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Precambrian Research 162 (2008) 540–558

Isotope chemostratigraphy of marbles in northeastern Mozambique:

Apparent depositional ages and tectonostratigraphic implications
V.A. Melezhik a,∗ , B. Bingen a , A.E. Fallick b , I.M. Gorokhov c , A.B. Kuznetsov c , J.S. Sandstad a ,
A. Solli a , T. Bjerkgård a , I. Henderson a , R. Boyd a , D. Jamal d , A. Moniz e
a Geological Survey of Norway, 7491 Trondheim, Norway
b Scottish Universities Environmental Research Centre, East Kilbride, Glasgow G75 0QF, Scotland, United Kingdom
c Institute of Precambrian Geology and Geochronology, nab. Makarova, 2, 199034 St. Petersburg, Russia
d Eduardo Mondlane University, P.O. Box 257, Maputo, Mozambique
e Provincial Directorate for Geology, Lichinga, Niassa Province, Mozambique

Received 20 February 2007; received in revised form 22 October 2007; accepted 10 November 2007

Abstract
Marbles are minor but characteristic components of metasedimentary units within nappes in the Pan-African Mozambique Belt in NE Mozam-
bique. Metasedimentary units remain largely undated, and carbon and strontium isotope stratigraphy of marbles has been used for indirect dating
of the depositional history in this part of the Mozambique Belt. Sixty-nine samples from nine occurrences of dolomite, calcite and magnesite
marbles in the Montepuez, Xixano, Lalamo, Ocua and Nampula metamorphic complexes were analysed for major and trace elements, and a subset
of 39 samples for C, O and Sr isotopes. The least altered ␦13 C values range from −3.5 to +7.1‰ (V-PDB) and 87 Sr/86 Sr ratios from 0.70504 to
0.70671. These values are considered as the best proxy to seawater composition at the time of deposition. The apparent deposition ages, derived
from available seawater evolution curves, range from c. 1250 to c. 660 Ma. An age of 1250–910 Ma is obtained from a tripartite marble unit
in the Montepuez Complex which is exposed in the Montepuez quarries. Five other age-groups are represented by marble units with apparent
depositional ages of 800–750 Ma (Xixano North), 800–660 Ma (Montepuez West), c. 750 Ma (Nampula), c. 740 Ma (Xixano South and Lalamo),
and 740–670 Ma (Montepuez East). The data suggest that: (i) Pan-African nappes in NE Mozambique include Neoproterozoic and probable
Mesoproterozoic sediments; (ii) Neoproterozoic rocks of the Xixano and Nampula complexes might have different ancestry and were tectonically
juxtaposed during the Neoproterozoic Pan-African orogeny.
© 2007 Elsevier B.V. All rights reserved.

Keywords: Mozambique; Marble; Calcite; Dolomite; Magnesite; Carbon; Oxygen; Strontium; Isotopes

1. Introduction
The Mozambique Belt in East Africa was first recognised
by Holmes (1951) who demonstrated a structural discontinuity
between the Tanzanian Craton and metamorphic complexes of
an apparent Mezoproterozoic age to the east. Later studies by
Pinna et al. (1993), Muhongo et al. (2001), Kröner et al. (2003)
and Johnson et al. (2005) have shown a complex history of the
belt, which experienced several tectonometamorphic events that
occurred between 1100 and 500 Ma. In northern Mozambique,
reconstruction of the geological evolution of the Mozambique
∗ Corresponding author. Tel.: +47 73 90 42 41; fax: +47 73 92 16 20.
E-mail address: victor.melezhik@ngu.no (V.A. Melezhik).
Belt is based on very few radiometric dates that constrain the
ages and provenances of the different tectonostratigraphic com-
plexes that constitute the belt. These dates (reviewed by Johnson
et al., 2005), obtained from igneous and metamorphic rocks by
the U–Pb, Sm–Nd and Rb–Sr methods, are rather few, gener-
ally lack high precision, and thus allow various interpretations
of the geological history (Holmes, 1951; Pinna et al., 1993;
Shackleton, 1996; Muhongo et al., 2001; Meert, 2003). More-
over, there is general lack of dates constraining depositional ages
of various supracrustal rocks that constitute the belt. To date,
there has been only one attempt to obtain depositional age from
metasedimentary rocks. The low-grade metalimestones of the
Geci group which was tectonically juxtaposed with granulite-
facies complexes in NW Mozambique, have been constrained to
630–585 Ma by means of isotope chemostratigraphy (Melezhik
et al., 2006).

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doi:10.1016/j.precamres.2007.11.002
 V.A. Melezhik et al. / Precambrian Research 162 (2008) 540–558
Marbles associated with metamorphosed complexes are
minor but consistent components of allochthonous units in the
Mozambique Belt in NE Mozambique, Tanzania and Madagas-
car (Pinna et al., 1993; Muhongo, 1994; De Wit et al., 2001;
Fernandez and Schreurs, 2003). The purpose of this work is to
provide further progress in understanding the geological history
of the region by constraining the depositional age of high-grade
marble formations in NE Mozambique with the tool of Sr and
C isotope chemostratigraphy. Extensive isotopic work in the
Caledonian orogenic belt (Melezhik et al., 2001a, b, 2002a,
b, 2003, 2005; Thomas et al., 2004; Slagstad et al., 2006) has
demonstrated that carbonate chemostratigraphy can be in prin-
cipal applied to high-grade marbles, thus providing the age
constraints necessary for improving reconstructions of the depo-
sitional history and tectonostratigraphic assembly of areas where
it is difficult to use other methods.
2. Geological background
Originally the Mozambique Belt, a high-grade north–south
trending orogenic belt in East Africa, was defined to have
formed as the result of a c. 1300 Ma single orogenic event
(Holmes, 1951). As more radiometric dates were generated, it
became apparent that the belt is the product of at least two oro-
genic cycles. Pinna et al. (1993) recognised high-grade gneisses,
granulites and migmatites comprising a Precambrian basement
which was intruded by orogenic plutonic rocks. These rocks
were emplaced and deformed during the 1100–850 Ma Mozam-
bican orogeny, approximately equivalent to the Mezoproterozoic
Kibaran orogeny of central Africa. A younger cycle involved the
deposition of limestones, phyllites, sandstones and conglom-
erates of marine origin, and some other rocks with possible
glacial affinities. The Geci group metalimestones, belonging to
this cycle, have an apparent depositional age of 630–585 Ma
(Melezhik et al., 2006).
Muhongo et al. (2001) and Kröner et al. (2003) constrained
the peak of high-grade metamorphism in northern Mozam-
bique to c. 615 Ma. Johnson et al. (2005) reviewed the newly
obtained radiometric dates and suggested that previous tectonos-
tratigraphic subdivisions in northern Mozambique should be
considered with caution.
New geological mapping at the 1:250,000 scale was accom-
plished in northern Mozambique between 2003 and 2006 by
the Geological Survey of Norway, the British Geological Sur-
vey and the National Directorate of Geology of Mozambique. It
resulted in acquisition of new petrographic, mineralogical, geo-
chemical, structural and geochronological data (Bingen et al.,
2006a, b, 2007). A simplified version of the new geological map
over northeasternmost Mozambique is presented in Fig. 1. This
map integrates new field, airborne geophysics, structural data
and a substantial database of U–Pb zircon and monazite ages
constraining magmatic and metamorphic events (Bingen et al.,
2006a, b, 2007). The map features a number of lithotectonic
units, designated as complexes. New geochronological data
(Bingen et al., 2006a, b, 2007) combined with results reported
by Kröner et al. (2001, 2003) and Jamal (2005) suggest that
the lithological complexes were metamorphosed, deformed and
541
imbricated during the Neoproterozoic Pan-African orogeny, and
were intruded by several generations of granites; the present-day
tectonostratigraphy in NE Mozambique is the result of several
phases of Pan-African orogenic processes.
Available data provide evidence for a Mesoproterozoic base-
ment, and an overlying Meso- to Neoproterozoic nappe system.
The basement is an integral component of the Nampula, Mar-
rupa and Nairoto complexes, and probably the Meluco Complex.
The basement is mainly made up of felsic orthogneiss with
magmatic crystallisation ages ranging from c. 1150 to 940 Ma
(Bingen et al., 2006a, b, 2007. It is locally unconformably over-
lain by a Neoproterozoic metasedimentary cover (e.g., Mecuburi
group, located SW of the area of Fig. 1). The Pan-African
nappes include the Xixano and Lalamo complexes. They are
mainly Neoproterozoic mafic to intermediate granulites, vari-
ous metasediments, metavolcanic rocks and felsic orthogneiss.
Enderbites, metagranites and metarhyolites yield magmatic
crystallisation ages between c. 820 and 740 Ma. The nappes
carry evidence for a pre- or early-Pan-African granulite-facies
metamorphism dated to 735 ± 5 Ma in the Xixano Complex. The
nappe system probably represents exotic or outboard continen-
tal fragments accreted to the basement during the Pan-African
orogeny. The main Pan-African orogeny took place between
580 and 530 Ma, and included at least two main phases, par-
tially overlapping in time (Bingen et al., 2006a, b, 2007). These
are (i) NW verging imbrication of the basement and transport of
the nappes over the basement, and (ii) folding of the basement
and nappes, especially along a NNE–SSW trend. The Ocua and
Montepuez complexes are partially interpreted as a melange con-
taining tightly folded lithologies belonging to both the basement
and the nappes. Available data provide only limited constraints
on the deposition of sedimentary sequences (e.g., Melezhik et
al., 2006). The present study addresses this problem.
3. Marble formations studied
Amphibolite-faces marbles occur sporadically in most
supracrustal complexes (Fig. 1) where they range in thickness
from less than a meter to hundreds of meters with lateral exten-
sion over 100 km. Those involved in our study are from the
Nampula, Montepuez, Xixano, Lalamo, and Ocua complexes
(Fig. 1). Marbles from the Montepuez Complex are the main tar-
get of the research. They were studied in commercially exploited
quarries near Montepuez (Fig. 1). Excellent man-made expo-
sures provide an opportunity for detailed study and systematic
sampling. The level of exposures of marbles from other com-
plexes allowed only limited sampling.
The present-day lithology of the Montepuez Complex
includes a variety of amphibolite-facies schists, amphibolites,
quartzites, felsic volcanites and several marble units. Marbles
exposed in four small quarries east of Montepuez comprise three
distinctive lenses dipping at 46–60◦ southeast. Their visible
thicknesses range between 20 and 50 m. The lenses are isocli-
nally folded, tectonically dissected, separated by thin slices of
mica schists and apparently represent a tectonically imbricated
unit. Three disparate marble lenses identified in the quarries
are designated as a tripartite marble unit. A structurally lower
542 V.A. Melezhik et al. / Precambrian Research 162 (2008) 540–558

