Applied Water Science (2020) 10:116

https://doi.org/10.1007/s13201-020-01189-0

ORIGINAL ARTICLE

Salinity and water effect on electrical properties of fragile clayey

sandstone
Mohamed Mahmoud Gomaa1

Received: 4 April 2019 / Accepted: 30 March 2020 / Published online: 21 April 2020
© The Author(s) 2020

Abstract
There are enormous variations in the electrical characteristics of rocks and minerals according to many factors. Electrical
measurements were taken to define the weight of these variations. Water saturation effect (partially and fully) on electrical
characteristics of loose clayey sandstone samples was studied. Measurements were taken at room temperature (~ 19 °C) and
a frequency range of (0.0005 Hz–100 kHz). Changes in water content are the only factor that controls changes in electrical
properties. Change in frequency with water content is an important factor for electrical properties. At relatively low frequen-
cies and low saturations, an interface between grains (charge accumulation at grain surfaces and bound water) is the dominat-
ing factor. Also, the bulk material properties at high frequency and full saturations are the controlling factors. At moderate
saturations, there are surface charge displacement and exchange of excess ions between grains. For high saturations, due
to existence of high mobilities of excess ions, the diffusion or membrane polarization is the main controlling mechanisms.
The water used in the sample is 4 g of NaCl/100 g of distilled water. The electrical conductivity of the samples increases
gradually with the addition of saline water. With an increase in frequency, variations of conductivity may be negligible.

Keywords  Electrical conductivity · Dielectric constant · Complex impedance · Saturation · Loose clayey sandstone ·
Frequency domain

Introduction geological mixtures. Generally, dielectrics may have some

weak bonded charged particles. When an external field is
Semiconductor materials may have conductivity values of applied, these weak charge bonds can be linked to form an
range of 1­ 0−4–10−9 S/cm. Dielectrics have conductivities electrical current. Ore-bearing rocks or ore minerals show
less than 1­ 0−9 S/cm. There is no precise boundary between semiconductor properties. Semiconductors conductivity is
conductors or insulators. Charge carriers (electrons) in very sensitive to minor changes in chemical composition
semiconductors are responsible for electrical conductivity. and accordingly to water quantity. Composite materials of
In dielectrics or insulator materials, charge carriers cannot ore minerals are supposed to have good sources of charge
move over large distances because the conducting paths carriers. If charge carriers are near the conduction band, then
are generally broken. Metals and semiconductors have the the transfer of electrons requires only a small energy (e.g.,
same charge carriers for electrical conductivity (electrons). increase in frequency or temperature). Electrical conduc-
Activation energy required for electrons is the basic differ- tion for semiconductors may be by electrons only. This is
ence between these two material types. In metals, activation dependent on the distance between energy levels.
energy needed is nearly zero, while in semiconductors, it is There is a very wide range of conductivity values for
up to several electron volts. Semiconductors are insulators rocks (~ 20 orders of magnitude). This is dependent on the
(nearly) at low temperatures. Charge carriers are not free constituents of the minerals constituting the rock mixture.
to move over large distances, especially in heterogeneous However, when the water is present in a rock sample, it
shows a huge dominant effect on electrical characteristics
* Mohamed Mahmoud Gomaa of sedimentary rocks. Also, the existence of salinity may add
[email protected] another dominant effect to the electrical properties. Impuri-
ties at samples may lead to huge electrical properties varia-
1
Geophysical Sciences Department, National Research tions, especially for saturated composites, in addition to the
Centre, El‑Behoos St., Dokki, Cairo, Egypt

