Reworked marine sandstone concretions: a

record of high-frequency shallow burial to

exhumation cycles

F. García-García, R. Marfil, G. A. De

Gea, A. Delgado, A. Kobstädt, A. Santos
& E. Mayoral

Facies
International Journal of Paleontology,
Sedimentology and Geology

ISSN 0172-9179
Volume 59
Number 4

Facies (2013) 59:843-861

DOI 10.1007/s10347-012-0335-z

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 Author's personal copy
Facies (2013) 59:843–861
DOI 10.1007/s10347-012-0335-z
ORIGINAL ARTICLE
Reworked marine sandstone concretions: a record
of high-frequency shallow burial to exhumation cycles
F. Garcı́a-Garcı́a • R. Marfil • G. A. De Gea •
A. Delgado • A. Kobstädt • A. Santos •
E. Mayoral
Received: 3 July 2012 / Accepted: 5 October 2012 / Published online: 30 October 2012
Ó Springer-Verlag Berlin Heidelberg 2012
Abstract Concretions, with abundant calcite-dolomite
cement-replacement textures originally hosted in shallow-
marine sandstones, were reworked into Lower Cretaceous
fluvio-deltaic conglomerates and shoreface sandstones
(External Zones, Betic Cordillera). A cycle of host sand
deposition, early diagenetic concretion formation and
concretion reworking is documented: (1) Well-sorted
shoreface sandstone deposited. (2) Spherical to ovoid,
non-ferroan calcite-cemented concretions formed below
flooding surfaces at shallow-burial depths during early
eodiagenesis. Non-ferroan calcite cements were precipi-
tated from the bicarbonate derived from seawater and from
dissolution of marine bioclasts, as shown by isotope anal-
yses. (3) Concretions were reworked and exposed on the
seafloor in a high-energy setting as indicated by the pres-
ence of numerous bivalve borings (Entobia ichnofacies),
F. Garcı́a-Garcı́a (&)
G. A. De Gea
Dpt. de Geologı́a, Facultad de Ciencias Experimentales,
Universidad de Jaén, Campus Universitario, 23071 Jaén, Spain
e-mail: fegarcia@ujaen.es
R. Marfil
A. Kobstädt
Dpt. de Petrologı́a y Geoquı́mica, Facultad de Ciencias
Geológicas, Universidad Complutense, 28040 Madrid, Spain
A. Delgado
Laboratorio de Isótopos estables, Instituto Andaluz de Ciencias
de la Tierra (CSIC-UGR), 18100 Armilla, Granada, Spain
A. Kobstädt
Friedrich-Schiller-Universität Jena, Jena, Germany
A. Santos
E. Mayoral
Dpt. de Geodinámica y Paleontologı́a, Facultad de Ciencias
Experimentales, Universidad de Huelva, 21071 Huelva, Spain
laminated micritic microbial crusts around the concretions,
and epilithobionts (oysters, barnacles and corals) on the
concretion surface. Concretions also appear as erosional
remnants on the floor of channels which were incised into
the shoreline sandstone when sea-level fell. (4) The fluvio–
deltaic channels were filled with sediment during flooding
in the late lowstand of sea-level. (5) The concretions are
partly dolomitized, and the presence of siderite, pyrite and
barite in the outer part of the concretions precipitated
before the dolomite, suggests that the latter formed during
shallow burial.
Keywords Calcite-cemented concretions
Early
diagenesis
Hiatus concretions
Shoreface sandstones

