Sedimentary Geology 235 (2011) 79–90

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Sedimentary Geology
j o u r n a l h o m e p a g e : w w w. e l s ev i e r. c o m / l o c a t e / s e d g e o

Cretaceous anoxic–oxic changes in the Moldavids (Carpathians, Romania)

Mihaela C. Melinte-Dobrinescu a,⁎, Relu-Dumitru Roban b
a
National Institute of Marine Geology and Geo-ecology, 23-25 Dimitrie Onciul Street, RO-024053 Bucharest, Romania
b
University of Bucharest, Faculty of Geology and Geophysics, 1 Nicolae Bălcescu Blvd., Bucharest, Romania

a r t i c l e i n f o a b s t r a c t

Article history: This study focused on the Cretaceous black shale successions, followed by red shales that crop out at the
Received 14 June 2009 outer regions of the Romanian Carpathians, in the Moldavids. The oldest parts of the black shale units
Received in revised form 26 April 2010 deposited in an abyssal plain during Late Valanginian–Late Barremian time; they are mainly characterized by
Accepted 12 June 2010
hemipelagic and pelagic muddy siliciclastic rocks and carbonates, commonly intercalated with fine-grained
Available online 12 June 2010
turbidites.
During the sedimentation of the middle part of the black shale units in the Late Barremian–Early Albian
Keywords:
Lower Cretaceous
interval, the depth of the basin increased, as the carbonate hemipelagic sedimentation was replaced by a
Laminated black shales mainly siliceous one. Only a few thin turbidite intercalations are present.
Upper Cretaceous Oceanic Red Beds The youngest part (Albian pro parte) of the black shale units is characterized by a turbiditic sedimentation,
Romania with mainly sandy sequences of middle and lower deep-water fans. We may assume that the depth of the
Pelagites and turbidites basin continuously decreased. The presence of authigenic glauconite in the Albian sandstones suggests a
palaeoenvironmental change, linked to the occurrence of oxygenated turbidity current circulation.
A significant shift in the sedimentation regime in the Eastern Carpathian Moldavids took place in the Late
Albian, when Cretaceous Oceanic Red Beds (CORB) occurred. This type of sedimentation lasted up to the
Coniacian. The lower part of the CORBs that contains radiolarites intercalated with variegated shales,
pyroclastic tuffs and thin sandstones is interpreted as a hemipelagic and pelagic sedimentation in the abyssal
plain environment, where rarely turbidites occurred. Upwards, there are mainly burrowed variegated red
and green shales. The youngest parts of CORBs are characterized by increased thickness and frequency of the
turbidites. While the main part of the CORB is carbonate free or has very low carbonate content, the upper
part of these strata becomes rich in marl and mudstone strata, indicating a decrease of the basin-depth.
The accumulation of black shales in the Eastern Carpathians during the Late Valanginian–Late Albian interval
is linked to the existence of a small, silled basin of the Moldavian Trough, in which restricted circulation led
to the density stratification of the water column, resulting in the deposition of anoxic Lower Cretaceous
sediments (i.e., the black shales). Because of the tectonic deformation that took place within the Lower–
Upper Cretaceous boundary interval, the restricted circulation had changed to an open circulation regime in
the Moldavian Trough. Hence, the anoxic regime was progressively replaced by an oxic one, across the
Albian–Cenomanian boundary interval. The beginning and the end of the CORBs in the Moldavid units
depend thus on various palaeogeographic and palaeoenvironmental settings, and it was controlled by the
regional tectonic activity.
© 2010 Elsevier B.V. All rights reserved.

1. Introduction
The transition from Cretaceous anoxic to oxic environments was
observed in many Tethyan areas (Jansa et al., 1979; Arthur and
Premoli Silva, 1982; Hu et al., 2005; Jansa and Hu, 2009), including the
Carpathians (Švábenická et al., 1997; Bąk, 1998; Michalík et al., 2002;
Wang et al., 2005; Melinte-Dobrinescu et al., 2009; Skupien et al.,
2009). In the Carpathian mountain belt, the sedimentation of the
Upper Cretaceous Oceanic Red Beds (referred as CORB by Hu et al.,
⁎ Corresponding author. Fax: + 40 212522594.
E-mail address: melinte@geoecomar.ro (M.C. Melinte-Dobrinescu).
2005) follows the Lower Cretaceous black shale deposition. It appears
that the development of Cretaceous black shales and CORBs is
somehow causally related (Hu et al., 2006). The anoxic–oxic changes
may reflect various Earth processes, such as palaeoceanographic shift,
tectonic movements, and/or climatic fluctuations that changed the
balance between carbon sources and sinks in the world ocean (Wang
et al., 2005; Hu et al., 2009).
Colour of sedimentary rocks is an important indicator of
environmental conditions in which they have formed. Gray and
black shale occurrence is commonly linked to increases in organic
matter content, and low oxygen content in bottom waters. In
turn, CORB indicate low organic matter content, but well-oxygenated
bottom conditions.

