Heliyon 6 (2020) e04668

Contents lists available at ScienceDirect

Heliyon
journal homepage: [Link]/heliyon

Research article

Risk assessment of drinkable water sources using gross alpha and beta
radioactivity levels and heavy metals
Oluwole J. Okunola a, *, Mark O.A. Oladipo b, Theophilus Aker a, Olayinka B. Popoola c
a
Department of Applied Chemistry, Federal University, Dutsin-Ma, Nigeria
b
Centre for Energy Research and Training, Ahmadu Bello University, Zaria, Nigeria
c
Department of Oncology, Federal Medical Centre, Gusau, Zamfara State, Nigeria

A R T I C L E I N F O A B S T R A C T

Keywords: The increase in economic activities as a result of population surge in Dutsin-Ma has culminated into increase in
Gross alpha waste and environmental quality degradation. Hence, this study examined the risk associated with different
Gross beta drinking water sources (dam water (DM), borehole water (BW), Hand dug well water (WW) and tap water (TW))
Heavy metals
in Dutsin-Ma, Katsina using concentrations of gross alpha (α) and gross beta (β) activity, and heavy metals
Risk
Environmental analysis
cadmium (Cd) and lead (Pb) in the water. A total of Thirty six (36) samples were collected from the study area.
Environmental assessment Standard methods were deployed for the determination of pH, concentration of gross alpha and gross beta activity
Environmental chemistry and concentrations of Cd and Pb in the water samples were done using chemical fraction method. The results of
Environmental hazard the pH showed values not within the recommended limits for drinking water quality with exception of 8.30
Environmental risk assessment (WW). Also, the measured activity concentrations of gross alpha in all water samples are below 0.1 Bq/L with few
Environmental science exceptions, while the measured activity concentrations of gross beta in 50% of the total water samples collected
Chemistry are higher than 1.0 Bq/L permissible limit. The mean annual dose equivalent all the water sources is higher than
0.1 mSv recommended dose for radionuclides in water, hence the life cancer risk assessment showed higher
values, indicating the water are unsafe for drinking. The results in this study showed that Cd and Pb in all the
water fractions (mobile, dissolved, total and particulate) are above the WHO recommended limit of 0.003 and
0.01 mg/L in drinking water. Similarly, the hazard index (HI) for the water samples are greater than one (1),
hence, a possible concern for potential carcinogenic effect for consumer of the water sources.

1. Introduction important factor in increasing the natural radiation exposure in humans

(UNSCEAR, 2000). These dependent upon the amount of radionuclides
The importance of water to human is numerous such that its avail- present in source rock, soils and other natural and artificial radionuclide
ability in quantity and quality becomes crucial to human survival. Water materials that the water comes in contact (Darko et al., 2014). Therefore,
is one of the essentials that support all forms of plant and animal life there is the need to determine the concentration of alpha and beta ra-
(Vanloon and Duffy, 2005) and it is obtained from two principal natural diations in water. The gross alpha and beta counting is the preliminary
sources; surface water such as fresh water lakes, rivers, streams and test, as stipulated in the World Health Organization guideline for water
ground water such as borehole water and well water (Mendie, 2005). quality determination (WHO, 2004). Also, due to its relatively stability,
However, the availability of quality water is of interest to the scien- low costs and simplicity, it has become a veritable tool for determination
tist, government and relevant stakeholders. Some of contaminant that of relative radioactivity levels in water (Jobb
agy et al., 2011; Sahin et al.,
affects the quality of water includes heavy metals, radionuclides and 2017).
gaseous emission etc. The natural radionuclides and their decay products In addition, heavy metals become toxic when their concentrations are
are usually present in all types drinking water sources (Rajamannan above the threshold recommended thereby damaging the life functions of
et al., 2013). an organism (Albergoni and Piccinni, 1983). Metals in natural waters can
Availability of Alpha and beta radiations known as high Linear Energy exist in truly dissolved colloidal and suspended forms. The proportion of
Transfer (LET) radiations in drinking water is considered to be an these forms varies with metals and for different water bodies.

* Corresponding author.
E-mail addresses: ookunola@[Link], okunolaoj@[Link] (O.J. Okunola).

[Link]
Received 3 June 2020; Received in revised form 23 June 2020; Accepted 5 August 2020
2405-8440/© 2020 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license ([Link]
nc-nd/4.0/).
O.J. Okunola et al. Heliyon 6 (2020) e04668

Figure 1. Map of the study area showing the sampling points.