Forced regressions
Sequence stratigraphy
Introduction
Concretions have attracted a long-term interest from
geologists, as well as gathering attention for an aesthetic
appreciation of their forms (Seilacher 2001). A variety of
scientific data has been derived from their study and the
information provided has been fundamental in under-
standing the early stages of diagenesis based on their
morphology and chemistry (trace elements and isotopes),
and the nature of the fluids involved and the petrophysical
properties of the original sediment (Bjorkum and
Walderhaug 1990; Abdel-Wahab and McBride 2001; Kra-
jewski and Luks 2003; McBride et al. 2003; Wanas 2008,
among others). The formation of concretions in marine
deposits has been linked to the petrophysical properties of
the original sediment and its ichnofossil content, as well as to
a typically low sedimentation rate, and, commonly, to a
connection with meteoric water associated with sea-level
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change. This has led to the linking of concretions to the
sequence stratigraphy of the succession (Taylor et al. 2000,
2004; Siggerud et al. 2000; Taylor and Gawthorpe 2003;
Machent et al. 2007) and relating different cementation
stages in the concretions to sea-level fluctuations (Coniglio
et al. 2000). Concretions may be reworked and colonized by
organisms (‘hiatus concretions’: i.e., concretions formed by
early cementation in predominantly siliciclastic sediments
which were subsequently reworked on to the seafloor, sensu
Voigt 1968). Palaeontological studies of concretions have
involved biostratigraphical, taphonomic, palaeoecological
and palaeoichnological data (Baird 1976; Hesselbo and
Palmer 1992; Doyle et al. 1998; Zaton 2010; Santos et al.
2011).
This paper provides a comprehensive study of concre-
tions from stratigraphic-sedimentological, palaeontological
and petrological–geochemical points of view to extract
information from these lithomarkers to reconstruct their
complex history. In addition to providing information on
their diagenesis, they also yield important data on sequence
stratigraphy, specifically on those stages with scarcely any
sedimentary record, such as sequence boundaries. The
concretions in this study from southern Spain record an
evolutionary history from their genesis within Lower
Cretaceous shoreface sandstones and their reworking into
younger fluvio–deltaic sandstones, to their burial diagene-
sis and later exposure on uplift.
Geological setting and sequence-stratigraphic
framework
The study section, located in the province of Jaén (southern
Spain), is within a Lower Cretaceous (Barremian to Early
Aptian) succession 160 m thick in the External Zones of
the Betic Cordillera (Fig. 1a). The succession consists of
six sharp-based forced-regressive shoreface sandstone
wedges (5–15 m thick). The sandstone packages abruptly
pinch out landwards into outer-ramp limestone and marl
(Los Villares Formation) (Fig. 1b–d). Sandstone tongues
were interpreted as deposits of prograding wave-dominated
shorefaces (LST—lowstand systems tract) distally evolv-
ing to thin micro-hummocky cross-stratified sandstone
beds alternating with marl deposited on a storm-wave
siliciclastic-dominated outer ramp (Fig. 1c) (Garcı́a-Garcı́a
et al. 2011). A plankton-rich marl-dominated deposit
overlying each sandstone package records the flooding of
these shoreface sandstones.
The tectonic structure of the study region is a large
anticlinal fold trending predominantly ENE–WSW and
verging slightly NW, cut by subvertical strike-slip faults.
The study section dips 55° north on the northwestern limb
of the fold structure.
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Samples and methods
The morphology, size, colour, grain-size, macro- and ichno-
fossil content, sedimentary structures, and distribution of
calcite-cemented concretions in the outcrop were recorded.
For the present study, several boulders were randomly
selected and their bioerosion structures identified, counted
and measured. The remains of bioeroding and encrusting
organisms were identified and counted. Bioerosional struc-
tures were measured using digital calipers. Composition of
the ichnocoenosis was determined on the basis of these data.
Fresh, unweathered 15–20 cm long cores of sandstone host-
rock and sandstone concretions (measured from the con-
cretion centre to the edge) were collected using a hand-held
coring machine. Thin-sections were prepared and polished
from 30 samples. The mineralogical composition of the
selected sandstones was determined by modal analysis (400
points per thin-section). The thin-sections were examined
under plane and cross-polarised light using an Olympus
BX51 microscope and an Olympus DP12 digital colour
camera. A semi-quantitative analysis of the mineralogical
composition was performed for all thin-sections in com-
parison with charts provided by Terry and Chilingar (1955).
CL petrography was undertaken on four polished thin-sec-
tions with a CITL Cold Cathodoluminescence 8200 MK4
(with an accelerating voltage of 12.5 kV and an intensity
of 200–280 lA) operated under standard conditions with
an intensity of 300–350 lm, an accelerating voltage of
12–16 kV, and 0.2–0.1 torr vacuum. To distinguish calcite
and dolomite, whole-rock sandstone samples were analysed
in the standard fashion by X-ray diffraction analysis (XRD)
using a Philips PW 1720 diffractometer equipped with
Cu(Ka) radiation. The evaluation was processed with the
Philips APD program. Cement textures, especially carbon-
ate, were investigated on carbon-coated polished thin-sec-
tions by scanning electron microscopy (SEM) and combined
qualitative chemical analyses (energy dispersive X-ray
microanalyzer, EDX) in secondary and backscattered elec-
tron modes with a JEOL JSM 6400. Eight representative
polished thin-sections were selected to determine quantita-
tively the mineral chemistry of the carbonates (93 analyses)
using a JEOL JXA-8900 electron microprobe (EMPA)
(15 kV accelerating voltage, 20 nA beam current, 5 lm
beam diameter). The detection limits are calculated as 2 s
background signals and are approximately 100 ppm for Mg,
150 ppm for Ca, 250 ppm for Mn, and 300 ppm for Fe. The
results were normalized to 100 mol% CaCO3, MgCO3,
FeCO3, SrO3, MnCO3. BSE images were recorded digitally
to visualize the zonation of carbonate cements.
Eleven samples were chosen for carbon and oxygen
stable isotope analysis. The measurements were carried out
by using a Delta XP (Thermo-Finnigan) mass spectrometer.
Samples containing mostly one dominant carbonate phase
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Facies (2013) 59:843–861
Fig. 1 a Location of the Betic Cordillera (grey) in the southern
Iberian Peninsula. b Geological map of the study area showing the
five conglomerate and sandstone shoreface wedges (1–5) hosting the
concretions (white arrows point to the wedge pinch-out) (modified
from Garcı́a-Garcı́a et al. 2011). c Correlation panel showing the
conglomerate and sandstone hosting the concretions. Note the incised
channels (a, b) filled by the concretions (logs are located in the
were preferentially selected. However, mixing of different