Fig. 1. Schematic geological map of northeastern Mozambique with emphasis on marble formations.

member of the unit is termed as Calcite-dolomite marble, a
structurally upper as White dolomite marble, and a middle as
Grey dolomite marble. The Calcite-dolomite marble is mainly
composed of pale grey, impure, thinly layered and medium
to coarsely crystalline calcite marbles (Fig. 2a). One 1.5 m-
thick bed of bluish, giantly crystalline, massive marble (Fig. 2b)
occurs in the middle part of the lens. The calcite marbles are
structurally overlain by pale grey, medium crystalline, layered,
dolomite marble. The Grey dolomite marble is dominated by
pale grey, medium-crystalline, dolomite marbles with thin lay-
 V.A. Melezhik et al. / Precambrian Research 162 (2008) 540–558 543

Fig. 2. Lithological varieties of some of the studied marbles. Montepuez Complex marbles: (a) Photograph of an inner corner of sawn surfaces in the quarry №
4 (Calcite-dolomite marble member) showing the typical style of tectonic deformation in the grey, banded, calcite marble; (b) photograph of a banding-parallel
surface in the quarry № 4 (Calcite-dolomite marble member) showing the bluish marble composed of giant calcite crystals; coin = 9 mm; (c) photograph of a sawn
surface in the quarry № 1 (White dolomite marble member) showing banded, pale grey, dolomite marble with numerous inclusions of amphibolite structurally
overlain by massive to weakly banded white dolomite marble with banding-parallel inclusions of amphibolite; hammer head = 12 cm. Marbles of other complexes:
(d) Pale pink, massive, medium-crystalline, dolomitised, magnesite marble from the Lalamo Complex; (e) back-scattered electron image of the micro-brecciated and
retrogressively dolomitised (Dol), calcitised (Cc) and serpentinised (Spt) Lalamo magnesite (Mg); (f) weathered surface of depositional carbonate breccia from the
Lalamo Complex; (g) photomicrograph of the Lalamo carbonate breccia showing dark and pale brown fragments cemented by white calcite.
544 V.A. Melezhik et al. / Precambrian Research 162 (2008) 540–558
ers of a dolomitised calcite marble. The White dolomite marble
is distinguished by its white colour and high purity. It con-
tains both dolomite and calcite marbles though the latter are
subordinate. The marbles include roughly equal volumes of mas-
sive and layered varieties and contain sporadic, layer-parallel,
strongly foliated amphibolite inclusions, apparently dissected
and dismembered thin mafic dykes or sills (Fig. 2c).
In the tripartite marble unit at Montepuez, both calcite and
dolomite marbles are composed of crystals arranged in hypid-
iomorphic, allotriomorphic and granoblastic textures. In calcite
marbles, accessory minerals are tremolite, quartz and muscovite,
whereas dolomite marbles additionally contain sizable amounts
of graphite and are commonly devoid of quartz.
Calcite and dolomite marble units occurring in the Mon-
tepuez Complex outside the quarries (termed in this article as
East and West marbles, Fig. 1), as well as most marble units
hosted by other complexes, are very similar to the marbles of
the tripartite unit. They are tectonically dissected bodies asso-
ciated with paragneisses. They are commonly rather pure and
composed of medium-crystalline calcite with variable amount
of dolomite. Impure, dolomitised marbles contain tremolite as
the result of quartz + dolomite metamorphic reaction. The mar-
ble lens sampled in the Ocua Complex is composed of pure
dolomite.
One lens from the Lalamo Complex (JS307, Fig. 1) con-
sists of magnesite and calcite marbles. The lens has a thickness
exceeding 200 m and it is traceable along strike over a distance
of 20 km. It is hosted by amphibolite-facies layered arenites with
layers of biotite gneiss and quartzite. The magnesite marble bed,
of unknown thickness, is composed of a pale pink, medium-
crystalline, massive lithology (Fig. 2d), which microscopically
appears to be brecciated (Fig. 2e). Extensional micro-fractures
are cemented by retrogressive dolomite and calcite, which are
replaced by later chlorite and serpentinite (Fig. 2e). The same
marble lens, though exposed 5 km north of the magnesite bed,
comprises brown, brecciated, and white, massive varieties of a
calcite marble. The former has a visible thickness of over 2 m and
a vuggy appearance on weathered surfaces (Fig. 2f). The breccia
consists of 0.5–5 cm large, red to pale brown, calcite marble frag-
ments cemented by coarsely crystalline white calcite (Fig. 2g).
There is no field evidence suggesting a postdepositional tectonic
brecciation, therefore the breccia is categorised as a collapse
breccia originated either from dissolution of evaporate minerals
or karstification.
4. Geochemistry
4.1. Analytical techniques
Major and trace elements were analysed by X-ray fluores-
cence spectrometry at the Geological Survey of Norway (NGU),
Trondheim, using a Philips PW 1480 X-ray spectrometer. The
precision (1σ) is typically around 2% of the major oxide present.
Acid-soluble Fe, Ca, Mg and Mn were analysed by ICP-AES at
NGU using a Thermo Jarrell Ash ICP 61 instrument. Detec-
tion limits for Fe, Mg, Ca, Mn and Sr are 5, 100, 200, 0.2
and 2 ppm, respectively. The total analytical uncertainty includ-
ing element extraction (1σ) is ±10% rel. Standard analytical
procedures have been used for measurement of total organic
carbon (TOC) at NGU. The TOC content has been measured
from acid-washed material via sealed tube combustion using a
Leco SC-444 instrument with a total analytical uncertainty of
±15% rel.
Oxygen and carbon isotope analyses of whole-rock marble
samples were carried out at the Scottish Universities Environ-
mental Research Centre, Glasgow, using the phosphoric acid
method of McCrea (1950) as modified by Rosenbaum and
Sheppard (1986) for operation at 100 ◦ C. Carbon and oxy-
gen isotope ratios in carbonate constituents of the whole-rock
samples were measured on a VG SIRA 10 mass spectrometer.
Analyses were calibrated against NBS 19, and precision (1σ) for
both isotope ratios is better than ±0.2‰. Oxygen isotope data for
dolomites were corrected using the fractionation factor 1.00913,
and 1.00933 for magnesite recommended by Rosenbaum and
Sheppard (1986). The ␦13 C data are reported in per mil (‰)
relative to V-PDB and the ␦18 O data in ‰ relative to V-SMOW.
Rb–Sr analyses were carried out at the Institute of Precam-
brian Geology and Geochronology of the Russian Academy of
Sciences (St. Petersburg) as specified in Gorokhov et al. (1995).
The Rb and Sr concentrations were determined by isotope dilu-
tion. Rb isotopic composition was measured on a MI 1320 mass
spectrometer. Strontium isotope ratios were measured on the
Thermo-Finnigan Triton thermal ionisation mass spectrometer
in static collection mode. All 87 Sr/86 Sr ratios were normalised to
a 86 Sr/88 Sr of 0.1194, and measurements of the NIST SRM-987
run with every batch averaged 0.710255 ± 8 (2␴mean , n = 11).
During the course of the study, the value obtained for the
87 Sr/86 Sr ratio of the USGS. EN-1 standard was 0.709191 ± 25
(2σ mean , n = 3).
4.2. Major elements
The major and trace element geochemistry of the tripartite
marble unit sampled in four quarries at Montepuez is based
on analyses of 56 samples (Table 1). Calcite (CM), dolomite
(DM) and dolomitised calcite (DCM) marbles have been iden-
tified in all three members of the unit. Both the calcite and
the dolomite marbles are relatively pure rocks. They are almost
devoid of Al2 O, Na2 O and K2 O (Table 1). The DM and DCM
are relatively enriched in SiO2 (up to 18.7 wt%, Fig. 3a). Sev-
eral samples of the DM contain sizable amounts of total organic
carbon (TOC, up to 0.6 wt%). We tentatively suggest a Mg/Ca
ratio of 0.1 as the boundary between the CM and the DCM. A
Mg/Ca ratio of 0.5 sets a lower limit for the DM. The CM is
characterised by variable Mg/Ca ratios ranging between 0.02
and 0.09 (Fig. 3a), whereas dolomitised varieties show ratios
between 0.37 and 0.50 (Table 1). Mg/Ca ratios of the DM range
between 0.51 and 0.63 (average, 0.58 ± 0.03, n = 43), which is
lower than that for stoichiometric dolomite (0.62), thus indicat-
ing incomplete dolomitisation. The DCM does not plot along the
limestone–dolostone mixing line (Fig. 3b) because both Mg and
Ca concentrations are low due to the high SiO2 content (Fig. 3a).
The East and West marbles in Montepuez Complex (Fig. 1)
are both pure calcite marbles with Mg/Ca ratios of 0.01 (Table 1).
Table 1
Chemical composition of Montepuez Complex marbles
Field # Lithology SiO2 (wt%) Al2 O3 (wt%) Na2 O (wt%) K2 O (wt%) TOC (wt%) Mg (wt%) Ca (wt%) Fe (ppm) Mn (ppm) Sr (ppm) Mg/Ca
Montepuez quarry 4, UTM 0497505, 8552297
Calcite-dolomite marble member
White to pale grey calcite marbles, partially dolomitised
Mvm040 Coarsely crystalline, weakly banded – – – – – 3.1 33.1 456 28 160 0.09
Mvm041 Coarsely crystalline, weakly banded 0.40 – – 0.04 – 1.9 34.7 312 18 167 0.05
Mvm042 Giant crystalline, massive – – – – – 0.69 37.0 72 4 116 0.02
Mvm043 Coarsely crystalline, banded – – – – – 2.4 34.3 358 14 135 0.07
Mvm044 Giant and medium-crystalline interbedded – – – – – 1.4 35.7 343 20 140 0.04
Mvm045 Coarsely to medium-crystalline, banded 0.04 0.04 – 0.03 – 2.3 34.3 344 12 145 0.07
BB037 Very coarsely-crystalline, massive – – – – – 2.5 33.4 405 18 132 0.07
Calcite marbles, intensively dolomitised
BB039 Pale brown, medium-crystalline 6.0 2.98 0.11 0.70 – 8.7 19.9 4080 150 83 0.44

