Environmental Earth Sciences (2021) 80:473

https://doi.org/10.1007/s12665-021-09766-5

ORIGINAL ARTICLE

Occurrence of uranopolycrase in pegmatite related to a Jurassic

granite pluton in Cheongwon, South Korea: mineral chemistry
and texture of a potential source of uranium and radon in a granite
aquifer
Jeong Hwang1   · Sung Won Kim2

Received: 25 May 2020 / Accepted: 10 June 2021

© The Author(s), under exclusive licence to Springer-Verlag GmbH Germany, part of Springer Nature 2021

Abstract
Cheongwon is well-known in South Korea for the abnormally high aqueous concentrations of U and Rn in the underlying
Jurassic granite aquifer. This study reports on the chemistry and texture of a new U-host mineral to indicate the effective
source of U in the granite aquifer, and discusses the implications of the occurrence of U near groundwater monitoring wells.
To investigate the internal fabric and homogeneity, the mineral chemistry and texture were examined using field-emission
scanning electron microscope and electron probe micro-analyzer, respectively. Uranopolycrase, a mineral of the euxenite
group, occurred as a large subhedral grains in a pegmatite related to a Jurassic granite pluton. A significant U content indi-
cated metamictization, which resulted in an optically isotropic body and generate cracks and voids. Elemental distribution
maps revealed that uranopolycrase had relatively low in U and Y contents, but high in Ti and Pb contents near a micro-
veinlet and void. These findings suggest that U could be preferentially leached out as a result of alteration and the loss of
A-site cations in metamict uranopolycrase. The alteration of metamict uranopolycrase is an effective process for releasing
radionuclides into the environment. Based on the U- and Ti-remobilized alteration texture, uranopolycrase is considered
to be the most important host mineral of the interpreting the availability of U- and Rn-supplies in the granite aquifer of the
study area in Cheongwon.

Keywords  Pegmatite · Uranopolycrase · Metamictization · Alteration · U-source · Granite aquifer

Introduction Many studies have reported high U and Rn concentra-

The high concentration level of radionuclides such as ura-
nium (U) and radon (Rn) in drinking water are harmful to
human health due to their toxicity and radioactivity (WHO
2011). In groundwater, U can occur naturally a result of
the dissolution of U-bearing minerals, which are particular
enriched in granites. The majority of Rn is produced by the
decay of U.
* Jeong Hwang
jeongha@dju.kr
1
Department of Geotechnical Disaster Prevention
Engineering, Daejeon University, Daejeon 34520,
Republic of Korea
2
Geological Research Center, Korea Institute of Geoscience
and Mineral Resources, Daejeon 34132, Republic of Korea
tions in groundwater in granite terrain worldwide. In Iddef-
jord granite from Norway, which has the highest prospect
of the occurrence of groundwater containing high level of
radioelements, the median of U and Rn concentrations were
15 µg/L and 2500 Bq/L, respectively. The highest U and Rn
concentrations were 170 µg/L and 8500 Bq/L, respectively
(Banks et al. 1995). It has long been known that Iddefjord
granite contains unusually high contents of U up to 50 ppm
(Lindahl 1983). The anomalously high radioactivity of
groundwater in the Helsinki region, which has concentra-
tions of U and Rn up to 14,870 μg/L and 32,592 Bq/L, is
caused by primary U-mineralization in granite (Asikainen
and Kahlos 1979). In the Karkonosze granite massif, which
has the highest prospect of the occurrence of water with
high radon concentrations in Poland, the median of Rn con-
centration was 106 Bq/L and the highest concentration of
Rn was 1465 Bq/L. The occurrence of water with a high Rn

