Energy Reports 8 (2022) 461–499

Contents lists available at ScienceDirect

Energy Reports
journal homepage: www.elsevier.com/locate/egyr

Review article

A review on underground hydrogen storage: Insight into geological

sites, influencing factors and future outlook
∗
Nasiru Salahu Muhammed a , Bashirul Haq a , , Dhafer Al Shehri a , Amir Al-Ahmed b ,
Mohammed Mizanur Rahman c , Ehsan Zaman d
a
Department of Petroleum Engineering, College of Petroleum Engineering and Geosciences, King Fahd University of Petroleum &
Minerals, Dhahran, 31261, Saudi Arabia
b
Interdisciplinary Research Center for Renewable Energy and Power Systems (IRC-REPS), King Fahd University of Petroleum &
Minerals, Dhahran 31261, Saudi Arabia
c
Interdisciplinary Research Center for Advanced Materials, King Fahd University of Petroleum & Minerals, Dhahran 31261, Saudi Arabia
d
Maintenance Manager, BOC Ltd, Canning Vale, Western Australia, WA 6108, Australia

article info a b s t r a c t

Article history: Without remorse, fossil fuels have made a huge contribution to global development in all of its forms.
Received 6 October 2021 However, the recent scientific outlooks are currently shifting as more research is targeted towards
Received in revised form 29 November 2021 promoting a carbon-free economy in addition to the use of electric power from renewable sources.
Accepted 1 December 2021
While renewable energy sources may be a solution to the anthropogenic greenhouse gas (GHG)
Available online xxxx
emissions from fossil fuel they are yet season-dependent faced with major atmospheric drawbacks
Keywords: which when combined with annually varying, but steady, energy demand, results in renewable
Hydrogen energy excesses or deficits. Therefore, it is essential to devise a long-term storage medium to balance
Underground hydrogen storage their intermittent demand and supply. Hydrogen (H2 ) as an energy vector has been suggested as a
Hydrodynamics viable method of achieving the objectives of meeting the increasing global energy demand. However,
Wettability
successful implementation of a full-scale H2 economy requires large-scale H2 storage (as H2 is highly
Capillary pressure
compressible). As such, storage of H2 in geological formations has been considered as a potential
Relative permeability
Diffusion solution where it can be withdrawn again at the larger stage for utilization. Thus, in this review, we
Solubility focus on the potential use of geological formations for large-scale underground hydrogen storage (UHS)
Adsorption where both conventional and non-conventional UHS options were examined in depth. Also, insights
Chemical reactions into some of the probable sites, and the related examined criteria for selection were highlighted.
Modeling The hydrodynamics of UHS influencing factors (including solid, fluid, and solid–fluid interactions) are
summarized exclusively. In addition, the economics and reaction perspectives inherent to UHS have
been examined. The findings of this study show that UHS, like other storage systems, is still in its
infancy. Further research and development are needed to address the significant hurdles and research
gaps found, particularly in replaceable influencing parameters. As a result, this study is a valuable
resource for UHS researchers.
© 2021 Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license
(http://creativecommons.org/licenses/by-nc-nd/4.0/).

Contents

1. Introduction....................................................................................................................................................................................................................... 462
2. Hydrogen and its properties ........................................................................................................................................................................................... 463
3. Underground gas storage ................................................................................................................................................................................................ 464
3.1. Conventional storage options ............................................................................................................................................................................. 465
3.1.1. Salt caverns ........................................................................................................................................................................................... 465
3.1.2. Aquifer ................................................................................................................................................................................................... 466
3.1.3. Depleted oil and gas reservoirs .......................................................................................................................................................... 467
3.2. Non-conventional storage options ..................................................................................................................................................................... 468
3.2.1. Abandoned coal mine .......................................................................................................................................................................... 468
3.2.2. Lined hard rock caverns ...................................................................................................................................................................... 469

∗ Corresponding author.
E-mail addresses: bhaq@kfupm.edu.sa, bhaq225@gmail.com (B. Haq).

https://doi.org/10.1016/j.egyr.2021.12.002
2352-4847/© 2021 Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).
N.S. Muhammed, B. Haq, D. Al Shehri et al. Energy Reports 8 (2022) 461–499

3.2.3. Refrigerated mined caverns ................................................................................................................................................................ 469

4. Principle types of underground hydrogen storage....................................................................................................................................................... 469
4.1. Underground storage of pure H2 ....................................................................................................................................................................... 469
4.2. Underground storage of a mixture with natural gas in H2 ............................................................................................................................ 470
4.3. Underground storage of rich H2 mixture with CO, CH4 and CO2 (syngas or town gas) ............................................................................ 470
4.4. Underground methanation reactor (UMR)........................................................................................................................................................ 470
5. Global outlooks and potential sites................................................................................................................................................................................ 470
6. Hydrodynamics of UHS influencing parameters........................................................................................................................................................... 471
6.1. Solid parameters .................................................................................................................................................................................................. 471
6.1.1. Absolute permeability.......................................................................................................................................................................... 471
6.1.2. Effective porosity.................................................................................................................................................................................. 473
6.2. Fluid parameters .................................................................................................................................................................................................. 474
6.2.1. Fluid density ......................................................................................................................................................................................... 474
6.2.2. Fluid viscosity ....................................................................................................................................................................................... 475
6.2.3. Fluid–fluid interfacial tension............................................................................................................................................................. 476
6.2.4. Solubility ............................................................................................................................................................................................... 476
6.2.5. Diffusivity .............................................................................................................................................................................................. 478
6.3. Solid–fluid parameters ........................................................................................................................................................................................ 478
6.3.1. Wettability ............................................................................................................................................................................................ 478
6.3.2. Solid–fluid interfacial tension ............................................................................................................................................................. 481
6.3.3. Capillary pressure................................................................................................................................................................................. 483
6.3.4. Relative permeability ........................................................................................................................................................................... 484
6.3.5. Mobility ratio ........................................................................................................................................................................................ 485
6.3.6. Adsorption–desorption ........................................................................................................................................................................ 485
7. Hydrogen reaction in the subsurface environments .................................................................................................................................................... 486
7.1. Methanogenesis.................................................................................................................................................................................................... 486
7.2. Acetogenesis ......................................................................................................................................................................................................... 487
7.3. Sulfate-reduction.................................................................................................................................................................................................. 487
7.4. Iron-reduction ...................................................................................................................................................................................................... 487
8. Modeling perspective of the UHS................................................................................................................................................................................... 487
9. Economics of UHS ............................................................................................................................................................................................................ 490
10. Prospects and challenges................................................................................................................................................................................................. 492
11. Lessons learned and recommendations ......................................................................................................................................................................... 493
Declaration of competing interest.................................................................................................................................................................................. 493
Acknowledgment .............................................................................................................................................................................................................. 494
References ......................................................................................................................................................................................................................... 494

