg L−1)
Parameter code 00552: oil-grse tot-hexn (mg L−1)
Parameter code 00556: oil-grse freon-gr (mg L−1)
Parameter code 00560: oil-grse freon-ir (mg L−1)
Parameter code 03582: oil and grease tot wtr (mg L−1)
Parameter code 45501: hydrocarbon ir (mg L−1)
Averages of all reported values in STORET for the parameter codes listed were compiled for each river (Table I-2) with the following assumptions (rivers not shown in Table I-2 did not have any usable oil and grease data):
Only ‘ambient’ readings in freshwater rivers were included; this means that values reported for industrial or municipal effluents, nonambient conditions, sediment, and/or ocean/estuary locations were not included in the average.
Some values were reported to be ‘off-scale low,’ which meant that the actual value was not known, but was known to be less than the value shown. To calculate our averages, we set these values to one-half their reported value.
For those rivers with data in the 1990s, average concentrations for that period were calculated.
An average annual load in tonne yr−1 was calculated for those rivers with reported oil and grease data by using the following formula:
TABLE I-1 Regions Searched for Oil and Grease and Hydrocarbon Data from STORET
River
Latitude
Longitude
Radius (mi)
Alabama-Tombigbee
32º00′00″, 30º00′00″
−87º15′00″, −88º15′00″
See notea
Altamaha
32º31′30″
−81º15′45″
50
Apalachicola
See note b
Brazos
29º34′56″
−95º45′27″
50
Colorado (TX)
28º58′26″
−96º00′44″
30
Columbia
46º10′55″
−123º10′50″
50
Copper (AK)
61º00′00″
−144º45′00″
50
Delaware
39º30′03″
−75º34′07″
30
Hudson
41º43′18″
−73º56′28″
40
James
37º24′00″
−77º18′00″
50
Mississippi
29º16′26″
−89º21′00″
50
Neuse
35º06′33″
−77º01′59″
50
Potomac
38º55′46″
−77º07′02″
75
Rio Grande
25º52′35″
−97º27′15″
30
Roanoke
35º54′54″
−76º43′22″
70
Sabine
30º18′13″
−93º44′37″
50
Sacramento
37º30′00″, 38º30′00″
−121º00′00″, −123º00′00″
See notea
St. Lawrence
45º00′22″
−74º47′43″
50
Santee
33º14′00″
−79º30′00″
40
San Joaquin
37º30′00″, 38º30′00″
−121º00′00″, −123º00′00″
See notea
Saskatchewan
See noteb
Savannah
32º31′30″
−81º15′45″
50
Susitna
61º35′00″
−150º22′00″
40
Susquehanna
39º42′00″
−76º15′00″
50
Trinity
29º50′10″
−94º44′57″
30
Yukon
62º45′00″
−164º30′00″
30
NOTES: aRectangular polygons formed by the latitudinal and longitudinal coordinates shown were requested for these rivers; bNo data were requested for the Appalachicola and Saskatchewan Rivers.
OCR for page 235
Oil in the Sea III: Inputs, Fates, and Effects
TABLE I-2 STORET Data Used to Calculate Average Oil and Grease Concentrations in Major Inland Rivers
River
Station name
Parameter code
# of observations
Date(s) of observations
Average concentration (mg L−1)
Columbia
Columbia River at Bradwood, OR
00550
27
4/24/74−10/17/78
1.80
Delaware
Delaware Rvr-2000 yds up buoy R6M-Marcus Hook
00556
107
5/23/88−12/29/98
6.00
Delaware (1990s)
Delaware Rvr-2000 yds up buoy R6M-Marcus Hook
00556
99
1/22/90−12/29/98
5.80
Hudson
Hudson River below Poughkeepsie, NY
00550
2
6/4/70−9/7/71
60.50
James
Buoy 8 (City of Hopewell)
00556
1
7/20/92
19.30
Mississippi
Mississippi River at Venice, LA
00556
229
10/4/73−11/19/96
1.74
Mississippi (1990s)
Mississippi River at Venice, LA
00556
46
1/11/90−11/19/96
0.84
Neuse
Neuse River at 3 locations
00550
7
6/6/73−6/7/73
0.00
Sabine
Sabine River at Ruliff, TX
00556
45
3/27/74−5/9/78
2.50
Sacramento
Sacramento River at Freeport, CA
00550
4
10/25/91−2/2/92
0.83
Susquehanna
Susquehanna R at Rte 40 bridge
00500
2
8/3/78
0.00
Trinity
Trinity River at Liberty, TX
00550
11
5/4/71−8/31/72
8.18
Equation I-1
Li=ciQi,
where Li= average annual load for river i (tonne yr−1),
ci= average oil and grease concentration for river i (mg L−1),
Qi= average annual flow for river i (m3 yr− 1),
tonne= 106 g.
The average annual flow (per calendar year) was determined from USGS daily flow data available for each of the rivers at the nearest nontidally influenced station to that of the reported oil and grease data (Table I-3). For calculations of loads using average concentrations in the 1990s only, average annual flows for those rivers were calculated using only daily flow data from the 1990s.
Using data obtained from the U.S. Bureau of the Census (1998), unit loads per urban land area were calculated as follows:
Equation I-2
where lai= unit load per urban land area for river i (g m−2 yr),
Aui= 1996 urban land area for river i (m2).
The 1996 urban land area in each river basin was determined by using Table I-1 in U.S. Bureau of the Census (1998), which contained land area data for metropolitan areas defined as of June 30, 1996. Metropolitan areas in this table were partitioned into the major river basins identified in Table I-1, coastal areas, the Great Lakes, or areas not discharging to the coast of the United States or Canada (e.g., Great Salt Lake basin). Metropolitan areas contributing urban runoff to the Great Lakes or areas not discharging to the coast of the United States or Canada were not included further in the analysis. It was assumed that oil and grease dis
TABLE I-3 USGS Gages Used to Calculate Average Annual Flows for Major Inland Rivers
River
Station name
Period of record used
Average annual flow (m3 yr−1)
Columbia
14246900: Columbia R at Beaver Army Terminal nr Quincy, Ore
1969, 1992-1997
220,892,000,000
Delaware
01463500: Delaware River at Trenton, NJ
1913-1997
10,441,000,000
Delaware (1990s)
01463500: Delaware River at Trenton, NJ
1990-1997
10,712,000,000
Hudson
01358000: Hudson River at Green Island, NY
1947-1996
12,365,000,000
James
02037500: James River near Richmond, VA
1938-1997
6,209,000,000
Mississippi
07289000: Mississippi River at Vicksburg, MS
1932-1997
537,114,500,000
Mississippi (1990s)
07289000: Mississippi River at Vicksburg, MS
1990-1997
625,760,000,000
Neusea
02089500: Neuse River at Kinston, NC
1983-1997
3,524,394,745
Sabine
08030500: Sabine River nr Ruliff, TX
1960-1997
7,043,181,292
Sacramento
11447650: Sacramento River at Freeport, CA
1949-1997
21,000,000,000
Susquehanna
01578310: Susquehanna River at Conowingo, MD
1968-1997
36,779,000,000
Trinityb
08067000: Trinity River at Liberty, TX
1977, 1979-1986
8,944,000,000
NOTES: aadjusted to Station 02091814 using 1997 data; bmissing flows regressed with Station 08066500: Trinity River at Romayor, TX (y = 0.8559x + 4047.8).
OCR for page 236
Oil in the Sea III: Inputs, Fates, and Effects
charged to the Great Lakes would be biochemically reduced, or would attach to solids and settle out during the extended residence time in the lakes and would therefore not make it to the ocean. Likewise, closed inland basins such as the Great Salt Lake would not discharge to the sea. (Contact NRC staff to obtain information describing how specific metropolitan areas were classified as contributing to major river basins.)
For the majority of the inland river basins, no usable oil and grease data were available in STORET. In addition, the number of observations for the Hudson, James, Neuse, Sacramento, and Susquehanna rivers was very small (2, 1, 7, 4 and 2, respectively). It was therefore decided to use an alternative procedure based on the unit loads of oil and grease per urban land area and per capita calculated from Steps 1-4 to estimate the contributions of oil and grease from these other river basins. The procedure was as follows:
The unit loads of oil and grease per urban land area calculated from Steps 1-4 were used for the other river basins with the following assumptions:
The Hudson and James rivers were assumed to have unit loads of oil and grease per urban land area of 12.22 g m−2 yr−1, the values calculated from 99 observations in the 1990s on the Delaware River. The high unit loadings on the Delaware River are likely due to the highly industrialized nature of the waterway, and the Hudson and James rivers are also very industrialized.