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concentration depends on the content of U in granitic rocks
(Przylibski et al. 2020).
Most of groundwater with high U and Rn concentration
has been reported to be associated within Jurassic granite,
which is the representative igneous rock in South Korea. In
Jurassic granite from Icheon, which has the highest prospect
for the occurrence of groundwater containing high concen-
trations of radioelements in South Korea, the median U and
Rn concentrations were 3 µg/L and 176 Bq/L, respectively,
while the highest U and Rn concentrations were 1640 µg/L
and 865 Bq/L, respectively (Cho and Choo 2019). Juras-
sic granites occur as an extensive deep-seated batholith and
outcrops in the central part of the Korean Peninsula (Fig. 1).
According to the close inspections of granite aquifer con-
ducted by the South Korean governmental authority, granitic
host rocks do not always play a conclusive role in enrich-
ing U and Rn concentrations in groundwater (NIER 2008,
2009).
Cheongwon is located in a Jurassic granite region in
South Korea, and has attracted attention to due to the abnor-
mally high U and Rn concentrations in the groundwater in
this region (Fig. 1). Cheongwon was selected as the study
area as the maximum U and Rn concentrations in borehole
groundwater have been found to be 683 µg/L and 477 Bq/L,
respectively, which highly exceed the guideline value set by
Fig. 1  Geological map of the study area (modified from Kwon and Jin 1974; Lee et al. 1996)
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Environmental Earth Sciences (2021) 80:473
the United States Environmental Protection Agency (NIER
2008; Jeong et al. 2011). The dissolved U in groundwater
can originate from minerals that contain U as their major or
minor component. Hwang et al. (2014) reported that uranif-
erous host rocks and U-minerals are the source of dissolved
U in groundwater in the Daejeon area, which is adjacent to
Cheongwon. Although many studies have determined the
source of dissolved U and Rn in the granite aquifer of the
study area (Choo 2002; Jeong et al. 2011; Cho et al. 2015),
the effective source of radionuclides, a problematic issue in
Korea, has not yet been ascertained.
U and Rn concentrations in groundwater are believed to
be directly controlled by three factors: hydrodynamic condi-
tions, the U content of rocks in the vicinity of the well and
mineralogy of U within the host rock (Banks et al. 1995).
Most radioelements in Jurassic granites occur as trace ele-
ments in some accessory mineral phases, such as monazite
and apatite (Cho and Choo 2019; Jeong et al. 2011). The
solubility of radionuclides trapped in these trace minerals
depends on geochemical parameters such as redox, and pH
conditions and alkalinity. The concentration of radionuclides
in groundwater does not appear to be correlated with most
geochemical parameters, and it might be confined to very
limited areas possibly due to the presence of veinlets or
a narrow alteration zone containing U-minerals (Cho and
Environmental Earth Sciences (2021) 80:473 Page 3 of 11  473
Choo 2019). The average content of U in Jurassic granites
is 2.3 ppm, which is much lower than the global average
of 5 ppm in acidic igneous rock (Hwang and Moon 2020).
Considering the geochemical conditions and the low content
of U in Jurassic granite, it is estimated that the remaining
factor, U-mineralogy of rocks, plays the most important role
in producing groundwater with high U and Rn contents in
Jurassic granite aquifers.
Acidic igneous rocks such as granite and pegmatite often
have higher than average content of U in the earth’s crust.
Despite a high U content, some rocks are not usually treated
as a source of U-pollution when their U-host minerals are
insoluble in groundwater (Skeppström and Olofsson 2007).
However, new U-host minerals might act as sources of
radioelements in groundwater if they are soluble enough to
allow the liberation of U from the mineral lattice. To inves-
tigate the sources of dissolved U and Rn in groundwater, it