V.A. Melezhik et al. / Precambrian Research 162 (2008) 540–558

Grey dolomite marbles
Mvm046 Medium-crystalline, banded 1.3 0.05 – 0.05 – 12.2 20.6 1300 48 58 0.59
Mvm047 Medium-crystalline, banded 0.48 0.02 – 0.03 – 12.4 21.0 1210 52 93 0.59
BB038 Medium-crystalline, banded – – – 0.03 – 12.2 20.8 1530 57 61 0.59
Montepuez quarry 3, UTM 0497650, 8552251
Grey dolomite marble member
Calcite marbles, intensively dolomitised
Mvm052 Grey, banded, medium-crystalline 2.1 – – – – 10.4 22.7 1690 91 83 0.46

Montepuez quarry 3, UTM 0497650, 8552251

Grey dolomite marble member
Dolomite marbles
Mvm051 Grey, medium-crystalline, banded 6.9 – – – 0.37 10.8 20.2 632 23 99 0.53
Mvm048 Grey, medium-crystalline, banded 0.1 – – – 0.13 12.7 20.6 1540 45 71 0.62
Mvm049 Grey, medium-crystalline, banded 3.0 – – – 0.60 12.0 20.4 1090 35 65 0.59
Mvm050 Grey, medium-crystalline, banded 7.5 – – – 0.33 10.9 19.9 798 27 104 0.55
Mvm053 White, medium-crystalline, banded 2.8 – – – – 11.7 21.3 1280 43 102 0.55
Mvm054 Grey, medium-crystalline, banded 7.1 – – – 0.30 10.7 19.3 666 24 76 0.55
Mvm055 Grey, medium-crystalline, banded 3.0 – – – – 12.0 20.5 2220 81 58 0.59
Mvm056 Grey, medium-crystalline, banded 0.82 – – – 0.32 12.7 21.4 1440 43 86 0.59
BB034 White, coarsely crystalline, massive 0.33 – – – 0.17 12.4 20.8 782 33 86 0.60
BB035 Pale grey, medium-crystalline, banded 7.7 – – – 0.26 10.2 19.2 386 16 99 0.53
Montepuez quarry 2, UTM 0497683, 8552084
White dolomite marble member
White calcite marbles, intensively dolomitised
BB031 Medium-crystalline, massive – – – – – 11.3 22.6 298 12 119 0.50

White dolomite marbles

BB029 Medium-crystalline, massive 1.8 – – – – 12.4 20.9 1530 73 83 0.59
BB030 Medium-crystalline, massive 3.6 – – – – 12.3 19.9 395 20 106 0.62
BB032 Medium-crystalline, massive 0.36 – – – – 12.6 20.4 513 19 71 0.62

Montepuez quarry 1, UTM 0497684, 8552072

White dolomite marble member
White calcite marbles, intensively dolomitised
Mvm065 Finely crystalline, massive 17.6 – – – – 6.7 18.0 328 13 82 0.37
Mvm066 Finely crystalline, massive 8.4 – – – – 9.4 20.6 493 24 99 0.46
Mvm074 Finely crystalline, massive 18.7 – – – – 6.4 17.4 736 52 70 0.37
Mvm075 Finely crystalline, massive 0.04 – – – – 11.2 22.9 758 61 112 0.49

545
 546
Table 1 (Continued )
Field # Lithology SiO2 (wt%) Al2 O3 (wt%) Na2 O (wt%) K2 O (wt%) TOC (wt%) Mg (wt%) Ca (wt%) Fe (ppm) Mn (ppm) Sr (ppm) Mg/Ca
White dolomite marbles
Mvm057 Medium-crystalline, massive; amphibolite inclusions 1.5 – – – – 12.6 20.9 1550 73 79 0.60
Mvm058 Medium-crystalline, massive; amphibolite inclusions 0.72 – – – – 12.4 20.7 1130 47 76 0.60
Mvm059 Medium-crystalline, massive; amphibolite inclusions 11.9 – – – – 9.2 18.1 1540 79 72 0.51
Mvm060 Medium-crystalline, massive; amphibolite inclusions 2.2 – – 0.02 – 12.5 20.8 715 36 78 0.60
Mvm062 Medium-crystalline, massive; amphibolite inclusions 3.8 – – – – 11.0 19.9 2740 98 86 0.55

V.A. Melezhik et al. / Precambrian Research 162 (2008) 540–558

Mvm061 Medium-crystalline, massive; amphibolite inclusions – – – – – 12.1 21.8 984 39 108 0.56
Mvm063 Finely crystalline, massive 6.8 – – – – 10.3 19.4 2050 79 88 0.53
Mvm064 Finely crystalline, massive 4.7 – – – – 11.0 20.5 806 40 85 0.54
Mvm067 Finely crystalline, massive 0.73 – – – – 12.1 21.6 1700 49 102 0.56
Mvm068 Finely crystalline, massive 0.08 – – 0.01 – 12.5 20.7 1530 58 80 0.60
Mvm069 Finely crystalline, massive 0.83 – – – – 12.3 21.1 1090 38 89 0.58
Mvm070 Finely crystalline, massive 0.22 – – – – 11.6 21.7 1150 42 108 0.53
Mvm071 Finely crystalline, massive – – – – – 12.4 21.3 447 26 77 0.58
Mvm072 Finely crystalline, massive 0.57 – – – – 12.1 22.1 211 10 98 0.55
Mvm073 Medium-crystalline, massive 0.56 – – – – 12.4 20.5 1570 53 94 0.60
Mvm076 Weakly banded with amphibolite inclusions – – – – – 13.3 21.1 2120 97 65 0.63
Montepuez quarry 1, UTM 0497684, 8552072
White dolomite marble member
White dolomite marbles
Mvm077 Medium-crystalline, massive – – – – 0.10 13.0 21.2 2360 69 89 0.61
Mvm078 Medium-crystalline, massive – – – – – 12.9 20.9 2290 72 86 0.62
Mvm079 Medium-crystalline, massive 0.23 – – – – 12.8 20.7 1100 48 91 0.62
Mvm080 Medium-crystalline, massive – – – – – 13.1 21.0 1180 54 84 0.62
Mvm082 Medium-crystalline, massive 1.8 – – – – 12.5 20.6 863 36 83 0.61
Mvm081 Medium-crystalline, massive 0.52 – – – – 12.2 21.6 507 26 90 0.56
Mvm083 Medium-crystalline, massive 2.1 – – – – 11.3 21.2 2160 70 92 0.53
Mvm084 Medium-crystalline, massive 4.4 – – – – 11.6 20.0 522 20 61 0.58
BB040 Medium-crystalline, massive 4.7 – – – – 11.1 20.1 976 55 121 0.55
BB041 Medium-crystalline, massive – – – – – 12.5 20.5 1210 84 96 0.61
BB042 Medium-crystalline, massive – – – – – 12.5 20.9 829 36 81 0.60
Marbles sampled outside the quarries
Calcite marbles
BB022 White, coarsely-crystalline – – – 0.01 0.17 0.34 37.2 155 17 4120 0.01
TBM-143A Pale grey, medium-crystalline 1.8 0.14 – 0.040 n.d. 0.38 37.2 715 41 1070 0.01
(–) Below detection limits: 0.01 wt% for K2 O; 0.1 wt.% for SiO2 , Al2 O3 , Na2 O and Corg . Mg, Ca, Fe, Mn, and Sr are acid soluble constituents determined by ICP–AES.
 V.A. Melezhik et al. / Precambrian Research 162 (2008) 540–558 547

Fig. 3. Cross-plots illustrating major geochemical and isotopic features of the tripartite marble unit of the Montepuez Complex.