2021a,b). However, these energy sources are season-dependent

1. Introduction faced with major atmospheric drawbacks (sunlight and inten-
sity level), and geographical constraints which when combined
The most expensive contributions to the rising energy con- with annually varying, but steady, energy demand, results in
sumption are population increase and individual income. When renewable energy excesses or deficits (Heinemann et al., 2021a).
the world’s population hits 8.7 billion people in 2035, an addi- According to the IEA, world wind electricity production increased
tional 1.6 billion people will require energy (Zhang et al., 2016a). from 104 TWh in 2005 to 838 TWh in 2015, and world solar elec-
However, one of the major challenges is the tension between tricity production also increased from 4 TWh in 2005 to 247 TWh
the rising energy demand and the scarcity of conventional fossil in 2015 (U.S. Energy Information Administration, 2017). Based
fuel resources. Furthermore, the impact and continuous increase on this data, it is clear that electricity generation is substantially
in the environmental consequences (e.g., climate change) due to increasing with much attention coming from natural gas, nuclear
fossil fuel utilization has made this issue a hot topic of debate. and non-hydropower renewables such as wind, solar, geothermal,
Fossil fuels without penitence have brought about significant tide/wave/ocean, biofuels, waste, and heat (U.S. Energy Informa-
development globally, with the considerable success recorded tion Administration, 2017). Despite the successes reported, the
over the different spans of life. The future is uncertain, and global outlook on emission remains complex (Mouli-Castillo et al.,
efforts are being put in place to reduce some of the anomalies 2021). One of such complexities, for instance, is the application
caused by fossil fuels with an emphasis on CO2 emission (Tang of heat in buildings as over 17.5% of global emission comes
et al., 2021). One such initiative is the United Nations Framework from associated activities such as direct combustion of fuels in
Convention on Climate Change (UNFCCC)’s 2015 Paris Agreement. cookers and boilers (Mouli-Castillo et al., 2021; Staffell et al.,
This agreement aims to reduce CO2 emissions by keeping global 2019). Other complexities include emission from transportation
average temperatures well below 2 ◦ C over pre-industrialized industries. This further implies that GHGs emission is still a chal-
levels, with a goal of 1.5 ◦ C, with the hope of reaching net-zero lenge to even the developed countries around the world as the
emissions in the second half of the century (Hassanpouryouzb use of natural gas as a prime source for heat via direct combustion
et al., 2021; Rogelj et al., 2016). In the recent COP26 Climate is still much high (Mouli-Castillo et al., 2021).
Change Conference in Glasgow, this pledge was reemphasized A large percentage of power is being generated from renew-
as many countries strengthened their country’s 2030 goal with able energy resources with a fluctuating output. In a large elec-
a new pledge targeted towards hitting net-zero emissions by tricity network system with low energy output, these renewable
2070 (IEA, 2021). power sources can be balanced by conventional power genera-
The demand for clean, and renewable energy has prompted tion. However, electricity networks with higher output capacity
academics to look at alternative energy sources including but will require an improved energy storage system. Though batter-
not limited to wind, and solar (Nanda et al., 2015; Okolie et al., ies, compressed air, capacitors, or flywheels are storage mediums,
462
N.S. Muhammed, B. Haq, D. Al Shehri et al.
they are only applicable for the short term and at low-scale
electricity storage. Thus, it is essential to devise a long-term
storage medium to balance the intermittent demand and sup-
ply challenges affecting renewable methods. One such balancing
mechanism, considered by many to be part of the solution, is
to use hydrogen as an energy vector (Mouli-Castillo et al., 2021;
Gahleitner, 2013).
Hydrogen (H2 ) is an attractive energy storage option with a
high specific energy capacity of 120 MJ/kg and a clean combus-
tion product (Energy.Gov, 2021). Currently, it is mostly produced
either via natural gas (steam methane reforming — SMR) using
fossil fuel feedstock (blue and gray hydrogen) with an energy effi-
ciency of 65–85% (Amid et al., 2016) or by water electrolysis using
renewable sources (i.e., power to gas) with an energy efficiency
of 55%–75% based on electrolyzer capacity (Gahleitner, 2013).
While the SMR method for blue H2 production is considered clean
because the produced CO2 can be sequestered, other SMR process
leading to gray H2 production is not environmentally friendly as it
often contains impurities such as CH4 , Ar, CO, CO2 , and N2 (Laban,
2020). As an energy carrier, H2 has a low density of 0.089 kg/m3 at
standard conditions and as such, large-scale volumes of H2 , much
beyond the scope of surface-based storage facilities, are required
to store energy in the scale of GWhr to TWhr (Hashemi et al.,
2021a) to effectively balance the consumer demand and supply
during peak periods.
Using geological formations such as salt caverns, aquifers,
depleted oil and gas fields (Zivar et al., 2021; Tarkowski, 2019),
hard rock caverns (Lord et al., 2014; Lemieux et al., 2019), and
coal seams (more recent) (Keshavarz et al., 2021; Iglauer et al.,
2021a), such large scale (G–TWh) of energy in the form of H2 can
be stored in the underground since it provides ample volume for
storing H2 at higher pressure (thus high energy densities). This
large-scale storage is conducted via gas immobilization mecha-
nisms such as structural/stratigraphy, residual/capillary, mineral,
and dissolution trapping (Kalam et al., 2020; Kumar et al., 2020;
Ali et al., 2021a) or adsorption trapping in the case of coal seams
(Iglauer et al., 2021a).
Numerous reviews exist in the literature for H2 storage out
of which most are either addressing physical (compressed, liquid
or cryogenic tanks) or chemical (sorbents, metals, or chemical
hydrides) storage phenomena or different aspects of its storage
efficiency. However, few recent reviews exist on the concept
of underground hydrogen storage (UHS) in geological forma-
tions (Heinemann et al., 2021a; Zivar et al., 2021; Osman et al.,
2021; Cyran, 2021; Dopffel et al., 2021; Thaysen et al., 2021;
AbuAisha and Billiotte, 2021; Pan et al., 2021a). For instance,
Zivar et al. (2021) reviewed contemporary research contribu-
tions on UHS both experimentally and numerically. Pan et al.
(2021a) critically discussed influencing parameters for UHS at
pore scale and their extended reservoir scale effects. The effect
of microbial growth in porous media for depleted oil and gas
reservoirs (using the UK as a case study) with emphasis on en-
vironmental controlling factors is also presented (Thaysen et al.,
2021). Scientific insights on the potential challenges involved
to achieve large-scale H2 storage in porous media were also
captured (Heinemann et al., 2021a). Laboratory insights on the
transport mechanism for H2 migration in a tight rock salt cav-
ing during cyclic operations have been discussed (AbuAisha and
Billiotte, 2021). Microbial side effects, knowledge gaps, risk, and
opportunities for successful UHS implementation were reported
by Dopffel et al. (2021). Specifically, the influence of impurities
and rock fabrics on the mechanical properties of rock salt was
studied by Cyran (2021). While some of these recent reviews are
gaining significant attention to promote UHS operations, several
new research datasets have been published afterward, and as
such, a complementary review presenting all these outcomes to
463
Energy Reports 8 (2022) 461–499
enhance our current understanding of the subject in a robust
but concise form is required. Thus, in this review, a critical and
comprehensive overview in addition to the existing data on UHS
is reported.
The following section (Section 2) of this study provides back-
ground information on H2 and its properties as they apply to
subsurface storage. While Section 3 discusses general subsurface
gas storage systems, Section 4 focuses on the forms in which
H2 is stored underground. Section 5 discusses some highlights
on studied possible sites worldwide as well as the selection
methodologies adopted by recent studies. The hydrodynamics of
the influencing parameters (which include solids, liquids, and
solid–liquid interactions) are covered in Section 6. This review
also outlines the potential H2 reactions intrinsic to UHS in Sec-
tion 7, and related modeling studies for UHS are presented in
Section 8. In Section 9, economic evaluations were briefly given
before addressing the problems and potential (Section 10). Lastly,
Section 11 of this review provided learning outcomes and recom-
mendations. This study aims to provide the reader with the nec-
essary robust but concise information on H2 subsurface behavior
during storage.
2. Hydrogen and its properties
H2 is a vital component of the energy supply chain that con-
tributes virtually in every sector such as stability of energy grids,
the share of renewable energies, fossil fuel conservation, and re-
duced environmental impact caused by energy generation (Zhang
et al., 2016a; Sgobbi et al., 2016). When 1 m3 (cubic meter) of H2
is burnt (combustion reaction), it produces around 120 MJ/kg of
energy (which is relatively high). However, it has a significantly
lower energy potential than methane, which has a 44 MJ/kg en-
ergy potential (Energy.Gov, 2021). Since the energy released from
the production of a unit of H2 is lower than that consumed, H2 is
not considered as an energy source (Zivar et al., 2021; Panfilov,
2016) but rather as an energy carrier. Again, its ease and ability to
convert into electricity or heat supports its efficiency as an energy
carrier due to its transport and energy storage capabilities (Zivar
et al., 2021). In addition to its convertibility, it is capable of
replacing almost 60% of the natural gas used for non-industrial
activities due to its substantial energy potential (Davison et al.,
2010). It has been reported that losses due to energy transport
in the form of gas could be as low as 0.1% when compared with
power network losses (8%) (Zivar et al., 2021). Hence, in power to
gas technology, care must be exercised to minimize such losses
during transportation to achieve an economic operation.
The knowledge of the physicochemical properties of H2 helps
in achieving a successful storage operation. Hydrogen occurs as
a diatomic gas (H2 ) with a density of 0.089 kg/m3 at standard
temperature (25 ◦ C) and pressure (1 bar). At a low temperature
(−262 ◦ C), it is regarded as a solid with a density of 70.6 kg/m3 ,
as shown in the phase diagram in Fig. 1. At a temperature of
−253 ◦ C and a density of 70.8 kg/m3 , the liquid state’s extension
falls within the narrow zone between the triple point and critical
point (Züttel, 2004). H2 has a high penetrability because it is
the smallest chemical particle in existence, and it diffuses in
solids faster than other gases like methane (Züttel, 2004). As
displayed in Table 1, H2 is about 8 times less dense than CH4
and 22 times less dense than CO2 implying that more space and
pressure will be required for H2 to store the same mass amount
of gas. H2 lower viscosity and molecular weight could result in
its leakage because it remains highly diffusive when subjected
to high overburden pressured layers as compared to CH4 (Gas
et al., 2003). However, its higher mobility (due to low viscosity
and density) indicates that a lower residual amount of H2 will be
found in the porous media after storage during the withdrawal
N.S. Muhammed, B. Haq, D. Al Shehri et al. Energy Reports 8 (2022) 461–499

Table 1
Physicochemical properties of H2 , CH4 , and CO2 (Ugarte and Salehi, 2021; H2tools, 2021).
Properties H2 CH4 CO2
Molecular weight 2.016 16.043 44.09
Density @ 25 ◦ C and 1 atm 0.089 kg/m3 0.657 kg/m3 1.98 kg/m3
Viscosity @ 25 ◦ C and 1 atm 0.89 × 10−5 Pa s 1.1 ×10−5 Pa s 1.49 ×10−5 Pa s
Solubility in pure water @ 25 ◦ C and 1 atm 16 × 10−4 g/L 22.7 × 10−3 g/L 1.45 × 10−3 g/L
Boiling point −253 ◦ C −162o C −78.44 ◦ C
Critical temperature −239.95 ◦ C −82.3 ◦ C −31 ◦ C
Critical pressure 12.8 atm 45.79 atm 72.79 atm
Heating value range 120–142 kJ/g 50–55.5 kJ/g –
Diffusion in pure water @ 25 ◦ C and 1 atm 5.13 × 10−9 m2 /s 1.85 × 10−9 m2 /s 1.60 × 10−3 m2 /s
Flash point −253 ◦ C −188 ◦ C –
Flammability range 4–75 ◦ C 5–15o C –
Research octane number (RON) >130 125 –
Auto ignition temperature 585 ◦ C 540 ◦ C –

