Journal of Petroleum Science and Engineering 200 (2021) 108387

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Journal of Petroleum Science and Engineering

journal homepage: http://www.elsevier.com/locate/petrol

On hydrogen wettability of basaltic rock

Ahmed Al-Yaseri a, Nilesh Kumar Jha b, *
a
School of Engineering, Edith Cowan University, 270 Joondalup Dr, Joondalup, 6027, WA, Australia
b
School of Petroleum Technology, Pandit Deendayal Petroleum University, Knowledge Corridor, Raisan, Gandhinagar, 382007, Gujarat, India

A R T I C L E I N F O A B S T R A C T

Keywords: One of the major challenges pertaining to a full hydrogen economy is hydrogen storage in the Earth’s subsurface
Hydrogen geo-storage formations, such as deep saline aquifers and depleted oil and gas reservoirs. Generally, sedimentary basins are
Hydrogen wettability considered for this purpose due to their potential for large-scale storage. However, basaltic formations are also in
Deep saline aquifer
comparable proportions having voluminous volcanic rocks, vast expansions, and high thickness. We, thus, in this
Basalt formation
work, evaluate brine/hydrogen/rock wettability of the real Basalt rock samples from CarbFix site in Iceland.
Wettability is one of the significant parameters that highly influences the spreading and migration of the gas (as
seen for CO2 capillary trapping investigations), interfacial area, mass transfer, and mineralization. We carried out
brine/gas/Basalt three-phase contact angle measurements for some gases (CO2, N2, and He) under storage
conditions of high temperature (323 K) and pressures (5, 10, 15, and 20 MPa). The analogy drawn from
developed correlation for H2 from the contact angle trend of He (density close to H2 density) and empirical
correlations reveals that a strong water-wetting state of Basalt can be expected for H2. The high water-wetting
state of Basalt in the presence of H2 at storage conditions may be suitable for capillary trapping of H2 for long
term storage in Basaltic formation.

1. Introduction Their storage possibilities in such mediums are currently being

Is hydrogen the future? The quest for sustainable and clean energy
and the immense potential of hydrogen as the energy source can lead to
an answer. The term "hydrogen economy" was proposed by John Bockris
in 1970, at General Motors (GM) Technical Center (Abe et al., 2019). In
this system, energy needs are supposed to be predominantly met by
hydrogen, including production, storage, and transportation (Liu et al.,
2020). Hydrogen production processes can be thermochemical, elec­
trolytic, biological, or solar water splitting (Das and Veziroǧlu, 2001;
van der Roest et al., 2020; Wang et al., 2012; Zivar et al., 2020). How­
ever, their large-scale storage, for the mid to long term to meet a sea­
sonal or throughout the year demand, is possible in subsurface
geological formations (Abe et al., 2019; Amid et al., 2016; Bünger, 2014;
Reuβ et al., 2017; Sainz-Garcia et al., 2017; Zivar et al., 2020). Although
hydrogen storage has been tried in caverns (excavated or solution mined
salt and other minerals) (Bünger, 2014; Heinemann et al., 2018; Lankof
and Tarkowski, 2020; Lemieux et al., 2019; Taylor et al., 1986), a severe
lack of data and knowledge regarding storage in porous geological
mediums (such as depleted oil and gas reservoirs, aquifers) is restricting
their implementation (Zivar et al., 2020).
assessed due to their potential for large-scale storage (Foh et al., 1979;
Lord et al., 2008; Zivar et al., 2020). These mediums, which is presently
under consideration, are the sedimentary formations (Foh et al., 1979;
Lord et al., 2008; Yekta et al., 2018; Zivar et al., 2020). The other pos­
sibility could be Basalt formations, voluminous volcanic rocks on Earth,
having vast expansions and thickness highly comparable to sedimentary
basins (Ernst, 2014). Basalt formations are known to have thicknesses in
several km, and these sizeable igneous rock fields can have several
hundreds of square km of area. Basaltic formation in mid-ocean ridges
(MORBS) constitutes the top 1–2 km of the oceanic crust covering
approximately two-thirds of the Earth’s surface beneath the oceans
(Roex, 2006). Therefore, the probability of finding a suitable Basalt
formation having adequate porosity, permeability, storage capacity, and
trapping efficiency is very high. (Goldberg et al., 2018; Iglauer et al.,
2020). This opportunity can be tapped for storing hydrogen and its
withdrawal when required.
Brine/gas/rock wettability in rock’s microstructural porous space is
one of the most crucial parameters which drive the spreading and
migration of the gas (as seen for CO2 storage), interfacial area, mass
transfer, and mineralization (Al-Khdheeawi et al., 2017; Al-Yaseri et al.,