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humidity saturation or effect (Leroy and Revil 2004; Men- (molecules), orientation polarization or charge transfer
delson and Cohen 1982; Gomaa and Kassab 2016; Kassab through ions or protons (in Helmholtz or diffuse double
et al. 2017‫)‏‬. layer). The surface proton conduction mechanism may be
The A.C. electrical characteristics of partially and fully satu- along hydroxylic groups or chains (Saarenketo 1998). The
rated loose clayey sandstone specimens, at frequency range of hydrogen ions may effectively conduct through water mol-
0.0005 Hz–100 kHz, were studied. Electrical properties change ecules of hydrogen bonds at adsorbed layers (Pride 1994).
from one sample to another because there are many texture dif- The process of polarization due to the presence of water
ferences between these samples (Gomaa et al. 2015a, b; Gomaa multilayers is much more effective than the orientation
and Abou El-Anwar 2015), with the existence of more conduc- polarization (Leroy and Revil 2004). At low saturations, a
tion paths from the saline water. Every sample has a separate local high charge density is present at grain surfaces, with a
structure and connections (texture). To eliminate the changes strong electrostatic field. These localized charges enhance
in texture and to remove any other differences (grain size, per- water dissociation to provide charge carriers (protons) to
meability, grain shape, structure, concentration, etc.), electrical make hopping transport[ (Garrouch
]+ 2001). The transport of
measurements were taken only on one sample with different charges occurs when H3 O releases a proton to the adjacent
water saturations (from partial to saturated). That material is molecule of water, while another proton is released after that
an example of a mixture of multicomponent system (sand, and so on (Garcia-Belmonte et al. 2003). At relatively high
clay, saline water and air). The main concentration of the used saturations, isolated water clusters are connected, and water
sample is sand (~ 70%) and clay (~ 30%). Grain size of sand in conduction occurs along with protonic transport (Dukhin
sample is in the order from 0.09 to 1.7 mm, and grain size of 1971; Pride 1994; Glover et al. 1994a, b).
clay in sample is in the order of ~ 60 µm. The specific surface conduction, at pure water, connected
In this article, an attempt was made to interpret the effect to the transfer of proton is ~ 2.4 × 10−9 S (Revil and Glover
of saline water on electrical characteristics of that loose 1998). Surface migration and diffusion are often greatly dis-
clayey sandstone specimen. Clayey sandstone specimens are tinguished than the mixture component polarization. Revil
good dielectrics at room temperatures with a conductivity of and Glover (1998) display that contribution of an electrical
the order from ~ 10−4 to ~ 10−6 S/m, when it is dry (Gomaa diffuse layer to surface conductivity is neglected (silica and
2009; Shaltout et al. 2012; Abou El-Anwar and Gomaa 2013, alumino-silicates). The main contribution is related to sur-
2016). The presence of some polarization processes with the face conductivity that resulted from counterions located at
surface conduction mechanisms on grain surfaces motivates the Stern layer. Surface mobility, at the Stern layer, is nearly
high values of dielectric constant (Chelidze et al. 1999; Ruf- ten times smaller than the bulk mobility. The independence
fet et al. 1991a, b). With applying an electric field, the ions of salinity is another contribution from the direct proton
polarize around the rock grains, giving rise to large dipoles transfer, on the mineral surface.
and large dielectric constants (Garrouch and Sharma 1994; At relative low frequencies, the dielectric distributions
Minor et al. 1998; Shilov et al. 2001). As the frequency resulted from polarization of counterions around particles
increases, ions could not follow the applied electrical field (Schwarz 1962). The displacement of counterions gives
and accordingly have less time to polarize and contribute abnormal dielectric constant. Abnormal dielectric constant
more to the conductivity, since they are more in phase with related to polarization of electrical double layer at grain inter-
the applied electric field (Gomaa and Abou El-Anwar 2017; face was discussed by Chelidze and Guéguen (1999). Applica-
Cole and Cole 1941). tion of an electric domain leads to migration and diffusion of
Existence of water at rock mixtures can be classified from charges and the existence of isolated clusters with excess of
electrical point of view as: adsorbed water, free water and negative and positive charges (on different sides of grains).
capillary water (Mitchell 1992; Saarenketo 1998). The pres- The large low-frequency polarization takes into account the
ence of minute water causes the increase in electrical values. heterogeneity in electrical charge distribution on grain inter-
The first additions of water form some separated clusters faces (Chelidze and Guéguen 1999). In this model, relaxa-
from each other, at the beginning (very small saturations). tion time depends on charges cluster size on mineral surfaces
With more additions of water, these separated clusters of rather than on particles grain size. The existence of excess or
water become connected and coat most of grain surfaces deficit produces ions to gather together and increase at inter-
(Gomaa 2008, 2013). Salinity of water adds more ions and faces, which are disjointed with surface (Wong 1979, 1987;
electrons to the conduction process in the sample. For the Mehaute and Crepy 1983).
partial saturation cases, water molecules (at the adsorbed The dielectric effect interaction between water and rock
layers) form vigorous links with surface grains and a certain (rock surface) was discussed at many studies (Knight and Nur
polarization mechanism may be arise (orientation polariza- 1987). They show that electrical characteristics increase with
tion or reversible hopping, Glover et al. (1994a). For the saturation increase. A critical saturation point may exist for
higher saturation cases, polarization may be by dipole saturated samples. Below that critical saturation, the resistivity