0037-0738/$ – see front matter © 2010 Elsevier B.V. All rights reserved.
doi:10.1016/j.sedgeo.2010.06.009
80 M.C. Melinte-Dobrinescu, R.-D. Roban / Sedimentary Geology 235 (2011) 79–90
Numerous dark-coloured, commonly laminated, organic-rich
sediments occur within Mesozoic sequences; they are frequently
associated with Upper Jurassic to Lower Cretaceous organic carbon
enriched claystones, clayey sandstones and limestones (Wignall,
1994; Pancost et al., 2004). Such beds that are more than 1-cm-thick
and contain more than 1% of total organic carbon (TOC) are described
as black shales (Pettijohn, 1957; Stow et al., 2001). In general, the
term of black shales is used for any dark-colored fine-grained organic
carbon rich sediment, in which TOC contents typically range from 1 to
15%. Many black shales are hemipelagites; some, such as black cherts
and organic rich limestones, are pelagites; others are fine grained
turbidites (Stow et al., 1996). Black shales are also characterized
geochemically by high Fe2+ and S2− contents and enrichments in
trace elements, such as Ba, Bi, Cr, Ni, Mo, V, Zn (Nijenhuis et al., 1999;
Lipinski et al., 2003). The sedimentation of black shales is mostly
ascribed to oxygen-poor bottom waters, typically accumulated in
deep-ocean basin setting, but they may also occur in shallower sites
(Wignall and Newton, 2001).
During the mid-Cretaceous, red oxic sediments, with low content
of preserved organic carbon, replaced the deposition of organic-rich
black shales in many of the Tethyan areas (Wang et al., 2005). This
type of sedimentation is found from low to middle palaeolatitudes up
to the end of the Cretaceous (Arthur and Premoli Silva, 1982; Hu et al.,
2005; Melinte and Jipa, 2005; Hu et al., 2006). Probably, CORB
sedimentation is a response to a palaeoclimatic and/or palaeoceano-
graphic fluctuations, but also is effected by tectonic activity and
synorogenic depositional processes (Hu et al., 2005; Wagreich and
Krenmayr, 2005; Neuhuber et al., 2007; Melinte-Dobrinescu et al.,
2009). The occurrence of CORB may also be linked to changes in
bioproductivity, triggered by major palaeoceanographic modifications
of the world oceans.
In this paper, we will discuss stratigraphy and examine genetic
relationship between Lower Cretaceous organic-rich black shales
deposition and overlaying Upper Cretaceous oceanic red beds from
the eastern part of the Romanian Carpathian region. We also
comment on causes of the Cretaceous anoxic–oxic changes as seen
in the Moldavid nappes of the Eastern Carpathians.
2. Geological setting
The Eastern Carpathians represent a segment (over 600 km long) of
the Carpathian tectonic chain. Inwards (westwards), this mountainous
chain is bordered by the Transylvanian Basin and the easternmost part
of the Pannonian Basin, while outwards (eastwards), it is bordered by
the Moldavian and Scythian Platforms (at the E) and by the Moesian
Platform (towards SE and S). The Eastern Carpathians are mainly
composed of Jurassic–Miocene sedimentary rocks, deposited in several
basins, folded and overthrusted on the Miocene sediments of the
Carpathian Foredeep. Imbrication and internal deformation of the
nappes occurred during several periods, from the Late Cretaceous up to
the Neogene (Săndulescu, 1980, 1984; Maţenco, 1997; Csontos and
Vörös, 2004).
Based on the age of the main deformation and the mutual areal
position, several tectonical units were recognized in the Eastern
Carpathians (Săndulescu, 1984), such as (from W to E): the Pieninids,
the Transylvanids, the Median Dacids, the Outer Dacids, and the
Moldavids (Fig. 1). The nappes of the Eastern Carpathians were grouped
into two main tectonic units (Săndulescu, 1975), which are the Dacids
(nappes mainly involved in the Cretaceous tectonic movements) and
the Moldavids (tectonic units folded mainly during the Miocene).
All the sections investigated by us are placed in the Moldavids that
represent a nappe system located at the outermost part of the Eastern
Fig. 1. a: Geologic map of Romania (simplified after Săndulescu, 1984) with the outline of the map b; b: Tectonic map of the Eastern Carpathians (modified after Săndulescu, 1984).
Sections discussed in this paper: A—Bota; B—Bicaz; C—Covasna.
Carpathians. Their sedimentary and post-tectonic covers are exclusively
composed of Lower Cretaceous–Cenozoic rocks (Săndulescu, 1984;
Ştefănescu and Micu, 1987; Ştefănescu, 1995). The oldest Moldavids,
namely the Inner Moldavids (i.e., Teleajen, Macla and Audia nappes)
contain only Cretaceous sediments and are located in the W (innermost)
part of this nappe system. The youngest Moldavids, described as the
Outer Moldavids (i.e., Tarcău, Vrancea and the Subcarpathian nappes)
contain Cretaceous–Cenozoic rocks, being placed at the E (outermost)
part of the nappe system.
The organic-rich black shales are the oldest sediments exposed in
the Eastern Carpathian Moldavid nappes. The western occurrence of
these sediments is known from the innermost part of the Moldavids
(i.e., the Teleajen Nappe), where they were sedimented during the
Late Valanginian–Late Hauterivian (Ion, 1975; Antonescu et al., 1978).
The most complete development of the Lower Cretaceous organic-rich
black shales in the Eastern Carpathians is known from the eastern part
of the Inner Moldavids (i.e., the Audia Nappe) and from the Outer
Moldavids, such as Tarcău and Vrancea nappes (Filipescu et al., 1963;
Săndulescu, 1984; Ştefănescu and Micu, 1987), where they belong to
the Audia Formation (Ştefănescu, 1976). The Lower Cretaceous
organic-rich black shales are overlain in all the Moldavids by Upper
Cretaceous Oceanic Red Beds (CORB), described under different
names (i.e., Bota-Botiţa, Cârnu-Şiclău and Tisaru formations - Băncilă,
1958; Filipescu et al., 1963), but displaying a similar lithology.
3. Materials and methods
We have studied several sections located in the Inner and Outer
Moldavids, displaying a continuous transition from organic-rich black
shales to CORB. However, we have selected to present herein only three of
the most representative sections, located at the southern and central parts
of the Eastern Carpathians, in the Audia and the Tarcău nappes. The most
complete investigated section is placed in the Audia Nappe, being located
in the Carpathian Bend region (Bota River, tributary of the Buzău Valley- A
in Fig. 1). Another section from the Audia Nappe, which displays only the
upper part of the black-shale succession, is situated in the central part of
the Eastern Carpathians (in the Bistriţa Valley, at Bicaz — B in Fig. 1). The
outermost section analyzed by us belongs to the Tarcău Nappe and it is
positioned in the S Eastern Carpathians (the Covasna Valley — C in Fig. 1).
All the above-mentioned sections were logged in detail, from lithological
and sedimentological points of view. To date the studied deposits,
calcareous nannoplankton analyses were achieved. Sampling was
realized at 25 cm intervals.
4. Results
4.1. Organic-rich black shales
In the southernmost investigated section, located in the Audia
Nappe (A in Fig. 1), the Audia Formation, 190 m in thickness, displays
all three members of the black shale strata (Figs. 2 and 3), which are
from the base to the top:
(i) The Lower Member, 80 m in thickness, that contains at its lower
part mainly laminated black shales. The upper part is composed
of decimetre-thick rhythmically alternating lithic and sublithic
sandstones, siltstones and dark grey shales. The organic rich black
shales amount up to 80% in this unit. Thin dm strata of siderite
limestones and siderites are also present. Rarely, cm up to dm
limestones (mudstones and wackestones), marls and cherts
could be observed. The sandstones and the limestones of this unit
appear as fining up sequences at intervals between 30 cm and
300 cm (Figs. 3 and 4).
M.C. Melinte-Dobrinescu, R.-D. Roban / Sedimentary Geology 235 (2011) 79–90 81
82 M.C. Melinte-Dobrinescu, R.-D. Roban / Sedimentary Geology 235 (2011) 79–90