Consequently, the toxicity and sedimentation potential of metals change day between 6:30 and 11:57 am. For the samples collection; Dutsin-ma
depending on their forms (Marcovachia et al., 2007). Non-essential town was stratified into four zones. Zone A is the Dutsinma Dam, Zone
metals often exert their action through their chemical similarity to B is the Hayin Gada, Zone C is the Dutsin-Ma Market/Kandangaru; and
essential elements for example, cadmium with copper or zinc (Marco- Zone D is the Tsamiya/Yarima as shown in Figure 1. Four (4) grab
vachia et al., 2007). samples were collected from each zone per source of water, then pooled
Dustin-Ma water resources of recent have been threatened by the together to give composite sample for a source. Samples were analyzed in
population growth due to the location of the Federal University coupled duplicates.
with other economic activities that follows. This has culminated into Random sampling technique was employed for selecting hand-dug-
generation of large waste worsen by poor disposal system which has wells, bore holes and tap water, except for Zone A, where three water
increased the level of heavy metals in water source to the water works samples of the dam water only were collected at different points. On the
(Okunola and Mainasara, 2016). whole, a total of Thirty six (36) samples were collected. Three (3) sam-
Survey of literature showed that there is no published information on ples were collected from each sample location as follows; three sampling
data related to radioactivity and heavy metal forms in different drinking
water sources in Dutsin-Ma especially since the coming o Federal Uni-
versity Dutsin-Ma. Hence, the present study was conceived to give a
baseline data information on these. Therefore, the present study aimed to Table 1. pH of different water sources. Gross alpha and beta concentrations in
determine natural radioactive using activities of gross alpha and gross water samples.
beta and heavy metals (Cd and Pb) concentrations in available drinking Sample pH
water sources in Dutsin-Ma. The data were used to calculate the carci- DW1 4.66
nogenic health risks that could emerge from the natural radioactivity and DW2 4.87
heavy metals accumulation in Dutsin-Ma drinking water. DW3 4.70
Mean ± SD 4.74 ± 0.11
2. Materials and methods WW1 8.30
WW2 7.58
2.1. Study area and sampling location WW3 7.30
Mean ± SD 7.73 ± 0.52
Dutsin-Ma town is the headquarters of Dutsinma Local Government BW1 5.57
Area in Katsina State, Nigeria. The Local Government has an area of BW2 5.80
about 527 Km2. The coordinates of Dutsin-Ma town lie between 12
270 BW3 5.80
18” N and 7
29’ 2900 E. Dutsinma LGA share its borders with Kurfi to the Mean ± SD 5.72 ± 0.13
north, Charanchi to the northeast, Kankia to the east, Matazu to the
TW1 6.51
southeast, Danmusa to southwest and Safana to the west.
TW2 7.02
Water samples were collected from four different sources of water in
TW3 6.70
Dutsin-ma, this includes; raw water from the dam (DW), Pipe-borne
Mean ± SD 6.74 ± 0.26
(TW), borehole (BW) and hand dug well water (WW). The samples
WHO (2011) 8.2–8.5
were collected in the month of June, 2016 during the early hour of the

2
O.J. Okunola et al. Heliyon 6 (2020) e04668

0.18
Table 2. Gross Alpha and Beta Activity in different water samples.
0.16
Sample Mean activity of Mean activity
gross alpha (Bq/L) of gross beta (Bq/L) 0.14

DW1 0.001  0.003 0.185  0.142 0.12

DW2 0.016  0.007 0.991  0.323
0.1
DW3 0.038  0.027 2.685  1.07
mSv/year
Mean 0.018 ± 0.012 1.287 ± 0.512 0.08
WW1 0.012  0.031 1.511  1.47
0.06
WW2 0.010  0.007 0.036  0.269
WW3 0.005  0.003 0.035  0.001 0.04

Mean 0.009 ± 0.014 0.527 ± 0.580

0.02
BW1 0.034  0.000 3.126  1.170
BW2 0.146  0.034 4.917  0.900 0
DW WW BW BW
BW3 0.043  0.030 4.157  1.230 Water source
Mean 0.074 ± 0.021 4.067 ± 1.100
TW1 0.003  0.006 0.112  0.293 Figure 3. Mean effective dose equivalent for gross beta in different water
TW2 0.002  0.008 0.008  0.003
sources. Relationship between beta and alpha activity concentrations.

TW3 0.037  0.03 2.014  1.27

Mean 0.014 ± 0.015 0.711 ± 0.522 State. Each of the 2 L water sample was evaporated using a hot plate.
*Standard Reference 0.1 1
When the sample in question were almost dried, it was transferred to the
*
crucible which was placed under an infrared radiator until constant
WHO (2011). weight was achieved. All the sample preparation and analysis proced-
ures, and equipment calibration were done according to Nwoke (2006)
location each for the different sources of water (hand-dug-wells, bore and Onoja et al. (2007).
holes, tap water and dam water). Each of the grab samples at each The gross α and β activities of the water samples were estimated ac-
location for a type of water source was pooled together to give a com- cording to Saleh and Shayeb (2014) as shown in Eq. (1)
posite sample. Hence a total of twelve (12) composite samples were
N
obtained Two (2) liters of High Density Polyethylene (HDPE) bottles Aα;β ¼ Effα;β
(1)
were used in the sample collection and in each, 1% (v/v) of 68.5–69% 60  100
 Vs
purity of concentrated nitric acid AnalaR was measured into the N is the separately net gross alpha or beta count rate (cpm),
container and made to volume with the sampled water and covered Effα,β is separately gross alpha or beta counting efficiency (in percent)
tightly using clean cellophane and the bottle cover as soon as possible to Vs is the volume of sample aliquot (in L) and 60 is the conversion
avoid absorption of radionuclides on the walls of the containers. The factor.
water samples were kept in the laboratory until analysis was carried out.
0.014
2.2. Determination of pH 0.012

0.01 R² = 0.991
The pH of samples was taken in-situ using the HANNA instrument HI
8014. The sensor was held in the sample until the pH value was stabilized 0.008
Beta Acvity (Bq/L)
within a one decimal range. Between the readings, the sensor was 0.006
cleaned or rinsed in distilled water. The pH meter was calibrated before
0.004
use using buffer solution of pH 4 and 9.
0.002

2.3. Sample preparation for gross alpha and gross beta determination 0
0 0.0005 0.001 0.0015 0.002 0.0025 0.003
Alpha Acvity (Bq/L)
Sample preparation and analysis was done at the Center for Energy
Research and Training (CERT) Ahmadu Bello University, Zaria, Kaduna Figure 4. Correlation between gross beta and gross alpha in dam water.