cement phases could not be entirely avoided. Those samples
containing both calcite and dolomite were treated according
to the Al-Aasm et al. (1990) method, which essentially
consists of three steps: (1) obtaining CO2 from calcite after
a 2 h reaction with phosphoric acid at 25 °C; (2) elimina-
tion of CO2 from residual calcite and, to a lesser extent,
from protodolomite-ankerite carbonates after reaction
between the insoluble residue and phosphoric acid over
24 h (at 25 °C); and (3) obtaining CO2 from dolomite by
reaction with phosphoric acid at 50 °C (12 h). The values
are reported as a percentage relative to the standard V-PDB.
Experimental error was less than 0.1 % for d 13C and d 18O.
All the samples were compared to a reference carbon
dioxide obtained from a calcite standard prepared at the
same time. The in-house standards Carrara and EEZ-1,
which have been previously compared with NBS-18 and
NBS-19, were used. The oxygen isotope ratios for dolomite
are calculated taking into account the fractionation factor
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map b). d Photograph of outcrop showing the 45° northward-dipping
folded section consisting of sandstone packages (1–6) alternating with
marl. Sandstone package bases are indicated. e Stratigraphic log 4
showing the distribution of sandstone concretions in the section (SB
4th-order sequence boundary and linked, FRWST forced-regression
wedge systems tract, LST lowstand systems tract, TST transgressive
systems tract, HST highstand systems tract)
for acid decomposition at 50 °C, 1.01057 for dolomite
(Rosenbaum and Sheppard 1986), and at 25 °C, 1.01044 for
calcite (Kim and O’Neil 1987).
Concretions in outcrop
Two types of concretion were distinguished on the basis of
two criteria: (1) whether they have colonized surfaces or not,
and (2) the type of host rock where the concretions occur:
(a) in the sandstone where they formed or (b) in sandy marl or
conglomerate into which they were reworked and deposited.
Concretions in their host sandstone
Description
The sandstone lithofacies forms amalgamated thickening-
upward, sharp-based units 5–15 m thick. Sandstone
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Fig. 2 Photo series from outcrop showing calcite-cemented concre-
tions in host sandstone (1st-sandstone package): a Spheroidal
coalesced concretions in the uppermost sandstone bed of a
thickening-upward shoreface sandstone-marl unit (Tu) (hammer for
scale), b spheroidal concretion 1 m in diameter. c Oval-shaped
concretion elongate in the bedding plane; beds thins towards the
packages abruptly pinch out landwards into outer-ramp
limestones and marls (see Fig. 1b, c). The average sand-
stone-to-silt ratio in this facies ranges from 1:1 in the lower
part to 10:1 in the upper part of the package. Sandstones
consist of low-angle cross-stratified or massive, medium-
grained well-sorted sands, which are friable. Sandstone
beds are poorly fossiliferous, containing organic material
such as coal and plant remains. The basal beds are nor-
mally-graded bioclastic grainstone to sandstone (less than
1 m thick). Mud clasts occur locally. The thickest and
uppermost sandstone bed of a thickening-upward unit,
below the overlying marl, commonly contains the calcite-
cemented concretions (see Fig. 2a).
The concretions range from 25 to 150 cm in diameter,
depending on the thickness of the host sandstone bed, and
they are roughly spherical (Fig. 2b) to horizontally elon-
gated (Fig. 2c). Globular and ovoid shapes are the most
common, although some of the concretions are hemi-
spherical. There are some clusters (Fig. 2d), but most
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proximal area (to the right), where the host sandstone bed pinches out
(hammer for scale). d A detail of (a) where clean, white, almost
spherical coalesced concretions elongate along the bedding plane
occur in a brown host sandstone bed (top to the left) interbedded with
marl. Note the left concretion flattened at the bed top (hammer for
scale)
concretions are semi-evenly spaced 1–3 m apart (centre to
centre). A row of clustered concretions and the longest axes
of elongate concretions are parallel to the bedding (see
Fig. 2c, d). No continuously cemented concretionary beds
occur. There are no visible concentric internal structures in
the concretions and no notable differences in composition
are observed from the cores to the concretion margins.
Some concretions preserve the original depositional low-
angle stratification, commonly marked by mud clasts. In
just one concretion was a 15 cm long mud clast found in
the core; otherwise, there do not appear to be any nuclei.
Interpretation
The approximately spherical shapes of the concretions
suggest that they formed at relatively shallow depth, where
sedimentation was rapid and before any compaction of the
sediment had taken place (Seilacher 2001). Concretion
morphologies are controlled by the petrophysics (especially
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Facies (2013) 59:843–861
permeability) of the host sediment so that in isotropic
sediments (sands and muds), concretions are normally
spherical if formed before compaction (see Fig. 2b); hori-
zontally-elongated ellipsoidal concretions tend to form
during compaction (permeability becomes reduced in the
vertical direction) (see Fig. 2c), and concretions with flat-
tened lower or upper faces (bread-loaf concretions, see
Fig. 2d) form when sedimentation rate was low and there
was a steep compactional gradient (Seilacher 2001). Con-
cretion size appears to be strongly controlled by sandstone
bed thickness. Flattening of the concretions parallel with
bedding is a natural consequence of diffusion-controlled
growth in a system where bioclastic carbonate is concen-
trated in layers (Bjorkum and Walderhaug 1990).
Reworked concretions
Description
Two groups of reworked concretion are distinguished on
the basis of the host sediment: (1) fine-grained sediment
and (2) conglomerate. The two types are laterally and
vertically related (see distribution in log of Fig. 1c).
(1) Reworked concretions in conglomerate Channels up
to 8 m deep (see Fig. 3a) and from 100 to 500 m wide (see
Fig. 2d) have been eroded into underlying sandstone and
filled with conglomerate. Clasts are well segregated in that
boulder- and cobble-sized clasts occur in the lower part of
the bed, pebbles in the middle part, and granules in the
upper part. Beds are characterized by normal grading and
the clasts are matrix-supported (locally clast-supported).
Clasts mainly consist of limestone pebbles (1–50 cm in
diameter) and spherical concretions (35–100 cm in diam-
eter), minor quartzite, and chert. Spherical concretions
chiefly occur in the lower part of the channel fill (Fig. 3a).
Some outsized angular sandstone clasts (2–4 m in diame-
ter) are present (Fig. 3b). Bivalves occur in the pebbly
matrix.
(2) Reworked concretions in fine-grained sediment This
facies is composed of marl, several hundreds of metres in
lateral extent, that contains a single layer of concretions.
Concretions are highly spherical (Fig. 3c), although some
have a gently flattened downward face; they are spaced
uniformly from 2 to 4 m apart. The most characteristic