Marbles of the Xixano and Nampula complexes commonly
contain a few percent of SiO2 and show variable degrees of
dolomitisation (Table 2). Some varieties contain sizable amounts
of Al2 O3 and TOC. The marble of the Ocua Complex is devoid
of SiO2 and Al2 O3 and is dolomitic in composition. The Lalamo
Complex contains numerous lenses of a relatively pure cal-
cite marble containing 0.6 to 6% SiO2 . The magnesite marble
(Mg/Ca = 1.1) has a low SiO2 content (1.8%) and is devoid of
Al2 O3 .
transitional position between the two end-members (Table 1).
The Mn and Fe concentrations in the Montepuez West and
East calcite marbles are 14–41 ppm and 155–755 ppm, respec-
tively. The dolomite and calcite marbles of the Nampula and
Ocua complexes are enriched in Mn (Table 2) relative to those
in the Montepuez Complex. The Xixano and Lalamo calcite
marbles are rather similar to the Montepuez Complex marbles.
The Lalamo magnesite marble has low Mn (23 ppm) and Fe
(250 ppm) concentrations.

4.3. Iron and manganese 4.4. Strontium

In the tripartite marble unit at Montepuez, average Mn
(47 ± 23 ppm, n = 43) and Fe (1208 ± 623 ppm) contents of
the DM are much lower than those commonly reported from
Proterozoic dolostones (Mn = 180 ppm, Fe = 2020 ppm, e.g.,
Melezhik et al., 2005). The CM contains less Mn (16 ± 7.3 ppm,
n = 7) and Fe (327 ± 122 ppm), whereas the DCM occupies a
In the tripartite marble unit at Montepuez, the Sr concen-
tration in the CM is low (142 ± 17 ppm, n = 7) and shows no
significant correlation with the Mg/Ca ratio (Fig. 3c). Con-
centrations of Sr and Mn are both low, and so is the Mn/Sr
ratio (0.11 ± 0.04, n = 7). The DCM and DM contain less Sr
(88 ± 15 ppm, n = 6; 86 ± 15 ppm, n = 43, respectively), with
 548
Table 2
Chemical composition of marbles from from Xixano, Lalamo, Ocua and Nampula complexes in NE Mozambique
Sample # Lithology SiO2 (%) Al2 O3 (%) Na2 O (%) K2 O (%) TOC (%) Mg (%) Ca (%) Fe (ppm) Mn (ppm) Sr (ppm) Mg/Ca

Xixano Complex
Calcite marble
IH04.027 Pale grey, medium-crystalline 1.2 0.29 – 0.04 – 0.40 36.2 798 81 1140 0.01

V.A. Melezhik et al. / Precambrian Research 162 (2008) 540–558

Calcite, partially dolomitised marbles
JS285 Impure, tremolite-bearing 7.6 – – 0.038 n.d. 2.7 29.4 236 117 58 0.09
JS299 Impure, tremolite-bearing 14.3 – – 0.013 n.d. 4.0 22.5 225 65 70 0.18
Calcite, intensively dolomitised marble
TBM126 Pale grey, medium-crystalline 2.2 – – 0.015 n.d. 10.2 22.9 373 18 88 0.45
Lalamo Complex
Calcite marble
JS200 Marble 0.57 0.05 – 0.03 0.41 0.22 36.8 36.4 15 2160 0.01
Calcite, partially dolomitised marble
JS303 Impure, tremolite-bearing 6.1 – – 0.037 n.d. 1.1 33.7 63.3 14 n.d. 0.03
Magnesite marble
JS307 Pink, brecciated, dolomitised 1.8 – – – n.d. 10.5 9.9 249 23 235 1.06
Ocua Complex
Dolomite marble
JS330 Grey, medium-crystalline – – – 0.003 n.d. 12.1 21.3 331 150 139 0.57
Nampula Complex
Calcite, partially dolomitised marbles
TBM097 Grey, medium-crystalline – – – – 0.36 3.78 31.9 736 271 234 0.12
TBM098 Pale grey, medium-crystalline 1.5 0.21 – 0.17 – 1.53 34.0 1030 187 239 0.05
RB823 Impure, tremolite-bearing 5.3 1.04 – 0.39 n.d. n.d. n.d. n.d. n.d. n.d. n.d.
Calcite, intensively dolomitised marbles
TBM-099 Impure, tremolite-bearing 7.9 1.24 0.19 0.19 – 6.07 22.4 1590 230 347 0.27
TBM-105 Pale grey, medium-crystalline 1.3 – – 0.02 0.34 8.65 24.3 792 186 189 0.36
AS04-26 Pale grey, medium-crystalline 2.1 0.09 – 0.01 0.33 6.62 26.3 321 201 163 0.25

(–) Below detection limits of 0.002 for MnO, 0.003 for K2 O, 0.004 for TiO2 , 0.01 for SiO2 , Al2 O3 , Stot, P2 O5 , 0.1 for Na2 O and TOC.
 V.A. Melezhik et al. / Precambrian Research 162 (2008) 540–558
maximum concentrations of 112 and 121 ppm, thus approaching
only the lowest concentration in the CM (Fig. 3c). The aver-
age Sr concentration of the DM is higher than that reported for
non-metamorphosed Proterozoic dolostones (54 ppm, n = 344;
Melezhik et al., 2005). Mn/Sr ratios range between 0.1 and 1.5
averaging 0.58 ± 0.33 (n = 43). In contrast, the Montepuez West
and East calcite marbles are rich in Sr (1070 and 4120 ppm,
respectively). The dolomitised calcite and dolomite marbles of
other complexes are characterised by moderate to low Sr con-
centrations. However, pure calcite marbles of the Xixano and
Lalamo complexes contain 1140 and 2160 ppm Sr, respectively
(Table 2). The Lalamo magnesite has a low Sr content (235 ppm).
4.5. Oxygen and carbon isotopes
Carbon and oxygen isotope data from the tripartite marble
unit at Montepuez comprise 24 analyses (Table 3). The δ18 O
values of the CM range between 14.6 and 20.3‰ (17.2‰ on
average, n = 7). The δ13 C values are all positive and cluster
tightly between +1.6 and +2.1‰ (+1.9 ± 0.2‰ on average)
(Table 3). There is a very weak positive correlation between
δ18 O and δ13 C (r = +0.53, n = 7, >80%). The DM is enriched in
18 O with respect to the CM (Fig. 3d) with δ18 O values tightly
clustering around 22.1 ± 0.4‰ (n = 12). δ13 C fluctuates between
−1.7 and +1.8‰ (Fig. 3e), and low values are associated with
high TOC content (Fig. 3f); all the samples with negative δ13 C
values contain graphite. There is no correlation between δ18 O
and δ13 C. The DCM shows both δ13 C (0.4–1.7‰) and δ18 O
(19.3–22.6‰) transitional from the CM to the DM.
The sample obtained from the Montepuez West calcite marble
is characterised by δ13 C (+0.1‰) and δ18 O (16.7‰), which are
within the range of the tripartite marble unit. In contrast, the
Montepuez East calcite marble shows much higher values for
both δ13 C (+4.7‰) and δ18 O (24.7‰).
The Xixano calcite marbles have δ13 C values fluctuating
between −1.1 and +3.8‰, whereas δ18 O ranges from 15.1 to
22‰ (Table 4). The Lalamo calcite marbles are characterised by
the highest δ13 C (+3.5 to +7.1‰) and δ18 O (26.1–28.4‰) val-
ues. Similarly, the magnesite marble has a high δ18 O (24.3‰)
whereas δ13 C is negative (−1.1‰). The Nampula calcite mar-
bles are uniformly depleted in 13 C (δ13 C = −3.5 to −2.0‰) and
have δ18 O in the range of 18.6–20.8‰.
4.6. Strontium isotope ratios
In the tripartite marble unit at Montepuez, strontium iso-
tope ratios have been obtained from 23 samples (Table 3).
87 Sr/86 Sr ratios measured from the CM range between 0.70508
and 0.70521 (n = 7), whereas those obtained from the DCM are
more radiogenic and fluctuate between 0.70531 and 0.70560
(n = 4). The DM has the most radiogenic 87 Sr/86 Sr ratios ranging
from 0.70540 to 0.70565 (n = 12) (Fig. 3h) with one outstanding
outlier at 0.70488. The 87 Sr/86 Sr ratios of the CM show a sig-
nificant negative correlation with the Sr concentration (Fig. 3g)
(r = −0.66, n = 7, 90%) and do not exhibit a correlation with the
Mg/Ca ratio.
549
The Montepuez West marble has a 87 Sr/86 Sr ratio of 0.70566,
which is more radiogenic than the calcite marbles in the tripartite
unit. The Montepuez East calcite marble has 87 Sr/86 Sr ratio of
0.70654, which is the most radiogenic of all in the Montepuez
Complex.
Among marbles of other complexes, the Xixano calcite
marbles show the greatest spread in 87 Sr/86 Sr ratios (0.70574
to 0.70666), with no dependence on the Sr concentration. In
contrast, 87 Sr/86 Sr ratios of the Lalamo calcite marbles corre-
late negatively with the Sr concentrations within the range of
0.70627–70699 (Table 4). The magnesite has the most radio-
genic value of 0.70699.
5. Geochemical screening for postdepositional resetting
of C-, O- and Sr-isotope systems
In general, the carbon isotopes are strongly buffered by the
high C concentrations in carbonate minerals relative to fluids
(Banner and Hanson, 1990; Jacobsen and Kaufman, 1999) and,
consequently, infiltration of externally derived fluids is likely
to have a relatively greater effect on O and Sr isotopes. Tra-
ditional screening procedures for postdepositional alteration of
carbonate, originally specified for non-metamorphosed or low-
grade rocks (Brand and Veizer, 1980; Veizer, 1983; Banner
and Hanson, 1990; Denison et al., 1998, 1994; Kaufman and
Knoll, 1995; Azmy et al., 1998; Jacobsen and Kaufman, 1999),
are of very limited use in the case studied here. In high-grade
metamorphic rocks, such screening could only detect the latest
geochemical alteration. For these reasons, the discrimination
technique has been based essentially on geochemical criteria,
namely on relative abundances of Mn, Rb and Sr (e.g. Brand
and Veizer, 1980). Elemental ratios, such as Mn/Sr, Fe/Sr, Ca/Sr
and Rb/Sr, as well as δ18 O values, are widely used as geo-
chemical criteria for detecting the least disturbed C-, O- and
Rb-Sr systems. Very variable values and dissimilar combina-
tions of the ratios have been used in the past (Asmerom et al.,
1991; Derry et al., 1992; Kaufman et al., 1993; Gorokhov et
al., 1995; Semikhatov et al., 2002; Kuznetsov et al., 2003). In
all cases, the choice is empirical and to some extent arbitrary.
The published data on non-metamorphosed limestones suggest
Mn/Sr = 0.065–0.02 and Mg/Ca < 0.02, whereas a significant
database obtained from high-grade calcite marbles (Melezhik
et al., 2003) suggests Mn/Sr < 0.02, Mg/Ca < 0.02. However,
such values have been chosen empirically during intensive stud-
ies in the Scandinavian Caledonides. The values may well be
different in cases where the rocks experienced a different geo-
logical history, and should therefore be used with caution. For
instance, Pili et al. (1997a, b) performed isotopic studies on mar-
bles from a large-scale granulite section in Madagascar, from
geological environments which are rather similar to those in
the study area. They reported that marbles from major shear
zones are depleted in 13 C down to −3‰ due to exchange with
mantle-derived carbon. Marbles from minor shear zones may
show significant isotopic variations at the metre scale reflect-
ing the heterogeneous distribution of fluid flow associated with
variable permeabilities. However, even granulite-grade marbles
 550
Table 3
Minerals in insoluble residue, Rb and Sr concentrations and isotopic ratios of marbles from the Montepuez Complex