0.035

0.03

0.025

0.02
mSv/year
0.015

0.01

0.005

0
DW WW BW BW
Water Source

Figure 2. Mean effective dose equivalent for gross alpha for different water sources.

3
O.J. Okunola et al. Heliyon 6 (2020) e04668

0.18

0.16
R² = 0.519
0.14

0.12

0.1
Beta Acvity
(Bq/L) 0.08

0.06

0.04

0.02

0
0 0.005 0.01 0.015 0.02 0.025 0.03 0.035
Aplha Acvity (Bq/L)

Figure 5. Correlation between gross beta and gross alpha in hand dug well water.

0.008
R² = 0.737
0.007

0.006

0.005

Beta Acvity (Bq/L) 0.004

0.003

0.002

0.001

0
0 0.5 1 1.5 2 2.5
Ahpha Acvity (Bq/L)

Figure 6. Correlation between gross beta and gross alpha in bore-hole water.

2.4. Chemical fractionation of samples

Chemical fractionation of water samples was carried out on the

principle proposed by B€ackstrӧm et al. (2003). Samples were subjected to
2.5 extraction separately using 3.2 ml of 65 %v/v concentrated HNO3 to give
2% HNO3 acidification in 100 ml of sample. The extraction was aimed at
differentiating fractions in three stages as follows: Dissolved fraction,
2 Mobile fraction and Total Fraction. The particulate concentration was
calculated as the difference between Fraction III and Fraction I.
R² = 0.999
1.5
Beta Acvity 2.5. Effective dose equivalent and lifetime risk assessment
(Bq/L)
1
The effective dose equivalent (DRw), total effective equivalent dose
(TEED) and lifetime risk index using concentrations of gross alpha and
0.5 beta activity were calculated using ICRP (1991), UNSCEAR (2000) and
Karahan et al. (2018).
0 DRwðα=βÞ ¼ Awðα=βÞ  DCFðα=βÞ  730 (2)
0 0.01 0.02 0.03 0.04
Alpha Acvity (Bq/L)
where DRW(α//β) is the dose equivalent effective (Sv/year), AW(α//β) is
Figure 7. Correlation between gross beta and gross alpha in tap water. activity (Bq/L), A daily water intake of 2 L/Day according to WHO
(2011) results in annual consumption rate of 730 L/year. DCF(α//β) is the

4
O.J. Okunola et al. Heliyon 6 (2020) e04668

Figure 8. Relationship between gross alpha and gross beta and pH in Dam water.

dose conversion factor for ingestion of the individual natural rafionu- ADI
HQ ¼ (6)
clides for adult, α ¼ 2.80  104 mSvBq1 and β ¼ 6.90  104 mSvBq1 RfD
(WHO, 2004).
where RfD is the chronic reference dose values of heavy metals, Cd ¼ 5.0
Total Equivalent Effective Dose ðmSvÞ ðTEEDðαþβÞ Þ ¼ DRwα þ DRwβ  104 mg/kg per day; Pb ¼ 3.5  103 mg/kg per day
(3)
X
n
ELCR ¼ ADIK  SFk (7)
Lifetime RiskðLRα Þ ¼ DRwðα=βÞ  DL  RF (4) k¼i

where DL is duration of life (70 years) and RF is risk factor recommended where K is the heavy metals (Cd and Pb), SFk are the average daily intake
as 7.3  102Sv1 (ICRP, 1991). and the cancer factor, respectively for the k, n is the number of heavy
metals. The SF for Cd ¼ 15 and Pb ¼ 8.5  101 mg/kg per day.
2.6. Risk assessment study for heavy metals
3. Results and discussion
Average daily intake of metals (ADI), Hazard quotients (HQ), excess
lifetime cancer risk (ELCR) and Hazard Index were calculated accord- 3.1. pH of water samples
ingly using Karahan et al. (2018).
The pH of water sample from different sources of water in Dutsin-Ma
C  IR  EF  ED is presented in Table 1. The pH ranged from 4.66 to 4.87 with a mean
ADI ¼ (5)
BW  AT value of 4.74  0.11 for raw water from the dam (DW), and from 7.30 to
8.30 with an mean value of 7.73  0.52 for hand-dug well water (WW),
where C is the concentration of heavy metal in water (), IR is the daily and from 5.57 to 5.80 with a mean value of 5.72  0.13 for borehole
intake of water, 2 L/day (WHO, 2011). ED is the exposure duration, 70 water (BW), and from 6.51 to 7.02 with an average value of 6.74  0.26
years. EF is the exposure frequency 365 days/year. BW is the body weight for tap water (TW). The lowest pH value 4.66 was obtained in water from
of the exposed individual (adult), 70 kg. AT is the time period over which the dam and maximum pH value 8.30 was obtained in well water.
the dose is averaged, 365  70 days for carcinogens and non-carcinogens.

5
O.J. Okunola et al. Heliyon 6 (2020) e04668

Figure 9. Relationship between gross alpha and gross beta and pH in hand-dug well water.

