Marine and Perroleum Geolo,yj~.Vol. 14. No. 5, pp. 565 -580.

1997
I 1 1997 Elsevier Science Ltd
All rights reserved. Printed in Great Britain
PII:SO264-6172(97)00022-6 0264-8 I72/97 $17.00 i 0.00
ELSEVIER

Experimental characterisation of the hydrocarbon

sealing efficiency of cap rocks

S. Schlijmer and B. M. Krooss*

Institute of Petroleum and Organic Geochemistry KG-41, Forschungszentrum Jiilich
GmbH, D-52425 JBlich, Germany

Received 13 April 1996; revised 17 February 1997; accepted 2 March 1997

Jurassic shales and mudrocks from the Haltenbanken area offshore Norway and red claystones
from Carboniferous and Permian intervals of Northern Germany were used in a study of the
hydrocarbon sealing efficiency of elastic sediments. The investigations comprised geochemical
and mineralogical analysis of the pelitic rocks, petrophysical characterisation by mercury poro-
simetry and specific surface area measurements, and laboratory experiments to assess the
transport properties with respect to both molecular transport (diffusion) and volume flow (Darcy
flow). Effective diffusion coefficients of methane in the water-saturated rock samples at 150°C lay
between 1.4x IO-” and 4.5x 10-‘0m2/s and showed a distinct correlation with TOC content.
Permeability coefficients, measured by means of a steady-state method, ranged from < 1 nDarcy
(4 loo*’ m2) for Permian (Rotliegend) and Carboniferous red claystones up to 4.3 PDarcy
(4.3 x 10~‘8m2) for a bioturbated Jurassic siltstone.
The experimental data were used to calculate maximum sustainable gas and petroleum column
heights, hydrocarbon leakage rates by pressure-driven volume flow (Darcy flow), and diffusive
gas losses for simple, hypothetical scenarios. Computed maximum gas column heights range
from 20m up to >2000m. Hydrocarbon column heights calculated on the basis of a rich con-
densate lay between 3 and 340 m. Depending on temperature, pressure, reservoir geometry and
seal thickness, diffusive losses can be expected to require tens of millions of years to significantly
affect the contents of commercial size natural gas reservoirs. 0 1997 Elsevier Science Ltd.

Keywords: cap rocks; shales; sealing efficiency; displacement pressure; permeability; porosity; diffusion
coefficient; methane; Haltenbanken; N German basin

The evolution of hydrocarbon accumulations on the geo- lithostatic stress. Over a range of effective stresses from
logic time-scale is a dynamic process which is controlled 2.5 to 60 MPa (36&87OOpsi) the permeabilities were
by the rates of supply and loss of petroleum. Improved found to range from 16 down to 0.1 nDarcy (nDarcy =
2D basin modelling techniques and upcoming 3D models nanodarcy; 1 nDarcy = lo-” Darcy = lo-” m’)
have the capability of treating oil and gas migration in In order to arrive at a better understanding and an
the context of basin evolution. These numerical methods improved quantification and prediction of sealing
require, however, reliable petrophysical and fluid trans- efficiencies of cap rocks an experimental study was carried
port parameters for the various lithologies encountered out on a number of selected cap rock lithologies from
in hydrocarbon systems. While the characterisation of offshore Norway and northern Germany. Using specially
the transport processes in reservoir rocks has become a designed experimental equipment (cf. Figure I) per-
well established discipline with a large knowledge-base, meability measurements down to the nanodarcy range
the corresponding information on low porosity and low were carried out on a total of 27 rock samples from seals
permeability source rocks and seal lithologies (‘cap of different sedimentological environments. The samples
rocks’) is scarce. As pointed out by Sylta (1993) cap rock were characterised by mineralogical, geochemical and
leakage is still one of the least studied processes in the petrophysical methods. In addition. diffusion coefficients
field of basin modelling. for methane were measured under elevated pressure and
Besides evaporitic sequences, which are commonly temperature conditions (3.0 MPa, 150°C) to quantify the
attributed excellent sealing efficiencies, shales represent rate and efficiency of molecular transport of natural gas
the most important cap rocks in many petroliferous through cap rocks.
areas. Presently only a limited data base is available on
petrophysical and transport properties of tight shales
and claystones (Bredehoeft and Hanshaw, 1968; Magara, Theory of hydrocarbon entrapment
1971; Brace, 1980; Morrow et al., 1984). Katsube et al.
The basic concepts of hydrocarbon entrapment are well
(1991) and Mudford et al. (1991) report permeability
established and have been discussed by a number of wor-
data for a small number of tight shales measured under
kers. Berg (1975) presents the concepts of capillary sea-
ling and its role in hydrocarbon migration and trapping.
*Author to whom correspondence should be addressed. A comprehensive overview of this mechanism has been

565
566 Hydrocarbon sealing efficiency of cap rocks: S. Schliimer and B. M. Krooss

capillary seal failure cannot be related to absolute hydro-

carbon column height but buoyancy pressures will still
represent a factor in controlling sealing efficiency in this
case. Lithologies with extremely high or ‘infinite’ capil-
douciou~-layered lary entry pressures are referred to as hydraulic seals
(Watts, 1987). Here seal failure is only possible by mech-
porous stainless anical fracturing due to build-up of excessive fluid pres-
steel disks
sure or tectonic events (cf. Caillet, 1993).
. rocksample
Permeabilit~~and relative permeability will control pet-
roleum fluid transport through the seal once the capillary
entry pressure has been exceeded. The hydrocarbon col-
umn heights within a reservoir will then be determined
by the relative rates of charge and leakage. Petroleum
leakage through an initially water-wet seal is likely to
change its wettability to oil-wet. This will result in a
reduction or complete loss of capillary sealing efficiency
(cf. Ingram and Naylor, 1996) and subsequently the leak-
age process will be controlled exclusively by permeability.
Figure 1 Schematic view of flow cell used for permeability and Permeability is also an important parameter con-
diffusion measurements on cap rocks
trolling overpressure build-up and decay in sedimentary
systems. The maintenance of anomalous fluid pressures
given by Schowalter (1979) while the work of Hubbert even over limited periods of geologic time requires the
(1953) emphasises the hydrodynamic aspects of hydro- permeability of sedimentary sequences to be extremely
carbon entrapment. Downey (1984) stresses the import- low. Bredehoeft and Hanshaw (1968) assume hydraulic
ance of seal characterisation in risk evaluation and points conductivities in the range of lO_“cm s’ corresponding
out that hydrocarbon seals need to be evaluated on a to permeabilities of lo-” m2 or 1 nDarcy. Permeability
‘micro’ and a ‘mega’ scale. The establishment of a link data for tight shales are required for the interpretation of
between the macro scale and petrophysical and transport overpressure and fluid how in sedimentary basins.
parameters which can only be measured experimentally Diffusion is a perpetual and ubiquitous process in sedi-
on the laboratory (micro) scale is one of the fundamental mentary basins and its role in hydrocarbon migration has
problems in the analysis of basinwide fluid flow. been analysed by several workers (e.g. Antonov, 1954,
Apart from events like seismically induced seal rupture 1958, 1964, 1970; Smith et al., 1971; Nesterow and
or tectonic deformations resulting in the formation of Uschatinskij, 1972; Leythaeuser et al., 1980, 1982; Krooss
conducting faults (which may persist only over limited and Schaefer, 1987; Krooss and Leythaeuser, 1988;
periods of geologic time) the retention of hydrocarbons Krooss rt LzI., 1992a, 1992b; Nelson and Simmons, 1992.
by overlying seals is controlled by the capillary entry 1995; Monte1 et al., 1993). Although some controversy
pressure, the permeability and relative permeability and persists on the quantitative aspects of this issue, diffusive
the extent of diffusive losses (molecular transport) transport, according to present understanding, may rep-
through the fluid-saturated pore space. resent a significant process in the dismigration of natural
C’apillur~l forces inhibit volume flow of a non-wetting gas in certain situations. Its relevance for oil dismigration
hydrocarbon phase through a seal until the pressure of is considered marginal. Numerical modelling based on
the underlying hydrocarbons exceeds the capillary entry experimental diffusion parameters (cf. Monte1 et al..
pressure. Leakage occurs when an interconnected flow- 1993; Hantschel et al., 1995) can help to identify situ-
path of the hydrocarbon phase forms across the pore ations where diffusion is of critical importance for the
system of the cap rock. In an analysis of various cap rock persistence of natural gas accumulations.
and fault seal situations Watts (1987) denotes these seals In the present study it was attempted to arrive at quan-
as membrane seals. The capillary sealing efficiency of titative data for the processes and mechanisms outlined
membrane seals depends critically on the wettability of above for a selection of potential seal rocks.
the cap rock. Problems relating to wettability changes
during hydrocarbon leakage and the reversibility of seal
failure are largely unexplored. Under hydrostatic con- Samples
ditions a hydrocarbon column of a certain height is
The samples used in this investigation originate from four
required to create the buoyancy pressure which can
wells in the Smorbukk field, Haltenbanken area, offshore
eventually compensate and exceed the capillary entry
mid-Norway and from several wells in northern
pressure. The dependence of the capillary sealing
Germany. The requirement of cored samples for the
efficiency on the petroleum fluid phases (gas and oil) has
experimental work imposed a serious limitation because
been discussed by Watts (1987). Gas-water interfacial
coring is usually performed in reservoir sequences and
tension is larger by around one order of magnitude than
cores from seal intervals are rare.
oil-water interfacial tension. As a consequence a gas cap
on top of an oil column will enhance the sealing efficiency.
Due to its lower density, a gas column will exert a higher Haltenbanken area
buoyancy pressure than an oil column of equal height. The geologic situation of Haltenbanken and the Smor-
Gas density is, however, strongly pressure dependent and bukk field has been described by various authors (e.g.
at greater depth the buoyancy forces exerted by gas Aasheim et al., 1986; Heum et al., 1986; Ungerer et al..
columns decrease substantially. 1987; Forbes et al., 1991; Ehrenberg et al., 1992).
In the case of overpressured reservoir compartments Fifteen samples from the Smarbukk field were used in
 Hydrocarbon sealing efficiency of cap rocks: S. Schltimer and B. M. Krooss 567