Fig. 1. H2 phase diagram (Tarkowski, 2019).
flammable. Thus, for a mixture with fuel content below the LEL
or above UEL, the fuel–air mixture becomes un-ignitable due
to lack of fuel or required amount of oxygen in the mixture
respectively (Mazloomi and Gomes, 2012).
The high penetrability of H2 in an underground context might
be problematic when using caverns as a storage facility because
caverns’ rocks are less sealing than aquifers and depleted hydro-
carbon reservoirs. The presence of water in the pore space, in
addition to the low solubility of H2 in water (0.00079 mol/mol
at 25 ◦ C) improves the tightness (sealing rigidity) of aquifers
and depleted oil and gas deposits (Tarkowski, 2019). Though salt
caverns do contain water (brine) and sump, they are primarily
influenced by H2 diffusion through the salt walls. Furthermore,
the presence of brine and sumps can lead to an increase in H2
humidity (Laban, 2020). More details on these characteristics of
the storage facilities are presented in the subsequent section.

stage which thus serves as a challenge to the containment of
the stored gas. This shows that, H2 storage will require a higher
capacity sealing system than CH4 and CO2 for high efficiency.
Further, its low solubility over CH4 in a hydrogen–methane–brine
system promotes less H2 loss due to dissolution even though
the high diffusivity promotes its losses via diffusion and dis-
persion (Amid et al., 2016; Zivar et al., 2021; Heinemann et al.,
2018). Unlike H2 and CH4 , CO2 can be stored in its supercritical
state due to its critical conditions (pressure and temperature)
adapting properties between liquid and gas. Besides, CO2 has a
higher solubility and diffusion compared to both H2 and CH4
when dissolved in water and as such, it forms carbonic acid which
is highly corrosive (Ugarte and Salehi, 2021).
Like any other fuel, H2 is flammable and potentially dangerous
and it shares many similarities with natural gas as both are lighter
than air (Abdel-Aal et al., 2005). Traditionally, fuels are burnt
only in the gaseous or vaporized state and H2 usually reaches its
gaseous state at a very low temperature based on its flashpoint.
Flashpoint on the other hand is the lowest temperature at which
fuel can vaporize to form a flame in the air in the presence
of an ignition source; and the lower the flashpoints the higher
the flammability (Astbury, 2008). Interestingly, H2 only requires
5% oxygen to maintain combustion whereas hydrocarbon-related
fuels require 12% (Abdel-Aal et al., 2005). This goes to show
that, H2 is inherently not an explosive until an ignition source is
activated. The low flashpoint of H2 over CH4 presented in Table 1
indicates its wider range of flammability. Thus, the lower the flash
point value of a gas, the wider the flammability range. The wide
flammability range between the lower explosion limit (LEL) and
upper explosion limit (UEL) results in several possibilities for H2
to be consumed as a fuel for combustion engines or turbines (Roy
et al., 2011; Momirlan and Veziroglu, 2005). LEL and UEL values
are the fuel concentration levels in the air to make the mixture
464
3. Underground gas storage
Gas storage is not a new concept. The advent of gas storage
in underground facilities is dated back to 1916 when natural
gas was stored in geological formations. The partially depleted
Ontario gas field (Canada) according to many is considered the
first successful underground storage project (Taylor et al., 1986).
Carbon geo sequestration (CGS) and natural gas are essential
analogs for H2 storage in the porous media. However, certain
operational differences (physical and chemical properties) unique
to H2 must be acknowledged for effective operation (Iglauer,
2017). An underground gas storage (UGS) facility is an artificially
created accumulation of gas in the natural environment at a
significant depth in the subsurface. It consists of the working
gas and the cushion gas. Traditionally, the working gas (i.e., H2
in this case), is the total amount of gas that is injected and
subsequently made available to customers after withdrawal. It
is one of the two operation specifications in addition to de-
liverability rate (i.e., injection and withdrawal rate of gas) that
characterized the reservoir. On the other hand, the cushion gas
(e.g., CO2 Oldenburg, 2003, CH4 Feldmann et al., 2016, N2 Feld-
mann et al., 2016; Pfeiffer and Bauer, 2015; Pfeiffer et al., 2017
and even H2 itself Lysyy et al., 2021) represents the unextracted
volume of gas that serves as a buffer for management purposes
and pressure maintenance (Amid et al., 2016) during injection
and withdrawal cycles (Lord et al., 2014). Again, it prevents
water from entering the stored compartment to enable optimum
storage space (Tarkowski, 2017).
While some studies suggested cushion gas selection based on
wettability as certain gases e.g., N2 (in sandstone/basaltic studies)
and CO2 (in mica study) exhibit higher wettability hence it will
promote easier separation during injection/withdrawal cycles,
others, however, attribute selection based on cost (Pfeiffer and
N.S. Muhammed, B. Haq, D. Al Shehri et al.
Bauer, 2015; Pfeiffer et al., 2017) as it reduces investment capac-
ity when using N2 and also facilitates the displacement of water
(based on its higher density and viscosity as compared to H2 ) to
achieved optimum storage space. Feldmann et al. also suggested
density difference as a basis for cushion gas selection (Feldmann
et al., 2016). In a recent study by some groups, the authors
highlighted that cushion gas to working gas capacity is largely
dependent on geological parameters including reservoir depth,
trap shape, and reservoir permeability (Heinemann et al., 2021b).
Additionally, the authors pointed out that, cushion gas cannot
increase the total storage capacity of a storage site but rather
plays a significant role in the exploitation of the available storage
capacity as efficiently as possible. All these above conditions
indicate the sequential approach used by different studies when
selecting cushion gas for UHS operation. However, the use of H2
itself as a cushion gas as suggested by Lysyy et al. (2021) remains
a major uncertainty thus, a rigorous simulation study is required
to investigate such assertions. Possibly, suggesting the use of
H2 as a cushion gas could be as a result of avoiding the effect
of mixing and dilution (https://youtu.be/2VqAeYU22n0) which is
often observed in other gases. However, this will be an economic
boost to the H2 project perhaps if achieved as it will go a long
way in reducing the cost associated with cushion gas application
during UHS operations.
Underground gas storage is useful because they (i) provide
safety for the stored gas (less sensitive to fire and attacks), (ii)
space management, (iii) economics, and (iv) availability of suit-
able geological formations that are similar to many countries
throughout the world (Tarkowski, 2019). Also, they are a better
option for storing excess produced electricity in the form of H2 for
future use when consumption needs exceed production as previ-
ously discussed. As a result, several initiatives have been funded
around the world to investigate the viability of H2 production,
transportation, storage, and utilization to boost the H2 economy.
Some of these projects launched include Roads2HyCOM (An-
derson et al., 2009), HyStorPor (Edlmann et al., 2021), HyUn-
der (Simon et al., 2015), H2 STORE (Henkel et al., 2013), AN-
GUS+ (Kabuth et al., 2017), SUN. STORAGE (RAG Austria, 2020),
Hychico (Pérez et al., 2016), ADMIRE (Hashemi et al., 2021a,b),
and many more. All these projects show the global commitment
towards meeting a long-term emission reduction goal in the
nearest future. Therefore, understanding the general outlooks and
research developments of the underground storage sites is highly
essential.
In this study, underground storage sites are grouped into
conventional (salt caverns, aquifers, and depleted hydrocarbon
reservoirs) and nonconventional (abandoned coal mines, lined
hard rock caverns, and refrigerated mined caverns). Despite only
two cases reported H2 storage in coal seams (Keshavarz et al.,
2021; Iglauer et al., 2021a) as of the time of this review, coal
seams are considered as the next phase in the future (due to
ongoing research and development of new storage frontiers), par-
ticularly in areas where the commonly used salt caverns, aquifers,
and depleted oil and gas reservoirs become inaccessible due to
technical occurrences. Each of these UGS alternatives has its own
set of characteristics, which will be detailed further below.
3.1. Conventional storage options
3.1.1. Salt caverns
Caverns are artificial chambers created (drilled) within salt
domes or bedded salt deposits in a thick cylindrical pit by con-
trolled freshwater injection from the surface down to the de-
posits. Solution mining (Lemieux et al., 2019) is the name given
to this essential process. Fig. 2 is a typical representation of
a salt cavern structure and the effect of different dissolution
465
Energy Reports 8 (2022) 461–499
techniques. A typical salt cavern can be up to 2000 m deep,
1,000,000 m3 volume, 300 to 500 m height, and 50 to 100 m
diameter, allowing for massive storage amounts (Michalski et al.,
2017) and a pressure window of 30 to 80% of the lithostatic
pressure (Stolten and Grube, 2010). Salt domes are solid and
homogeneous bodies, hence, building a cavern which is struc-
turally robust for an operating depth of fewer than 2000 meters
is easier. However, at a depth beyond 2000 m, salt deformation
may occur due to increased pressure and temperature even when
a well-engineered cavern is constructed (Bruno and Dusseault,
2002). On the other hand, bedded salts are thinner layers found
at a considerably shallower depth than domes, with salt halite
(e.g., NaCl) alternating with non-soluble beds such as dolomite,
anhydrite, and shale (Foh et al., 1979; Han et al., 2006). It is
critical to note that UHS caverns built on bedded salt formations
are thinner and less stable due to the rock type’s high degree of
heterogeneity (Bruno and Dusseault, 2002; Han et al., 2006).
Clearly, caverns’ long-term structural stability and serviceabil-
ity depend on their material heterogeneity and complex geome-
tries (Kumar et al., 2021), thus, understanding their influence
on the state of stress is highly essential. Rock salts are known
to undergo a non-linear creep deformation due to the long-
term loading effect caused by underground storage (Kumar et al.,
2021). Primarily, creep processes are a phenomenon where a solid
material permanently deforms with time under the influence of
continuous mechanical stress. The solid material upon application
of external load could undergo any of the three stages of creep
namely — transient (primary or reduced), steady (secondary or
stationary), and tertiary (accelerated) (Altenbach and Naumenko,
2007) depending on the confinement space and time, thus, pre-
dicting the accurate resultant stress evolution and deformation
overtime for the safety of the storage facility even up to abandon-
ment phase is critical. Deformation mechanism of creep in salt
caverns are often governed by either the motion of grains within
the crystal structure or by a range of grain boundary processes as
it was reported that dislocation creep and solution-precipitation
creep (refer to Kumar et al., 2021) are the two main deformations
mechanisms that have been investigated via laboratory test and
micro-structural analysis. A few studies have also investigated
the influence of geometrical and material heterogeneity on the
state of stress (and deformation) in salt caverns over a long-
time loading using different frameworks (models and numerical
experiments) (Firme et al., 2016, 2019; Castelletto et al., 2017;
Kumar and Hajibeygi, 2021; Khaledi et al., 2016). While success