It was assumed that Alaskan rivers (i.e., Copper, Susitna, and Yukon rivers) did not contribute significant loads of oil and grease to the ocean.
All other rivers for which measured data were not adequate or were unavailable were assumed to have unit loads of oil and grease per urban land area of 1.25 g m−2 yr−1. This value was based on the average annual loading for 1990s data from the Mississippi and Delaware rivers together divided by the urban areas in both basins. Rivers for which this value applied included the Alabama-Tombigbee, Altamaha, Apalachicola, Brazos, Colorado (Texas), Columbia, Neuse, Potomac, Rio Grande, Roanoke, Sabine, Sacramento, St. Lawrence, Santee, San Joaquin, Saskatchewan, Savannah, Susquehanna, and Trinity rivers.
Using data obtained from the U.S. Bureau of the Census (1998) and Statistics Canada (2000), the annual loads per unit land area (Lai) were calculated as follows:
Equation I-3
where lai was the unit load for river i as described in Step 5.a. The urban land area, Aui, was calculated in the same manner as described in Step 4 for metropolitan areas in the United States. For metropolitan areas in Canada, Aui was calculated using data from Statistics Canada (2000).
Calculations for the Coastal Zones of the United States and Canada
For the United States, metropolitan areas in U.S. Bureau of the Census (1998) were classified as contributing to coastal basins if they fell within one of the 451 coastal counties defined by Culliton et al. (1990). The individual coastal basin metropolitan areas were then aggregated into the appropriate coastal zones in Figure 1-7. The data for 1997 urban land area for metropolitan areas as of June 30, 1996 (U.S. Bureau of the Census, 1998) were then compiled for each coastal zone. Similarly, data from Statistics Canada (2000) for Canadian metropolitan areas along the coast were grouped into the appropriate coastal zones.
The annual load Lai was calculated for urban areas in each coastal zone i in the United States and Canada using Equation I-3. The unit load per urban land area for coastal zone i, lai, was 12.22 g m−2 yr−1 for coastal zone D, and 1.25 g m−2 yr−1 for all other coastal zones. The unit loads were set at higher values for Coastal Zone D because that is the coastal zone to which the Delaware River discharges. (Contact NRC staff to obtain information describing how specific metropolitan areas were classified as contributing to various coastal zones.)
Because almost one-fourth of the crude oil distillation capacity of the United States is located along the Gulf coast (Radler, 1999), the petroleum refining industry discharges a substantial amount of additional oil and grease to coastal waters in that area. To estimate this contribution, data for oil refineries in Louisiana and Texas (from Radler, 1999) were used to estimate the operating capacity of coastal refineries in these states (Table I-4). The petroleum hydrocarbon discharge was determined by multiplying the operating capacity by an assumed rate of hydrocarbon loss that corresponded to effluent guidelines for these discharges (American Petroleum Institute, National Ocean Industries Association, and Offshore Operators Committee, 2001):
Daily maximum:
6.0 lbs per 1000 barrels of crude produced
Monthly average:
3.2 lbs per 1000 barrels of crude produced
Calculations using each of these guidelines were made, and the average of the two calculations was used as a best estimate of the loadings. This discharge was added to the coastal discharge for coastal zone G.
OCR for page 237
Oil in the Sea III: Inputs, Fates, and Effects
TABLE I-4 Estimated Petroleum Hydrocarbon Discharge to Gulf Coast from Petroleum Refining Industry
State
No. of Operable Refineries on Coasta
Crude Distillation Capacitya (bbl d−1)
Crude Distillation Capacityb (106 tonne yr−1)
Oil and Grease Discharge—Lowc (tonne yr−1)
Oil and Grease Discharge—Highd (tonne yr−1)
Oil and Grease Discharge—Averagee (tonne yr−1)
Texas
14
2,836,100
125466.7
1,503
2,160
2,817
Louisiana
7
948,105
124210.5
502
722
942
TOTAL
21
3,784,205
2,005
2,882
3,759
NOTES: aSOURCE: Radler (1999); b106 tonne yr−1 = 19,000 bbl d−1; cassuming 3.2 lbs of oil and grease are produced per 1000 bbl produced; dassuming 6.0 lbs of oil and grease are produced per 1000 bbl produced; eaverage of low and high estimates.
The total oil and grease loading was determined by adding discharges from inland rivers, urban coastal areas, and the petroleum refinery discharges in the Gulf of Mexico to the appropriate coastal zones.
World Estimates of Oil and Grease
The data used for the calculations of oil and grease loading for North America were not available for other regions of the world. Therefore, a method was needed to extrapolate the North American calculations to the rest of the world. It is widely thought that land-based contributions of oil and grease are due primarily to vehicle operation and maintenance (Bomboi and Hernández, 1991; Fam et al., 1987; Hoffman and Quinn, 1987a, 1987b; Latimer et al., 1990; Latimer and Quinn, 1998; Zeng and Vista, 1997). Thus, oil and grease loading estimates for the world were based on the number of motor vehicles in different regions of the world as reported by World Resources Institute (1998). Oil and grease loading per vehicle in North America (the United States and Canada) was estimated by using Equations I-4 and I-5.
Equation I-4
VEHNA=PNAvehNA=304,078,000×0.72
=218.936,160veh
where VEHNA =
number of vehicles in North America,
PNA =
population of North America (World Resources Institute, 1998),
vehNA =
number of vehicles per capita in North America (World Resources Institute,1998).
Equation I-5
where lNAA =
loading per vehicle in North America based on urban area calculations of total annual load,
LNAA =
annual load of land-based contributions of oil and grease in North America based on urban area calculations (from previous calculations; see Table F-9).
The numbers of vehicles in regions of the world were determined by applying Equation I-4 to regional data in World Resources Institute (1998). These numbers of vehicles were then multiplied by the loading per vehicle in North America obtained from Equation I-5 to obtain a world estimate of loading of oil and grease to the sea via land-based contributions. Because data on actual vehicle usage and maintenance in other countries were unavailable, it was assumed that the loadings of oil and grease per vehicle in North America were representative of oil and grease loadings per vehicle in other parts of the world. This assumption was considered reasonable because, while motor vehicles in other countries of the world are not as well maintained as vehicles in North America and therefore would likely contribute more oil and grease per vehicle while running, motor vehicles are less frequently used in other regions of the world.
Calculations for the Coastal Basins of Mexico
Because of a lack of data regarding urban land area for metropolitan areas in Mexico, the following method was used to calculate the land-based contributions of oil and grease to coastal zones H and I:
Oil and grease loading from Mexico was estimated using Equation I-4 with population and per capita motor vehicle data from World Resources Institute (1998), and then multiplying by the estimated loading per vehicle for the United States and Canada. These calculations yielded a total oil and grease loading from Mexico of 165,801 tonne yr−1.
Metropolitan areas in Mexico with populations of more than 100,000 inhabitants as of 1990 (United Nations, 1998) were partitioned into either coastal zone H or I depending on whether urban drainage from those areas drained to the Gulf of Mexico (zone H) or the Pacific Ocean (zone I). Mexico City and urban areas to the north and east drain to the Grand
OCR for page 238
Oil in the Sea III: Inputs, Fates, and Effects
Drainage Canal, eventually flowing to the Gulf of Mexico (National Research Council, 1995b), and were therefore included in coastal zone H. (Contact NRC staff to obtain a listing of the urban areas and corresponding 1990 populations in each coastal zone.)
The oil and grease loading calculated in Step 1 was allocated to each coastal zone according to the percentage of the Mexican urban population allocated to that coastal zone. Thus, 65 percent of the total oil and grease loading from Mexico was allocated to coastal zone H, and the rest was allocated to coastal zone I.
Estimates of Petroleum Hydrocarbons and Polycyclic Aromatic Hydrocarbons
The land-based loading calculations of oil and grease described thus far were based on available data from the STORET database that was measured using either the Soxhlet extraction method or liquid-liquid extraction method. These methods determine groups of substances with similar physical characteristics on the basis of their common solubility in a specified solvent (American Society for Testing and Materials, 1999). Thus, “oil and grease” as measured by these methods includes not only petroleum hydrocarbons but also other substances, such as lipid material (American Society for Testing and Materials, 1999; Hoffman and Quinn, 1987a). An investigation was done of published literature to determine if quantifications have been made of the amount of petroleum hydrocarbons or polycyclic aromatic hydrocarbons (PAH) in oil and grease. The literature search revealed a scattering of studies that were generally focused on oil and grease data or specific hydrocarbons, but seldom on total hydrocarbons in oil and grease (Table I-5).
