Chemosphere: Luisa Torres, Om Prakash Yadav, Eakalak Khan
Chemosphere: Luisa Torres, Om Prakash Yadav, Eakalak Khan
Chemosphere: Luisa Torres, Om Prakash Yadav, Eakalak Khan
Chemosphere
journal homepage: www.elsevier.com/locate/chemosphere
Department of Civil and Environmental Engineering, North Dakota State University, Fargo, ND 58108, USA
Department of Industrial and Manufacturing Engineering, North Dakota State University, Fargo, ND 58108, USA
h i g h l i g h t s
g r a p h i c a l a b s t r a c t
a r t i c l e i n f o
a b s t r a c t
Article history:
Received 22 September 2016
Received in revised form
19 November 2016
Accepted 25 November 2016
A holistic risk assessment of surface water (SW) contamination due to lead-210 (Pb-210) in oil produced
water (PW) from the Bakken Shale in North Dakota (ND) was conducted. Pb-210 is a relatively long-lived
radionuclide and very mobile in water. Because of limited data on Pb-210, a simulation model was
developed to determine its concentration based on its parent radium-226 and historical total dissolved
solids levels in PW. Scenarios where PW spills could reach SW were analyzed by applying the four steps
of the risk assessment process. These scenarios are: (1) storage tank overow, (2) leakage in equipment,
and (3) spills related to trucks used to transport PW. Furthermore, a survey was conducted in ND to
quantify the risk perception of PW from different stakeholders. Findings from the study include a low
probability of a PW spill reaching SW and simulated concentration of Pb-210 in drinking water higher
than the recommended value established by the World Health Organization. Also, after including the
results from the risk perception survey, the assessment indicates that the risk of contamination of the
three scenarios evaluated is between medium-high to high.
2016 Elsevier Ltd. All rights reserved.
1. Introduction
Oil produced water (PW) generated during the owback process
628
2. Methodology
2.1. Method overview
A risk assessment focused on three scenarios that could result in
SW contamination was conducted. The rst scenario is storage tank
overow that reaches SW that is nearby the oil well pads. The
second scenario is leakage in pipes, storage units, and other
equipment, that reaches SW. The third scenario is accidents related
to trucks transporting PW which cause spills that reach SW. These
scenarios were selected because they were found to be common in
reported spills and media coverage in ND (Guerin, 2015; Kusnetz,
2012; ND DoH, 2015). Other scenarios that could contribute to
SW contamination such as runoff and melting snow were not
considered because of supporting data unavailability and high
variability of environmental conditions.
This research uses a combination of stochastic and deterministic
methods to analyze the risks of Pb-210 in each scenario. These
methods were combined because of the variability in the type of
data used. First, the historical TDS data, reported spills, and truck
crashes were analyzed using Palisade's @Risk tool. Second, due to
extremely limited data, the Ra-226 level in the Bakken was calculated based on a generalized linear regression model between
observed TDS and Ra-226 levels from different locations including
Pennsylvania, Texas, New York, and Wyoming.
Third, the Rutherford-Soddy's decay law was used to simulate
the decay of Ra-226 into Pb-210. @Risk was used to determine the
type of probability distribution followed by the simulated values of
Ra-226 and the parameters that describe that probability distribution. The probability distribution parameters (i.e. shape and
scale) of Ra-226 were included in the estimation of Pb-210 because
they capture the variability of the non-normal distribution of Ra-
226 data due to different factors which could not have been
considered if point estimates were used. The predicted Pb-210
concentration was used to assess the exposure by oral ingestion.
The exposure concentration was estimated using the QWASI model
that simulates chemical fate in lakes. Furthermore, a survey was
distributed in several counties in ND to collect data from different
stakeholders including general public, oil eld and truck operators,
and emergency management personnel and/or individuals in
charge of PW management (hereinafter experts). The survey
collected data on the knowledge, opinions, and concerns of each
stakeholder related to PW management. The data was analyzed to
quantify awareness and perception of the risks of each scenario
where PW could reach SW. The results from the survey were
included in the risk characterization of each scenario.
Finally, a semi-quantitative risk assessment matrix was used to
translate the results obtained in the previous steps of the risk
assessment into quantitative measurement based on low, mediumlow, medium-high, and high risk. Also, a sensitivity analysis was
carried out to evaluate the variation in the Pb-210 levels if the
simulated Ra-226 concentrations were underestimated or overestimated by 25%e50% compared to actual levels. The entire
methodology is summarized in Fig. 1.
629
regarding truck crashes in the State (Figs. S1 and S2, SM) (ND DoT,
2015).