has been recorded in terms of cavern shape, elastic and inelastic
creep properties, and sensitivity analysis to evaluate which pa-
rameters often constitute the structural stability of salt caverns, it,
therefore, becomes significant to highlight that technical feature
are the most important factor in cavern design as compared to
porous media (aquifer and depleted hydrocarbon reservoirs).
Caverns are often regarded as the best option for UHS due to
their low gas permeability, good rheology — which contributes
to excellent sealing strength, and ability to redistribute stresses
via viscous-plastic deformation (Lemieux et al., 2019). Because
of the sealing nature of evaporite (such as anhydrite, gypsum,
and rock salts) and the mechanical stability of salt caverns, the
injection and withdrawal process is suitable for medium and
short-term storage (Sainz-Garcia et al., 2017). Furthermore, due
to the high salinity nature, caverns may not be affected by in-
situ biological activities of microorganisms because microbes’
activities are ineffective at this condition (Gregory et al., 2019;
Jaakkola et al., 2016). These, however, are often applicable to
artificially built salt caverns as they are generally prone to lower
risk of microbial activities. However, in a naturally occurring
high salt environment (i.e., salt lakes or salt ponds), salt-tolerant
(halotolerant) or salt-loving (halophilic) microorganisms may be
N.S. Muhammed, B. Haq, D. Al Shehri et al.
Fig. 2. Salt cavern schematic showing different dissolution setups (Wallace et al., 2021).
present thus salt caverns does not significantly prevent the risk
of microbial reactions via H2 consumption (Dopffel et al., 2021).
The major point of note will be how and to what extent are
these special microorganisms introduced into the caverns. Dopffel
et al. suggested either the water used for melting the caverns
during injection or a continuous long-term operation may have
promoted their formation (Dopffel et al., 2021). Similarly, H2 S due
to sulfate-reducing bacteria may also be present in salt caverns
(Laban, 2020).
During the design and planning phase, the depth and thickness
of the salt beds, the composition of the distributed rock in the
reservoir, and solubility are all-important selection criteria for
UHS in salt deposits. As previously stated, certain properties
increase the tightness of the rock; however, this may be ham-
pered by non-salt rock intercalations in the salt beds, which may
result in migration pathways for the stored gas (Tarkowski, 2019).
Cushion gas requirements for salt caverns can vary substantially
due to site-specific factors such as depth and the required storage
capacity (Lord et al., 2014). For example, more cushion gas is re-
quired in a cavern with a higher depth due to increased pressure,
resulting in more compressed gas storage, whereas caverns with
a lower depth require less cushion gas, which helps to reduce
operational costs (Zivar et al., 2021). Cushion gas capacity of
about 22 and 33% of the volumetric capacity implying up to 78%
working gas has been reported (Wallace et al., 2021). Despite
their size, some salt caverns have been identified as possible UHS
sites (Michalski et al., 2017; Tarkowski and Czapowski, 2018;
Liebscher et al., 2016; Stone et al., 2009; Lord, 2009; Crotogino
et al., 2018). The three-salt cavern reported in the UK in 1972, two
salt caverns in the US in 1983, and the Kiel town gas project in
Germany are all examples of successful H2 storage. The projects’
experience suggests that H2 may be stored in salt caverns for a
long time (Panfilov, 2016; Stone et al., 2009; Simón et al., 2014).
On a more general note, salt caverns face significant issues
such as the need for more water for leaching and the proper
disposal of the brine collected. Other technical factors such as
distance from the major pipelines and the availability of techno-
logical waters are two more elements that must be considered
for economic reasons (Zivar et al., 2021). Because all processes
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(multiple injection and withdrawal per year) are carried out using
a single well, developing salt caverns is less expensive than other
subsurface projects (Wallace et al., 2021). It is worth noting that
the casing and installation’s strength is determined by the gas
capacity and position, the deposits (salt dome or bedded salt), and
the possible cavern’s size. Salt caverns are particularly important
since they are the most acceptable alternative for storing peak
gas reserves due to their simplicity of control during injection and
withdrawals (Tarkowski, 2019).
3.1.2. Aquifer
An aquifer is a subsurface layer of permeable and porous rock
that is filled with fresh or saline water and is often hundreds of
feet deep. In the absence of caverns and depleted hydrocarbon
reservoirs, they are primarily utilized for UHS. They present better
UHS options since they are commonly found in all sedimentary
basins around the world. The storage mechanism for aquifer and
depleted hydrocarbon reservoirs are similar since they are both
characterized as porous and permeable. However, basic geological
requirements must be satisfied, such as (i) the host rock for
injection has good reservoir properties, and (ii) the host rock for
injection has good qualities to prevent the migration of the stored
gas (Tarkowski, 2019). An aquifer schematic showing the porous
and permeable formation (before and after H2 injection), as well
as an impermeable seal for preventing vertical migration due to
buoyancy and an anticline trap to prevent lateral migration of H2
away from the well for effective plume build-up, is presented in
Fig. 3.
When H2 is injected into an aquifer that was previously filled
with water, a change in density occurs between the injected
gas and the liquid due to a rise in pressure, causing the liquid
to be displaced downward or sideways to create storage space.
A liquid–gas interface is generated as a result of the continual
increase in pressure during injection activities, in addition to the
displacement. Unfortunately, the established interface becomes a
disadvantage to the UHS via aquifer because it affects the with-
drawal process. As a result, the gas–liquid interface movement
during H2 withdrawal is projected to lead to the simultaneous
generation of liquid during gas withdrawal (Zivar et al., 2021;
N.S. Muhammed, B. Haq, D. Al Shehri et al.
Fig. 3. Aquifer schematic (a) before H2 injection, and (b) after H2 injection (Wallace et al., 2021).
Pfeiffer and Bauer, 2015). It is critical to emphasize that the
volume of gas that may be stored is determined by the reser-
voir volume and porosity, and the temperature and pressure of
the stored gas (Tarkowski, 2019). Cushion gas requirements for
aquifers are generally higher than those for depleted reservoirs
because the naturally existing gas found in some depleted reser-
voirs to counteract the total volume needed is not available. As a
result, the amount of cushion gas in aquifers could be as high as
80% of the entire reservoir capacity indicating that working gas
could be as low as 20% (Lord et al., 2014).
Several factors are reported to have an impact on the UHS
operation via aquifers, including undetected leakage (migration)
along faults, biological processes, and H2 reactivity with miner-
als in the reservoir rock. Most importantly, because geological
knowledge specific to the aquifer type may not be available,
aquifer storage is significantly more expensive than depleted oil
and gas reservoirs (Lord et al., 2014). As a result, new wells must
be drilled to conduct a more thorough and exhaustive investi-
gation. Furthermore, since the probability of H2 leaking to the
surface in an aquifer is low, an underground safety device such as
a subsurface safety valve (SSSV) can be built into the well during
construction to automatically avoid any possible problems (Zivar
et al., 2021; Tarkowski, 2019).
Currently, no pure 100% H2 storage has been successfully
achieved in aquifers. However, the town gas project (produced
by gasification of coal which contains notable amounts of H2
and other components) has been documented as the few storage
aquifer project in Europe (Liebscher et al., 2016). These aquifers
reported are Ketzin in Germany, Lobodice in the Czech Republic,
and Beynes in France (Panfilov et al., 2006; Kruck et al., 2013).
Aquifers are the ideal option for seasonal H2 storage (Sainz-Garcia
et al., 2017).
3.1.3. Depleted oil and gas reservoirs
To date, the depleted reservoir is the conventional storage
means for natural gas. They are characterized as porous and
permeable hydrocarbon reservoirs located thousands of feet be-
neath the subsurface with almost all the recoverable products
being extracted (Tarkowski, 2019). In specific terms, they can be
considered as a portion of an aquifer (geological traps) where
only residual amounts of water exist within the pores which
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Energy Reports 8 (2022) 461–499
are predominantly occupied with trapped oil/gas (Wallace et al.,
2021) [see Fig. 4]. Generally, they are easy to develop, operate and
maintain due to the already existing infrastructure with proven
integrity (Lemieux et al., 2019). Depleted hydrocarbon reservoirs
have proven credence since; they have previously trapped hy-
drocarbon that migrated from the underlying source rocks and
has a well-identified geological structure. The trapping system is
either structural (anticline) or stratigraphic (impermeable layer),
depending on the nature of the reservoir diagenesis (Lord et al.,
2014). They serve as a suitable storage container, with suffi-
cient permeability to meet the operational flow and a successful
trapping system to prevent fluid migration via leaking.
In comparison to aquifer UHS options, depleted gas reservoirs
are more advantageous in that the existence of the remaining gas
serves as a benefit to prevent a massive amount of cushion gas
required for pressure maintenance during operations. Between
50 to 60% cushion gas is required as compared to the 80% for
aquifer (Lord et al., 2014; Wallace et al., 2021). However, if
the remaining gas in the depleted reservoir affects the purity
of the injected gas (i.e., H2 ), then it can hinder the integrity
of the stored gas during withdrawal (Kruck et al., 2013). Both
aquifer and depleted hydrocarbon storage options however are
the best choices for seasonal gas storage due to their flexibility of
cycling (Tarkowski, 2019; Sainz-Garcia et al., 2017).
When planning and developing the UGS or UHS facilities in a
depleted gas deposit, it is critical to stop gas extraction as soon
as possible. This enables storage to be built in less time and
at a lesser cost. In around five years, newly built UGS facilities
usually reach their anticipated exploitation parameters. During
this time, formation waters that invaded the gas deposit after
its exploitation ended are being discharged (Tarkowski, 2019). As
a point of note to depleted gas reservoirs, the underground gas
maximum pressure in the site is often greater than the original
reservoir pressure. This suggests that more gas can be stored than
initially present in the reservoir (Zivar et al., 2021). In the case
of a depleted oil reservoir with no preceding gas, more thorough
knowledge is required because various reactions could compro-
mise the injected gas’s integrity. For example, residual oil in the
reservoir may cause a chemical reaction that converts injected H2
gas to methane, lowering H2 purity and possibly causing the oil to
dissolve and become irreversibly lost forever (Zivar et al., 2021).
Table 2 present a summary of the different characteristics of the
conventional UHS facilities.
N.S. Muhammed, B. Haq, D. Al Shehri et al. Energy Reports 8 (2022) 461–499