Eganhouse and Kaplan’s (1982) study of effluents from wastewater treatment plants in southern California remains the principal study that estimated the proportion of total hydrocarbons in oil and grease. The factor of 0.38 that was applied to oil and grease estimates in the previous National Research Council (1985) report to estimate petroleum hydrocarbon contributions from municipal wastewaters was obtained from the Eganhouse and Kaplan (1982) study. However, wastewater effluent in southern California is not representative of the petroleum hydrocarbon fraction in oil and grease in river water because there are many sources of petroleum hydrocarbons and oil and grease besides municipal wastewaters, the composition of petroleum-derived hydrocarbons varies widely from place to place, and there could be other sources of hydrocarbons such as those produced naturally by aquatic organisms that could be included in oil and grease measurements (Laws, 1993).
New studies were not available that compared concentrations of PAH or total hydrocarbons to oil and grease in water, but Michel (2001) provided data of measured total PAH on the lower Mississippi River in December 2000. These measurements were taken as a result of a spill on the river, but the background measurements of total PAH at three river stations varied from 100 to 156 ng L−1, with an average of 128.3 ng L−1. Using the average oil and grease concentration for the Mississippi River of 0.84 mg L−1 from the STORET data (see Table I-2), the estimated percentage of PAH in oil and grease in the Mississippi River would be about 0.015% based on the average total PAH concentration.
PAH typically constitute 0.1-1% of total petroleum hydrocarbons in oil (Wang et al., 1999b). However, since PAH are fairly soluble in water, they likely constitute a larger portion of total petroleum hydrocarbons in oil in water, so the range was expanded to 0.1-10% of total petroleum hydrocarbons, which was verified with comparisons of relative amounts of measured PAH and total hydrocarbons in water in studies in the literature (Table I-6). Thus, estimates of total petroleum hydrocarbons in the Mississippi River based on the December 2000 average PAH data of Michel (2001) would be from 1280 to 128,000 ng L−1. These estimates, when compared to the measured average oil and grease concentrations in the Mississippi River, are 0.15% to 15% of oil and grease, with a best estimate of 1.5%. The best estimate of total hydrocarbon loading from land-based sources was therefore calculated as 1.5% of the best estimate of oil and grease loading.
RESULTS
The average annual loads of oil and grease discharged to the sea were calculated for those rivers with reported oil and grease data in STORET (Table I-7). These total loads were then normalized to unit loads per urban land area. The final estimates of land-based contributions of oil and grease to the sea via all major inland river basins in the United States and Canada were then determined using the 1990s oil and grease data for the Delaware and Mississippi Rivers (Table I-8) with urban land area data from U.S. Bureau of Census (1998) and Statistics Canada (2000). About two-fifths of the estimated loading in North America was determined from actual measured data in STORET, with the remainder determined using the unit load approach.
The estimates of land-based contributions of oil and grease to the sea from both major inland rivers and coastal areas in the United States and Canada were totaled by coastal basin (Table I-9). Table F-9 also shows calculated values for coastal zones in Mexico, but these loads were not included in the totals for North America (i.e., the United States and Canada). The total loading for North America (3.4 million tonne yr−1) was used to obtain a world estimate of land-based oil and grease loading (9.4 million tonne yr−1; Table I-10). The regional distribution of this loading shows that North America and Europe contribute the majority of land-based oil and grease to the sea.
A factor of 0.015 was applied to the total oil and grease loading to estimate the fraction of hydrocarbons in oil and grease. The estimated worldwide loading of hydrocarbons to
OCR for page 239
Oil in the Sea III: Inputs, Fates, and Effects
TABLE I-5 Summary of Literature Review for Oil and Grease, Hydrocarbon, and Polycyclic Aromatic Hydrocarbon (PAH) Data Due to Land-based Discharges
Citation
Description
Abdullah et al. (1994)
Hydrocarbons (in oil equivalents) in ocean in Peninsular Malaysia
Abdullah et al. (1996)
Oil and grease and hydrocarbons (in oil equivalents) in ocean in Peninsular Malaysia
Baker (1983)
Synthesis of world hydrocarbon inputs
Bamford et al. (1999a)
PAH in the Patapsco River, an urbanized subestuary of the Chesapeake Bay
Bidleman et al. (1990)
Hydrocarbons in South Carolina estuaries
Bomboi and Hernández (1991)
PAH and hydrocarbons in urban runoff in Madrid, Spain
Burns and Saliot (1986)
Synthesis of hydrocarbon budget for Mediterranean Sea
Carey et al. (1990)
Hydrocarbons and PAH in the Mackenzie River, Canada
Cole et al. (1984)
PAH in urban runoff
Connell (1982)
Hydrocarbon budget for estuary near New York, NY
Cross et al. (1987)
PAH and hydrocarbons in coastal Los Angeles, CA
Crunkilton and DeVita (1997)
PAH in Lincoln Creek, WI
DeLeon et al. (1986)
PAH and hydrocarbons in the Mississippi River
Eganhouse and Kaplan (1981)
Hydrocarbons in urban runoff in southern California
Eganhouse et al. (1981)
Hydrocarbons in urban runoff in southern California
Fam et al. (1987)
PAH and hydrocarbons in urban runoff from watersheds in San Francisco Bay, CA
Frankel (1995)
Synthesis of world oil and grease in industrial discharges
Freedman (1989)
Synthesis of hydrocarbon inputs to world’s oceans
Fulton et al. (1993)
PAH in South Carolina estuaries
Gleick (1993)
Synthesis of oil and grease in industrial discharges
Gupta et al. (1981)
Oil and grease in highway runoff at several locations in US; FHWA report
Hall and Anderson (1988)
Hydrocarbons in urban runoff in Burnaby, British Columbia, Canada
Hoffman et al. (1983)
Hydrocarbons in urban runoff in Narragansett Bay, RI
Hoffman et al. (1984)
PAH in urban runoff in RI
Hoffman et al. (1985)
PAH and hydrocarbons in highway runoff in RI
Hoffman and Quinn (1987a, 1987b)
Oil and grease, PAH and hydrocarbons in wastewater treatment plant effluent and urban runoff in combined sewer overflows in RI
Horsfall et al. (1994)
Hydrocarbons in New Calabar River, Nigeria
Hunter et al. (1979)
Hydrocarbons in urban runoff for Philadelphia, PA
Ishaq (1992)
Oil and grease in urban runoff in Riyadh, Saudi Arabia
Ishaq and Alassar (1999)
Oil and grease in urban runoff in Dharan City, Saudi Arabia
Jensen and Jørgensen (1984)
Synthesis of oil and grease and hydrocarbon inputs to the Baltic Sea
Kneip et al. (1982)
Synthesis of oil and grease and hydrocarbons in nonpoint source pollution to New York Bight
Latimer et al. (1990)
PAH and hydrocarbons in urban runoff in Rhode Island
Latimer and Quinn (1998)
Hydrocarbons in dry weather inputs to Narragansett Bay, RI
Laws (1993)
Synthesis of world hydrocarbon inputs
Levins et al. (1979)
Oil and grease in sewage treatment plant effluents at locations in US; EPA report
Lopes and Dionne (1998)
Synthesis of oil and grease, PAH, and hydrocarbons in highway runoff and urban stormwater
MacKenzie and Hunter (1979)
PAH and hydrocarbons in urban runoff for Philadelphia, PA
Makepeace et al. (1995)
Synthesis of oil and grease and hydrocarbons in urban runoff
Mastran et al. (1994)
PAH in Occoquan Reservoir, VA due to boating activity
McCarthy et al. (1997)
PAH in Slave River, Canada
McFall et al. (1985)
PAH in water column of Lake Pontchartrain, LA
Michael (1982)
Synthesis of oil and grease and hydrocarbon inputs to New York Bight
NOAA (1987)
Oil and grease, PAH and hydrocarbon inputs to Narragansett Bay, RI
NRC (1985)
Synthesis of world oil and grease and hydrocarbon inputs to the ocean
Odokuma and Okpokwasili (1997)
Oil and grease in New Calabar River, Nigeria
OTA (1987)
Synthesis of oil and grease contributions to coastal waters in US
Owe et al. (1982)
Hydrocarbons in urban runoff for Syracuse, NY
Perry and McIntyre (1986)
Oil and grease and PAH in highway runoff near London, UK
Perry and McIntyre (1987)
Oil and grease and PAH in highway runoff near London, UK
Petty et al. (1998)
PAH in Missouri River following flood of 1993
Pham and Proulx (1997)
PAH in Montreal wastewater and St. Lawrence River
Pham et al. (1999)
PAH in Montreal wastewater and St. Lawrence River
Rifai et al. (1993)
Oil and grease inputs to Galveston Bay, TX
Roesner (1982)
Synthesis of oil and grease in urban runoff at various locations in US
Rogers (1994)
Synthesis of oil and grease in combined sewer overflows and urban runoff
Schiff and Stevenson (1996)
Oil and grease in urban runoff in San Diego, CA
OCR for page 240
Oil in the Sea III: Inputs, Fates, and Effects
Citation
Description
Shaheen (1975)
Oil and grease in dust in Washington, DC area; EPA report
Stenstrom et al. (1984)
Oil and grease in urban runoff in Richmond, CA
Stenstrom et al. (1987)
Oil and grease and PAH in urban runoff in the San Francisco Bay Area, CA
Telang et al. (1981)
Hydrocarbons in the Marmot Basin, Alberta, Canada
Tomlinson et al. (1980)
Oil and grease in combined sewer overflows, storm drains in Seattle, WA; EPA rpt
USEPA (1996)
Synthesis of impaired rivers and streams due to oil and grease pollution
USEPA (1998)
Synthesis of impaired estuaries due to oil and grease pollution
USEPA (1999)
Synthesis of oil and grease in industrial discharges in US
Wakeham (1977)
Hydrocarbon budget for Lake Washington, WA
Walker et al. (1999)
PAH in urban runoff to Passaic River, NJ
Whipple and Hunter (1979)
Hydrocarbons in urban runoff to the Delaware estuary
Yamane et al. (1990)
Hydrocarbons and PAH in stormwater runoff in Tama River Basin, Tokyo, Japan
Yunker and MacDonald (1995)
PAH in the Mackenzie River, Canada
Yunker et al. (1991)
PAH in the Mackenzie River, Canada
Zeng and Vista (1997)
PAH near San Diego, CA
NOTES: NOAA = National Oceanic and Atmospheric Administration; NRC = National Research Council; OTA = Office of Technology Assessment; USEPA = U.S. Environmental Protection Agency
TABLE I-6 Comparisons of PAH and Total Hydrocarbon Concentrations in Water in Literature
Reference
Description
Total PAH or Aromatics (ng L−1)
Total Hydrocarbons (TH) (ng L−1)
Ratio of PAH:TH
Bomboi and Hernández (1991)
Urban runoff in Madrid, Spain
27,800
1,181,800
0.0235
DeLeon et al. (1986)
Mississippi River
79
435
0.1816
Eganhouse and Kaplan (1981)
Los Angeles River storm runoff (est.)