Sample # Minerals in insoluble residue Mg/Ca Mn/Sr δ13 C (‰) δ18 O (‰) Rb (ppm) Sr (ppm) 87 Rb/86 Sr 87 Sr/86 Sr (measured) 87 Sr/86 Sr (initial)a

Montepuez quarry 4, UTM 0497505, 8552297

Calcite-dolomite marble member
Calcite marbles, partially dolomitised
Mvm040 – 0.09 0.17 +2.0 17.9 0.12 170 0.0021 0.70510 0.70507
Mvm041 Mu, Am (Qu, Tlc) 0.05 0.11 +1.7 18.9 0.14 169 0.0024 0.70516 0.70512
Mvm042 – 0.02 0.04 +2.1 20.3 0.13 123 0.0031 0.70521 0.70516
Mvm043 – 0.07 0.10 +2.0 16.8 0.11 144 0.0022 0.70514 0.70511
Mvm044 – 0.04 0.15 +1.6 14.6 0.12 150 0.0023 0.70508 0.70504
Mvm045 (Mu) 0.07 0.08 +1.9 15.1 0.13 145 0.0026 0.70518 0.70514
BB037 – 0.07 0.13 +1.8 16.6 0.09 128 0.0021 0.70520 0.70517
Montepuez quarry 3, UTM 0497650, 8552251

V.A. Melezhik et al. / Precambrian Research 162 (2008) 540–558

Grey dolomite marble member
Calcite marble, intensively dolomitised
Mvm052 Am, Qu 0.46 1.09 +0.4 19.3 0.18 83 0.0063 0.70531 0.70521
Dolomite marbles
Mvm051 Am, Qu 0.53 0.23 −1.5 22.7 0.22 122 0.0053 0.70565 0.70557
Mvm050 Am, Qu 0.55 0.26 −1.7 21.7 0.09 110 0.0024 0.70561 0.70557
Mvm053 Am (Tlc) 0.55 0.42 +1.4 22.4 0.12 106 0.0033 0.70546 0.70541
Mvm054 Am 0.55 0.32 −1.6 22.0 0.12 78 0.0045 0.70553 0.70546
Mvm056 – 0.59 0.50 −0.4 22.7 0.14 85 0.0048 0.70555 0.70547
Montepuez quarry 2, UTM 0497683, 8552084
White dolomite marble member
Calcite marble, intensively dolomitised
BB031 – 0.50 0.097 +1.8 22.0 0.07 124 0.0017 0.70540 0.70537
Montepuez quarry 1, UTM 0497684, 8552072
White dolomite marble member
Calcite marble, intensively dolomitised
Mvm065 Am 0.37 0.16 +1.3 22.2 0.14 80 0.0051 0.70561 0.70553
Mvm066 Am 0.46 0.24 +1.5 22.6 0.1 99 0.0030 0.70560 0.70555
Mvm075 Am 0.55 0.55 +1.7 21.4 0.08 116 0.0020 0.70551 0.70548
Dolomite marbles
Mvm061 – 0.56 0.36 +0.7 19.5 0.11 108 0.0030 0.70488 0.70483
Mvm064 Am 0.54 0.47 +1.6 22.6 0.09 92 0.0029 0.70565 0.70560
Mvm067 Am (Tlc) 0.56 0.48 +1.4 22.0 0.09 104 0.0025 0.70548 0.70544
Mvm070 – 0.53 0.38 +1.7 22.2 0.09 113 0.0023 0.70556 0.70552
Mvm071 Qu 0.58 0.34 +1.8 21.8 0.07 82 0.0025 0.70562 0.70558
Mvm072 Am 0.55 0.11 +1.8 21.2 0.08 102 0.0023 0.70552 0.70548
Mvm081 Tlc, Am, Qu 0.56 0.29 +1.3 21.7 0.06 92 0.0019 0.70556 0.70553
Marbles sampled outside the quarries
Calcite marbles
BB022 – 0.01 0.004 +0.1 16.7 0.23 4125 0.0002 0.70566 0.70566
TBM143A Qu, Fsp 0.01 0.04 +4.7 24.7 1.31 1040 0.0037 0.70654
a For marbles sampled in quarries, the initial strontium ratio was calculated under the assumption that the age of these rocks is equal to 1200 Ma; for other samples—equal to 750 Ma. Abbreviations: Am –

amphibole; Fsp – feldspar; Mu – muscovite; Qu – quartz; Tlc – talc. Rb and Sr concentrations were determined by standard isotope dilution and solid-source mass spectrometry.
Table 4
Minerals in insoluble residue, Rb and Sr concentrations and isotopic ratios of marbles from Xixano, Lalamo, Ocua and Nampula complexes in NE Mozambique

Sample # Minerals in insoluble residue Mg/Ca Mn/Sr δ13 C ‰ δ18 O Rb Sr 87 Rb/86 Sr 87 Sr/86 Sr (measured) 87 Sr/86 Sr (initial)a

Xixano Complex
Calcite marble

V.A. Melezhik et al. / Precambrian Research 162 (2008) 540–558

IH04.027 (Mu) 0.01 0.07 −1.1 15.1 0.25 1190 0.0006 0.70616 0.70615
Calcite, partially dolomitised marbles
JS285 Am, Mu 0.09 2.0 +2.4 22.0 0.25 60.6 0.0121 0.70666 0.70653
JS299 Px 0.18 0.9 −0.2 19.0 0.29 73.5 0.0116 0.70574 0.70562
Calcite, intensively dolomitised marble
TBM-126 Am (Tlc, Qu, Mu) 0.45 0.2 +3.8 19.0 0.49 82 0.0175 0.70631 0.70612
Lalamo Complex
Calcite marble
JS200 Grph, Am, Mu, Fsp 0.01 0.007 +7.1 26.1 0.12 2105 0.0002 0.70671 0.70671
Calcite, partially dolomitised marble
JS303 Qu, Am, Px 0.03 n.d. +3.5 28.4 0.73 3930 0.0005 0.70627 0.70626
Ocua Complex
Dolomite marble
JS330 – 0.57 1.1 +0.4 23.1 0.22 130 0.005 0.70684 0.70679
Nampula Complex
Calcite, partially dolomitised marbles
TBM-097 – 0.12 1.16 −3.5 19.6 0.04 229 0.0005 0.70594 0.70593
TBM-098 n.d. 0.05 0.78 −2.0 19.9 n.d. n.d. n.d. n.d. n.d.
Calcite, intensively dolomitised marbles
TBM-099 n.d. 0.27 0.66 −2.8 18.6 n.d. n.d. n.d. n.d. n.d.
TBM-105 n.d. 0.36 0.98 −2.9 20.8 n.d. n.d. n.d. n.d. n.d.
AS04-26 n.d. 0.25 1.23 −2.9 20.1 n.d. n.d. n.d. n.d. n.d.
a The initial strontium ratio was calculated under the assumption that the age of these rocks is equal to 750 Ma. Abbreviations: Am – amphibole; Fsp – feldspar; Grph- graphite; Mu – muscovite; Px – pyroxene;

Qu – quartz; Tlc – talc. Rb and Sr concentrations were determined by standard isotope dilution and solid-source mass spectrometry.

