Journal of Environmental Radioactivity 192 (2018) 143–149

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Journal of Environmental Radioactivity

journal homepage: www.elsevier.com/locate/jenvrad

Monitoring of tritium concentration in Hanoi's precipitation from 2011 to T

2016
Ha Lan Anh∗, Vo Thi Anh, Trinh Van Giap, Nguyen Thi Hong Thinh, Tran Khanh Minh, Vu Hoai
Isotope Hydrology Laboratory, Institute for Nuclear Science and Technology (INST), 179 HoangQuocViet, CauGiay, Hanoi, Vietnam

A R T I C LE I N FO A B S T R A C T

Keywords: Tritium is a radioisotope of hydrogen and a component of the water molecule. It is a marker for reservoirs such
Tritium (3H) as the stratosphere, troposphere, and oceans involved in the hydrological cycle. Tritium monitoring is an es-
Precipitation sential research tool in hydro-climate, dating for water and recharge groundwater. The Isotope Hydrology
Hanoi Laboratory has collected monthly precipitation samples in Hanoi for tritium concentration analysis. This paper
Liquid scintillation analyzer
reports the tritium concentrations in precipitation in the city from 2011 to 2016. The results show that monthly
tritium concentration reached a maximum of 7.07 Tritium Units (TU) in August 2011. The mean annual tritium
concentration stabilized from 2.03 to 3.36 TU. It suggests that tritium in monitoring station precipitation is
predominantly natural. The seasonal variation trend of 3H in precipitation at the Hanoi station is similar to those
monitored at the Hong Kong station. The correlation of tritium and rainfall was also estimated.

1. Introduction
Tritium (3H, T) is the radioactive isotope of hydrogen and an emitter
of soft beta radiation with 18.6 keV energy. The recently re-evaluated
half-life value of tritium equals 4500 ± 8 days corresponding to
12.32 ± 0.02 tropical years (Lucas and Unterweger, 2000). It may be
of either natural and human-made origin.
Tritium is naturally produced due to nuclear reactions in the upper
atmosphere between atmospheric nitrogen and high-energy cosmic
rays. The mean rate of natural tritium production is estimated to be
0.25 atoms cm−3s−1, which corresponds to an annual natural pro-
duction of about 0.20 kg tritium or 7.0 × 1016Bq (Craig and Lal, 1961;
Lebaron-Jacobs et al., 2009). It is estimated that 55% of the natural
production of tritium occurs in the stratosphere (Masarik and Beer,
1999). Tritium is rapidly oxidized into tritiated water (HTO) and
transferred into the troposphere where it is removed by precipitation
(Ehhalt et al., 2000). It comes to the Earth in the form of precipitation
and atmospheric moisture and is then transported in the environment
through the hydrological cycle.
Tritium is also produced anthropogenically by a variety of nuclear
activities. One example was the atmospheric testing of nuclear weapons
between 1945 and 1963 which released approximately 650 kg
(2.3 × 1020 Bq) of tritium. However, most of the tritium introduced
into the environment between 1945 and the late 1960s has disappeared
by radioactive decay and dilution in the world oceans (Cauquoin et al.,
2015).
Nuclear facilities that release tritium into the environment include
pressurized water reactors, irradiated fuel reprocessing and recycling
plants and reactors dedicated to tritium production. Tritium in irra-
diated fuel is mainly retrieved during reprocessing when the fuel is
sheared. It is found in the form of tritiated water in liquid effluent most
of which is released into the sea (Lebaron-Jacobs et al., 2009).
Tritium is a useful environmental tracer. It is a marker for reservoirs
such as the stratosphere, troposphere, and oceans involved in the hy-
drological systems. It is widely applied as a semi-quantitative tool for
the identification of modern recharge, dating, infiltration condition and
groundwater balance (Allison and Hughes, 1975; Huang and Pang,
2010; Zhang and Ye, 2011; Yangui et al., 2012). Recently, tritium is
increasingly being applied to calibrate and validate three-dimensional
groundwater flow and solute transport models of aquifer systems at the
regional scale (Povinec et al., 2010; Zuber et al., 2011). Tritium is used
for understanding and quantification of the processes determining the
flow of water through the soil-plant-atmosphere system. It is, therefore,
an essential prerequisite for modeling 3H transfers in terrestrial eco-
systems to help improve management of irrigation or water utilization
in agriculture (Connan et al., 2015).
Tritium dating of groundwater in the Hanoi region was conducted in
the Institute for Nuclear Science and Technology (INST) Isotope
Hydrology Laboratory. It has been used to study the hydraulic inter-
action between Holocene and Pleistocene aquifers in the south of
Hanoi. The tritium data have been used to characterize hydrogeological
features of groundwater. Several studies on arsenic mobilization in