feature of these reworked concretions is that their surfaces
are intensely bored by bivalves represented by three ich-
nospecies of Gastrochaenolites: G. torpedo (Kelly and
Bromley, 1984), G. lapidicus (Kelly and Bromley, 1984)
and G. ornatus (Kelly and Bromley, 1984) (Fig. 4a–c). In
some concretions, at least 70 per cent of their exposed
surface is bioeroded in this way. The borings appear on the
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upper faces of the hemispherical concretions (not on the
lower planar surface) and around the lateral surface. Gas-
trochaenolites is the only ichnotaxon present, and it is
fairly evenly distributed over the surfaces at approximately
320 individuals per square metre. All Gastrochaenolites
are perpendicular to the surface. The ichnospecies G. la-
pidicus is the most common, whereas G. torpedo makes up
about 20 % of the borings. The average cross-section of the
circular structures is 1.3 cm. Where G. lapidicus is well
preserved the length reaches 9 cm, the apertural width is
1.5 cm, the main chamber is 3.9 cm, and the neck is
3.6 cm long. G. torpedo has an aperture width between
1.2–2.1 cm and a length between 10.1–13.9 cm. Where the
density of Gastrochaenolites is high, crossovers occur
either between G. torpedo and G. lapidicus (Fig. 4c) or just
between G. lapidicus (Fig. 4d). In almost all cases, the
upper parts of the borings have been truncated by marine
erosion (Fig. 4a), and it can be estimated that 80 % of the
total length of a boring has been eroded, implying a
reduction of 6–10 cm in relation to the original boring.
The surfaces of some concretions are extensively cov-
ered by a red iron-oxide mineral coating several millime-
tres in thickness (Fig. 5a). This iron crust also coats the
insides of the borings. The encrusting epibiota on these
reworked concretions, includes Ostrea sp., barnacles
(Balanus sp.) (Fig. 5b) and corals (Fig. 5c). The valves of
Ostrea, both those cemented directly on the substrate and
those found inside the borings, are always disarticulated
and some are penetrated with borings produced by clionid
sponges (Entobia) (Fig. 5d).
Interpretation: The bioeroded surface of the reworked
concretions with its rockground biota has an impoverished
ichno-assemblage of bioerosion structures composed
exclusively of truncated Gastrochaenolites borings (Fig. 6a).
More delicate bioerosion structures, such as Caulostrepsis
Clarke (1908) or Maeandropolydora Voigt (1968) (see
e.g., Lee et al. 1997; de Gibert et al. 1998; Santos et al.
2011), are absent. This impoverished bioerosion ichno-
assemblage corresponds to the Entobia ichnofacies of
Bromley and Asgaard (1993), and is typical of hard, lithified
surfaces associated with rocky shores. Bivalve borings were
the first colonizers to develop after the concretions were
reworked. The shallowness of most of the truncated Gas-
trochaenolites suggests that any other bioerosion structures
on the surface would have been eroded away by the strong
marine corrasion (Santos et al. 2008). Cross-cutting rela-
tionships between Gastrochaenolites support the argument
for the existence of at least two phases of colonization of the
substrates (Fig. 6a, b). The distribution of borings all
around the spherical concretions indicates they were rotated
regularly. Borings only occurring around the convex-up
surface of the hemispherical concretions (not on the lower
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Fig. 3 a Incised channel in shoreface sandstone filled by normal-
graded limestone pebbles (allochthonous clasts) and bored sandstone
concretions. b Angular and partly bored outsized sandstone clast in
planar surface) indicate that flat concretions were not
moved. The preservation of the Gastrochaenolites and the
taphonomic characteristics of the epilithobiont fauna indi-
cate strong erosion under high-energy conditions (Fig. 6c).
After the boring activity, an important erosive event
reduced the depth of the borings by up to 80 %.
The friable, poorly-cemented host sandstone between
the concretions was winnowed out by waves and currents.
The erosion of the concretions could have been facilitated
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conglomerate consisting of allochthonous Jurassic limestone clasts.
c Bored sandstone concretion isolated in pelagic marl
by crustaceans that excavated dwelling burrows within the
poorly cemented sands adjacent to the concretion edge
(Hesselbo and Palmer 1992). The intense bioerosion of the
concretions indicates a lengthy time of exposure on the
seafloor in a shallow-marine setting. There was probably
also a delay in the input of coarse sediment from local
rivers. The limestone clasts in the conglomerate are rarely
bioeroded or encrusted, suggesting rapid deposition and
burial compared to the reworked concretions.
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Facies (2013) 59:843–861
Fig. 4 Photo series from outcrop showing colonized calcite-cemented
concretions weathered out of their host sandstone: a Dense Gastro-
chaenolites lapidicus borings on the concretion surface. Dashed line
marks the boundary between the bored area (seafloor-exposed area) and
non-bored area (buried sandstone) (hammer for scale). b Detail of
Sandstone petrography and geochemistry of cements
Concretions and host sandstones are remarkably similar in
petrographic and isotopic character.
Sandstone petrography
Detrital mineralogy
The sandstone is mainly arkose and subarkose (Fig. 7a, b).
The dominant grain-type is monocrystalline quartz
(55–65 %), followed by polycrystalline quartz (5–10 %)
and chert (\5 %). K-feldspar ranges from 18 to 23 % and
plagioclase from 1 to 2 %. The intrabasinal carbonate
grains (micritic—microsparitic and fossiliferous grains)
range from 5 to 10 % and muscovite from 1 to 2 %. Some
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bivalve borings (Gastrochaenolites lapidicus). c Large-scale vertical
Gastrochaenolites torpedo boring crossed by G. lapidicus (white
dashed lines). d Gastrochaenolites lapidicus borings crossing each
other (white arrows)
zones, especially the concretion rims, have very red, oxi-
dized grains and particle relics that may possibly be
microbial (Fig. 7c, d). In all samples, a small amount of
metamorphic rock fragments can be recognized. Most
clasts can be classified as low-grade metamorphic and
consist mostly of phyllite and metaquartzite. Accessory
detrital components comprise biotite and heavy minerals,
mostly consisting of zircon and tourmaline. In addition,
bioclasts present include bivalves, brachiopods, ostracods,
foraminifera, ooids and peloids.
In general, the sandstone is medium- to fine-grained,
with the most common grain diameters ranging from 80 to
125 lm. A minority of samples have a bimodal grain-size
distribution, in general where they are in contact with more
micritic zones of the concretions. Most sandstone is mod-
erately to well sorted and shows angular to subangular
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Fig. 5 a Highly ferruginous concretion with a red iron-oxide cap
several millimetres in thickness (camera cap for scale). b Encrusting
organisms on the concretion surface. Black arrows oysters, white