13
Applied Water Science (2020) 10:116 Page 3 of 9  116

Fig. 1  Change in dielectric 1E+014

constant with frequency at
different saturation levels of
saline water (4 g/100 g of NaCl) 1E+013

Dielectric constant
[(1) diamond, (2) square, (3)
triangle, (4) circle, (5) inverted 1E+012
triangle, (6) times symbol, (7)
star symbol, (8) asterisk, (9)
oplus symbol, (10) open square 1E+011
with times symbol]
1E+010

1E+009

1E+008
1
2
1E+007 3
4
1E+006 5
6
1E+005 7
8
9
1E+004
10
Frequency (Hz)
1E+003

1E-004 1E-003 1E-002 1E-001 1E+000 1E+001 1E+002 1E+003 1E+004 1E+005

decreases gradually with saturation, and above it, the resistiv- The real part of the complex relative dielectric constant
ity decrease slower. Power law is controlled by permittivity (𝜀) is 𝜀� = Cp d∕𝜀0 A , and the imaginary part is 𝜀�� = Gp d∕w𝜀0 A ,
as a function of frequency (w) which is due to randomness of where A is the cross-sectional area of the sample ­(m2),
the grains and constituents within the samples (Jonscher 1999; d is its thickness (m), 𝜀0 is the permittivity of free space
Gomaa et al. 2018). ( 8.85 × 10−12 F/m), and w is the angular frequency. The con-
ductivity and dielectric constant equations are 𝜎 = dGp ∕A
Experimental procedures (S/m), 𝜀� = Cp ∕C0 , C0 = (A∕d)𝜀0 (F).
Sample weight dry was measured and at full saturation, by
Electrical properties measurements were taken on a thin disk- putting it in pressure vessel, then evacuating the vessel from
shaped loose clayey sandstone of thickness 10 mm and diam- air, allowing distilled water to flow into the vessel. Subsequent
eter 37 mm. measurements with the determination of weight were made
Non-polarizing Cu/CuSO4 gel electrodes were used at while the sample was let to dry. The saturation levels were
measurements (Gomaa and Alikaj 2009; Alikaj 1989). The calculated as
electrode impedance was very small within the used frequency
Swet − Sdry
( )
range. WS = × 100
Data were collected in the frequency range from 0.0005 Hz Sdry
to 100 kHz using a Hioki 3522-50 LCR Hitester Impedance
Analyzer connected to the non-polarizing electrodes. A volt- where WS denotes water saturation %; Swet wet sample
age of 1 V was applied. weight; and Sdry dry sample weight.
The measured electrical properties parameters are the par- The porosity 𝜙 of the sample (~ 13%) was calculated by
allel capacitance and conductance Cp (F) and Gp (S) and the (
Ssat − Sdry
)
series impedance Z at different frequencies. The maximum 𝜙= × 100
𝜌w × V
error of instrument is of the order of 7%. The complex relative
dielectric constant is 𝜀∗ = 𝜀� − i𝜀��.

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Fig. 2  Change in conductiv- 1E+001

ity with frequency at different
saturation levels of saline water
(4 g/100 g of NaCl) [(1) dia-
mond, (2) square, (3) triangle,

Conductivity (S/m)
(4) circle, (5) inverted triangle,
(6) times symbol, (7) star
symbol, (8) asterisk, (9) oplus 1E+000
symbol, (10) open square with
times symbol]