is important to identify U-host minerals and to determine
whether they have chemistry and texture from which U can
be liberated easily under geologic surface conditions.
For this purpose, this study reports on a new U-host min-
eral and its chemistry and texture, and uses this information
to indicate the effective source of U in the Cheongwon gran-
ite aquifer. The mineral texture, chemistry and elemental
distribution map of the new U-mineral were examined using
electron microprobe. Further, a potential source of uranium
and radon in a granite aquifer near the borehole groundwater
are discussed.
Study area
Geological setting
One of the major igneous activities in South Korea occurred
during Late Triassic to Middle Jurassic period. The grani-
toids of this age are traditionally called “Daebo granitoids”.
Jurassic granite in South Korea tends to be distributed along
a NNE-SSW direction (Korean tectonic line) and occupies
almost one third of the country’s area. The Jurassic granite
in Cheongwon, belongs to a part of the “Cheongju granite
pluton”, and consists of medium to coarse grained biotite
granite and porphyritic granite (Fig. 1). Some of the bio-
tite granite occasionally occurs as porphyritic granite with
megacrystic feldspar (3 to 5 cm in length; Fig. 2a). These
two types of granite have a gradational boundary, which sug-
gests that they have the same parental magma origin (Kwon
and Jin 1974; Lee et al. 1996). Biotite schist, a metamor-
phic rock of the Precambrian, was intruded by granite and
occurs as a roof pendant in high-altitude areas such as the
top of mountains. The U–Pb zircon age of biotite granite is
170 Ma, and its major and trace element patterns suggest
that it is subduction-related I-type granite, while the Sr–Nd
isotopic compositions indicate crustal and mantle origins
(Cheong et al. 2011).
Hydrogeology
Groundwater radionuclide data from 20 wells drilled in
granite around the study area were obtained from the
National Institute of Environmental Research (NIER 2008).
The median U and Rn concentrations were 1.8 µg/L and
78 Bq/L, respectively. All data points, except one, were
below the maximum U contamination level (30 µg/L) and
the alternative maximum Rn contamination level (148 Bq/L)
as per USEPA standards. However, anomalously high U and
Rn concentrations of 178 µg/L and 477 Bq/L, respectively,
were reported in one well of the study area; therefore, the
Korean administrative authority closed it. To investigate
the source of radionuclides in groundwater, a test borehole
has been drilled and monitored in the study area which is
a region of great concern due to the high radionuclides in
groundwater (Fig. 1). A 120 m deep borehole was drilled to
investigate the relationships between the geochemical envi-
ronment and the natural occurrence of radioactive materials.
For this purpose, six groundwater samples were collected
at different depths from − 10 to − 120 m using a double-
packed system (Jeong et al. 2011). The pH and EC of the
groundwater ranged from 5.6 to 8.3 and 469 to 609 µS/cm,
respectively. The hydrochemistry of the groundwater shows
that it was of Ca-HCO3 type. The U and Rn concentrations
in the groundwater were 0.03 ~ 683 µg/L and 48 ~ 281 Bq/L,
respectively. The concentrations of U and Rn are highest at
depths from − 50 to − 70 m, and show positive correlations
at each depth. Jeong et al. (2011) reported some accessory
mineral phases such as monazite and apatite as source min-
erals of U and Rn in groundwater; however, a reasonable
source material has not yet been determined, despite many
studies on the minerals of granite aquifers.
Pegmatite occurrence
Pegmatite occurs in porphyritic granite near the contact
with biotite schist. The mineral composition of pegmatite
is simple; it contains massive quartz and blocky white feld-
spar of plagioclase and microcline (Fig. 2b). In the vicinity
of pegmatite, the host rock has been altered to leucocratic
by veinlets, within which chlorite and epidote are abundant
(Fig. 2c). In altered granite, plagioclase has been changed
to sericite or muscovite and epidote, and almost all biotite