∗
Corresponding author.
E-mail address: halananh@vinatom.gov.vn (H.L. Anh).

https://doi.org/10.1016/j.jenvrad.2018.06.009
Received 20 November 2017; Received in revised form 29 May 2018; Accepted 8 June 2018
Available online 20 June 2018
0265-931X/ © 2018 Elsevier Ltd. All rights reserved.
H.L. Anh et al.
groundwater were conducted in the Hanoi region with the use of tri-
tium tracer. Tritium dating could allow for estimating the As mobili-
zation rate from sediment into groundwater (Nhan et al., 2006; Postma
et al., 2007; Larsen et al., 2008).
The concentration of tritium activity is commonly expressed as
tritium units (TU); one TU corresponds to 0.11919 ± 0.00021 Bq/kg
of water (Gröning and Rozanski, 2003). The concentration of tritium in
precipitation is monitored by the Global Network of Isotopes in Pre-
cipitation (GNIP), and the database is available through the IAEA. In
the course of the GNIP activities, monthly precipitation samples were
collected from over 1000 stations in more than 125 countries in the past
and Hanoi was one of them.
The Hanoi monitoring station has been set up at the Institute for
Nuclear Science and Technology since 2003 and has contributed data
from 2004 to 2007 to the GNIP. Tritium data obtained from the IAEA
database is used to model the global distribution of tritium (Doney
et al., 1992; Zhang and Ye, 2011; Cauquoin et al., 2015) and a detailed
study of tritium in precipitation over Australia was published by Tadros
et al. (2014). Results from previous research have shown that tritium in
precipitation has been decreasing toward natural levels, which are less
than 10 TU (Cartwright and Morgenstern, 2012; Michel, 2015;
Cauquoin et al., 2015; Harms et al., 2016).
This paper presents the concentration of tritium in precipitation in
Hanoi collected from 2011 to 2016 (21004′53.5″N, 105079′86.7″E) to
determine the concentration of tritium in recent times; how this value
compares to natural tritium levels; how tritium concentration changes
seasonally and how the precipitation amount effects the concentration
of tritium. The results provide tritium reference data for future en-
vironmental and hydrological studies in Hanoi.
2. Material and methods
Our study included 70 precipitation samples collected between
January 2011 and December 2016 in Hanoi. The construction of the
precipitation sampling device and the procedure used for rainwater
collection were based on sampling procedures for the IAEA's isotope
hydrology of water resource program. Precipitation was sampled on a
monthly basis and also randomly by event, i.e. as soon as possible after
each rain event. Collected samples were poured into 5-liter plastic
bottles with tight caps to avoid evaporation. Samples were labeled with
codes, dated and kept in a cool, dark place. At the end of the month, all
the water from the 5-liter containers was mixed and shaken before re-
filling it to 500 mL bottles which were then tightly capped for further
treatment and measurement of tritium concentration.
As the concentration of tritium in rainwater was expected to be low,
in the laboratory, tritium was subject to electrolytic enrichment in
order to improve the precision of the beta activity counting. The elec-
trolytic enrichment of tritium in water samples is described in detail
elsewhere, e.g. K. Rozanski (2000), Plastino, et al. (2007). The proce-
dure applied is described below.
Tritium activity of the precipitation samples was enriched using an
electrolytic enrichment system. It has 20 cells of volume 500 mL and an
electrolysis control unit that were supplied by IAEA. The electrolysis
occurred in the electrolyzed medium NaOH, at the maximum current of
10A, for a time of 190 h and a total electric charge of 1426 Ah/sample.
Prior to enrichment, the water samples were distillated until dryness for
the elimination of all minerals present. We checked pH and electrical
conductivity values of each distilled sample with Seven Multi Metter
Toledo, pH around 7.0, EC < 30.0 μS/cm. If these pH and EC target
values were not reached, samples were distilled again. Each enrichment
sequence comprised 15 precipitation samples, 2 samples of dead water,
and 3 samples of spike water that were diluted based on the NIST-
SRM4926E reference with certificate issues date 07 February 2011
(Radioactivity, 2011). The use of standard and dead water is necessary
to correct for the enrichment efficiency and for the background. Dead