The nannofossil assemblages are scarce and poorly preserved, but

can be assigned to the NC5 (upper part), NC6, NC7 and lower part of
the NC8 calcareous nannoplankton zones of Roth (1983) (Fig. 2).
These biozones are covering the Late Barremian–Early Albian interval
(Scott, 2009b).

(iii) The Upper Member of the Audia Formation is composed of

40 m rhythmically alternating successions of black shales and
dm up to m subquartzous sandstones, with the latter showing
parallel lamination and current ripples (Figs. 3 and 4). Some
levels include is a high content of macroscopically visible
glauconitic peloids. At the base of the sandstone beds, fine-
grained conglomerates could be observed. The sandstones
represent 50% up to 80% of the Upper Member deposits. The
identification of the calcareous nannofossil zones and subzones
NC8B, NC9 and NC10 (lower part) of Roth (1983) indicates an
Early to Late Albian age (Scott, 2009a,b) for the Upper Member
(Fig. 2).

The northern studied section of the Audia Nappe is located in the

central part of the Eastern Carpathians, at the Bicaz, Bistriţa Valley
(section B in Fig. 1). There, only the Upper Member of the Audia
Formation, 40 m in thickness, is exposed (Figs. 3 and 4). It is
comprised by dm up to m thick subquartzous sandstones, locally
with fine-grained conglomerates at the base, and thin cm black shales.
The sandstones constitute up to 50% of the unit (Fig. 5).
The sandstones and shales are organized in fining up sequences, of
20–50 cm thick. These sequences contain sandy levels that show at
the base normal grading, than horizontal parallel- and crossed-
laminated structures, followed by siltstones and shales. Based on the
identified calcareous nannoplankton assemblages, that were assigned
to the NC8B, NC9A, NC9B and NC10 zones, the age of the studied
succession is Early to Late Albian.
We also investigated the Lower Cretaceous black shales of the
Outer Moldavids (i.e., in the Tarcău Nappe) from the Covasna Valley
(section C in Fig. 1), displaying the succession of its three members
(lowest first):

(i) The Lower Member that is composed of 40 m laminated black

Fig. 2. Lithostratigraphy and biostratigraphy based on calcareous nannoplankton of the
black shale and CORB units of the Moldavid nappes (Eastern Carpathians). NK — calcareous
nannofossil zones and subzones after Bralower et al. (1989); NC — calcareous nannofossil
zones and subzones after Roth (1983); UC — calcareous nannofossil zones and subzones
after Burnett (1998); FO — first occurrence.
The calcareous nannofossils identified within the Lower Member
show the presence of the NK3B nannofossil subzone of Bralower et al.
(1989), as well as of the NC4 calcareous nannofossil zone of Roth
(1983) (Fig. 2). These nannofossil zones cover the Late Valanginian–
Early Hauterivian interval in the Romanian Carpathians (Melinte and
Mutterlose, 2001; Barbu and Melinte-Dobrinescu, 2008). The upper
part of the Lower Member is of Late Hauterivian–Late Barremian age,
as indicated by the presence of the NC5 calcareous nannofossil zone
(including its subzones) of Roth (1983).
(iii) The Upper Member is made up of 40 m thick black shales and
(ii) The Middle Member of the Audia Formation, 70 m thick, is mainly
composed of laminated black shales, commonly interbedded
with black cherts, the later lithological feature distinguishing this
unit from the older Lower Member (Figs. 3 and 4). The cherts
yield pinch and swell structures. Sporadically, thin cm levels of
breccias and conglomerates with granodiorite clasts occur. Thin
cm beds of sandstones occur in the whole unit, with higher
frequency towards the upper part of this member (Figs. 3 and 4).
shales with rare intercalations of sandstones, the later yielding
parallel lamination and frequently ripple marks. Common beds or
lenses of siderites and limestones are present. Thin cm up to dm
mudstones, wackestones and marls were mostly encountered in
the middle part of this unit. Rare cm nodular and lenticular cherts
could be also observed, mainly towards the upper part of this
member (Figs. 3 and 4). The calcareous nannoplankton assem-
blages of this unit are of Early Hauterivian-Late Barremian in age,
covering the NC4 and NC5 calcareous nannofossil zones (Fig. 2).
(ii) The Middle Member, 80 m thick, is lithologically similar to the
Lower Member, being composed of laminated black shales, but
with thicker and more frequent levels of lithic sandstones, as well
as interbedded black cherts (Figs. 3 and 4). Rarely, sideritic and
micritic limestones, as well as lenticular and nodular siderites are
present (Fig. 5). Breccias with granodiorite fragments also
occurred. Based on calcareous nannofloral analysis, the age of
this unit is Late Barremian–Early Albian, an interval covered by
the NC6, NC7 and NC8 calcareous nannoplankton zones (Fig. 2).
intercalated grey-green quartzous sandstones; it has a distin-
guishing feature that is the common presence of glauconite.
The decimetre-thick sandstones are separated by centimetre-
thick black shales (Figs. 3 and 4). The sandstones represent
around 70–80% of the whole Upper Member. We identified in
this lithological unit calcareous nannofloras belonging to the
NC8, NC9 and NC10 (lower part) zones, which indicate an Early
to Late Albian age (Fig. 2).
 M.C. Melinte-Dobrinescu, R.-D. Roban / Sedimentary Geology 235 (2011) 79–90 83

Fig. 3. Lithostratigraphy of the black shale and CORB units in the Moldavids (Eastern Carpathians). Legend: 1 — Conglomerates and breccias; 2 — Sandstones and greywackes; 3 — Siltstones;
4 — Organic-rich black shales; 5 — Variegated red and green shales; 6 — Cherts and radiolarites; 7 — Pyroclastic tuffs; 8 — Siderites; 9 — Limestones (mudstones and wackestones); 10 —
Marls; 11 — Nodules; 12 — Pinch and swell structures; 13 — Trace-fossil burrows; 14 — Foraminifera bioclasts; 15 — Indeterminable calcareous bioclasts; 16 — Spicules of siliceous sponges;
17 — Radiolarian bioclasts; d1 — location of sedimentological logs of Figs. 4 and 6. Grain size classes: c—clay; t—silt; s—sand; g—gravel.

