Contributions to
Contrib. Mineral. Petrol. 66, 409-414 (1978)
Uranium in Metamorphic Rocks
Jaroslav Dostal 1 and Silvio Capedri a
i Department of Geology, Saint Mary's University, Halifax, N.S., Canada
Istituto di Mineralogia e Petrologia, Universita di Modena, Italy
Abstract. The distribution of U has been studied in
two metamorphic rock-series with a gradient of re-
gional metamorphism. One series ranges from the
lowest greenschist to amphibolite facies and the other
one shows increasing metamorphic grade from am-
phibolite to granulite facies. Several medium and high
pressure granulitic inclusions from alkali basalts were
also analyzed. The abundances of U in the rocks
do not appear to be affected by metamorphism below
the granulite facies grade. Granulites are depleted in
U in comparison with equivalent rocks of amphibolite
facies grade. There are also differences in their U
distribution, as the bulk of U in amphibolite facies
rocks is located along the fractures and cleavage
planes of ferro-magnesian minerals and in U-rich ac-
cessories, while in granulites, most of the U resides
in accessory minerals. It seems that the depletion of
U in granulites is due to a loss of U which is not
located in accessory minerals or in the crystal struc-
ture of rock-forming minerals and may also be related
to a migration of hydrous fluids, perhaps during dehy-
dration.
Introduction
The behaviour of uranium during metamorphic
processes is still not well known. Several recent studies
(Lambert and Heier, 1968; Heier, 1973)have shown
that granulite facies rocks are depleted in U compared
to rocks of lower metamorphic grades. There are also
indications that some U might be already lost at a
moderate grade of progressive metamorphism (Heier
and Adams, 1965; Lambert and Heier, 1967). How-
ever, the actual mechanism or reactions leading to
the release of U during metamorphism are not well
established and it has even been suggested that the
low abundance of U in granulites is a primary feature,
Mineralogy and
Petrology
9 by Springer-Verlag 1978
unrelated to metamorphism (Holland and Lambert,
1973; D u p u y et al., 1977). Furthermore, only a few
data have been reported on the location of U in meta-
morphic rocks and whether the bulk of U is present
in major rock-forming minerals, U-rich accessories
or is concentrated along the grain boundaries, frac-
tures etc. is not exactly known.
The purpose of this study is to present data on
the abundances of U in rocks of different metamor-
phic grades and their constituent minerals, to com-
pare the concentration of U in some of these rocks
with that of several other elements (K, Rb, Ba, Zr,
and Ti) and to evaluate the behaviour of U during
regional metamorphic processes.
Two rock-series with progressively increasing
grade of metamorphism, one ranging from the lowest
greenschist to amphibolite facies and the other from
amphibolite to granulite facies, have been analyzed
together with several granulitic inclusions from alkali
basalts.
Geological Notes and Sample Descriptions
The first series, the Devonian Littleton formation of New Hamp-
shire, comprises pelitic rocks with a grade of metamorphism vary-
ing from below the lowest greenschist facies (fossiliferous shales)
to amphibolite facies. The petrography and geochemistry of this
progressively metamorphosed formation were described by Shaw
(1954, 1956). According to their grade of metamorphism, Shaw
(1954) subdivided the rocks into three groups. The low-grade rocks
(mainly lower greenschist facies) include shales and slates. The
medium-grade rocks (predominantly lower amphibolite facies) are
schists which do not contain sillimanite or are not adjacent to
sillimanite-bearing rocks and are usually composedof quartz, mus-
