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Study of uranium toxicity using low-background gamma-ray spectrometry

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Study of uranium toxicity using low-
background gamma-ray spectrometry

A. Srivastava, V. Chahar, V. Sharma,

Y. Sun, R. Bol, F. Knolle, E. Schnug,
F. Hoyler, N. Naskar, S. Lahiri &
R. Patnaik
Journal of Radioanalytical and
Nuclear Chemistry
An International Journal Dealing with
All Aspects and Applications of Nuclear
Chemistry

ISSN 0236-5731
Volume 314
Number 2

J Radioanal Nucl Chem (2017)

314:1367-1373
DOI 10.1007/s10967-017-5466-9

1 23
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 Author's personal copy
J Radioanal Nucl Chem (2017) 314:1367–1373
DOI 10.1007/s10967-017-5466-9

Study of uranium toxicity using low-background gamma-ray

spectrometry
A. Srivastava1 • V. Chahar1 • V. Sharma1 • Y. Sun2 • R. Bol2 • F. Knolle3 •

E. Schnug4 • F. Hoyler5 • N. Naskar6,7 • S. Lahiri6,7 • R. Patnaik8

Received: 18 August 2017 / Published online: 9 September 2017

Ó Akadémiai Kiadó, Budapest, Hungary 2017

Abstract The natural activity of 238U, 232Th and 40K Keywords Uranium
Animal fossils
Gamma-ray
present in soil, fertilizer and palaeosols besides animal spectrometry
Cancer
Diagenetic processes
fossils was determined using low background gamma ray
spectrometry. The highest uranium activity level were
found in animal fossils of geogenic origin compared to Introduction
palaeosols, soils and fertilizers, a result of post-mortem
uranium assimilation in these fossils via diagenetic pro- Naturally occurring radioactive materials viz. radionuclides
cesses. Hence, geogenic mobilization is likely a major like 40K and the radionuclides belonging to the uranium
cause of elevated uranium levels in Malwa region of and thorium decay series are not object of concern as the
Punjab, also known for higher than normal cancer radiation emitted by them is similar to that of normal
incidence. background level. However, anthropogenic intervention
has many a times led to unwanted increase in their con-
centration and associated radiative effects. Therefore, the
need for their control through regulation has been sug-
& A. Srivastava gested by experts to avoid enhanced radiation exposure to
alok@pu.ac.in the general population by them.
A number of researchers have lately reported that the
1
Chemistry Department, Centre for Advance Studies, Panjab ground water in certain districts of Punjab State especially
University, Chandigarh 160014, India
those located in the Malwa region have high natural ura-
2
Institute of Bio- and Geosciences, IBG-3 Agrosphere, nium concentration. Kumar et al. [1] reported natural ura-
Forschungzentrum Juelich, 52425 Jülich, Germany
nium concentration ranging between 2 and 644 ppb with a
3
Geo Park Harz, Braunschweiger Land, Ostfalen Network, mean of 73.1 ppb while Saini and Bajwa [2] reported
Grummetwiese 16, 38640 Goslar, Germany
uranium concentration from 5.9 to 645 ppb in ground water
4
Department of life Sciences, Technical University of samples collected from Faridkot, Mansa and Bathinda
Braunschweig, Pockelsstrasse 14, 38106 Brunswick,
Germany
districts using laser fluorescence spectrometry. Bajwa et al.
5
[3] have reported uranium concentration from 0.5 to
Nuclear Science Division, Aachen University of Applied
Sciences, Heinrich-Mussmann Strasse-1, 52428 Jülich,
579 ppb with a mean of 73.5 ppb. Alrakabi et al. [4] have
Germany reported concentration varying between 3 and 212 ppb in
6
Department of Environmental Science, University of
Bathinda using X-ray fluorescence technique. The elevated
Calcutta, 35 Ballygunge Circular Road, Kolkata 700019, level of uranium was reported earlier too [5–7] but was not
India taken seriously despite the uranium concentration being
7
Chemical Sciences Division, Saha Institute of Nuclear significantly higher than the 30 ppb permissible limit rec-
Physics, 1/AF Bidhannagar, Kolkata 700064, India ommended for drinking water by World Health Organiza-
8
Geology Department, Panjab University, Chandigarh 160014, tion (WHO) [8] and United States Environmental
India Protection Agency (USEPA) [9] and the higher 60 ppb