water was groundwater taken from a well outside Hanoi city at a depth
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Journal of Environmental Radioactivity 192 (2018) 143–149
of 140 m and its tritium concentration was < 0.2 TU, as checked at the
IAEA Isotope Hydrology Laboratory (Vienna, Austria) and at the
Bhabha Atomic Research Center (BARC, India). The enrichment effi-
ciency of the equipment was better than a factor of 25.
After tritium enrichment, the water samples, usually reduced to
10–13 ml. The samples were transferred into round bottom glass flasks
and mixed with 6 g of anhydrous PbCl2 to neutralize the alkaline ma-
terial, and then to distillation to remove the precipitate. These enriched
and alkaline free water samples were mixed with 10 ml of Ultima Gold
LLT - low level of tritium cocktail (PerkinElmer) and then subject to
counting for the tritium activity in a liquid scintillation analyzer, LSC
(TriCarb 3170 TR/SL-Packard). Counting efficiency of the LSC was
corrected using the external standard channel ratio (ESCR) method and
it was better than 55% for tritium. The counting time for samples was
set to 100 min and repeated 10 times for each sample to ensure that
counting precision would be better than 10% for an activity range
below 10 TU.
Evaluating the measurement data and calculating the tritium con-
centration in the samples were guided by Gröning and Rozanski's
method (Gröning and Rozanski, 2003). The lower limit of detection of
the analysis is AT = 0.46 TU. Measurement uncertainty was up to 20%
with samples AT ≤ 1.0 TU and less than 10% with AT > 1.0 TU. Data
presented for the mean annual tritium concentration has been weighted
by the amount of precipitation and calculated using the method out-
lined by the IAEA (Technical report series No. 331, 1992).
3. Result and discussion
3.1. Statistical distribution and sources of tritium in precipitation
The results for tritium in precipitation at monthly intervals are
given in Table 1. The mean of month tritium concentration in pre-
cipitation samples that were collected in 6 years at Hanoi station was
2.54 ± 1.28 TU. The highest tritium concentration value, 7.07 ± 0.65
TU, was found in Aug 2011 and the lowest value, 0.51 ± 0.11 TU, was
found in June 2011.
The tritium values distribution is represented on a histogram and
can be approximated by a Gaussian distribution and frequency curve
has R2 of 0.94 with P < 0.0002 (Fig. 1). The results of test distribution
using a normal Q-Q plot show that the regression line has an R2 of 0.88
with P = 2.27*10−33 (Fig. 2). In both of figure, frequency distribution
and Q – Q plots show that the tritium concentration data follow a
Gaussian distribution. This result of tritium distribution agrees fully
with Harms's report about precipitation in California published in 2016
(Harms et al., 2016).
The results show that 90% of the values of tritium concentration in
Hanoi's precipitation are less than 5 TU, this value is approximately
equivalent to the natural distribution of tritium activity in precipitation
(less than 10 TU). In tropical regions tritium concentrations are around
and less than 5 TU, mostly due to the cosmogenic tritium production
term and the transport process of radionuclides in the tropic known as
the Hadley cell (Cauquoin et al., 2015; Paul Martin & John L. Mc Bride,
2012; Begemann and Libby, 1957). The average annual values for tri-
tium concentration in precipitation between 2011 and 2016 are pre-
sented in Fig. 3. Precipitation in Hanoi has low tritium concentrations,
most of the values are around 2–3 TU, and some values are very low,
less than 1 TU. This can be explained as a large fraction of the Hanoi
precipitation is from water evaporation of oceanic origin, particularly
the Indian Ocean, with the concentration less than 1 TU (Povinec et al.,
2010). Water vapor over the ocean is depleted in tritium due to the
relatively reduced transfer of HTO compared with non-tritiated water
by evaporation exchange from the ocean. Therefore precipitation at the
sampling sites is affected by coastal proximity where rainwater has
lower tritium concentration owing to a large fraction of the precipita-
tion being diluted by molecular exchange of tritium between the rain
droplets and ocean water evaporation. Some values are larger than 5
H.L. Anh et al. Journal of Environmental Radioactivity 192 (2018) 143–149