The WHO guideline for drinking water quality prescribed pH range of 3.2. Gross alpha and beta concentrations in water samples
8.2–8.8 (WHO, 2011), however, the values obtained in this study with
exception of 8.30 (WW1) are all below the recommended limits for The activity concentrations of gross alpha and gross beta in water
drinking water quality. pH can be influenced by various chemicals, and samples collected from different sources in Dutsin-Ma town are given in
biological processes, geographical and environmental processes. It may Table 2. As shown in Table 2 the activity concentration of gross alpha in
be concluded that drinking water from dam, boreholes, and tap-water in dam water (DM) ranged from 0.001  0.003 Bq/L to 0.038  0.027 Bq/L
Dutsin-Ma metropolis are contaminated and not suitable for drinking and with an average value of 0.018  0.012 Bq/L, hand-dug well water (WW)
other domestic uses. The analysis of variation (ANOVA) test shows sig- varied from 0.005  0.003 to 0.012  0.031 Bq/L with an average value
nificant different in pH values at various point. The mean pH values along of 0.009  0.014 Bq/L. The minimum and maximum gross alpha activity
the point are similar to typical values as (4.5–8.5) reported by concentration for borehole water (BW) was 0.034  0.000 Bq/L and
(Mccutchen et al., 1992), but otherwise lower than 7.3–8.1 recorded for 0.146  0.034 Bq/L, respectively, and the mean value was 0.074  0.021
tap by Korkmaz et al. (2016). Bq/L. Also, the range of 0.002  0.008 Bq/L, to 0.037  0.03 Bq/L, was

6
O.J. Okunola et al. Heliyon 6 (2020) e04668

Figure 10. Relationship between gross alpha and gross beta and pH in borehole water.

recorded for tap water (TW) with an average value of 0.014  0.015 Bq/ lower than 0.1 Bq/L, except for BW2 which is slightly above the
L. permissible limit.
The highest gross alpha activity in the water was measured in BW2 as The gross beta activity concentration ranged from 0.185  0.142 Bq/
shown in Figure 2. This could be due to the geological setting of the L to 2.685  1.07 Bq/L with an average value of 1.287  0.512 Bq/L for
underground water source. The lowest gross alpha activity in water samples DW. For the activity concentration of sample WW, lowest and
samples was found in DW1, a surface water supply. The gross alpha ac- highest values of 0.035  0.001 Bq/L and 1.511  1.47 Bq/L was
tivity in water samples is primarily comprised uranium decay products recorded respectively with an average value of 0.527  0.580 Bq/L. The
such as 226Ra (Malanca et al., 1998), and national and world recom- gross beta activity concentrations of BH and TP water samples ranged:
mends the gross alpha activity concentration to be 0.1 Bq/L (SON, 2007; 3.126  1.170 Bq/L - 4.917  0.900 Bq/L and 0.008  0.003–2.014 
WHO, 2011). Hence, the results obtained in this study showed that the 1.27 Bq/L with average values of 4.067  1.100 Bq/L and 0.711  0.522
measured activity concentrations of gross alpha in all water samples are Bq/L, respectively. The highest gross beta activity in the water samples

7
O.J. Okunola et al. Heliyon 6 (2020) e04668

Figure 11. Relationship between gross alpha and gross beta and pH in tap water.

was found in sample BW2 as shown in Figure 3. This could be due to high 3.3. Relationship between beta and alpha activity concentrations
level of agricultural activities around the area releasing phosphate into
water. While the lowest gross beta activity in water samples was found in The correlation between activity concentration of gross beta and alpha in
TW2. The variation in water sample between water sources or among the dam water, hand-dug well water, borehole water and tap water are presented
same water source could be origin of water resources and environmental in Figures 4, 5, 6, and 7, respectively. The analysis was done to ascertain
factor. availability of the same radionuclides for the beta and alpha activities of i,n the
The gross beta activity in water sample is primarily contributed from water of the same source (Agbalagba et al., 2013). The figures showed the
228
Ra and 210Pb (WHO, 2004). and national and world recommends the linear correlation of alpha and beta concentration in the water sources. The
gross alpha activity concentration to be 1.0 Bq/L (SON, 2007; WHO, results showed significant R2 values: 0.991, 0.519, 0.737 and 0.999 for dam
2011). Hence, the results obtained in this study showed that The results water, hand-dug well water, borehole water and tap water, respectively. This
obtained show that the measured activity concentrations of gross beta in indicates that same radionuclides are responsible for the activities of beta and
six water samples; DW3, WW1, BW1, BW2, BW3, and TW3 representing alpha particles in the water samples. Also, this validates the prediction of gross
50% of the total water samples collected are higher than 1.0 Bq/L alpha activity concentration in the samples. Similar reports are made by
permissible limit. Agbalagba et al. (2013) and Alomari et al. (2019).

8
O.J. Okunola et al. Heliyon 6 (2020) e04668

Table 3. Comparison of the gross alpha and beta activity concentration in this study and other studies.

Concentration of gross alpha (Bq/L) Concentration of gross beta (Bq/L) Type of water References
0.001–0.038 0.991–2.685 Dam water This study
0.005–0.012 0.035–1.511 Well water This study
0.034–0.146 3.126–4.917 Borehole water This study
0.002–0.037 0.008–2.014 Tap water This study
31.46 50.14 bottled drinking water Ismail et al. (2009)
1299 582 Groundwater Fasae (2013)
174 222.5 portable drinking water Fasae (2015)
45.9 91.2 Natural spring Kobya et al. (2015)
1.57 1.62 Ground water Alomari et al. (2019)
0.18 0.21 Drinking water Forte et al. (2007)
0.0002–0.015 0.0252–0.2644 Tap water Damla et al. (2006)
0.006–0.125 0.001–0.667 Tap ans river water Korkmaz et al. (2016)
0.012 0.234 Tap water Saleh et al. (2015)
0.11–16 0.10–16.90 Thermal spring water Sahin et al. (2017)
0.0157–0.1427 0.0893–0.400 Borehole and well water Darko et al. (2014)

Table 4. The Annual effective dose equivalent lifetime cancer risk and total equivalent effective dose for different water sources.

