U.S. Department of the Interior

U.S. Geological Survey

Scientific Investigations Report 2011–5135

Radium Content of Oil- and Gas-Field Produced Waters 

in the Northern Appalachian Basin (USA): 

Summary and Discussion of Data

Radium Content of Oil- and Gas-Field Produced Waters 

in the Northern Appalachian Basin (USA): 

Summary and Discussion of Data

By E.L. Rowan, M.A. Engle, C.S. Kirby, and T.F. Kraemer

Scientific Investigations Report 2011–5135

U.S. Department of the Interior

U.S. Geological Survey
U.S. Department of the Interior

KEN SALAZAR, Secretary

U.S. Geological Survey

Marcia K. McNutt, Director

U.S. Geological Survey, Reston, Virginia: 2011

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Suggested citation:

Rowan, E.L., Engle, M.A., Kirby, C.S., and Kraemer, T.F., 2011, Radium content of oil- and gas-field produced waters 

in the northern Appalachian Basin (USA)—Summary and discussion of data: U.S. Geological Survey Scientific 

Investigations Report 2011–5135, 31 p.

(Available online at http://pubs.usgs.gov/sir/2011/5135/)
iii

Contents

Abstract...........................................................................................................................................................1

Introduction.....................................................................................................................................................1

Background.....................................................................................................................................................2

Data Sources and Analytical Methods ......................................................................................................5

New York State Department of Environmental Conservation Report (1999)...............................5

New York State Department of Environmental Conservation, Draft Supplemental 

Generic Environmental Impact Statement (2009) ..............................................................6

Pennsylvania Department of Environmental Protection Report (1992)........................................6

Pennsylvania Department of Environmental Protection Reports 

(Unpublished Data, 2009–2010) .............................................................................................7

Dresel and Rose (2010).........................................................................................................................7

This Study...............................................................................................................................................7

Results .............................................................................................................................................................8

Salinity and Radium..............................................................................................................................8

Gross Alpha and Beta Particle Emissions ........................................................................................9

Discussion.......................................................................................................................................................9

Salinity and Dilution..............................................................................................................................9

Radium Activities in Context .............................................................................................................12

Summary........................................................................................................................................................15

Acknowledgments.......................................................................................................................................15

References Cited..........................................................................................................................................15

Figures

1. Radioactive decay chains for U-238 and Th-232 .....................................................................3

2. Map showing locations of wells with data compiled for this study.....................................4

3. Differences between measurements of duplicate and replicate analyses of Ra-226 

and Ra-228 in produced water samples in relation to the mean activity of the sample 

for data from Gilday and others (1999)......................................................................................6 

4. Measured activities for total radium (Ra-226 + Ra-228) and Ra-226 for each 

of the data sources used in the study .......................................................................................8

5. Gross alpha and beta particle activities in relation to the activities of Ra-226 

and Ra-228, respectively ...........................................................................................................10

6. Total radium activity, Ra-228/Ra-226, and total dissolved solids (TDS) as a function 

of time since initiation of flowback..........................................................................................11 

7. Activities of Ra-226 and total radium (Ra-226+Ra-228) in relation to total dissolved 

solids (TDS)..................................................................................................................................13

8. Total radium and Ra-228/Ra-226 plotted against the age of the producing formation.. 14
iv

Tables

1. Well locations and related information compiled for samples used in this study...........19

2. Ra-226, Ra-228, gross alpha, and gross beta activities measured in samples 

of produced water for wells listed in table 1..........................................................................26 

Units and Conversions

pCi/L – picocuries per liter

dpm – disintegrations per minute

Bq – becquerels

1 pCi = 0.037 Bq; 1 Bq = 27.03 pCi

1 pCi = 2.22 dpm; 1 dpm = 0.4505 pCi
Abstract

Radium activity data for waters co-produced with oil and 

gas in New York and Pennsylvania have been compiled from 

publicly available sources and are presented together with new 

data for six wells, including one time series. When available, 

total dissolved solids (TDS), and gross alpha and gross beta 

particle activities also were compiled. 

Data from the 1990s and earlier are from sandstone and 

limestone oil/gas reservoirs of Cambrian-Mississippian age; 

however, the recent data are almost exclusively from the 

Middle Devonian Marcellus Shale. The Marcellus Shale 

represents a vast resource of natural gas the size and 

significance of which have only recently been recognized. 

Exploitation of the Marcellus involves hydraulic fracturing 

of the shale to release tightly held gas. Analyses of the water 

produced with the gas commonly show elevated levels of 

salinity and radium. 

Similarities and differences in radium data from reservoirs of different ages and lithologies are discussed. The range 

of radium activities for samples from the Marcellus Shale 

(less than detection to 18,000 picocuries per liter (pCi/L)) 

overlaps the range for non-Marcellus reservoirs (less 

than detection to 6,700 pCi/L), and the median values are 

2,460 pCi/L and 734 pCi/L, respectively. A positive correlation between the logs of TDS and radium activity can be 

demonstrated for the entire dataset, and controlling for this 

TDS dependence, Marcellus shale produced water samples 

contain statistically more radium than non-Marcellus samples. 

The radium isotopic ratio, Ra-228/Ra-226, in samples from 

the Marcellus Shale is generally less than 0.3, distinctly lower 

than the median values from other reservoirs. This ratio may 

serve as an indicator of the provenance or reservoir source of 

radium in samples of uncertain origin.

Introduction

Radium forms naturally from the decay of uranium and 

thorium, elements that commonly occur in sandstones and 

shales in sedimentary environments. Radium has been documented in the formation waters in many sedimentary basins 

(for example, Fisher, 1998). In the northern Appalachian 

Basin, radium has been measured in the water co-produced 

with gas and oil (that is, produced water3) from reservoirs 

of Cambrian-Mississippian age. Radioactive isotopes are 

commonly quantified in terms of “activity concentration” or 

simply “activity,” which in this context refers to a number 

of disintegrations per unit time. For consistency with the 

studies cited, activity units of picocuries per liter (pCi/L) are 

used here to define the activity of radium in produced water 

samples. 

In surface and shallow subsurface environments, radium 

can be relatively soluble and, therefore, mobile in groundwater 

over a range of pH and Eh (redox) conditions (Langmuir and 

Riese, 1985; Sturchio and others, 2001). Radium also may 

be adsorbed onto clay particles or onto oxide grain coatings 

(Krishnaswami and others, 1982; Ames and others, 1983; 

Sturchio and others, 2001). As a radioactive element, radium 

may represent a potential health hazard if released into the 

environment. The half-lives of the two principal isotopes of 

radium, Ra-226 and Ra-228, are 1,600 and 5.75 years, respectively (Akovali, 1996; Artna-Cohen, 1997), and approximately 

10 half-lives are required for a radioactive element to decay to 

negligible quantities. Chemically, radium behaves in a manner 

similar to calcium and is capable of bioaccumulation in plants 

and animals. There is a significant body of research aimed at 

quantification of radium uptake in crops and livestock that 

make up the human food chain (for example, Tracy and others; 

1983; Bettencourt and others, 1988; Linsalata and others, 

Radium Content of Oil- and Gas-Field Produced Waters 

in the Northern Appalachian Basin (USA): 

Summary and Discussion of Data

By E.L. Rowan,1 M.A. Engle,1 C.S. Kirby,2 and T.F. Kraemer1

1

U.S. Geological Survey, Reston, Virginia.

2

Bucknell University, Lewisburg, Pennsylvania.

3

The term “produced water” in this report represents water produced from an oil or gas well at any point during its life cycle. The term, therefore, includes 

waters produced immediately after hydraulic fracturing, with compositions close to those of the injected fluid, as well as waters produced after months or years 

of production, whose compositions resemble formation water. 
2 Radium Content of Oil- and Gas-Field Produced Waters in the Northern Appalachian Basin: Summary and Discussion

1989). Most of these studies were conducted in areas where 

uranium mining had previously taken place; however, it is not 

known whether similar investigations have been conducted 

in regions where oil- and gas-field produced waters are the 

source of radium. The purpose of this report is to compile 

and present data from multiple sources to facilitate ongoing 

research. 

Activity data for radium-226 (Ra-226) and radium-228 

(Ra-228) in oil- and gas-field produced waters from New 

York and Pennsylvania have been compiled from publicly 

available sources and combined with new data for six wells 

(tables 1 and 2, p. 19–31). Measurements of total dissolved 

solids (TDS) and of gross alpha and beta activities were also 

tabulated when available. Unstable (radioactive) isotopes 

decay by emitting alpha and beta particles; therefore, alpha 

and beta activities can serve as rough indicators of the 

presence of radioactive elements. 

The publicly available radium data were obtained 

from the New York State Department of Environmental 

Conservation (NYSDEC), the Pennsylvania Department of 

Environmental Protection (PA DEP), and the Pennsylvania 

Geological Survey. Most of these data are available online, 

although the most recent Marcellus Shale produced water 

data were available only from the regional PA DEP offices. 

Three of the studies, Gilday and others (1999), Pennsylvania 

Department of Environmental Protection (1992), and Dresel 

and Rose (2010), provide data from wells producing from 

reservoirs of Cambrian-Devonian age. In contrast, the analyses 

reported by the New York State Department of Environmental 

Conservation (2009) and by the Pennsylvania Department of 

Environmental Protection (unpub. data, 2009–2010) are for 

produced waters predominantly from the Devonian Marcellus 

Shale. 

Background

The Appalachian Basin comprises a vast accumulation 

of sedimentary rock west of the Appalachian Mountains, 

extending from Quebec and Ontario south through New York, 

Pennsylvania, Ohio, West Virginia, to Alabama. Hydrocarbons 

are produced throughout the basin from reservoirs of Cambrian-Pennsylvanian age (Legall and others, 1981; Milici and 

others, 2003). In recent years, however, the Middle Devonian 

Marcellus Shale has become the focus of gas exploration and 

production, particularly in Pennsylvania, New York, and West 

Virginia. 

A regional comparison of produced water salinities 

indicates that Appalachian Basin salinities are high relative 

to other oil- and gas-producing basins in the United States 

(Breit, 2002). The compilation yielded a median TDS of about 

250,000 milligrams per liter (mg/L) for the Appalachian Basin 

(USA), which was exceeded only by the median salinity for 

the Michigan Basin (about 300,000 mg/L). The data presented 

here indicate a wide salinity range for water produced from 

the Marcellus Shale, from less than 1,500 mg/L to greater than 

300,000 mg/L. The lower salinities may be attributed in part to 

dilution with less saline fluid injected during hydraulic fracturing, but the upper end of the salinity range is comparable to 

the waters produced from the underlying Lower Devonian and 

older reservoirs as well as some of the overlying Devonian 

reservoirs (Rowan and others, 2010). 

The Marcellus Shale is an organic-rich shale that is both 

the source rock and the reservoir for an extensive natural gas 

resource (Harper, 2008). Shale-gas accumulations, such as 

the Marcellus, are termed “unconventional” or “continuous” 

because the gas is dispersed within a stratigraphic interval 

rather than confined by a conventional structural or stratigraphic trap. The process of “hydraulic fracturing” commonly 

is used to access the gas in a continuous reservoir. In this 

process, water is pumped into a well at pressures high enough 

to fracture the rock, and the newly created fracture network 

allows gas that is tightly held in micropores or adsorbed 

onto clay particles to be released. The injected fluid may be 

freshwater or relatively dilute, or alternatively, it may have 

been recycled, that is, produced from one well and then used 

to hydraulically fracture a new well. The water flowing from 

hydraulically fractured wells initially reflects the composition 

of the injected fluid, but with time shifts toward salinities 

and inorganic chemical compositions similar to the fluids in 

adjacent formations (for example, Rowan and others, 2010). 

