GeolCarp_Vol69_No6_515

GEOLOGICA CARPATHICA

, DECEMBER 2018, 69, 6, 515–527

doi: 10.1515/geoca-2018-0030

www.geologicacarpathica.com

Multiphase carbonate cementation in the Miocene

Pétervására Sandstone (North Hungary): implications

for basinal fluid flow and burial history

EMESE SZŐCS



and KINGA HIPS

MTA–ELTE Geological Geophysical and Space Science Research Group, 1117 Budapest, Pázmány sétány 1/C, Hungary;



meseszocs@gmail.com

(Manuscript received June 10, 2018; accepted in revised form November 28, 2018)

Abstract: The paper focuses on the reservoir heterogeneity of a sandstone formation in which the main issue is

the evaluation of diagenetic features. Integrated data from field observations as well as petrographic and geochemical

analyses from surface and core sections from different structural settings were applied. In the shallow marine Pétervására

Sandstone, eogenetic minerals are comprised of calcite, pyrite and siderite; mesogenetic minerals are albite, ankerite,

calcite, quartz, mixed layer clays and kaolinite. Dissolution occurred during mesogenetic and telogenetic phases. Ankerite

is only present in the core setting, where the sandstone is at ca. 900 m depth and diagenetic calcite predates quartz

cementation. Based on stable isotopic values (δ

V-PDB

−18.3 to −11.4 ‰ and δ

V-PDB

−9.5 to −7.2 ‰), diagenetic

calcite is of mesogenetic origin and was precipitated from fluids migrated along fault zones from the underlying, organic

matter-rich formation. In outcrop setting, on the other hand, calcite is present in a larger quantity and postdates quartz

cementation. Carbon isotope data (δ

V-PDB

= −9.9 to −5.1 ‰) indicate less contribution of light isotope, whereas more

negative oxygen isotopic values (O

V-PDB

= −13.1 to −9.9 ‰) likely imply higher temperature of mesogenetic fluids.

However, carbon–oxygen isotope covariation can indicate precipitation from meteoric fluid. In this case, further analyses

are required to delineate the final model.

Keywords: calcite, diagenesis, sandstone petrography, stable isotopes, fluid flow, lower Miocene.

Introduction

Studies of reservoir analogue sections provide useful data for

subsurface reservoir modelling. In the case of clastic deposits,

the depositional facies is commonly the major control on

reservoir architecture, but diagenetic cementation can be

an effec tive modifying factor. Carbonate cement in sandstones

plays a substantial role in reservoir quality evolution (e.g.,

Morad 1998; El-ghali et al. 2006; Gier et al. 2008; Karim et al.

2010; Oluwadebi et al. 2018). Concretionary calcite cementa-

tion of various origins was reported from numerous sandstone

formations (e.g., McBride et al. 1994; El-ghali et al. 2006;

Van Den Bril & Swennen 2008; Wanas 2008; Bojanowski et

al. 2014). Other diagenetic carbonates, such as siderite (Mozley

1989; Pye et al. 1990; Baker et al. 1995; Makeen et al. 2016)

and ankerite or ferroan dolomite (Hendry et al. 2000; Hendry

2002; Lima & De Ros 2002), can also influence the reservoir

quality. Diagenetic carbonate minerals provide data about

the burial history and chemistry of diagenetic fluids.

In this study, diagenetic features of the early Miocene

Pétervására Sandstone are presented. This formation is a hydro-

carbon reservoir rock in the central part of Hungary, whereas

in the northern part only traces of bitumen occur (Lakatos et

al. 1991; Kázmér 2004). Sztanó (1994) described and inter-

preted the sedimentary geometries within the siliciclastic

succession deposited in tide-dominated shallow water. This

paper documents the results of petrographic and geochemical

analysis in core and outcrop samples; based on these data

the burial history was reconstructed. The correlation of

the studied sections revealed the spatial variability of diage-

netic processes, especially calcite cementation and its contri-

bution to the heterogeneity of the reservoir rocks.

Geologic setting

The Pétervására Sandstone Formation can be found in

the northern part of Hungary and the southern part of Slovakia;

it covers an area of 1500 km

(Fig. 1). It consists of medium to

coarse-grained, cross-stratified glauconitic sandstone punc-

tuated by conglomerate beds and fine-grained, thick-bedded to

massive sandstone (Sztanó 1994). The thickness of the forma-

tion is 200‒600 m.

In the Oligocene, the Paratethys Basin (a large inland sea)

formed in the Alpine‒Carpathian depositional area (Báldi 1983;

Rögl & Steininger 1983). This basin was made up of a chain

of basins with varying structural developments. The Péter-

vására Sandstone was formed in the North Hungarian Bay,

an embayment of the Paratethys, where tide-influenced depo-

sition began in the Early Miocene (Eggenburgian). This bay

was connected to the Paratethys through the Eastern Slovakian

Seaway (Sztanó & Boer 1995). The Late Oligocene‒Early

Miocene deep marine siltstone formation is overlain by shal-

low marine sandstone that reflects a shallowing-upward trend

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(Báldi & Báldi-Beke 1985). The Eocene‒Lower Miocene

sedi mentary sequence ends with non-marine deposits fol-

lowed by a 25-m-thick coal formation (Báldi & Báldi-Beke

1985; Sztanó & Tari 1993).

The Pétervására Sandstone is composed of four shore-

parallel facies units (Sztanó & Tari 1993), which were formed

in gradually shallower water depth from offshore to onshore

from base to top. These are the following: 1) fine, rippled, silty

sand, the transition toward the time-equivalent Szécsény Slier;

2) fine to medium-grained sandstone with decimetre-scale

cross-bedding; 3) medium to coarse-grained sandstone,

characterized by large-scale cross-bedding with sets up to

10 m in height; 4) conglomerate lobes of 1.5‒3 m height.

The influence of tidal motions is the most evident in facies

units deposited in shallow water. In the decimetre-scale

cross-bedded sandstone, the foresets are covered by mud

drapes. The sandy material was derived from the south,

whereas coarse-grained sand to pebble-sized components

have the same source area as the coeval Darnó Conglomerate

(Sztanó & Józsa 1996). The latter formation is located near

the Darnó Fault and its components were derived from

the Meliata‒Szarvaskő Nappe of the Bükk Unit, which con-

sists of Triassic‒Jurassic ocean-floor basalt and radiolarite.