covite, biotite, staurolite and garnet and sometimes feldspars in
subordinate amounts. The high-grade rocks (middle amphibolite
facies) either contain sillimanite or are adjacent to sillimanite-bear-
ing rocks. They are made up of quartz, muscovite, biotite and
sillimanite with subordinate garnet and feldspars. The detailed geo-
chemical study of Shaw (i954, 1956)has shown that the formation
represents an isochemically metamorphosed sequence as far as the
major and several trace elements are concerned.
O010-7999/78/0066/0409/$01.20
410
The second set of samples was collected in the valley of the
river Strona (Valle Strona) in the Western Italian Alps. The exten-
sively studied metamorphic sequence 0f the Valle Strona (Bertolani,
1968; Mehnert, 1975; Rivalenti, 1966; Sighinolfi, 1969) is a part
of the Ivrea Zone and consists of alternating bands of metasedimen-
tary and mafic metaigneous rocks with a well defined metamorphic
gradient ranging from amphibolite to granulite facies. The amphi-
bolite facies section comprises graphite-bearing biotite gneisses and
striped amphibolites. Biotite gneisses are made up of quartz, K-
feldspar, plagioclase and subordinate garnet and sillimanite, while
amphibolites consist predominantly of amphibole and plagioclase.
The granulite facies sequence is also composed of mafic metaig-
neous and metasedimentary ("acid") rocks (Mehnert, 1975). The
"acid" granulites include narrow banded types (stronalites) con-
taining predominantly quartz, plagioclase, perthitic K-feldspar and
garnet and rocks with migmatitic character. Mafic granulites are
composed mainly of pyroxene and plagioclase, sometimes with
garnet and/or amphibole. Mehnert (1975) and Sighinolfi and Gor-
goni (1978) have argued that the amphibolite-granulite sequence
of the Valle Strona was formed by a progressive regional metamor-
phism of the same formations with a relatively uniform pre-meta-
morphic composition. Thus "acid '~ and mafic granulites are prob-
ably the higher metamorphic grade equivalents of biotite gneisses
and amphibolites, respectively.
Granulitic inclusions are from the Neogene basaltic pipe of
Bournac (Velay), Massif Central, France (Leyreloup, 1973, 1974).
The petrography and geochemistry of the inclusions were given
by Leyreloup et al. (1977) who have shown that the rocks have
compositions similar to tholeiitic basalts. Some inclusions represent
medium pressure granulites while others contain high pressure
granulitic assemblages corresponding to a depth of about 25 km
(Leyreloup et al., 1977).
Analytical Methods
K, Rb, Ba, Ti, and Zr were determined by X-ray fluorescence
while the analyses of U were done by a fission track technique
using Lexan detectors and a neutron dose ~ 1017 n/cm 2. Standard
glasses of 0.33 ppm U were used for calibration. The uranium
concentrations were determined from the measured fission track
densities by comparing them in the samples and standards. U
in the whole-rocks was determined in pellets of homogenized sam-
ples according to the method described by Fischer (1970). In each
whole-rock pellet, about 5000 traces were counted. The distribution
and concentration of U in the individual phases were studied on
polished thin section by fission track mapping (Kleeman and Lo-
vering, i967). The precision and accuracy of the data can be judged
from the replicate analyses of the standard rock BCR-1 (Table 1).
The precision of the values for the mineral phases is lower (up
to 40%). Each value for the major rock-forming minerals given
in Table 2 is an average of the determinations of 10-20 grains.
Due to the small size of the grains and the high concentrations,
the precision of U data for accessory minerals is poor, with an
error probably up to 80%.
Results
Whole Rocks