Hayes (2009), for example, examined the chemistry of 

produced water samples collected from 12 Marcellus Shale 

wells at 1-, 5-, 14-, and 90-day intervals following hydraulic 

fracturing. The water injected into these wells was essentially 

fresh, with a median TDS of less than 1,000 mg/L, but within 

90 days, the salinities had increased to a median value exceeding 200,000 mg/L TDS. 

Ra-226 and Ra-228 are the decay products of U-238 and 

Th-232, respectively (fig. 1; Ivanovich, 1992). Once formed, 

radium may remain within the original host mineral or other 

solid phase, or may be released into the adjacent pore water. 

Lithologies that contain substantial amounts of uranium and 

(or) thorium can, therefore, have measurable amounts of 

radium dissolved in their pore waters. The data compiled in 

this report span most of the oil- and gas-producing regions of 

the Appalachian Basin in Pennsylvania and New York (fig. 2), 

and show significant levels of radium in produced water 

samples from Cambrian-Mississippian reservoirs. 

Dissolved radium occurs predominantly as the Ra+2

ion, but also forms complexes with chloride, sulfate, and 

carbonate ions (Rose and Korner, 1979; Kraemer and Reid, 

1984; Langmuir and Riese, 1985; Sturchio and others, 2001). 

Aqueous radium may remain in solution, be adsorbed from 

pore water onto oxide grain coatings or clay particles by ion 

exchange, or may substitute for cations, such as Ba+2, Ca+2, 

and Sr+2, during precipitation of mineral phases, such as barite, 

anhydrite, and calcite. Radium sulfate (RaSO4) is much less 

soluble than barite, anhydrite, and other sulfate minerals, 

but rarely occurs as a separate mineral phase. When alkali 

earth sulfates precipitate, however, radium present in solution 
Background 3

Figure 1. Radioactive decay chains for (A) U-238 and (B) Th-232. Times shown are half-lives: y, years; d, days; 

h, hours; m, minutes; s, seconds. Ra-226 and Ra-228 (shaded) are the primary isotopes of interest in this study. 

Half-lives were obtained from the National Nuclear Data Center (http://www.nndc.bnl.gov/chart/).

U-238 U-234

2.5 x 105

 y

Th-230

7.5 x104

 y

Po-214

1.6x10-4s

Ra-226

1600 y

Rn-222

3.8 d

Po-218

3.1 m

Bi-214

19.9 m

Pb-214

26.8 m

Pb-210

22.2 y

Pb-206

(stable)

Po-210

138.4 d

Bi-210

5.0 d

Th-234

24.1 d

Pa-234

6.7 h

Th-232

1.4 x 1010 y

Po-212

3.0 x10-7 s

Th-228

1.9 y

Ra-224

3.6 d

Ac-228

6.15 h

Rn-220

55.6 s

Po-216

Bi-212

60.6 m

TI-208

3.05 m

Pb-212

10.6 h

Pb-208

(stable)

Ra-228

5.75 y

Uranium

Protactinium

Thorium

Radium

Radon

Polonium

Bismuth

Lead

Thorium

Actinium

Radium

Radon

Polonium

Bismuth

Lead

Thallium

A. Uranium-238

EXPLANATION

Alpha decay

Beta decay

EXPLANATION

Alpha decay

Beta decay

B. Thorium-232

Figure 1

0.145 s

4.5 x 109

 y
4 Radium Content of Oil- and Gas-Field Produced Waters in the Northern Appalachian Basin: Summary and Discussion

Figure 2. Locations of wells with data compiled for this study.

Erie

Elk

Lewis

Tioga

York

Erie

Oneida

Potter

Steuben

Centre

Herkimer

Berks

Otsego

Jefferson

Delaware

Bradford

Pike Lycoming

Clinton

Butler

Oswego

Clearfield

Bedford

Allegany

Warren

McKean

Luzerne

Crawford

Indiana

Somerset

Blair

Cattaraugus

Wayne

Fayette

Perry

Cayuga

Tioga

Bucks

Lancaster

Franklin Chester

Ontario

Broome

Chautauqua

Mercer

Chenango

Wayne Monroe

Clarion

Cambria

Onondaga

Schuylkill

Venango

Madison

Monroe

Greene

Huntingdon

Adams

Allegheny

Yates

Fulton

Washington

Cecil

Westmoreland

Forest

Jefferson

Niagara

Wyoming

Armstrong

Susquehanna

Beaver

Cortland

Sullivan

Genesee

Harford Salem

Union Carbon

Tompkins

Orleans

Snyder

Cumberland

Chemung

Wyoming

Lebanon

Schuyler

Dauphin

Livingston

Mifflin

Hamilton

Columbia

Seneca

Juniata Lehigh

Cameron

New Castle

Montgomery

Lackawanna

Lawrence

Gloucester

Northumberland

Northampton

Delaware

Montour

Philadelphia

Harford

Sullivan

MARYLAND

PENNSYLVANIA PENNSYLVANIA

PENNSYLVANIA

PENNSYLVANIA

PENNSYLVANIA

NEW YORK

OHIO

WEST VIRGINIA

NEW JERSEY

PA DEP (1992) NYSDEC (Gilday and others, 1999)

NYSDEC (2009) PA DEP (unpub. data, 2009–2010)

Base from U.S. Geological Survey digital data

EXPLANATION

Dresel and Rose (2010)

This study

80° 78° 76°

44°42°40°

0 50 75 100 25 MILES

0 80 120 40 KILOMETERS

Pennsylvania

NewYork

New Jersey

Map Area

WestVirginia

LAKE ONTARIO

LAKE ERIE
Data Sources and Analytical Methods 5

coprecipitates as a solid-solution, preferentially enriching the 

solid phase and depleting the solution of radium (Langmuir 

and Riese, 1985). 

Data Sources and Analytical Methods

The sources of data in this report (tables 1 and 2) are 

discussed below together with the available information 

on quality assurance/quality control (QA/QC), analytical 

methods, and uncertainty. The U.S. Environmental Protection 

Agency (USEPA) method codes refer to standard analytical 

procedures defined by the USEPA (Krieger and Whittaker, 

1980; Eaton and others, 2005).

New York State Department of Environmental 

Conservation Report (Gilday and others, 1999)

The New York State Department of Environmental 

Conservation (NYSDEC) conducted a study titled “An 

Investigation of Naturally Occurring Radioactive Materials 

(NORM) in Oil and Gas Wells in New York State,” in which 

produced water, oil, sludge, and other waste materials were 

sampled from oil and gas wells in New York State (Gilday 

and others, 1999). Analyses were reported for a total of 

57 brine samples collected from 48 oil or gas well sites, with 

9 duplicate or replicate samples (table 1). The NYSDEC report 

indicates that the brines were sampled from storage tanks, but 

the length of time between production and sample collection is 

unknown. The wells in this study produced hydrocarbons and 

water from formations of Cambrian through Lower Devonian 

age, with one sample of possible mixed Lower Silurian and 

Upper Devonian reservoir origin (table 1). Several of the wells 

produced from the Lower Devonian Oriskany Sandstone and 

Helderberg Limestone. Silurian reservoirs provided samples 

from the Akron Sandstone, Bass Islands Dolomite, Medina 

Sandstone, and Rochester Shale. Ordovician reservoirs 

included sandstones within the Queenston Shale. 

Analyses of radium activity in the NYSDEC report 

were determined using gamma-spectrometry as well as 

alpha-spectrometry in some cases. Gamma-spectrometry 

compares the gamma-ray wavelengths emitted by radioactive 

material with the emission spectra of known radioactive 

elements. In some instances, the signal emitted by a daughter 

product can be more accurately identified and quantified than 

that of its parent isotope. Laboratories may therefore elect 

to report a daughter product activity as representative of its 

radium parent’s activity in an appropriately prepared sample. 

Gilday and others (1999) considered that the Ra-226 daughter 

products Pb-214 and Bi-214 were the most reliable indicators 

of Ra-226 activity, and they selected the larger of the Pb-214 

and Bi-214 values to represent the Ra-226 activity. Gilday 

and others (1999) considered Ac-228 activity to be the most 

reliable indicator of Ra-228 activity, and Pb-212, which occurs 

lower on the decay chain (fig. 1), was seldom used. 

The values listed in table 2 are consistent with the 

approach of Gilday and others (1999), but several instances 

differ from the values highlighted in their report as representative of a given sample. At one well (no. 76), the Pb-212 

activity was anomalously high, 23,900 pCi/L, relative to a 

corresponding Ac-228 activity of 1,500 pCi/L. Gilday and 

others (1999) concluded that the Pb-212 value was erroneous, 

although this was the value they highlighted as representative 

of the sample. At a second well (no. 82), a Pb-212 activity of 

7,650 pCi/L also appeared to be anomalously high relative 

to the Ac-228 activity of 1,110 pCi/L. In both instances, the 

Ac-228 rather than the Pb-212 activities are used to represent 

Ra-228 in table 2. Pb-212 activities were used in only five 

instances where Ac-228 was not reported. In wells where 

duplicate analyses were available, (nos. 38, 56, 79, and 80), 

the averages are given in table 2. 

All of the samples collected by Gilday and others (1999) 

were analyzed by an outside contract laboratory, and a subset 

of nine samples was also analyzed by the NYSDEC Bureau 

of Pesticide and Radiation laboratory. Some interlaboratory 

comparison and QA/QC information was provided in that 

report and is discussed below. Ideally, metrics of both analytical accuracy (proximity of measured value to the “true” value) 

and precision (measurement reproducibility) are presented. 

Because no analyses of reference materials or other standards 

were reported, the analytical accuracy for the included data 

is unknown. Sample precision was examined by comparing 

data for analyses of duplicate4 and replicate5 samples (fig. 3). 

Despite the reported “internally consistent results” from 

each laboratory, the measurement uncertainty ranges did not 

overlap in five out of nine brine samples analyzed by both 

laboratories. A single outlier exhibited an exceptionally high 

difference of 143 percent between replicate analyses for 

Ra-226. 

These findings indicate that sample precision is generally 

better (less than 20 percent discrepancy between duplicate 

or replicate samples) for samples that contained greater than 

500 pCi/L, but poor agreement in interlaboratory comparisons 

indicates there may be bias between data sources. The 

magnitude of the biases, however, appears to be in the tens of 

percents while radium activities in brine samples range over 

more than four orders of magnitude. This comparison suggests 

that even the higher end of analytical imprecision observed in 

the data does not significantly affect the magnitude of radium 

activities reported.

4

Duplicate refers to individual samples from a single source collected at the 

same place and time.

5

Replicate refers to a repeat analysis made on the same sample or aliquots of 

the same sample.
6 Radium Content of Oil- and Gas-Field Produced Waters in the Northern Appalachian Basin: Summary and Discussion

New York State Department of Environmental 

Conservation, Draft Supplemental Generic 

Environmental Impact Statement (2009)

In 2009, the NYSDEC released a study titled “Draft 

Supplemental Generic Environmental Impact Statement 

related to Marcellus Shale Gas Development” (New York 

State Department of Environmental Conservation, 2009). 