Table 1 Table 1 (continued)

Time-series of tritium concentration in rainwater at the Hanoi station
3 3
(21004′53.5″N, 105079′86.7″E, 11m asl) from 2011 to 2016. Date H, TU H Error, TU Precipitation, mm

3 3
Date H, TU H Error, TU Precipitation, mm Average 2.54
Stdev 1.28
11-Jan 4.92 0.45 9.3
11-Feb 3.32 0.32 17.5
11-Mar 4.84 0.47 105.8
TU, which could result from the re-evaporation of continental water
11-Apr 2.81 0.28 42
11-May 2.99 0.28 149 which has higher tritium concentrations than does cloud water.
11-Jun 0.51 0.04 395.5
11-Jul 0.69 0.06 254.4 3.2. Seasonal trends
11-Aug 7.07 0.65 313.2
11-Sep 0.66 0.04 247.6
11-Oct 0.52 0.09 177.6 To gain insights into the temporal variability of tritium content in
11-Nov 6.91 0.51 31.8 rainwater (T), one can represent T as the product of three components
11-Dec 5.12 0.42 51.5 as follows:
12-Jan 2.33 0.23 20.3
12-Feb 2.02 0.19 16.5 T = L . S. I (1)
12-Mar 2.97 0.30 16.9
12-Apr 2.97 0.28 31.8 where L is the inter-annual trend component (in TU), S is the seasonal
12-May 2.5 0.22 387.7 index, and I is the irregular index. These three components can be de-
12-Jun 2.54 0.23 268.9
lineated by using statistical procedures as described in Pindyck and
12-Jul 2.36 0.24 388.3
12-Aug 1.39 0.11 478.1
Rubinfeld (1998).
12-Sep 2.05 0.23 54.7 Tritium concentrations in the atmosphere are known to vary across
12-Oct 1.71 0.13 77.5 latitude and between seasons (Hauglustaine and Ehhalt, 2002; Paul
12-Nov 1.63 0.15 34.8 Martin & John L. Mc Bride, 2012; Tadros et al., 2014). A number of
12-Dec 0.65 0.04 25.7
studies have shown that a clear maximum is observed in early spring
13-Jan 3.14 0.21 47.43
13-Feb 2.27 0.23 11.43 extending into summer. This is explained by the stratosphere - to-tro-
13-Mar 2.03 0.26 15.92 posphere exchange which is the main mechanism that transports tri-
13-Apr 1.63 0.13 76.23 tium enriched water evaporation to the troposphere annually during
13-May 2.97 0.15 320.99 the spring, temporarily elevating the tritium levels, followed by an
13-Jun 1.22 0.19 248.64
13-Jul 2.12 0.27 389.88
autumn minimum (Rozanski et al., 1991; Alley, 1993; Yasunari and
13-Aug 2.05 0.14 690.78 Yamazaki, 2009). In Hanoi, we can see this trend but it is less pro-
13-Sep 2.06 0.27 454.59 nounced and “springtime tritium peak” doesn't clearly occur because
13-Oct 1.79 0.14 10.18 precipitation in Hanoi is deeply affected by moisture from the sea so
13-Nov 1.22 0.12 85.32
that it is quite similar compared to the coastal site. Fig. 4 depicts the
13-Dec 1.91 0.11 23.88
14-Jan 0 seasonal index of tritium in precipitation based on monthly data aver-
14-Feb 1.22 0.24 4.17 aged over the 2011–2016 period. The tritium concentration in spring
14-Mar 2.47 0.28 62.5 extended into early summer January to May and in the winter from
14-Apr 1.75 0.27 138.6 October to December (dry season) is higher than tritium concentration