arrow barnacles. c A coral colony cemented to the exposed surface of
grains with low sphericity. On average, floating grains and
isolated contacts are the most abundant grain contacts
(Fig. 7a, b). Detrital quartz and feldspar grains are locally
corroded by carbonate cement. Textural evidence from CL
implies that detrital feldspars were partly affected by cal-
cite replacement, albitization and minor dissolution
(Fig. 7a, b). The loss of porosity is mainly caused by cal-
cite cement-replacement and mechanical compaction,
principally of the micritic carbonate grains, whereas the
siliciclastic grains are floating. Porosities derived from
semi-quantitative determinations range from 1 to 2 %.
Microfractures and microporosity in micritic material
provide slightly higher porosity levels.
Authigenic mineralogy
A range of authigenic minerals includes carbonates (calcite
and dolomite), pyrite (Fig. 7e), Fe-oxides, barite (Fig. 7f),
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a concretion (camera cap for scale). d Detail of an oyster showing
Entobia borings (black arrows) inside an eroded Gastrochaenolites
lapidicus. Scale bar 1 cm
phosphate, rare peloids of glauconite, illite and kaolinite.
Illite appears as epimatrix replacing feldspars. K-feldspar
overgrowths are locally detected under CL (Fig. 7b).
Albitization of feldspars is also observed under CL
(Fig. 7b). Quartz cement occurs rarely (1–3 %) and it
forms syntaxial overgrowths generally showing some
subrounded faces indicating a probable inherited origin.
Euhedral prismatic crystals of quartz are rare. Fe-oxides are
commonly associated with dolomite, later affected by
dedolomitization (Fig. 8a, b). The Fe-oxides are very
scarce or absent in sandstone cemented only by poikilo-
topic calcite. However, in most samples of the concretion
rims, Fe-oxides appear as aggregate-like clusters in the
intergranular pore space of former carbonate cement, as
mineral coatings, along crystal edges inside dolomite
cement crystals, and replacing organic remains (Fig. 8a, b).
Fine, dispersed leaflets of Fe-oxide occur on a sub-lm
scale and reach 10 vol% in some instances. Barite is
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Facies (2013) 59:843–861
Fig. 6 Reconstructed sequence of events affecting sandstone con-
cretions exposed as boulders prior their final burial. a Bioerosion
event: 1 Gastrochaenolites lapidicus; 2 Gastrochaenolites torpedo.
b Second bioerosion event. G. lapidicus crossing previous bivalve
borings. c Physical erosion event. All Gastrochaenolites were
strongly eroded and reduced to 80 % of their initial size. d Encrusting
locally found as rounded grains, but also as an authigenic
phase (0.05–2 %); it is present as aggregates replacing
organic matter in the rims of concretions (Fig. 7f). Kao-
linite is scarce and only found in a few samples as a trace
constituent, usually enclosed in poikilotopic calcite
cement. It is faintly distinguished by SEM (Fig. 8c) and
EMPA analyses. Kaolinite normally appears in secondary
pore spaces, possibly replacing detrital feldspars, and
crystal sizes reach no more than 5 lm.
Authigenic carbonates are the dominant pore-filling
cement and include calcite and dolomite (Fig. 8a–c). Barite
cement is relatively common in the marginal zones of the
concretions.
Calcite cements Calcite is the most common authigenic
mineral (20–40 vol%) (Table 1). Four calcite phases are
recognized: (1) poikilotopic cement (Fig. 8d); (2) micro-
sparitization of former carbonate intraclasts (Figs. 7a, b,
8d, e); (3) calcite replacement resulting from dedolomiti-
zation of internal zones of dolomite (Fig. 8f); and (4)
calcite filling cavities. Type (1) calcite cement mostly
occludes the pore space with a poikilotopic texture forming
crystals of 50–150 lm. This phase is volumetrically the
851
event. 3 oysters, 4 corals, 5 barnacles. A red iron-oxide cap (brown
layer) was precipitated. e New erosion event. Disarticulation of
oysters and removal of the barnacles’ plates. f Third erosion event.
Clionid sponges occupied the inside valves of oyster to develop
Entobia borings (6)
most important and usually forms *90 % of all the calcite
cement. Floating grains are slightly deformed and cemen-
ted by this type of calcite (Fig. 8e). However, a clear
separation between different generations of poikilotopic
calcite is not possible. Under CL, this calcite shows a dark
red to reddish-orange luminescence (Fig. 8e). The mi-
crosparitic calcite (type 2 calcite) commonly has slight
orange-ish-yellow luminescence (Figs. 7b, 8a, b). Type (3)
calcite cement replaces authigenic dolomite where regular
zoning is visible under BSE microscopy; under CL it is
very dark (Fig. 9b) due to the low Mn and high Fe con-
tents, as the chemical analyses and the SEM images show
(Figs. 9c, d). In some samples, calcite cement type (4)
forms palisade-like or micro-sparitic patches in the last
cavities in an advanced phase of precipitation. Under CL,
this cement is zoned orange and yellow. In the centre of the
concretions, type (2) microsparite and subordinate patches
of poikilotopic calcite are the most widespread. However,
calcite types (1) and (3) are most abundant near the mar-
gins of the concretions. The average composition of pore-
filling calcites ranges from Ca0.98Mg0.01Fe0.01CO3 to
Ca0.91Mg0.04Fe0.05CO3 (Table 1). Usually the manganese
and strontium contents are close to their detection limits
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852
Fig. 7 a, b Thin-section photomicrograph (crossed polars and
cathodoluminescent image of the same area showing early orange
calcite cement replacement in an arkosic sandstone at the centre of the
concretions. Notice one of the K-feldspars showing dark overgrowths
under CL. c, d BSE images of the concretion margin between
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Facies (2013) 59:843–861
sandstone and sandy marl showing oxidized microbial organic matter.
e BSE image of the concretion margin enclosing framboidal pyrite in
poikilotopic calcite cement. f BSE image of barite crystals replacing
organic matter in the sandy marl of the concretion margin
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Facies (2013) 59:843–861
Fig. 8 a Thin-section photomicrograph (crossed polars) of dolomi-
tized arkosic sandstone showing several rhombohedral crystals
including Fe-oxides on their growing edges. b Detail in BSE of the
zoned dolomite crystals, showing dolomite core and Fe-oxide
included in the outer faces. c BSE image of dedolomitized grains
showing faint zoned dolomite bands with low Mg contents. Detrital
tourmaline enclosed in the dedolomitized zone and the replacement of
853
kaolinite fibres for the last calcite cement is visible in the bottom right
of the image. d, e Thin-section photomicrograph (crossed polars) and
cathodoluminescent image of the central part of a concretion showing
poikilotopic calcite cement with orange luminescence (and some
yellow patches). f BSE image of the concretion border showing
generalized calcite cores rich in Fe-oxides, one narrow zone of
dolomite, and one last phase of calcite cement
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854 Facies (2013) 59:843–861