4.2. CORBs zous sandstones rich in glauconitic levels is conformably covered by

In the investigated Moldavid sections, the black shale units are
directly overlaying by CORBs (Figs. 2 and 3). CORBs were previously
described as Bota–Botiţa Formation in the Audia Nappe and Cârnu–
Şiclău Formation in the Tarcău Nappe (Săndulescu et al., 1981), even
though they display a similar lithology. In all the above-mentioned
units, CORB deposition began during the upper part of the Albian
(Fig. 2), in the NC10 calcareous nannoplankton zone of Roth (1983),
respectively in the UC0 Zone of Burnett (1998).
In the Audia Nappe, the Upper Member of the Audia Formation
(composed of organic-rich black shales interbedded with subquart-
the CORB of the Bota–Botiţa Formation, 125 m in thickness (Fig. 5).
The top of the CORB is unconformably covered by the massive
sandstones of the Siriu Formation (Figs. 2 and 3). The base of this
lithological unit contains, in the Covasna Valley, centimetre-thick
radiolarites alternating with red and green or even grey siliceous
shales (Figs. 3 and 6). Thin cm pyroclastic tuff levels are also present.
The middle part of the CORBs from the Audia Nappe is dominated by
variegated red and green shales. Towards the upper part, silts,
variegated shales, micritic limestones, as well as centimeter-thick
sandstones, with parallel lamination, and fine-grained conglomerates
are present. The thickness and the grain size of the sandstones and
84 M.C. Melinte-Dobrinescu, R.-D. Roban / Sedimentary Geology 235 (2011) 79–90
Fig. 4. Logs of representative sequences of the black shale units (the Audia Formation) in
the Covasna section (Tarcău Nappe). For lithological legend and location of logs, see Fig. 3.
Legend of the sedimentary internal structures: 1. Massive; 2. Normal grading; 3. Horizontal
parallel lamination; 4. Cross lamination, asymmetrical current ripples. Grain size classes: c—
clay; t—silt; sf—fine sand; sm—medium sand; sc—coarse sand; g—gravel.
conglomerates increased towards the top of CORBs. The whole
sequence yielded a coarsening upward tendency. The age of the
Bota–Botiţa Formation is Late Albian–Coniacian pro parte (Fig. 2), an
interval covered by the UC0–UC10 calcareous nannoplankton zones of
Burnett (1998).
At the Tarcău Nappe, in the exposed section of the Covasna Valley
(section C in Fig. 1), the CORB unit, namely the Cârnu–Şiclău
Formation (65 m in thickness), is conformably overlaying the Upper
Member of the Audia Formation and is unconformably covered by the
calcareous turbidites of the Horgazu Formation (Fig. 2). The base of
the CORB is composed of red radiolarian rocks with different degree of
chertification, interbedded with thin grey and green shales (Fig. 5). A
few centimetre-thick tuff intercalations also occur (Figs. 3 and 6).
Within the upper part of the Cârnu–Şiclău Formation, red shales are
more numerous, being interbedded with green and light grey ones.
These variegated couplets are the main lithological feature of this unit.
Towards the top, the CORBs grade into a grey and reddish muddy
limestone succession, interbedded with decimetre-thick lithic and
bioclastic sandstones, with parallel lamination and ripple marks. The
amount of siliciclastic rocks increased to the upper part of the CORB
unit; cm up to dm conglomerates and breccias occur. Some breccia
levels contain fragments of granodiorites (Figs. 3 and 6).
Previous studies (Neagu, 1970; Ion and Szasz, 1994) indicate that
planktonic foraminifera are very rare in the Cârnu–Şiclău Formation,
and were identified only near its top. On a contrary, the lower part of
this unit is rich in agglutinated foraminifers and commonly contains
pyritized radiolarians (Neagu, 1968, 1990; Bubík, 2005). The
calcareous nannoplankton of the Cârnu–Şiclău Formation belong to
the UC0–UC10 biozones of Burnett (1998), indicating that the age of
these deposits is Late Albian–Early Coniacian.
5. Discussion
5.1. Sedimentologic and genetic significance
5.1.1. Black shales
The laminated organic-rich black shales are the main lithological
component of the Upper Valanginian–Upper Albian Audia Formation.
They also occur, within the Albian–Cenomanian boundary interval, as cm
levels interbedded in the CORB units of the Moldavids. These shales are
composed of phyllosilicates, quartz and subordinately siliceous bioclasts
(radiolarian and sponge spicules); they also include carbonate bioclasts
with foraminifera, bivalve and echinids (Grigorescu, 1971; Papiu and
Alexandrescu, 1976; Grasu et al., 1988). In the Eastern Carpathians, in
the northern outcrop area of the Audia Nappe (Bistriţa Valley), the main
constituent of the black shales is illite (21–56%), followed in descending
order by detritic quartz, chalcedony and opal (jointly amounting 18–
24%), chlorite (2–8%), calcite and dolomite (making together 1–15%), and
pyrite (0–2%), after Papiu and Alexandrescu (1976).
A high content of organic matter was identified in the laminated
black shales. In the Audia Formation (Audia Nappe), the total organic
carbon (TOC) of the laminated black shales varies from 1.05% up to
3.35% (Balteş et al., 1984; Lafargue et al., 1994). In the same formation,
but at the outer tectonic position (in the Tarcău Nappe), the average
TOC of the Lower Member is 3.2%, but some layers contain up to 5.5%
of TOC (Filipescu et al., 1966; Balteş et al., 1984). The TOC decreases in
the Middle and Upper members down to 1.8%, and 1.1%, respectively.
The bitumen analyses indicate average values for C = 78.86,
H = 10.87, N = 0.30 and O = 9.97 (Grasu et al., 1988). The above-
mentioned authors concluded that the organic matter is mainly
sapropelic, kerogen type I and subordinately humic.
The dominance of the illite, detritic quartz clasts, chloritized micas,
associated with siliceous and carbonate bioclasts in the dark grey
shales suggests that these deposits are mainly clastic and were
deposited from hemipelagic suspensions into a deep sea abyssal plain
environment.
The dark grey up to the black colour of the shales is due to the anoxic
depositional conditions that led to the conservation of the organic
matter and to the reduction of the iron oxides, allowing the formation of
the pyrite and siderite during diagenesis. It was assumed that the anoxic
palaeoenvironment was linked to the palaeotopography of the narrow
 M.C. Melinte-Dobrinescu, R.-D. Roban / Sedimentary Geology 235 (2011) 79–90 85