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1368 J Radioanal Nucl Chem (2017) 314:1367–1373

recommendation limit of Atomic Energy Regulatory sediments suggest a channel flood plain and Piedmont-type
Board, Government of India (AERB) [10]. Indeed it was deposit, i.e., fluviatile environment while in contrast the
only after reports of children suffering due to uranium lower Siwalik indicated a fluvial deltaic environment.
related complications were brought to the public notice for Phadke et al. [19] found that the uranium hosted sandstone
the first time by Blaurock-Busch et al. [11] that a spurt of transition in the middle and upper Siwaliks are mostly
activity started in this direction. Additionally, Blaurock- litharenites and felspathic wacke, while in the lower
Busch et al. [12] in a later publication further emphasized Siwalik transitions they are sublitharenites and quartz
the detrimental effect of uranium by postulating that it arenites. Overall geochemical and tectonic attributes also
possibly could be the main cause of breast cancer in Pun- indicate that Siwaliks are indeed a rich sedimentary ura-
jabi women from Malwa region, where incidence of cancer nium province.
is already reported to be much higher than the national
average of India.
A number of possible hypotheses have been put forward Materials and methods
to explain the abnormal uranium presence in Malwa region
of Punjab: (i) fallout from the Gulf war, (ii) industrial Sample collection and preparation
effluents, (iii) geogenic origin, (iv) water percolating
through fly ash dumps of thermal power station and For the collection of fossils and palaeosols geological field
(v) excess application of phosphate containing fertilizers to sampling between Pathankot in the west and Poanta Saab
agricultural fields. in the east was undertaken. We avoided the areas that were
The main objective of the present work was to follow up already sampled during our previous study [13] as already
and examine the proposed suggestion from a recent study shown in Fig. 1. The sample sites were marked using
on geogenic mobilization of uranium by Patnaik et al. [13] Garmin-12 GPS with an accuracy of 3 m. These sites were
that postulated that the most plausible origin of the uranium then correlated to fairly well dated (palaeomagnetically,
problem observed in Malwa region of Punjab could be of a biostratigraphically and tephrachronologically) Siwalik
geogenic nature. Several field trips were conducted to sections to get their ages in million years (Ma). The
collect additional fossils and palaeosols from those regions, Siwalik section that have been chosen for such correlation
which could have had links with ancient channels, possibly were the Ghaggar River section exposed east of Chandi-
feeding the ground water channels of Malwa region of garh [20], the Haripur Khol section [21], the Patiali section
Punjab not represented in the earlier reported work as [22] and the Khetpurali section [23]. Sections that are sit-
shown in Fig. 1. In addition a number of soil samples uated far away from magnetostratigraphically dated sec-
representing wide variety of soil types in and outside the tions were tentatively dated based on the faunal content and
Malwa region as shown in Fig. 2 were also collected and broad lithology.
analyzed. Samples of fertilizer, soil, palaeosols and fossils were
Kaul et al. [14] have identified more than 350 uranium obtained from different locations in Punjab and Himachal
rich provenances in major distinct stratigraphic sequences Pradesh. The locations of palaeosols and fossils from the
of the Siwalik group, i.e. upper part of lower Siwaliks, Siwalik region lying in the states of Punjab and Himachal
upper part of middle Siwaliks and lower part of upper Pradesh are shown in Fig. 1, whereas Fig. 2 shows the
Siwaliks. Coffinite, uraninite and pitchblende are the locations of the districts from where the soil samples were
principle ores here. In addition secondary uranium con- collected. Twenty-one soil samples were collected from
taining minerals like bayleyite, azurite, schoepite, swar- different locations from depth ranging between 15 and
lzite, malachite and tyuyamunite, etc., have also been 30 cm. Stones and organic materials were physically sep-
identified. Sharma et al. [15] reported uranium mineral- arated and then were allowed to dry at room temperature.
ization of uraninite and uranophane in pre-Siwalik sedi- The dried samples were further pulverized to yield a fine
mentary rocks of upper Dharmsala Formation. Kumar et al. homogenized powder. 50 g of each of the homogenized
[16] noted that the Siwalik sedimentation is an example of samples were then packed in standard plastic Petri dishes
intraplate subduction and is made up of clastic fluvial with diameter of 75 mm. The petri dishes were then
sediments of Middle Miocene to Middle Pleistocene age. tightened and sealed with adhesive tape. The sealed petri
Furthermore, Parkash et al. [17] highlighted that the dishes were left for 5 weeks to establish secular equilib-
Siwalik group is made up of conglomerates at the top and rium between each parent and daughter radionuclides. The
the lower portion is made up of sandstone and mudstone. activity of 214Pb and 214Bi and activity of 228Ac and 208Tl
Clays, grained sand, silt, and calcite are the matrix material can then be used respectively to determine the activity of
238
of these hosted sandstones for uranium mineralization. U and 232Th but only when the decay rate of progeny
According to Tandon [18] the middle and upper Siwalik