1E-001

1E-002

Frequency (Hz)
1E-003

1E-004 1E-003 1E-002 1E-001 1E+000 1E+001 1E+002 1E+003 1E+004 1E+005

where Ssat = saturated sample weight, 𝜌w = water density polarization is not present at continuous conductor links.
(~ 1), and V is the sample volume. Charge carriers may move over a large distance through
sample under the effect electric fields. The polarization
of space charges takes place when charge carriers are
Interpretation and discussions obstructed. Charge carriers are trapped at the ends of
grain (or cluster) interfaces, or when these charges are
In rocks containing saline liquids, the dominant conduc- not able to be discharged freely, or when it is replaced at
tion comes from saline liquids, while the other rock texture electrodes. The accumulation of charge carriers increases
(i.e., liquid or grains) may be negligible compared to it. the permittivity or dielectric constant of samples. At low
At normal temperatures, when there are very rich dissemi- frequency, charges have enough time to gather together
nated ores, the rock texture conductivity cannot be negli- at interfaces of the conducting clusters, and accordingly,
gible. Conversely, at very high temperatures, the conduc- dielectric constant increases. At relatively high frequency,
tivity of the semiconductor of minerals has the dominant these charge carriers do not possess enough time to gather
effect. Liquids contribute to electrical conduction by their together at these interfaces of the conducting clusters, and
paths between pore spaces. Saline liquids have more con- accordingly, dielectric constant decreases.
duction energy than usual liquids because there are more The dielectric constant and conductivity increase with
free charges from the saline itself. Voids between grains increase in relative saturation level. Figure 1 shows the
determine the shape of electric paths and accordingly their change in dielectric constant with frequency at different
interface interaction with the solid grains. saturation levels of saline water (4 g/100 g of NaCl). Fig-
The existence of disconnected links of semiconduc- ure 2 shows the change in conductivity with frequency
tor or insulator in the sample leads to polarized space at different saturation levels of saline water (4 g/100 g of
charge at the ends of the semiconductors. This is usually NaCl). At first partial saturation case, there are some iso-
present at partial saturations, while, for full saturations, lated clusters of water around grains and the pores are

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Applied Water Science (2020) 10:116 Page 5 of 9  116

Fig. 3  Variation of complex 1E+005

resistivity plane as a function of
frequency at different saturation
levels of saline water (4 g/100 g 1
of NaCl) [(1) diamond, (2) 2

Im Z (Ohm)
square, (3) triangle, (4) circle, 3
(5) inverted triangle, (6) times 8E+004
4
symbol, (7) star symbol, (8) 5
asterisk, (9) oplus symbol, (10)
6
open square with times symbol]
7
8
6E+004
9
10

4E+004

2E+004

Re Z (Ohm)
0E+000

0E+000 2E+004 4E+004 6E+004 8E+004 1E+005

partially filled with air and/or water. With increase in samples ( Fe2 O3 , MgO , Na2 O , TiO2 , Cu , Mn and Zn ) lead
the saturation of saline water, the adsorbed water forms to high abnormal dielectric constant values. These ore clay
some monolayers of water throughout grains which are mineral chains in the samples are disconnected by SiO2 . At
completely bound to grain surfaces and cannot participate relatively low frequencies, a dielectric constant of samples
to the conduction current (contribute only to the diffu- is related to the interface between grains at the dead ends of
sion current). This adsorbed water properties are totally the conducting chains. This interface dielectric constant is
different from the bulk water (Hoekstra and Doyle 1971; much higher than an intrinsic bulk dielectric constant of the
Knight and Endres 1990). With more increase in satura- sample. Also, the dielectric constants increase monotoni-
tion of saline water and at higher saturations, the adsorbed cally with a further increase in the degree of saline water
water makes connected clusters of water. Due to increase saturation. Electrical properties are affected by salinity dis-
in saline water saturation, the adsorbed water coats, com- tribution at grain surfaces and show a great dependence on
pletely, the grain surfaces and the small isolated clusters the cluster interconnection (chemical interaction or surface
begin to contact with each other, forming small islands activity). These remarkable differences and changes in the
of water between grains. At the beginning, these discon- texture connections of the samples will, without doubt, result
nected islands are still isolated from each other and the in different amounts of electric properties. More clearly, the
inner water monolayers are strongly bonded to the surface saline water saturation in the samples has a much higher
(Glover et al. 1994a). Lately, after the saturation concen- dielectric constant and conductivity at relatively low fre-
tration increases, the isolated clusters become gradually quencies due to free ions at saline water combined with
connected with continuous fluid films that finally are con- conducting ore clay minerals in the samples ( Fe2 O3 , MgO ,
nected between the two electrodes. Na2 O , TiO2 , Cu and Mn ); charges move freely at the liquid.
Dielectric constant values (Fig.  1) at low frequency The connection between the different discontinuous con-
(0.0005 Hz) vary from 1010 for low saturated loose clayey ducting clusters within the whole composite, without doubt,
sandstone to 2 × 1013 for full saline water saturation, while decreases the whole surface area of the cluster in addition
the values at high-frequency range ( 105 Hz) from 2 × 103 for to overall charge transportation capability. Generally, above
low saline water saturation of loose clayey sandstone to 104 the critical saturation, the broken clusters begin to connect
for full saline water saturation. The ore clay minerals in the leading to the mutual decrease in the dielectric constant. At