have been altered to chlorite. The plagioclases in both of
pegmatite and granite have been changed to sericite and
replaced by fresh microcline. Pegmatite is cut by fracture
filling veinlets which include muscovite, biotite and epidote.
U-minerals including rare-earth-elements (REEs), occur
along fractures or vug-filling muscovite veinlets (Fig. 2d).
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 473   Page 4 of 11
Fig. 2  Photographs of outcrops and hand specimens from study area.
a Porphyritc biotite granite intruded by pegmatite vein along the frac-
ture. b Pegmatite with massive quartz and blocky white feldspar. c
Host rock of pegmatite altered to leucocratic with small veinlets of
The REE mineralization of the Chungju-Goesan area, which
is located in north-eastern part of the study area, has been
reported to be closely related to Jurassic igneous activity
with the intrusion of biotite granite and pegmatite (Cheong
et al. 2015; Kang et al. 2018).
Materials and methods
Two pegmatite samples showing higher radioactivity were
selected using a portable spectrometer (Fig. 2), and two
polished thin sections were carefully prepared for the min-
eralogical study (Fig. 3). The mineralogical characteristics
including texture and chemistry were examined using an
optical and electron microprobe. The electron microprobe
analyses were performed on polished thin sections. The
texture and composition of minerals were simultaneously
analyzed using a field emission scanning electron micro-
scope (FE-SEM, Hitachi S-4800, Japan) and an electron
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Environmental Earth Sciences (2021) 80:473
chlorite and epidote. d Muscovite veinlet with U-mineral along the
fracture or vug in feldspar and quartz. chl chlorite, ep epidote, K-fd
K-feldspar, mus muscovite, pl plagioclase, qz quartz
probe micro-analyzer (EPMA, Shimadzu 1610, Japan)
at the Korea Basic Science Institute (KBSI) Smart Open
Lab. The FE-SEM was equipped with an energy disper-
sive X-ray spectroscope (EDS) and a backscatter electron
image (BSE) detector (X-max 50 ­m m 2, Oxford). The
Operating conditions were a 15 kV accelerating voltage,
a 10 nA emission current, and a 5–200 nm sized beam.
The EPMA is equipped with a four tunable wavelength-
dispersive spectrometer (WDS). The operating conditions
were 15 kV accelerating voltage, a 50 nA beam current,
52.5° take off angle, and 0.5–1 μm sized beam. The min-
eral chemistry was obtained using the WDS and EDS. The
detection limits were 0.1–0.05 wt. % depending on the
analyzed element. The raw intensities were converted into
element concentrations using the automated ZAF matrix-
correction software. An element map and BSE images
were acquired for each polished thin section to study the
internal fabric of the mineral aggregates and the homoge-
neity of the element distribution.
Environmental Earth Sciences (2021) 80:473 Page 5 of 11  473
Fig. 3  Textural patterns of uranopolycrase in pegmatite. a Transmit-
ted optical microscope image of uranopolycrase crystal included in
K-feldspar shown in brown to dark. Thin section open nicol. b Subhe-
dral uranopolycrase crystal. BSE image c Transmitted optical micro-
Results
Mineral occurrence
U-minerals occurred along fracture filling veinlets in the
pegmatite sample. Visual observations revealed that the
crystals are opaque and submetallic luster, and polarizing
microscope observations showed a brown to dark coloration
and isotropic property. The crystals occurred either as a large
subhedral grains enclosed in a microcline vug (Fig. 3a, b) or
as a subhedral elongated grains associated with muscovite,
biotite, and chlorite (Fig. 3c, d).
Mineral chemistry
The mineral chemistry was examined using EPMA (WDS
mode) and SEM (EDS mode) (Fig. 4). The analytical data
indicated that the U-mineral was composed of U 23–27
wt.%, Ti 16–26 wt.%, Nb 9–24 wt.%, Y 7–10 wt.%, Ta
0–3 wt.%, Th 1–5 wt.%, and Ca 0–2 wt.%. This mineral
scope image of uranopolycrase crystal included in a veinlet with mus-
covite and biotite. Biotite altered to chlorite. Thin section open nicol.