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J Radioanal Nucl Chem (2017) 314:1367–1373 1369

Fig. 1 Geological map of the

area and the sample sites
modified after White et al. [35]

and parent nuclides have become equal, i.e. after the out using Genie 2 k software. Pitchblende standard ura-
establishment of secular equilibrium. nium ore (IAEA) was used for efficiency calibration while
energy calibration was done using 137Cs, 60Co and 133Ba
Radioactivity measurement point source. To minimize statistical error counting period
for each sample and background was kept in the range of
The activity measurements were carried out in Aachen 80,000–100,000 s and 100,000–250,000 s respectively.
238
University of Applied Sciences, Juelich Germany as well U activity was determined from gamma energy transi-
as in Saha Institute of Nuclear Physics, Kolkata, India tion of 214Pb at 295.1, 351.9 keV and gamma ray photo
using low background gamma ray spectrometric setups peak of 214Bi at 609.1 keV. 232Th activity was determined
having high purity germanium detectors. The resolution using gamma ray photo peaks of 228Ac at 338.3, 911.2
and relative efficiency of the CANBERRA’s 747 model along with 583.2 keV photo peak of 208Tl. 1460.8 keV
used at the SINP (Saha Institute of Nuclear Physics), photo peak was used for 40K determination. The further
Kolkata, India, are 3.1 keV at 1332.5 keV and 50% details related to statistical treatment of data, selection of
respectively. The detectors in Juelich had comparable peaks, counting time and efficiency calibration besides
resolution but their relative efficiency was lower by 10%. statistical treatment of data can be had from earlier
To minimize the background radiations interferences the reported work [13, 24–26]. The final estimation of the
HPGe detector in Saha Institute of Nuclear Physics was activity per kg (Bq kg-1) was done by comparator method
kept inside a 9.5 mm thick carbon jacket around 10 cm as described in Ref. [26].
thick lead shied. Data analysis of the samples was carried

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Fig. 2 Map of the region from