Appendix 13 of the document, “NYS Marcellus Radiological 

Data from Production Brine,” lists gross alpha, gross beta, and 

activities of Ra-226 and Ra-228 for water samples collected 

from 12 gas-producing Marcellus Shale wells in New York 

State. Appendix data were presented in table form without 

accompanying text, information relating to QA/QC, or analytical methods. However, well lease names and API numbers, 

towns, and counties were provided, allowing well locations 

and related information to be obtained from the State database 

(http://www.dec.ny.gov/; fig. 2; tables 1 and 2). Activities 

of uranium, thorium, and the anthropogenic isotopes, 

cesium-137, cobalt-60, ruthenium-106, and zirconium-95, 

were listed in the appendix, but are not compiled in this report. 

Pennsylvania Department of Environmental Protection 

Report (1992)

In 1991, the PA DEP conducted field work for a study of 

salinity and radium activities in produced waters, sludge, and 

other related waste from oil and gas wells in Pennsylvania. 

The results were compiled in a report titled “NORM Survey 

Summary” and released the following year (Pennsylvania 

Department of Environmental Protection, 1992). The wells 

sampled for the study produced hydrocarbons and water 

from Lower Silurian–Upper Devonian Formations, with one 

sample thought to be from an Ordovician reservoir. Although 

the Marcellus Shale falls within this stratigraphic interval, the 

study long pre-dated the recent (2005–present) focus on the 

Marcellus Shale as an unconventional gas resource. Among 

the most commonly sampled reservoirs were sandstone in the 

Silurian Medina Group, the Lower Devonian Oriskany Sandstone, Huntersville Chert, and Onondaga Limestone, as well as 

Upper Devonian sandstones (table 1). About three-fourths of 

the samples were taken from storage tanks, or separator tanks, 

and the remaining samples were collected from surface pits or 

diked areas (table 1). The length of time between hydrocarbon 

production and sample collection is unknown, and therefore, 

Ra-228 activity may have been markedly reduced by natural 

decay. Brines that accumulated in open pits presumably would 

have been subject to evaporation and (or) dilution by rain. 

Figure 3. Differences between measurements of duplicate and replicate analyses 

of Ra-226 and Ra-228 in produced water samples in relation to the mean activity of 

the sample for data from Gilday and others (1999). The solid lines represent 10 percent 

and 20 percent relative difference between duplicates/replicates using the method of 

Thompson and Howarth (1978). Samples with higher radium activities generally have 

better measurement precision, that is, lower percentage differences. Absolute measurement difference, in picocuries per liter

Mean activity, in picocuries per liter

600

0

400

200

0 500 1,000 1,500 2,000

>20%

10–20%

<10%

Ra-226

EXPLANATION

Ra-228
Data Sources and Analytical Methods 7

In addition to brine samples, samples of sludge, drill 

cuttings, and pipe scale from brine treatment facilities, pipe 

yards, disposal wells, and other facilities were analyzed, but 

these results were not compiled in this report. No information 

on the laboratory, analytical methods, uncertainties, or QA/QC 

was included with the PA DEP (1992) report. 

Pennsylvania Department of Environmental Protection 

Reports (Unpublished Data, 2009–2010) 

A number of the annually filed “Form 26R” (Chemical 

Analysis of Residual Waste, Annual Report by Generator) 

waste reports related to shale gas production were obtained 

from the PA DEP. The forms and accompanying chemical 

analyses are filed annually with the PA DEP by generators 

of liquid or solid waste, including oil and gas well operators. 

The 26R forms can be viewed at the DEP regional offices 

by appointment, or photocopies can be requested from the 

DEP. The DEP offices in Williamsport and Pittsburgh were 

visited during the spring and summer of 2010, and the 

available 26R forms pertaining to liquid waste generated at 

gas well sites were electronically scanned. Additional data 

were obtained by correspondence with the Meadville, Pa., 

office. Radium activities from the 26R forms were included in 

this report only when the well name and related information 

could be obtained for a given sample. Information obtained 

from 26R forms filed with the PA DEP during 2009–2010 

for a total of 23 wells was compiled and included in tables 1 

and 2. In most instances, the TDS values of the samples were 

also available. Time series data were available for four wells 

(table 2). When duplicate analyses were provided, the average 

value is shown in table 2.

Laboratory notes accompanying 26R forms reported to 

the PA DEP varied substantially between individual wells, 

but all included the laboratory name and, in some cases, 

the analytical method and QA/QC information. Despite the 

numerous different reporting entities, the radiochemical data 

reported in the 26R forms were obtained from only four 

different laboratories, and all are accredited in accordance with 

the National Environmental Laboratory Accreditation Program 

(NELAP). 

Gross alpha and beta emission measurements included 

in the PA DEP 26R forms were determined by methods that 

include standard and modified versions of EPA Method 900.0 

(Gross Alpha and Gross Beta Radioactivity in Drinking 

Water) and Standard Method 7110C (Eaton and others, 2005). 

No duplicate samples, replicate analyses, or other QA/QC 

information were available for either the gross alpha or beta 

results. 

When methods for radium analysis were reported, Ra-226 

activity typically was measured using gamma-spectrometry, 

and in some cases by alpha-spectrometry, using standard 

USEPA methods: EPA Method 901.1 (Gamma Emitting 

Radionuclides in Drinking Water), EPA Method 903.0 

(Alpha-Emitting Radium Isotopes in Drinking Water), and 

EPA Method 903.1 (Radium-226 in Drinking Water Radon 

Emanation Technique). Radium-228 was analyzed using 

similar methods: EPA Method 901.1 (Gamma Emitting 

Radionuclides in Drinking Water) and EPA Method 904.0 

(Radium-228 in Drinking Water). For the four sets of duplicate 

Ra-226 and Ra-228 analyses, the discrepancies were less than 

7 percent, with one exception: Ra-226 analyses in duplicate 

samples from well no. 1 differed by 72 percent. 

Dresel and Rose (2010)

A recent publication by Dresel and Rose (2010) reports 

the produced water analyses originally conducted as part of 

a Master’s thesis at Pennsylvania State University (Dresel, 

1985). Of the 40 samples collected, Ra-226 analyses are 

reported for six wells producing hydrocarbons and water from 

Lower Silurian–Upper Devonian sandstone reservoirs; Ra-228 

values are not reported. Most of the samples in this study were 

collected from the wellhead rather than secondary storage 

units (table 1). The Ra-226 activities reported were determined 

by measurement of radon-222 activity at secular equilibrium 

(Rose and Korner, 1979), using a method equivalent to USEPA 

Method 903.1 (Krieger and Whittaker, 1980). Detailed QA/QC 

information was not available.

This Study

Radium activities have been determined at the U.S. Geological Survey (USGS) for samples from six additional 

Marcellus Shale gas wells in Pennsylvania. Samples were 

collected from five of the wells (nos. 127–131, tables 1 

and 2) as part of a study by Pritz (2010). The precise localities 

of these wells in Bradford County are confidential, and they 

are represented in figure 2 by a single point. Well no. 132 was 

sampled jointly by the USGS, the Department of Energy, and 

industry collaborators on successive dates, thus providing time 

series information. Analyses of the samples were conducted 

at the USGS radiochemistry laboratory in Reston, Virginia. 

Two to four duplicates of each sample from well no. 132 were 

prepared and analyzed, and the average values are reported in 

table 2. 

In the samples from well no. 132, radium was chemically 

separated from the water by coprecipitating it with barium 

sulfate. The precipitate was then placed in the well of a high 

purity germanium detector, and quantitative analysis of the 

Ra-226 and Ra-228 content of the precipitate was performed 

by gamma-spectrometry using a technique adapted from 

Moore (1984). As discussed above for the New York State 

data of Gilday and others (1999), Ra-228 was quantified by 

measuring the intensity of gamma rays emitted by Ac-228, 

and Ra-226 was quantified by measuring the intensity of the 

gamma rays emitted by Pb-214 and Bi-214. As described in 

Kraemer (2005), the gamma-ray spectrometry systems were 

calibrated using standardized radium isotopic solutions. 
8 Radium Content of Oil- and Gas-Field Produced Waters in the Northern Appalachian Basin: Summary and Discussion

Uncertainties for these analyses are listed in table 2 as 

+/– one standard deviation from the mean peak intensity and 

represent the “counting error” for a specific analysis. When 

duplicate samples were prepared, that is, reprecipitated, and 

analyzed, the range of the discrepancies matched closely with 

the range for the counting error: 0.2–8.5 percent. However, 

the discrepancies between analyses of duplicate samples were 

most commonly 2–4 percent higher than the counting error. In 

all cases, the maximum error did not exceed +/– 8.5 percent. 

Results

Salinity and Radium

Salinities, reported as TDS, were available for approximately one-half of the produced water samples and ranged 

from 1,470 to 402,000 mg/L with a median of 157,000 mg/L 

TDS (table 2). The median total radium (defined here as 

Ra-226 + Ra-228) activity for the non-Marcellus Shale produced water samples is 1,011 pCi/L compared with 2,460 for 

Marcellus Shale produced water samples and 5,490 pCi/L for 

the Marcellus produced water data for New York State (fig. 4; 

New York State Department of Environmental Conservation, 

2009; Pennsylvania Department of Environmental Protection, 

unpub. data, 2009–2010; this study). For comparison, the 

total radium limit for industrial effluent is 60 pCi/L, and the 

drinking water limit is 5 pCi/L (U.S. Environmental Protection 

Agency, 1976; Hess and others, 1985; U.S. Nuclear Regulatory Commission, 2011). 

In the NYSDEC (2009) study, salinities were not 

reported; however, two wells, no. 28 and no. 33, were 

resampled and analyzed by Osborn and McIntosh (2010), 

yielding respective salinities of 206,446 and 205,102 mg/L 

TDS. Samples at two additional wells, no. 24 and no. 25, 

both from depths of approximately 2,600 feet (ft), exhibited 

very low total radium activities (less than 1 pCi/L), although 

the activities of the remaining sites exceeded 1,900 pCi/L 

(fig. 4; table 2). The reason for the low radium content of 

these samples is unknown, but they may have been composed 

largely of water injected for hydraulic fracturing, which often 

is of lower salinity and radium content than the formation 

water. 

In Pennsylvania, the range of total radium activities 

for the Marcellus Shale samples (Pennsylvania Department 

Figure 4. Measured activities for total radium (Ra-226 + Ra-228) and Ra-226 for each of the data sources used in 

the study. The three datasets for produced water from Marcellus Shale wells are shown on the left; the remaining 

three datasets are for non-Marcellus Shale wells. The number of points in each dataset is shown in parentheses, 

and the median values are plotted as heavy black lines. For reference, the dashed line shows the industrial effluent 

discharge limit (60 pCi/L) for Ra-226 (U.S. Nuclear Regulatory Commission, http://www.nrc.gov/reading-rm/

doc-collections/cfr/part020/appb/Radium-226.html).

0

1

10

100

1,000

10,000

100,000

Ra-226

Ra (total)

Ra (total)

Ra (total)

Ra-226

Ra (total)

Ra-226

Ra (total)

Ra-226

PA DEP (2009–2010, 

unpub. data)

(25)

this study

(14)

NYSDEC (2009)

(13)

NYSDEC 

(Gilday 

and others, 1999)

(48)

PA DEP (1992)

(37)

Dresel and Rose 

(2010)

(6)

Ra (total), Ra-226, in picocuries per liter

Ra-226

Marcellus Shale data

Ra-226
Discussion 9

of Environmental Protection, unpub. data, 2009–2010) is 

similar to the Marcellus data from New York but is more 

evenly distributed (less clustered) over the range. Dilution 

of formation water with the relatively freshwater from the 

hydraulic fracturing process may have been an important 

factor influencing the distribution of both salinity and radium 

content. The time interval between hydraulic fracturing and 

sample collection is known in only a few cases. 