d Euhedral uranopolycrase crystal. BSE image bt: biotite, chl: chlo-
rite, K-fd: K-feldspar, mus: muscovite, qz: quartz, Ur: uranopolycrase
chemistry is very similar to the euxenite group minerals
(EGMs). The general formula of EGMs is A ­ B2O6 where
the octahedral position A is occupied by Y, REEs, Ca, U
and Th, while the hexahedral position B is occupied by
Ti, Nb, and Ta. Based on EGM chemistry, the simpli-
fied structural formula from the WDS data can be writ-
ten as ­(U 0.6 Y 0.4 Ca 0.2 Th 0.1 ) 1.3 (Ti 1.2 Nb 0.6 Ta 0.2 ) 2.0 O 6 or
­(U0.6Y0.4Th0.1)1.1(Ti1.4Nb0.7)2.1O6, which reflect that U and
Ti almost dominate over Y and Nb, respectively. From our
chemical data, it is possible to infer the simplified chemical
formula of (U,Y)(Ti,Nb)2O6, which is corresponds to ura-
nopolycrase, one of the EGM species.
The ­AB2O6 phases with Y and Ti as the dominant A- and
B-site cations, respectively, corresponded to polycrase and
aeschynite, which are undistinguishable from each other in
chemical composition. To resolve the difficulty of chemi-
cally differentiating the ­AB2O6 phases, the abundances of
U and Th can potentially be used to discriminate between
polycrase and aeschynite (Ewing 1976; Hanson et al. 1992).
It has been proposed that Ti-dominant ­AB2O6 oxide with a
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 473   Page 6 of 11
Fig. 4  BSE image (top left) and WDS spectra (1–3) show the occur-
rence and chemical composition of U-mineral phases. The chemical
compositions of analysis point-1 correspond to uraninite, and points-2
sum of U­ O2 > ­ThO2 should be called polycrase. By compar-
ing the chemical data for the ideal formula of polycrase,
Y(Ti,Nb) 2O 6, with those of the uranopolycrase, (U,Y)
­ 3+
(Ti,Nb)2O6, found in the study area, the substitution of Y
4+ 4+
by ­U  and ­Th was determined to be coupled with the
substitution of N ­ b5+ and T
­ a5+ by ­Ti4+ in uranopolycrase
(Aurisicchio et al. 1993).
Element distribution
High-resolution quantitative compositional mapping with
low detection limits was obtained using WDS on EPMA
results. This technique has proved to be very useful and pow-
erful for imaging small-scale compositional heterogeneities
in mineral phases. Figure 5 shows the maps for U, Y, Ti,
and Nb as major elements and Pb as a trace element, which
comprise uranopolycrase. In these element maps, higher
concentrations are displayed from yellow to red, whereas
lower concentrations are displayed as green to blue. The
relative concentrations of a given element are expressed in
false colors, whereby the ‘warm’ shades stand for a higher
13
Environmental Earth Sciences (2021) 80:473
and -3 to uranopolycrase. Uranopolycrase include rutile, zircon and
thorite. rt: rutile, zr: zircon, thr: thorite
content. The relative concentrations were acquired in counts
per second. Thus, due to the different sensitivities for indi-
vidual elements, a given color in one map does not corre-
spond to the same concentration on elemental another maps.
The mapped area is shown as the BSE image in the upper
left corner of Fig. 5. The BSE image reveals textural details
formed by a micro-veinlet and void in the uranopolycrase.
With the exception of the region near the veinlet and void,
the BSE image of the uranopolycrase sample can be recog-
nized into two zones; gray and dark gray. When comparing
the map for U with the BSE image, it can be seen that the
gray zone was consistent with the U-rich part, while the
dark gray zone was relatively U-deficient. The heterogene-
ous irregular zoning seen in the BSE images was caused by
variation in U (Fig. 5). The U-deficient zone was observed to
be brown under the polarizing microscope, while the U-rich
zone was darker (Fig. 3a, c).
The maps for U, Y, Ti, and Nb exhibited heterogeneous
elemental distributions around the veinlet and void. The
whitest part of the veinlet shape in BSE image was consist-
ent with the highest U concentration area that did not contain
Environmental Earth Sciences (2021) 80:473 Page 7 of 11  473
Fig. 5  BSE image (top left) for