Sample Annual Effective Dose Equivalent (mSv) Lifetime Cancer Risk (mSv/year) Total Equivalent Effective Dose (mSv)

DRα DRβ LRα TEEDαþβ

DW1 0.0002 0.0932 0.0010 0.0934
DW2 0.0033 0.4992 0.0167 0.5024
DW3 0.0078 1.3524 0.0397 1.3602
Average 0.0037 0.6483 0.0191 0.6520
WW1 0.0025 0.7611 0.0125 0.7635
WW2 0.0020 0.0181 0.0104 0.0202
WW3 0.0010 0.0176 0.0052 0.0187
Average 0.0018 0.2656 0.0094 0.2675
BW1 0.0069 1.5746 0.0355 1.5815
BW2 0.0298 2.4767 0.1525 2.5065
BW3 0.0088 2.0939 0.0449 2.1027
Average 0.0152 2.0484 0.0776 2.0636
TW1 0.0006 0.0564 0.0031 0.0570
TW2 0.0004 0.0040 0.0021 0.0044
TW3 0.0076 1.0145 0.0386 1.0220
Average 0.0029 0.3583 0.0146 0.3612

Figure 12. Comparison of average total equivalent effective dose for difference water sources.

9
O.J. Okunola et al. Heliyon 6 (2020) e04668

Figure 13. Comparison of average lifetime cancer risk in difference water sources r.

Figure 14. Concentration of Cd in different fraction of water sources.

Figure 15. Concentration of Pb in different fraction of water sources.

3.4. Relationship between gross alpha and beta activity concentrations and
pH

The correlation between pH and activity concentrations of gross beta

and alpha in dam water, hand-dug well water, borehole water and tap
Table 5. Correlation of Cd among fractions in water.
water are presented in Figures 8, 9, 10, and 11, respectively. From the
Parameter CdDissolved CdMobile CdTotal CdParticulate figures, R2 values of 0.737 and 1.000 (DW), 0.777 and 0.926 (WW),
CdDissolved 1.000 0.994 and 0.671 (BW) and 0.880 and 0.894 (TW) for pH vs activity
CdMobile 0.857** 1.000 concentrations of gross alpha and pH vs activity concentrations of gross
CdTotal 0.822* 0.958** 1.000 beta in the samples. High positive R2 between the parameters indicates
CdParticulate 0.456 0.773* 0.880** 1.000 that pH is responsible for the activity concentrations of gross alpha and
** beta in the samples. This report showed similar trends of significant
Correlation is significant at the 0.01 level (2-tailed).
* relationship between the pH and gross alpha and gross beta activity at pH
Correlation is significant at the 0.05 level (2-tailed).

10
O.J. Okunola et al. Heliyon 6 (2020) e04668

reported for drinkable water in Nigeria (Ogundare and Adekoya, 2015).

Table 6. Correlation among Pb fractions in water. The mean value obtained for all the water sources is higher than 0.1 mSv
Parameter PbDissolved PbMobile PbTotal PbParticulate recommended dose for radionuclides in water. The implication of this is
PbDissolved 1.000 possible health risks to consumers of this water sources in Dutsin-Ma.
PbMobile 0.400 1.000
The lifetime cancer risk assessment in the water samples as shown in
PbTotal 0.937** 0.574 1.000
Table 4 revealed the range of 0.0010–0.0397 with a mean value of
0.0191, 0.0052 to 0.0125 with a mean value of 0.0094, 0.0355 to 0.1525
PbParticulate 0.022 0.579 0.369 1.000
with a mean value of 0.0736 and 0.0021 to 0.0386 with a mean value of
**
Correlation is significant at the 0.01 level (2-tailed). 0.0146 for dam water, well water, borehole water and tap water,
respectively. The highest average value was obtained in borehole water
and the least in well water as shown in Figure 13. Comparison of the
< 8.3 (Alomari et al., 2019). This shows that pH of the samples are results with other study shows that values obtained in this study is higher
responsible for the activity concentration of the gross alpha and beta. than mean of 10.12  105 reported for drinking water in Turkey (Kobya
Comparison of the results obtained in this study with literatures is et al., 2015). Generally, the results show that there is risk for consump-
presented in Table 3. The table below shows that the activity concen- tion of the waters, hence, the waters are unsafe for drinking.
tration of gross alpha and beta are lower than reported studies in Nigeria
(Fasae, 2013, 2015). The tap water results for concentration of gross 3.5. Concentration of Cd in the water fractions
alpha and beta in this study is higher than similar studies reported in
literature (Damla et al., 2006; Darko et al., 2014; Saleh et al., 2015 The results of chemical fractionation of different water samples for Cd
Korkmaz et al., 2016). For the ground water: borehole and well water, is presented in Figure 14. The concentrations of Cd ranged from 0.650 –
the activity concentration of gross alpha and beta are higher and lower 1.53 mg/L, 0.683–1.900 mg/L, 0.717–2.533 mg/L and 0.066–1.117 mg/
than reports of Kobya et al. (2015) and Alomari et al. (2019), repectively L for dissolved, mobile, total and particulate fractions. The highest con-
as shown in Table 3. The higher or lower activity concentrations of gross centration of the fractions for all samples was obtained in dam water
alpha and beta in this study compare to other studies is due to the (DW) sample with exception of particulate fraction which presented
geological properties of the underground source of water and the activ- highest concentration for well water. Analysis of variation (ANOVA)
ities carried out around the water source. among the samples fractions showed the statistical differences of Dis-
The radiological risk indexes of different drinking water sources are solved ¼ 0.079, Mobile ¼ 0.025, Total ¼ 0.005, and Particulate ¼ 0.074
presented in Table 4. The indexes Includes annual effective dose equiv- of different fractions. The results in this study showed that Cd is above
alent lifetime cancer risk and total equivalent effective dose. The annual the recommended limit of 0.003 mg/L (WHO, 2011). Analyses of rela-
effective equivalent dose for alpha (DRα) ranged from 0.0002 to 0.0298 tionship among the fractions for Cd are shown in Table 5. Significant
mSv with the highest and lowest values obtained for borehole water and correlations (p < 0.05) observed among the fractions indicates that the
dam water, respectively. Also, the annual effective equivalent dose due to sources Cd in these fractions are same.
beta activity (DRβ) ranged from 0.0040 to 2.4767 mSv with the lowest
recorded in tap water and the highest in borehole water. The total 3.6. Concentration of Pb in the water fractions
equivalent effective dose in the water sources showed mean value of
0.6520, 0.2675, 2.0636 and 0.3612 mSv for dam water, well water, The mean concentration of Pb in different fractions of the water using
borehole water and tap water, respectively with the lowest mean value chemical fractionation methods are presented in Figure 15. Analysis of
recorded in the well water and highest mean value recorded in broehole variation (ANOVA) among the fractions showed statistical differences;
water as shown in Figure 12. The value obtained in this study is lower Dissolved is 0.582, Mobile is 0.912, Total is 0.504, and Particulate is
than values recorded by Agbalagba et al. (2013) and higher than 0.0678 0.904. The concentrations of Pb varied from 0.292 mg/L (BW) – 0.798