Table 1 Sample information and petrophysical parameters of cap rocks from Haltenbanken and the North German Basin

HG
Permeability Specific surface displacement
Sample Death TOC Porosity [nDarcy; area pressure DP
no. Formation Rock type [r;ll [%I I%1 10 “rn2] [m2g ‘I [MPal

Haltenbanken
HI Melke homogeneous claystone 3972.4 0.54 2.8 6.9 7.38 64
H2 Melke homogeneous silty 3973.7 1.35 2.2 1072 6.29 77
claystone
H3 Melke coarse grained siltstone 3976.6 0.77 6.7 8.4 26.75 51
with detrital hlorite
H4 Melke homogeneous claystone 4184.7 2.49 3.1 4.3 10.23 80
H5 Melke micritc limestone (siderite) 4197.5 1.06 1.6 44.0 2.35 170
H6 Melke homogeneous claystone 4209.5 2.82 2.8 36.3 9.52 81
H7 Melke homogeneous claystone 4227.7 0.84 3.0 1.9 7.3 5
H8 Not finely laminated, TOC- 4043.5 5.44 1.7 3.3 4.02 74
rich clay/siltstone
H9 Upper Ror coarse grained bioturbated 4145.7 1.03 1.5 4325 3.65 2
siltstone
HI0 Lower Ror coarse grained bioturbated 4495.8 0.57 4.4 1214 3.26 2
siltstone
HI1 Lower Ror claystone with minor 4683.1 1.56 1.5 12.1 1.59 71
interlayers of silt
HI2 Tilje alternate bedding of clay, 4238.4 0.85 2.6 15.1 4.87 37
silt and sand (ripple marks)
HI3 Tilje alternate bedding of 4263.5 0.91 1.7 10.7 2.66 17
quartz-free clay layers and
coarse grained silt
HI4 Tilje fine and regularly 4527.4 0.3 1.7 7.3 4.98 47
laminated silt/claystone
HI5 Tilje claystone with minor 4560.0 1.78 0.7 13.5 1.47 45
interlayers of silt

North German Basin

Nl Upper Rotliegend red claystone 1482.2 0.03 0.9 n.m. 10.54 45
N2 Upper red claystone 1837.3 0.04 0.3 75.7 4.21 46
Carboniferous
N3 Upper Rotliegend fanglomerate 4979.9 0.03 6.6 1370 2.55 5.9
N4 Upper Rotliegend fanglomerate 4990.2 0.02 6.6 1350 3.23 6.1
N5 Upper Rotliegend red claystone 4643.4 0.04 0.7 7.8 25.32 175
N6 Upper Rotliegend red claystone 4655.1 0.05 0.7 0.62 21.58 51
N7 Upper Rotliegend red claystone 4796.2 0.03 0.5 50.0 9.1 51
N8 Upper red claystone 4053.1 0.05 1.9 13.3 5.26 62
Carboniferous
N9 Upper red claystone 3572.2 0.07 0.8 26.6 9.73 124
Carboniferous
NIO Upper red claystone 3394.7 0.02 0.6 3.5 4.34 (1.8)
Carboniferous
Nil Upper red claystone 3396.5 0.02 0.4 1.8 4.71 (5.3)
Carboniferous
N12 Upper red claystone 1549.6 0.03 1.5 <O.l 6.14 25
Carboniferous

a regional comparison of the transport properties of top addition. two Upper Rotliegend fanglomerate samples
and intraformational seals (Tuhle I). The selection com- (N3, N4) were included to assess their potential sealing
prised seven samples (Hl&H7) from the Upper Jurassic efficiency as lateral elements in stratigraphic traps and
Melke Formation, one sample each from intrafor- in combined traps associated with synsedimentary fault
mational seals of the middle Jurassic Not (H8) and Upper systems.
Ror (H9) formations, two samples from the Lower Ror The samples came from a depth interval between 1480
(H 10 & H 11) and four samples from the lower Jurassic and 5000m. Two wells were located in the inverted part
Tilje formation (H12-H 15). The depth of the samples of the Lower Saxony Basin, so that the maximum burial
ranges between 3972 and 4683 m below sea-floor level. of the cap rock samples was much greater than the
present-day depth of 1500 m.

North German basin

Twelve samples were taken from seven different locations Methods
in the southern part of the North German Basin, the
North German Lower Saxony Aucalogen and the Geochemicul and mineralogical anulysis
Pompeckji block. The selection (Table I) comprised six The samples were characterised by standard geochemical
red claystones from the Upper Carboniferous (N2, NS- and mineralogical methods. These comprised X-ray
N12) and four red claystones from the Lower Permian diffraction analysis, microscopical examination by trans-
Rotliegend (N 1. N5-N7) formations, respectively. In parency light microscopy on thin sections and scanning
568 Hydrocarbon sealing efficiency of cap rocks: S. Schliimer and 9. M. Krooss

electron microscopy (SEM) on selected samples. Total

quartz content was quantified by XRD-measurements
against an internal standard (TiOZ). The total amount
of phyllosilicates was estimated by the aluminium oxide
content (measured with X-ray fluorescence spectrometry,
XRF) assuming an average of 40% Al,O, in micas and
clay minerals and due to the fact that other Al,O,-bearing
minerals (feldspars) were nearly absent. Organic and
inorganic carbon (for calculation of carbonate content)
and total sulphur to estimate the pyrite and sulphate
content were measured by standard LECO-analysis. Due
to the low TOC-content of the samples from northern
Germany, ROCK-EVAL analysis was only carried out
log (P/[MPa])
on the samples from Haltenbanken.

PetrophJkcal methods
Specific swface area. The specific surface area is
one of the factors affecting the permeability of soils and
sedimentary rocks and appears in semi-empirical
relationships like the Kozeny-Carman formula (see
below). Specific surface areas of the rock samples were
determined by nitrogen adsorption using a MICRO-
MERITICS Gemini 2360 instrument. Cuttings with a
grain size < 1 mm were dried for 72 h at 80 ‘C. Approxi-
mately 3.5 g were then filled into a glass tube and degassed
at 130 ‘C for 2 h. After cooling the sample tube to liquid 1 10 100 1000

nitrogen temperature, the adsorbed nitrogen volume was R I4

Figure 2 Capillary pressure curve from mercury porosimetry
determined at five different pressures ranging from 5 to
measurement: (a) intrusion volume vs mercury pressure; (b)
20% of the saturation pressure P,). The evaluation was intrusion volume vs equivalent pore radius and pore radius dis-
carried out according to a modified BET formula (Bru- tribution
nauer et cil., 1938) for low relative pressures.