1,600,000
13,100,000
0.1221
Hunter et al. (1979)
Philadelphia urban runoff
1,120,000
3,690,000
0.3035
Maldonado et al. (1999)
Black Sea
0.045−2.219
1.61−100
0.00045−0.0279
TABLE I-7 Calculated Annual and Unit Loads of Oil and Grease for Major Inland Rivers in North America with STORET Data
River
Land Areaa (m2)
Populationb
Average Annual Load (tonne yr−1)
Unit Load per Urban Land Area (g m−2 yr−1)
Columbia
30,466,548,140
1,263,460
397,606
13.05
Delaware
5,082,592,668
967,893
62,646
12.33
Delaware (1990s)
5,082,592,668
967,893
62,130
12.22
Hudson
21,972,423,133
1,432,124
748,083
34.05
James
7,686,825,713
354,043
119,834
15.59
Mississippi
463,617,454,706
40,383,189
934,579
2.02
Mississippi (1990s)
463,617,454,706
40,383,189
525,638
1.13
Neuse
10,472,875,923
1,162,035
0
0
Sabine
6,964,737,028
374,973
17,608
2.53
Sacramento
30,438,835,267
2,152,519
17,430
0.57
Susquehanna
27,400,261,216
2,788,354
0
0
Trinity
23,581,064,748
4,683,013
73,162
3.10
NOTES: aSource: U.S. Bureau of the Census (1998), Table B-1; includes dry land and land temporarily or partially covered by water; bSource: U.S. Bureau of the Census (1998), Table B-1; based on areas defined as of June 30, 1996.
the sea from land-based sources was therefore 141,000 tonne yr−1 (Table I-11).
A factor of 0.00015 was applied to the total oil and grease loading to estimate the fraction of PAH in oil and grease. The estimated worldwide loading of PAH to the sea from land-based sources was therefore 1,400 tonne yr−1 (Table I-11).
Discussion
The method used to estimate land-based oil and grease, hydrocarbon, and PAH contributions to the sea involved a large degree of uncertainty due to a number of factors, including (but not limited to):
OCR for page 241
Oil in the Sea III: Inputs, Fates, and Effects
TABLE I-8 Final Estimates of Land-based Contributions of Oil and Grease to the Sea via Major Inland River Basins in North America
River
No. of Observations
Avg. Conc. Oil & Grease, Ci (mg L−1)
Average Annual Flow, Qi (m3 yr−1)
Urban Land Area in Watershed, Aui (m2)
Annual Load, Lai (tonne yr−1) Unit Load per
Urban Land Area, Lai (g m−2 yr−1)a
Calculated from STORET data
Delaware (1990s)
99
5.80b
10.7×109
5.1×109
62,130
12.22
Mississippi (1990s)
46
0.84b
625.8×109
463.6×109
525,638
1.13
Subtotal
468.7×109
587,768
Calculated using alternative method
Alabama-Tombigbee
19.8×109
24,890
1.25
Altamaha
5.5×109
6,896
1.25
Apalachicola
21.7×109
27,223
1.25
Brazos
14.4×109
18,039
1.25
Colorado (TX)
14.9×109
18,670
1.25
Columbia
30.5×109
38,206
1.25
Copper
0
0
0
Hudson
22.0×109
268,593
12.22
James
7.7×109
93,964
12.22
Neuse
10.5×109
13,133
1.25
Potomac
2.0×109
2,446
1.25
Rio Grande
43.8×109
54,982
1.25
Roanoke
4.8×109
6,057
1.25
Sabine
7.0×109
8,734
1.25
Sacramento
30.4×109
38,171
1.25
St. Lawrence
19.7×109
24,699
1.25
San Joaquin
46.0×109
57,647
1.25
Santee
26.8×109
33,573
1.25
Saskatchewan
34.7×109
43,542
1.25
Savannah
6.3×109
7,954
1.25
Susitna
0
0
0
Susquehanna
27.4×109
34,361
1.25
Trinity
23.6×109
29,572
1.25
Yukon
0
0
0
Subtotal
419.4×109
851,352
Average
2.68
Total
888.1×109
1,439,352
NOTES: aUnit loads shown for alternate method rivers are those used to calculate annual load; bfreon-gr method used to measure oil and grease concentrations.
TABLE I-9 Final Estimates of Land-based Contributions of Oil and Grease to the Sea by Coastal Zones in North America and Mexico
Coastal Zone
Description
Urban Population in Watershed, Pi (1997)
Urban Land Area in Watershed, Aui (m2)
Annual Load, Lai (tonne yr−1)
Unit Load per Urban Land Area, Lai (g m−2 yr−1)a
A
No urban areas
0
0
0
0
B
Coastal
0
0
0
0
Saskatchewan
293.1×103
34.7×109
43,542
1.25
Subtotal
293.1×103
34.7×109
43,542
C
Coastal
632.3×103
6.8×109
8,529
1.25
St. Lawrence
5,647.8×103
19.7×109
24,699
1.25
Subtotal
6,280.1×103
26.5×109
33,228
D
Coastal 44,
843.3×103
121.7×109
1,487,571
12.22
Delaware
967.9×103
5.1×109
62,130
12.22
Hudson
1,432.1×103
22.0×109
268,593
12.22
James
354.0×103
7.7×109
93,964
12.22
Potomac
99.1×103
2.0×109
2,446
1.25
Susquehanna
2,788.4×103
27.4×109
34,361
1.25
Subtotal
50,484.8×103
185.8×109
1,949,065
OCR for page 242
Oil in the Sea III: Inputs, Fates, and Effects
Coastal Zone
Description
Urban Population in Watershed, Pi (1997)
Urban Land Area in Watershed, Aui (m2)
Annual Load, Lai (tonne yr−1)
Unit Load per Urban Land Area, Lai (g m−2 yr−1)a
E
Coastal
11,839.8×103
79.8×109
100,104
1.25
Altamaha
454.6×103
5.5×109
6,896
1.25
Neuse
1,162.0×103
10.5×109
13,133
1.25
Roanoke
337.1×103
4.8×109
6,057
1.25
Santee
3,198.3×103
26.8×109
33,573
1.25
Savannah
457.2×103
6.3×109
7,954
1.25
Subtotal
17,449.2×103
133.7×109
167,717
F
Coastal
5,355.1×103
42.3×109
53,108
1.25
Alabama-Tombigbee
1,601.4×103
19.8×109
24,890
1.25
Apalachicola
4,016.9×103
21.7×109
27,223
1.25
Subtotal
10,973.3×103
83.9×109
105,222
G
Coastal
10,127.3×103
75.3×109
94,398
1.25
Gulf coast refineriesb
—
—
2,882
—
Brazos
987.8×103
14.4×109
18,039
1.25
Colorado (TX)
1,173.7×103
14.9×109
18,670
1.25
Mississippi
40,383.2×103
463.6×109
525,638
1.13
Rio Grande
1,410.0×103
43.8×109
54,982
1.25
Sabine
375.0×103
7.0×109
8,734
1.25
Trinity
4,683.0×103
23.6×109
29,572
1.25
Subtotal
59,139.9×103
642.6×109
752,913
Hc
Coastal and inland rivers
30,159.2×103
108,189
I
No urban areas
0
0
0
0
Jc
Coastal and inland rivers
16,060.2×103
57,612
K
Coastal
18,331.5×103
98.9×109
123,976
1.25
L
Coastal
7,686.2×103
43.3×109
54,349
1.25
Sacramento
2,152.5×103
30.4×109
38,171
1.25
San Joaquin
2,382.3×103
46.0×109
57,647
1.25
Subtotal
12,221.1×103
119.7×109
150,168
M
Coastal
5,946.3×103
54.0×109
67,725
1.25
Columbia
1,263.5×103
30.5×109
38,206
1.25
Subtotal
7,209.7×103
84.5×109
105,931
N
Coastal
2,136.0×103
3.5×109
4,332
1.25
O
Coastal
869.9×103
1.6×109
1,949
1.25
P
Coastal
251.0×103
4.4×109
5,514
1.25
Copper
0
0
0
0
Susitna
0
0
0
0
Subtotal
251.0×103
4.4×109
5,514
Q
Coastal
0
0
0
0
Yukon
0
0
0
0
Totalc
188,277.0×103
1,419.7×109
3,443,557
NOTES: aUnit loads shown are those used to calculate corresponding annual load; bSee Table I-4 for calculation of refinery loading; cTotal does not include Coastal Zones in Mexico.