Sandstone was studied in outcrop and core sections,

located in various structural settings (Fig. 2). At Kishartyán,

the sandstone crops out in a 32 m-high and

300 m-long section (Fig. 2B). This section exhi-

bits an coarsening-upward and thickening sand-

stone superposed by conglomerate beds (Sztanó

1994). A petrographic and diagenetic study of

the outcrop at Kishartyán was provided by Szőcs

et al. (2015).

In the core section (Sámsonháza 16; Sh-16/a),

the studied sandstone occurs from 842 to 1009 m

(below surface) where fine to coarse-grained

sandstone is intercalated by conglomerate beds

(Fig. 2A).

According to hydrogeologic studies, two dis-

tinct hydrologic systems were detected in

the sub surface basinal deposits of the study area:

(1) an upper, gravity-driven meteoric water flow

and (2) a lower, compaction-driven brine water

flow (Tóth & Almasi 2001; Horváth et al. 2015).

Based on pore-water data, the same systems are

recognisable in the studied core section. The pore-

water in sandstone (analysed at 890 m depth) is

of the Na-HCO

-Cl type with 3104 mg/l total

dissolved solids (TDS) at 37

C with 2.4 bar

pressure (Hámor 1985). This indicates meteoric

water recharge into the porous formation and

it indicates a normal geothermal gradient. On

the other hand, in the underlying siltstone at

1150 m, which has much lower porosity than

the sandstone, the pore-water temperature is 68

This latter temperature indicates a much higher

geothermal gradient that is due to the elevated

heat flow which affected the basinal deposits during

the Miocene‒Pliocene synrift phase (Horváth et al. 2015).

Hydrocarbon system of the North Hungarian

Palaeogene Basin

Palaeogene formations in the Pannonian Basin are consi-

dered to be a significant hydrocarbon system (Horváth &

Tari 1999). In this system the most active source rocks are

the Upper Eocene and Lower Oligocene Tard Clay and

the Lower Oligocene Kiscell Clay, with average TOC values

of 0.5–1 wt. % which locally rise up to 4.5 wt. % (Milota et al.

1995; Badics & Vető 2012). Maturation has likely occurred in

the Late Miocene and/or Pliocene during maximal heat flow

(Milota et al. 1995). The most effective traps are structural,

stratigraphic and combination ones. Oligocene turbidite and

the studied sandstone formation are the reservoir rocks of this

hydrocarbon system.

In the eastern part of the basin, near the study area, a few

hydrocarbon exploration wells encountered oil shows (Kázmér

2004). The equivalent unit of the studied sandstone is a reser-

voir rock in the Gödöllő–Tóalmás–Tura–Jászberény area,

but the reservoir intervals of wells were not cored (Lakatos et

al. 1991).

Fig. 1. Location of the study area. Surface distribution map of the Pétervására

Sandstone Formation (Sztanó 1994) and geologic map of the area (Márton & Fodor

1995) showing locations of the studied outcrop and a core section.

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Methods

Thirty-two sandstone samples were collected

from the outcrop at Kishartyán (Fig. 2B) by ham-

mer and by drilling horizontally from the rock

surface to 30 cm depth with 3 and 5-cm-diametre

cores (Fig. 2C, D). The samples were collected

along vertical and horizontal sections. Five sand-

stone samples from the core section of the bore-

hole Sámsonháza 16 (Sh-16/a) were collected

from the depth interval of 840 to 1000 m

(Fig. 2A). Samples from outcrop and borehole

represents the following facies unit of the Péter-

vására Sandstone: 2) fine to medium-grained

sand stone with decimetre-scale cross-bedding;

3) medium to coarse-grained sandstone, charac-

terized by large-scale cross-bedding with sets up

to 10 m in height (cf. Sztanó 1994). Samples

were impregnated in blue epoxy under vacuum

and 30 µm-thick thin sections were prepared.

Thin sections were stained with Alizarin Red S

and K-ferricyanide as described by Dickson

(1966) in order to determine carbonate minerals.

They were examined by conventional micro-

scopic petrographic methods. Point counting was

performed on 18 samples to investigate quantita-

tive composition and pore volume. In each sample,

350 points were counted. Catho doluminescence

(CL) studies were performed using a MAAS-

Nuclide ELM-3 cold-cathode CL device on

polished thin sections. A microscope equipped

with an Hg vapour lamp and filters for blue light

excitation (450–490 nm) was used to detect orga-

nic matter in the samples. The filter set was com-

posed of a diachromatic beam splitter (510 nm)

and a barrier filter (515 nm).

X-ray diffraction analysis of ˂ 2 µm fractions

was carried out using a Siemens D 5000-type dif-

fractometer (Cu Kα). The sandstone was crushed

and treated with 10 % C

O solution and then

washed with distilled water. Oriented XRD

mounts were prepared by pipetting the clay suspension onto

glass slides and were analysed after air-drying and after vapour

saturation with ethylene glycol at 60 °C for 12 hours. An Amray

1830i-type Scanning Electron Microscope equipped with

INCA Energy-dispersive X-ray spectrometer was used in

the secondary electron (SE), backscatter electron (BE) and

cathodoluminescent (CL) modes on polished thin sections and

in broken surfaces. The chemical composition of minerals was

established with JXA-8530F-type Electron Probe Micro-

analyses. Stable carbon and oxygen isotopic analyses were

carried out by a Finnigan MAT delta S-type mass spectrometer

after samples being pulverized and using a conventional

anhydrous phosphoric acid digestion method under vacuum.

The results are expressed in δ-notation on the Vienna PDB

standard.

Results

Sandstone petrography of detrital grains

The studied intervals consist of fine to very coarse-grained

sandstone, in which sorting ranges from moderate to well,

with angular to well-rounded detrital grains. The sandstone

is classified as litharenite and feldspathic litharenite, with

the average framework of Q

(outcrop samples) and

(core samples; Fig. 3) according to the Folk (1974)

classification.

Quartz is the most abundant detrital mineral. Monocrystalline

quartz usually exhibits straight, occasionally sweeping extinc-

tion. Polycrystalline quartz is slightly less abundant than

monocrystalline quartz. Chert and radiolarite fragments are

Fig 2. A — Lithology of the core section Sh-16/a. Only three calcite-cemented

beds (LF3) are present. B — Lithology in the outcrop section at Kishartyán. Due to

high variability, lithofacies distribution is not marked here. C, D — Distribution of

lithofacies in outcrop samples.