Mercuryporosimetry. Mercury porosimetry was per-

formed to determine the total porosity and capillary sea- cedure used in this work to represent the pore structure
ling efficiency of the cap rocks samples. In order to and quantify the capillary sealing efficiency of sedi-
minimize surface effects the measurements were carried mentary rocks. The volume of mercury entering the pore
out with cylindrical plugs of 1 cm diameter and 44.5 cm system of the rock sample is plotted as a function of
length. Capillary entry curves were recorded with a pressure on a logarithmic scale (Hg intrusion curve). The
QUANTACHROME AUTOSCAN 60 porosimeter. The pressure at which mercury starts to penetrate into the
equivalent pore radius r was computed according to the largest pores of the pore system (after correction for
capillary pressure equation (Washburn, 1921; Purcell, surface roughness effects) is denoted as entry pressure
1949; Rootare, 1970): (RP). The two other characteristic pressure values cor-
respond to the inflexion point (PP) of the sigmoidal capil-
r= _~rm, lary pressure curve and the intersection (DP) of the
tangent to this inflexion point with the logarithmic pres-
sure axis. The inflexion point marks the pressure at which
where
the incremental rate of intrusion of mercury with increas-
P,. = capillary pressure [Pa]
ing pressure is highest and, in terms of pore size distri-
y = interfacial tension [Nm-‘I, (yHg,alr= 0.471 Nm-‘)
bution, it represents the most prominent pore radius.
0 = wetting angle, (OHplldlT= 140’)
Another common representation of the capillary pressure
According to this equation the radius of pores access- curve as a function of equivalent pore radius is given in
ible to mercury intrusion depends on the pressure applied. Figure 2b. The first derivative of this curve showing the
In the present study mercury intrusion was measured up corresponding pore size distribution is also included.
to a pressure of 345 MPa (3.45 kbar, 50,OOOpsi) cor- Mercury capillary pressure curves are used to estimate
responding to a minimum equivalent pore radius of the displacement pressure, which is a critical parameter
2.1 nm (21 A). Porosity values derived from these for hydrocarbon sealing capacity. Displacement pressure
measurements consequently encompass only the volume is defined as that pressure required to form a continuous
of pores with larger equivalent radii. Many of the pelitic filament of non-wetting fluid through the largest con-
rock samples investigated had a considerable portion of nected pore throats of the rock (Schowalter, 1979).
micropore volume (pore radii ~2.1 nm) which was Schowalter (1979) performed unidirectional capillary-
beyond the scope of resolution of mercury porosimetry. breakthrough experiments with nitrogen and mercury on
In some instances an indirect estimate of the total laboratory samples of sandstone, chalk and silty shale up
porosity, including microporosity could be derived from to pressures of 34MPa (5,000 psi). Non-wetting phase
the diffusion experiments (see below). saturations required for the establishment of an inter-
Figure 2a shows a mercury capillary pressure curve to connected pathway across the length of the samples
describe the terminology and the interpretation pro- ranged between 4.5 and 17.0%. Based on this evidence
 Hydrocarbon sealing efficiency of cap rocks: S. Schliimer and B. M. Krooss 569

Z,,,=6

o.tm _

0.000

4oo.w 3oa.w 3MI.M 340.00 320.00 3oo.w 2m.04 200*00 240.00 220.00 100.00 100.00 IKLW MO.00 110.00 Loo.* 00.00 60.00 40.00 20.04

bond Size Rb
Figure 3 Results of a numerical drainage experiment for a statistically homogeneous medium (10’ IO. 10 lattice). The saturation curves
represent averaged values of 20 realisations. Computations were performed both without and with consideration of entrapment of
wetting fluid. Snw(Rb) denotes the non-wetting phase saturation as a function of bond size (Rb). The fraction of isolated (entrapped)
wetting phase is indicated by (I-Swi(Rb)). SnwBB(Rb) is the saturation of the ‘backbone’ of interconnected, transporting non-wetting
phase (modified after Fiebig and Krooss, 1995)

Schowalter ( 1979) used the value of capillary pressure in good agreement with the experimental observations
at a mercury saturation of 10% as an estimate for the by Schowalter (1979). The backbone saturation, i.e. the
displacement pressure. Omzidirectiorzal mercury intru- number and volume of conducting pathways, increases
sion measurements performed on drill cuttings of the with increasing pressure (decreasing bond size R,,)
same rocks (up to 10 MPa; 1450 psi) tended to yield lower because the system was simulated with a semi-permeable
displacement pressures (based on 10% mercury satu- membrane at the outlet side retaining the non-wetting
ration) than cylindrical plugs. These results indicate that fluid phase. In the absence of this boundary condition
conventional mercury porosimetry tends to under- the backbone saturation would remain low after the onset
estimate the capillary sealing efficiency. The utilisation of percolation. The curve denoted with (l-S{,.(&)) rep-
of cylindrical core plugs for (omnidirectional) mercury resents the volume of irreducible saturation of the wetting
porosimetry, as in the present study, may be expected to phase due to entrapment and isolation by non-wetting
reduce this discrepancy to some extent but it must be fluid.
acknowledged that mercury intrusion and drainage are Numerical experiments for different systems show that
not equivalent processes and therefore the assessment breakthrough during drainage generally occurs at higher
of sealing efficiency based on conventional mercury capillary pressure values than predicted by omni-
porosimetry is only a first-order approach. directional mercury porosimetry. This result, too, con-
The numerical simulation of bond percolation pro- forms with the experimental findings of Schowalter
cesses (cf. Fiebig and Krooss, 1995) is a helpful tool in (1979).
the elucidation of the displacement behaviour of a non- As indicated above, the assessment of capillary sealing
wetting fluid in a porous medium as a function of pore- efficiency on the basis of conventional mercury poro-
size distribution, co-ordination number of pores and geo- simetry poses some inherent problems and is, at best,
metrical arrangement of domains with different pore size semi-quantitative. The experiments of Schowalter ( 1979)
distributions. Furthermore this technique can be used to and numerical simluations indicate that for homogeneous
document the differences between omnidirectional mer- rocks with simple, monomodal capillary pressure curves
cury intrusion and drainage processes. Simulations of the pressure corresponding to a saturation value around
this kind have been carried out for a number of different 10% provides a reasonable estimate for the displacement
scenarios (Fiebig, unpublished results). Figure 3 shows pressure. For more complex, heterogeneous lithologies
an example of calculated fluid saturations for a unidi- with bimodal or polymodal capillary pressure curves, the
rectional drainage process in a laterally closed three- geometrical arrangement of different pore-size domains
dimensional pore network with a co-ordination number becomes the determining factor. In particular for lami-
(Z,) of 6. The onset of percolation of the non-wetting nated, anisotropic lithologies, information obtained from
fluid through the pore network corresponds to the first omnidirectional mercury intrusion measurements is not
non-zero saturation value of the ‘backbone’ curve sufficient to characterise capillary sealing efficiency.
(SiB( R,,)). At this point the total non-wetting phase satu- In the present work, mercury porosimetry data were
ration (S ,,,,(It,,)) amounts to approximately 13% which is evaluated by a standard method (see above). The con-
570 Hydrocarbon sealing efficiency of cap rocks: S. SchlLimer and B. M. Krooss

10 100 IO 100
Pressure[MPa] Pressure[MPa]

18
16

14
s
s 12

E 10

z8

g 6

p4

- 0
1 10 100 1000
Pressure[MPa] Pressure[MPa]

30 30

25 25

75 a
5 20 5 20

E
/
I 15 f 15
s" 2 / H4

2 IO Et IO
B B

5 5

0 0
1 10 100 1000 1 IO 100 1000

Pressure[MPa] Pressure[MPa]
Figure 4 Capillary pressure curves from mercury porosimetry for cap rocks from northern Germany (N] and Haltenbanken (H]: (a]
Carboniferous claystones (N); (b) Rotliegend claystones (N]; (c] Rotliegend fanglomerates (N]; fd] Lower Jurassic claystones (Tilje, H];
(e] Middle Jurassic claystones (Ror and Not, H]; ff] Upper Jurassic (Melke, H]

struction of the tangent for the assessment of the dis- view of a flow cell which was used for both the diffusion
placement pressure value (DP) is based on the steepest and permeability measurements. Cylindrical sample
slope found in the experimental curve. For simple, mono- plugs with a diameter of 28.5 mm and a thickness between
modal intrusion curves this pressure corresponds to 6 and 20mm are machined from the core samples and
roughly 10% mercury saturation. For the more complex placed between two pistons. Porous stainless steel discs
intrusion curves displacement pressures cannot be on both sides of the sample plugs act as fluid reservoirs.
derived without ambiguity. A more reliable assessment Conduits within the pistons are used for introduction and
of the sealing efficiency would require unidirectional removal of fluids during the experiments.
measurements at high pressure levels. The displacement The flow cell shown in Figure I does not allow for
pressures (DP) for mercury obtained from the evaluation controlled application of axial load. A tri-axial flow cell
procedure are indicated on the corresponding capillary is presently used to perform permeability and diffusion
pressure curve in Figure 4. measurements as a function of effective stress.