TABLE I-10 World Estimates of Land-based Sources of Oil and Grease to the Sea
Region
Population (WRI 1998)
Motor Vehicles Per Capita (WRI 1998)
Number of Vehicles
Loading per Vehicle (tonne veh−1)
Loading (tonne yr−1)
Africa
778,484,000
0.02
15,569,680
0.01573
244,889
Europe
729,406,000
0.27
196,939,620
0.01573
3,097,582
North America
304,078,000
0.72
218,936,160
0.01573
3,443,557
Central America
130,710,000
0.11
14,378,100
0.01573
226,147
South America
331,889,000
0.09
29,870,010
0.01573
469,813
Asia
3,588,877,000
0.03
107,666,310
0.01573
1,693,439
Oceania
29,460,000
0.43
12,667,800
0.01573
199,247
Total
9,374,674
OCR for page 243
Oil in the Sea III: Inputs, Fates, and Effects
TABLE I-11 Final Estimates of Worldwide Land-based Contributions of Hydrocarbons and Polycyclic Aromatic Hydrocarbons (PAH) to the Sea
World Region
Coastal Zone
Description
Hydrocarbons (tonne yr−1)
PAH (tonne yr−1)
North Americaa
A
No urban areas
0
0
B
Coastal
0
0
Saskatchewan
653
7
Subtotal
653
7
C
Coastal
128
1
St. Lawrence
370
4
Subtotal
498
5
D
Coastal
22,314
223
Delaware
932
9
Hudson
4,029
40
James
1,409
14
Potomac
37
0
Susquehanna
515
5
Subtotal
29,236
292
E
Coastal
1,502
15
Altamaha
103
1
Neuse
197
2
Roanoke
91
1
Santee
504
5
Savannah
119
1
Subtotal
2,516
25
F
Coastal
797
8
Alabama-Tombigbee
373
4
Apalachicola
408
4
Subtotal
1,578
16
G
Coastal
1,416
14
Gulf coast refineriesb
43
0
Brazos
271
3
Colorado (TX)
280
3
Mississippi
7,885
79
Rio Grande
825
8
Sabine
131
1
Trinity
444
4
Subtotal
11,294
113
Ha
Coastal and inland rivers
1,623
16
Ia
No urban areas
0
0
J
Coastal and inland rivers
864
9
K
Coastal
1,860
19
L
Coastal
815
8
Sacramento
573
6
San Joaquin
865
9
Subtotal
2,253
23
M
Coastal
1,016
10
Columbia
573
6
Subtotal
1,589
16
N
Coastal
65
1
O
Coastal
29
0
P
Coastal
83
1
Copper
0
0
Susitna
0
0
Subtotal
83
1
Q
Coastal
0
0
Yukon
0
0
Subtotala
51,653
517
Africa
3,673
37
Europe
46,464
465
Central America
3,392
34
South America
7,047
70
Asia
25,402
254
Oceania
2,989
30
TOTAL
140,620
1,406
NOTES: aSubtotal for North America does not include Coastal Zones in Mexico; bSee Table I-4 for calculation of refinery loading.
OCR for page 244
Oil in the Sea III: Inputs, Fates, and Effects
Lack of data; only nine major rivers in the United States had oil and grease data in the U.S. Environmental Protection Agency’s STORET data base, and several of these consisted of very few observations.
Differences in measuring and reporting data; most of the available oil and grease data in STORET was gathered using either the Soxhlet extraction method or the liquid-liquid extraction method. The minimum detection limit (denoted off-scale low in the STORET records) and approach for reporting values measured below the detection limit varied with location and time. For example, the minimum detection limit on the Delaware River was 2 mg L−1 for data reported from 1988-1994, and 5 mg L−1 for data reported after 1994. By comparison, the minimum detection limit on the Mississippi River was 1 mg L−1 for the entire period of record (1973-1996).
Adjustment of off-scale low measurements; these values were set to half their reported value even though the actual value was unknown.
Estimating the proportion of petroleum-related hydrocarbons and PAH in oil and grease measurements
Quantifying the uncertainty in the estimates presented in this analysis was not possible, but a reasonable estimate of the low and high ranges of the calculated oil and grease values was made by assuming that the data available from the 1990s for the Mississippi and Delaware rivers, respectively, represented the low and high bounds of oil and grease unit loading for the rivers for which STORET data were unavailable in the 1990s, and for coastal zones in North America and the world (Table I-12). Based on these assumptions, the range of worldwide loadings of land-based sources of oil and grease to the sea was 4.5 million−33.3 million tonne yr− 1, with a best estimate of 9.4 million tonne yr−1. The values shown in Table I-12 also reflect low, best, and high estimates of oil and grease loadings from Gulf coast refineries. Calculations of oil and grease discharges using daily maximum guidelines (6.0 lbs per 1000 barrels of crude produced) were used as a high estimate of these loadings, while calculations using the monthly average guidelines (3.2 lbs per 1000 barrels of crude produced) were used as a low estimate. The average of the two calculations was used as a best estimate of the loadings.
Estimates of total petroleum hydrocarbons in the Mississippi River were based on the December 2000 average PAH data of Michel (2001), the assumption that PAH constitute 0.1%−10% of total petroleum hydrocarbons, and the 1990s’ measured average oil and grease concentration of 0.84 mg L−1. Thus, using the lower bound of PAH fraction in total hydrocarbons, a lower bound for estimated hydrocarbons in oil and grease was 0.15%, while an upper bound of hydrocarbons as 15% of oil and grease was determined assuming PAH constitute 10% of total petroleum hydrocarbons. The final range of estimates of total hydrocarbons were therefore made by assuming that the low estimate corresponded with the low percentage of total hydrocarbons (i.e., 0.15%) in the low estimate of oil and grease loading, the best estimate corresponded with 1.5% of total hydrocarbons in the best estimate of oil and grease loading, and the high estimate corresponded with the high percentage of total hydrocarbons (i.e., 15%) in the high estimate of oil and grease loading (Table I-13). Thus, the range of land-based petroleum hydrocarbon loading to the sea was 6,800−5,000,000 tonne yr−1, with a best estimate of 141,000 tonne yr−1.