Table 1 Chemical composition of representative carbonate compo- The outer part or external rim is slightly depleted in mag-
nents of the concretions determined by microprobe analyses (in mole nesium and iron. Intraclasts replaced by calcite show a very
percentage)
pure composition of CaCO3. There are no systematic dif-
Concretions CO3 ferences between analysed calcite samples from different
Ca Mg Fe Mn Sr locations within the concretions.

Calcite cement Dolomite cement-replacement Dolomitized zones in the

Poikilotopic concretions are located in the marginal areas and are
Average 97.6 1.1 1.1 \d.I. 0.2 related to remains of microbial organic matter. They have
Minimum 91.4 0.2 \d.I. \d.I. \d.I. significant Fe contents that were derived from original
Maximum 99.6 3.7 5.3 0.3 0.8 pyrite and siderite precipitates. Barite cement replace-
Zoned ments of organic matter and scarce phosphate are also
Average 96.5 3.0 0.3 0.1 0.1 present. The appearance of dolomite varies considerably,
Minimum 95.2 0.4 0.2 \d.I. 0.1 but where found this cement ranges from (5 to 15 vol%).
Maximum 99.1 4.4 5.3 0.2 0.2 Dolomite occurs as a pore-fill, composed of euhedral
Core crystals locally interspersed with opaque inclusions
Average 94.2 4.4 1.3 \d.I. 0.1 (Fig. 9a). Early dolomite has replaced carbonate and feld-
Minimum 87.4 2.5 0.2 \d.I. 0.1 spar grains. Dolomite post-dates mechanical compaction
Maximum 97.0 10.1 2.9 \d.I. 0.1 and predates the last calcite cement (type 4). The rhombo-
Rim hedral dolomite is clearly zoned, showing a calcite core and
Average 96.4 3.2 0.3 \d.I. 0.1 usually one dolomite zone including Fe-oxides on the
Minimum 95.7 2.4 0.2 \d.I. 0.1 growing edges. Under CL it is dark or non-luminescent
Maximum 97.3 3.9 0.3 \d.I. 0.1 (Fig. 9b) due to the low concentration in Mn (\25 ppm)
Replacive and the high or variable Fe content as the main quencher
Average 99.9 0.1 \d.I. \d.I. \d.I. (Budd et al. 2000). The dominant dark luminescence of
Minimum 99.8 0.1 \d.I. \d.I. \d.I. the dolomite cement-replacement (Fig. 9b), punctuated by
Maximum 99.9 0.1 \d.I. \d.I. \d.I. the hairline-thin brightness of faintly luminescent zones,
Components suggests very low concentrations of Mn. The chemical
Micritic composition of dolomite is (Mg0.40Fe0.03Ca0.56)CO3,
Average 98.8 0.8 0.3 \d.I. 0.1
generally has iron contents up to 5.3 mol% FeCO3 and an
Minimum 98.6 0.5 0.2 \d.I. \d.I.
average of 3.4 mol%. The magnesium contents range
Maximum 99.0 1.2 0.5 \d.I. 0.2
between 27.0 and 45.0 mol% MgCO3. Manganese and
strontium are below the detection limit. Figure 9d shows
Bioclasts
growth zones which are separated by ferric iron layers.
Average 98.7 0.7 0.5 \d.I. 0.1
Semi-quantitative analyses of zoned dolomite, calcite
Minimum 98.7 0.7 0.4 \d.I. 0.1
core, and oxidized organic matter (hematite) are shown in
Maximum 98.8 0.7 0.5 \d.I. 0.1
Fig. 9e.
Dolomite cement
Rhombohedral
Diagenetic sequence
Average 56.4 40.1 3.4 \d.I. 0.1
Minimum 53.5 27.0 0.8 \d.I. 0.1
The sequence for the formation of concretions and asso-
Maximum 70.0 45.0 5.3 0.1 0.2
ciated authigenic minerals is as follows: (1) The poikilo-
\d.l. below detection limit topic calcite cement-replacement occurred in the first stage
of eodiagenesis at shallow burial and under suboxic geo-
chemical conditions (some grains of phosphatized and
(Table 1). Some samples show a trend towards increasing glauconitized fossils are present); (2) As a result of the
Mn (up to 0.3 mol% MnCO3) and Sr contents (up to presence of organic matter and microbial laminated crust,
0.8 mol% SrCO3) during crystal growth. Barium in the siderite and pyrite precipitation occurred, as the SEM
different phases of calcite cement is mostly below the images and BSE analyses show in the marginal zones of
EMPA detection limit. Calcite replacing former dolo- the concretions. This stage was probably in the sulphate-
mite rhombs has a variable composition. The core of these reduction zone of eodiagenesis; (3) The beginning of
rhombs has an obvious signature from the previous dolo- dolomitization of the concretions and formation of barite
mite and an average composition of Ca0.94Mg0.05Fe0.01CO3. cement occurred slightly later, but still during shallow

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Facies (2013) 59:843–861
Fig. 9 a, b Thin-section photomicrograph (crossed polars) and cathod-
oluminescent image of a dolomitized concretion border under CL
showing reddish-orange carbonate grains and dark dolomite cement
visible only from the idiomorphic rhomboidal edges. c, d BSE images of
the concretion border showing the abundant Fe-oxides deposited in pores
burial; (4) During the reworking of the concretions (telo-
diagenesis stage) dedolomitization occurred. The calcite
precipitated then has a higher Fe-oxide content and a red
855
between the grains and intercalated in the dolomite growth lines. e BSE
image and semi-quantitative analyses of a zoned dolomite crystal
showing the different composition of the calcite core (1B) with low
contents in Fe and Mg and other zones, close to the quartz grain (1C), very
rich in Fe-oxides. The dolomite zone (1A) is also rich in Fe-oxides
colour. The diagenetic sequence of the authigenic minerals
and also the geochemical conditions of formation are
shown in Table 3.
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856 Facies (2013) 59:843–861

Table 2 Stable carbon and oxygen isotopic data for calcite and dolomite cements in the concretions (and a concretion-attached oyster shell)
Sample Concretion type Calcite Dolomite
13 18
d C % (V-PDB) d O % (V-PDB) d13C % (V-PDB) d18O % (V-PDB)

1st sandstone package

SC-4 In situ (b) -1.70 -1.48 -2.62 -6.03
SC-1B In situ (b) -1.92 -2.17 -2.00 -3.89
CU11-4 In situ (b) -1.08 -2.32 0.52 -5.70
CU11-5 In situ (n) -1.55 0.66
CU11-6 In situ (m) -2.06 -3.53
CU11-7 In situ (b) -1.90 -3.63 -3.16 -4.49
Exhumed package
CU11-8 Recycled (b) -0.83 -6.47 -1.32 -7.65
CU11-5 Recycled (b) -1.55 -3.04 -1.70 -4.12
CU11-2 In situ (b) -1.03 -3.90 -0.86 -4.89
CU11-3 In situ (b) -1.34 -3.57 0.99 -5.15
SC-7C Oyster shell (b) -0.49 -0.24
Nucleus, middle and marginal samples represent different locations of samples in a 1 m-diameter spheroidal concretion
n nucleus of concretion, m middle part of concretion, b concretion border