Measurement of permeability and diffusion Permeability measurements

coefficients
For the permeability measurements the arrangement of
The experimental equipment used to study transport pro- rock sample, porous discs and pistons was surrounded
cesses in sedimentary rocks was developed at the For- by a PTFE shrink tube and placed into a thin-walled
schungszentrum Jiilich. It consists of flow cells and (0.15 mm) aluminium tube. Application of a confining
peripheral instrumentation to perform volume flow and pressure between 15 and 20 MPa (22,000&29,000 psi)
diffusion measurements on sedimentary rocks at elevated assured a leak-tight seal around the sample and prevented
pressures and temperatures. Figure I shows a schematic bypassing of water during the permeability measure-
 Hydrocarbon sealing efficiency of cap rocks: S. Schldmer and 6. M. Krooss 571

ments. In accordance with the maturity stage of the shale Results

samples the mineralogical analysis showed no evidence
of swelling clay minerals (smectites). Therefore the use of Miizernlog_vund geochemistrj~
brine could be avoided and the permeability measure- The cap rock samples showed significant differences in
ments were performed with fresh water. All permeability their mineralogical and geochemical composition. While
tests in this study were carried out at room temperature. the Jurassic clay-and siltstones of the Haltenbanken Area
A modified HPLC pump (SHIMADZU, LC6A) was contained between 0.3 and 5.5O/~ total organic carbon
used in a constant pressure mode to generate a pressure (TOC) (Tuhk I) the mostly red coloured claystones from
gradient across the sample. To obtain measurable flow North Germany were practically devoid of organic mat-
rates the upstream pressures were set to values between ter (TOC < 0.05%).
3 and 8 MPa (4,300-l 1.600 psi). Depending on sample The ranges of mineral contents of the two sample sets
thickness the corresponding pressure gradients reached are listed in Tcrhlr 2. In terms of mineralogical com-
up to 850 MPa m-‘. Permeability tests with different pres- position the samples from Haltenbanken showed a wider
sure gradients on the same sample indicated no measur- variation than the cap rocks from the North German
able deviation from Darcy’s law under the experimental Basin. Quartz contents ranged from 16 to 48X, illite
conditions used. Due to the dependence of permeability contents between 30 and 60%. and kaolinite and chlorite
on effective stress (cf. Katsube et ul., 1991) high fluid amounted up to 40% and 20X, respectively. Most
pressures associated with high pressure gradients may, samples contained traces of mixed-layered minerals
however, affect indirectly the permeability of mudrocks (smectite/illite). Pyrite ranged between 0.5 and 5%.
by reducing effective stress. and carbonate-content (predominately siderite) was usu-
The permeability measurements were performed in a ally low, except for the samples H6 (I 3%) H 13 (14%)
steady-state mode. The flow was monitored auto- and H9. a massive micritic limestone. Feldspar (plagio-
matically via the pumping rate required to maintain the clase) was extremely rare. SEM examination revealed
upstream pressure. In addition the fluid volume passing some heavy minerals (zircon, apatite. rutile).
through the sample was measured in a graduated burette The red claystones from the North German Basin
at the downstream side of the flow cell and compared to showed a rather homogeneous macroscopic and micro-
the results of the automatically recorded flow readings scopic structure as well as a relatively uniform bulk min-
for consistency. No specific procedure was employed to eralogical composition. They were dominated by illite
saturate the samples with water prior to the experiment. (48875%) and quartz (7730%, Trrhlc I)). Kaolinite and
Instead, the flux was monitored until it had decreased to chlorite contents amounted to 8% and 10% respectively.
a constant value (usually 5510 h after the start of the SEM analysis revealed carbonate (calcite), feldspar
experiment, depending on permeability). (plagioclase and rarely K-feldspar) and sulfates (barite.
Depending on sample thickness. fluid viscosity and anhydrous gypsum) in most of these samples. Hematite
measuring time permeabilities down to the range of was present in all samples from North Germany.
0.1 nDarcy (IO-” m’) can be determined with this exper-
imental set-up. Petroplz_bkal properties
The evaluation was performed according to Darcy’s Spec$c swjilce urea. Specific surface areas for the
law: clay- and siltstones from both sample sets ranged between
1.5 and IO m’g-’ (Tc~hle I). Exceptionally high values, in
excess of 20m’g-‘. were found for one coarse-grained
J, = -! grad P [ms-‘1
siltstone from the Melke formation containing detrital
chlorite (sample H3) and for two red claystones (N5 and
Here J,. denotes volume flow, k the permeability N6) from the North German Upper Rotliegend. Sample
coefficient (m2), ye the fluid viscosity (Pas) and P the H3 had a comparatively high porosity (6.7X, determined
fluid pressure (Pa). Depending on the room temperature by Hg porosimetry; see below) whereas its permeability
water viscosity was taken as 9.5-9.09 x 10p4Pas was relatively low. Samples N5 and N6, apart from their
(9.5-9.09 x lO_‘cP). higher specific surface areas, did not show any excep-
tional petrophysical properties. Mercury intrusion yiel-
ded porosity values of only 0.7% but the capillary
D@sion experiments pressure curves (see below) indicated the presence of sig-
Diffusion coefficients for methane were measured on
water-saturated samples under elevated pore pressure
and temperature conditions (3 MPa and 15OC) with the Table 2 Mineralogical composition and TOC-content of the cap
same flow cell as in the permeability measurements. The rock samples under investigation
sample plugs were first wrapped with a lead foil (thickness
Mineral Haltenbanken Area North German
0.25 mm) and then placed into a thin-walled (0.15 mm) component [weight %I Basin [weight %I
copper tube. After mounting the arrangement of rock
sample and pistons into the flow cell (Figure 1) appli- quartz 16-48 7-30
cation of a confining pressure of 3540MPa for a short illite 30-60 48-75
kaolinite 3-40 3-8
time ensured a diffusion-tight seal around the rock chlorite 1-19 O-IO
samples. The diffusion experiment was started by intro- illite/smectite-ml traces -
ducing a free gas phase of methane into the lower com- siderite o-14
partment (stainless-steel porous disk) of the flow cell. The calcite traces o-12
pyrite 0.5-5 -
aqueous phase in the upper compartment was sampled
feldspar traces traces
at regular time intervals (l-4 h) and its methane content TOC 0.3-5.5 < 0.05
determined by an automatic analytical unit.
572 Hydrocarbon sealing efficiency of cap rocks: S. Schllimer and B. M. Krooss