The application of the PAH data of Michel (2001) on the Mississippi River involved uncertainties regarding the degree to which that data were representative of distributions of PAH in land-based discharges to the sea via rivers and coastal discharges. Part of this uncertainty arises from the lack of consistent PAH measurements in the water column. A review of STORET and the USGS’ National Water Information Service (NWIS) data revealed less than a dozen measurements of PAH above detection limits on rivers in the United States. Furthermore, reported water column PAH concentrations in the literature were not consistent with respect to the constituents reported, did not use the same measurement methods, and/or did not include particulate and dissolved concentrations of PAH. Nonetheless, literature-reported data and data provided by Baker (2001) on the Susquehanna River indicated that the Michel (2001) data were within a reasonable range for river total PAH concentrations. Thus, the range of the background measurements of total PAH on the Mississippi River by Michel (2001) (i.e., 100 to 156 ng L−1, with an average of 128.3 ng L−1) were compared with the average oil and grease concentration for the Mississippi River of 0.84 mg L−1 to determine the estimated range of PAH in oil and grease as 0.012% to 0.019%, with a best estimate of 0.015%. The low estimate of PAH loading to the sea from land-based sources was therefore estimated as 0.012% of the low estimate of oil and grease loading, and the high PAH loading estimate was calculated as 0.019% of the high estimate of oil and grease loading. The best estimate of PAH loading from land-based sources was calculated using 0.015% of the best estimate of oil and grease loading (Table I-13). The range of PAH loading to the sea from land-based sources was 500−6,300 tonne yr−1, with a best estimate of 1,400 tonne yr−1.
Comparison of Estimates of Land-Based Loading with Other Estimates
The average oil and grease loading of 2.68 g m−2 yr−1 estimated in this study (see Table I-8) was comparable to oil and grease loadings estimated for urban areas in other studies (Table I-14). The range of estimates presented in the current analysis (1.13−12.22 g m−2 yr−1) encompassed the estimates of the previous studies. Perry and McIntyre’s (1986) estimate was actually an event-based calculation that should be higher than an annual load. In addition, the estimates by
OCR for page 245
Oil in the Sea III: Inputs, Fates, and Effects
TABLE I-12 Ranges of Worldwide Land-based Contributions of Oil and Grease to the Sea
Unit Load Based on Urban Area (g m−2 yr−1)
Annual Load (tonne yr−1)
World Region
Coastal Zone
Description
Low
Best Est.
High
Low
Best Est.
High
North Americaa
A
No urban areas
0
0
0
0
0
0
B
Coastal
0
0
0
0
0
0
Saskatchewan
1.13
1.25
12.22
39,367
43,542
424,440
Subtotal
39,367
43,542
424,440
C
Coastal
1.13
1.25
12.22
7,711
8,529
82,137
St. Lawrence
1.13
1.25
12.22
22,330
24,699
240,759
Subtotal
30,041
33,228
323,896
D
Coastal
1.13
12.22
12.22
137,971
1,487,571
1,487,571
Delaware
12.22
12.22
12.22
62,130
62,130
62,130
Hudson
1.13
12.22
12.22
24,912
268,593
268,593
James
1.13
12.22
12.22
8,715
93,964
93,964
Potomac
1.13
1.25
12.22
2,211
2,446
23,843
Susquehanna
1.13
1.25
12.22
31,066
34,361
334,943
Subtotal
267,005
1,949,065
2,271,044
E
Coastal
1.13
1.25
12.22
90,504
100,104
975,790
Altamaha
1.13
1.25
12.22
6,234
6,896
67,218
Neuse
1.13
1.25
12.22
11,874
13,133
128,021
Roanoke
1.13
1.25
12.22
5,476
6,057
59,043
Santee
1.13
1.25
12.22
30,353
33,573
327,262
Savannah
1.13
1.25
12.22
7,191
7,954
77,533
Subtotal
151,633
167,717
1,634,867
F
Coastal
1.13
1.25
12.22
48,015
53,108
517,689
Alabama-Tombigbee
1.13
1.25
12.22
22,503
24,890
242,625
Apalachicola
1.13
1.25
12.22
24,613
27,223
265,366
Subtotal
95,131
105,222
1,025,680
G
Coastal
1.13
1.25
12.22
85,345
94,398
920,166
Gulf coast refineries
—
—
—
2,005
2,882
3,759
Brazos
1.13
1.25
12.22
16,309
18,039
175,838
Colorado (TX)
1.13
1.25
12.22
16,879
18,670
181,989
Mississippi
1.13
1.13
1.13
525,638
525,638
525,638
Rio Grande
1.13
1.25
12.22
49,709
54,982
535,947
Sabine
1.13
1.25
12.22
7,896
8,734
85,137
Trinity
1.13
1.25
12.22
26,736
29,572
288,257
Subtotal
730,517
752,913
2,716,731
Ha
Coastal and inland rivers
52,405
108,189
383,817
I
No urban areas
0
0
0
0
0
0
Ja
Coastal and inland rivers
27,906
57,612
204,387
K
Coastal
1.13
1.25
12.22
112,086
123,976
1,208,486
L
Coastal
1.13
1.25
12.22
49,137
54,349
529,786
Sacramento
1.13
1.25
12.22
34,511
38,171
372,087
San Joaquin
1.13
1.25
12.22
52,118
57,647
561,928
Subtotal
135,767
150,168
1,463,800
M
Coastal
1.13
1.25
12.22
61,230
67,725
660,166
Columbia
1.13
1.25
12.22
34,542
38,206
372,425
Subtotal
95,772
105,931
1,032,591
N
Coastal
1.13
1.25
12.22
3,916
4,332
42,223
O
Coastal
1.13
1.25
12.22
1,762
1,949
19,002
P
Coastal
1.13
1.25
12.22
4,985
5,514
53,746
Copper
0
0
0
0
0
0
Susitna
0
0
0
0
0
0
Subtotal
4,985
5,514
53,746
Q
Coastal
0
0
0
0
0
0
Yukon
0
0
0
0
0
0
Subtotala
1,667,983
3,443,557
12,216,509
Africa
118,619
244,889
868,779
Europe
1,500,400
3,097,582
10,989,115
Central America
109,541
226,147
802,290
South America
227,567
469,813
1,666,729
Asia
820,264
1,693,439
6,007,717
Oceania
96,511
199,247
706,856
TOTAL
4,540,885
9,374,674
33,257,994
NOTES: aSubtotal for North America does not include Coastal Zones in Mexico.
OCR for page 246
Oil in the Sea III: Inputs, Fates, and Effects
TABLE I-13 Ranges of Worldwide Land-based Contributions of Hydrocarbons and Polycyclic Aromatic Hydrocarbons (PAH) to the Sea
Hydrocarbons (tonne yr−1)
PAH (tonne yr−1)
World Region
Coastal Zone
Description
Low
Best Est.
High
Low
Best Est.
High
North Americaa
A
No urban areas
0
0
0
0
0
0
B
Coastal
0
0
0
0
0
0
Saskatchewan
59
653
63,666
5
7
81
Subtotal
59
653
63,666
5
7
81
C
Coastal
12
128
12,471
1
1
16
St. Lawrence
33
370
36,114
3
4
46
Subtotal
45
498
48,584
4
5
62
D
Coastal
207
22,314
223,136
17
223
283
Delaware
93
932
9,320
7
9
12
Hudson
37
4,029
40,289
3
40
51
James
13
1,409
14,095
1
14
18
Potomac
3
37
3,576
0
0
5
Susquehanna
47
515
50,241
4
5
64
Subtotal
401
29,236
340,657
32
292
431
E
Coastal
136
1,502
149,368
11
15
185
Altamaha
9
103
10,083
1
1
13
Neuse
18
197
19,203
1
2
24
Roanoke
8
91
8,856
1
1
11
Santee
46
504
49,089
4
5
62
Savannah
11
119
11,630
1
1
15
Subtotal
227
2,516
245,230
18
25
311
F
Coastal
72
797
77,653
6
8
98
Alabama-Tombigbee
34
373
36,394
3
4
46
Apalachicola
37
408
39,805
3
4
50
Subtotal
143
1,578
153,852
11
16
195
G
Coastal
128
1,416
138,025
10
14
175
Gulf coast refineries
3
43
564
0
0
1
Brazos
24
271
26,376
2
3
33
Colorado (TX)
25
280
27,298
2
3
35
Mississippi
788
7,885
78,846
63
79
100
Rio Grande
75
825
80,392
6
8
102
Sabine
12
131
12,771
1
1
16
Trinity
40
444
43,239
3
4
55
Subtotal
1,096
11,294
407,510
88
113
516
Ha
Coastal and inland rivers
79
1,623
57,573
6
16
73
I
No urban areas
0
0
0
0
0
0
Ja
Coastal and inland rivers
42
864
30,658
3
9
39
K
Coastal
168
1,860
181,273
13
19
230
L
Coastal
74
815
79,468
6
8
101
Sacramento
52
573
55,813
4
6
71
San Joaquin
78
865
84,289
6
9
107
Subtotal
204
2,253
219,570
16
23
278
M
Coastal
92
1,016
99,025
7
10
125
Columbia
52
573
55,864
4
6
71
Subtotal
144
1,589
159,889
11
16
196
N
Coastal
6
65
6,333
0
1
8
O
Coastal
3
29
2,850
0
0
4
P
Coastal
7
83
8,062
1
1
10
Copper
0
0
0
0
0
0
Susitna
0
0
0
0
0
0
Subtotal
7
83
8,062
1
1
10
Q
Coastal
0
0
0
0
0
0
Yukon
0
0
0
0
0
0
Subtotala
2,502
51,653
1,832,476
200
517
2,321
Africa
178
3,673
130,317
14
37
165
Europe
2,251
46,464
1,648,387
180
465
2,088
Central America
164
3,392
120,343
13
34
152
South America
341
7,047
250,009
27
70
317
Asia
1,230
25,402
901,158
98
254
1,141
Oceania
145
2,989
106,028
12
30
134
TOTAL
6,811
140,620
4,988,699
545
1,406
6,319
NOTES: aSubtotal for North America does not include Coastal Zones in Mexico.