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also common, and these are generally more rounded than

quartz grains. The total amount of quartz and chert varies

between 23 and 43 %. The total feldspar content is around 5 %

in core samples and 7 % in outcrop ones. K-feldspar is often

associated with kaolinite and is more abundant than

plagioclase.

The amount of metamorphic lithic fragments ranges

between 11 and 39 %. They are composed of micaschists with

muscovite, quartz, chlorite, gneiss, and quartzite. Plutonic

rock fragments (granitoids, microdiorites), volcanic and

ophio litic ones are also common (average 7 %). Detrital dolo-

mite averages 5 % (outcrop samples) and 11 % (core samples).

Limestone fragments and bioclasts are scarce. Muscovite,

chloritized biotite, glauconite group minerals, and fragments

of metamorphic minerals such as garnet, rutile, and staurolite,

are also present. The matrix content of sandstone can reach

25 %. However, some of the samples are totally matrix-free.

Pseudomatrix represented by mica and clay-rich rock frag-

ments is also present.

Lithofacies types and distribution

Based on point counting and microscope observations, three

main lithofacies types were distinguished. Porous sandstone

(LF1) with porosites of 10‒25 % is the most common one in

the outcrop as well as in the core (Fig. 4A). Matrix-rich sand-

stone (LF2) has high detrital and diagenetic clay mineral con-

tent and includes clay laminae located between the foresets

(Fig 4B). Cement-rich sandstone (LF3) has porosity lower

than 10 % and calcite content is between 12 and 27 % (Fig. 4C).

Sandstone in these lithofacies can be classified as graywacke.

In addition, in the core section a semi-consolidated sand was

classified as LF4. This lithofacies was not analysed in this

study. The spatial distribution of these lihofacies is irregular in

the outcrop, and gradual transitions are observed in both out-

crop and core sections (Fig. 2C, D). Both in core and outcrop

sections the porous sandstone (LF1) is the predominant litho-

facies, whereas matrix-rich sandstone (LF2) is subordinate.

The cement-rich sandstone (LF3) is relatively widespread in

the outcrop section. In the core, three calcite-cemented layers

with a thickness of 10 cm can be found in the lower part of

the section (Fig. 2A).

Petrography of diagenetic components

Deformation of ductile grains such as mica, glauconite and

lithoclasts are common in both studied sections. In calcite-free

intervals (LF1, LF2) of core section, linear contacts are

observed and selective fracturing of rigid grains such as dolo-

mite, quartz and feldspar also occurs (Fig. 4A). In calcite-

cemented sandstone (LF3) of core section, point contacts are

dominant. In outcrop section (LF1, LF2, LF3), linear or

concavo-convex grain contacts are more abundant than point

contacts; in addition, microstylolite is also encountered

(Fig. 4C). Accordingly, the grade of compaction is low to

moderate in calcite cemented sandstone (LF3) of core section

and high in every other lithofacies.

The observed diagenetic minerals are various carbonates,

quartz, albite, K-feldspar, kaolinite, mixed-layer illite/smec-

tite, framboidal pyrite and glauconite. Pyrite occurs as fine

framboidal crystals (< 2 µm). The pyrite crystals are scattered

around mottles of clay minerals or mica, or engulfed by coarse

carbonate crystals. Glauconite is present as peloids and

pore-filling of bioclasts. The latter case suggests diagenetic

origin. Diagenetic albite is present as a replacive phase in

Fig. 3. Ternary diagram for the detrital components. Q = quartz,

F = feldspar, L = lithoclasts / rock fragments after Folk (1974).

Fig. 4. Photomicrographs (PPL) of sandstone from various lithofacies. A — Porous sandstone (LF1) with abundant inter-granular and secon-

dary skeletal pores (thin section impregnated with blue-dye epoxy). Pre-compactional grain-rimming siderite cement around dolomite grains

is present. B — Matrix-rich sandstone (LF2) where authigenic siderite is scattered in matrix. C — Tightly-cemented sandstone (LF3). Post-

compactional blue-stained, iron-bearing replacive (Cal2K) and cement calcite (Cal3K) is ubiquitous (thin section stained by Dickson solution).

(A, B samples from core, C sample from outcrop.) Dol = dolomite, Fsp = feldspar, Qz = detrital quartz, Sd = siderite, Sp = secondary porosity.

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detrital K-feldspar grains along fractures or as euhedral over-

growth cement. These are non-luminescent and have a chemi-

cally pure albite composition (Fig. 5A, B). K-feldspar over-

growth cement appears in porous sandstone (LF1) as thin,

non-luminescent rims and it is present only in those sides of

detrital grains which are not in contact with other grains

(Fig. 5C). Both diagenetic albite and K-feldspar are common

in the outcrop samples, whereas these minerals are scarce or

totally missing in the core section. Small quantities of quartz

overgrowth cement can be found in calcite-cement free (LF1)

intervals of the core section and both in calcite-cemented

(LF3) and calcite cement-free (LF1, LF3) intervals of the out-

crop (Fig. 5D). Kaolinite is the most common clay mineral.

The pore-filling kaolinite, in the largest quantity, appears as

well-developed blocky and vermicular crystals of several tens

of microns (Fig. 5D, E). Kaolinite associated with detrital

muscovite is also abundant and it is localised between 001

surfaces that had been separated by expansion (Fig. 5F).

In the intragranular and compaction-reduced intergranular

pores, along with abundant microporosity a limited quantity of

small blocky kaolinite crystals is attached to the surface of

plagioclase grains (Fig. 5G). Kaolinite can be found in calcite

cement-free intervals (LF1) of the core section and in every

lithofacies of the outcrop section. Other clay minerals in

the outcrop and the core section consist of mixed layer

illite-smectite (I/S), smectite, illite and chlorite (Fig. 5H, I).