nificant micropore volume (equivalent pore radii range betwzcn 25 and 30 ALIg- ‘. The intrusion volumes
< 2.1 nm). The indirect assessment of the porosity based of the shale cap rocks from Haltenbanken are consistently
on the results of the diffusion experiments yielded sig- higher than 4~11g-~’ with a maximum value (27/!1 g ‘)
nificantly higher values (2.5-3%) lending further support found for the coarse-grained siltstone H3.
to the presence of an extensive micropore system. Three of the Carboniferous samples (N8. N9. N 12)
show distinctly bimodal pore-size distributions (&JWY
4a). The steep slopes at the end sections of the curves
Mercury porosimetry
(small equivalent radii) indicate the presence of micro-
Pnrositj, pore volume beyond the resolution of the mercury
Significant porosity differences were found between the porosity measurement.
sample sets from the Norwegian Shelf and from northern The capillary pressure curves of the Rotliegend samples
Germany (Table I). For the relatively homogeneous in Figure 4h show, as a common feature, a gradual, steady
North German red claystones, porosities were mostly increase with decreasing equivalent pore volume indi-
below 1%. The highest values (around 7%) were mea- cating a wide pore size distribution. None of the curves
sured for the two fanglomerate samples N3 and N4. has a distinct inflexion point so that a most prominent
Due to their higher silt content porosity values of the pore radius cannot be identified. The final intrusion vol-
Haltenbanken samples were larger and ranged usually umes lie between 1.5 and 3.5/llg-‘.
between 1 and 3%. The highest porosity (6.7%) was The two fanglomerates (Figure 4~) have sigmoidal
measured for sample H3. capillary pressure curves with final entry volumes
Porosities were also derived from the results of between 35 and 3O/llg-‘. The inflexion points rep-
diffusion experiments with the assumption that the resenting the most prominent pore radii lie between 30
diffusing hydrocarbon gas resided exclusively in the pore and 50 nm.
water and no sorption took place. These calculations Due to their more heterogeneous composition the cap
were performed using a value of 419 ppm for the aqueous rock samples from Haltenbanken show a wide variability
solubility of methane under experimental conditions in capillary pressure curves (Figure 4&f). This variability
(150 C, 3 MPa). Figure 5 shows a comparison of the is evident even for samples within the same formation
porosities derived from mercury injection and diffusion taken at different locations less than 10 km apart.
experiments for the TOC-free samples from North Ger- Maximum pore entry volumes range from 10 ,~1gg’ in
many. For samples N3, N8, N 10 and N 11, a relatively the Tilje formation up to 27 /tlg-’ in the Melke. The
good agreement between the two porosity measurements minimum value was 2.5plg-’ (sample H15, Tilje fm.).
was found. For samples N5, N6 and N9 the elevated Both bimodal and monomodal curve shapes are encoun-
porosity values from the diffusion experiments as com- tered. The extremely wide pore-size distribution indi-
pared to the mercury porosimetry data indicate a sig- cated by curve HlO (Figure 4e) is attributed to the biot-
nificant micropore volume not accessible to mercury urbations observed in this siltstone sample. A similar
intrusion. This result is supported by the shapes of the feature. though less distinct, is observed in curve H9. For
corresponding experimental capillary pressure curves (see most samples mercury intrusion tends to start gradually
below). at relatively low pressures, i.e. large equivalent pore radii.
Due to their significant organic matter content the The micritic limestone (H5) from the Melke formation
assumption of absence of sorption was not justified for (Fi_qurc $f’) is a notable exception. Mercury intrusion
the Haltenbanken samples. Interpretation of the diffusion starts only at equivalent pore radii below 6&7nm, cor-
results in terms of porosity was therefore not possible. responding to mercury entry pressures between 20 and
30 MPa (29,00043,500 psi).
CupdIary pressure cun~es The standard evaluation of mercury porosimetry
experiments comprises the computation of the total
The capillary pressure curves for all rock samples ana-
intrusion volume, porosity, void ratio, smallest and lar-
lysed in this study are shown in Figure 4. The final
gest equivalent pore radius, most frequent pore radius etc.
intrusion volumes (corresponding to the smallest access-
and basic statistics of the pore size distribution. This
ible equivalent pore radius) lie below 3.5 ,LIIgg’ for most
evaluation method is readily applicable for well-shaped
N-German samples. Two samples from the Car-
capillary pressure curves like those obtained with the
boniferous have slightly larger pore volumes (5-7 ~1 gg ‘).
fanglomerates. For the pelitic rocks investigated in this
Intrusion volumes for the two fanglomerate samples
study, however, the limitations of mercury porosimetry
are evident. Although practically all samples have a
measurable permeability, indicative of an interconnected
pore network. a significant portion of the pore-size dis-
tribution extends in many cases beyond the experimental
limit of 2.1 nm of equivalent pore radius. In the absence of
a distinct inflexion point within the experimental pressure
range a displacement pressure cannot be readily derived
from the capillary pressure curves. In Figure 6 this case
is documented for a Rotliegend red claystone sample
(N7) where the maximum slope of the curve coincides
with its end point. The displacement pressure resulting
from the standard evaluation procedure is indicated but,
N3 NS N6 NB N9 NIO Nli NIL?
Sample due to the incomplete representation of the pore size
Figure5 Porosityvaluesfor shales from the North German Basin distribution, it can only be considered as a rough esti-
derived from mercury porosimetry and diffusion experiments mate. Shales exhibiting mercury capillary pressure curves
 Hydrocarbon sealing efficiency of cap rocks: S. SchlCimer and B. M. Krooss 573

with intrusion volumes below 2 ~1 g- ’up to the maximum

pressure of 345 MPa (50,000 psi). Due to unspecific curve
shapes the results obtained for samples NlO and N 11 are
considered unrealistic. For two samples (N5 and N9)
the evaluation yielded mercury displacement pressures in
excess of 100 MPa (14,500 psi) whereas the values for the
other samples range between 25 and 61 MPa (3630 and
8850 psi).
Displacement pressures computed for the two fan-
glomerate samples (N3 and N4;) were 5.8 and 6.6MPa
1.0 10.0 100.0 1000.0 (841 and 957 psi), respectively. Although these values are
Pressure [MPa]
much lower than for the claystones the capillary sealing
Figure 6 Standard evaluation of mercury intrusion curve for a efficiency of this rock type is still considerable.
Rotliegend claystone

Transport parameters
of this type must probably in any case be classified as Permeability. The permeabilities of the pelitic cap
hydraulic rather than membrane seals. rocks investigated were consistently far below the limit
of routine permeability measurements performed in the
petroleum industry (Tuble 1). The Jurassic shales and
Capillary sealing efficiency
siltstones from the Halten-Terrace ranged mostly
With respect to the inherent limitations discussed above, between 5 and 50 nDarcy (I nDarcy = IO-” Darcy =
the displucement pressure (DP) (Figure 2~) should only lo-” m’). Substantially higher values, from 1000 up to
be viewed as an approximation to the capillary sealing 4300 nDarcy (l-4.3 LIDarcy) were found only for the two
efficiency of fine-grained sedimentary rocks. The DP bioturbated siltstones (H9, HlO) and one silty shale (H2).
values obtained from the evaluation of the mercury The minimum permeability encountered was slightly
porosity data of the individual cap rock samples are listed below 2 nDarcy (sample H7).
in Tuble 1. For one of the Haltenbanken samples (H15) For the samples from North Germany the permeability
and five claystones from northern Germany (N2, N5, measurements yielded values ranging from below the
N6, N7, N9) the capillary pressure curves did not show detection limit of 0.1 nDarcy (sample N12) up to
distinct inflexion points within the experimental pressure 75 nDarcy for the red claystones and siltstones. The per-
range. The corresponding entry pressures for the most meabilities of the two fanglomerate samples N3 and N4
prominent pore radius (PP) were thus greater than lay around 1350 nDarcy.
z 3.45 kbar (50,000 psi) and the displacement pressures
(LIP) given in Table I must be considered as lower limits. D@sion parameters. The results of the diffusion
The Jurassic claystones from Haltenbanken show a measurements are listed in Table 3. Thirteen experiments
wide range of displacement pressures (2-170 MPa; 29t& were performed with water-saturated rock samples at
24,600psi) reflecting the large variability in rock fabric 150 C and a fluid pressure of 3 MPa (30 bar). Diffusion
and composition. The highest displacement pressure was coefficients for the red claystones from the Lower Saxony
found for a micritic limestone (H5; 170 MPa; 24600psi) Basin ranged between 1.O and 2.6 x IO “I m’s ’whereas
and the lowest values (2 MPa; 290psi) for two bio- the highest diffusion coefficient (4.46 x 10. “‘m’s ‘) was
turbated siltstones (H9, HlO) and a claystone (H7; found for the fanglomerate sample N3 in accordance with
5 MPa; 725 psi). Interestingly, this latter sample had the its high porosity (6.6%) and permeability (1370 nDarcy).
lowest permeability of the Haltenbanken sample set Methane diffusion coefficients for the samples from
(1.9 nDarcy). Haltenbanken were generally lower than those measured
Four of the claystone samples from northern Germany for the claystones from N Germany and ranged between
(N2, N7, N 10 and N 11) yielded capillary pressure curves 1.4x IO-” (sample H8) and 1.14x lO~~“‘m’ss (sample

Table 3 Results of methane diffusion experiments on cap rocks at 150°C and 3 MPa gas
pressure

Bulk rock methane

Methane diffusion concentration (under
coefficient (150°C) experimental conditions)
Sample Depth [ml TOC [%I [m* s- ‘I [gCH, mm3 rock]
____-_
H4 4184.7 2.49 1.97EE11 38.40
H5 4197.5 1.06 4.66E - 11 19.80
H6 4209.5 2.82 3.05E - 11 31.80
Ha 4043.5 5.44 1.40E-11 29.73
HI4 4527.4 0.3 l.l4E-10 17.26
N3 4979.9 0.03 4.46E-10 24.96
N5 4643.4 0.04 2.45E- 10 16.31
N6 4655.1 0.05 2.59E- 10 11.93
N8 4053.1 0.05 2.21E-10 5.13
N9 3572.2 0.07 1.91EE10 11.52
NIO 3394.7 0.02 9.57E-11 1.33
Nil 3396.5 0.02 1.60E-10 3.06
N12 1549.6 0.03 l.O2E-10 2.58
574 Hydrocarbon sealing efficiency of cap rocks: S. Schliimer and B. M. Krooss