Gross Alpha and Beta Particle Emissions

Emission of alpha and beta particles accompanies the 

decay of Ra-226 and Ra-228, respectively (fig. 1), and the 

USEPA has established the measurement of gross alpha 

and beta as a method of screening samples for the presence 

of radium (Hess and others, 1985; Buckwalter and Moore, 

2007, p. 48). Gross alpha and beta data were available for 

two datasets (New York State Department of Environmental 

Conservation, 2009; Pennsylvania Department of Environmental Protection, unpub. data, 2009–2010) and are plotted 

with Ra-226 and Ra-228, respectively (figs. 5A–B). On log-log 

scales, gross alpha and gross beta activities are linearly 

correlated with Ra-226 and Ra-228, confirming their value 

as indicators of radium activity. Although these isotopes are 

unlikely to be the only sources of alpha and beta particles, the 

correlations shown in figures 5A–B suggest that they are likely 

to be the dominant sources for these samples. 

Discussion

Salinity and Dilution

Several studies of Appalachian Basin formation water 

chemistry have shown general trends of increasing salinity 

with depth and age of the reservoir (for example, Stout and 

others, 1932; Poth, 1962; Breen and others, 1985); however, 

high salinities can occur even at relatively shallow depths. A 

salinity-depth curve for Mississippian-Devonian formation 

waters in eastern Ohio showed greater than 100,000 mg/L 

TDS at 1,000 ft (Stout and others, 1932, p. 18). Poth (1962, 

p. 37–38, table 6) noted that on the basis of a limited set of 

samples, an equilibrium salinity had apparently been reached 

in Middle Devonian and older reservoirs, and water produced 

from these units have a dissolved solids content of about 

300,000 mg/L. In the dataset compiled here, produced water 

salinities from the Middle Devonian Marcellus Shale commonly range from 100,000 to 200,000 mg/L TDS (table 2). 

Despite the presence of evaporites in the Silurian Salina 

Group in parts of New York and Pennsylvania, many authors 

consider that the salinity of the produced waters in much of 

the Appalachian Basin originated from the evaporative concentration of seawater (for example, Stout and others, 1932; 

Sanders, 1991; Dresel and Rose, 2010; Osborn and McIntosh, 

2010). Brines derived from seawater evaporation are enriched 

in bromide and can be distinguished from brines formed by 

dissolution of evaporites on the basis of relations among 

Na, Cl, and Br (Walter and others, 1990). Brines produced 

with gas from Marcellus Shale wells after salinities have 

reached a plateau share similar major ion chemistries with 

formation waters from the overlying and underlying Devonian 

formations and show similar Na-Cl-Br relations (Osborn and 

McIntosh, 2010; Rowan and others, 2010). On the basis of 

these chemical similarities, a similar origin for the salinity of 

waters produced from the Marcellus Shale and from adjacent 

overlying and underlying formations can be hypothesized. 

Blauch and others (2009), however, reported small lenses 

of halite and other salts in core from the Marcellus Shale and 

suggested that dissolution of these minerals contributed to the 

salinity of the produced waters. They also described minor 

volumes of salts, but noted that similar occurrences have not 

previously been reported in the literature on the Marcellus. 

Where present, salt lenses would contribute to total salinity, 

but it is difficult to assess their distribution or quantify their 

contribution to total fluid salinity. The elevated bromide 

concentrations and Na-Cl-Br relations suggest that the 

dominant source of salinity for Marcellus Shale waters, and 

for other formations in the stratigraphic section, originated as 

evaporatively concentrated seawater. 

Dilution of formation water with relatively freshwater 

injected during the hydraulic fracturing may account for some 

of the lower salinity values. For example, in well no. 11 salinities were measured 14 and 90 days after hydraulic fracturing 

and showed an increase with time (fig. 6A; table 2). In well 

no. 5, successive salinity measurements made 17 days apart 

also showed increased salinity with time (table 2). In a more 

detailed study by Hayes (2009), repeated measurements of 

produced water salinity up to 90 days after hydraulic fracturing showed increases in salinity with time from less than 1,000 

mg/L to greater than 100,000 mg/L TDS. The marked increase 

in salinity with time is interpreted to represent a decreasing 

proportion of the lower salinity injected fluid and an increasing proportion of the saline formation water returning to the 

surface. As mentioned previously, dissolution of mineral 

phases such as halite, if present, could also contribute salinity. 

For data compiled from the PA DEP 26R forms, when the 

sample collection date occurred less than 90 days from the 

initiation date of drilling, it seems plausible that salinities less 

than 100,000 ppm TDS may have been affected by dilution of 

the formation water with the water injected during hydraulic 

fracturing. 

Like salinity, radium in the produced waters increases 

with time following hydraulic fracturing. A well producing 

gas from the Marcellus Shale in Greene County, Pa. (no. 132), 

was sampled daily for the first 5 days, then on days 7, 15, 

and 20 following hydraulic fracturing. The radium data for 

these samples are discussed below, but the salinity data are 

not yet available. The hydraulic-fracturing supply water was 

a mix of water recycled from similar gas wells nearby and 

more dilute surface water. Following hydraulic fracturing, the 

total radium activity in the produced water increased sharply 
10 Radium Content of Oil- and Gas-Field Produced Waters in the Northern Appalachian Basin: Summary and Discussion

Figure 5. (A) Log of gross alpha particle activity in relation to the log of Ra-226 activity and (B) log of gross beta 

particle activity in relation to the log of Ra-228 activity. Gross beta activities below the reported detection limit in 

well nos. 17 and 33 are not plotted or used in the best fit line.

y = 1.35x – 2.05

R2

 = 0.78

–1.0

0.0

1.0

2.0

3.0

4.0

5.0

0.0 1.0 2.0 3.0 4.0 5.0

Log gross alpha, in picocuries per liter

Log Ra-226, in picocuries per liter

Ra-226, in picocuries per liter

0.1

1

10

100

1,000

10,000

100,000

1 10 100 1,000 10,000 100,000

Figure 5.

B

A Gross alpha, in picocuries per liter

y = 1.34x – 2.14

R2

 = 0.54

–2.0

–1.0

0.0

1.0

2.0

3.0

4.0

0.0 1.0 2.0 3.0 4.0 5.0

Log gross beta, in picocuries per liter

Gross beta, in picocuries per liter

Log Ra-228, picocuries per liter

Ra-228, in picocuries per liter

0.01

0.1

1

10

100

1,000

10,000

1 10 100 1,000 10,000 100,000
Discussion 11

Figure 6. (A) Total radium activity and total dissolved solids related to time since initiation of flowback for 

well no. 11, Washington County, Pa. (B) Total radium activity (left axis, squares) and Ra-228/Ra-226 (right axis, 

diamonds) related to time since initiation of flowback for well no. 132, Greene County, Pa.

EXPLANATION

Total radium

Ra-228/Ra-226

Total radium

EXPLANATION

Total dissolved solids

0

1,000

2,000

3,000

4,000

5,000

6,000

7,000

0 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19

Days since initiation of flowback

Total radium, in picocuries per liter

0.10

0.15

0.20

0.25

0.30

0.35

0.40

Ra-228/Ra-226, in picocuries per liter

0

500

1,000

1,500

2,000

2,500

3,000

3,500

4,000

0 10 20 30 40 50 60 70 80 90

Days since initiation of flowback

Total radium, in picocuries per liter

0

50,000

100,000

150,000

200,000

Total dissolved solids, in milligrams per liter

20

B

A
12 Radium Content of Oil- and Gas-Field Produced Waters in the Northern Appalachian Basin: Summary and Discussion

during the first week from the activity of the supply water 

(about 1,600 pCi/L) to a plateau at about 6,100 pCi/L (fig. 6B). 

The increase in radium activity is interpreted as the result 

of equilibration between the injected water, whose radium 

activity is relatively low, and the radium that is present in the 

reservoir, either adsorbed onto mineral surfaces or dissolved 

in pore water. An anomalously low value on day 7 remains 

as yet unexplained; close agreement between multiple repeat 

analyses of the original sample conducted on different dates 

rules out an instrumental or analytical error as an explanation. 

The Ra-228/Ra-226 ratio for this fluid decreased from the 

initial value of 0.23 in the injected water to 0.12. Following 

an unexplained increase on day 7, the ratio returned to about 

0.16. Low isotopic ratios reflect the low Th/U ratio that 

generally characterizes the Marcellus Shale. The evolution of 

total radium and Ra-228/Ra-226 with time displays a fairly 

consistent pattern, with the exception of day 7. The area 

being drained by the well on this day may have intersected 

a “pocket” of chemically distinct water, possibly a sandy 

horizon in the shale or a fracture intersecting a distinct facies. 

Radium Activities in Context

In a study of NORM (naturally occurring radioactive 

material) in oil- and gas-producing regions, Fisher (1998) 

compiled radium activity data for nine sedimentary basins 

in the United States and Europe. In separate studies, Ra-226 

activities were reported for formation water samples from 

clastic aquifers in the U.S. Gulf Coast (Kraemer and Reid, 

1984) and from carbonate aquifers in the U.S. midcontinent 

(Sturchio and others, 2001). Radium activity ranges for these 

regions generally are comparable to those compiled here for 

the Appalachian Basin. The highest reported values found 

in literature are from the Donieper-Donets Basin, Ukraine 

(Gutsalo, 1964, cited in Kraemer and Reid, 1984) and from 

the Texas Panhandle (see references cited in Fisher, 1998); the 

high end of the Ra-226 activities ranges exceeded 4,500 pCi/L 

in the Ukraine and 5,000 pCi/L in the Texas Panhandle. In this 

report, several Ra-226 activities of approximately 4,000 pCi/L 

have been compiled for samples from non-Marcellus reservoirs, but the Marcellus Shale data range higher, with several 

activities exceeding 10,000 pCi/L (table 2; fig. 7). 

Relationships between salinity and radium activity 

have been documented in a number of studies (for example, 

Kraemer and Reid, 1984; Fisher, 1998; Sturchio and others, 

2001). Fisher (1998), however, pointed out that chloride 

or TDS concentrations “best predict radium activity in 

waters from reservoirs that are lithologically relatively 

homogeneous.” Despite their origin in reservoirs of varying 

ages and lithologies, the non-Marcellus Shale data indicate a 

positive correlation between salinity and both total radium and 

Ra-226 activities. Salinity (TDS) is plotted with total radium 

and Ra-226 in figures 7A–B. Use of the longest-lived isotope, 

Ra-226, may reduce some of the scatter induced in the data by 

sample collection at varying, or unknown, time intervals since 

brine production at the wellhead. A year after production at 

the wellhead, for example, the activities of the shorter-lived 

Ra-228 isotope would be reduced by approximately 11 percent 

because of natural decay. 

Analysis of covariance (ANCOVA6) was used to statistically examine the effect of Marcellus versus non-Marcellus 

sample origin on the linear relationship between TDS and 

radium activity. The resulting linear regression models yield 

nearly identical slopes in the trends of log total radium in 

relation to log TDS and log Ra-226 in relation to log TDS. 

However, the regression intercepts for the Marcellus Shale 

data are 0.4 and 0.55 log units (2.5 and 3.5 times, respectively) 

higher for total radium and Ra-226, respectively, than for 

the non-Marcellus samples. Produced water samples from 

the Marcellus Shale are, therefore, enriched in radium to a 

statistically significant degree (p<0.05) relative to samples 

from other formations in the basin. This relative enrichment is 

also illustrated in figure 8A. 