551
552 V.A. Melezhik et al. / Precambrian Research 162 (2008) 540–558
outside shear zones have carbon and oxygen isotopic composi-
tions similar to their protoliths (Pili et al., 1997a, b).
5.1. Montepuez Complex marbles
The Montepuez CM from the tripartite unit shows significant
fluctuations in δ18 O and a weak positive correlation between
δ18 O and δ13 C, which are indicative of postdepositional reset-
ting. Based on the observed alteration trends (Fig. 3e, d and f),
we tentatively suggest that +2‰ and 20‰ represent the least-
altered δ13 C and δ18 O values, respectively. In the DM, low δ13 C
is associated with high TOC content (Fig. 3f), and such an
effect can be attributed to a local isotopic exchange between
organic matter/graphite and dolomite. There is no correlation
between δ18 O and δ13 C, and the overall δ18 O values show an
overlap with those reported from non-metamorphosed, Protero-
zoic dolostones (e.g., Melezhik et al., 2005). This may suggest
a high degree of preservation of original δ18 O values in the DM.
The observed alteration trend (Fig. 3d and f) suggests +1.8‰
and 22‰ as the best proxies for initial ␦13 C and ␦18 O values,
respectively.
In the tripartite unit, the 18 O depletion of the CM relative
to the DM can be attributed to a sequence of events. The par-
tial dolomitisation of limestones commonly creates enhanced
porosity and permeability, whereas intensively and completely
dolomitised rocks become largely impermeable. As the result,
the partially dolomitised rocks should be more sensitive towards
exchange of their oxygen isotopes with infiltrating postdeposi-
tional fluids, whereas the δ13 C would be sufficiently buffered by
the dissolving calcite precursor (cf. Banner and Hanson, 1990;
Land, 1992). Because diagenetic and metamorphic alterations
affect carbonate material in a similar way (Nabelek, 1991), we
are not in a position to distinguish between the two.
In the tripartite marble unit, the strontium isotope ratios of
the CM are less radiogenic than DCM, and both have less
radiogenic ratios in comparison with the DM (excluding one
outlier, Fig. 3h). Such features can be reconciled if the dolomite
exchanged Sr with dolomitising fluids. This inference is in
agreement with the relative enrichment of the dolomite in 18 O.
However, significant negative correlation between 87 Sr/86 Sr
ratios and the Sr concentration in the CM (Fig. 3g), and the
absence of 87 Sr/86 Sr correlation with the Mg/Ca ratio, sug-
gest that the CM were affected by an additional episode of
postdepositional alteration, which was not associated with the
dolomitisation. Based on the reasoning outlined above and con-
sidering all observed alteration trends (Fig. 3g and h), the least
radiogenic 87 Sr/86 Sr ratio of 0.70508 is tentatively suggested as
the least altered value for the CM. However, the relatively low
Sr concentration in the CM was probably not sufficient to pro-
vide a strong buffer for the Sr isotope system against multiple
alterations, although this is currently impossible to quantify.
Table 5
Chemical composition and strontium isotope ratio of amphibolite boudin in marbles from the Montepuez quarry
Sample # SiO2 (%) Al2 O3 (%) Fe2 O3 (%) TiO2 (%) MgO (%)
BB036 40.7 15.9 15.6 3.63 6.37
Sample Mvm061 of the dolomite marble, the outlier, yielded
an exceptionally low 87 Sr/86 Sr ratio of 0.70488. This is coupled
with depletion in 18 O, and therefore, has no obvious explanation
in terms of preservation potential. The sample was obtained from
the unit containing abundant dismembered amphibolite bod-
ies. The amphibolite occurring in the quarries is characterised
by a low 87 Sr/86 Sr ratio (0.70403). The amphibolite contains
320 ppm Sr (Table 5), which is three times higher than in the
dolomite marbles. Thus, the most probable explanation for the
low 87 Sr/86 Sr in the outlier is an isotopic exchange between the
amphibolite and the dolomite. The low ␦18 O value is consistent
with this model.
The Montepuez West marble shows similarities to those
studied in the quarries, whereas the Montepuez East marble is
distinctly different in that its δ13 C (+4.7‰) and δ18 O (24.7‰)
values are enriched in heavy isotopes. These enriched values plot
outside any alteration trends associated with the tripartite marble
unit and therefore cannot be explained as the result of a higher
degree of preservation. We tentatively suggest that the calcite
was precipitated from seawater with different C- and O-isotopic
composition.
The Montepuez West and East calcite marbles are distin-
guished by higher 87 Sr/86 Sr ratios (Table 3). Because these
rocks have Sr concentrations (1040–4125 ppm) one order
of magnitude higher than that of the CM in the tripar-
tite unit, their more radiogenic strontium isotope ratios are
very unlikely to be attributable to postdepositional alterations.
Instead, they apparently represent marbles whose carbonate
precursor was originally precipitated from seawater with a dif-
ferent isotopic composition. This is particularly true for the
Montepuez East 13 C-rich marble. As far as the Montepuez
West marble is concerned, it was certainly derived from an
aragonite precursor as indicated by the very high Sr abun-
dance. This suggests that the latter may represent not only
a different age but also that it may signify a different depo-
sitional setting or a different postdepositional geochemical
history.
5.2. Marbles of other complexes
A limited database on marbles (Table 4) sporadically occur-
ring in several other complexes (Fig. 1) does not allow for robust
screening against postdepositional resetting of C, O and Rb/Sr
isotope systems. However, several samples are characterised by
exceptionally high Sr concentrations, which should provide a
sufficient buffer against postdepostional resetting. Such sam-
ples can be considered as retaining 87 Sr/86 Sr ratios close to
depositional values. In the Xixano Complex, this applies to
the South marble lens (IH04.027, Fig. 1) having 1190 ppm Sr
and 87 Sr/86 Sr of 0.70616. Interestingly, the Xixano North mar-
ble (JS299, Fig. 1), has a significantly lower Sr concentration
CaO (%) Na2 O (%) K2 O (%) Rb (ppm) Sr (ppm) 87 Rb/86 Sr 87 Sr/86 Sr
11.2 2.41 0.16 1.18 320 0.0118 0.70403
 V.A. Melezhik et al. / Precambrian Research 162 (2008) 540–558
Fig. 4. Temporal trends of 87 Sr/86 Sr and ␦13 C in seawater and apparent deposi-
tional ages of the studied marbles from NE Mozambique. The 87 Sr/86 Sr reference
curve (green) is based on Melezhik et al. (2001 and references therein) and
Kuznetsov et al. (2003 and references therein) (red symbols) modified by using
data from Kuznetsov et al. (2005, 2006) and the database compiled by Shields
553
(73 ppm) combined with the lower 87 Sr/86 Sr ratio of 0.70574,
which cannot be attributed to a postdepositional resetting.
Two samples, representing different marble units in the
Lalamo Complex, namely the Centre and South marbles (Fig. 1),
yielded very high Sr concentrations (3939 and 2102 ppm), but
however have different 87 Sr/86 Sr ratios (Table 4). Because of
strong buffering abilities against postdepositional alterations,
both ratios are probably very close to depositional values; thus
calcite in these two marbles was very likely precipitated from
isotopically different seawaters.
The Nampula marbles have negative δ13 C values, which dis-
tinguish them from other marbles in the study area. The δ13 C
values show a very limited spread, implying that they may reflect
the isotopic composition of seawater. Importantly, despite a low
Sr concentration, the 87 Sr/86 Sr ratio (0.70594) is much lower in
comparison to the Sr isotope ratios of the Sr-rich Lalamo and
Xixano marbles. This again suggests that the Nampula carbon-
ates reflect the isotopic composition of a different seawater.
6. Implications for isotope chemostratigraphy
Strontium isotope stratigraphy has the potential to pro-
vide indirect dating of Neoproterozoic sedimentary carbonates
because of the gradual, though irregular, increase in 87 Sr/86 Sr
from c. 850 to c. 550 Ma (Fig. 4); and also because Sr has a
long residence time relative to seawater, resulting in a uniform
87 Sr/86 Sr ratio in seawater at any given time (Veizer et al., 1999).
However, sampling of carbonate sequences through Neopro-
terozoic time remains incomplete and precise radiometric ages
are not always available. Because of this, there have been sev-
eral disagreements among investigators as to how to construct
the seawater reference curve (see discussion in Melezhik et al.,
2001b and Kuznetsov et al., 2003, 2005). The result of the dis-
cussion was the reference curve (Fig. 4) which has been used in
this study.
In the case of high-grade metamorphic rocks, when the Sr
concentration in carbonates is low, the Rb/Sr system might have
been reset while the carbon isotope system may still retain
the original ratio. This is because the sediment/water ratios
of diagenetic-metamorphic systems (cf. Banner and Hanson,
1990) are about 101 , 102 –103 and 104 for oxygen, strontium
and carbon, respectively (cf. Land, 1992). Therefore, although
the strontium isotope ratios of carbonates are a better proxy for