uranopolycrase showing grayish
and dark grayish zones, and
EPMA elemental maps showing
the heterogeneous irregular
zoning caused by the variations
in U, Ti, and Pb. The scale (see
right hand side bars) is in color
intensity, but differs from ele-
ment to element
any Y, Ti or Nb, which means that the phase of veinlet was
uraninite ­(UO2). In the BSE image of Fig. 5, the veinlet
appears in dark gray and the void as black. The veinlet con-
tained the highest Ti concentration phase, which indicates
the occurrence of rutile (­ TiO2). In the area of the veinlet and
void, a rich distribution of Ti and Pb were found, whereas
this area was deficient in U and Y. Although the Pb-bearing
phase was not identified precisely, a Pb-oxide was expected
because no sulfur peak was detected in the EDS with the
exception of galena (PbS) in Fig. 7. A negative correlation
was found between Ti-Pb and U especially near the veinlet
and void.
Discussion
Petrogenetic significance of uranopolycrase
occurrence
Uranopolycrase was named as the U-dominant ana-
logue of polycrase-(Y), and its name has been approved
by the International Mineralogical Association (IMA
1990–046) (Fourestier 2002). Elba Island in Italy is the
most well-known localities for the occurrence of a peg-
matite related to a granodiorite pluton (Aurisicchio et al.
1993). It was reported for the first time with the chemical
formulae of (­ U0.62Y0.29Th0.07Nd0.01Ca0.02Mn0.03)Σ=1.04 and
­(Ti1.46Nb0.30Ta0.12)Σ=1.94O6. The formulae show that the min-
eral has U-Y and Ti-Nb as the dominant A- and B-site cati-
ons, respectively. The predominance of U at the A-site and
Ti at the B-site distinguishes uranopolycrase from EGMs,
which occur primarily as accessory minerals in granites and
pegmatites (Gaines et al. 1997).
The geochemical characteristics of Nb–Ta minerals in
pegmatite rocks provide information about their petrogen-
esis. The (Y, REE, U, Th)–(Nb, Ta, Ti) oxides such as EGMs
are mainly present in REE-enriched granitic pegmatite and
are derived mainly from A- and I-type fractionated gran-
ites (Černy and Ercit 2005). The opposite research results
have been reported for the geochemical and isotopic char-
acteristics of the Cheongju granite pluton in the study area.
Uchida et al. (2012) reported that the northern and southern
plutons are classified as S-type and I-type granites, respec-
tively. Cheong et al. (2011) reported that the geochemical
13
 473   Page 8 of 11
signature suggests I-type granite, meanwhile the Sr–Nd iso-
topic signature indicate S-type granite. Sometimes, I-type
granite can show an S-type signature when they are highly
fractionated (Chappell and White 1992). The occurrence of
pegmatite including EGMs supports that the hypothesis that
granite in the study area is an I-type granite rather than an
S-type granite.
Metamictization of uranopolycrase
Minerals containing U and Th are commonly metamict due
to accumulated α-recoil damage. Some minerals such as zir-
con, titanite, and REE-oxides commonly become metamict,
whereas minerals such as monazite and apatite preserve their
crystalline state, even if they experienced similar radiation
doses (Nasdala et al. 2001). Brannerite ­(UTi2O6), the ana-
logue of uranopolycrase ((U,Y)(Ti,Nb)2O6), normally alters
to a T
­ iO2 phase via leaching of U with the corresponding Ti
no longer fitting the structure of brannerite; consequently,
Ti is released to form rutile (Ramdhor 1980). The EGMs
are typically metamict owing to the incorporation of U and
Th. Metamictization of EGMs is a common phenomenon
that results in the modification of the primary texture and
chemical composition (Szuszkiewicz et al. 2016). Metamic-
tization of minerals causes changes in volume and mechani-
cal properties. Roudil et al. (2008) reported that radioactive
decay includes the formation of cracks and porosity within
the U-mineral due to the release of daughter gases (e.g., He
and Rn). Many cracks are also due to stress induced by the
increased volume that accompanies metamictization. The
uranopolycrase of the study area was observed to be opti-