* Corresponding author.
E-mail address: nilesh.jha@spt.pdpu.ac.in (N.K. Jha).

https://doi.org/10.1016/j.petrol.2021.108387
Received 1 October 2020; Received in revised form 1 January 2021; Accepted 7 January 2021
Available online 11 January 2021
0920-4105/© 2021 Elsevier B.V. All rights reserved.
A. Al-Yaseri and N.K. Jha Journal of Petroleum Science and Engineering 200 (2021) 108387

2016a; Al-Yaseri et al., 2016b; Blunt, 2017; Chen et al., 2020; Fauziah et Table 1
al, 2019, 2020; Sarmadivaleh et al., 2015; Tiab and Donaldson, 2012). Experimental conditions and measured/calculated contact angles.
Wettability information concerning brine/H2/Basalt is presently un­ Gas Pressure/ Measured contact Calculated Densitya/
known due to the hydrogen geological storage hypothesis’s novelty in MPa angle/◦ equilibrium kg m− 3
such porous mediums. Therefore, in this work, we demonstrate that Advancing Receding
contact angle/◦
strong to weak water wetting conditions can be anticipated at realistic
CO2 0.1 0 0 0 1.64
storage conditions. The investigation was carried out by analogy drawn 5 45 40 42.61 104.84
from the developed empirical correlations from Basalt wettability’s 10 52 48 50.05 384.34
experimental results for other volatile gases. Note that experiment in a 15 59 55 57.04 699.75
lab environment directly involving a large volume of hydrogen under 20 65 62 63.52 784.29
high pressure and temperature conditions is also currently being eval­ N2 0.1 0 0 0 1.043
uated due to challenges such as its high activity, high compressibility, 5 18 14 16.2 51.93
low viscosity, and metal embrittlement (Zivar et al., 2020). 10 24 20 22.14 102.5
15 32 28 30.1 150.4
20 40 37 38.54 194.8
2. Experimental procedure
He 0.1 0 0 0 0.3
5 15 13 14.05 7.45
2.1. Sample characterization 10 18 16 17.04 14.5
15 24 22 23.03 21.19
Basalt samples used in this work is retrieved from cores collected 20 26 24 25.03 27.65
during coring of well KB-01 at a depth of 535 m, well located at CarbFix H2 0.1 0 0.07
injection site, Iceland (Aradóttir et al., 2012; Gislason et al., 2010; 5 9.88 3.77
Snæbjörnsdóttir et al, 2017, 2018). These middle-aged (between 300, 10 13.5 7.54
15 16.36 11.31
000 and 500,000 years) samples from Pleistocene are fine-grained 20 18.79 15.08
crystals having olivine tholeiitic composition with smectite and calcite
a
as secondary alteration minerals (Alfredsson et al., 2013). Total organic (Linstrom and Mallard, 2001), Error of contact angle measurements are
within ±3◦
carbon (TOC) of very tight (porosity < 1%) samples were measured to be
700 ppm. The non-glassy part of the samples is found (from XRD) to be
composed of labradorite (59 wt%), augite (37%), montmorillonite (4 wt 1991; Merath, 2008) with Young’s equation, we have the macroscopic
%), and quartz (0.3 wt%). equation (Al-Yaseri et al., 2016b; Garcia et al., 2008; Gatica et al., 2004)
given as
2.2. Experiments I
cosθl = Δρ − 1 (2)
γlg
Cut Basalt samples of size ~0.5 cm × 1 cm × 1 cm was cleaned with
air plasma for a minute to remove organic contaminants superficially ∞
∫
Where, I = − V(z)dz is van der Waal’s potential integral (Garcia et al.,
from the surface, only to an insignificant extent, though (as TOC is high). zmin