Table 3 Interpretation of concretion history during a high-frequency (4th order) cycle related to sea-level fluctuations
Sample Pore
Petrography
Concretion Key location Diagenetic water Fossils/
Host rock Morphology cement-replacement Geochemistry Sea-level Timing
type facies in stage cement ichnofossils
mineralogy texture
concretion origin
non- micro-
ferroan sparite, shallow burial
spherical centre High HCO 3- marine
calcite, poikilotopic (suboxic stage)
phosphate cement
pyrite
eodiagenesis,
crystals microbial
sulphate
petrofacies and Fe2+, S sulphate
non- reduction zone
and framboids, reduction
exhumated sandstone flooding
horizontally- geochemical siderite
concretion

4th-order cycle (above 200 kyr)

elongated to facies
zoned, 2+
flattened dolomite Fe
rhombohedral
side eodiagenesis
barite, To marine
poikilotopic
margin ferroan mesodiagenesis
mosaic +2 +3
calcite Fe to Fe
cement
Gastrochaenolites
entobia
exhumed sandstone or shell
attached oysters, falling sea
in situ sandy marl any shape biofacies calcite exhumation
level
concretion barnacles and
corals

erosional
remnants lowest sea
reworked conglomerate mainly
within level to
concretion spherical
incised transgressive
channel

Light grey concretion formation, white exhumation event, dark grey concretion reburial. Petrographic. geochemical and environmental factors of
each stage are shown

Carbon and oxygen isotopes
The stable oxygen and carbon isotopes (d18O and d13C) of
calcite and dolomite were determined in cements of two
groups of concretions: (1) in situ concretions located in
the first sandstone package, and (2) reworked concretions
(in host marl or conglomerate) (Fig. 10). The d18O isotopic
data show relatively variable values for both calcite (0.66
to -6.47 % V-PDB) and dolomite (-0.69 to -7.65 %
V-PDB), with the majority of values in the range of -3 to
-4 % (Table 2). Carbon values cluster around -1.5 %.
Isotopic values within a concretion (see n, m, and b values
in Fig. 10) display a trend of more negative d18O values
from the core to the margin. The d18O values of the