HI 3). The low effective diffusion coefficients must be

viewed as a consequence of the organic matter content of
the Jurassic shales. Sorption of the methane in this
organic matter significantly reduces the rate of molecular
transport.
The effective diffusion coefficient is a measure of the
molecular mobility of the diffusing species reflecting the
rate of displacement of individual molecules and, as a
consequence, the rate of advancement of a diffusion
front. The diffusive transmissibility of seal rocks for gases
is not controlled exclusively by the effective diffusion 1.0~.12
0.0 1.0 2.0 3.0 4.0 6.0 6.0
coefficient but also by the concentration (Cbulk) of the TOC %
diffusing species in a volume of rock. This concentration Figure 7 Diffusion coefficients of methane vs the organic carbon
is related to the partial pressure @) of the gas in the content of shale samples
reservoir by a partition coefficient (fi) also denoted as gas
capacity (Antonov, 1954).
10000 I.E.17
CbulL = /l-p [gCH, m-j rock] n

1000 ‘b II l.E-18
The gas capacity is a function of temperature, porosity, z

and organic matter content. The bulk rock methane con-

centrations under the experimental pressure and tem-
perature conditions can be derived from the results of
the diffusion measurements (Krooss and Schaefer, 1987;
Krooss and Leythaeuser, 1988). The concentrations
1.E-21
found in this study range from 1.3 up to almost 40g
CH,m-’ rock. i.e. they extend over more than one order 0.1 4 1, i 1622
of magnitude. With the experimental gas pressure of 1 10 100

3 MPa of pure methane and neglecting, as a rough Specific surface area [mVg]

approximation, the partial pressure of the water and Figure 8 Permeability vs specific surface area for shale cap rocks
fugacity coefficients, the gas capacities (/3) can be com- from N Germany and Haltenbanken

puted to range between 0.43 and 13.3 g CH,m-’

rock/MPa at the measuring temperature of 150°C. In
principle, the gas capacity can be used to compute the meability evolution of sediments with increasing burial
bulk phase methane concentration at a given gas partial depth and predict the formation properties. As pointed
pressure. However, as neither the pressure nor the tem- out by Hilfer (1992) such relationships should be looked
perature dependence of this parameter has been estab- at as a statement about the consolidation process of geo-
lished in detail, the resulting concentration values should logical formations or rock types and not as general
be considered tentative. relations between permeability and bulk porosity
The Kozeny-Carman equation is a widely used
relationship for permeability estimates (England et al.,
Correlations 1987; Mudford and Best, 1989; Mudford et cd., 1991).
Attempts to find correlations between the petrophysical The equation relates the permeability coefficient (k) to
and transport parameters measured in this study were the porosity (4) and the specific surface area (s) of the
largely unsuccessful. This is only partly due to the limited porous medium according to:
number of samples analysed. Petrophysical properties 4’
and sealing efficiency are primarily controlled by lith- k = c,/LsS’( 1 - 4,’
ology and diagenetic effects, and experience shows that
no simple relationships exist between the various par- li permeability coefficient [m’]
ameters. Thus, among the Haltenbanken claystones the $ porosity
sample with the lowest permeability (H7; 1.9nDarcy) S specific surface area [m’ kg-‘]
has one of the lowest capillary entry pressures, while its C,b_, KozenyyCarman constant [m’kg-‘1
porosity (3%) and specific surface area (7 m2 g- ‘) are not
This equation was originally established for sandstones
exceptional. and unconsolidated soils. Its validity for tight, con-
A distinct correlation was found between the TOC
solidated claystones is speculative and has not been tested
values of the Haltenbanken shales and the methane in detail.
diffusion coefficients as shown in Figure 7. Furthermore. a
Attempts to represent the permeability data obtained
general tendency of permeability decrease with increasing
for pelitic rocks in this study by the Kozeny-Carman
specific surface area can be inferred from Figure 8.
relationship were unsuccessful.
However, no correlation exists between the diffusion
In Figure 9 the permeability values of all samples mea-
coefficients and petrophysical parameters like perme-
sured in this study are plotted versus porosity. In the
ability or porosity.
porosity range up to 3% the permeability coefficients
vary over two orders of magnitude and no general trend
Porosity-permeabilit?) relationships can be observed. Calculated curves superimposed on this
Porosity-permeability relationships are used in basin diagram with a Kozeny-Carman constant of 5 * lOpI3
modelling and petroleum engineering to estimate the per- m” kg -’ and different specific surface areas predict a dras-
 Hydrocarbon sealing efficiency of cap rocks: S. Schlbmer and B. M. Krooss 575

IE-17 Table 4 Parameters used for the calculation of maximum gas

and petroleum (condensate) column heights retained by dif-
IE-18 ferent seal lithologies

0.042 N m ’(42 dyn cm ‘)

0.005Nm ’(5 dyncm ‘)
0.471 N m ’(471 dyn cm ‘1
1095kgm ’
240kgm 3
383kgm 3
1E-22 140”
0”
C,,,,,, = 5.0~10”’ m’kg-’
1E-23
0 1 2 3 4 5 6 7
Porosity [%]

Figure 9 Permeability vs porosity diagram for pelitic rocks from

Haltenbanken and northern Germany. Kozeny-Carman curves curves, the above procedure involves several unknowns
from different specific surface areas are superimposed. which may critically influence the hydrocarbon column
prediction. While interfacial tensions (;I) of hydrocarbon-
water systems in the temperature and pressure ranges of
interest have been measured or can be estimated with
tic decrease in permeability for porosities below 1% some confidence, the wettability of the seal represents a
which does not correspond to the experimental results. major problem. Commonly a wetting angle (H) of zero
is assumed. implying a completely water-wet seal. This
Quarhfication qfsealing #ciency and leakage assumption is likely to be wrong for seals containing
processes significant amounts of organic matter. Wettability data
The focus of the present study was on the test and appli- for tight shales are practically non-existent. The com-
cation of experimental methods for the characterisation plexity of this problem is increased by potential wett-
of the sealing efficiency of fine-grained elastic sedimentary ability changes of seals due to petroleum generation or
rocks. In the following discussion the experimental results impregnation.
are used in simple scenarios to demonstrate the pro- Using the above scheme, maximum gas column heights
cedures for the quantification of hydrocarbon losses were calculated based on the DP values indicated in Fig-
through different seal rocks and to compare the relative ure 4 and listed in Table I. The computation was per-
importance of leakage mechanisms. These predictions formed with the parameters shown in Table 4. Tuhle 5
can only be of a very general nature. Ultimately, the data lists the computed maximum gas column heights for cap
obtained from this laboratory study should be applied to rock samples from northern Germany and Halten-
specific case histories in the context of integrated basin banken. The Haltenbanken reservoir fluids are mainly
studies. This is the only way to take into account the rich gas condensates (GOR 1500-1800 Std. m3 rn-‘;
complexity of the geological framework and the variety Ehrenberg et d., 1992). Therefore an additional cal-
of processes involved during the different stages of basin culation was performed for the samples from this area
evolution and reservoir formation. based on an average petroleum density of 383 kgm ’
and an oil- water interfacial tension of 5 IO- ’N mm ‘. All
Capillaq~ seuling qfficierzcy and hydrocarbon column column heights were calculated for hydrostatic
heights conditions. In overpressured reservoirs capillary failure
The computation of maximum hydrocarbon column and bleed-off of hydrocarbons will depend to a lesser
heights from mercury capillary pressure data is an estab- extent on hydrocarbon column heights.
lished procedure discussed in detail by Berg (1975). The capillary pressure data in Tubh 1 and the values
Schowalter (1979) and Watts (1987). Commonly the in Tuble 5 indicate that the capillary sealing efficiency of
capillary pressure of the hydrocarbon-water system the rocks investigated in this study is generally excellent.
(Pc,_) is equated to the buoyancy pressure of a free Computed maximum gas column heights for most of the
hydrocarbon column (/z,,,). Rotliegend and Carboniferous red claystones from the
North German Basin lie mostly above 600m and even
the fanglomerate samples can hold gas columns of more
than 80 m. Depending on burial depth and efl‘ective stress,
gas pressures required for capillary leakage to occur
would most probably exceed the mechanical strength of
the lithologies so that the corresponding seals can be
classified as hydraulic.
With the exception of the bioturbated siltstones of the
Ror Formation the gas sealing capacity of the Hal-
Here s is the acceleration due to gravity and p denotes tenbanken cap rocks is also excellent. This holds also for
the density of the formation water (p,,,,,) and the hydro- the sealing capacity for an oil condensate calculated
carbon fluid (phc). Due to the capillary pressure exerted under the assumption of a water-wet pore system. Due
by the non-wetting fluids in the reservoir rock, the actual to the geologic situation the capillary sealing efficiency
hydrocarbon column heights in reservoirs will usually plays only a minor role in the Haltenbanken area. The
be somewhat smaller than the values calculated by this Carboniferous and Upper Jurassic shales overlying the
procedure. reservoir formations are generally overpressured and act
Apart from the uncertainties associated with the therefore as pressure seals (Ehrenberg et cd., 1992). In
interpretation of the experimental capillary pressure particular in the eastern section of the Smmrbukk field a
576 Hydrocarbon sealing efficiency of cap rocks: S. Schltimer and 6. M. Krooss