Fig. 4. (a) An overview of a depleted reservoir condition, (b) microscopic image of reservoir pores filled with oil, and (c) shows how injected H2 occupies the pores
while oil evacuates the pores (Wallace et al., 2021).

Table 2
UHS characteristics for different geological formations.
Source: Modified after (Visser, 2020).
Geological Storage Discharge Initial cost Cyclic cost Seismic risk Chemical Cushion gas Leakage Usability
type capacity rate conversion requirement risks purpose
rate
Caverns Based on High High Low Low Low Low Low Frequent
cavern size
Aquifer High Low Average Average High High High High Seasonal
Depleted High Average Average Average Average Average Average High Seasonal
reservoirs

3.2. Non-conventional storage options
The UGS potential outlined in the previous section is unique
to H2 storage and other related gases (CO2 , CH4 , town gas, and
syngas). Other storage solutions become necessary where typical
storage choices for UGS storage are not available, such as the
Northeast, Southeast Atlantic, and Pacific Northwest. The geology
of these areas is dominated by coal, shale, and igneous and
metamorphic rocks. Because of the constant demand for natural
gas in these areas, alternative storage options such as aban-
doned mines, hard rock caverns, and refrigerated mining caverns
have been implemented. As for completeness to the known UGS
in the literature, a summary of these storage repositories and
some published literature on their use in gas storage is briefly
discussed.
3.2.1. Abandoned coal mine
Coal mines are places where coal is extracted underground.
They are prized for their high energy content and are commonly
utilized to generate power. Steel and cement sectors, for example,
employ coal as a fuel for ore mining and cement manufacturing,
respectively (Deng et al., 2019; Schissler, 2004; Jonek-Kowalska,
2018). Sites in which natural resources such as coal, salt, or
468
limestone were previously mined, can under certain conditions
be converted into gas storages if the underground workings are in
a very homogeneous, tight, and stable rock type (Crotogino et al.,
2018).
Abandoned coal mines are those where mining operations
have been completed or the coal beneath the surface is uneco-
nomical to remove. As a result, these locations are being inves-
tigated as prospective gas storage sites (e.g., CO2 and CH4 ) (Jalili
et al., 2019). The amount of natural gas that may be stored in a
coal mine is determined by the adsorption rate of the unmined
coal as well as the volume mined. The mining history and geology
surrounding the mine are critical for a coal mine to be appro-
priate for natural gas storage because they inform the required
pressure and strategy for the operation. The mined coal seam, like
other conventional methods (caverns and porous media), must be
protected by an impermeable layer to achieve successful gas trap-
ping. The pressure at which the mine may operate is determined
by the geology and surrounding hydrostatic pressure (Lord, 2009).
Natural gas, in this context, has been the most widely used
gas since 1961. Three cases have been recorded from around the
world. Two of these are in Belgium (the abandoned coal mines
of Peronnes and Anderlus) and the other is in the United States
(the abandoned coal mine of Leyden) (Ridge, 1998; Piessens and
N.S. Muhammed, B. Haq, D. Al Shehri et al.
Dusar, 2004). These projects were designed to satisfy peak de-
mand while avoiding natural gas peak pricing (Jalili et al., 2019).
All three have now been decommissioned (Lord, 2009). Nev-
ertheless, due to their annual recycling flexibility, abandoned
coal mines are still being investigated as an alternate option for
storing significant volumes of gas (Ridge, 1998).
The Leyden mine formation in Colorado is made up of an
underlying aquifer that is sealed by 20-meter-thick impermeable
claystone. Alternating layers of concrete and gravel were used
to seal the abandoned shafts. The mine was initially built to
supply gas to the Denver area during high-demand periods. It
could cycle for more than 100 days a year, allowing it to satisfy
daily fluctuations in gas demand. The Public Serving Company of
Colorado (PSCo) began gas storage in the late 1950s, according
to the Environmental Protection Agency (EPA), and roughly 750
Mm3 was stored (Ridge, 1998). Similarly, the Anderlus and Per-
onnes mines have had success with natural gas seasonal storage.
Specifically, the Anderlus operation began from 1857 to 1969 and
was capable of storing around 180 Mm3 of CH4 based on reservoir
volume, whereas the Peronnes mine, which lasted from 1860 to
1969, was only capable of holding 120 Mm3 of CH4 . However, the
storage mechanism is through CH4 adsorption on the surface of
coal within its micropore structures (Lord, 2009).
3.2.2. Lined hard rock caverns
Caverns, as previously mentioned, are artificial chambers exca-
vated in sedimentary deposits such as salt domes or bedded thin
layers; however, not all sedimentary regions are sedimentary;
some are metamorphic or igneous. Improved technology has re-
cently been investigated for creating caves (either by shaft sinking
or blasting) and encasing them with steel or plastic liners (Lord
et al., 2014; Lemieux et al., 2019). Using hydrostatic pressures
from groundwater or water curtains, the designed lining operates
as an impervious layer that facilitates total containment of the
stored gas. In comparison to unlined caverns that are not entirely
impervious, these caverns must be operated at a higher pressure.
Lined hard rock caverns, like salt caverns, can be withdrawn in
multiple cycles and can deliver large amounts of gas (Sofregaz
US Inc, 1999).
The strain on the lining is mainly determined by the amount
of rock deformation (Sofregaz US Inc, 1999). The concrete layer is
then built during the design phase to transfer the pressure load
from the cavern to the surrounding rock and to provide a smooth
surface for the lining. Stainless steel or polypropylene plastic can
be used to make liners (Lord et al., 2014; Lord, 2009). The follow-
ing conditions must be met to ensure the lining’s effectiveness.
These are (i) should be gas-tight and chemical-resistant, (ii) not
designed to carry the load, and (iii) resist small elastic or plastic
deformation that may occur at the host rock’s surface (Sofregaz
US Inc, 1999; Glamheden and Curtis, 2006). Furthermore, the
cushion gas injected to maintain pressure within the storage
system will be minimal because hard rock caverns are structurally
stable. In addition, a groundwater drainage system is installed
around the cavern’s periphery to alleviate hydrostatic pressure
against the liner during depressurization (Sofregaz US Inc, 1999).
This new storage system has been used to store natural gas
in both unlined (Haje project, Czech Republic) and lined (Skallen
project, Sweden) hard rocks (Lemieux et al., 2019). Similarly, the
Nuclear Waste Management Organization (NWMO) and Ontario
Power Generation (OPG) investigated the feasibility of storing
waste in deep geological repositories in both sedimentary and
crystalline rock formations. This demonstrates the possible stor-
age capacity of hard rock for gases, and it is envisaged that, with
continued study and development, H2 -based storage initiatives
would eventually become the next focus in this storage facility
in areas where traditional ways are unavailable (Lemieux et al.,
2019).
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Energy Reports 8 (2022) 461–499
3.2.3. Refrigerated mined caverns
The unveiling of hard rock caverns explained previously indi-
cates the high economics involved in construction and installa-
tions if implemented. However, in terms of excavation costs, a
less expensive storage solution known as refrigerated mined cav-
erns could be used as a replacement. In this technology, the gas is
chilled to a specific temperature before being placed into storage.
As with gases, the effect of cooling brings about compression and
reduction in temperature (cryogenic) which results in less storage
volume. It is reported that gas cooled to −40◦ F will require
less storage space because the volume is reduced by 50% (Lord,
2009). They have good storage potential, a lot of flexibility, cycle
capacity, and a large delivery rate. They are also thought to be the
optimal storage solutions in locations where salt deposits are not
present. Based on their multiple cyclicities, they can be used as a
storage option for seasonal periods (Freeway, 1998).
Because refrigerated mined caverns are not lined, igneous and
metamorphic rock is preferred. They must be self-supporting and
impermeable. There should be no faults, joints, or shear zones
in the primary (host) rock (Freeway, 1998). As with any caverns,
the required amount of cushion gas hugely depends on the depth
and since the design of a refrigerated mined caverns is limited
to a depth range of 2500 to 3000 m, minimum cushion gas
is required to maintain the pressure of the stored gas through
fissures and crack to reduce the water influx from the surface.
A more significant proportion of cushion gas prevents the gas
from recompressing during withdrawal, whereas a lower amount
allows for smaller caverns with more working gas. Furthermore,
the maximum working pressure should not be higher than the
hydrostatic pressure (Freeway, 1998).
4. Principle types of underground hydrogen storage
UHS clearly represents a unit of the entire energy cycle, (ini-
tial energy production – conversion or not to H2 –H2 storage –
reconversion or not of H2 to other energy type – and energy
consumption). The objectives and methods of UHS are strongly
reliant on the interaction of all of these aspects. If the goal is
to store pure H2 and use it in fuel cells later, for example, any
chemical modification of H2 during storage should be avoided.
On the contrary, if the H2 is to be used in gas-fired turbines or
injected into natural gas pipelines, the addition of methane or
other energy carriers to the stored gas is likely to be welcomed.
On this note, four forms of underground storage can be distin-
guished depending on the manner of the energy used initially
for the production, the form of the final energy consumed, the
methods of energy conversion, and the combination between
these elements.
4.1. Underground storage of pure H2
In this method, only the pure form of H2 is stored under-
ground, and the destination of the final form of the pure H2 is
fuel cell application (Panfilov, 2016). Salt caverns, with a high
degree of purity characterized by a very low risk of potential
gas contamination by impurities, are the most convenient storage
sites for ultra-pure H2 . The pure H2 is mainly produced through
chemical or thermal electrolysis from the excess renewable elec-