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Page 6 of 9 Applied Water Science (2020) 10:116

1E+005 4E+004

Im Z (Ohm)

Im Z (Ohm)
8E+004

3E+004

6E+004

2E+004

4E+004

1E+004
2E+004

Re Z (Ohm)
0E+000 Re Z (Ohm)
0E+000
0E+000 2E+004 4E+004 6E+004 8E+004 1E+005
0E+000 1E+004 2E+004 3E+004 4E+004

2E+004 4E+003
Im Z (Ohm)

Im Z (Ohm)
1E+004 3E+003

8E+003 2E+003

4E+003 1E+003

Re Z (Ohm) Re Z (Ohm)
0E+000 0E+000

0E+000 4E+003 8E+003 1E+004 2E+004 0E+000 1E+003 2E+003 3E+003 4E+003

1E+003 6E+002
Im Z (Ohm)

Im Z (Ohm)

8E+002

4E+002

6E+002

4E+002

2E+002

2E+002

Re Z (Ohm)
0E+000 Re Z (Ohm)
0E+000
0E+000 2E+002 4E+002 6E+002 8E+002 1E+003
0E+000 1E+002 2E+002 3E+002 4E+002 5E+002 6E+002

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◂Fig. 4  Variation details of complex resistivity plane as a function of saturated clayey sandstone samples to 10 S/m for high saline
frequency at different saturation levels of saline water (4  g/100  g of
water saturation (this is nearly the saline water conductiv-
NaCl) [(1) diamond, (2) square, (3) triangle, (4) circle, (5) inverted
triangle, (6) times symbol, (7) star symbol, (8) asterisk, (9) oplus ity). Low-frequency zone is characterized by existence of
symbol, (10) open square with times symbol] continuous links of water with clay minerals between the
electrodes, thus causing nearly constant conductivity with
frequency. Even with the successive additions of saline water
the present case, the salinity only increases and the clusters concentration, the conductivity values change about three
do not increase. Accordingly, dielectric constant increases decades, while with the successive increase in frequency at
monotonically due to increase in charges of the saline water. the whole frequency extension, the maximum conductiv-
In the present case, the clusters of the saturated clayey sand- ity values change about half decade. The continuous con-
stone sample are not completely connected and accordingly duction paths of saline water between the grains increase
dielectric constant is high even with an increase in sample with increasing saline water content; thus, the conductivity
salinity. increases. The samples that have the same concentrations
At low frequency, the dielectric constant has a power- of water, clay and sand may not have the same behavior of
law dependence ( 𝜀 ∝ f −𝛼 , Fig. 1), which is not changed at electrical properties due to change in the texture from one
a certain frequency (100 Hz). At high frequency (above sample to another (Efros and Shklovskii 1976; Knight 1983;
100 Hz), the power-law dependence on dielectric con- Olhoeft 1985; Sen 1989; Levitskaya and Sternberg 2000).
stant may be present with a different value of 𝛼 exponent. Figures 3 and 4 show the complex resistivity plane rep-
That high-frequency region begins at nearly 100 Hz for resentation of the sample at different saturation levels of
low saturation, while it takes the whole frequency range saline water (4 g/100 g of NaCl). The data are exhibited in
at higher saline water saturations. For very high-saline- two Figs. 3 and 4 due to a wide range of values on a linear
saturation samples, there is (nearly) only one region of scale. Figure 3 shows all the saturations in one curve, and
dispersion of dielectric constant in the whole frequency Fig. 4 shows the details of the other ten saturations. For
range. The frequency separating regions 1 and 2 (Fig. 1) low-saline-water-saturation case, nearly two incomplete
increases with increase in water saturation above a critical semicircles can be identified for seven saline saturations. As
value (Wilkinson et al. 1983). The physical mechanisms the saline water saturation increases, the first low-frequency
supposed for relatively low saturations can be either the dampened semicircle is getting bigger and the second high-
orientation polarization or the transfer of charges (protons frequency dampened semicircle is getting smaller. This