The average Contents o f U a n d o t h e r l i t h o p h i l e ele-
ments in 18 r o c k s f r o m the L i t t l e t o n f o r m a t i o n , subdi-
J. Dostal and S. Capedri: Uranium in Metamorphic Rocks
v i d e d a c c o r d i n g to m e t a m o r p h i c grade into three
g r o u p s (Shaw, 1954), are given in Table 1. The u r a -
n i u m c o n c e n t r a t i o n in the i n d i v i d u a l s a m p l e s varies
b e t w e e n 1.3 a n d 3.2 p p m ( A p p e n d i x 1). The values
are well within the range o f the U a b u n d a n c e s o f
N o r t h A m e r i c a gray a n d green shales ( A d a m s a n d
W e a v e r , 1958) a n d o f recent pelagic sediments f r o m
the Pacific a n d A t l a n t i c oceans (c.f. R o g e r s a n d
A d a m s , 1974). A c o m p a r i s o n o f the three g r o u p s o f
r o c k s with different m e t a m o r p h i c grades (Table 1)
shows t h a t there is no significant c h a n g e in the a b u n -
dances o f U a n d o t h e r a n a l y z e d elements in pelitic
rocks with increase o f the m e t a m o r p h i c g r a d e u p to
the a m p h i b o l i t e facies.
F o u r t y - o n e a m p h i b o l i t e facies r o c k s a n d thirty-
five granulites a n a l y z e d f r o m the Valle S t r o n a include
b o t h m e t a i g n e o u s (mafic) a n d m e t a s e d i m e n t a r y
(" a c i d " ) rocks. The average c o n t e n t o f the a n a l y z e d
e l e m e n t s in the r o c k s f r o m the Valle S t r o n a is given
in T a b l e 1. The average o f U in the m e t a s e d i m e n t a r y
r o c k s o f the a m p h i b o l i t e facies is very similar to t h a t
o f the L i t t l e t o n f o r m a t i o n , a l t h o u g h the i n d i v i d u a l
s a m p l e s have a greater range o f U c o n c e n t r a t i o n s ,
v a r y i n g f r o m 0.92 to 3.4 p p m ( A p p e n d i x 1).
C o m p a r e d to a m p h i b o l i t e facies rocks, the " a c i d "
granulites are d e p l e t e d in U, R b a n d K b y f a c t o r s
o f a b o u t 3, 2.6 a n d 1.5, respectively. The d e p l e t i o n
o f U, R b a n d K in granulites is also a c c o m p a n i e d
by higher K / R b a n d lower R b / B a a n d U / K x 104 ra-
tios. O n the o t h e r h a n d , Z r a p p e a r s to be slightly
e n r i c h e d in granulites c o m p a r e d to a m p h i b o l i t e facies
rocks.
The U c o n t e n t o f mafic rocks o f a m p h i b o l i t e facies
is within the range o f the U a b u n d a n c e s o f a m p h i b o -
lites f r o m the C a n a d i a n shield (Eade a n d F a h r i g ,
1973) a n d f r o m A u s t r a l i a ( L a m b e r t a n d Heier, 1968).
In c o m p a r i s o n with a m p h i b o l i t e s , mafic granulites
are lower in U by a f a c t o r o f a b o u t 2.4 a n d have
a lower U / K x 104 ratio. G r a n u l i t e s also have slightly
lower c o n t e n t s o f K a n d R b a l t h o u g h the difference
is n o t statistically significant. Ti, Zr, a n d Ba do n o t
seem to be affected by the increase o f m e t a m o r p h i s m .
A d e p l e t i o n o f K, Rb, a n d U in granulites similar
to t h a t f r o m the Valle S t r o n a has been r e p o r t e d f r o m
n u m e r o u s high grade m e t a m o r p h i c areas ( L a m b e r t
a n d Heier, 1968; Heier, 1973). The U c o n t e n t o f high
a n d m e d i u m pressure granulitic inclusions f r o m Bour-
nac varies in a n a r r o w r a n g e f r o m 0.07 to 0.12 p p m
( A p p e n d i x 1).
The absence o f a distinct c o r r e l a t i o n o f U with
K, Rb, Ba, Zr, a n d Ti a n d in fact also with all m a j o r
elements (our u n p u b l i s h e d d a t a ) in the a n a l y s e d r o c k -
series indicates t h a t the b u l k o f U does n o t reside
in the m a j o r r o c k - f o r m i n g minerals.
J. Dostal and S. Capedri: U r a n i u m in Metamorphic Rocks 411