where soil samples were
collected

Results and discussion expected since urea is an organic compound consisting of

carbon, hydrogen and nitrogen only.
The activity of uranium in fossils and palaeosols collected It is observed from Tables 1 and 2 that the activity of
from Siwaliks is shown in Table 1 whereas Table 2 shows uranium in fossils and palaeosols collected from the
the activity of naturally occurring uranium, thorium and Siwaliks was higher than that in soil samples collected
potassium in samples of top soils of Punjab. The standard from different locations in Punjab. It is also evident that the
deviation shown along with the mean is based on three mean activity of uranium 42.7 Bq kg-1 in the soils col-
different measurements. The overall uncertainty values lected from locations where uranium related health prob-
range between 10 and 20% based on counting statistics, lems have been reported is comparable to the activity of
calibration and weighing error. The activity of radionu- uranium 42.3 Bq kg-1 in samples collected within the
clides 238U, 232Th and 40K in the soil respectively varied unaffected region.
from 31.6 to 50.1 Bq kg-1, 37.1 to 52.9 Bq kg-1 and 446 Furthermore, the phosphate based fertilizers showed
to 687 Bq kg-1 and showed mean values of 42.7, 45.8 and significant presence of uranium ranging between 83.7 and
587 Bq kg-1. The compilation of the data reported by 2179 Bq kg-1. The uranium in Punjab soil could either be
earlier researchers [27–29] from the same region showed of geogenic origin or derived from anthropogenic use of
that in general the uranium activity in soil ranged between fertilizers [31, 32]. The fertilizer derived uranium load on
14.5 and 94.8 Bq kg-1 with a mean of 35.6 Bq kg-1. The soil in the worst scenario involving delivery of phosphatic
mean activity of uranium obtained in the present work is fertilizer to top soil having a thickness of 20 cm and bulk
found to be comparable with that of the normal range in density of 1.58 mg/m3 [33] was evaluated. A value of
world soils as reported in UNSCEAR report 1993 [30]. The 35 mBq kg-1 per year was obtained assuming application
activity of 238U and 40K in fertilizer samples determined in of phosphatic fertilizer containing 2179 Bq kg-1 of ura-
the present work is shown in Table 3. The phosphate based nium, the highest value obtained in the present work
fertilizer samples did show significant amount of uranium besides further assuming that the average consumption of
with their activity ranging from 83.7 to 2179 Bq kg-1 phosphatic fertilizers was 50.6 kg per hectare per year
whereas in the potassium based fertilizer sample activity based on the fertilizer consumption data provided in liter-
2755 Bq kg-1 of potassium was observed. No uranium, ature [12].
thorium or potassium was observed in case of urea as This indicates that in the last 50 years from the time
when chemical fertilizers were introduced in India one

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Table 1 Activity (Bq kg-1) of uranium in fossils and palaeosols

238
Sample ID Name Siwalik formation and age U content (Bq kg-1) Location

F1 NaladKhad Locality (NKL) Middle, 11 Ma 53.0 ± 5.9 NaladKhad (H.P.)