Table 7. Health Risk due to concentration of Cd in different water sources. Table 8. Health Risk due to concentration of Pb in different water sources.

Sample Fractions ADI HQ ELCR Sample Fractions ADI HQ ELCR

BW Dissolved 0.026 5.237 0.393 BW Dissolved 0.008 2.384 0.007
Mobile 0.037 7.331 0.550 Mobile 0.010 2.947 0.009
Total 0.040 7.903 0.593 Total 0.012 3.339 0.010
Particulate 0.013 2.666 0.200 Particulate 0.003 0.955 0.003
Mean 0.029 5.784 0.434 Mean 0.008 2.406 0.007
DW Dissolved 0.045 9.046 0.678 DW Dissolved 0.023 6.510 0.019
Mobile 0.054 10.854 0.814 Mobile 0.013 3.816 0.011
Total 0.072 14.474 1.086 Total 0.028 8.114 0.024
Particulate 0.027 5.429 0.407 Particulate 0.006 1.604 0.005
Mean 0.050 9.951 0.746 Mean 0.018 5.011 0.015
TW Dissolved 0.019 3.714 0.279 TW Dissolved 0.017 4.902 0.015
Mobile 0.020 3.903 0.293 Mobile 0.018 5.073 0.015
Total 0.020 4.094 0.307 Total 0.020 5.657 0.017
Particulate 0.002 0.380 0.029 Particulate 0.003 0.755 0.002
Mean 0.015 3.023 0.227 Mean 0.014 4.097 0.012
WW Dissolved 0.030 6.000 0.450 WW Dissolved 0.013 3.731 0.011
Mobile 0.045 9.046 0.678 Mobile 0.015 4.339 0.013
Total 0.062 12.380 0.929 Total 0.016 4.600 0.014
Particulate 0.032 6.380 0.479 Particulate 0.003 0.869 0.003
Mean 0.042 8.451 0.634 Mean 0.012 3.385 0.010

11
O.J. Okunola et al. Heliyon 6 (2020) e04668

Figure 16. Hazard Index of fractions of different water sources in Dutsin-Ma.

Figure 17. Average hazard Index of different water sources in Dutsin-Ma.

mg/L (DW) for dissolved fraction, 0.361 mg/L (BW) – 0.622 mg/L (TW) obtained in this study for ADI, HQ and ECLR is higher than values re-
for mobile fraction, 0.409 mg/L (BW) – 0.994 mg/L (BW) for total ported for the same indexes by Karahan et al. (2018) for drinking water.
fraction and 0.093 mg/L (TW) – 0.192 mg/L (DW) for particulate frac- Also, the results of ADI of Pb showed that particulate fraction and
tion. The highest concentration of 0.994 mg/L was recorded for sample total fractions has the lowest and highest values, respectively in the
DW of total fraction. Similarly, the values obtained in different water drinking water sources. The highest value of 0.028 was recorded for dam
fractions for Pb is above recommended limit of 0.01 mg/L for drinking water (DM) with mean value of 0.018 for the fractions. The mean HQ
water (WHO, 2011). According to Watershed Protection Plan Develop- decreases in the following order DW > TW > WW > BW. The highest and
ment Guidebook, (2005) Lead sources are batteries, gasoline, paints, lowest values of 8.114 and 0.755 were recorded for total and particulate
caulking, rubber, and plastics. Lead can cause a variety of neurological fractions, respectively. The excess lifetime cancer due to Pb calculated
disorders. In children, it inhibits brain cell development. The analyses of showed that sample DW has the highest risk index compare to other
relationship among the fractions for Pb are shown in Table 6. Significant water samples. Similarly, the values obtained in this study for ADI, HQ
correlations (p < 0.05) observed among the fractions indicates that the and ECLR is higher than values reported for the same indexes by Karahan
sources of these fractions are same. et al. (2018) for drinking water.