An important mechanism by which salinity controls 

radium activity involves competition between Ra+2 and 

other multivalent ions for adsorption sites primarily on clay 

minerals (Kraemer and Reid, 1984). In low salinity fluids, 

radium tends to be adsorbed onto mineral surfaces and with 

increasing salinity radium is progressively desorbed and 

released into solution. Sturchio and others (2001) presented 

a salinity-dependent distribution coefficient (K) between 

dissolved radium and radium adsorbed onto clay particles and 

oxide grain coatings. The logs of K and TDS show a linear 

relationship with negative slope, indicating less adsorption 

of radium at higher salinities and, therefore, more radium in 

solution (Sturchio and others, 2001, fig. 7).

In a study of saline groundwater systems in the midcontinent with TDS concentrations reaching 250,000 mg/L, 

Sturchio and others (2001, fig. 5) used equilibrium speciation 

calculations to demonstrate that Ra+2 was the predominant 

dissolved radium species, independent of salinity. In their 

analysis, Ra+2 never accounted for less than 77 percent of the 

total dissolved radium over a range of fluid chemistries. The 

next most abundant species, RaCl+, gained significance with 

increasing salinity and Cl–/SO4

–2 ratios. Additionally, Sturchio 

and others (2001) reported that radium forms strong organic 

complexes at elevated salinities, which may be significant 

because limited, unpublished data for organic compounds in 

Appalachian Basin produced waters have shown significant 

concentrations of acetate and other anions of carboxylic acids.

Dissolved radium measured in produced water samples 

originates from the decay of the parent isotopes, U-238 

and Th-232, in uranium- and thorium-bearing minerals or 

organic material contained in the host formation. The physical 

transfer of radium from the solid to the aqueous phase is 

discussed and illustrated in Fisher (1998, fig. 2) and Sturchio 

and others (2001). Uranium and thorium, unlike radium, are 

poorly soluble in the oxygen-poor, reducing conditions that 

6

See Crawley (2007), for example, for additional discussion of the 

ANCOVA and related statistical methods.
Discussion 13

Figure 7. (A) Log activity of total radium (Ra-226 + Ra-228) in relation to log total dissolved solids and (B) log activity 

of Ra-226 in relation to log total dissolved solids. Linear regression lines are shown for data from the Marcellus 

Shale (red), and for non-Marcellus Shale (blue) data; the lines are solid over the range of the data and dashed where 

extrapolated. Radium analyses listed as “ND” or not detected (well nos. 2 and 14) indicate values below the reported 

level of quantification (LOQ), 1 pCi/L. These points were replaced by one-half of the LOQ, or 0.5 pCi/L, and are plotted 

as open squares, but are not included in the regression. A reported Ra-226 activity of 0 (well no. 123) was replaced 

by 0.5 pCi, and is plotted as an open circle, but was not included in the regression.

Marcellus Shale Data

EXPLANATION

Non-Marcellus Shale Data

Marcellus ND

Non-Marcellus ND

Marcellus Shale Data

EXPLANATION

Non-Marcellus Shale Data

Marcellus ND

Non-Marcellus ND

Log Ra-226 = 1.56 x Log TDS – 5.60

Log Ra-226 = 1.56 x Log TDS – 5.05

Log total Ra = 1.55 x Log TDS – 4.86

Log total Ra = 1.55 x TDS – 5.26

Figure 7.

A

B

–1.0

0.0

1.0

2.0

3.0

4.0

5.0

3.0 4.0 5.0 6.0

Log total dissolved solids (TDS), in milligrams per liter

Log Ra-226, in picocuries per liter

0.1

1.0

10

100

1,000

10,000

100,000

1,000 10,000 100,000 1,000,000

Total dissolved solids (TDS), in milligrams per liter

Ra-226, in picocuries per lite

–1.0

0.0

1.0

2.0

3.0

4.0

5.0

3.0 4.0 5.0 6.0

Log total dissolved solids (TDS), in milligrams per liter

Log total radium, in picocuries per liter

0.1

1.0

10

100

1,000

10,000

100,000

1,000 10,000 100,000 1,000,000

Total dissolved solids (TDS), in milligrams per liter

Total radium, in picocuries per liter
14 Radium Content of Oil- and Gas-Field Produced Waters in the Northern Appalachian Basin: Summary and Discussion

Figure 8. (A) Total radium and (B) Ra-228/Ra-226 plotted against the age of the producing formation. For formations with 

large numbers of analyses, the median is shown as a solid black dot. 

Upper Devonian sandstones

Middle Devonian, Marcellus Shale

Middle Devonian, Huntersville Chert

Middle Devonian, Onondaga Limestone

Lower Devonian, Oriskany/Ridgely Sandstone

Lower Devonian, Helderberg Limestone

Upper Silurian, Bass Islands/Akron Dolomite

Lower Silurian, Medina/Tuscarora Sandstone

Upper Orodvician, Queenston Shale

Ordovician, undifferentiated

Upper Cambrian, Theresa Sandstone

Unknown age Median

EXPLANATION

Upper Devonian sandstones

Middle Devonian, Marcellus Shale

Middle Devonian, Huntersville Chert

Middle Devonian, Onondaga Limestone

Lower Devonian, Oriskany/Ridgely Sandstone

Lower Devonian, Helderberg Limestone

Upper Silurian, Bass Islands/Akron Dolomite

Lower Silurian, Medina/Tuscarora Sandstone

Upper Orodvician, Queenston Shale

Ordovician, undifferentiated

Upper Cambrian, Theresa Sandstone

Unknown age Median

EXPLANATION

Figure 8.

A

B Ordovician Cambrian Silurian DevonianUpper

Middle

Lower

Upper

Middle

Lower

Upper

Middle

Lower

Upper

Middle

Unknown Ordovician Cambrian Silurian DevonianUpper

Middle

Lower

Upper

Middle

Lower

Upper

Middle

Lower

Upper

Middle

Unknown

0.0 1.0 2.0 3.0 4.0

Ra-228/Ra-226

Formation Age

Total radium, in picocuries per liter

Formation Age

0 2,000 4,000 6,000 8,000 10,000 12,000 14,000 16,000
References Cited 15

are typical of oil- and gas-producing horizons and are likely 

to be more concentrated in mineral phases or organic matter 

than in solution (Langmuir and Herman, 1980; Kraemer and 

Reed, 1984; Fisher, 1998; Sturchio and others, 2001). Thus, 

dissolved radium that is in secular equilibrium with its parent 

isotopes of uranium and thorium at depth in a reservoir may be 

isolated from its parents when pumped to the surface. 

In addition to displaying higher radium activities for a 

given salinity, produced water samples from the Marcellus 

Shale have distinctly lower Ra-228/Ra-226 ratios (median of 

0.16) than those of non-Marcellus samples (median of 1.1; 

figs. 8A–B), reflecting the Th/U ratio of the reservoir lithologies. Organic carbon has long been known to play a role in 

concentrating uranium (Swanson, 1960, 1961; Szalay, 1964), 

and recent work by Bank and others (2010) has documented 

a close spatial association between the organic matter and 

uranium in the Marcellus Shale. As an organic-rich black 

shale, the Marcellus is readily identified on geophysical logs 

by its high gamma-ray signal (Schmoker, 1981; Harper, 2008). 

In eastern Pennsylvania, numerous minor occurrences 

of uranium have been reported in upper Paleozoic sandstones 

surveyed at roadside outcrops (Klemic, 1962). If the uranium 

enrichment is assumed to extend into the subsurface, it 

provides a potential source for the radium reported in nonMarcellus Shale produced waters, and as discussed above, 

high formation water salinity can account for elevated radium 

activities in solution. 

The Ra-228/Ra-226 ratios span a wide range among the 

non-Marcellus produced waters, and the highest values occur 

in samples from the Lower Silurian Medina Group/Tuscarora 

Sandstone. The median ratio for Medina/Tuscarora produced 

water samples is 1.61 (fig. 8B). Interestingly, this ratio is 

consistent with the data compiled by Vengosh and others 

(2009, fig. 4), which suggest an average isotopic ratio of 

approximately 1.6 for sandstones worldwide. The sandstones 

of the Upper Devonian Bradford Group have lower isotopic 

ratios (median, 0.78), possibly because of the interfingering of 

sandstone with siltstone and shale beds in this interval. 

Summary

Produced water salinities from reservoirs in rocks of 

Cambrian-Devonion age in the Appalachian Basin commonly 

exceed 100,000 mg/L, and far exceed the salinities of many 

other oil- and gas-producing regions in the United States, 

including basins in California, the Great Plains, and Colorado 

Plateau. In many basins, radium activity is correlated with 

salinity, and particularly among samples from lithologically 

homogeneous reservoirs, salinity may be used as an indicator 

of radium activity. The data compiled for Pennsylvania 

indicate a relationship similar to that described in other basins; 

total radium and Ra-226 activities are linearly correlated with 

TDS. Salinity was not reported in the datasets for New York. 

The radium activities in non-Marcellus produced waters 

in this report are broadly comparable to those reported in 

other studies of deep sedimentary basins with highly saline 

formation water. In the produced water dataset for the 

Marcellus Shale in New York, total radium activities have a 

distinctly higher median (5,490 pCi/L) than reported for other 

formations in the Appalachian Basin, and range to higher 

values than reported in other basins. Produced waters from 

the Marcellus in Pennsylvania have similar ranges to the New 

York data, but a lower median value (1,727 pCi/L), interpreted 

as being due, at least in part, to dilution of formation water by 

formation water injected for hydraulic fracturing. 

In the data compiled here, Ra-228/Ra-226 ratios in 

produced water from the Marcellus Shale are most commonly 

less than 0.3, and samples from non-Marcellus reservoirs 

generally have Ra-228/Ra-226 ratios greater than 1. Elevated 

total radium activities combined with low Ra-228/Ra-226 

ratios characterize produced waters from the Marcellus Shale, 

and these characteristics might be used to constrain the origin 

of samples of unknown provenance. 

Acknowledgments

Funding for this project was provided by the USGS 

Energy Resources Program and the USGS Toxic Substances 

Hydrology Program. Reviews by Zoltan Szabo and James 

Otton and comments provided by Robert Zielinski are 

gratefully acknowledged. Insightful comment and discussion 

was provided by Richard Hammack and Daniel Soeder 

(U.S. Department of Energy National Energy Technology 

Laboratory). 

References Cited

Akovali, Y.A., 1996, Nuclear data sheets for A = 226: Nuclear 

Data Sheets, v. 77, p. 433–470, accessed July 13, 2011, at 

http://www.nndc.bnl.gov.