seawater isotopic composition, δ13 C may provide a better result
for low-Sr marbles.
The apparent depositional ages of the studied rocks have
been constrained by projection of the ‘least altered’ isotopic
values obtained from the marble formations onto the δ13 C and
the 87 Sr/86 Sr seawater reference curves. The time when both
the δ13 C and the 87 Sr/86 Sr intercepts are in agreement has been
considered to represent an apparent depositional age (Fig. 4).
and Veizer (2002 and references therein) (green symbols). The least altered
87 Sr/86 Sr δ13 C ratios of the marble units are shown by horizontal lines. Vertical,
arrowed-head lines indicate apparent depositional ages (see discussion in the
text).
554 V.A. Melezhik et al. / Precambrian Research 162 (2008) 540–558
6.1. The Montepuez Complex marbles
The upper age limit for sedimentation within the Montepuez
Complex can be constrained by the penetrative 580–530 Ma
high-grade metamorphism (e.g., Bingen et al., 2006a, b, 2007).
However, the lower age limit cannot be constrained by any,
currently available, published data. Thus, within limitations of
‘isotope stratigraphy’, one should initially consider a wide time
interval from the Archaean up to 580 Ma. Within this time span,
the least altered initial ratio 87 Sr/86 Sr of 0.70504 projected onto
the seawater curve sets the apparent depositional age of the tri-
partite marble as Mesoproterozoic at around c. 1250 Ma (Fig. 4).
The global carbon isotope records offer additional con-
straints. Kah et al. (1999) reported that δ13 C values of −1.0
to +4.0‰ are characteristic for the interval between approxi-
mately 1300 and 800 Ma. This pattern is distinct from that of
older Mesoproterozoic successions, which record values near
0‰, and suggests that the 1300–800 Ma moderately positive
values may be useful for broad time correlation. In the late
Palaeoproterozoic (1800–1500 Ma) the secular δ13 C curve is
flat, relatively monotonous and fluctuates close to zero much like
that seen in the Mesoproterozoic (Lindsay and Brasier, 2002).
Thus, considering all limitations, ages older than 1300 Ma are
not credible, as the Montepuez carbonates have slightly elevated
δ13 C values fluctuating between +1.6 and +2.0‰, thus distinct
from those close to zero. Moreover, Palaeoproterozoic carbon-
ates are characterised by a much lower 87 Sr/86 Sr (Shields and
Veizer, 2002).
The currently available Sr-isotope database includes a rather
limited number of analyses involved in the constructed reference
curve. Therefore, there is chance for more fluctuations than it is
shown in Fig. 4, however, combined Sr- and C-isotope data sug-
gest that an apparent depositional age cannot be younger than
910 Ma. The relatively low Sr concentrations in the Montepuez
marbles might not have provided sufficient buffer against post-
depositional resetting of the Sr isotope system. Consequently,
the apparent depositional age interval of 1250–910 Ma should
be considered as a minimum age.
The 87 Sr/86 Sr (0.70566) and δ13 C (+0.1‰) values obtained
the Montepuez West marble, when projected onto the seawa-
ter curve, give several interceptions; however, both ratios agree
at 800, 750 and 660 Ma, which can be considered as apparent
depositional ages. The Montepuez East marble has 87 Sr/86 Sr of
0.70654. This, combined with δ13 C of +4.7‰, corresponds to a
740 or 700–660 Ma seawater (Fig. 4).
6.2. Marbles of other complexes
In the Xixano Complex only the South marble (IH04.027)
could be considered to retain an 87 Sr/86 Sr ratio close to the
depositional value due to the high Sr concentration (1190 ppm).
The 87 Sr/86 Sr of 0.70616 and δ13 C of −1.1‰ intersects on the
seawater reference curve agree at 740, 720 and 670 Ma. Two
younger intercepts should not be considered because the Xix-
ano Complex underwent metamorphism at 735 ± 5 Ma (Bingen
et al., 2006a, b, 2007). The 87 Sr/86 Sr and ␦13 C of the North
Xixano marbles intercepts the reference curve at 800, 750 and
660 Ma. The younger intercept should not be considered for the
reason explained above. The least altered 87 Sr/86 Sr of 0.70574 is
significantly lower than the ratio in the South marble. However,
the low Sr concentration (73 ppm) suggests that the Rb/Sr sys-
tem might have experienced a postdepositional alteration, and
therefore 800, and 750 Ma should be considered as the upper
limit for an apparent depositional age.
In the Lalamo Complex, both the Centre and South marbles
(Fig. 1) are exceptionally rich in Sr and their 87 Sr/86 Sr ratios may
therefore be a robust proxy for coeval seawater. The 87 Sr/86 Sr
of 0.70627 and δ13 C of +3.5‰ for the Lalamo Centre marble
has a joint intercept at 740 or 670 Ma. Although both 87 Sr/86 Sr
(0.70671) and δ13 C (+7.1‰) ratios of the Lalamo South marble
differ, they provide a similar apparent depositional age at 740 or
670 Ma (Fig. 4). As in the Xixano Complex, the younger inter-
cept at 670 Ma is in conflict with magmatic ages ranging between
753 ± 10 and 696 ± 13 Ma (Bingen et al., 2006a, b, 2007), and
thus should not be considered as an apparent depositional age.
All marbles sampled in the Nampula Complex have rel-
atively low Sr concentration (up to 350 ppm, Table 3). The
limited database (Table 4) does not allow reliable discrimination
against postdepositional resetting of the Rb/Sr system. Conse-
quently the 87 Sr/86 Sr ratio of 0.70594 obtained from one of the
Nampula Complex marbles may not represent a robust proxy
for coeval seawater. However, the ratio can set an upper age
limit for deposition. Several intercepts on the 87 Sr/86 Sr refer-
ence curve can be reconciled with δ13 C of −3.5‰ at c. 750 Ma
(Fig. 4). The age cannot be older than 800 Ma, because δ13 C
values significantly below −1.0‰ are not characteristic of the
1300–800 Ma interval (Kah et al., 1999) and the late Palaeopro-
terozoic (1800–1500 Ma) (Lindsay and Brasier, 2002).
7. Implications for tectonostratigraphy and basin
evolution
Apparent carbonate depositional ages obtained by isotope
chemostratigraphy (Table 6) can provide insight into basin evo-
lution during the Mezo-Neoproterozoic in NE Mozambique,
which cannot be done at present by any other means. However,
apparent ages should be treated with caution for two reasons: (i)
a possible, unresolved, postdepositional resetting; and (ii) a pos-
sible bias towards exposed and selectively sampled marble units.
Therefore, initial 87 Sr/86 Sr ratios might have been lower, and so
apparent depositional ages older, and the age coverage obtained
for each complex might be incomplete. Further, we consider only
complexes that contain marbles for which apparent depositional
ages have been obtained.
The apparent carbonate depositional ages cluster in six
groups (Table 6), namely (1) 1250–910 Ma (tripartite marble unit
of the Montepuez Complex); (2) 800 or 750 Ma (Xixano North
marble); (3) 800, 750 or 660 Ma (Montepuez West marble); (4)
c. 750 Ma (Nampula marble); (5) c. 740 Ma (Xixano South and
Lalamo Centre and South marbles); and (6) 740, or 700–670 Ma
(Montepuez East marble). All groups, except group 1, have over-
lapping apparent ages. The apparent depositional ages of groups
2, 3 and 6 are tentatively considered undistinguishable. Although
the isotopic composition of the Nampula marble (group 4) has
 V.A. Melezhik et al. / Precambrian Research 162 (2008) 540–558
Table 6
Summary of the least altered 87 Sr/86 Sr and δ13 C ratios, and apparent depostional ages of marble units in NE Mozambique
Complex Occurrence 87 Sr/86 Sr
Montepuez Montepuez quarries 0.70504
Xixano Xixano North 0.70574
Montepuez Montepuez West 0.70566
Nampula Nampula 0.70594
Xixano Xixano South 0.70616
Lalamo Lalamo Centre 0.70627
Lalamo Lalamo South 0.70671
Montepuez Montepuez East 0.70654
a unique resolution at c. 750 Ma, this apparent depositional age
overlaps with those of the Xixano North (group 2) and Mon-
tepuez West (group 3) marbles. Similarly, the c. 740 Ma Xixano
South and Lalamo Centre and South marbles (group 5) overlaps
with the apparent depositional age of the Montepuez East mar-
ble (group 6). Individual marble units within the c. 750 and c.
740 Ma groups are rather inhomogeneous in terms of 87 Sr/86 Sr
ratios, highly variable in Sr abundance; the Nampula marble is
significantly depleted in 13 C, whereas the Lalamo South marble
is considerably enriched in 13 C (Table 6). All these differences
suggest that their carbonates originally precipitated from differ-
ent seawater, and that the depositional ages of individual marble
units might be also different. This is, however, impossible to
resolve within the limitations of the isotope chemostratigraphy
approach (Fig. 4)
7.1. The Montepuez Complex
The Montepuez Complex contains marble units showing
at least two different depositional ages. The oldest age of
1250–910 Ma was obtained from the tripartite marble unit at
Montepuez quarries. The two younger marble units, one with
the apparent depositional ages at c. 800, 750 or 660 Ma (West
marble), and the other at c. 740 or between 700–670 Ma (East
marble), have carbon and Sr isotopic compositions that cor-
respond to significantly different seawaters (Table 6). From