OCR for page 247
Oil in the Sea III: Inputs, Fates, and Effects
TABLE I-14 Comparison of Estimated Loading of Oil and Grease in Urban Areas
Location
Unit Load per Urban Land Area (g m−2 yr−1)
Reference
Comments
United States and Canada
2.68
This work
Los Angeles River, Calif.
1.28
Eganhouse and Kaplan (1981)
Total hydrocarbons
Narragansett Bay, R. I.
2.13
Hoffman et al. (1983)
Petroleum hydrocarbons
United Kingdom (roadway runoff)
11.016
Perry and McIntyre (1986)
Calculated from oil mass loading of 0.17 kg ha−1 mm of runoff−1 and annual average rainfall of 648 mm
Richmond, Calif.
1.25
Stenstrom et al. (1984)
Hoffman et al. (1983) and Eganhouse and Kaplan (1981) were actually for hydrocarbons, which constitute part, but not all, of oil and grease. Thus, the lower loadings calculated in those studies agree nicely with the loading estimate from the current study.
The estimate of total oil and grease loading was also compared with estimates of dissolved organic carbon (DOC) inputs to the sea from land-based sources (Table I-15). Since oil and grease constitutes a small part of DOC, the current estimates of oil and grease loading should be considerably lower than estimates of DOC flux. This was confirmed for published estimates of global contributions of DOC from rivers to oceans, although the current estimates of oil and grease loading were higher on the Delaware River than corresponding published estimates of DOC flux by Leenheer (1982).
The current study’s best estimates of oil and grease loadings to coastal zone G were on the order of 800,000 tonne yr− 1, which was much greater than the 27,000 tonne yr−1 estimated by the Caribbean Environment Programme (1994) for the Gulf coast of the United States. It is likely that the Caribbean Environment Programme (1994) data included neither the Mississippi River, which accounted for over 500,000 tonne yr−1 of the oil and grease loading in the current study, nor the contributions from Gulf coast refineries. Thus, the corresponding current best estimate was about 10 times greater than the Caribbean Environment Programme (1994) estimate of loading of oil and grease to the Gulf coast.
The calculations of oil and grease loadings presented in this analysis were based on unit loadings per urban land area. Comparison calculations were also made based on unit loadings per capita urban population using 1997 urban populations in the United States obtained from U.S. Bureau of the Census (1998) and 1996 urban populations in Canada from Statistics Canada (2000). These calculations resulted in oil and grease loadings of the same magnitude as calculations based on unit loadings per urban land area (Table I-16).
To test the assumption that the measured oil and grease concentrations used for the current analysis were representative of ambient concentrations in North American rivers, average measured oil and grease concentrations for the 1990s STORET data on the Mississippi and Delaware rivers were compared with a database consisting of all of the 1990s oil and grease measurements gathered from STORET (145 data points) and 704 additional data points from USGS sampling stations on rivers in Louisiana in the 1990s (Table I-17 and Figure I-1). For the Mississippi River and Louisiana sampling, the minimum detection limit was 1 mg L−1, while the minimum detection limit on the Delaware River was either 2 mg L−1 or 5 mg L−1. Measurements reported to be less than the minimum detection limit were assumed to be half of their reported value (i.e., if a measurement was reported as <1 mg L−1, 0.5 mg L−1 was entered in the database).
The comparisons shown in Table I-17 and Figure I-1 indicate that the oil and grease concentrations used for the Mississippi River in this analysis corresponded nicely with the separate measurements in Louisiana by the USGS and hence the overall database. This result was not surprising since a large portion of the Louisiana data were also measured on the Mississippi River. The Delaware River concentrations were higher than the other 1990s data collected, but the high industrialization of that river could account for higher oil and grease discharges. Thus, the oil and grease concentrations obtained from the STORET database were reasonable.
As a further test of the reasonableness of the estimates of land-based loadings of oil and grease presented here, these loads were compared to oil consumption. According to a recent BP Amoco report (BP Amoco, 2000), North America consumed 1047.1 million tonnes of oil in 1999. Assuming that all of the 3.4 million tonne yr−1 of oil and grease estimated in this study as returning to the sea from land-based sources were petroleum-derived, then only about 0.3 percent of consumed oil was returned to the sea from land-based sources. Furthermore, BP Amoco (2000) estimated that the North American annual consumption of oil was broken down as follows:
Gasoline
428.8 million tonne yr−1
Middle Distillates
319.6
Fuel Oil
77.3
Other
221.4
Total
1047.1 million tonne yr−1
Again, assuming that (1) all gasoline products were completely consumed by use (although PAH in urban runoff are
OCR for page 248
Oil in the Sea III: Inputs, Fates, and Effects
TABLE I-15 Comparison of Published Estimates of Dissolved Organic Carbon (DOC) Inputs from Land-based Sources to Oil and Grease Loadings Estimated in this Study
Reference
Description
Estimated DOC Flux (tonne C yr−1)
Estimated Oil and Grease Loading (tonne yr−1)
Percent of DOC Flux
Degens and Ittekkot (1983)
DOC transported by rivers into ocean
285,000,000
9,374,674
3.29
Degens et al. (1991)
DOC flux from Africa
24,700,000
244,889
0.10
Degens et al. (1991)
DOC flux from Asia
94,000,000
1,693,439
1.80
Degens et al. (1991)
DOC flux from North America
33,800,000
3,443,557
10.19
Degens et al. (1991)
DOC flux from South America
44,200,000
469,813
1.06
Kobak (1988)a
Inflow of organic matter with river runoff
210,000,000
9,374,674
4.46
Leenheer (1982)
DOC flux from Alabama-Tombigbee
537,000
24,890
4.64
Leenheer (1982)
DOC flux from Apalachicola
136,000
27,223
20.02
Leenheer (1982)
DOC flux from Columbia
1,346,000
38,206
2.84
Leenheer (1982)
DOC flux from Delaware
50,000
62,130
124.26
Leenheer (1982)
DOC flux from Mississippi
3,477,000
525,638
15.12
Leenheer (1982)
DOC flux from Potomac
1,070,000
2,446
0.23
Leenheer (1982)
DOC flux from Sacramento
77,000
38,171
49.57
Leenheer (1982)
DOC flux from Susitna
231,000
0
0.00
Leenheer (1982)
DOC flux from Susquehanna
225,000
34,361
15.27
Leenheer (1982)
DOC flux from Yukon
2,411,000
0
0.00
Leenheer (1982)b
DOC flux from United States
10,156,000
3,443,557
33.91
Meybeck (1988)c
DOC export as estimated by morphoclimatic zones
234,200,000
9,374,674
4.00
Pocklington and Tan (1983)
DOC flux from St. Lawrence
1,710,000
24,699
1.44
Schlesinger (1997)
Riverine flux of dissolved organic carbon
400,000,000
9,374,674
2.34
Siegenthaler and Sarmiento (1993)d
River inputs
800,000,000
9,374,674
1.17
Spitzy and Ittekkot (1991)
Global riverine DOC flux
218,000,000
9,374,674
4.30
NOTES: aAs cited in Kagan (1995); bLeenheer (1982) calculation is for US only; calculations in this work are for North America; cAs cited in Spitzy and Ittekkot (1991); dAs cited in McCarthy (2000).
FIGURE I-1 Plot of percent exceedence values for 1990s STORET data (Delaware and Mississippi Rivers), 1990s USGS Louisiana data, and all data combined.