of a diffuse double layer or ions in the Helmholtz) along is a representation of the decrease in the resistance. The
with hydroxylic bonds or groups (surface charge trans- characteristic frequency that separates the two dampened
fer) at Stern layer (Schwan et al. 1962; Schwarz 1962). semicircles increases with the addition of saline water. Also,
There is a relaxation time distribution due to existence of the depression of the dampened semicircles increases with
different polarization discontinuous clusters of different an increase in the saline water saturation, i.e., increase in
dimensions on grains surfaces (Dukhin 1971; Gomaa and the conductivity (Grant 1958). Such dominance of the real
Elsayed 2009; Gomaa et al. 2009). resistivity over the imaginary resistivity, due to increase in
Charges either diffuse along with the discontinuous clus- saline water saturation, is representative to increase in con-
ters (of saline water) coating the grains or diffuse through tinuous conductor paths in the sample. The low-frequency
the bulk of the conducting grains of the specimen. When part of the dampened semicircle is a representation of the
charge surfaces contacts with liquid water, electrolytes are resistivity that controls the diffusion in addition to electrode
originated and the electrical field associated with ionic devi- polarization, which is dependent on saline water saturation
ation causes electrical conduction (Knight and Nur 1987). (Macdonald 1974; Roberts and Lin 1997; Knight and Nur
In the conductivity curves (Fig. 2), two adjacent regions 1987). Frequency domain of electrode effect extends to
are found with power law 𝜎 ∝ f 𝛼 of conductivity, with fre- higher frequencies with the addition of saline water (Knight
quency, with different slopes. In the first region, at relative and Nur 1987).
low frequencies, for low and high saline saturations, there
is slight dispersion of the conductivity. That region ends at
nearly 1 Hz for most of saturated samples. For very high Conclusion
saturations (above 1 Hz), no frequency dispersion is pre-
sent at the whole frequency range. Results of conductivity, Effects of saline water (4 g/100 g of NaCl) saturations on
at low frequency (0.0005 Hz), vary from 9 × 10−3 S/m for the electrical conductivity and dielectric constant, as a func-
low saturated clayey sandstone samples to 4 S/m , for high tion of frequency (0.0005 Hz–100 kHz), for partially and
saline water saturation. Also, results of the conductivity for fully saturated clayey sandstone samples are investigated.
high frequency ( 105 Hz) range from 2 × 10−2 S/m for low

13
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properties of magnetite intruded by magma, Egypt. Geophys J
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Open Access  This article is licensed under a Creative Commons Attri- Gomaa MM, Abou El-Anwar E (2015) Electrical and geochemical
bution 4.0 International License, which permits use, sharing, adapta- properties of tufa deposits as related to mineral composition in
tion, distribution and reproduction in any medium or format, as long South Western Desert, Egypt. J Geophys Eng 12(3):292–302
as you give appropriate credit to the original author(s) and the source, Gomaa MM, Abou El-Anwar E (2017) Electrical, mineralogical, and
provide a link to the Creative Commons licence, and indicate if changes geochemical properties of Um Gheig and Um Bogma Formations,
were made. The images or other third party material in this article are Egypt. Carbonates Evaporites 1–14
included in the article’s Creative Commons licence, unless indicated Gomaa MM, Alikaj P (2009) Effect of electrode contact impedance on
otherwise in a credit line to the material. If material is not included in a. c. electrical properties of wet hematite sample. Mar Geophys
the article’s Creative Commons licence and your intended use is not Res 30(4):265–276
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