Fig. 5. a: Upper Barremian deposits of the Audia Formation (Middle Member in the Covasna Valley, Tarcău Nappe); b: Upper Albian deposits of the Audia Formation (Upper Member
in the Bicaz Valley, Audia Nappe); c: Upper Albian black shales (Upper Member of the Audia Formation) overlain by the CORB of the Bota–Botiţa Formation (Bota Valley, Audia
Nappe); d: Upper Albian CORB of the Cârnu–Şiclău Formation (Covasna Valley, Tarcău Nappe).

basin of the Moldavids, in which the restricted circulation did not allow
the exchange between surface and bottom waters, leading to the density
stratification. Noteworthy, the quantity of bitumen type A extracted in
chloroform is low, between 0.07% and 0.13% (Grasu et al., 1988); hence,
the potential for hydrocarbon generation is weak for the Lower Member
of the black shale units, moderate for the Middle Member and
insignificant for the Upper Member (Balteş et al., 1984).
5.1.2. Siderites
The presence of this type of rocks is a lithological feature of the
Lower Member of the Audia Formation. The siderites are intercalated
in the laminated black shales as nodules or stratiform, irregular lentils,
yielding a variable thickness, cm up dm.
The chemical analysis of the siderites from the Audia Formation
(Lower Member) indicate the presence of SiO2 (6–20%), Al2O3 (2–5%),
Fe2O3 (0.5–19%), FeO (5–38%), CaO (5–40%), MgO (1–2) and MnO
(0.01–0.8%) (Savul et al., 1965; Papiu and Alexandrescu, 1976). These
data show that the siderites are not exclusively composed of FeCO3, but
they are also marly, due to their significant content of silica and
aluminium. The presence of Fe2O3 is probably due to the oxic con-
ditions generated during late diagenesis stage. The genesis of the
siderites in the Moldavid black shales units started during an early
diagenesis stage. We may suppose a scenario as proposed by Berner
(1985) and Tucker (1991), suggesting that siderites precipitated
during a high carbonate activity and a low sulphide one, in a methanic
environment.
5.1.3. Cherts and radiolarites
Siliceous rocks were mainly identified in the black shale units of the
Moldavids (frequently in the Lower and Middle members of the Audia
Formation, and rarely in the Upper Member of this unit). Overall, they
occur in the Valanginian–Albian interval. These rocks are also present in
the lower part of the CORB unit of the Moldavid nappes.
The centimetre-thick black siliceous shales and cherts of the Lower
Member of the Audia Formation, yielding pinch and swell structures,
contain sponge spicules, radiolarian tests, as well as microcrystalline
silica; the latter component amounts to 50–70% (Grigorescu, 1971;
Grigorescu and Anastasiu, 1976). As it is expected, the siliceous rocks
of the Middle Member of the Audia Formation yielded a high content
of SiO2 (90%) and a less amount of Al2O3 (4%), Fe2O3 (1.5%), MnO
(0.05%) and MnO (0.5%), according to Filipescu et al. (1966).
Cherts and radiolarites are also present in the lower part of the
Moldavid CORB units (in the Upper Albian–Turonian interval), forming
centimetre-thick couplets with variegated shales. They yield different
degrees of chertification. Possibly, towards the upper part they were
intrabasinal reworked, as they show horizontal parallel laminated
structures. They mainly contain SiO2, over 80% (Papiu et al., 1983), and
less amounts of Al2O3 (between 12 and 20%), and in order of decrease
abundance Fe2O3 (between 4% and 6%), K2O (up to 3.5%), MgO (up to 2%)
and CaO (up to 1%) (Papiu et al., 1983).
The siliceous levels represent pelagic and hemipelagic accumula-
tions of a deep-sea abyssal plain environment. The sponge spicules,
commonly occurring within the Valanginian–Albian interval, may be
reworked form the deep shelf area. The silica source could be, at least
for the Cenomanian–Turonian interval, enhanced by volcanism and
alteration of the pyroclastic tuffs. The clayey intercalations associated
with the siliceous rocks of the CORB contain agglutinated foraminif-
eral assemblages with “Rhizammina” sp. and few elements of
“Krasheninnikov fauna”, such as Praecystammina globigerinaeformis,
Recurvoidella insueta and Trochammina gyroidinaeformis. The presence
of the above-mentioned assemblages argues also for an abyssal
paleoenvironment (Bubík, 2005; Melinte-Dobrinescu et al., 2009).
86 M.C. Melinte-Dobrinescu, R.-D. Roban / Sedimentary Geology 235 (2011) 79–90