14-May 4.71 0.31 104.46
14-Jun 2.6 0.2 271.34
in end of summer and autumn from June to September (rainy season).
14-Jul 2.1 0.21 477 The mean values for the two periods were 2.73 TU and 2.17 TU, re-
14-Aug 1.98 0.26 116.69 spectively, and their difference is significant at p = 0.04 (t-test).
14-Sep 1.89 0.2 236.38 The seasonality of tritium in rainwater largely reflects the different
14-Oct 2.38 0.21 92.33
sources and transport patterns of moisture under the East Asian mon-
14-Nov 2.85 0.24 33.12
14-Dec 4.37 0.37 8.5 soon regime in North Viet Nam. In summer, moisture is transported by
15-Jan 2.87 0.19 23.95 the southeast monsoon from low latitude areas over the Pacific and
15-Feb 2.86 0.19 16.31 Indian Oceans, rains occur under cyclonic conditions prevailing during
15-Mar 2.35 0.21 89.68 monsoon recession or in association with the low pressure systems
15-Apr 0.00
15-May 3.03 0.13 40.25
developed in the area north of the Inter-Tropical Convergence Zone
15-Jun 2.2 0.15 140.13 (ITCZ). Moisture transported from these systems is not expected to be
15-Jul 2.38 0.09 257.83 highly abundant in tritium, so by the end of summer, concentrations of
15-Aug 3.49 0.18 247.70 tritium are quite low.
15-Sep 1.19 0.1 325.55
In winter, meanwhile, Hanoi is largely affected by the northeast
15-Oct 2.37 0.16 33.97
15-Nov 1.44 0.12 139.11 monsoon that brings in continental cold air (CCA) from the high-pres-
15-Dec 1.85 0.14 19.36 sure area over eastern Siberia heavy rains do not occur as the ITCZ and
16-Jan 2.5 0.23 116.18 associated low pressure systems have been moved far south. However,
16-Feb 3.61 0.31 3.06 this is the most humid period with light rains and drizzle frequently
16-Mar 2.24 0.23 24.46
16-Apr 3.42 0.32 119.24
occurring in Hanoi as the Asiatic high pressure center has shifted to the
16-May 1.73 0.14 245.32 east and the CCA becomes saturated after having traveled long dis-
16-Jun 2.71 0.32 73.60 tances over the South China Sea. As a result, high tritium abundance in
16-Jul 2.26 0.21 263.27 rainwater should be expected in this winter period. The difference in
16-Aug 2.46 0.22 377.92
the latitude of moisture sources is a major factor explaining the sea-
16-Sep 2.14 0.18 142.96
16-Oct 5.07 0.28 99.99 sonality of tritium content in Hanoi's rainwater.
16-Nov 2.17 0.22 6.11 The combination with the data available in the region, tritium
16-Dec 3.19 0.31 2.80 concentrations in rainwater at the Hong Kong station (22°31′66.7″N,
114016′66.7″E) were retrieved from the IAEA website, Global Network
for Isotopes in Precipitation (GNIP). Looking at the tritium database in

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H.L. Anh et al. Journal of Environmental Radioactivity 192 (2018) 143–149

Fig. 1. Statistical distribution of tritium concentration in Hanoi's precipitation.