Table 5 Maximum gas and oil column heights computed from displacement pressure (DP) values of cap rocks

Maximum gas column Maximimu oil column

Sample Depth height based on DP height based on DP
no. Formation Rock type [ml [ml [ml

Haltenbanken
HI Melke homogeneous claystone 3972.4 887 127
HZ Melke homogeneous silty claystone 3973.7 1066 152
H3 Melke coarse grained siltstone with detrital 3976.6 710 101
chlorite
H4 Melke homogeneous claystone 4184.7 1117 160
H5 Melke micritc limestone (siderite) 4197.5 2353 336
H6 Melke homogeneous claystone 4209.5 1125 161
H7 Melke homogeneous claystone 4227.7 68 10
H8 Not finely laminated, TOC-rich clay/siltstone 4043.5 1025 147
H9 Upper Ror coarse grained bioturbated siltstone 4145.7 28 4
HI0 Lower Ror coarse grained bioturbated siltstone 4495.8 24 3
HI1 Lower Ror claystone with minor interlayers of silt 4683.05 986 141
HI2 Tilje alternate bedding of clay, silt and sand 4238.4 511 73
(ripple marks)
HI3 Tilje alternate bedding of quartz-free clay 4263.5 236 34
layers and coarse grained silt
HI4 Tilje fine and regularly laminated 4527.4 652 93
silt/claystone
HI5 Tilje claystone with minor interlayers of silt 4560 620 89
North German Basin
Nl Upper Rotliegend red claystone 1482.22 620
N2 Upper Carboniferous red claystone 1837.3 643
N3 Upper Rotliegend fanglomerate 4979.92 81
N4 Upper Rotliegend fanglomerate 4990.2 93
N5 Upper Rotliegend red claystone 4643.4 2425
N6 Upper Rotliegend red claystone 4655.05 706
N7 Upper Rotliegend red claystone 4796.15 703
N8 Upper Carboniferous red claystone 4053.1 859
N9 Upper Carboniferous red claystone 3572.2 1714
NlO Upper Carboniferous red claystone 3394.7 -
Nil Upper Carboniferous red claystone 3396.5 -
N12 Upper Carboniferous red claystone 1549.6 348

strong pressure gradient is directed downwards from the Here, J, 1 is the gas volume flux in (m’ m-’ s- ‘; gas volume
Upper Jurassic Melke formation into the underlying Jur- under subsurface conditions!) through the top of the layer
assic reservoir sections. The investigation of the for- and P, and P2 (in Pa) are the gas phase pressures at the
mation mechanisms and longevity of pressure seals bottom and at the top, respectively. The gas flux can be
represents another important aspect in the assessment of converted to standard pressure and temperature con-
sealing efficiency and petroleum reservoir dynamics. ditions using the ideal gas law.
The gas flux after capillary seal failure through a seal
Hydrocurbotz leakage by Darq~Jlow of 1OOm was computed with the parameters listed in
In a normally-pressured reservoir, hydrocarbon leakage Table 6. The calculation was performed using the dis-
will occur when the buoyancy of the hydrocarbon column placement pressures (DP) for the corresponding rocks
exceeds the capillary pressure of the seal. In over- (Table I). The compressible flow rates (Table 7) for this
pressured reservoir compartments the direction and scenario range from 10” up to 10’ Std m3m-“m.y.-‘.
intensity of fluid flow is controlled by the global pressure Average gas contents of commercial size reservoirs are in
field and buoyancy plays only a minor role. The leakage the range of tens to hundreds of Std m’m-’ with
rate by volume (Darcy) flow after breakthrough is con- maximum values of 1500 Stdm3mp’ (cf. Krooss and
trolled by the permeability coefficient, the fluid viscosity Leythaeuser, 1997). Consequently, gas leakage by com-
and the pressure gradient. The situation is complicated pressible Darcy flow under the above assumptions will
by the fact that leakage through an initially water-wet seal result in practically instantaneous loss of commercial size
will proceed as a two-phase flow. Consequently, relative reservoir contents on the geologic time scale.
permeabilities, depending on the saturation state of the This simple calculation disregards, however, the two-
pore system ought to be known as a prerequisite for a phase character of the compressible flow gas dismigration
quantitative description of this process.
The compressible Darcy flow of a gas phase through a
porous layer (seal) of thickness A.\- (in m) is computed Table 6 Hypothetical scenario used for calculation of Darcy flow
according to: of gas and petroleum through a 100 m seal

J = _k*(P$-Pf) bottom of seal 5000 m (16,404 ft)

E.2 top of seal 4900 m (16,076 ft)
q * 2 * P2 - As pressure at top 49 MPa (7,107 psi)
gas viscosity (rf& 3.00E - 05 Pa. s (3.00E - 02 centipoise)
k = permeability coefficient [m’] oil viscosity (tf,,,) l.OOE-03 Pa .s (1.0 centipoise)
q = viscosity [Pa s]
 Hydrocarbon sealing efficiency of cap rocks: S. Schliimer and B. M. Krooss 577

Table 7 Calculated compressible Darcy flow of gas after capillary failure

Sample Gas displacement Compressible Darcy flux

no. Formation Depth [ml pressure [MPal PI [MPal P2 IMPal (@DP) [Std m3 m ’ m.y. ‘1

Haltenbanken
HI Melke 3972.4 7.44 57.44 49.0 2.22E+05
H2 Melke 3973.7 8.94 58.94 49.0 4.12E+07
H3 Melke 3976.6 5.95 55.95 49.0 2.19E+05
H4 Melke 4184.7 9.37 59.37 49.0 1.73E+05
H5 Melke 4197.5 19.74 69.74 49.0 3.88E+06
H6 Melke 4209.5 9.44 59.44 49.0 1.47E+06
H7 Melke 4227.7 0.57 50.57 49.0 l.O6E+04
H8 Not 4043.5 8.60 58.60 49.0 1.22E+05
H9 Upper Ror 4145.7 0.24 50.24 49.0 1.90E+07
HI0 Lower Ror 4495.8 0.20 50.20 49.0 5.16E+06
HI1 Lower Ror 4683.1 8.27 58.27 49.0 4.31E+05
HI2 Tilje 4238.4 4.29 54.29 49.0 2.95E+05
HI3 Tilje 4263.5 1.98 51.98 49.0 l.l5E+05
HI4 Tilje 4527.4 5.47 55.47 49.0 1.75E+05
HI5 Tilje 4560.0 5.20 55.20 49.0 3.12E+05