Ames, L.L., McGarrah, J.E., and Walker, B.A., 1983, Sorption 

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16 Radium Content of Oil- and Gas-Field Produced Waters in the Northern Appalachian Basin: Summary and Discussion

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Table 1 19

Table 1. Well locations and related information compiled for samples used in this study. The Well/Sample ID column assigns a unique number to each sample; digits to the right of the decimal (for example, “5.1,” “5.2”) indicate a time series or multiple samples taken from a well on different dates to characterize changes over time.—Continued[Sh., shale; Ss., sandstone; Dolo., dolomite; Fm., formation; Gp., Group; L., lower; M., middle; U., upper; undiv., undivided]

Well / 

Sample ID

Sample 

collection date State County Township Longitude Latitude Description of sample site Producing formation Producing formation age Well type

Source: PA DEP (2009–2010)

1 11/18/2009 PA Clinton Chapman –77.56 41.37 Storage tank Marcellus Sh. Devonian, M. Gas2 11/20/2009 PA Clinton Beech Creek –77.68 41.20 Storage tank Marcellus Sh. Devonian, M. Gas3 6/1/2009 PA Bradford Burlington –76.60 41.74 Marcellus Sh. Devonian, M. Gas4 8/24/2009 PA Lycoming Penn –76.63 41.28 Marcellus Sh. Devonian, M. Gas5.1 3/18/2009 PA Lycoming Penn –76.66 41.27 Marcellus Sh. Devonian, M. Gas5.2 3/30/2009 PA Lycoming Penn –76.66 41.27 Marcellus Sh. Devonian, M. Gas6 12/21/2009 PA Tioga Charleston –77.21 41.79 Marcellus Sh. Devonian, M. Gas7 12/21/2009 PA Tioga Richmond –77.13 41.78 Marcellus Sh. Devonian, M. Gas8 9/8/2009 PA Centre Burnside –78.05 41.13 Impoundment Marcellus Sh. Devonian, M. Gas9 1/8/2010 PA Forest Jenks –79.16 41.55 Tank or lined pit Marcellus Sh. Devonian, M. Oil10 12/30/2009 PA Potter East Fork –77.88 41.61 Marcellus Sh. Devonian, M. Gas11.1 4/9/2009 PA Washington Cross Creek –80.39 40.26 Marcellus Sh. Devonian, M. Gas11.2 6/29/2009 PA Washington Cross Creek –80.39 40.26 Marcellus Sh. Devonian, M. Gas12 12/30/2009 PA Tioga Gainesville –77.56 41.69 Marcellus Sh. Devonian, M. Gas13 12/30/2009 PA Tioga Gainesville –77.58 41.68 Tuscarora Fm. Silurian, L. Gas14 1/7/2010 PA Potter West Branch –77.62 41.67 Marcellus Sh. Devonian, M. Gas15 12/16/2009 PA Clearfield Lawrence –78.45 41.17 Marcellus Sh. Devonian, M. Gas16 12/22/2009 PA Westmoreland Washington –79.57 40.49 Marcellus Sh. Devonian, M. Gas17 12/7/2009 PA Westmoreland Washington –79.56 40.50 Marcellus Sh. Devonian, M. Gas18 11/13/2009 PA Westmoreland Bell –79.55 40.51 Marcellus Sh. Devonian, M. Gas19 9/18/2009 PA Westmoreland Hempfield –79.65 40.28 Marcellus Sh. Devonian, M. Gas20 7/16/2009 PA Westmoreland Hempfield –79.57 40.50 Marcellus Sh. Devonian, M. Gas21 7/23/2009 PA Indiana Rayne –79.04 40.75 Marcellus Sh. Devonian, M. Gas22 7/31/2009 PA Westmoreland Washington –79.58 40.50 Marcellus Sh. Devonian, M. Gas23 8/13/2009 PA Westmoreland Bell –79.54 40.50 Marcellus Sh. Devonian, M. Gas
20 Radium Content of Oil- and Gas-Field Produced Waters in the Northern Appalachian Basin: Summary and Discussion Table 1. Well locations and related information compiled for samples used in this study. The Well/Sample ID column assigns a unique number to each sample; digits to the right of the decimal (for example, “5.1,” “5.2”) indicate a time series or multiple samples taken from a well on different dates to characterize changes over time.—Continued [Sh., shale; Ss., sandstone; Dolo., dolomite; Fm., formation; Gp., Group; L., lower; M., middle; U., upper; undiv., undivided] Well / Sample ID Sample collection date State County Township Longitude Latitude Description of sample site Producing formation Producing formation age Well type Source: NYSDEC (2009) 24 4/1/2009 NY Steuben Avoca –77.41 42.40 Marcellus Sh. Devonian, M. Gas 25 4/1/2009 NY Steuben Avoca –77.42 42.41 Marcellus Sh. Devonian, M. Gas 26 4/2/2009 NY Chenango Oxford –75.61 42.45 Marcellus Sh. Devonian, M. Gas 27.1 10/7/2008 NY Steuben Caton –77.04 42.05 Marcellus Sh. Devonian, M. Gas 27.2 4/1/2009 NY Steuben Caton –77.04 42.05 Marcellus Sh. Devonian, M. Gas 28 10/8/2008 NY Schuyler Orange –77.08 42.28 Marcellus Sh. Devonian, M. Gas 29 4/1/2009 NY Steuben Woodhull –77.44 42.02 Marcellus Sh. Devonian, M. Gas 30 4/1/2009 NY Steuben Troupsburg –77.47 42.02 Marcellus Sh. Devonian, M. Gas 31 4/6/2009 NY Schuyler Dix –76.94 42.34 Marcellus Sh. Devonian, M. Gas 32 4/6/2009 NY Schuyler Dix –76.94 42.34 Marcellus Sh. Devonian, M. Gas 33 3/26/2009 NY Schuyler Orange –77.07 42.29 Marcellus Sh. Devonian, M. Gas 34 4/6/2009 NY Schuyler Reading –76.91 42.44 Marcellus Sh. Devonian, M. Gas 35 10/8/2008 NY Schuyler Orange –77.06 42.29 Marcellus Sh. Devonian, M. Gas Source: NYSDEC (1999) 36 NY Cattaraugus –78.66 42.42 Brine tank Medina Gp. Silurian, L. Gas 37 NY Cattaraugus –78.66 42.42 Brine tank Medina Gp. Silurian, L. Gas 38 NY Cattaraugus –78.68 42.44 Brine tank Medina Gp. Silurian, L. Gas 39 NY Cattaraugus –78.68 42.47 Brine tank (rusted) Medina Gp. Silurian, L. Gas 40 NY Cattaraugus –78.72 42.46 Brine tank Medina Gp. Silurian, L. Gas 41 NY Cattaraugus –78.71 42.46 Brine tank Medina Gp. Silurian, L. Gas 42 NY Erie –78.47 42.93 Bottom of brine tank Medina Gp. Silurian, L. Gas 43 NY Genesee –78.46 42.93 Bottom of brine tank Medina Gp. Silurian, L. Gas 44 NY Genesee –78.46 43.03 Brine tank, subsurface Medina Gp. Silurian, L. Gas 45 NY Genesee –78.45 43.02 Brine tank Medina Gp. Silurian, L. Gas

46 NY Genesee –78.25 43.05 Brine tank Medina Gp. Silurian, L. Gas
Table 1 21

Table 1. Well locations and related information compiled for samples used in this study. The Well/Sample ID column assigns a unique number to each sample; digits to the right of the decimal (for example, “5.1,” “5.2”) indicate a time series or multiple samples taken from a well on different dates to characterize changes over time.—Continued[Sh., shale; Ss., sandstone; Dolo., dolomite; Fm., formation; Gp., Group; L., lower; M., middle; U., upper; undiv., undivided]

Well / 

Sample ID

Sample 

collection date State County Township Longitude Latitude Description of sample site Producing formation Producing formation age Well type

Source: NYSDEC (1999)—Continued

47 NY Genesee –78.26 43.05 Brine tank, 

subsurface 

Medina Gp. Silurian, L. Gas

48 NY Genesee –78.30 42.95 Brine tank, 

subsurface 

Medina Gp. Silurian, L. Gas

49 NY Genessee –78.30 42.88 Brine tank Medina Gp. Silurian, L. Gas50 NY Wyoming –78.10 42.82 Brine tank 

(rusted) 

Theresa Ss. Cambrian, U. Gas

51 NY Wyoming –78.10 42.83 Brine tank Theresa Ss. Cambrian, U. Gas52 NY Wyoming –78.12 42.82 Brine tank Medina Gp. Silurian, L. Gas53 NY Wyoming –78.11 42.81 Brine tank Theresa Ss. Cambrian, U. Gas54 NY Wyoming –78.36 42.74 Brine tank Medina Gp. Silurian, L. Gas55 NY Cayuga –76.64 42.91 Spigot, base of 

brine tank 

Queenston Sh. Ordovician, U. Gas

56 NY Cayuga –76.65 42.91 Spigot, base of 

brine tank 

Queenston Sh. Ordovician, U. Gas

57 NY Seneca –76.86 42.84 Spigot, base of 

brine tank 

Queenston Sh. Ordovician, U. Gas

58 NY Seneca –76.85 42.84 Spigot, base of 

brine tank 

Queenston Sh. Ordovician, U. Gas

59 NY Seneca –76.90 42.78 Spigot, base of 

brine tank 

Rochester Sh. Silurian, L. Gas

60 NY Genesee –77.98 42.93 Brine tank Medina Gp. Silurian, U. Gas61 NY Livingston –77.91 42.94 Brine tank Medina Gp. Silurian, L. Gas62 NY Ontario –77.54 42.81 Brine tank Medina Gp. Silurian, L. Gas63 NY Chautauqua –79.52 42.38 Bottom of brine 

tank 

Medina Gp. Silurian, L. Gas

64 NY Chautauqua –79.72 42.27 Bottom of brine 

tank 

Medina Gp. Silurian, L. Gas

65 NY Chautauqua –79.58 42.16 Brine tank Medina Gp. Silurian, L. Gas
22 Radium Content of Oil- and Gas-Field Produced Waters in the Northern Appalachian Basin: Summary and Discussion Table 1. Well locations and related information compiled for samples used in this study. The Well/Sample ID column assigns a unique number to each sample; digits to the right of the decimal (for example, “5.1,” “5.2”) indicate a time series or multiple samples taken from a well on different dates to characterize changes over time.—Continued [Sh., shale; Ss., sandstone; Dolo., dolomite; Fm., formation; Gp., Group; L., lower; M., middle; U., upper; undiv., undivided] Well / Sample ID Sample collection date State County Township Longitude Latitude Description of sample site Producing formation Producing formation age Well type Source: NYSDEC (1999)—Continued 66 NY Chautauqua –79.54 42.08 Brine tank Bass Islands Dolo. Silurian, U. Oil 67 NY Chautauqua –79.43 42.09 Brine tank Medina Gp. Silurian, L. Gas 68 NY Chautauqua –79.47 42.13 Brine tank Bass Islands Dolo. Silurian, U. Oil 69 NY Chautauqua –79.42 42.16 Brine drain tank Bass Islands Dolo. Silurian, U. Oil 70 NY Erie –78.89 42.54 Brine tank Onondaga Ls. Devonian, M. Gas 71 NY Chautauqua –79.01 42.38 Brine tank Medina Gp. Silurian, L. Gas 72 NY Chautauqua –79.16 42.31 Brine tank Medina Gp. Silurian, L. Gas 73 NY Chautauqua –79.19 42.31 Bottom of stock tank Devonian, U., undiv. Devonian, U. Gas–Oil 74 NY Chautauqua –79.24 42.23 Bottom of stock tank Bass Islands Dolo. Silurian, U. Oil 75 NY Chautauqua –79.36 42.17 Brine tank Bass Islands Dolo. Silurian, U. Gas–Oil 76 NY Chautauqua –79.38 42.22 Brine tank Medina Gp. Silurian, L. Gas 77 NY Chautauqua –79.30 42.16 Brine tank Medina Gp. Silurian, L. Gas 78 NY Chautauqua –79.27 42.07 Brine tank Medina Gp. Silurian, L. Gas 79 NY Erie –78.79 42.56 Brine tank Medina Gp. Silurian, L. Gas 80 NY Allegany –77.92 42.01 Brine tank Oriskany Ss. Devonian, L. Gas 81 NY Allegany –77.95 42.01 Brine tank Oriskany Ss. Devonian, L. Gas 82 NY Tioga –76.26 42.03 Brine tank Helderberg Ls. Devonian, L. Gas 83 NY Tioga –76.31 42.00 Brine tank Helderberg Ls. Devonian, L. Gas
Table 1 23

Table 1. Well locations and related information compiled for samples used in this study. The Well/Sample ID column assigns a unique number to each sample; digits to the right of the decimal (for example, “5.1,” “5.2”) indicate a time series or multiple samples taken from a well on different dates to characterize changes over time.—Continued[Sh., shale; Ss., sandstone; Dolo., dolomite; Fm., formation; Gp., Group; L., lower; M., middle; U., upper; undiv., undivided]

Well / 

Sample ID

Sample 

collection date State County Township Longitude Latitude Description of sample site Producing formation Producing formation age Well type

Source: PA DEP (1992)

84 PA Allegheny S. Fayette –80.21 40.36 Diked area Gas85 PA Armstrong Cowanshannock –79.26 40.79 Tank Devonian, U. Gas86 PA Armstrong Cowanshannock –79.25 40.78 Tank Catskill/Lock 

Haven Fms.