Fig. 5. Diagenetic minerals. A, B — Replacive non-luminescent albite in mottles of light-blue luminescent detrital K-feldspar. The majority of

detrital grains are non-luminescent, whereas pore-occluding and replacive calcite exhibit bright orange luminescent colour. (A: CL image and

B: BSE image, sample from outcrop). C — Detrital K-feldspar grain with post-compactional overgrowth cement (SE image, sample from

outcrop). D — Quartz cement (Qo), diagenetic vermicular kaolinite (Kln), and siderite cement (Sd) in open pore space (SE image, sample from

borehole). E — Siderite cement exhibits flattened rhombohedral shape around dolomite grains. Siderite is partially replaced by ankerite

(arrow). Secondary skeletal porosity is formed by dissolution of K-feldspar grains whereas pore-reducing kaolinite cement is also present (BSE

image, sample from core). F — Diagenetic, pore-filling kaolinite (Kln) localised between 001 surfaces of detrital mica (Ms), separating them

by expansion (BSE image, sample from outcrop). G — Pore-filling kaolinite booklets (arrows) which overlap the linear contact of quartz grains

(Q) (SEM–SE, sample from outcrop). H — Mixed-layer grain-coating smectite-illite. I — Showing a detail of H in higher magnification where

mixed-layer clays are covered by calcite plates of micron size (Cal3S) (SEM–SE, sample from core). Abbreviations: Ab = albite, Ank = ankerite,

Dol = dolomite, I/Sm = mixed layer illite-smectite, Kfs = K-feldspar, Kfs au = authigenic K-feldspar, Kln = kaolinite, Ms = muskovite, Qz = detrital

quartz, Qzau = quartz overgrowth cement, Sd = siderite, Sp = secondary porosity.

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Diagenetic carbonate minerals

Carbonate minerals, including siderite, ferroan dolomite/

ankerite, ferroan and non-ferroan calcite, are present in both

studied sections. In outcrop samples these minerals are present

in a higher amount, but in lower variability than in samples

from core. Calcite is the volumetrically most abundant diage-

netic mineral phase, varying between 0 and 25 %. The propor-

tion of siderite and ferroan dolomite/ankerite is less than 5 %.

In the outcrop, calcite-cemented lenses appear in every 30‒50 cm

interval and they also form continuous cemented layers.

In the core, calcite cement is encountered only in a few layers,

which are less than 10 cm in thickness. Ferroan dolomite/

ankerite is only present in the core section. The petrographic

features of diagenetic carbonates are different in the outcrop

and in the core; therefore, they are described separately.

Core section

The majority of diagenetic carbonate minerals are equally

distributed in every lithofacies. Calcite phases (Cal1S, Cal2S)

are only present in cement-rich sandstone (LF3), while tiny

crystal plates (Cal3S) are confined to LF1 and LF2. Siderite

crystals exhibit small, flattened rhombs (10‒30 µm). They are

commonly associated with detrital dolomite grains as

grain-rimming cement (Figs. 5E; 6A, B, C). Locally they are

also scattered in the matrix. Siderite ranges from 1 to 6 %, and

is non-luminescent.

A thin alteration rim on dolomite grains exhibits bright

orange luminescence colour and is slightly enriched in Fe

(Fig. 6B). Ferroan dolomite/ankerite (sensu Nickel & Grice,

1998) is present in small quantity (< 5 %). The detrital dolo-

mite as well as the siderite cement are partially replaced by

anhedral crystals of ferroan dolomite/ankerite that can achieve

several tens of microns in size (Fig. 6B, C). They are non-

luminescent, and are characterized by mottled BSE image.

These crystals include remnants of siderite of small size.

In porous-sandstone (LF1), ankerite is rarely present within

detrital dolomite grains, as irregular mottles arranged in

the network (Fig. 5E) or as vertical hairline veins (Fig. 6C).

In cement-rich sandstone (LF3) the amount of siderite is lower

than in porous sandstone.

Calcite-cemented sandstone (LF3) is present only in the lower

part of the section. Calcite (Cal1S and Cal2S) occurs as

a pore-occluding phase in the form of mosaic spar or micro-

spar crystals (Fig. 6D, E). In the porous sandstone (LF1), on

the other hand, calcite occurs as micron-sized plates (Cal3S),

which cover the surface of smectite and smectite/illite

(Fig. 5H, I).

In calcite-cemented sandstone, the cement crystals com-

monly exhibit two zones. The first one (Cal1S) stains pink

and shows bright orange luminescence colour (Fig. 6D, E).

On the other hand, the second zone (Cal2S) stains blue and

shows dull red luminescence (Fig. 6D, E). The calcite crystals

also replace detrital dolomite grains and diagenetic minerals,

such as siderite and ferroan dolomite/ankerite (Fig. 6B).

The calcite cement surface is occasionally covered by residual

organic matter.

Outcrop section

Pseudomorph of flattened rhombohedral crystals composed

of iron oxides are present around dolomite grains and scat-

tered in the matrix. These crystals show voluminous micro-

porosity and, as the crystal shape suggests, they were formed

via alteration of siderite. Calcite is present exclusively in

the calcite-cemented sandstone lithofacies (LF3). The crystals

exhibit various petrographic characters and occur as replacive

and cement phases. Calcite spars, which occlude the intergra-

nular pore space where the framework grains have mainly point

contacts, have a very thin, non-luminescent first growth band

(Cal1K). This zone occurs as an uneven rim around grains.

In other cases, calcite crystals (Cal2K, Cal3K) commonly

engulf detrital grains having linear contacts or microstylolitic

surfaces (Fig. 6F, G, H, I). The replacive calcite (Cal2K) stains

mauve to blue and exhibits mottled to dull red luminescence

colour (Fig. 6F, G). The cement phase (Cal3K), which occurs

in compaction-reduced intergranular pore space and as

a second growth band of mosaic crystals following Cal1K,

exhi bits growth zonation via mauve and blue staining and

bright orange and dull red luminescence colour (Fig. 6F, G).

The replacive calcite (Cal2K) occurs as either mosaic crys-

tals (and among them, the remnants of various minerals can be

commonly found), or as poikilotopic crystals which include

remnants of detrital and diagenetic minerals (Fig. 6H). These

remnants are detrital plagioclase, K-feldspar, quartz, dolomite,

rock fragments of magmatic and volcanic origin, as well as

diagenetic minerals, such as altered siderite (Fig. 6I). The size

and shape of the mosaic crystal sets, as well as of the poikilo-

topic crystals among the framework grains, are similar to

detrital grains (Fig. 6G, H).