cally isotropic and included fracture filling micro-veinlets
and voids (Fig. 5). These optical and textural character-
istics suggest that it has been either partly or completely
metamicted.
In oxides of EGMs, only uranopolycrase contains U as
an essential constituent. It occurs as large crystals with a
high U-content of up to 27 wt. % in the study area. The
high U content of uranopolycrase indicates a strong radioac-
tive nature, which promotes to metamictization. Quantita-
tive analyses of the chemical composition were carried out
using an EPMA with a WDS after conducting detailed EDS
semi-quantitative analytical measurements of the chemical
components of uranopolycrase. However, the total chemical
content of the data was fairly at < 80 wt. %, which was prob-
ably due to post-metamictization that reduced the atomic
density and resulted in a decrease in the oxide of EGMs
(Lumpkin and Ewing 1984).
Alteration of uranopolycrase
The alteration of metamict mineral is an effective process
for releasing radionuclides into the environment (Geisler
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Environmental Earth Sciences (2021) 80:473
et al. 2005). Owing to their significant concentrations in U
and Th, Nb–Ta oxides usually experience strong structural
damage resulting from radioactive decay (Ewing 1975). This
alteration leads to increases in the vacancies due to increased
hydration and the leaching of A-site cations (Lumpkin and
Ewing 1995). Pöml et al. (2007) reported that the REEs, Y,
and most of the U were removed from metamict betafite,
(Y,U,Ce)2(Ti,Nb,Ta)2O6(OH), thus leaving Ti, Nb and Ta
behind during the alteration process. This suggests that U
could be preferentially leached out as a result of alteration
and the loss of A-site cations in metamict mineral. U-con-
taining minerals undergo a process of structural breakdown
such as metamictization, during which the daughter radio-
nuclides are not normally captured within the host lattice,
rather they migrate within or outside the mineral. Lead (II)
is not compatible with the crystalline structure of U-minerals
because of differences in ionic radii and valences. There-
fore, Pb tends to leave the U-mineral crystal structure during
alteration events (Janeczek and Ewing 1992; Alexander and
Kyser 2005).
Our observations are consistent with numerous exist-
ing research results, whereby the highest Ti and Pb zones
were found to be close to the veinlet or void, which was
deficient in U and Y (Fig. 5). These characteristics reflect
the Pb-redistribution due to the radioactive decay process
(Macmillan et al. 2016). Figure 6 displays the elemental
maps enlarged the lower left of Fig. 5, which show that the
­TiO2 phase was common near the veinlet and void, whereas
U and Y were very rare. The T ­ iO2 phase can commonly
occur around micro-cracks and voids as a result of the loss of
A-site cations in uranopolycrase. A uraninite (­ UO2) veinlet
was observed along the dark gray part of the BSE image,
within which U was deficient (Fig. 7). This suggests that
the uraninite veinlet could have been formed by the fracture-
controlled metasomatism of U followed by micro-cracking.
The BSE images in Figs. 6 and 7 include patches of voids
and U- or Ti–rich veinlets that exhibit a fine-scale altera-
tion. The alteration was readily apparent along the voids
and micro-veinlets, some of which contained precipitates
of Pb. The BSE images of Figs. 5 and 6 reveal secondary
mineral phases such as rutile which are usually present when
dissolution—precipitation reactions occur, as these allow
the remobilization of U (Guastoni et al. 2019). Based on
existing research results, it is suggested that rutile (­ TiO2)
and uraninite (­ UO2) were formed during metamictization
and the alteration of uranopolycrase.
Source of dissolved radionuclides
Metamictization as well as the alteration of EGMs are
common phenomena that result in the modification of the
primary chemical composition (Szuszkiewicz et al. 2016).
When U-minerals retaining radioactive decay are exposed
Environmental Earth Sciences (2021) 80:473 Page 9 of 11  473