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Facies (2013) 59:843–861
Fig. 10 Cross-plot of d13C
versus d18O for calcite and
dolomite cements in the
concretions (n, m, b—nucleus,
middle part, and margin,
respectively, of a 1 m-diameter
in situ concretion from the 1st
sandstone package)
dolomite (-0.69 to -7.65 % vs. V-PDB) are variable with
d13C values less dispersed (Table 2; Fig. 10).
Interpretation
d18O and d13C values from the concretion core cements are
the most similar to the isotopic values obtained from sea-
water (represented by the oyster shell isotope signatures,
Fig. 10). The d18O data are similar to that of shallow burial
calcite cement from slightly modified, marine-derived
pore-water of siliciclastic deposits (Wanas 2008). The
isotopic values from the concretion core cement indicate
that the concretions started to grow during early and
shallow burial. The d13C data of calcite cements around
-1.5 % may indicate a calcite cement source from bicar-
bonate supplied from seawater and dissolution of marine
bioclasts (Wanas 2008). There is agreement that nucleation
occurs in shell-rich layers by diagenetic redistribution of
calcareous fossils originally contained in marine sand-
stones (Bjorkum and Walderhaug 1990; Abdel-Wahab and
McBride 2001).
Discussion: concretion history and sequence
stratigraphy
Sequence stratigraphic setting of the concretions
The history of the calcite-cemented concretions in shallow-
marine sandstones has been interpreted from a compre-
hensive study of their facies context, petrographic and
geochemical data, and microstratigraphy of the reworked
features on the concretion surfaces. Several phases can be
857
recognized in the complex history of the concretions: (1)
host sandstone sedimentation (Fig. 11a); (2) concretion
formation (Fig. 11b); (3) reworking of concretions; (4)
concretion colonization by hard-substrate boring organisms
(Fig. 11c); and (5) encrustation, disarticulation and bioe-
rosion prior to the final burial (Figs. 11d, e). The phases of
reworked concretion formation are described into a
sequence stratigraphy setting following nomenclature in
Catuneanu et al. (2011).
Host sandstone sedimentation (forced regressive or 1st
falling stage parasequence—FSST) and concretion growth
(flooding stage)
Although calcite-cemented sandstone concretions have
been reported in sediments from different depositional
systems, most concretions have been documented in shal-
low-marine progradational sandstone sequences with int-
erbedded mudstones interpreted as shelf-margin deltas,
wave-dominated deltas, and shoreface wedges, as in this
study (Fitzsimmons and Johnson 2000; Bhattacharya and
Willis 2001; McBride et al. 2003; Machent et al. 2007;
Garcı́a-Garcı́a et al. 2011). Only occasionally have they
been documented in fluvial sandstones (McBride and
Milliken 2006). The sedimentological and petrographic
features of forced-regressive shoreface sands (falling-stage
parasequence) favoured the formation of these diagenetic
concretions: clean and well-sorted (therefore presumably
with high porosity and permeability) sandstones overlying
mudstones (see McBride et al. 2003; Wanas 2008) with
abundant carbonate bioclasts. Concretions mainly occur at
the top of the thickening-upward sandstone units of
shoreface wedges overlain by transgressive marls (Fig 11a,
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858
Fig. 11 Sketches showing the different stages of concretion history
and sequence stratigraphic implications: a Deposition of host sand-
stones in shoreface settings during the lowstand sea-level stage. b Early
diagenetic concretions formed in shoreface sandstones below a flooding
surface. c Exhumation of concretions and formation of a coastal
pavement of concretions bored by Lithophaga and cannibalization of
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Facies (2013) 59:843–861
the layer of concretions that fell and rolled (mainly the spherical
concretions) into incised channels from the channel wall. d Fluvial to
deltaic currents transporting allochthonous clasts filled and overflowed
the incised channels during a new lowstand sea-level stage. e Burial of
concretions and filled incised channels with overlying basinal marl
deposited during the flooding stage
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Facies (2013) 59:843–861
b). Calcite cementation is promoted by long-term residence
in shallow-burial anaerobic diagenetic zones, a condition
met beneath flooding surfaces (Taylor et al. 2000) when the
sedimentation rate is generally low. Slow deposition also
provides time to dissolve marine shells and for the bicar-
bonate to be precipitated as calcite cement (Taylor et al.
2000; McBride et al. 2003). In lower shoreface to offshore
transition successions, early cementation associated with
flooding surfaces, followed by continued cementation
during burial, were the predominant cementation mecha-
nisms (Machent et al. 2007).
Sea-level fall and concretion exhumation: Boring
and encrustation
The falling stage is represented by a surface of erosion
cutting into the upper part of the preceding falling-stage
parasequence. Sea level was lowered below the top of the
previous shoreface sandstone package (1st FSST). The
reworking occurred when sea level fell below the brink
point or offlap break of the prograding shoreface sigmoids.
The fully-cemented concretions at the top of the shoreface
sandstone package were reworked into a shoreline setting
and bored and encrusted on the seafloor (Fig. 11c, d). The
exhumation of the concretions confirms that these struc-
tures must have originated during early diagenesis at
shallow depth. Bored spherical concretions fell from the
channel walls on to the channel floor. The bored spherical
sandstone concretions come from the layers of concretions
exhumed in the earlier stages of incision.
Allochthonous clasts of Jurassic limestone fill the incised
channels. The channel-filling fluvio-deltaic conglomerates
laterally onlap layers of concretions not cannibalized by the
incision surface (granule sediment filling borings in the
concretions). The channel-fills represent the lowstand sys-
tems tract deposits (Fig. 11d), before the overlying trans-
gressive (TST) marls were deposited (Fig. 11e).
Bored, encrusted and granule-attached isolated concre-
tions embedded in marl represent the remains of the
sequence boundary discontinuity; they are the key to the
recognition of a ‘shale-on-shale’ erosion surface sensu
Baird (1976). Thus, the recognition of layers of reworked
concretions (‘hiatus concretions’) in the subsurface, and
their implications for the cementation history, can be used
to evaluate the potential of shoreface sandstones as
hydrocarbon reservoirs.
Timing of the reworked concretion formation
In the study of concretions it is of interest to know the
duration and rate of growth (Wilkinson and Dampier
1990). Theoretical models to determine the time for the
growth of large concretions are not easy to apply since
859
there are many unknown variables (Abdel-Wahab and
McBride 2001; McBride et al. 2003). Therefore, the issue
can only be addressed by indirect means. According to
Berner (1968), the growth rate (k) for a concretion depends
on the square of its radius (m) and the time of growth (Ma)
(where k = t/r2). Available biostratigraphic data from
nannofossils and, locally, planktonic foraminifera and
ammonites from the section where these Cretaceous con-
cretions occur (see de Gea 2004; Garcı́a-Garcı́a et al. 2011
and log in Fig. 1 from this paper) allow an estimation of a
maximum of just over 1 Ma for deposition during the
Latest Barremian–Earliest Aptian interval (uppermost part
of the Micrantholithus hoschulzii Zone and the earliest part
of the Hayesites irregularis nannofossil Zone). If the sed-
imentation rate was uniform, layers of reworked concre-
tions (concretions resulting from a cycle of formation and
exhumation) in each sandstone package developed during
fourth-order fall-to-rise cycles of relative sea-level change
in the 200 ky range (Garcı́a-Garcı́a et al. 2011). Therefore,
the constant growth rate (k) of 0.5–1 m diameter concre-
tions is between 3.2 and 0.8, and this is in agreement with
recently estimated growth rates (Abdel-Wahab and
McBride 2001; McBride et al. 2003). Biostratigraphic data
confirm the close relationship between concretions and
high-frequency sea-level fluctuations (Coniglio et al. 2000;
Taylor and Gawthorpe 2003).
Conclusions
Calcite-cemented concretions in marine sandstones can
represent lithomarkers recording high-frequency (fourth-
order) shallow burial to exhumation cycles. Concretions
typically form during early diagenesis and, if reworked
during a subsequent sea-level fall, they can be used to
identify sequence boundaries (‘hiatus-concretions’).
An integrated analysis (stratigraphic, sedimentological,
palaeontological, petrographic and geochemical) of con-
cretions is necessary to reconstruct their complex history.
The history of the reworked concretions described here
involved the following stages: (1) concretion formation
within forced-regressive shoreface sandstones by calcite
cement derived from marine pore seawater (no meteoric
water isotopic signal was found in calcite cement) and
skeletal carbonates shortly after burial, encouraged by a
low sedimentation rate during flooding, (2) reworking of
the concretions occurred when sea level fell below the top
of shoreface sandstones, (3) incision by channels exposed
the concretions such that they accumulated on the floor of
the channels, (4) colonization of the reworked concretions
by bioeroding (Entobia ichnofacies) and epilithobiont
organisms took place in a littoral to shallow-marine envi-
ronment (5) lowstand fluvio-deltaic deposits passed
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860
through the channels and buried the concretions. Stages
2–4 represent the fall of sea level, so the exhumation fea-
tures in concretions (boring, encrusting by a shoreline
fauna and sand wave-winnowing) record the sequence
boundary. Dolomite and barite replacement took place
towards the margins of the concretions at relatively shallow
burial depths during eo- to meso-diagenesis that was con-
trolled by bacterial oxidation of organic matter and influ-
enced by the Redox conditions of the depositional and
diagenetic environments.
Acknowledgments This research was supported by the projects
CGL2009-10329, CGL2009-07830/BTE, CGL2009-05768-E/BTE,
CGL2007-65832/BTE and CGL2010-15372 financed by the Spanish
Ministry of Education and Science (MEC), the European Foundation
of Regional Development (FEDER), and Research Group RNM-200
and 316of the Junta de Andalucı́a. R. Marfil was supported by Project
UCM-CAM CCG07-UCM-AMB 2299. Grupo 910404 ‘‘Petrologı́a
Aplicada al análisis de cuencas y a la conservación del Patrimonio
Geológico’’. A. Santos received financial support from the Ministry of
Science and Technology of Spain in the form of a Juan de la Cierva
contract (Refa JCI-2008-2431). D. Daniel Garcia from the Centre
SPIN, Departement GENERIC, Ecole Nationale Superieure des
Mines des St. Etienne, France is gratefully acknowledged for studying
the samples under cathodoluminescence microscopy. Stable isotopes
analysis was carried out in Instituto Andaluz Ciencias de la Tierra
(CSIC). We are indebted to Eugenio Baldonedo Rodriguez and
Alfredo Larios for their valuable help with the SEM and EMPA
analyses respectively. Christine Laurin is thanked for the English
version of the text.
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