Porosity

Intergranular porosity, modified by compaction and minor

cement precipitation, is observed in LF1 (Fig. 7A). Secondary

intragranular porosity is associated with detrital K-feldspar

and plagioclase (Fig. 7B, C). In addition, very small remnants

of feldspar and scattered flattened rhombohedral cement occur

in oversized pores, suggesting secondary pore formation via

enlargements of the primary one (Fig. 7A). In the outcrop

samples, the intragranular dissolution pores are cemented by

kaolinite (Fig. 7B) or calcite (Fig. 6I). In the core samples,

these pores are open and the partially dissolved feldspar grains

are engulfed by calcite (Fig. 7C). The porosity of the studied

sandstone ranges from <1 % to 25 %. In the porous sandstone

from the outcrop, the average value of the modified inter-

granular porosity is 13 %, whereas intragranular porosity is

around 3.5 %. These values are 7 % and 2 % in the core.

In calcite-cemented sandstone (LF3) and matrix-rich sand-

stone (LF2), the total value of porosity is generally below 5 %,

and it is slightly lower in the core than in the outcrop.

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−11.4 ‰, whereas the δ

V-PDB

values range between −9.5

and −7.2 ‰. Calcite in the outcrop yielded δ

V-PDB

values

ranging from −9.9 to −5.1 ‰ and δ

V-PDB

values of −13.1 to

−9.9 ‰, respectively (Fig. 8).

Geochemical composition of carbonate minerals

The chemical composition of diagenetic carbonates shows

slight or moderate variations. Siderite is relatively rich in

MgCO

(4.2‒18.7 %) and CaCO

(7‒12 %) and poor in

MnCO

(0.3‒1.3 %), whereas FeCO

content varies between

68.5 and 81.9 %. In ankerite/ferroan dolomite crystals,

the FeCO

/MgCO

proportion commonly decreases from core

to edge, varying between 0 and 1.4. The MnCO

content is

below 0.6 %. The bright orange luminescent alteration rim

of detrital dolomite grains is enriched in iron compared to

the grains.

In core samples, the first-generation calcite crystals (Cal1S)

are free of, or very poor in, Mn and Fe. The second-generation

crystals (Cal2S) have variable Mn and Fe content. In core

samples, FeCO

varies between 0 and 1.9 %, MnCO

between

0 and 0.5%, and MgCO

between 0.3 and 2.4%. In outcrop

samples, dull red luminescent calcite (Cal2K) stains blue and

it is Fe-rich, while, mauve-stained calcite of bright orange

luminescent colour (Cal3K) is Mn-rich. FeCO

content of

calcite varies between 0.5 and 2.8 %, whereas that of MnCO

is between 0.3 and 1.6 %. The MgCO

content of the calcite

in outcrop samples is below 0.8 %; however, the majority of

the calcite does not contain measurable Mg. It was not possi-

ble to measure Cal1K due to its small size.

Discussion

Paragenetic sequence

Based on petrographic and geochemical observations

the paragenetic sequence was established (Fig. 9). Diagenetic

realms are adapted from the model by Morad et al. (2000).

Eogenesis and early mesogenesis

The early diagenetic components are recognised in terms of

their relation to mechanical compaction.

Interpretation of peculiar calcite phases

In the outcrop section, where Cal1K is present, point-con-

tacts are characteristic; otherwise, linear contacts occur. Since

Fig. 7. Porosity types in sandstone. A — Skeletal and enlarged intergranular porosity. The dissolved grain was likely dolomite, indicated by

remnants of siderite crystals (optical photomicrograph, sample from core). B — Secondary porosity and microporous kaolinite inside a detrital

feldspar grain (SEM–BSE, sample from outcrop.). C — Open secondary porosity within euhedral albite. The grain is surrounded by diagenetic

calcite (Cal2K) which indicates that the feldspar dissolution post-dated the calcite cementation (SEM–BSE, sample from core). Dol = dolomite,

Kfs = K-feldspar, Kln = kaolinite, Qz = detrital quartz, Sd = siderite, Sp = secondary porosity.

Fig. 8. Cross-plot of the stable isotope values of the studied calcite.

Arrows show the influence of methanogenic fermentation, bacterial

sulphate reduction, salinity and temperature after (Allan & Wiggins

1993).

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the Cal3K phase occurs in crystallographic continuity with

non-luminescent Cal1K, the latter is interpreted as replace-

ment of a precursor carbonate cement. The compactional fea-

tures of the grains and the textural relationship of the crystals

suggest that the precursor phase of Cal1K was precipitated

during an early stage of diagenesis, and was replaced by

Cal3K during mesogenesis.

In core section (LF3), calcite cement (Ca1S) can also be

inferred as pre-compactional from point contacts and linear

contacts of neighbouring grains.

Other components

These components are similar in core and outcrop sections.

In the studied samples, glauconite formed in the intragra-

nular pores of bioclasts during early marine diagenesis by

a bacte rially catalysed process likely similar to what was

described by Odin & Matter (1981). In matrix-rich sandstone,

fram boidal pyrite was precipitated via the alte ration pro-

cesses of organic matter in the zone of bacterial sulphate

reduction, likely during the early stage of diagenesis (e.g.,

Berner et al. 1985). Early calcite phases and siderite were

precipitated in the primary pore space, indicating eogenetic

origin. Later on, illitisation of smectite as well as albitisation

of K-feldspar and plagioclase occurred in the studied sand-

stone, as discussed by (Land & Milliken 1981) in the Oligocene

Frio Formation.

Late mesogenesis in core section

In the core section, ankerite and albite formation pre-dated

calcite (Cal2S), since ankerite and albite crystals are engulfed

by Cal2S spars. Quartz cement is only present in calcite-free

intervals (LF1, LF2), which indicates that quartz formation

post-dated that of calcite. Later on, kaolinite replaced the

feldspar grains and partial dissolution of feldspars led to for-

mation of secondary intragranular porosity. The amount of

secondary porosity and kaolinite is much higher in LF1 and

LF2, suggesting that diagenetic calcite hindered this process.

In LF1 and LF2 a micron-sized calcite phase (Cal3S), present

in small quantities in the euhedral surfaces of kaolinite and

quartz, is the latest diagenetic mineral.

Late mesogenesis and telogenesis in outcrop section

In the outcrop section, quartz cement precipitation, forma-

tion of the kaolinite via feldspar replacement and secondary

porosity were widespread in LF1, LF2 and LF3. These pro-

cesses were post-dated by the volumetrically significant cal-

cite formation (Cal2K and Cal3K) in LF3. As K-feldspar

cementation occurs only in calcite-free sandstone (LF, LF2),

this suggests that K-feldspar cementation probably post-dated

calcite cementation.