Fig. 6  BSE image (top left) and

elemental maps showing the
elemental redistribution with
U-Y-deficient and Ti-rich com-
position along a veinlet and void

Fig. 7  BSE image (top left)

and elemental maps showing
the occurrence of uraninite as a
veinlet along dark grayish zone
of U-deficiency in uranopoly-
crase, where Pb is only found as
a small spot of galena (PbS)

13
 473   Page 10 of 11
to a fluid, the generation of cracking and porosity facilitate
the percolation of fluid and the alteration to a more suscep-
tible mineral (Macmillan et al. 2016). The alteration and
dissolution of metamict uranopolycrase contributes U to
geological fluids, both hydrothermal and meteoric fluids,
thus suggesting that it should be a good source of radionu-
clides to groundwater.
The main source rock and mineral for U and Rn in the
groundwater of the study area had been reported as biotite
schist and monazite, respectively (Jeong et al. 2011). How-
ever, it could be considered as an unexpected situation in
Korea because high U and Rn concentrations in groundwa-
ter can occur in granitic rock areas. Although U partitions
strongly with phosphate, and can therefore occur at a high
concentration in monazite, its relatively low abundance in
biotite schist and insolubility in groundwater mean that, it is
unlikely to contribute significant radionuclides to groundwa-
ter (Smedley et al. 2006). In U-enriched granites, however,
high-U minerals such as uraninite, thorite and a variety of
U-Nb-Ti oxides often account for over 50% of the whole-
rock value. The availability of the U held in these important
contributors depends on a variety of factors including the
compositional variation, the degree of alteration or metam-
ictization, and the textural relationships of major minerals
(Basham et al. 1982). The identification and characterization
of U-species is therefore of great importance to U fertility
studies; however, their presence is frequently not recognized
due to their low modal abundance. Hence, further integrated
mineralogical and geochemical research was required to
investigate the U fertility of the granite aquifer in the study
area. Uranium-bearing oxide minerals are easily dissolved
and are probably the most important source of dissolved U
to groundwater as a result of altered granite terrains under
oxidizing conditions (Cabral Pinto et al. 2014). The results
of the U-mineral chemistry and U-Ti remobilized alteration
texture determined in the present study suggest that urano-
polycrase is the most important host mineral for interpreting
the availability of U and Rn supplies in the studied granite
aquifer.
Conclusion
This study examined the use of U-host mineral chemistry
and texture as an indicator of the effective source of radionu-
clides in a granite aquifer. Uranopolycrase, one of the EGM
species, was observed as a subhedral grains along a fracture
filling veinlet in a pegmatite related to a Jurassic granite
pluton. A significant U content of 23 to 27 wt. % indicated
that uranopolycrase had been metamicted which caused an
optically isotropic property and generated cracks and voids.
The element distribution maps revealed that uranopolycrase
was clearly depleted in U and Y, whereas there were higher
13
Environmental Earth Sciences (2021) 80:473
contents of Ti and Pb near micro-veinlets and voids. These
findings suggest that U could be preferentially leached out as
a result of alteration and the loss of A-site cations in meta-
mict uranopolycrase. Metamictization of uranopolycrase
facilitates the percolation of fluids and altered it to a more
susceptible mineral. The alteration of metamict uranopoly-
crase is an effective process for releasing radionuclides into
the environment. Based on the U- and Ti-remobilized altera-
tion texture, uranopolycrase is considered to be the most
important host mineral for interpreting the availability of
U- and Rn-supplies in the granite aquifer of the study area.
Acknowledgements  This work was supported by the Korean Research
Foundation (Project no. 2019R111A3A01059901). We appreciate the
contribution of the anonymous reviewers, and thank Park JI and Lee
YB for discussions and their help with the FE-SEM and EPMA analy-
ses at the Korea Basic Science Institute (KBSI) Smart Open Lab.
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