the tectonostratigraphic implications, it is important to note
that the 800–660 Ma marble is closely linked spatially to
the 1250–910 Ma marbles exposed in the Montepuez quarries
(Fig. 1).
The 1250–910 Ma marbles represent the oldest dated carbon-
ate rocks in the Montepuez Complex. No depositional basement
to the marbles is currently known at the present day. The
1250–910 Ma estimate suggests that the Pan-African nappe
system in NE Mozambique may carry Mesoproterozoic sed-
imentary rocks, and not only Neoproterozoic lithologies, as
suggested by zircon-monazite geochronology of orthogneisses.
The 1250–910 Ma marbles are low-Sr, intensively dolomi-
tised rocks. Compilation of depositional settings of Mezo-
Neoproterozoic dolostones suggests that dolostones and
dolomitised limestones are common features of intertidal,
supratidal and peritidal settings, whereas limestones tend to
accumulate in shelf and deep basinal environments, very often
below storm waves (Muir et al., 1980; Delaney, 1981; Tucker,
1983a, b; Lindsay, 1987; Preiss, 1987; Southgate, 1989). In
555
␦13 C (‰) Age (Ma) Age-group
+2.0 c. 1200 1
−0.2 800 or 750 2
+0.1 800, 750 or 660 3
−3.5 c. 750. 4
−1.1 c. 740 5
+3.5 c. 740 5
+7.1 c. 740 5
+4.7 700–670 or 740 6
view of the very limited sedimentological evidence, the robust
reconstruction of depositional settings is not possible.
The 800–660 Ma (Montepuez West) and 740–670 Ma (Mon-
tepuez East) marble units are composed of Sr-rich calcite,
suggesting an aragonite precursor. The marbles of these two
units show considerable isotopic differences (Table 3). The sig-
nificant enrichment of the East marble in 13 C suggests enhanced
burial of organic matter coeval with the carbonate deposition.
Overall, the isotopic dissimilarities of the East and West mar-
bles, combined with a considerable spatial separation by thick
piles of gneisses and schists, would argue for their accumu-
lation in two unrelated basins. However, care must be taken
in comparison of the carbon and strontium isotopic records
due to the greatly different residence times of C (∼105 years)
and Sr (∼3 × 106 years) in oceanic waters, and consequently
their respective response time to perturbations (e.g., Derry et
al., 1992; Richter and Turekian, 1993). The greatest temporal
change confidently documented in seawater 87 Sr/86 Sr is at a rate
of ∼69 × 10−6 Myr−1 that has occurred between 40 and 25 Ma
in the Cenozoic (e.g., Elderfield, 1986). If such a rate is applied
to the two youngest carbonate units, the required difference in
their time of deposition should be not less than 10 Ma. How-
ever, this can neither prove nor disprove whether or not the two
younger marbles belonged to two separated depositional cycles.
We tentatively imply isolated carbonate platform settings for the
two younger marble units of the Montepuez Complex because
they are composed of high-Sr, pure, calcite marbles. However,
the limited nature of the geological information available is
acknowledged.
7.2. The Xixano Complex
The Xixano Complex includes two marble units whose iso-
topic composition is respectively consistent with c. 800 and
750 Ma, and c. 740 Ma seawater. Although their apparent depo-
sitional ages are rather similar, the marble units are separated in
space and have a significant difference in 87 Sr/86 Sr (Table 6).
These two sedimentation episodes are preceded by a volcanic-
arc type felsic volcanism dated to 818 ± 10 Ma (Bingen et al.,
2006a, b, 2007). However, detailed geological relationships
between the sedimentary and volcanic rocks remain unknown.
There is no sedimentological evidence elucidating depositional
settings of carbonates in the Xixano Complex. Tentatively, one
volcanic and two sedimentary events are suggested as one
continuous depositional cycle, until new data would suggest
556 V.A. Melezhik et al. / Precambrian Research 162 (2008) 540–558
otherwise. The 818 Ma volcanic rocks and 800–740 Ma carbon-
ate units and volcanic rocks underwent only amphibolite-facies
metamorphism, and thus their deposition-metamorphic history
must be considered separately from that of the mafic and ender-
bitic orthogneisses affected by granulite-facies metamorphism
at 735 ± 4 Ma in the same complex (Bingen et al., 2006a, b,
2007). Such heterogeneity is considered to be the result of tec-
tonic juxtaposition of two plates with different ancestries during
the Neoproterozoic stacking event.
7.3. The Lalamo Complex
Based on the results described above, the geological history
of the Lalamo Complex very likely includes development of
one carbonate basin with an apparent age of c. 740 Ma. Two
synorogenic granitic plutonic events dated to 753 ± 10 Ma and
696 ± 13 Ma in the Lalamo Complex (Jamal, 2005; Bingen
et al., 2006a, b, 2007) may imply that the development of
this carbonate-depositing basin falls in between the two oro-
genic events. This also may imply that these complexes could
have different ancestries and were tectonically juxtaposed prior
to or during the 560–530 Ma Pan-African orogeny. However,
since the time constraint for the carbonate deposition remains
imprecise, both above inferences require corroboration by more
precise age determinations.
7.4. The Nampula Complex
The Nampula Complex is regarded as one of the basement
complexes in NE Mozambique. It is mainly made up of Meso-
proterozoic orthogneiss ranging in age between c. 1150 and
1020 Ma (Kröner et al., 1997; Bingen et al., 2006a, b, 2007).
The Sr- and C-isotopic compositions of marble interbedded
with graphite schist and paragneiss in the northeastern part
of the complex, south of the Ocua Complex (Fig. 1), sug-
gest much younger depositional ages, at around c. 750 Ma.
The difference over 300 Ma between the older igneous rocks
and the younger marbles, both subsequently involved in the
Pan-African deformation and high-grade metamorphism, can-
not easily be reconciled within a model of the coherent
tectonostratigraphic unit which experienced a single cycle of
deposition–deformation–metamorphic history. The data suggest
that the marble-bearing sequences represent either an uncon-
formable Neoproterozoic cover, or tectonic slices, belonging
to the Neoproterozoic nappe system, folded together with the
basement lithologies.
8. Conclusions
1. Calcite, dolomite and, to a lesser extent, magnesite marbles
are minor but characteristic components of several metased-
imentary units of unknown age within tectonic nappes in the
Neoproterozoic Mozambique Belt of NE Mozambique.
2. Carbon and strontium isotope stratigraphy of marble units
has been applied for indirect dating of carbonate sedimenta-
tion and to provide a complementary and independent insight
into the depositional history and tectonic development of NE
Mozambique within a previously established tectonostrati-
graphic and geotectonic framework.
3. Despite amphibolite-facies Neoproterozoic metamorphism,
some marbles retain δ18 O (V-SMOW) as high as 28.4‰,
suggesting well-preserved depositional signatures. High
Sr-abundances in several marble units (1000–4000 ppm)
provided strong buffering of the Sr-isotope system against
postdepositional resetting.
4. The overall spread of the least altered δ13 C (−3.5 to +7.1‰)
and 87 Sr/86 Sr (0.70504–0.70671) values from the Nampula,
Montepuez, Xixano and Lalamo marbles suggests several
discrete apparent depositional ages within the 1250–660 Ma
time interval. The apparent depositional age of the Ocua
marble was not resolved.
5. The 300 Ma time lag between felsic volcanism
(1250–1200 Ma) and carbonate deposition (c. 750 Ma)
in the Nampula Complex suggests either a non-depositional
unconformity between the two cycles or different ancestry
and tectonic juxtaposition during the Neoproterozoic
Pan-African orogeny.
6. Juxtaposition of amphibolite-grade Xixano Complex mar-
bles (originally deposited between 800–750 and at c. 740 Ma)
with 735 Ma granulites implies different ancestry of these
rock assemblages.
7. Apparent carbonate depositional ages suggest that the Nam-
pula, Montepuez, Xixano and Lalamo complexes do not
represent contiguous tectonostratigraphic units and that they
may in fact consist of juxtaposed nappe units.
Acknowledgements
This work is the part of the Mineral Resources Management
Capacity Building Project, Republic of Mozambique; Com-
ponent 2: Geological Infrastructure Development Programme:
Geological Mapping (Lot 1) financed by the Nordic Develop-
ment Fund. The C and O isotope analyses were performed at the
Scottish Universities Environmental Research Centre supported
by the Consortium of Scottish Universities and the Natural
Environment Research Council. The Rb–Sr isotope study at
the Institute of Precambrian Geology and Geochronology (St.
Petersburg) was partly supported by the RFBR Project 05-05-
65329. We are grateful to G.V. Konstantinova, N.N. Melnikov
and E.P. Kutyavin for their assistance in the Rb-Sr analytical
work as well as T.L. Turchenko for the XRD analyses of sili-
ciclastic constituents of the carbonate rocks. Two anonymous
reviewers and the Editor are acknowledged for constructive crit-
icism leading to improvements in the manuscript.
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