3.7. Health risk assessment of Cd and Pb in the fraction of the water 3.8. Comparison of hazard index (HI) among the drinking water sources
samples
The hazard index due to the Cd and Pb loads in fractions of the
The calculated ADI, HQ and ELCR of Cd and Pb in different water drinking water sources are presented in Figures 16 and 17. The results
fraction are shown in Tables 7 and 8. The results of ADI showed that showed value higher than one for all the fractions in the water sources.
particulate fraction and total fractions has the lowest and highest values Hence, since the HI value exceeds one, there may be concern for potential
of Cd, respectively in the drinking water sources except for well water carcinogenic effects (Karahan et al., 2018) on consumers of this water in
(WW) that showed the lest concentration in the dissolved fraction. The Dutsin-Ma.
highest value of 0.072 was recorded for dam water (DM) with mean
value of 0.050 for the fractions. The HQ decreases in the following order 4. Conclusion
DW > WW > BW > TW. The highest and lowest values of 14.474 and
0.380 were recorded for total and particulate fractions, respectively. The This study is the first of its kind in the area of study to determine the
excess lifetime cancer due to Cd calculated showed that sample DW has radioactivity levels in various sources of drinking water using concen-
the highest risk index compare to other water samples. The values trations of gross alpha and gross beta activity and determine the