Origin and sources of diagenetic carbonates

Siderite

Siderite is one of the earliest diagenetic carbonate forms

present in each lithofacies in both core and outcrop section.

Substitution of Mg and Ca for Fe in crystals suggests marine

pore-waters and eogenetic precipitation (Mozley 1989).

The penecontemporaneous formation of siderite and pyrite

was documented by several studies (Pye et al. 1990; Moore et

al. 1992; Karim et al. 2010). Pyrite formation could occur in

a bacterial sulphate reduction zone. Formation of iron-sulphide

in small amounts in these environments allows the increase of

, necessary for siderite formation (Morad 1998). The for-

mation of siderite requires reducing, non-sulphidic pore-

waters, usually evolving in suboxic and microbial

Fig. 9. Paragenetic sequence.

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methanogenetic zones (Morad 1998). Fe in siderite usually

originates from alteration of iron rich detrital minerals (Zhang

et al. 2001).

Ankerite — core section

Ankerite formation in sandstone was documented in asso-

ciation with thermal decarboxylation of organic matter

(Kantorowicz 1985; Calvo et al. 2011; Khalifa et al. 2017)

where the Mg originated from clay mineral transformations

(e.g., Hendry 2002). In the studied sandstone, the chemical

heterogeneity which was observed in the composition of

ankerite reflects the geochemistry of both pore-water and

precursor siderite mineral phase (Fig. 6E, F). Diagenetic reac-

tions in neighbouring lithologic units can be a possible

extrernal source of ankerite through cross-formational fluid

flow.

Calcite — core section

The calculated precipitation temperature of calcite is

55–65

C, based on the measured oxygen isotope values

(Cal1S and Cal2S), using the oxygen isotopic composition of

Early Miocene sea water of the Central Paratethys (Abreu &

Anderson 1998) and the oxygen isotope fractionation factor of

calcite-water (Friedman & O’Neil 1977). The measured δ

V-PDB

data show strong negative values (−18,3 to −11,4 ‰),

which indicate an addition of isotopically light carbon from

an organic source. Isotopically light carbon was likely released

during thermal decarboxylation of organic matter, since

the calculated temperature corresponds to that process (cf.

Lonoy et al. 1986; Wang et al. 2016). This is in accordance

with the presence of residual organic matter as mineral cement

covering the calcite crystals. Accordingly, only a minor

amount of hydrocarbons migrated from underlying shales

after thermal maturation. Grundtner et al. (2017) reported

similar isotopic values in calcite cement of Upper Eocene

sandstone from the North Alpine Foreland Basin (Austria)

and concluded that cementation occurred during advanced

stage of sulphate reduction. The possible source of Mg in

this calcite can be the ankerite which was replaced by these

calcite phases. Ankerite filled hairline fractures of com-

pactional origin in dolomite grains in calcite-free sandstone

(LF1, LF2), and the lack of this phenomenon in cemented

sandstone (LF3) indicates that uneven calcite cement

(Cal1S) was precipitated in primary pore space prior to

the compaction.

Micron-sized calcite plates (Cal3S) post-date kaolinite and

secondary porosity on feldspar and occur only in calcite-free

intervals (LF1, LF2). This represents the latest diagenetic

event that differs from the previous calcite-precipitating

stages. Considering that the chemistry of present-day pore-

water is characteristic for evolved meteoric waters, the rock-

water interaction likely resulted in dissolution of unstable

minerals, and precipitation of minor calcite cement (Cal3S)

(Yuan et al. 2017; Wang et al. 2018).

Calcite — outcrop section

Volumetrically significant calcite phases (Cal2K, Cal3K)

post-date quartz cementation in the outcrop section. As

reported by McKinley et al. (2002), quartz formation gene-

rally requires a minimum temperature of 80

C, suggesting

that in calcite, formation occurred after the sandstone reached

the burial depth necessary for this temperature. The measured

oxygen isotope values of calcite are enriched in light isotope.

These data suggest precipitation either from formation water

of elevated temperature or from meteoric water. In the first

case, the calculated formation temperature is 75‒90

C, by

using the equation of Friedman & O’Neil (1977) and consi-

dering isotopic values of Early Miocene sea water of Central

Paratethys (Abreu & Anderson 1998). In the second case,

the calculated temperature of calcite formation is 15‒20

where isotope values of Pleistocene meteoric water are taken

into account for comparison (Siklósy et al. 2011; Virág et al.

2013). Carbon isotopic values (from −9,9 to −5,1 ‰) are less

enriched in light isotopes compared to the core samples.

Source rocks in the underlying formation are present in limited

quantity, and their thickness increases toward the cored sec-

tion (Kázmér 2004; Badics & Vető 2012). This can explain

a smaller contribution of light isotope from the organic source.

A comparable carbon isotopic ratio can occur in the case of

meteoric water recharge, when the light carbon was derived

from the soil zone through decay of plant remnants (e.g.,

El-ghali et al. 2006). Accordingly, in the case of the outcrop

section, two possible scenarios can be described for the origin

of Ca12K and Cal3K calcites. These volumetrically signifi-

cant calcite phases were either precipitated in the mesogenetic

realm from a formational fluid enriched in light isotopes

through organic matter maturation, or in the telogenetic zone

from meteoric water recharge during basin inversion.

The studied sandstone is relatively poor (<2 %) in bioclast

and limestone rock fragments; tightly calcite-cemented zones

are not restricted to layers with abundant fossils or carbonate

rock fragments (cf. Grundtner et al. 2016). These indicate that

such grains cannot be considered as an internal source for dia-

genetic calcite. Other possible internal source of calcite can be

feldspar dissolution and clay mineral transformations (Dutton

2008). The relatively high quantity of diagenetic calcite sug-

gests an external source, which could be the underlying calca-

reous marl or overlying bioclastic limestone.

Origin and sources of other diagenetic minerals

The distribution and petrographic features of diagenetic

minerals, except for carbonates, are very similar in each litho-

facies of the core and outcrop sections. The diagenetic realms

and origin of these minerals were interpreted based on litera-

ture data.

In the realm of mesogenesis the partial albitisation of detri-

tal feldspar and illitisation of smectites were widespread in

both sections (cf. Saigal et al. 1988; Aagaard et al. 1990).