Table 1. Average element concentrations and ratios in several suites of metamorphic rocks

n U K Rb Ba Zr Ti U / K x 10* K/Rb Rb/Ba

Littleton LG 7 2.15 3.42 162 550 220 0.56 0.63 211 0.29
(0.40) (0.52) (25) (74) (34) (0.08)
MG 5 2.13 3.59 163 555 222 0.57 0.59 220 0.29
(0.36) (0.59) (37) (184) (18) (0.04)
HG 6 2.24 3.84 170 637 187 0.67 0.58 226 0.27
(0.62) (0.55) (27) (165) (45) (0.06)
Valle Strona mafic AF 18 0.54 0.58 16 166 119 1.14 0.93 363 0.10
(0.20) (0.24) (11) (109) (46) (0.39)
GF 11 0.22 0.45 11 136 107 0.93 0.49 409 0.08
(0.16) (0.25) (9) (91) (49) (0.39)
metasedimentary AF 23 2.29 2.83 131 563 210 0.57 0.81 216 0.23
(0.68) (0.89) (48) (227) (80) (0.18)
OF 24 0.74 1.93 50 551 293 0.72 0.38 386 0.09
(0.36) (1.01) (35) (340) (166) (0.43)
Bournac MP 6 0.10
(0.02)
HP 2 0.11
(0.02)
BCR-1 1.79 1.46 47 648 184 1.33
(0.20) (0.05) (2) (15) (7) (0.02)

K and Ti in wt%, U, Rb, Ba, and Zr in p p m ; n = n u m b e r of samples; values in b r a c k e t s = s t a n d a r d deviation; grade of m e t a m o r p h i s m :

L G = l o w grade (mainly lower greenschist facies), M G = medium grade (lower amphibolite facies), HG=high grade (middle amphibolite
facies), A F = a m p h i b o l i t e facies, G F = g r a n u l i t e facies, M P = m e d i u m pressure granulite facies, H P = high pressure granulite facies

Table 2. U concentrations (in ppb) of individual mineral phases of some metamorphic rocks

No. Rock type plg kf q cpx opx am bi gr s ru ap sph z 22

1 metasedimentary AF 22 15 <5 31 40 > 5000 1870

t metasedimentary AF 17 26 32 7300 I200
1 metasedimentary AF 25 21 <5 42 > 5000 6300 2470
1 metasedimentary AF 21 <5 44 > 5000 1700
1 metasedimentary GF 27 42 > 5000 > 5000 650
1 metasedimentary GF 5 <5 22 7 > 4000 > 4000 552
1 metasedimentary GF 24 3 65 > 5000 > 5000 132
1 metasedimentary GF 22 52 > 5000 > 5000 825
1 mafic AF 28 42 > 5000 360
1 mafic AF 10 26 > 5000 352
1 mafic AF 26 55 67 27 > 5000 213
1 mafic AF 15 50 > 5000 659
1 mafic GF < 10 < 15 > 5000 20
1 mafic GF 7 64 21 > 5000 > 5000 191
l mafic GF 12 30 7500 > 5000 400
l mafic GF 15 26 > 5000 > 5000 205
2 mafic MP 10 33 14 15 30 9300 7600 80
2 mafic MP 11 56 12 16 7200 8800 72
2 mafic MP 8 22 11 6700 116
2 mafic HP 11 16 23 46 4100 119
2 mafic HP 10 11 19 5200 95

No. 1 =Valle Strona, No. 2 = B o u r n a c pipe

AF= amphibolite facies, GF= granulite facies, MP = m e d i u m pressure granu[ite facies, H P = high pressure granulite facies
plg= plagioclase, kJ= K-feldspar, q = q u a r t z , cpx = c~inopyroxene, opx = orthopyroxene, am = a m p h i b o l e , bi=biotite, g r = g a r n e t , s = spinel,
ru=rutile, a p = a p a t i t e , sph=sphene, z = z i r c o n , S = w h o l e - r o c k (determination of the homogenized whole-rock pellets)
412 J. Dostal and S. Capedri: Uranium in Metamorphic Rocks