(The fitted curve is Gaussian with an R2 = 0.94 and P < 0.0002).

both Hanoi (Fig. 3) and Hong Kong (Fig. 5), the mean tritium con-
centrations were less than 5 TU with respective values were 2.54 TU
and 3.65 TU despite different period. Besides, it is interesting to note
that a similar trend of tritium seasonality was also observed at the Hong
Kong station, Fig. 6 describes the seasonal index of tritium in rainwater
at the Hong Kong station that was derived from the same statistical
approach applied for the data processing for the Hanoi station. The
similarity of tritium in rainwater observed at Hanoi and at Hong Kong
could be explained by the fact that precipitation at the two stations not
only has the same sources of moisture but also has the same common
features in the transport process in tropical regions.

3.3. Precipitation amount effect

Fig. 2. Normal Q - Q plot of tritium for test distribution. Precipitation amount effect is evaluated from the monthly tritium
data. To determine the extent of the amount effect we normalized the
month's tritium value to the 12-month average and determined the
correlation with monthly rainfall and the result doesn't show a clearly

Fig. 3. Arithmetic means of tritium concentration in Hanoi's precipitation statistic for six years.

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H.L. Anh et al. Journal of Environmental Radioactivity 192 (2018) 143–149

Fig. 4. The seasonal index (S) of tritium concentration in rainwater recorded in the Hanoi station during 2011–2016.

Fig. 5. Arithmetic means of tritium concentration in Hongkong's precipitation statistic from 1997 to 2007.

Fig. 6. The seasonal index (S) of tritium concentration in rainwater recorded in the Hong Kong station during 1996–2007.

significant correlation (Fig. 7). Precipitation amount effect is con- during the rainy season. The rainfall during the dry season is monsoonal
sidered actually due to the timing of the stratosphere-troposphere ex- and is small or even rainless, this can explain for the non-correlation
change with respect to the seasonal rainfall (Tadros et al., 2014) but between tritium concentration and rainfall.
precipitation in Hanoi is deeply affected by moisture from the sea

147
H.L. Anh et al.
Fig. 7. Normalized tritium vs rainfall amount and linear regression.
4. Conclusions
The monthly concentration of tritium in recent precipitation in
Hanoi varied between 0.51 and 7.07 TU and is described by a Gaussian
distribution. The mean annual tritium concentration, weighted by the
amount of precipitation, stabilized from 2.08 to 2.62 TU, which sug-
gests that the tritium in precipitation at the monitoring station is pre-
dominantly from natural contributions. Some months values are larger
than 5 TU, which may be affected by re-evaporated continental water.
Tritium concentrations in precipitation vary between seasons and
the tritium concentration in the dry season is higher than in the rainy
season. This can be explained by stratosphere - to-troposphere ex-
change, but it was less pronounced because precipitation in Hanoi is
deeply affected by the moisture from the sea. In Hanoi, no correlation
was found between tritium concentrations and monthly precipitation
amount.
The tritium data measured in precipitations and different water
types in our project can be used for environmental, hydrological, hy-
drogeological and eco-geological studies in Vietnam.
Acknowledgments
Supporting for this monitoring project has been provided by the
International Atomic Energy Agency through the Technical Co-opera-
tion Project VIE8/0/16. The authors would like to acknowledge the
Ministry of Natural Resources and Environment and Institute for
Nuclear Science and Technology for their support in this study. We
express our gratitude to Dr. Pham Duy Hien, Dr. Dang Duc Nhan, Mr.
Oliver Kracht and reviewers who made many substantial suggestions
which greatly helped in improving this paper.
Appendix A. Supplementary data
Supplementary data related to this article can be found at http://dx.
doi.org/10.1016/j.jenvrad.2018.06.009.
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