Given the similar quantity of diagenetic albite, quartz, and

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illite in the studied sandstone, the sources of ions for these

reactions were most likely internal or from the clay-rich layers

of the sandstone. Post-compactional K-feldspar overgrowth

cement, present only in the outcrop section, could have been

precipitated from evolved meteoric water at near-surface

p/T condition. K

was possibly sourced from the alteration of

clay minerals (Morad et al. 1989; Maraschin et al. 2004).

Diagenetic kaolinite was probably sourced from the weathe-

ring of feldspars (Marfil et al. 2003; Waldmann & Gaupp

2016; Yuan et al. 2017)

Thermal history and fluid flow

Core section

Limited pore-water data available from the Sh-16/a core

section suggest a complex hydrogeologic system. Elevated

temperature values (68

C at 1100 m) in calcareous marls,

directly underlying the Pétervására Sandstone, are characte-

ristic for the formation water of those deposits which were

affected by the high heat flow in the Pannonian Basin

(95 mW/m

; Lenkey et al. 2001). High heat-flow values

originated from the Middle Miocene extension and thinning of

the lithosphere (Royden & Baldi 1988). Accordingly, the fluid

originating from the underlying formation could have been

the source of calcite cement. Moreover, together with these

fluids, minor hydrocarbons also migrated from marls.

Significant negative shift of carbon isotopic values of calcite,

and additionally the residual bitumen on crystal surfaces, sug-

gest that calcite was precipitated from formation fluids con-

nected to organic matter maturation.

The present day pore-water of the studied sandstone in

the core section at ~880 m has a much lower temperature

(37

C) and a composition characteristic for evolved meteoric

waters (cf. Yuan et al. 2015). Based on the geodynamic evolu-

tion of the basin, the studied sandstone formation was also

affected by the high heat flow (Lenkey et al. 2001), but

later on was recharged by gravity-driven, regional meteoric

flow sys tems (Tóth & Almasi 2001; Horváth et al. 2015).

The evol ved meteoric fluid is likely responsible for dissolution

and kaolinite formation. Micron-sized calcite plates (Cal3S)

could also have been precipitated from the meteoric fluid.

Outcrop section

The studied section is located at the proximity of a large-

scale normal fault, in a hanging wall setting (Püspöki et al.

2017 ). The diagenetic minerals association suggests that cal-

cite cementation (Cal2K, Cal3K) post-dated quartz cementa-

tion, which approximately took place when the Pétervására

Sandstone reached its maximum burial depth around 8–11 Ma

(Petrik et al. 2014; Beke 2016). Accordingly, calcite cementa-

tion either occurred during late mesogenesis (75–90

C), or

later on, in relation to uplift and telogenesis (15–20

C). During

basin inversion, progressive recharge of meteoric water led to

the precipitation of telogenetic minerals such as K-feldspar.

Conclusions

• The diagenetic history of the Lower Miocene Pétervására

Sandstone in outcrop and borehole setting was

reconstructed.

• In litharenite and feldspathic litharenite, the most significant

eogenetic minerals, precipitated in a marine environment,

are siderite, calcite, pyrite; the mesogenetic minerals are

replacive albite, ankerite, calcite, quartz, mixed layer clays

and kaolinite. Minerals of telogenetic origin are kaolinite,

K-feldspar and possibly a minor amount of calcite.

• Mesogenetic ankerite occurs only in the core section,

whereas telogenetic K-feldspar is characteristic solely for

the outcrop section.

• The geochemical composition of diagenetic carbonate

minerals shows a wide variability. Elemental composition

of siderite is characteristic for marine pore-water. Calcite in

core samples is relatively enriched in MgCO

probably due

to replacement of ankerite.

• In the core section, sandstone is at ca. 900 m depth and

diagenetic calcite pre-dates quartz cementation. Based on

stable isotopic values (δ

V-PDB

−18.3 to −11.4 ‰ and

V-PDB

−9.5 to −7.2 ‰) the diagenetic calcite is of

mesogenetic origin and was precipitated from fluids

migrated along fault zones from the underlying, organic

matter-rich formation. The formation temperature calcu-

lated for calcite is of 55‒65 °C.

• In the outcrop setting, the calcite is present in larger quantity

and post-dates quartz cementation. Carbon isotope data

(δ

V-PDB

= −9.9 to −5.1 ‰) indicate less contribution of

light isotopes, whereas more negative oxygen isotopic

values (O

V-PDB

= −13.1 to −9.9 ‰) likely indicates a higher

temperature of mesogenetic fluids. However, carbon-oxy-

gen isotope covariation can point to precipitation from

a meteoric fluid.

• Additionally, a minor amount of calcite of likely eogenetic

origin was observed in the outcrop section; telogenetic

calcite precipitation connected to modified meteoric pore

fluids was observed in the core section.

Acknowledgements: This paper is based on the MSc thesis of

E. Szőcs. We are grateful to Attila Demény for stable isotopic

measurements, to Tibor Németh for clay mineralogical analy-

sis and to Tomáš Mikuš for electron microanalysis. Orsolya

Sztanó, Barbara Beke, László Fodor, Sándor Józsa, Zsolt

Bendő, Gergely Surányi, Orsolya Győri, Andrea Mindszenty,

Zsófia Poros, Balázs Szinger, István Vető, Szilvia Simon and

Miklós Varga are acknowledged for the discussion on the topic

and their help in field work. The cores were provided by

the core sample storage of the Hungarian Office for Mining

and Geology in cooperation with the Geological and Geophy-

sical Institute of Hungary. The project was partially supported

through the New National Excellence Program of the Ministry

of Human Capacities, Hungary (ÚNKP-17 to E. Szőcs). The

authors appreciate the constructive comments and suggestions

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of anonymous Referees, Handling Editor and Managing

Editor. The authors are grateful to Henry Lieberman for

English grammar correction.

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SZŐCS and HIPS

GEOLOGICA CARPATHICA

, 2018, 69, 6, 515–527

Supplement

Appendix 1: Quantitative composition of sandstone according to point counting (%).