tricity (e.g., windmills, solar cells) or from the nuclear plant, as
seen in Fig. 5. As a result of the method used in production and
the intermittent mode of functioning coupled with the strong nat-
ural fluctuations (Kabuth et al., 2017), part of the excess energy
produced is stored for future application. Later, the stored H2 is
extracted and reconverted via an electrolyzer during periods of
increasing demand, and then converted back to electricity in fuel
cells which is applied in vehicles.
N.S. Muhammed, B. Haq, D. Al Shehri et al.
Fig. 5. Energy cycle of the excess electricity production converted to H2 , stored in a salt cavern, extracted during periods of increased consumption, and reconverted
into electricity in fuel cells for vehicles (Panfilov, 2016).
Fig. 6. Energy cycle consisting of renewable electricity or a nuclear plant source, an electrolyzer, and underground storage site of natural gas, from which the gas
produced is injected into a gas pipeline (Panfilov, 2016).
4.2. Underground storage of a mixture with natural gas in H2
Pure H2 in this case, is produced through water electrolysis
before injecting into an underground site containing natural gas
for transportation. The industry currently allows only a small
amount of H2 (6 to 15%) so that the energy potential of the
stored gas is not reduced substantially (Panfilov, 2016). Fur-
thermore, the durability of the gas transport system (pipeline
in this case), which is often affected by H2 embrittlement, is
not damaged during transportation. This form of H2 storage is
applied for transportation purposes, especially when a long dis-
tance between the production site of the CH4 gas and consumer
market is less than 2000 km (He et al., 2019). Different separation
techniques, including pressure-swing adsorption (operates at <
20% H2 concentration), membrane separation (at relatively higher
H2 concentration), and electrochemical H2 separation, are used to
separate the blended H2 and CH4 before consumption (used as
fuel). The energy cycle for this process is shown in Fig. 6.
4.3. Underground storage of rich H2 mixture with CO, CH4 and CO2
(syngas or town gas)
Syngas is produced through the mixture of H2 (20%–40%) with
CO whereas town gas is the mixture of H2 (50%–60%) with CO
and CH4 . CO is regarded as an energy carrier in either case,
but with a lower potential than H2 . The presence of CO2 largely
depends on the production technique; thus CO2 may be present
in both syngas and town gas respectively (Panfilov et al., 2006;
Panfilov, 2010). This type of mixture is formed through superfi-
cial or underground coal gasification, which involves introducing
vapor at 1073 K together with O2 to represent coal combustion.
It is reported that the latest version of this technology (coal
gasification) allows about 70% H2 for the mixture and it can be
consumed in two forms namely (i) as electricity in gas turbines
via thermo-mechanical conversion and (ii) as fuel for lighting
and heating especially in the case of town gas (Panfilov, 2016).
The energy cycle shown in Fig. 7 consists of a coal gasification
plant for syngas or town gas production, with the UHS options
(aquifer, cavern, or depleted reservoir) and a gas-fired turbine for
gas conversion to electricity or direct fuel application.
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Energy Reports 8 (2022) 461–499
4.4. Underground methanation reactor (UMR)
This form of H2 storage was first suggested by Panfïlov (Pan-
filov, 2010). As compared to syngas or town gas, UMR represents
an H2 mixture with CO2 in the presence of methanogenic bacteria.
The key difference between both forms is that the latter enriches
the energy potential of the gas by transforming the mixture of H2
and CO2 into CH4 , and it is often found in porous media UHS sites
(aquifer and depleted gas reservoir). In addition, underground
H2 methanation can occur at low temperatures due to bacteria,
which is potentially more cost-effective than the current com-
mercial process, which uses high temperatures and expensive
catalyzers (Panfilov et al., 2016). Furthermore, the CO2 proportion
injected is completely converted to CH4 ; thus, UMR resulting gas
is injected into a grid of natural gas and is used as fuel, whereas
syngas or town gas proportions of the various components are
not controlled, and the resulting gas is converted to electricity.
5. Global outlooks and potential sites
Globally, successful H2 storage in underground geological for-
mations is limited to the caverns and aquifers discussed in the
previous section. However, there is yet to be a report in the
literature on 100% pure H2 storage based on the hydrogen storage
forms discussed in the previous section. In particular, a British
company’s salt caverns in Teesside, UK, successfully stored H2
(95% H2 and 3%–4% CO2 ) at a depth of 400 m, whereas Conoco
Phillips’ salt caverns on the US Gulf Coast in Texas, operated by
Conoco Phillips, successfully stored H2 (95% H2 and 3%–4% CO2 )
at a depth of 1000 m. The Kiel town gas project in Germany rep-
resents the salt cavern H2 storage facility that has been recorded,
with a 60% capacity. On the other hand, the aquifer projects cases
reported are Ketzin in Germany, Lobodice in the Czech Republic,
and Beynes in France. The summary of their field project under
different operating conditions is presented in Table 3.
Engineers and scientists have recently become more inter-
ested in exploring the storage and conversion of H2 into a differ-
ent energy form as a result of the ongoing effort for a carbon-free
H2 economy. Most crucially, geological locations become relevant
N.S. Muhammed, B. Haq, D. Al Shehri et al.
Fig. 7. Energy cycle, including the storage of a rich H2 blend with CO and CO2 (Panfilov, 2016).
Table 3
Worldwide successful H2 storage sites (Liebscher et al., 2016; Kruck et al., 2013).
Salt caverns
Field name (s) Country Depth (m)
Teesside UK 400
Clemens USA 1,000
Moss Bluff USA 1,200
Kiel Germany – 32,000
Aquifers
Field name (s) Country Depth (m)
Lobodice Czech Republic 400–500
Beynes France 430
Ketzin Germany 200–250
if they store energy and are located in a favorable area near re-
newable energy generation plants. However, several parameters
must be met to ensure a safe and successful operation before
commencing a storage project. These factors include, but are not
limited to, the type of storage and capacity of the gas stored,
location, in-situ chemical stability, and the process’ overall eco-
nomic evaluation. This is demonstrated as several methodologies
such as technical, environmental, social, and dynamics of the
reservoir including depth, thickness, porosity, permeability, and
brine mineralogy are used for site selection (Table 4).
The investigation has also confirmed that selection criteria
for carbon geo-sequestration and natural gas storage processes
are sometimes used as a template for UHS operations. This is
evident as recent methodologies use algorithms for preliminary
evaluation, characterization, and selection of the geological struc-
ture (Netl, 2010). For instance, Llamas and Cienfuegos (2012)
suggested the use of a multi-criteria framework including tech-
nical (geology, tectonics, hydrogeology, capacity, and CO2 state)
and socioeconomic (quality and quantity of geological data, CO2
sources, location, population density, and environmental aspects)
for decision making purpose. Hsu et al. applied analytical net-
work process (ANP) for CO2 geological selection (Hsu et al.,
2012). Deveci used a fuzzy multi-criteria decision making (Fuzzy
TOPSIS, Fuzzy ELECTRE I, and Fuzzy VIKOR) for the CO2 loca-
tion selection problem in Turkey (Deveci et al., 2015) whereas
Çetin Demirel et al. applied Choquet integral fuzzy-based multi-
criteria decision-making method for natural gas storage site se-
lection (Çetin Demirel et al., 2017). In the H2 context, Iordache
et al. (2019) proposed the use of the additive ratio assessment
(ARAS) method and interval type-2 hesitant fuzzy sets (IT2HFSs)
for UHS selection in Romania. Similarly, Pamucar et al. (2020)
developed a novel hybrid fuzzy neutrosophic numbers-based
decision-making analysis for UHS operation using Romania as a
case study. In Poland, Lewandowska-Śmierzchalska et al. (2018)
proposed an analytical hierarchical process (AHP) framework to
map the entire geological formations for UHS potential based
on weighing factors were they observe that reservoir lithology
(33.2%), stage of exploration (32.1%), type of salt deposit (12.2%),
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Energy Reports 8 (2022) 461–499
Volume (m3 ) Operating conditions H2 (%)
3 × 70,000 each 45 bars 95
580,000 70–137 bars 95
566,000 55–152 bars 95
100 bars 60
Volume (m3 ) Operating conditions H2 (%)
– 90 bars/34 ◦ C 54
3.3 × 108 – 50
– – 62
reservoir volume (10.2%), depth of reservoir (6.3%) and geother-
mal gradient (6%) plays a major role for UHS assessment of the
entire proposed 77 locations by Tarkowski (2017). The author’s
AHP framework found that out of the 77 proposed sites, only
47 met the UHS condition with a total of 11 out 19 for salt
caverns, 14 out of 19 for aquifers, 22 out 39 for depleted oil and
gas reservoirs (Lewandowska-Śmierzchalska et al., 2018). This
therefore shows the active research and drive by researchers in
demystifying various geological formation for UHS to increase the
H2 economy.
6. Hydrodynamics of UHS influencing parameters
Appropriate selection of a feasible and safe storage site cru-
cially depends on the understanding of H2 transport character-
istics in the subsurface. In the previous sections, an overview of
the UHS sites, selection criteria, and other intriguing factors have
been outlined. This section of the review extensively discusses the
underlying physics behind the flow of H2 in porous media and the
hydrodynamics and geomechanics involved in solid (rock), fluid,
and solid–fluid mechanics.
Solid, fluid, and solid–fluid properties are major phenomenon
that governs the simulation, development, and prediction of H2
storage performance as well as the flow behavior in porous
media. However, to achieve this outcome, requisite information
(data) is required. According to the literature survey, the cur-
rent research outlook indicates that the availability of such data
needed to study the flow dynamics of UHS is still in infancy.
Nevertheless, the few available and current data on this aspect
is presented to further deepen the understanding of UHS. The
following factors, as illustrated in Fig. 8 are used to explain the
solid, fluid, and solid–fluid mechanics in UHS.
6.1. Solid parameters
6.1.1. Absolute permeability
Permeability (k) is a measure of the ease with which a porous
medium will transmit fluid, whereas absolute permeability (ka ) is
N.S. Muhammed, B. Haq, D. Al Shehri et al. Energy Reports 8 (2022) 461–499