5.1.4. Siliciclastic rocks

The siliciclastic rocks are characteristic for the Upper Member of the
Audia Formation. Sporadically, these rocks are present in the Lower and
Middle members of the Audia Formation and towards the upper part of
the CORB units (i.e., Bota–Botiţa and Cârnu–Şiclău formations).
The siliciclasts are massive and normally graded sandstones,
locally with basal fine-grained conglomerates, followed by sandstones
with parallel lamination and ripple marks and by silts and shales;
overall, they show a fining up tendency. Complete sequences as above
described were only rarely encountered. Often, some terms are
missing, such as the basal conglomerates or the sandstones; hence,
sequences containing conglomerates directly overlain by silts and
shales are present. The thickness of these sequences, dominated by
massive and normal graded sandstones, is variable, from a maximum
1.5 m in the Upper Member of the Audia Formation to less than 20 cm
in the other analyzed stratigraphic units.
The described sequences could be assigned to classical turbidites,
most of them incomplete. We identified several coarse sequences,
representing the R3–S2 divisions, as described by Lowe (1982) and
characterizing the middle and deep water fans (Mutti and Ricci Lucci,
1972; Walker, 1978). Other sequences represent the Ta-e terms of
Bouma (1962), most of them incomplete.
From petrographical point of view, the sandstone sequences show
differences in the studied units. For instance, the sandstones of the
Lower and Middle members of the Audia Formation are lithic and
contain green anchimetamorphic clasts, probably derived from an
outer source that is the East European Platform.
The arenites of the Upper Member of the Audia Formation are mainly
represented by sublithic or subquartzous sandstones, with high quartz
content (up to 90%), followed by feldpars, micas, metamorphic and
sedimentary lithoclasts, heavy minerals, as well as siliceous and car-
bonate bioclasts (Grigorescu, 1971; Grigorescu and Anastasiu, 1976).
Some levels contain authigenic glauconite, up to 14%. The source of the
Upper Member arenites is also an outer (eastern) one (Săndulescu,
1984).
In the CORB units of the Moldavids nappes (i.e., Cârnu–Şiclău and
Bota–Botiţa formations), the sandstones, which occur towards the
upper part (mainly in the Coniacian stage) are lithic, containing meta-
morphic and sedimentary rock fragments, muscovite and a carbonate
cement. The provenance of the clasts depends on the location in the
basin. In the internal area of the Moldavid basin, the fragments derived
from an inner, western, source (Papiu and Alexandrescu, 1976). In the
Outer Moldavid basin, the origin of the clasts is multiple, being located
in the intrabasinal flexural bulges as well as in an outer, eastern, source
that is the Eastern European Platform (Vârban, 2003).

5.1.5. Limestones and marls

In the Lower Member of the Audia Formation exposed in the Covasna
Valley, carbonate levels occur as centimetre marls or biomicrites (with
b10% bioclasts), containing mainly planktonic foraminifera (Grigorescu,
1971). In the Middle Member of the above-mentioned unit, the
carbonate levels are marls, as well as bioaccumulated limestones with
terrigenous material and metasomatic calcite cement. The analyses of
these carbonate levels from the northern part of the Audia Nappe
indicate the following composition (Papiu and Alexandrescu, 1976):
SiO2 (6–70%), Al2O3 (0.5–8.5%), Fe2O3 (0.3–12.5%), FeO (3.5–38%), CaO
(5.5–44.5%), MgO (1.5–9%) and K2O (0.3–1.5%). The mineralogical
composition of the same rock is illite (0–21%) chlorite (0.5–5%), quartz
and chalcedony (0–60%), feldspar (0–8.5%), calcite and dolomite (0–
84%), as well as pyrite (0–1.30%). The upper part of CORBs from the
Moldavid external structures (i.e., the Tarcău and the Vrancea nappes)