2.3. Determination of Pb-210 concentrations
There were two steps in determining Pb-210 concentration. Ra226 concentration was estimated and then Pb-210 was calculated
based on the decay of Ra-226. In ND, data on radium in PW has not
been reported in the USGS PW database and to our knowledge, only
one study by Lauer et al. (2016) has measured Ra-226 in PW from
the Bakken but the data was based on only three samples. Because
of this, it is necessary to use a simulation approach to determine the
radium concentration. Since there is not enough data on Ra-226
from the Bakken, three different datasets from previous studies
were analyzed (Table S3a, SM). The rst dataset, which comes from
Pennsylvania and New York, was obtained from Rowan et al., 2011.
The second set, which is from Texas, was found in Fisher (1995).
Lastly, the third set, which is from Pennsylvania and Wyoming, was
retrieved from the USGS PW database for the wells that were
monitored for TDS and Ra-226 levels. Using a total of 331 data
points from the three datasets, a linear regression model with an Rsquared value of 0.80 (Tables S3b and S3c, SM) was developed as
follows:
Predict Pb-210
concentration based on
Ra-226 distribution and
decay law
Sensitiviy analysis
Simulate Ra-226
probability distribution
Analysis of results
Collect data
(1)
Fig. 1. Process followed to perform a holistic risk assessment of Pb-210 surface water contamination.
630
(2)
Pb
Ra el(1)
226
(3)
631
noted that the reports do not indicate whether these small water
bodies are directly connected to drinking water sources. Only the
incident in Williams County in January 2015, where almost 3
million gallons were spilled, impacted a drinking water source. The
spill affected the Blacktail Creek and Little Muddy River which ow
into the Missouri River, a drinking water source (Lauer et al., 2016).
In the second step of the risk assessment, the exposure to Pb210 by oral ingestion was calculated based on the average initial
concentration of 540 pCi/L determined previously. The exposure
assessment was based on the scenario where PW is accidentally
spilled and reaches a SW body that serves as human drinking water
source. The actual exposure to Pb-210 is the concentration that
remains after the contaminant undergoes different chemical and
physical processes, which happen naturally, and after the SW is
treated by different methods.
For the exposure scenario where PW reaches a SW body, the
characteristics of Lake Sakakawea were used. This lake was chosen
because it is a major source of SW for several cities in ND including
Dickinson, Williston, Garrison, and Parshall (City of Williston
(2014); ND DoH, 1999), and because it is located close to the regions with high density of oil wells. Table S5 in SM summarizes the
inputs and the sources used in the simulation. Some required inputs were not found in the literature and in these cases the default
values given by QWASI were applied (Figs. S7 and S8, SM). In
addition, processes in the air compartment were ignored because
Pb atmospheric deposition in ND is not signicant (Fig. S9, SM) (U.S.
Environmental Protection Agency, 2011).
The results from QWASI indicated that the Pb-210 concentration
that remains in the water compartment is 1.81 103 ng/L or
approximately 140 pCi/L. For detailed results, please see Figs. S10a
and S10b in SM. Among methods to remove radioactive materials
from drinking water is lime softening, ion exchange, and activated
carbon (U.S. Environmental Protection Agency, 2015). The average
removal efciency of these three methods is approximately 88%
(U.S. Environmental Protection Agency, 2015) which means that the
nal concentration after treating the water is 17 pCi/L.
Becquerels per liter (Bq/L) is another unit for radioactivity and
since 1 pCi/L is equal to 0.037 Bq/L (Keith et al., 2012) then, 17 pCi/L
is equivalent to 0.63 Bq/L. For comparison, some of the maximum
allowable levels of lead in drinking water are 0 mg/L established by
the U.S. Environmental Protection Agency, 1 pCi/L or less based on
the National Interim Primary Drinking Water Regulations, 0.1 Bq/L
according to the World Health Organization (WHO), and 0.2 Bq/L in
Canada (Shammas and Wang, 2016; U.S. Environmental Protection
Agency, 2012; Velten and Jacobs, 1982; World Health Organization,
n.d.). The concentration of Pb-210 to which a person could be
exposed to in the simulated case exceeds these standards.
To characterize the risk of each scenario, a 4 4 risk matrix
(Food and Agriculture Organization of the United Nations, n.d.)
shown in Fig. 2 was used. The risk matrix, or C L matrix, combines
consequences (C) and the probability or likelihood (L) of those
consequences happening. As seen in Table 1, C and L are divided
into four different levels. The L levels are remote, unlikely, possible,
and likely which are dened based on the probability of the event
occurring (Table 1) (Food and Agriculture Organization of the
United Nations, n.d.; Mosleh and Bari, 1998; Stouffer et al., 2015).
The four levels of C are minor, moderate, major, and extreme.
They are based on the maximum allowable concentration of the
chemical under study (Brereton and Alenbach, 1998; Stouffer et al.,
2015). For this risk assessment, the limit value used for Pb-210 in
drinking water was 0.1 Bq/L established by the WHO (n.d.). This
recommended value was used because a limit in terms of radioactivity has not been established in the U.S. (Velten and Jacobs,
1982). Table 1 describes the different consequence levels.