OCR for page 249
Oil in the Sea III: Inputs, Fates, and Effects
TABLE I-16 Comparison of Estimates of Worldwide Land-based Contributions of Oil and Grease to the Sea Based on Unit Loads per Urban Land Area and Unit Loads per Capita Urban Population
World Region
Coastal Zone
Description
Annual Load Based on Pop. (tonne yr−1)
Annual Load Based on Area (tonne yr−1)
North Americaa
A
No urban areas
0
0
B
Coastal
0
0
Saskatchewan
41,655
43,542
Subtotal
41,655
43,542
C
Coastal
8,987
8,529
St. Lawrence
80,278
24,699
Subtotal
89,265
33,228
D
Coastal
2,878,535
1,487,571
Delaware
62,130
62,130
Hudson
91,929
268,593
James
22,726
93,964
Potomac
1,409
2,446
Susquehanna
39,634
34,361
Subtotal
3,096,364
1,949,065
E
Coastal
168,292
100,104
Altamaha
6,462
6,896
Neuse
16,517
13,133
Roanoke
4,792
6,057
Santee
45,462
33,573
Savannah
6,499
7,954
Subtotal
248,024
167,717
F
Coastal
76,118
53,108
Alabama-Tombigbee
22,762
24,890
Apalachicola
57,096
27,223
Subtotal
155,976
105,222
G
Coastal
143,951
94,398
Gulf coast refineriesb
2,882
2,882
razos
14,040
18,039
Colorado (TX)
16,683
18,670
Mississippi
525,638
525,638
Rio Grande
20,042
54,982
Sabine
5,330
8,734
Trinity
66,565
29,572
Subtotal
795,130
752,913
Ha
Coastal and inland rivers
157,387
108,189
I
No urban areas
0
0
Ja
Coastal and inland rivers
83,810
57,612
K
Coastal
260,566
123,976
L
Coastal
109,253
54,349
Sacramento
30,596
38,171
San Joaquin
33,863
57,647
Subtotal
173,711
150,168
M
Coastal
84,521
67,725
Columbia
17,959
38,206
Subtotal
102,480
105,931
N
Coastal
30,361
4,332
O
Coastal
12,364
1,949
P
Coastal
3,568
5,514
Copper
0
0
Susitna
0
0
Subtotal
3,568
5,514
Q
Coastal
0
0
Yukon
0
0
Subtotala
5,009,464
3,443,557
Africa
356,249
244,889
Europe
4,506,162
3,097,582
Central America
328,984
226,147
South America
683,454
469,813
Asia
2,463,506
1,693,439
Oceania
289,851
199,247
TOTAL
13,637,670
9,374,694
NOTES: aSubtotal for North America does not include Coastal Zones in Mexico; bSee Table F-4 for calculation of refinery loading.
OCR for page 250
Oil in the Sea III: Inputs, Fates, and Effects
TABLE I-17 Comparison of STORET Oil and Grease Data Used in this Study with 1990s USGS Oil and Grease Data for Louisiana
Description
Delaware River
Mississippi River
USGS Data
All Data
Statistics
Number of observations
99
46
704
849
Minimum concentration (mg L−1)
1.0
0.5
0.5
0.5
Maximum concentration (mg L−1)
122.7
6
81
122.7
Average concentration (mg L−1)
5.80
0.84
1.27
1.77
Standard deviation (mg L−1)
13.21
0.94
4.65
6.35
Percent exceedence
Mississippi 1990s average = 0.84 mg L−1
100 percent
24.6 percent
21.1 percent
30.4 percent
Delaware 1990s average = 5.80 mg L−1
21.2 percent
2.3 percent
2.6 percent
4.7 percent
automobile exhaust based), and (2) fuel oil was completely consumed (i.e., there was no oily waste discharged by users of fuel oil), then the land-based sources would be derived only from the use of middle distillate fractions that end up on the land surface or in municipal and industrial discharges. Expressing the best estimate of the land-based oil that was returned to the sea as a fraction of the total middle distillate consumption gives a ratio of 3.4/320, or 1.1 percent, which is still a very small percentage.
Table I-18 shows comparisons of the computed land-based loads presented in the current study for North America and other locations with the BP Amoco (2000) data. Note the ratio of land-based sources was very consistent for all countries shown.
The best estimate of petroleum hydrocarbon loading from land-based sources was about 8 times smaller than the best estimate from the National Research Council (1985), and was much smaller than other previous world estimates (Table I-19). Although estimates presented here were considerably different than the studies in Table I-19, the calculations used in this analysis were based on more measured data than in these previous studies, including the National Research Council (1985). The approach used in the current study was also consistent with methods for estimating pollutant loads from urban runoff. The upper range of the current estimates agreed fairly well with previous studies, but the 1990s STORET data suggest that the best estimate may be much lower than previous studies indicated.
Literature-reported data and data provided by Baker (2001) on the Susquehanna River confirmed that the Michel (2001) data were within a reasonable range for river total PAH concentrations (Table I-20). In addition, estimation of river PAH concentrations were made using average annual flows calculated from available flow data (Table I-3) with PAH loadings calculated for corresponding rivers in this study (Table I-13). The average of these calculated concentrations ranged from 242 to 2,900 ng L−1, with a best average concentration of 800 ng L−1 (Table I-21). While this concentration was greater than ambient river concentrations reported by other studies, it represents a conservative estimate of PAH concentrations in river water using the best available data. Furthermore, the calculated concentrations of PAH in the Mississippi River corresponded nicely with the range of total PAH measured by Michel (2001).
TABLE I-18 Comparison of Oil Consumption with Estimated Oil and Grease Loading from Land-based Sources to the Sea
Location
1999 Oil Consumptiona (million tonne yr−1)
Oil and Grease Loading to the Sea from Land-based Sourcesb (million tonne yr−1)
Ratio of Oil and Grease Loading to the Sea to Oil Consumption (percent)
North America
1047.1
3.4
0.3
South and Central America
218.8
0.7
0.3
Europe
755.2
3.1
0.4
Africa
115.5
0.2
0.2
NOTES: aSource: BP Amoco (2000); bCalculated in this study.
OCR for page 251
Oil in the Sea III: Inputs, Fates, and Effects
TABLE I-19 Comparison of Petroleum Hydrocarbon Loading Estimates from Land-based Sources from this Work and Other Studies
Hydrocarbon Loading (tonne yr−1)
Reference
Comments
Low
Best Estimate
High
World estimates
Baker (1983)
Petroleum hydrocarbons from municipal wastes, industrial waste, and runoff
700,000
1,400,000
2,800,000
National Research Council (1985)
World estimate of land-based sources
600,000
1,200,000
3,100,000
Van Vleet and Quinn (1978)
Petroleum hydrocarbons from municipal wastes only based on Rhode Island treatment plants
—
200,000
—
This work
World estimate of land-based sources
6,800
141,000
5,000,000
Ratio (this work: National Research Council [1985]
0.01
0.12
1.61
North American estimates
Eganhouse and Kaplan (1982)
US input of petroleum hydrocarbons based on mass emission rate for wastewater effluent in southern California
—
120,600
—
This work
North American estimate of land-based sources
2,500
52,000
1,800,000
TABLE I-20 Comparisons of Total PAH Concentrations in Literature, Baker (2001), and Michel (2001)
Reference
Description
Range or Average Measured Total PAH Concentrations (ng L−1)
Baker (2001)
Susquehanna River, Pennsylvania
17.01−150.81
Bidleman et al. (1990)
Sampit River, South Carolina
6.8
Gustafson and Dickhut (1997a)
Elizabeth River, Virginia
91.4
Gustafson and Dickhut (1997b)
York River, Virginia
29.15
Michel (2001)a
Mississippi River, Louisiana
100−156
Ollivon et al. (1999)
Seine River, France
94.44
Ollivon et al. (1999)
Marne River, France
148.35
aData used in the current study.
TABLE I-21 Estimated Concentrations of Polycyclic Aromatic Hydrocarbon Concentrations Based on Calculated Loadings
Estimated Concentration (ng L−1)
River
Annual Flow (106 m3 yr−1)
Low
Best
High
Columbia
220,892
19
26
320
Delaware
10,712
696
870
1,102
Hudson
12,365
242
3,258
4,127
James
6,209
168
2,270
2,875
Mississippia
625,760
101
126
160
Neuse
3,524
404
559
6,902
Sabine
7,043
135
186
2,297
Sacramento
21,000
197
273
3,366
Susquehanna
36,779
101
140
1,730
Trinity
8,944
359
496
6,124
Average
95,323
242
820
2,900
aEstimated oil and grease loading for Mississippi River was the same for low, best and high estimates of PAH loading (see Tables I-12 and I-13).
OCR for page 252
Oil in the Sea III: Inputs, Fates, and Effects
This page in the original is blank.
Representative terms from entire chapter:
grease loading