Average surface roughness (having a significant impact on the sub­ 2008; Gatica et al., 2004) and Δρ = ρlf − ρg (ρg is gas density and ρlf is a
strate’s contact angle measurements) in terms of root mean square value function of the substrate specific liquid/gas densities) (Merath, 2008).
was measured to be 210 nm (using an atomic force microscope, DSE Thus, combining this relation with equation (2) and after rearrange­
95–200 instrument). Such roughness magnitude has an insignificant ment, we get
effect on contact angle values (Al-Yaseri et al., 2016a; Alnili et al., ( )
2018). Synthetic reservoir brine of 2.2 M ionic strength was prepared cosθl = −
I
ρg +
I
ρlf − 1 (3)
from de-ionized water having an individual salt concentration of 4 wt% γlg γlg
each of NaCl and CaCl2, 1 wt% each of MgCl2, and KCl.
Advancing and receding contact angles were used to calculate
Subsequently, we measured the advancing (θA ) and receding (θR )
Young’s equilibrium contact angle, θl using the following relation
brine contact angles along the brine/gas/rock three-phase contact line,
(Chibowski and Terpilowski, 2008; Tadmor, 2004):
Table 1, as per the method described in our earlier work at the storage
( )
conditions (temperature ~ 323 K, pressures ~ 5, 10, 15, and 20 MPa) ra cos θA + rr cos θR
θl = cos− 1 (4)
(Al-Anssari et al., 2018; Al-Yaseri et al., 2016a; Ali et al., 2019; Arif rA + rR
et al., 2016; Iglauer et al., 2015; Jha et al., 2019, 2020). There were
√̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅ √̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅
three gases used in this process: CO2, N2, and He, respectively. { } { }
3 (sin θA )3 3 (sin θR )3
With. rA = 2 − 3 cos θA + (cos θA )3
and rR = 2 − 3 cos θR + (cos θR )3
2.3. Equilibrium contact angle calculation Equilibrium contact angles of brine, θl , in the presence of respective
gases as a function of pressure are plotted in Fig. 1. In this Figure, θl for
Subsurface flow processes are highly dependent on the three-phase brine/H2/Basalt is predicted based on the developed correlation. It has
contact angles (Blunt, 2017; Øren et al., 1998; Valvatne and Blunt, already been observed that the density of gas has a strong influence on
2004). In simpler terms, the contact angle (θl ) of a liquid droplet over the the contact angle (Al-Yaseri et al., 2016b), which is also regardless of the
rock surface in presence of a gas can be related to the interfacial tensions type of gas on most occasions (Zivar et al., 2020). We chose He for the
of the combinations of respective two phases, and is given by the purpose of developing this correlation as He density is closely matched
Young’s equation (Young, 1805): to those of H2 as a function of pressure, Fig. 2. The linear relation be­
(
γgs − γls
) tween cos θl and pressure has an R2 value of 0.96, which is a very good
cosθl = (1) match. The relation can be presented by
γgl
cos θl = − 0.0034ρ + 0.998 (5)
Where γ gs , γ ls , and γgl are interfacial tensions at gas/solid, liquid/solid,
and gas/liquid interfaces, respectively. Thus, using the known densities of H2, we calculated θl at pressures
Using the sharp-kink approximation (Dietrich and Napiãrkowski, 5, 10, 15, and 20 MPa, respectively, Table 1.