Appendix 2: Chemical composition of diagenetic carbonate minerals in the Pétervására Sandstone.

samples from outcrop

samples from core

lithofacies

LF1 porous sandstone

LF2 matrix-rich

sandstone

LF3 cement-rich sandstone

LF3

LF2

LF1

sample

B-7/c B-11/a D-20

A-3 B-10/a B-11/b B-9/b

A-2 B-13/e A-4 B-13/c A-5 B-12/b B-14/c B-10/b 988m 903m 873m

grains

quartz+ chert

feldspar

magmatic +

metamorphic

rock fragment

volcanic rock

fragment

bioclast

iron oxide

dolomite

matrix matrix

cement

calcite

replacive

calcite

siderite

pores

intergranular

intragranular

Sample number

Mineral

CaCO

MnCO

MgCO

FeCO

SrCO

(Mass %)

Total (Mass %)

core sample 988

calcite

98.54

0.08

0.65

1.93

0.10

44.72

101.73

core sample 988

calcite

98.35

0.30

1.39

0.03

0.00

44.20

100.26

core sample 988

calcite

100.38

0.12

0.43

1.79

0.15

45.15

102.91

core sample 988

calcite

100.73

0.22

0.88

0.11

0.06

44.93

102.06

core sample 988

calcite

98.79

0.30

1.23

0.01

0.00

44.23

100.37

core sample 988

calcite

99.57

0.14

0.34

1.35

0.02

44.55

101.45

core sample 988

calcite

99.93

0.16

1.65

0.01

0.04

44.89

101.83

core sample 988

calcite

95.23

0.03

1.40

0.08

0.09

43.07

97.50

core sample 988

calcite

99.54

0.26

0.74

0.02

0.03

44.32

100.66

core sample 988

calcite

98.01

0.23

1.33

0.13

0.00

43.97

99.76

core sample 988

calcite

101.26

0.25

2.22

0.05

0.00

45.79

103.75

core sample 988

calcite

100.03

0.29

1.71

0.00

45.00

102.04

core sample 988

calcite

99.69

0.27

1.81

0.07

0.00

45.02

102.02

core sample 988

calcite

101.20

0.05

0.88

0.02

0.03

44.97

102.12

core sample 988

calcite

97.49

0.25

2.00

0.03

0.02

44.14

99.98

core sample 988

calcite

100.43

0.27

1.20

0.22

0.07

45.04

102.25

core sample 988

calcite

96.76

0.16

0.64

0.06

0.11

43.03

97.78

core sample 988

calcite

100.01

0.46

1.34

0.28

0.00

45.01

102.20

core sample 988

calcite

100.90

0.14

1.17

0.06

0.04

45.04

102.25

core sample 988

calcite

98.98

0.26

2.44

0.10

0.00

44.92

101.75

core sample 988

calcite

101.56

0.28

1.55

0.09

0.07

45.66

103.58

FLUID FLOW ACTIVITY DURING BURIAL (PÉTERVÁSARA SANDSTONE, NORTH HUNGARY)

GEOLOGICA CARPATHICA

, 2018, 69, 6, 515–527

Sample number

Mineral

CaCO

MnCO

MgCO

FeCO

SrCO

(Mass %)

Total (Mass %)

outcrop sample PB5b

calcite

98.90

1.11

0.37

0.65

0.05

44.39

101.12

outcrop sample PB5b

calcite

98.59

1.31

0.34

0.64

0.01

44.25

100.84

outcrop sample PB5b

calcite

99.13

1.28

0.62

0.97

0.00

44.80

102.04

outcrop sample PB5b

calcite

95.33

1.20

0.39

0.72

0.01

42.87

97.67

outcrop sample PB5b

calcite

97.12

1.28

0.69

1.08

0.05

43.99

100.25

outcrop sample PB5b

calcite

99.30

0.99

0.29

0.63

0.03

44.44

101.24

outcrop sample PB5b

calcite

95.65

1.52

0.67

1.00

0.00

43.44

98.96

outcrop sample PB5b

calcite

97.22

1.63

0.66

0.98

0.02

44.13

100.56

outcrop sample PB5b

calcite

97.66

1.25

0.39

0.91

0.00

44.00

100.27

outcrop sample PB5b

calcite

95.88

1.26

0.73

0.98

0.03

43.41

98.88

outcrop sample PB5b

calcite

97.69

1.23

0.37

0.76

0.00

43.97

100.14

outcrop sample PB5b

calcite

96.60

0.49

0.57

1.31

0.18

43.57

99.23

outcrop sample PB5b

calcite

96.34

1.12

0.31

0.55

0.03

43.19

98.38

outcrop sample PB5b

calcite

97.40

1.22

0.40

0.72

0.04

43.79

99.78

outcrop sample PB5b

calcite

98.95

0.28

0.55

2.78

0.17

45.03

102.77

outcrop sample PB5b

calcite

98.17

1.18

0.44

0.99

0.03

44.25

100.86

988 an 5

ankerite

56.54

0.53

22.35

18.42

0.08

43.75

97.91

988 an 7

ankerite

55.33

0.48

17.39

23.80

0.04

42.71

97.16

core sample 873

ankerite

55.67

0.51

18.82

22.11

0.08

43.00

97.34

core sample 873

ankerite

54.64

0.50

18.46

22.73

0.00

42.62

96.55

core sample 873

siderite

10.82

0.43

10.75

75.43

0.00

39.19

97.45

core sample 873

siderite

10.09

1.29

5.58

80.44

0.03

38.91

98.31

core sample 873

siderite

10.32

0.69

11.25

74.48

0.06

39.02

96.91

core sample 873

siderite

8.72

0.93

15.42

70.92

0.00

39.38

96.40

core sample 873

siderite

11.10

0.35

17.12

68.54

0.04

40.13

97.41

core sample 988

siderite

7.04

0.91

18.75

69.62

0.02

39.72

96.42

core sample 873

siderite

12.08

1.04

11.41

73.66

0.02

40.59

99.85

core sample 873

siderite

8.60

1.26

4.25

81.89

0.00

37.89

96.55

core sample 873

siderite

10.53

1.12

8.07

76.53

0.02

39.35

98.02

core sample 873

ankerite

55.81

0.33

19.29

21.60

0.04

43.03

97.21

core sample 988

dolomite

52.79

0.00

44.69

0.03

0.01

46.48

97.40

core sample 988

dolomite

57.89

0.06

44.31

0.20

0.00

48.64

102.40

outcrop sample PB5b

dolomite

53.80

0.00

45.57

0.27

0.02

47.49

99.54

core sample 873

dolomite

53.99

0.02

43.15

0.80

0.00

46.86

98.43

Appendix 2 (continued): Chemical composition of diagenetic carbonate minerals in the Pétervására Sandstone.