Devonian, U. Gas

87 PA Cambria Susquehanna –78.76 40.70 Tank Venango Gp. Devonian, U. Gas88 PA Cambria Barr –78.83 40.66 Tank Lock Haven 

Fm.

Devonian, U. Gas

89 PA Centre Curtin –77.77 41.11 Tank Catskill/Lock 

Haven Fms.

Devonian, U. Gas

90 PA Centre Burnside –77.87 41.12 Tank Catskill/Lock 

Haven Fms.

Devonian, U. Gas

91 PA Clearfield Jordan –78.61 40.83 Tank Catskill/Lock 

Haven Fms.

Devonian, U. Gas

92 PA Clearfield Burnside –78.72 40.84 Tank Lock Haven 

Fm.

Devonian, U. Gas

93 PA Clinton Beech Creek –77.70 41.17 Tank Lock Haven 

Fm.

Devonian, U. Gas

94 PA Clinton Beech Creek –77.74 41.15 Tank Medina Gp. Silurian, L. Gas95 PA Crawford Beaver –80.41 41.81 Tank Medina Gp. Silurian, L. Gas96 PA Elk Highland –78.83 41.54 Separator tank Bradford Gp. Devonian, U. Oil97 PA Elk Highland –78.93 41.51 Tank Devonian Oil98 PA Erie Millcreek –80.17 42.08 Tank Medina Gp. Silurian, L. Gas99 PA Erie Conneaut –80.44 41.89 Tank Huntersville 

Chert

Devonian, M. Gas

100 PA Fayette Springfield –79.36 39.97 Tank Oriskany Ss. Devonian, L. Gas101 PA Fayette Springfield –79.40 39.96 Tank Huntersville 

Chert

Devonian, M. Gas

102 PA Forest Howe –79.14 41.56 Tank battery Warren sand Devonian, U. Oil103 PA Forest Kingsley –79.29 41.58 Tank Devonian, U., 

undiv.

Devonian, U. Oil

104 PA Indiana Cherryhill –78.82 40.74 Tank Kane sand Devonian, U. Gas
24 Radium Content of Oil- and Gas-Field Produced Waters in the Northern Appalachian Basin: Summary and Discussion Table 1. Well locations and related information compiled for samples used in this study. The Well/Sample ID column assigns a unique number to each sample; digits to the right of the decimal (for example, “5.1,” “5.2”) indicate a time series or multiple samples taken from a well on different dates to characterize changes over time.—Continued [Sh., shale; Ss., sandstone; Dolo., dolomite; Fm., formation; Gp., Group; L., lower; M., middle; U., upper; undiv., undivided] Well / Sample ID Sample collection date State County Township Longitude Latitude Description of sample site Producing formation Producing formation age Well type Source: PA DEP (1992)—Continued 105 PA Indiana Burrell –79.17 40.48 Tank Fifty Foot sand Devonian, U. Gas 106 PA Indiana White –79.19 40.65 Tank Gas 107 PA Jefferson Bell –78.90 40.97 Tank Devonian, U., undiv. Devonian, U. Gas 108 PA McKean Wetmore –78.87 41.63 Separator pit Unknown Oil 109 PA McKean Lafayette –78.72 41.83 Pit Oriskany Ss. Devonian, L. Oil 110 PA Somerset Middlecreek –78.92 40.06 Tank Oriskany Ss. Devonian, L. Gas 111 PA Somerset Lincoln –79.07 40.08 Tank Huntersville Chert Devonian, M. Gas 112 PA Tioga Union –76.96 41.57 Drill pit Ordovician Gas 113 PA Venango Cornplanter –79.59 41.48 Separator Red Valley sand Devonian, U. Oil 114 PA Venango Allegheny –79.55 41.57 Pit Venango Gp. Devonian, U. Oil 115 PA Warren Pleasant –79.19 41.81 Pit Medina Gp. Silurian, L. Oil 116 PA Warren Southwest –79.57 41.63 Tank Medina Gp. Silurian, L. Gas 117 PA Warren Watson –79.25 41.76 Pit Devonian, U., undiv. Devonian, U. Oil 118 PA Washington Cecil –80.24 40.33 Separator Devonian, U. Oil 119 PA Westmoreland Washington –79.58 40.49 Tank Venango Gp. Devonian, U. Gas 120 PA Westmoreland Hempfield –79.53 40.26 Tank Venango Gp. Devonian, U. Gas Source: Dresel and Rose (2010) 121 1982 PA Indiana Banks –78.85 40.87 Wellhead Devonian, U., undiv. Devonian, U. Gas 122 1982 PA Indiana South Mahoning –79.14 40.78 Wellhead Devonian, U., undiv. Devonian, U. Gas 123 1982 PA Warren Pleasant –79.21 41.82 Wellhead Glade sand Devonian, U. Oil 124 1982 PA Crawford Fairfield –80.14 41.49 Wellhead Medina Gp. Silurian, L. Gas 125 1982 PA Centre Boggs –77.84 41.00 Separator Tuscarora Fm. Silurian, L. Gas 126 1982 PA Somerset Black –79.11 39.93 Separator Ridgeley Ss. Devonian, L. Gas
Table 1 25

Table 1. Well locations and related information compiled for samples used in this study. The Well/Sample ID column assigns a unique number to each sample; digits to the right of the decimal (for example, “5.1,” “5.2”) indicate a time series or multiple samples taken from a well on different dates to characterize changes over time.—Continued[Sh., shale; Ss., sandstone; Dolo., dolomite; Fm., formation; Gp., Group; L., lower; M., middle; U., upper; undiv., undivided]

Well / 

Sample ID

Sample 

collection date State County Township Longitude Latitude Description of sample site Producing formation Producing formation age Well type

Source: Pritz (2010), this study

127 04/09 PA Bradford Marcellus Sh. Devonian, M. Gas128 04/09 PA Bradford Marcellus Sh. Devonian, M. Gas129 04/09 PA Bradford Marcellus Sh. Devonian, M. Gas130 04/09 PA Bradford Marcellus Sh. Devonian, M. Gas131 04/09 PA Bradford Marcellus Sh. Devonian, M. Gas

Source: This study

132.1 12/8/2010 PA Greene –80.05 39.88 Separator Marcellus Sh. Devonian, M. Gas132.2 12/29/2010 PA Greene –80.05 39.88 Separator Marcellus Sh. Devonian, M. Gas132.3 12/30/2010 PA Greene –80.05 39.88 Separator Marcellus Sh. Devonian, M. Gas132.4 12/31/2010 PA Greene –80.05 39.88 Separator Marcellus Sh. Devonian, M. Gas132.5 1/1/2011 PA Greene –80.05 39.88 Separator Marcellus Sh. Devonian, M. Gas132.6 1/2/2011 PA Greene –80.05 39.88 Separator Marcellus Sh. Devonian, M. Gas132.7 1/4/2011 PA Greene –80.05 39.88 Separator Marcellus Sh. Devonian, M. Gas132.8 1/12/2011 PA Greene –80.05 39.88 Separator Marcellus Sh. Devonian, M. Gas132.9 1/17/2011 PA Greene –80.05 39.88 Separator Marcellus Sh. Devonian, M. Gas
26 Radium Content of Oil- and Gas-Field Produced Waters in the Northern Appalachian Basin: Summary and Discussion Table 2. Ra-226, Ra-228, gross alpha, and gross beta activities measured in samples of produced water for wells listed in table 1. Analytical uncertainties are included when known.—Continued [TDS, total dissolved solids; mg/L, milligram per liter; pCi/L, picocurie per liter; ND, not detected] Well / Sample ID TDS (mg/L) Gross alpha (pCi/L) +/– Gross beta (pCi/L) +/– Ra-226 (pCi/L) +/– Ra-228 (pCi/L) +/– Total radium (pCi/L) Ra-228/ Ra-226 Method, method codes Source: PA DEP (2009–2010) 

1 54,000 436 32.2 121 8.2 556 0.28 SM2540C; EPA904.0, 903.02 16,200 14 2 1,322 86 ND 1.8 ND 0.3 SM2540C, 7110C; EPA 900.0, 903.0, 904.03 333,000 19,220 2,843 7,944 1,320 50 1.3 37 3.3 87 0.73 SM2540C; EPA 900.0 903.0, 904.04 61,800 6,159 743 1,325 190 430 11.0 51 8.9 482 0.12 SM2540C; EPA 900.0, 903.0, 904.05.1 38,200 454 126 149 78 66 4.0 2.2 0.9 68 0.03 SM2540C; EPA 900.0, 903.0, 904.05.2 82,600 1,644 371 745 242 239 9.7 38 6.3 277 0.16 SM2540C; EPA 900.0, 903.0, 904.06 40,880 7,512 750 732 16,920 3,283 1,125 227 18,045 0.07 EPA 903.1, 904.07 21,960 4,074 980 757 11,120 2,204 1,287 261 12,407 0.12 EPA 903.1, 904.08 124,000 1,525 110 657 76 2,182 0.43 SM18 2540C; EPA 901.1 Mod.9 284,000 11,810 2,482 1,060 759 4,184 789 1,074 202 5,258 0.26 SM20 2540C; EPA 903.1, 904.010 157,000 7,330 460 1,180 180 8,510 0.16 SM18 2540C; EPA 901.1 Mod.11.1 157,000 951 86 703 69 1,654 0.74 SM18 2540C; EPA 901.1 Mod.11.2 200,000 1,280 130 1,110 120 2,390 0.87 SM18 2540C; EPA 901.1 Mod.12 183,000 7,530 1,141 2,683 372 562 26 648 67 1,210 1.15 SM18 2540C; EPA 900.0, 903.0, 904.013 358,000 10,356 2,186 11,595 723 892 32 2,589 128 3,481 2.90 SM18 2540C; EPA 900.0, 903.0, 904.014 1,470 ND 3 78 4 ND 0.31 ND 0.39 1.00 SM2540C; EPA 900.0, 903.0, 904.015 288,900 19,240 7,049 1,268 106 1,374 0.08 SM2540C16 24,700 318 453 340 590 103 24 168 32 271 1.63 SM2540C; EPA 900.0Mod., 903.1, 904.017 88,500 3,640 1,004 ND 631 1,042 197 298 59 1,340 0.29 SM2540C; EPA 900.0Mod., 903.1, 904.018 116,000 2,320 800 2,077 929 1,037 200 515 97 1,552 0.50 SM2540C; EPA 900.0Mod., 903.1, 904.019 32,500 733 175 81 61 554 104 5.5 1.9 559 0.01 SM2540C; EPA 900.0Mod., 903.1, 904.020 45,400 845 213 379 116 66 4.05 1.4 0.3 67 0.02 SM2540C; EPA 900.0, 903.0, 904.021 46,460 820 249 505 140 76 2.7 23 2.4 99 0.30 SM2540C; EPA 900.0, 903.0, 904.022 47,800 585 163 536 83 36 1.75 2.7 0.2 39 0.08 SM2540C; EPA 900.0, 903.0, 904.023 125,100 2,103 631 1,574 335 229 6.8 56 6.5 285 0.25 SM2540C; EPA 900.0, 903.0, 904.0
Table 2 27