Fig. 6. Logs of representative sequences of the CORB unit (the Cârnu–Şiclău Formation)
in the Covasna section (Tarcău Nappe). For lithological legend and location of logs, see
Fig. 3. Grain size classes: c—clay; t—silt; sf—fine sand; sm—medium sand; sc—coarse
sand; g—gravel.
 M.C. Melinte-Dobrinescu, R.-D. Roban / Sedimentary Geology 235 (2011) 79–90
become more carbonatic, having a high content of CaCO3 (36–44%) and
less of Al2O3 (3.8–8.3%) (Grasu et al., 1988). Probably, these marly and
carbonate rocks are hemipelagic accumulations, with clay minerals and
biogenic material (sponge spicules, echinoids and foraminifers) that
derived from the shelf.
5.1.6. Variegated couplets of CORB
The variegated (red, green and light grey) centimetre-thick couplets
represent the main part of investigated CORBs (i.e., Bota–Botiţa and
Cârnu–Şiclău formations), except for the lowest part of these units
(mainly composed of red shales, radiolarites and cherts), and the
uppermost part, where frequently siliciclastic rocks occur. The red
shales are mainly composed of clay minerals, detritic quartz and
bioclasts with radiolarians, foraminifera and microcrystalline silica. The
green terms of variegated couplets are composed of phyllosilicates in
the Audia and Tarcău nappes (Papiu et al., 1983) while, in the outermost
Moldavids structures (i.e., the Vrancea Nappe) they are mainly marls or
limestones (mudstones or wackestones) (Vârban, 2003).
In the Audia and Tarcău nappes, the red shales contain illite (35–51%),
quartz and chalcedony (21–43%), kaolinite (5–10%), feldspars (4–6%);
chlorite (∼3%); hematite (2–3%), as well as calcite and dolomite (0.2–
1.5%). The chemical analysis indicate a high amount of SiO2 (60–70%),
together with Al2O3 (12–19%), Fe2O3 (4–6%), FeO (∼1%), MgO (∼2%), CaO
(∼1%), Na2O (0.6–0.7%), K2O (2–3%) and TiO2 (∼0.5%). The green
shales yielded illite (41–44%), quartz and chalcedony (29–31%), kaolinite
(8–10%), feldspars (∼6%), chlorite (5–8%), hematite (0.4–0.7%), calcite
and dolomite (1–2%). The green shales contain, similar to the red ones,
high percentages of SiO2 (63–64%), and, in descending order, Al2O3
(∼17%), Fe2O3 (2–3%), FeO (1.7–2.9%), MgO (∼2%), CaO (∼1%), Na2O
(0.6–0.7%), K2O (2–3%) and TiO2 (∼0.5%) (Papiu et al., 1983).
In the Audia and Tarcău nappes, the hematite of the red levels is up to
3%, while in the green levels the hematite is less than 0.5%. Both red and
green levels contain terrigenous clay minerals, such as illite, kaolinite
and chlorite. After Papiu et al. (1983), some chlorites, at least those
occurring towards the lower part of CORB units, are produced by the
diagenetic weathering of the pyroclastic tuffs. However, the pyroclas-
tites are present only in the older parts of the CORB units (within the
Upper Albian–Cenomanian interval), while variegated couplets are
mainly present towards the upper part, within the Turonian–Coniacian
interval.
Vârban (2003) suggested that, at least for the CORBs of the Moldavid
outer structures (i.e., Vrancea Nappe), a primary depositional alterna-
tion of red shales and white limestones (mudstones and wackestones)
could be imagined. The above-mentioned author hypothesized that
the deposition of these couplets took place exclusively under oxic
conditions; as argues, he invoked the absence of any black shales and
pyrite and the presence of bioturbations both in the red and green terms
of the couplets. The iron oxide source is represented by continental
lateritic soils. During diagenesis, reducing interstitial fluids migrated
preferentially in the more permeable carbonate levels overprinting the
green colour.
During redox processes, the oxygenation should be produced by
oxygen-rich currents, which induced to the clastic material the red
colour by hematite formation. It is also possible that an arid climate of
those times led to the accumulation of red soils on emerged coastal
plains; transgression could have led to redeposition of sediments rich in
Fe-hydroxides into the marine environment, generating the CORBs that
are now preserved. We assume that the chlorites were oxidized on the
land at different intervals, related to short regional climate fluctuations,
resulting in the alternating red and green shales. A similar lithology
consisting of variegated red and green couplets may be produced by the
intermittent occurrence of bottom-oxygenated currents.
5.1.7. Pyroclastic tuffs
Pyroclastic tuffs were identified within the lower part of CORB units
(in the Bota–Botiţa and Cârnu–Şiclău formations of the Audia and,
87
respectively, Tarcău nappes). They occur as green-yellowish centi-
metre-thick strata, showing a good lateral continuity. The chemical
analysis indicates the following content (Papiu and Alexandrescu,
1976): SiO2 (75–91%), Al2O3 (3.5–8.5%), Fe2O3 (0.5–2.5%), FeO (0.7–1%),
CaO (0.1–0.4%), MgO (0.5–6%), K2O (0.5–1.5%), Na2O (0.1–0.5), TiO2
(0.1–0.4) and P2O5(0.02–0.7). The same authors identified in the
mineralogical composition: quartz and chalcedony (jointly amounting
66–87%), feldspars (1.8–5.25), illite (8.5–19%) and chlorite (2.20–8.2%).
Sporadically, pyrite also occurs.
Some authors assumed that the sources of these rocks are the calc-
alkaline magmatic eruptions of an island arc type (Rădulescu and
Dimitrescu, 1982). This volcanism was associated with the deformations
that took place at the end of the Lower Cretaceous in the Western
Transilvanids (Săndulescu, 1984), located now in the Apuseni Moun-
tains. The illite, kaolinite and the terrigenous clasts were transported
from the continent. After accumulation, the pyroclastites were involved
in diagentical processes. The resulted silica favoured the development of
the radiolarian communities (Papiu and Alexandrescu, 1976). The argil-
lization processes continued during middle and late diagenesis stages.
5.2. Palaeogeographic setting
The Moldavids, where the black shales accumulated during Early
Cretaceous times, constitute one of the largest nappe systems of the
Eastern Carpathians. The black shale deposition took place in a very
deep environment, on the abyssal plain of the Moldavian Trough, with
depths near the calcite compensation depth (CCD). The occurrence of
the black shales in the Eastern Carpathians is linked to the existence of
a narrow basin, formed on a thinned continental crust of the passive
northern margin of western Tethys Realm (Săndulescu et al., 1981;
Papiu et al., 1983). There, the anoxic to dysoxic bottom waters led to
the deposition of organic-rich black shales that accumulated at a low
rate, from 2 up to 5 cm/kyr (Ştefănescu and Melinte, 1996).
A similar Early Cretaceous tectonic setting as recorded in the
Eastern Carpathians characterizes the Silesian Nappe of the Outer
Polish Carpathians. This represents a deep, long trough, restricted
towards N by the Subsilesian Submerged Ridge and towards S by the
Silesian Ridge (Książkiewicz, 1975; Golonka et al., 2000). In this
trough, the Lower Cretaceous sediments were also deposited around
the CCD (Golonka et al., 2002).
Within the Albian–Cenomanian boundary interval, due to the
overthrusted processes, which affected the Outer and Marginal Dacids,
situated at the western part of the Moldavid Basin, and to the
appearance of flexural bulge zones (Bădescu, 2005), previously ascribed
to intrabasinal cordilleras (Murgeanu, 1937), the circulation pattern
changed in the Moldavian Trough. This modification is indicated by the
common presence of macroscopically visible authigenic glauconite in
the Albian sandstones of the Upper Member of the Audia Formation,
linked to the circulation, in the Moldavid Basin, of the oxygenated
turbidity currents. Towards the end of the Albian, the anoxic–dysoxic
regime (expressed by the deposition of the dark grey laminated shales