2
A. Al-Yaseri and N.K. Jha
Fig. 1. Equilibrium brine contact angles for CO2, N2, He, and predicted equi­
librium brine contact angles for H2 on Basalt substrate as a function of pressure
at constant temperature (323 K).
Fig. 2. Cosine of the equilibrium brine contact angles for He and predicted
equilibrium brine contact angles for H2 on Basalt substrate as a function of gas
density at constant temperature (323 K).
3. Results and discussion
We can observe that θl for H2 increases with an increase in pressure
like those observed for other gases, which is also consistent with liter­
ature data (Al-Yaseri et al., 2016a; Chiquet et al., 2007; Iglauer et al.,
2015; Sarmadivaleh et al., 2015). Also, all predicted θl for H2 is less than
those of He, N2, and CO2 for pressures greater than 0 MPa in the order of
CO2 > N2 > He > H2. This implies that the Basalt surface is strongly
water-wet (Jha et al., 2019) in the presence of H2, thus suggesting that
residual and capillary trapping in their pores will be greatest under the
storage condition (Iglauer, 2017; Krevor et al., 2015; Rahman et al.,
2016). This further implies that the trapping potential of Basalt is very
high for H2. Thus, it could be expected to have high containment secu­
rity in such formations for a more extended period if H2 is injected
successfully. Contrarily, the intermediate wetting state of rock, as seen
for CO2 at higher pressures, significantly increases gas movement up­
ward (as predicted), thus, reducing storage capacities jeopardizing
containment security (Al-Khdheeawi et al., 2017). Nevertheless, more
CO2 wetting (i.e., intermediate water-wet to CO2 wet) state of Basalt
may be favorable for Basalt-CO2 mineralization, thus, mineralization
trapping, if wet scCO2 dominates the rock-fluid interactions and
3
Journal of Petroleum Science and Engineering 200 (2021) 108387
concomitant mineralization (Loring et al., 2011; McGrail et al., 2009;
Schaef et al., 2013). In high contrast, the strongly water-wet state of
Basalt rock can be much favorable for H2 non-permanent storage (yet
with high containment security) as mineralization may not be possible
in storage conditions. At the storage condition (i.e., at 20 MPa and 323
K), the reported solubilities, in terms of molality (m), of CO2, N2, He, and
H2 are approximately 1.39 m (Deng et al., 2018), 0.55 m (Sun et al.,
2001), 0.078 m (Wiebe and Gaddy, 1935), 0.139 m (Chabab et al.,
2020), respectively. We can also see that both H2 and He have very low
solubilities as compared to CO2 and N2, further indicating the choice of
He in this work is a good approximation. Moreover, H2 dissolution in
brine is also low (even less than methane) due to the presence of salt;
(Krader and Franck, 1987); loss of H2 will be ceased both due to lower
dissolution and any possible mineralization. Thus, the possibilities of
dissolution trapping of H2 are very low, which might also be desirable in
its non-permanent geo-storage. But the loss of H2 by leakage can be
expected due to its high diffusion coefficient as seen for its high diffusion
in pure water. (SIMBECK, 2003) It would be interesting to investigate
how the effective diffusion coefficient, if adjusted for tortuosity and
salinity in real porous media (Shen and Chen, 2007), affects H2 leakage
potential. Comparatively, the reported derived contact angle data (in
terms of cos θ) from the capillary pressures and relative permeabilities
measurements for the hydrogen-water system for sandstone at the
storage conditions (shallow: 5.5 MPa, 293 K and deep: 10 MPa, 318 K) is
0.93 (θ ~ 22◦ ) and 0.82 (θ ~ 35◦ ), respectively (Yekta et al., 2018).
Thus, the reported data for sandstone at the storage conditions suggests
a strong water-wetting state too, which, however, is less intense than
reported in this work (which is an advantage).
The withdrawal of stored H2 at high rates to meet the frequent
market demands necessitates the injection of a cheap cushion gas (such
as N2) prior to the injection of H2 to maintain the formation pressure so
that the efficiency of the withdrawal cycle could be enhanced (Carden
and Paterson, 1979; Oldenburg, 2003; Zivar et al., 2020). An insignifi­
cant amount of loss of H2 may be expected due to mixing, which hardly
influences the safety and economics during the injection-withdrawal
cycle, as observed for natural gas storage-withdrawal (Bilgesu, 2006;
Foh et al., 1979). Thus, from Fig. 1, it can be clearly observed that
water-wet conditions for brine/N2/Basalt are significantly lower than
that for H2. Relatively more N2 wetting than H2 wetting can be favorable
for steady withdrawal as the wetting condition will be somewhat
favorable for further N2 injection for formation pressure maintenance.
4. Conclusion
The possibilities of H2 storage in a subsurface porous medium (such
as depleted oil and gas sandstone/carbonate reservoirs, aquifers, etc.)
for large-scale storage for its potential future demand driven usage in
short to long term is currently under assessment. However, a severe lack
of data on brine/gas/rock interactions restricts their implementation to
achieve a hydrogen economy. Moreover, despite their vast expansion on
the Earth’s surface, Basaltic formations have never been considered for
hydrogen storage like CO2 storage. Thus, in this work, we carried out
wettability measurements, which is crucial for capillary or residual
trapping, for some gases (CO2, N2, and He) by brine/gas/Basalt three-
phase contact angle measurements under storage conditions of high
temperature (323 K) and pressures (5, 10, 15, and 20 MPa). Thus, the
analogy drawn from developed correlation for H2 from the contact angle
trend of He (density close to H2 density) and empirical correlations re­
veals that a strong water-wetting state of Basalt can be expected for H2.
The strong water-wetting state of Basalt (even higher than that of
sandstone) in the presence of H2 can be highly favorable for capillary or
residual trapping of H2. Lower dissolution of H2 in brine further ceases
its loss due to mineralization (as hypothesized for CO2). Further,
wettability characterization also reveals that relatively higher N2 wet­
ting of Basalt rock makes N2 suitable to use as a cushion gas as it can be
injected for formation pressure maintenance for steady H2 withdrawal to
A. Al-Yaseri and N.K. Jha
meet the demand. However, H2 leakage potential needs to be investi­
gated due to its effective diffusion when adjusted for tortuosity and
salinity through brine in a real porous media. This study has implica­
tions on the large scale H2 subsurface storage by capillary or residual
trapping in a Basaltic formation.
Credit author statement
Ahmed Al-Yaseri: Conceptualization, Methodology, Resources,
Validation, Formal analysis, Investigation, Data Curation, Writing -
Original Draft, Writing - Review & Editing, Project administration.
Nilesh Kumar Jha: Conceptualization, Methodology, Validation,
Formal analysis, Investigation, Data Curation, Writing - Original Draft,
Writing - Review & Editing, Project administration.
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Acknowledgment
The authors wish to acknowledge the Carbfix consortium, especially
Dr. Sandra Snæbjörnsdottir and Prof. Stefan Iglauer, for providing the
Basalt cores.
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