Table 4
Selected works of literature on the studied criteria for potential global sites for H2 storage.
Salt caverns
Country Region/location Properties Study outlook(s) Reference
Denmark • Lille Thorup • Pressure = 50–100 bar • Potential use of CH4 site for Sorenson (2007)
• Temperature = H2 storage
40–50 ◦ C
• Depth = 1270–1690 m
• Capacity
= 445 × 106 Nm3

Turkey • Tuz Golu gas site • Pressure = 220 bar • Potential use of CH4 site for Ozarslan (2012)
• Depth = 1100–1400 m H2 storage
• Capacity = 12
×630, 000 m3

Turkey • Named A1 by the – • Risk and socio-economic Deveci (2018)

authors characteristics
Canada • Salina A2 unit • Depth = 525 m • Potential use of CH4 site for Lemieux et al. (2019)
• Capacity = 9.5 million H2 storage Mineralogy and
m3 geological criteria’s e.g., depth
• Thickness = 45 m

Canada • Salina B unit • Depth = 400 m • Potential use of CH4 site for Lemieux et al. (2019)
• Capacity = 6.4 million H2 storage Mineralogy
m3 conditions
• Thickness = 90 m

Romania • Ocna Mures – • Location and geology Iordache et al. (2014)

• Targu Ocna • Brine availability and
• Cacica consumption

Germany • Northern Westfalen Capacities • Economics viability of Michalski et al. (2017)

• Northwest • 2.4 billion m3 converting CH4 gas storage to
• Central • 4.6 billion m3 H2 storage
• 1.8 billion m3 • Suitability of location

Poland • Gora – • Lithology and the type of Lewandowska-Śmierzchalska et al. (2018)

salt deposit
• Geothermal gradient
• Exploration stages
• Reservoir depth and volume

Poland • Damaslawek – • Size and depth of the salt Tarkowski and Czapowski (2018)
• Lanieta dome
• Lubien • Structural complexity
• Goleniow • Existing geological reports
• Izbica and salt reserves capacity
• Kujawska • Salt dome recognition
• Debina

Aquifer(s)
Country Region/location Properties Remark Reference
Poland • Chabowo – • Exploration stages Lewandowska-Śmierzchalska et al. (2018)
• Reservoir depth and pore
volume
• Tectonic activity
• Overburden rock lithology

Spain • San Pedro belt • Permeability = 100 • Recovery ratio for seasonal Sainz-Garcia et al. (2017)
mD storage of H2 produced from
• Porosity = 20% wind power

Canada • Mount Simon • Pressure = 76 bar • Analyzed based on the Lemieux et al. (2019)
• Porosity = 15% previous application on Carbon
• Depth = 800 m capture and sequestration
• Capacity (CCS)
= 725 × 106 tons ofCO2

(continued on next page)

the measure of the ease of flow of a single fluid through the reser-
voir rock. It is an intrinsic reservoir rock property (i.e., fluid, and
solid–fluid interactions do not influence ka ) that is independent
of the type of fluid (gas, water, oil) provided the fluid occupies
100% of the conductive pore space. It is a function of pore size
472
distribution only (Pan et al., 2021a; Secchi et al., 2016; Bocquet
and Charlaix, 2010). Darcy’s law presented in Eq. (1) is used to
determine permeability (especially in macropores) under the fol-
lowing conditions – (i) a laminar subsurface flow (non-turbulent),
(ii) no reaction between rock and fluid, and (iii) one phase present
N.S. Muhammed, B. Haq, D. Al Shehri et al. Energy Reports 8 (2022) 461–499

Table 4 (continued).
Depleted reservoirs
Country Region/location Properties Remark Reference
Germany • Schleswig-Holstein • Pressure = 65 bar • Feasibility of H2 storage into Pfeiffer and Bauer (2015)
• Porosity = 13%–33% the proven possible natural gas
• Permeability = reservoir
2.1–572 mD • Storage performance
• Depth = 400–490 m deliverability

Poland • Przemysl – • Overburden rock lithology Lewandowska-Śmierzchalska et al. (2018)

• Tectonic and diagenetic
activity
• Reservoir depth and pore
volume

UK • Midland Valley • Permeability = • Geological uncertainty Heinemann et al. (2018)

2.1–572 mD • Storage capacity
• Thickness =
400–490 m

UK • Rough gas storage • Pressure = 50–100 bar
facility, • Porosity = 20%
• Permeability = 75 mD
• Depth = 2743 m
• Capacity = 48 million
m3
• Chemical stability Amid et al. (2016)
• Biological consumption
• Leakage challenges
• Operational condition