interbedded with glauconite sandstones) shifted to an oxic one (which
led to the occurrence of CORBs). In all Moldavid units, towards the end of
the Albian stage, black shales were progressively replaced by red shales.
In other European Tethyan regions, such as the central Italy, CORB
sedimentation started from in the Late Albian–Early Cenomanian
interval (Hu et al., 2006; Hu et al., 2009). In the Pieniny Klippen Belt of
the Polish Inner Carpathians (Bąk, 1998), as well as in the Rhenodanu-
bian Flysch Zone of Austria (Wagreich et al., 2006) the beginning of the
CORB sedimentation was in the Late Albian. A comparable setting of the
CORB deposition as recorded in the outer part of the Eastern Carpathians
was identified in the Polish Outer Carpathians, where Upper Cretaceous
red shales also directly overly the black shales (Bąk, 2006, 2007).
However, the duration of the CORB sedimentation is different in the sub-
basins of the Polish Outer Carpathians, where it was terminated by the
influx of terrigenous turbidites (Geroch et al., 1967), similarly to the
88 M.C. Melinte-Dobrinescu, R.-D. Roban / Sedimentary Geology 235 (2011) 79–90
Austrian Rhenodanubian Flysch (Wagreich et al., 2006). We may
suppose that the beginning and the end of the CORBs is not a global
event, but it depends of different palaeogeographic and palaeoenviron-
mental settings, being also driving by the regional tectonics and the basin
configuration.
6. Conclusions
In the Eastern Carpathians, black shales intercalated with carbonates
(marls and micrites) firstly appeared in the Valanginian, with the latter
rocks progressively diminishing up to the Aptian. During the Late
Valanginian–Late Barremian interval, carbonate hemipelagites and
pelagites, with rare siliceous rocks, accumulated in the Moldavids.
These sediments of an abyssal plain are interbedded with thin distal
siliciclastic and bioclastic turbidites. Taking into account the presence of
the green anchimetamorphic clasts of the turbidites, we may assume a
provenance from the East European Platform.
For the Late Barremian–Early Albian, a similar palaeoenvironmental
setting could be assumed, consisting of anoxic sedimentation in the
abyssal plain, with rare turbidites having the same eastern, outer, source
that is the East European Platform. Additionally, the occurrence of
siliceous deposits in the above-mentioned interval is possibly linked to
the shift of CCD depth, or the increasing subsidence, together with the
change in the bottom current circulation.
During the Early Albian–Late Albian interval, the pelagic sedimen-
tation shifted to a turbidite one. The anoxic–dysoxic environment is
replaced by a more oxic one, a change that is indicated by the rich
authigenic glauconite levels encountered in sandstones, implying the
presence of Fe3+.
A major modification in the depositional regime occurred within
the latest Albian, when red, non-calcareous shales, were deposited
above the black shales interbedded with glauconitic sandstones. The
deposition of the Upper Cretaceous red, mostly non-calcareous shales
is prevalent in all tectonic units of Moldavids and signifies a major
change from an anoxic or dysoxic environment to an oxic depositional
environment.
From the end of the Albian up to the Cenomanian, CORBs were
deposited as pelagic and hemipelagic sediments in the abyssal plain,
where red and green radiolarites, siliceous muds and thin pyroclas-
tites accumulated during fall out processes. Notably, dark grey shales
are still present in the lower part of the Moldavid CORB units. During
the upper part of the CORBs (the Turonian–Coniacian interval), a
decrease of the basin depth could be assumed. The pelagites and the
hemipelagites of the abyssal plain were progressively replaced by the
siliciclastic deposits of turbidite lobes. This change is also supported
by the fluctuation of foraminiferal assemblages. Within the lower part
of the CORB (i.e., Upper Albian–Upper Cenomanian), agglutinated
foraminiferal assemblages with “Rhizammina” sp. and few elements of
“Krasheninnikov fauna” (such as Praecystammina globigerinaeformis,
Recurvoidella insueta and Trochammina gyroidinaeformis) are indica-
tive of an abyssal paleoenvironment. Upwards in the CORB, within the
Upper Cenomanian–Lower Turonian interval, as the palaeoenviron-
ment shifted from the abyssal to the lower slope, the microfaunal
assemblages become dominated by the Recurvoides–Karrerulina–
Uvigerinammina. In the Upper Turonian–Coniacian CORB, the agglu-
tinated foraminiferal assemblages are dominated by Nothia sp., which
occur together with Recurvoides and Karrerulina taxa, suggesting a
lower slope palaeoenvironment.
To summarize, the identified lithofacies types suggest the presence
of two major coarsening upward sequences: (i) A Valanginian–Upper
Albian sequence, which contains in the lower part sediments deposited
in an abyssal plain, such as dark grey shales, siderites, cherts, marls and
limestones, with thin turbidites interbedded; the upper part is mainly
characterized by the presence of coarser turbidites, related to a middle
fan palaeoenvironment; (ii) An Upper Albian–Coniacian sequence,
which contains in its lower part deposits of an abyssal plain, such as
radiolarites, as well as red and green shales, alternating with thin
turbidites; the upper part mainly includes turbidites of an outer deep
water fan.
The presence of the above-mentioned sequences indicates that
major progradations took place in the Upper Albian and in the Lower
Coniacian intervals. These processes are related to the increase of the
sediment supply during the two above-mentioned intervals, or to the
decrease of the basin depth, by the migration of the depocentre. These
changes could be linked to the tectonic activity of those times,
especially to the Intra-Albian tectonic phase that was very intense in
the Eastern Carpathian area, including the Moldavids.
Probably many factors forced the worldwide change of the Early
Cretaceous anoxic conditions (represented by black shales) to the Late
Cretaceous oxic conditions, when CORB where deposited in the Tethys
(Jansa and Hu, 2009; Wagreich, 2009). The most common assump-
tions suggested changes in the ocean circulation, ocean chemistry,
bioproductivity, and climate. Study of the termination of the CORB
deposition in the Carpathian area placed in a foreground the influence
of regional factors, such as tectonics and regional palaeogeographic
setting. This conclusion emanates from our study demonstrating that
the CORB deposition began in the Eastern Carpathians during the Late
Albian only in the outer units (i.e., the Moldavids), effected regionally
by the intensification of mid-Cretaceous tectonic movements.
Acknowledgments
We thank to Dan Jipa (National Institute of Marine Geology and Geo-
ecology, GEOECOMAR Bucharest) for the fruitful discussion and
comments on an earlier version of this paper. The authors are also
indebted to Titus Brustur and Stefan-Andrei Szobotka (National Institute
of Marine Geology and Geo-ecology, Bucharest), for the assistance
during field trips in the Eastern Carpathians. This paper is a contribution
to the IGCP Project 555 ‘Rapid Environmental/Climate Change in the
Cretaceous Greenhouse World: Ocean–Land Interaction’. We are
thankful to Xiumian Hu for his helpful comments. The authors are
indebted to Luba Jansa and Robert Scott, who made useful suggestions
and improvements. We are indebted to Michael Wagreich, who made a
very useful and careful review that significantly improved this paper. We
thank the financial support of the Grant CNCSIS - Programme type
EUROCORES ESF no.2/2009 (integrating Project FROM SOURCE TO SINK-
A TOPO-EUROPE Collaborative Project).
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