F2?? Fossil mammalian Bone (DKB-2) Tatrot, 2.5 Ma 208 ± 10.5 DevniKhadri (H.P.)
F3 Turtle Bone (TBM) Upper, 1.5 Ma 1518 ± 13.8 Mirzapur (H.P.)
??
F4 Fossil mammalian Bone (DKB-1) Tatrot, 2.5 Ma 212 ± 8.3 DevniKhadri (H.P.)
F5 Elephant Tusk (ETT) Upper, 1 Ma 2030 ± 32.2 Taranpur (H.P.)
F6?? Fossil Elephant Jaw Bone (MEJ) Tatrot, 2.5 Ma 2491 ± 60.3 Masol (H.P.)
F7 Tusk Elephant (TET) Upper, 3 Ma 599 ± 7.9 Trilokpur (H.P.)
F8?? Fossil Turtle Carapace (MT) Tatrot, 2.5 Ma 683 ± 10.8 Masol (H.P.)
F9 Fossil Bone (FBR) Upper, 1.8 Ma 3583 ± 45.5 Rail (H.P.)
F10?? Sandstone (between palaeosols) (HSST) Tatrot, 2.5 Ma 1109 ± 30.2 HaripurKhol (H.P.)
F11 Fossil Bone (FBBN) Upper, 1 Ma 29 887 ± 454.7 Bana (H.P.)
F12 Fossil Bone (FBGM) Upper, 1.5 Ma 1038 ± 9.9 GoluMajra (H.P.)
F13?? Calcrete from Kanthro Village (KPS) Tatrot, 2.5 Ma 46.7 ± 3.5 Kanthro (Saketi, H.P.)
F14 Fossil Bone (FBMJ) Upper, 1 Ma 1765 ± 19.6 MajraJattan (H.P.)
F15?? Calcareous nodules (RPS-B) Chinji, 13 Ma 60.0 ± 3.4 Ramnagar (J&K)
F16 Fosssil Wood (FWT) Upper, 3 Ma 1536 ± 13.5 Trilokpur (H.P.)
F17?? Large mammal bone Pinjor, 2 Ma 4837 ± 113.5 Moginand Village (Hr)
Fragment (MB)
F18 Bovid Horn (BHR) Upper, 2 Ma 1797 ± 15.4 Raipur (H.P.)
??
F19 Large mammal bone DhokPathan, 9 Ma 1760 ± 31.6 Haritalyangar (H.P.)
Fragment (HB-K6)
F20 Elephant Tusk (ETS) Upper, 2.6 Ma 856 ± 9.0 Sakili (H.P.)
F21?? Elephant Tusk (DKT) Tatrot, 2.5 Ma 704 ± 24.5 DevniKhadri (H.P.)
F22 Fossil Bone (FBT) Upper, 1 Ma 705 ± 8.1 Tunderwal (H.P.)
F23?? Crocodilian bone (RBK) Chinji, 13 Ma 1254 ± 26.9 Ramnagar (J&K)
F24 Fossil Bone (FBN) Upper, 4 Ma 258 ± 4.1 Nalagarh (H.P.)
F25?? Elephant tooth (KET) Tatrot, 2.5 Ma 1019 ± 23.0 Khetpurali (H.P.)
F26 Fossil Bone (FBB) Upper, 1 Ma 1026 ± 10.9 Bhanewal (H.P.)
F27 Fossil Bone (FBPK) Upper, 2.5 Ma 15 597 ± 196.2 Pathankot (H.P.)
F28 PancehkulaIchno Fossil (PKIF) Upper, 2 Ma 42.5 ± 6.2 Panchkula (H.P.)
P1 Palaeosol (MPS) Upper, 2 Ma 87.7 ± 9.3 Markanda (H.P.)
P2?? Palaeosol (HPS-D) DhokPathan, 8.85 Ma 214 ± 2.0 Haritalyangar (H.P.)
P3?? Palaeosol (KHPS) Tatrot, 2.5 Ma 76.1 ± 2.5 Khetpurali (H.P.)
P4 Palaeosol (PSN) Upper, 4 Ma 129 ± 3.1 Nalagarh (H.P.)
P5?? Palaeosol (MPS-N) Tatrot, 2.5 Ma 85.8 ± 2.3 Moginand (H.P.)
P6 Sand Stone with mud pebbles (SSTT) Upper, 3 Ma 33.7 ± 2.9 Trilokpur (H.P.)
P7?? Calcareous Palaeosol (SPS) Tatrot, 2.5 Ma 45.7 ± 1.4 Saketi (H.P.)
P8?? Maroon colour palaeosol (HPSK) DhokPathan, 9 Ma 48.4 ± 2.7 Kursai (H.P.)
P9?? Palaeosol with nodules (NPS) Pinjor 2 Ma 45.5 ± 3.5 Nadah (Haryana)
??
Note Sample ID bearing ( ) correspond to the earlier reported data [13]

would have added anthropogenically 1.7 Bq kg-1 uranium lower would have been the activity of fertilizer derived
activity per hectare to the top soil. However in reality the uranium in ground water. The uranium enriched ground
activity would have been much lower as over the years a water in the affected region has been found generally to be
part of it would have got phyto-accumulated and a part present at depths ranging between 30 and 135 m. Therefore
would have seeped out of top soil. It is worthwhile to point it is unlikely that the fertilizer derived uranium would have
out here that further the water table from the seepage point

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1372 J Radioanal Nucl Chem (2017) 314:1367–1373