Minerals Discussion and Conclusions

The abundances of U in the rocks do not appear
to be affected by metamorphism below the granulite
In order to evaluate whether the distribution of U
facies grade. The granulites are, however, depleted in
in the amphibolite facies rocks differs from that of
U in comparison with equivalent rocks of amphibolite
granulites, several rocks of both facies were studied
facies grade. There is also a difference in the distribu-
by fission track mapping. The abundances of U in
tion of U in rocks of these two facies. In rocks of
the mineral phases of some representative metamor-
the amphibolite facies, the bulk of U is located along
phic rocks are given in Table 2 and were determined
the fractures and cleavage planes of ferromagnesian
in clear unfractured crystals. The homogeneous distri-
minerals and in accessory minerals while in granulites,
bution of tracks and the uniformity of the U content
most of the U resides in accessories. Comparable
of individual phases throughout a given sample sug-
rocks of both facies usually contain the same U-rich
gest that these values represent U in solid-solution.
accessory minerals (zircon, apatite, sphene, rutile) and
In amphibolite facies rocks, in general, the major
there are no indications that accessory minerals in
rock-forming minerals have a very low concentration
granulites are more abundant or richer in U than
of U (Table 2) most of which is concentrated along
those of amphibolite facies rocks. This suggests that
the fractures, margins and cleavage planes of mainly
the depletion of U in granulites is mainly due to
ferromagnesian minerals (10-200 times higher in U
an absence or a very low amount of U associated
than minerals) and in accessory minerals (apatite, zir-
with the fractures and cleavage planes of minerals
con, sphene, rutile) with U contents in the order of
in the rocks of this facies.
several ppm (Table 2). In some rocks, opaque min-
The low content of U in granulites is frequently
erals (magnetite-ilmenite) also have a high content
attributed to partial melting (e.g. Fyfe, 1973).
of U. Due to an inhomogneous and highly variable
Anatexis and removal of granitic melt can explain
distribution of U along the fractures and cleavage
the simultaneous depletion of several lithophile ele-
planes, the mass balance calculations for U in these
ments such as K, Rb, Cs and U observed in many
rocks can be at most only approximate. The rough
granulite facies regions. However, some mafic granu-
estimates indicate that about 60 70% of U in metase-
lites of basaltic composition, which probably did not
dimentary rocks of amphibolite grade is located along
undergo partial melting and do not differ in their
the cleavage planes and fractures of biotite and to
K and Rb abundances from equivalent amphibolites,
a lesser degree of garnet. The remaining U resides
are also depleted in U (c.f. Lambert and Heier, 1968).
predominantly in accessory minerals, frequently en-
A possible explanation is that U which is not located
closed in biotite. In amphibolites, the bulk of U is
in accessory minerals or in crystal structures of major
concentrated along the cleavage planes, fractures and
rock-forming minerals is leached and removed by mi-
margins mainly of amphibole (50 60%), and in acces-
grating hydrous fluids perhaps related to dehydration.
sory minerals.
Such a process may also explain the depletion of
The bulk of U in granulite facies rocks is present
U in high grade " a c i d " or "intermediate" metamor-
in accessory minerals (apatite, zircon, sphene, rutile).
phic rocks with " n o r m a l " K/Rb ratios reported from
Compared to amphibolite facies rocks, the amount
some areas (e.g. Kalsbeek, 1976). Furthermore, the
of U along the cleavage planes, fractures and grain
loss of U in granulitic rocks by migrating fluid phases
boundaries is very small or frequently not even detect-
couId be one of the reasons for the availability of
able. The U content of major rock-forming minerals
U during the Preeambrian when many major U depo-
is low (Table 2) and comparable to that of amphibo-
sits are known to have been formed.
lite facies rocks. Table 2 shows that the overall distri-
bution of U in granulitic inclusions from the Bournac Acknowledgements. We thank Drs. D.M. Shaw, C.A.R. Albu-
querque, C.R. Naeser and K.R. Ludwigfor their critical comments
pipe is rather similar to that of granulites from the and Dr. C. Dupuy for providingsamples from Bournac. The study
Valle Strona with the bulk of U residing in accessory was supported by the National Research Council of Canada and
minerals. the Italian Consiglio Nazionale della Ricerche.
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414 J. Dostal and S. Capedri: Uranium in Metamorphic Rocks

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