Each of the three scenarios that could result in SW
632
a)
b)
4
12
16
12
Scenarios 1 and 3
Scenario 2
10
15
20
25
12
16
20
12
15
10
Scenario 2 =
Scenario 1 = 11
Low
Medium-high
Medium-low
High
Scenario 3 = 9
Fig. 2. Scores for each scenario using a: a) 4 4 risk matrix for technical risk and b) 5 5 risk matrix for combined technical and social risks.
Table 1
Measurements of risk likelihood and risk consequence or impact (Pb-10 concentration in contaminated water) used for the risk matrix.
Level
1
2
3
4
Likelihood
Consequence or Impact
Description
Characteristics
Description
Remote
Unlikely
Possible
Likely
Minor
Moderate
Major
Extreme
<0.1 Bq/L
0.1e10 Bq/L
10 - 100 Bq/L
>100 Bq/L
did not indicate their place of residence within the State, 46% lived
in Cass County while the remaining 19% were in other counties
including 11 oil-producing counties. The majority of participants
was 18e24 years old and had a 4-year college degree (38% and 39%,
respectively). For the purpose of this study, only 7 questions out of
25 were used because they were focused on measuring the level of
risk perception and awareness of PW. The remaining questions will
be analyzed and presented in a different study.
The participants were asked to rank their level of concern of
each scenario where PW could reach SW. For the storage tank
overow scenario, 41% responded to be not at all to slightly concerned. For the equipment failure and truck accident scenarios, the
majority indicated to be moderately to extremely concerned (57%
and 49%, respectively). Some questions in the survey were focused
on obtaining the opinion of experts in ND which represented 8% of
Table 2
Parameters used to calculate the holistic risk score of each scenario evaluated. The
technical risk scores were obtained from the 4 4 risk matrix. The perceived risk
scores were obtained from the survey and converted to PAF values.
Parameter
Scenario 1
Scenario 2
Scenario 3
Technical risk
Perceived risk (PAF):
Level of concern with PW
Level of familiarity with PW-MGMT
Level of awareness with PW-content
Experts' opinion-risk perception
1.625
2
1.625
1.75
0.5
2
1.625
1
0.5
2
1.625
1
633
1:625 0:15 2 0:20 1:625 0:35 1:75 0:30
z11
Risksc1 4 4
1
(4)
For this study, four PAF (pafi ) were considered, each one with an
assigned weight (ai ). The values the PAF can take vary from 0.5 to 2
so that the Rtech can be reduced by half, increased by 2 folds, or in
between. The weight assigned to each PAF ranges from 0 to 1 so that
the total sum of the weights equals 1. The weights were assigned
based on the importance of the survey question or PAF to capture
the risk perception of each stakeholder. The four PAF and their
respective weights are: 1) level of concern with PW e 15%; 2) level
of familiarity with PW management e 20%; 3) level of awareness
with PW content e 35%; and 4) opinion of experts on risk perceptions e 30%.
Likert scales were used in the survey to measure the level of
concern, awareness, and familiarity. Each scale has 5 levels and
each one has a score (i.e. 5, 4, 3, 2, 1). For the quantication process,
Using the same method, the calculated risks for scenario 2 and 3
are approximately 19 and 9, respectively (see the SM for further
detail). The results indicate that by adding the quantied social risk
perception the risk of each scenario incremented. Based on the
color code from a 5 5 matrix the risk is low if the score is 1e3
(green), medium-low if it is 4e6 (yellow), medium-high if it is 8e12
(orange), and high if the score is between 15 and 25 (Fig. 2b). Then,
scenarios 1 and 3 are medium-high risk and scenario 2 is considered high risk.
The data collected with the survey indicate that the public is not
getting enough objective information about PW coming from the
oil wells in ND. This has caused overestimated and biased risk
perceptions. According to the results, people overestimated the risk
of each scenario by 25%e75%. Poor social perception or lack of
awareness about risk involved poses more risk on people that do
not take preventive measures.
3.5. Sensitivity analysis
In this study, the main input to simulate Pb-210 concentration
was the Ra-226 initial concentration. If the real average level of
radium in PW was underestimated or overestimated, the average
concentration of Pb-210 would be different. To know how much the
output would change if actual Ra-226 level varied between 25% and
50%, a sensitivity analysis of four scenarios (Table 3) was performed.
Table 3 shows that the mean Pb-210 concentration varied
signicantly compared to the mean base (540 pCi/L) when the Ra226 input changed. To understand the effects of these variations,
Table 3
Four different sensitivity analysis scenarios where the initial concentration varied 25% and 50% were evaluated. The nal Pb-210 remaining in treated water is shown (in Bq/
L) for each sensitivity analysis scenario.
Scenario
Ra-226
Ra-226
Ra-226
Ra-226
25%
25%
50%
50%
underestimation
overestimation
underestimation
overestimation
674.54
404.81
809.52
269.85
173.41
104.35
208.70
69.36
0.77
0.46
0.93
0.31
634
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