Table 2 Activity (Bq kg-1) of soil samples collected from different uranium bearing minerals [14, 15]. Furthermore, Taskin
locations in Punjab State et al. [34] have reported that rain and other water flows do
Sample locations U (Bq kg-1) Th (Bq kg-1) K (Bq kg-1) transport radionuclides present in the rocks to soil. Kaul
et al. [14] corroboratively suggested that uranium enrich-
Ferozepur** 39.1 ± 2.7 43.3 ± 3.1 617 ± 11.0
ment is primarily due to the remobilization by ground
Faridkot** 50.1 ± 3.2 51.2 ± 3.5 564 ± 10.6 water. Additionally, fossils and palaeosols collected in our
Mansa** 46.9 ± 3.1 49.3 ± 3.4 552 ± 10.2 study from the surface were most likely exposed to the
Fazilika** 39.7 ± 2.8 43.6 ± 3.1 589 ± 10.5 ancient geogenic channels enriched in uranium before
Sangarur** 46.2 ± 3.0 47.2 ± 3.3 561 ± 10.3 being uplifted by tectonic activity. Since uranium remo-
Muktsar** 38.9 ± 2.7 39.9 ± 2.9 573 ± 10.3 bilization by ground water is a norm rather than exception,
Bathinda** 43.7 ± 2.9 48.8 ± 3.4 590 ± 10.6 there is every possibility that this ancient ground water
Moga 42.2 ± 2.8 45.4 ± 3.2 644 ± 11.2 system has been feeding the current ground water channels
Ludhiana 48.5 ± 3.0 50.8 ± 3.5 687 ± 11.8 of the Malwa area, where deep drilling for water is gen-
Gurdaspur 31.6 ± 2.3 37.1 ± 2.7 578 ± 10.3 erally being resorted to for agricultural farming.
Jalandhar 46.2 ± 3.0 48.2 ± 3.4 612 ± 10.9
Amritsar 49.8 ± 3.2 52.9 ± 3.5 645 ± 10.8
Nawasahar 42.0 ± 2.8 46.3 ± 3.2 591 ± 10.9 Conclusions
Fatehgarh Sahib 47.3 ± 3.1 49.6 ± 3.4 604 ± 10.7
Barnala 43.7 ± 2.9 47.6 ± 3.3 615 ± 10.8 In conclusion it can be stated that in the light of the earlier
Patiala 35.3 ± 2.4 37.6 ± 2.7 479 ± 8.9 results, the findings of the present work gives a much
Kapurthala 47.5 ± 2.4 50.3 ± 3.3 591 ± 10.2 clearer indication that uranium mobilization in Malwa
TaranTaransahib 45.7 ± 3.3 50.1 ± 3.4 5647 ± 10.3 region could very well be attributed to geogenic reasons. It
Mohali 38.0 ± 2.6 41.0 ± 2.9 446 ± 8.8 would be worthwhile to start a new research program with
Ropar 41.4 ± 2.8 42.3 ± 3.0 624 ± 10.9 focus on age determination of the ground water supposedly
Hoshiarpur 32.4 ± 2.3 39.9 ± 2.8 608 ± 10.4 enriched with Uranium to further confirm the geogenic
origin of uranium toxicity observed in the Malwa region of
Note Sample locations bearing (**) refer to samples collected from
Malwa region Panjab known for higher than normal cancer incidence.

Acknowledgements The authors are grateful to Prof. M. Caffee,

Director, Purdue Rare Isotope Measurement (PRIME) Laboratory,
Table 3 Activity (Bq kg-1) of uranium and potassium in different Purdue University, USA and Prof. S. Good, Biological and Ecological
phosphate based (PF), nitrogen–phosphate–potassium based (NPKF) Engineering Department, Oregon State University, USA for their
and urea based (UF) fertilizer samples valuable suggestions to obtain more meaningful information from the
data collected. Alok Srivastava is thankful to Alexander von Hum-
238
Sample ID fertilizer U (Bq kg-1) 40
K (Bq kg-1) boldt Foundation, Germany for providing fund to carry part of the
research work in Aachen University of Applied Sciences, Juelich,
PF-1 83.7 ± 8.0 22.6 ± 7.4 Germany. Vikash Chahar is grateful to UGC for Junior Research
PF-2 2179 ± 12.5 68.8 ± 4.1 Fellowship. Rajeev Patnaik was supported by MOES project (MoES/
PF-3 1213 ± 9.5 106 ± 3.6 P.O. (Geoscience)/46/2015). The gamma ray spectrometric experi-
mental facility provided through UGC-CAS funding to Department of
NPKF-1 115 ± 1.3 2755 ± 11.9 Chemistry, Panjab University, Chandigarh used for initial screening
UF-1 Not detected Not detected of the samples is also thankfully acknowledged. The support from
Department of Atomic Energy through TULIP program to SINP is
also gratefully acknowledged. N. Naskar is thankful to UGC for
providing Research Fellowship. The contribution of Mr. S. Mohr from
Harz National Park, Goslar, Germany in the form of drawing the
played a significant role in bringing about enrichment of
figures is also gratefully acknowledged.
uranium in ground water of Malwa region of Punjab State.
The comparison of the mean activity of uranium present
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