Table 2. Ra-226, Ra-228, gross alpha, and gross beta activities measured in samples of produced water for wells listed in table 1. Analytical uncertainties are included when known.—Continued[TDS, total dissolved solids; mg/L, milligram per liter; pCi/L, picocurie per liter; ND, not detected]

Well / 

Sample 

ID

 TDS 

(mg/L) 

Gross 

alpha 

(pCi/L)

 +/– 

Gross 

beta 

(pCi/L)

+/– Ra-226 (pCi/L) +/– Ra-228 (pCi/L) +/– Total radium (pCi/L) Ra-228/ Ra-226 Method, method codes

 Source: NYSDEC (2009) 

24 70 48 7 54 0.163 0.20 0.029 0.22 0.192 0.175 25 54.6 37 59 58 0.195 0.16 0.428 0.34 0.623 2.195 26 3,914 813 715 202 1,779 343 201 39 1,980 0.113 27.1 17,940 8,634 4,765 3,829 2,472 484 874 174 3,346 0.354 27.2 3,968 1,102 618 599 7,885 1,568 234 51 8,119 0.030 28 206,446 14,530 3,792 4,561 1,634 2,647 494 782 157 3,429 0.295 29 9,426 2,065 2,780 879 4,049 807 826 160 4,875 0.204 30 7,974 1,800 1,627 736 5,352 1,051 138 37 5,490 0.026 31 10,970 2,363 1,170 701 6,125 1,225 516 99 6,641 0.084 32 20,750 4,117 2,389 861 10,160 2,026 1,252 237 11,412 0.123 33 205,102 18,330 3,694 ND 654 13,510 2,655 929 179 14,439 0.069 34 16,550 3,355 1,323 711 15,140 2,989 957 181 16,097 0.063 35 123,000 23,480 12,000 2,903 16,030 2,995 912 177 16,942 0.057 

 Source: NYSDEC (1999) 

36 669 88 1,100 250 1,769 1.644 γ-spectrometry37 402 68 402 γ-spectrometry38 1,164 93 429 27 1,593 0.369 γ-spectrometry39 398 64 234 182 632 0.588 γ-spectrometry40 259 47 259 γ-spectrometry41 409 60 409 γ-spectrometry42 413 61 856 222 1,269 2.073 γ-spectrometry43 260 43 703 194 963 2.704 γ-spectrometry44 63 71 63 γ-spectrometry45 169 86 565 254 734 3.343 γ-spectrometry46 306 126 568 248 874 1.856 γ-spectrometry47 175 100 255 179 430 1.457 γ-spectrometry48 347 55 347 γ-spectrometry49 290 50 460 172 750 1.586 γ-spectrometry
28 Radium Content of Oil- and Gas-Field Produced Waters in the Northern Appalachian Basin: Summary and Discussion Table 2. Ra-226, Ra-228, gross alpha, and gross beta activities measured in samples of produced water for wells listed in table 1. Analytical uncertainties are included when known.—Continued [TDS, total dissolved solids; mg/L, milligram per liter; pCi/L, picocurie per liter; ND, not detected] Well / Sample ID TDS (mg/L) Gross alpha (pCi/L) +/– Gross beta (pCi/L) +/– Ra-226 (pCi/L) +/– Ra-228 (pCi/L) +/– Total radium (pCi/L) Ra-228/ Ra-226 Method, method codes Source: NYSDEC (1999)—Continued 50 764 81 433 242 1,197 0.567 γ-spectrometry 51 450 66 326 319 776 0.724 γ-spectrometry 52 477 65 651 306 1,128 1.365 γ-spectrometry 53 708 71 350 297 1,058 0.494 γ-spectrometry 54 238 117 269 52 507 1.130 γ-spectrometry 55 1,240 100 1,290 130 2,530 1.040 γ-spectrometry 56 823 69 1,333 450 2,156 1.620 γ-spectrometry 57 557 67 933 230 1,490 1.675 γ-spectrometry 58 465 65 977 230 1,442 2.101 γ-spectrometry 59 ND γ-spectrometry 60 369 61 890 227 1,259 2.412 γ-spectrometry 61 538 72 625 207 1,163 1.162 γ-spectrometry 62 146 92 146 γ-spectrometry 63 187 20 80 29 267 0.427 γ-spectrometry 64 324 36 503 30 827 1.552 γ-spectrometry 65 444 47 1,690 55 2,134 3.806 γ-spectrometry 66 1,550 110 319 60 1,869 0.206 γ-spectrometry 67 366 45 1,660 47 2,026 4.536 γ-spectrometry 68 654 36 1,440 50 2,094 2.202 γ-spectrometry 69 1,040 40 387 32 1,427 0.372 γ-spectrometry 70 64.2 27.0 83 12 147 1.294 γ-spectrometry 71 148 17 100 23 248 0.676 γ-spectrometry 72 160 35 574 31 734 3.588 γ-spectrometry 73 185 20 86 25 271 0.467 γ-spectrometry 74 953 64 444 45 1,397 0.466 γ-spectrometry 75 585 67 585 γ-spectrometry 76 951 109 1,500 170 2,451 1.577 γ-spectrometry 77 484 32 1,420 50 1,904 2.934 γ-spectrometry

78 156 35 504 36 660 3.231 γ-spectrometry
Table 2 29

Table 2. Ra-226, Ra-228, gross alpha, and gross beta activities measured in samples of produced water for wells listed in table 1. Analytical uncertainties are included when known.—Continued[TDS, total dissolved solids; mg/L, milligram per liter; pCi/L, picocurie per liter; ND, not detected]

Well / 

Sample 

ID

 TDS 

(mg/L) 

Gross 

alpha 

(pCi/L)

 +/– 

Gross 

beta 

(pCi/L)

+/– Ra-226 (pCi/L) +/– Ra-228 (pCi/L) +/– Total radium (pCi/L) Ra-228/ Ra-226 Method, method codes

 Source: NYSDEC (1999)—Continued

79 111 35 60 23 170 0.538 γ-spectrometry80 901 52 250 42 1,151 0.278 γ-spectrometry81 691 26 154 30 845 0.223 γ-spectrometry82 3,760 100 1,110 60 4,870 0.295 γ-spectrometry83 1,620 110 1,790 60 3,410 1.105 γ-spectrometry

 Source: PA DEP (1992) 

84 143,432 512 202 714 0.395 85 315 165 480 0.524 86 20 13 33 0.650 87 175,296 1,408 904 2,312 0.642 88 195,404 1,154 1,083 2,237 0.938 89 222,672 163 126 289 0.773 90 252,980 1,489 636 2,125 0.427 91 185,146 2,015 1,749 3,764 0.868 92 230,924 107 77 184 0.720 93 194,902 731 491 1,222 0.672 94 153,096 811 530 1,342 0.653 95 396,012 599 1,683 2,282 2.810 96 31,502 15 18 33 1.150 97 25,159 23 26 49 1.143 98 390,928 628 1,478 2,106 2.355 99 378,148 588 1,483 2,072 2.521 100 341,918 4,685 2,038 6,723 0.435 101 354,034 566 2,110 2,676 3.728 102 130,588 42 42 84 1.000 103 86,988 39 56 95 1.427 104 186,736 2,019 2,196 4,215 1.088 105 198,668 2,575 1,866 4,441 0.725 106 121,928 450 313 763 0.696 
30 Radium Content of Oil- and Gas-Field Produced Waters in the Northern Appalachian Basin: Summary and Discussion Table 2. Ra-226, Ra-228, gross alpha, and gross beta activities measured in samples of produced water for wells listed in table 1. Analytical uncertainties are included when known.—Continued [TDS, total dissolved solids; mg/L, milligram per liter; pCi/L, picocurie per liter; ND, not detected] Well / Sample ID TDS (mg/L) Gross alpha (pCi/L) +/– Gross beta (pCi/L) +/– Ra-226 (pCi/L) +/– Ra-228 (pCi/L) +/– Total radium (pCi/L) Ra-228/ Ra-226 Method, method codes Source: PA DEP (1992)—Continued 107 1,280 848 2,128 0.663 108 36,470 8 12 20 1.446 109 185 184 370 0.995 110 176,676 203 1,543 1,746 7.601 111 182,274 1,988 499 2,487 0.251 112 1,137 1,457 2,594 1.281 113 114,208 12 30 42 2.500 114 36,282 54 77 131 1.426 115 59,554 34 27 61 0.794 116 395,440 795 968 1,763 1.219 117 125,264 275 187 462 0.680 118 134,164 255 456 711 1.788 119 221,134 170 46 216 0.271 120 402,148 857 71 928 0.083 Source: Dresel and Rose (2010) 121 253,000 1,900 1,900 122 244,000 200 200 123 91,000 0 0.0 124 257,000 500 500 125 259,000 5,300 5,300 126 302,000 5,000 5,000 Source: Pritz (2010), this study 127 122,527 2,653 11 318 22 2,971 0.120 γ-spectrometry 128 250,112 3,082 21 935 27 4,018 0.303 γ-spectrometry 129 134,880 1,958 26 572 37 2,530 0.292 γ-spectrometry 130 222,681 1,486 13 472 23 1,957 0.317 γ-spectrometry 131 117,259 1,756 6 377 10 2,133 0.215 γ-spectrometry
Table 2 31

Table 2. Ra-226, Ra-228, gross alpha, and gross beta activities measured in samples of produced water for wells listed in table 1. Analytical uncertainties are included when known.—Continued[TDS, total dissolved solids; mg/L, milligram per liter; pCi/L, picocurie per liter; ND, not detected]

Well / 

Sample 

ID

 TDS 

(mg/L) 

Gross 

alpha 

(pCi/L)

 +/– 

Gross 

beta 

(pCi/L)

+/– Ra-226 (pCi/L) +/– Ra-228 (pCi/L) +/– Total radium (pCi/L) Ra-228/ Ra-226 Method, method codes

 Source: This study

132.1 1,312 19 300 23 1,612 0.229 γ-spectrometry132.2 3,363 21 542 19 3,905 0.161 γ-spectrometry132.3 4,372 39 577 19 4,949 0.132 γ-spectrometry132.4 4,892 38 599 29 5,491 0.122 γ-spectrometry132.5 5,110 18 626 20 5,736 0.123 γ-spectrometry132.6 5,210 31 614 32 5,824 0.118 γ-spectrometry132.7 3,105 26 686 30 3,791 0.221 γ-spectrometry132.8 5,446 28 820 17 6,266 0.151 γ-spectrometry132.9 5,272 88 846 33 6,118 0.160 γ-spectrometry

Manuscript approved on August 4, 2011.

Prepared by the USGS Science Publishing Network, 

Raleigh Publishing Service Center

Edit and layout by Kay P. Naugle

Graphics by Francisco A. Maldonado
Rowan and others—Radium Content of Oil- and Gas-Field Produced Waters in the Northern Appalachian Basin—Scientific Investigations Report 2011–5135