North German Basin

Nl Upper Rotliegend 1482.2 5.20
N2 Upper Carboniferous 1837.3 5.39 55.39 49.0 1.81E+06
N3 Upper Rotliegend 4979.9 0.68 50.68 49.0 8.22E+06
N4 Upper Rotliegend 4990.2 0.78 50.78 49.0 8.58E+06
N5 Upper Rotliegend 4643.4 20.34 70.34 49.0 7.07E+05
N6 Upper Rotliegend 4655.1 5.92 55.92 49.0 1.61 E+04
N7 Upper Rotliegend 4796.2 5.89 55.89 49.0 1.29E+06
N8 Upper Carboniferous 4053.1 7.20 57.20 49.0 4.15E+05
N9 Upper Carboniferous 3572.2 14.38 64.38 49.0 1.66E+06
NIO Upper Carboniferous 3394.7 0.21 50.21 49.0 1.51E+04
Nll Upper Carboniferous 3396.5 0.62 50.62 49.0 l.OlE+04

process. Furthermore it can be assumed that in many research. The pressure situation in the Haltenbanken
instances the capillary pressures required for gas leakage shows that permeability and Darcy flow have a much
to take place are never reached. more important impact on the sealing efficiency in an
A similar computation was performed for incom- indirect way by governing the formation and longevity
pressible Darcy flow of oil through the Haltenbanken of pressure seals.
seal lithologies. The viscosity was estimated as lop3 Pas
(Table 6). Due to the lower oil-water interfacial tension
(5 x 10-j N rn-‘), breakthrough pressures for oil are con-
siderably lower than for gas. Table 8 shows that the The permeability measurements reported in this study
calculated Darcy fluxes for oil at the corresponding dis- were not performed under controlled effective stress con-
placement and percolation pressures vary by more than ditions. The axial stress acting upon the samples during
three orders of magnitude. the experiments was controlled by the degree of tighten-
The above calculations must be considered as tentative. ing of the bolts during assembly of the flow cell and the
Too many unknowns are still involved and a more precise thermal expansion of the components during heating.
calculation must take into account the variation and Only very few permeability data for tight lithologies have
interrelationship of numerous parameters. The validity been reported in the literature. Katsube et al. (1991)
of Darcy’s law and a possible transition from volume present vertical permeability measurements for two shale
flow to molecular transport are issues that require further samples at effective pressures (BP) ranging up to 60 MPa
(600 bar) and derive the following functional relation-
ship:
Table 8 Calculated Darcy flow of oil after capillary failure
k = k,.exp(-MAP)
Incompressible
flow of oil k, = 118 x IO _ “‘rn’
Sample No. Formation PI IMPa] P2 [MPa] [m3m ~2m.y.-‘]
IX= 0.074MPa ’
Haltenbanken
HI Melke 50.9 49.0 4.1 According to this relationship the permeability of a
H2 Melke 51.1 49.0 693 shale should decrease to 0.5 on an effective pressure
H3 Melke 51.1 49.0 24 increase by 1OMPa. Assuming that in the experiments
H7 Melke 50.1 49.0 0.6
reported here the confining pressure (10-l 5 MPa; 145(r
H8 Not 51.0 49.0 2.1
H9 Upper Ror 50.0 49.0 1402 2200 psi) corresponded approximately to the axial stress, a
HI0 Lower Ror 50.0 49.0 392 rough extrapolation to a depth of 5000 m with an effective
HI1 Lower Ror 510 49.0 7.5 stress of 70 MPa (10,100 psi) yields a decrease in per-
HI2 Tilje 50.5 49.0 7.2 meability by a factor of 50-100. Recent measurements
HI3 Tilje 50.2 49.0 4.2
HI4 Tilje 50.6 49.0 3.8
performed in our laboratory support this trend but also
HI5 Tilje 50.6 49.0 6.9 indicate that slightly different rock types (lithologies)
show different effective stress-permeability relationships.
578 Hydrocarbon sealing efficiency of cap rocks: S. Schliimer and 9. M. Krooss

Estimation of diffusive losses methane is attributed the same solubility characteristics

in organic matter as in water.
Using the effective diffusion coefficients reported in this
The cumulative amount (Q,,) of methane difl‘used from
work the steady-state diffusive flux across a cap rock can
the reservoir into the cap rock of thickness (I) was com-
be calculated according to Fick’s first law of diffusion:
puted as a function of time (1) according to the relation-
J = - DctlVChulh ship for diffusive transport in a plane sheet (cf. Krooss 01
L/I., 1993a. I993b).
The bulk volume concentration of the diffusing species
required for this calculation can be determined from the
gas capacity. It should be noted, however, that gas
capacities are temperature-dependent and not readily
available for different temperature ranges. Here C, is the bulk rock methane concentration and D
As a first approximation the gas concentration per the effective diffusion coefficient.
volume of cap rock can be determined from the porosity The cumulative diffusive losses were calculated over a
and the saturation concentration of methane in the pore period of 200 m.y. for the rock samples from N Germany
water under the envisaged subsurface conditions. Meth- whereas a shorter diffusion period of 50 m.y. was chosen
ane concentrations in water as a function of pressure, for the Haltenbanken samples. The results for the latter
temperature and salinity have been reported in the litera- show that diffusive losses after 50m.y. reach values
ture (Haas, 1978; Battino, 1984). between 120 and 520 Std m’ methane per m’ of cap rock
To compare the sealing efficiency of the different cap area (Figure 10) and lie between 20 and 50 Std m3 rn- ’
rock types examined in this study a simple scenario was during the first 5 m.y.
chosen and diffusive fluxes through different rock types The computed cumulative diffusive losses for the sam-
were calculated. ples from the N German basin (Figure II) extend over a
The scenario assumes a cap rock of 1OOm thickness much wider range. Apart from the fanglomerate sample
overlying a gas reservoir filled with methane. The sub- (N3) they lie between 100 and 5000 Std m3 methane rn--’
surface fluid pressure (pore pressure) was taken as for a period of 200m.y. The Upper Carboniferous sam-
50 MPa (7,250psi). the temperature as 150 ‘C and the ples N IO. N I I and N 12 have a better sealing efficiency
salinity of the formation water as 5000ppm NaCI. The with respect to diffusive transport than the samples from
parameters used in the calculations are summarised in Haltenbanken. Over a period of 50m.y. the computed
Table 9. diffusive losses are below or only slightly above 100 Std
Bulk rock methane concentration under subsurface m3 methane mm2.
conditions was calculated from the bulk rock methane Published data indicate that gas charges in commercial
concentrations (C~~~mcn’) determined during the gas fields world-wide range mostly between 150 and 1500
diffusion experiments (3 MPa, 1SO’C, fresh water) and Std m’ mm2 (Krooss and Leythaeuser, 1997). With the
the methane concentrations in water under experimental above diffusive flux rates periods of several tens of million
(C;Tt;immt) and subsurface ( Cg~;~~&wa,rr) conditions. years are required to substantially affect the gas content
respectively: of a commercial gas reservoir.
The rate of diffusive gas losses from reservoirs depends
rcserwir = ~~~ynent . CtE;;:& watrr on a number of parameters like seal thickness, reservoir
c bulb
(yxrmlent
Udter geometry, diffusion coefficients, gas capacity of the cap
rock, pressure and temperature. These need to be evalu-
This computation implies that under both exper- ated individually for a given scenario in the context of
imental and subsurface conditions the methane resides the evolution of the sedimentary basin.
exclusively in solution in the water-saturated pore space
of the cap rock. This assumption is probably not correct
for those samples from the Haltenbanken area containing Summary
significant amounts of organic matter. Here the exper-
The systematic investigation of the petrophysical and
imental results indicate considerable sorption of methane
transport parameters of shale samples from the
on or in the organic matter which on the one hand
Haltenbanken area and the North German Basin has
increases the gas storage capacity of the rock and on the
other hand reduces the effective diffusion coefficients.
Presently practically no information is available on the 1000

sorption capacity of organic matter for methane at high

pressures and temperatures. With the above assumption

Table 9 Hypothetical cap rock scenario for the computation of

diffusive losses

cap rock thickness IOOm (328ft)

depth of reservoir/seal 5000 m (16,404 ft)
boundary
reservoir temperature 150°C (302°F)
hydrostatic pressure 50 MPa (7,252 psi) I
C”“‘“’ 419 ppm 0 10 20 30 40 50
exper,ment
Ctormatlpnwater 4610 ppm Time [m.y.]
reSBrYO,r
salinity 5000 ppm Figure 10 Cumulative diffusive methane losses calculated for a
conversion factor (methane) 1.478sd. m3(15”C, 1 atm) kg ’ hypothetical 100 m cap rock with experimental data for different
Haltenbanken shales
 Hydrocarbon sealing efficiency of cap rocks: S. Schlbmer and 6. M. Krooss 579

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Acknowledgements solubilities of methane in water and aqueous sodium chloride
solutions up to 25 weight percent, 360 C, and 138 MP, United
This work was performed in the context of the German States Department of the Interior, Geological Survey, Open-
Norwegian Geoscientific Co-operation supported by The File, pp. 41, Report No. 78-1004.
Hantschel, T., Krooss, B. M., Wygrala, B. P. and Muscio, G. P.
Federal Ministry of Education, Science, Research and
A. (1995) Comparative Study of Separate Phase Flow and
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stats oljeselskap a.s. (Statoil) and Deutsche Wissen- Technical Exhibition - Glasgow, Scot/and, Extended
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