12
O.J. Okunola et al. Heliyon 6 (2020) e04668

concentrations of Cd and Pb in different fractions of water using chemical Jordan: groundwater quality, annual effective dose and lifetime risk assessment.
J. Water Health 7 (6), 957–970.
fractionation. From the results obtained in the study, it clearly showed
B€ackstrӧm, M., Nilsson, U., Hakanssan, K., Allard, B., Karlsson, S., 2003. Speciation of
that drinking water in Dutsin-Ma is contaminated and pose great health heavy metals in road runoff and roadside total deposition. Water Air Soil Pollutes.
risk to the rising population of students and workers in the town. The 147.
calculated risk indices showed the profile of DW > WW > BW > TW with Damla, N., Cevik, U., Karahan, G., Kobya, A., 2006. Gross α and β activities in tap waters
in Eastern Black Sea region of Turkey. Chemosphere 62 (6), 957–960.
respect to the potential hazard exposure due to drinking of the water. Darko, G., Faanu, A., Akoto, O., Atta-Agyeman, F., Aikins, M.A., Agyemang, B.,
Given the significant level of Pb and Cd in the water consumed by Ibrahim, A., 2014. Assessment of the activity of radionuclides and radiological
members of the community studied, there is no doubt that appreciable impacts of consuming underground water in Kumasi, Ghana. Environ. Earth Sci.
Fasae, K.P., 2013. Gross alpha and beta activity concentrations and committed effective
amounts would have accumulated in the bodies of these individuals. dose due to intake of groundwater in ado-ekiti metropolis; the Capital City of Ekiti
Hence, a public health challenge because of the association of elevated State, Southwestern, Nigeria. J. Nat. Sci. Res. 3, 61–66.
systemic Pb and Cd with significant morbidities. The mean annual Fasae, K.P., 2015. Gross alpha and beta activity concentrations in portable drinking water
in ado- ekiti metropolis and the committed effective dose. Int. J. Adv. Res. Phys. Sci.
effective dose value obtained for all the water sources is higher than 0.1 2, 1–6.
mSv recommended dose for radionuclides in water. The implication of Forte, M., Rusconi, R., Cazzaniga, M.T., Sgorbati, G., 2007. The measurement of
this is possible radiological health risk to consumers of this water sources radioactivity in Italian drinking waters. Microchem. J. 85 (1), 98–102.
ICRP, 1991. 1990 recommendations of the international commission on radiological
in Dutsin-Ma. Finally, data obtained in this study is a baseline informa- protection. ICRP publication 60. Ann. ICRP 21 (1-3).
tion that can used for future evaluation of drinking water in the area. Ismail, A.M., Kullab, M.K., Saq’an, S.A., 2009. Natural radionuclides in bottled drinking
water in Jordan and their committed effective doses. J. Phys. 2, 47–57.
Jobb
agy, V., K
av
asi, N., Somlai, J., Dombov
ari, P., Gy€
ongy€
osi, C., Kov
acs, T., 2011. Gross
Declarations
alpha and beta activity concentrations in spring waters in Balaton Upland, Hungary.
Radiat. Meas. 46, 159–163.
Author contribution statement Karahan, G., Taskin, H., Bingoldag, N., Kapdan, E., Yilmaz, Y.Z., 2018. Environmental
impact assessment of natural radioactivity and heavy metals in drinking water
around Akkuyu nuclear power plant in Mersin province. Turk. J. Chem. 42, 735–747.
Oluwole J. Okunola, Olayinka B. Popoola: Conceived and designed Kobya, Y., Taşkın, H., Yeşilkanat, C.M., Çevik, U., Karahan, G., Çakır, B., 2015.
the experiments; Analyzed and interpreted the data; Wrote the paper. Radioactivity survey and risk assessment study for drinking water in the Artvin
Mark O. A. Oladipo: Conceived and designed the experiments; Per- province, Turkey. Water Air Soil Pollut. 226, 49.
Korkmaz, M.E., Agar, O., Sahin, M., 2016. Gross α and β activity concentrations in various
formed the experiments; Wrote the paper. water from Karaman, Turkey. Environ. Earth Sci. 75, 14.
Theophilus Aker: Conceived and designed the experiments; Analyzed Malanca, A., Repetti, M., Macedo, H.R., 1998. Gross alpha and beta-activities in surface
and interpreted the data; Contributed reagents, materials, analysis tools and ground water of Rio Grando do Norte, Brazil. Appl. Radiat. Isot. 49, 893–898.
Marcovachia, J., Botte, S., Frejie, R., 2007. Heavy metal, major metals, trace elements. In:
or data; Wrote the paper. Nollet, L.M. (Ed.), Handbook of Water Analysis, second ed. London CRC press,
pp. 275–311.
Funding statement Mccutchen, S., C Martin J, L., Barnwell, T., 1992. Water quality. In: Maidment, D.R. (Ed.),
Handbook of Hydrology. M.C. Graw-Hill, Inc. Publisher, USA.
Mendie, U., 2005. The nature of water. In: The Theory and Practice of Cleanwater
This research did not receive any specific grant from funding agencies Production for Domestic and Industrial Use in Lagos. Lacto-Medals Publishers,
in the public, commercial, or not-for-profit sectors. pp. 1–21.
Nwoke, J.E., 2006. Measurement of Gross Alpha and Beta Radioactivity in River Kaduna.
[Link]. Thesis ABU Zaria (Unpublished).
Competing interest statement Ogundare, F.O., Adekoya, O.I., 2015. Gross alpha and beta radioactivity in surface soil
and drinkable water around a steel processing facility. J. Radiat. Res. App. Sci. 8,
The authors declare no conflict of interest. 411–417.
Okunola, O.J., Mainasara, A.Y., 2016. Quality Assessment of the treatment process of
Dutsin-ma water works. FUDMA J. Sci. Edu. Res. (FJSER), Special Ed. 2 (1), 16–24. A
Additional information Publication of Faculty of Science and Education. Federal University Dutsin-ma.
Onoja, R.A., Akpa, T.C., Mallam, S.P., Ibeanu, I.G.E., 2007. Survey of gross alpha and beta
activity in well water from Zaria and its environs. Niger. J. Phys. 19 (1), 39–47.
No additional information is available for this paper. Rajamannan, A., Viruthagiri, G., Jawahar, K.S., 2013. Natural radionuclides in ceramic
buildings materials available in Cuddalore district, Tamil Nadu, India. Radiat.
Acknowledgements Protect. Dosim. 156 (4), 531–534.
Sahin, M., Korkmaz, M.E., Agar, O., Dirican, A., 2017. A study of gross alpha and beta
measurements for thermal springs in Central Anatolia, Turkey. Environ. Earth Sci. 76,
The authors wish to acknowledge the assistance and support provide 121.
by Professor Adeyemo and Mr. I. A. Bappah of the Center for Energy Saleh, M.A., Ramli, A.T., bin Hamzah, K., Alajerami, Y., Abu Mhareb, M.H., Aliyu, A.S.,
Hanifah, N.Z.H.B.A., 2015. Natural environmental radioactivity and the
Research and Training (CERT), Zaria-Nigeria in sample analysis and data corresponding health risk in Johor Bahru District, Johor, Malaysia. J. Radioanal.
interpretation. Nucl. Chem. 303, 1753–1761.
Saleh, H., Shayeb, M.A., 2014. Natural radioactivity distribution of southern part of
Jordan (Maan) soil. Ann. Nucl. Energy 65, 184–189.
References
SON, 2007. Nigeria Standard for Drinking Water Quality, 554. Nigeeria Industrial
Standard, NIS.
Agbalagba, E.O., Avwiri, G.O., Chadumoren, Y.E., 2013. Gross alpha and beta activity UNSCEAR (United Nations Scientific Committee on the Effects of Atomic Radiations),
concentration and estimation of adults and infants dose intake in surface and ground 2000. Sources and Effects of Ionizing Radiation. Report to the General Assembly.
water of ten oil fields environment in western Niger delta of Nigeria. J. Appl. Sci. United Nations, New York.
Environ. Manag. 17 (2), 267–277. Vanloon, G.W., Duffy, S.J., 2005. The Hydrosphere in Environmental Chemistry: A Global
Albergoni, V., Piccinni, E., 1983. Biological response to trace metalsand their biochemical Perspective, second ed. Oxford University press, New york, pp. 197–211.
effects. In: Leppard, G.G. (Ed.), Trace Element Speciation in Surface Water and its WHO, 2004. Guidelines for Drinking Water Quality, third ed., 1. Recommendations.
Ecological Implications. Plenum Press, New York, pp. 159–175. WHO, 2011. Guidelines for Drinking-Water Quality, fourth ed. WHO Library Cataloguing-
Alomari, A.H., Saleh, M.A., Hashim, S., Alsayaheen, A., Abdeldin, I., khalaf, R.B., 2019. in Publication Data NLM classification, Geneva, p. 675. WA.
Measurement of gross alpha and beta activity concentration in groundwater of

13