Fig. 8. UHS and its influencing parameters.

at 100% pore space saturation (Afagwu et al., 2021a; Sander et al.,
2017; Eltom et al., 2021).
Q µ∆L
ka =
A∆P
Where Q denotes the volumetric flow rate (liquid/gas), µ is the
fluid viscosity, ∆L is the distance (physical) between the injection
and withdrawal well, A is the cross-sectional area, and ∆P is the
pressure differential.
Fig. ( 9 describes the relationship between ka and effective
stress σeffective which is defined as the difference between the
)
overburden and formation pressures (Zhong et al., 2020; Li et al.,
2014; Chen et al., 2019; Hu et al., 2020). Based on the illustra-
tion from Fig. 9, ka decrease with σeffective during loading cycles
for all the rock sample whereas ka increases again with σeffective
during unloading. Because coal, limestone, and shale are typically
fractured reservoirs, the response of ka to σeffective is very large (Li
et al., 2014; Chen et al., 2019; Hu et al., 2020; Ju et al., 2017;
Zheng et al., 2017). In UHS operations, H2 injection and with-
drawal represent the unloading and loading cycles respectively,
thus, ka increases during H2 injection phase and decreases during
H2 withdrawal phase. Meanwhile, ka response for sandstone and
limestone is larger than shale (Sander et al., 2017), suggesting
(1) that H2 injection in sandstone and limestone reservoirs will be
more energy efficient (Pan et al., 2021a).
The absolute permeability presented in Fig. 9 could be as-
sumed as quantitative and not qualitative as other artifacts such
as slippage effect could influence the transportation of H2 gas.
However, since H2 is considered as a very light gas with a higher
diffusion propensity on the rock wall, therefore, diffusion can
occur even in different pore conditions, and as such quantifying
such effect is essential through studying the dispersion–diffusion
of H2 in saturated reservoir conditions and rock type.
6.1.2. Effective porosity
Porosity (φ ) is the percentage of void space in a rock. Absolute
porosity (φabs ) refers to the ratio of the total pore volume to the
bulk volume, whereas effective porosity (φeffective ) is the ratio of
the interconnected pore volume to the bulk volume (Ma et al.,
2020); thus, it is expected that only the connected end pores
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N.S. Muhammed, B. Haq, D. Al Shehri et al. Energy Reports 8 (2022) 461–499

Fig. 9. Absolute permeability against effective stress.

Source: Data obtained from Zhong et al. (2020), Li
et al. (2014), Chen et al. (2019), Hu et al. (2020) and
Dong et al. (2010).

Fig. 10. Effective porosity against effective stress.

Source: Data obtained from Zhong et al. (2020), Li
et al. (2014), Chen et al. (2019), Hu et al. (2020)
and Dong et al. (2010).

will contribute to H2 flow in UHS. H2 storage capacity (C) at the
reservoir scale is expressed as Eq. (2).
C = L × W × T × (φeffective ) × SH2 (2)
Where L is the formation length, W is the formation width, T is
the formation thickness, and SH2 is the H2 saturation, which is
defined as the ratio of H2 -filled pore volume to total pore volume.
On the other hand, saturation (S) is the proportion of specific fluid
volume in pore space to total pore volume (Pan et al., 2021a).
C is proportional to φeffective as an increase in connected end,
pores will promote storability. φeffective on the other hand, it
is a function of σeffective and lithology (Li et al., 2014; Zheng
et al., 2015) as illustrated in Fig. 10. Because φeffective is larger
in conventional reservoirs (sandstone and limestone) than in un-
conventional reservoirs (coal and shale), the storage capacity will
be significantly increased. This could be ascribed to the measure-
ment techniques for the φeffective . In conventional rocks, φeffective
is measured using a helium pycnometer, while a more complex
method is applied for coal (Zhang et al., 2016b; Ju et al., 2018)
and shales (Arif et al., 2021a) which are both unconventional
474
rocks. As a result, the UHS forecast in unconventional reservoirs
is highly unpredictable. In comparison to ka (refer to Fig. 9),
similar behavior is observed as φeffective decreases with σeffective
during loading cycles whereas it increases with σeffective during
unloading cycles; however, the response of φeffective to σeffective , is
often smaller than the response of ka to σeffective (Hu et al., 2020;
Dong et al., 2010).
6.2. Fluid parameters
6.2.1. Fluid density
Due to geothermal and hydrostatic gradients (Iglauer, 2018),
this component significantly impacts the influence of pressure
and temperature (Pan et al., 2019) on the formation depth in UHS.
The density of H2 (ρH2 ) increases substantially with pressure and
marginally with temperature, as shown in Fig. 11. As an example,
when the pressure climbed from 0.5 MPa to 16 MPa, at 298 K, ρH2
increased from 0.4 kg/m3 to 12 kg/m3 , yet at 20 MPa, when the
temperature increased from 313 K to 373 K, ρH2 decreased from
14 kg/m3 to 11 kg/m3 . At 30 MPa, 40 MPa, and 50 MPa, the same
N.S. Muhammed, B. Haq, D. Al Shehri et al. Energy Reports 8 (2022) 461–499

Fig. 11. H2 density against pressure.

Source: Data obtained from Heine-
mann et al. (2021a), Van Der Gulik
et al. (1988), Michels et al. (1957),
Gracki et al. (1969), Cheng et al.
(2020) and Gonzalez et al. (1967).

Fig. 12. H2 , CH4 , CO2 , and H2 O densities against pressure.

Source: Data obtained from Heinemann et al. (2021a), Van
Der Gulik et al. (1988), Michels et al. (1957), Gracki et al.
(1969), Cheng et al. (2020) and Gonzalez et al. (1967).

trend was found, showing that ρH2 seldom rises with temperature
(as expected).
A similar observation was made when comparing CH4 density
(ρCH4 ), and CO2 density (ρCO2 ) as seen in Fig. 12. ρCH4 increased
from 0.6 kg/m3 to 136 kg/m3 at 323 K with increased pressure
(0.2 MPa to 20 MPa), but ρCO2 increased from 1.5 kg/m3 to
784 kg/m3 . In contrast to ρCH4 and ρCO2 , ρH2 is often relatively low
at elevated pressure values and is less responsive to pressure and
temperature impacts. Furthermore, it is shown that ρH2 is much
smaller than H2 O density (ρH2 O ) under the same thermophysical
conditions. This substantial H2 -brine density difference suggests
that a strong gravity segregation effect (Rossen et al., 2010;
Ide et al., 2007; Han et al., 2016; Rabinovich and Cheng, 2020;
Jamshidnezhad et al., 2010) will be formed during UHS operation,
475
resulting in a greater upward movement of H2 to the caprock than
CH4 and CO2 gases.
6.2.2. Fluid viscosity
Fluid viscosity (µ) is essential in the UHS operation’s injection
and withdrawal stages because it measures the fluid’s flow capac-
ity. When fluid viscosity is combined with relative permeability
that is expressed as a mobility ratio (Muhammed et al., 2020), it
can be used to determine the fluid–fluid interfacial stability and
viscous fingering (Zhang et al., 2011; Wang et al., 2013; Chang
et al., 2019) (see Section 6.3.5). This, however, leads to surface
leakages of gases (CO2 , CH4 , and H2 ) and low injection sweep
efficiency (Carden and Paterson, 1979).
The H2 viscosity (µH2 ) is affected by pressure and temperature,
as seen in Fig. 13. At 10 MPa, for example, a rise in µH2 from
N.S. Muhammed, B. Haq, D. Al Shehri et al.
Fig. 13. H2 , CH4 , CO2 , and H2 O viscosities against pressure.
Source: Data obtained from Heinemann et al. (2021a), Pan
et al. (2019), Van Der Gulik et al. (1988), Michels et al.
(1957), Gracki et al. (1969) and Cheng et al. (2020).
9.6 × 10−3 mPa s to 10.7 × 10−3 mPa s was found when the
temperature increased from 313 K to 373 K (Fig. 13(a)); at 20
MPa, 30 MPa, 40 MPa, and 50 MPa, the same incremental trend
was observed. Furthermore, when pressure was increased from
0.1 MPa to 50 MPa at 373 K, the µH2 increased significantly from
10.4 × 10−3 mPa s to 11.8 × 10−3 mPa s (Heinemann et al., 2021a).
In the case of CH4 viscosity (µCH4 ) and CO2 viscosity (µCO2 )
(Fig. 13(b)), a pressure increase from 0.1 MPa to 48 MPa at 373 K
results in an increase in µCH4 from 13.6 × 10−3 mPa s to 26 × 10−3
mPa s. This implies that µCH4 acts similar to µH2 at low pressure
but behaves more than twice as well at high pressures. On the
other hand, µCO2 increased much more from 15.1 × 10−3 mPa
s to 138.6 × 10−3 mPa s with pressure (0.1 MPa to 50 MPa; at
298 K), showing that µCO2 is ten times greater than µH2 at high
pressures but remains the same at lower pressure. The increase
in viscosity in denser gases is attributed to density properties,
as denser gases have more robust collision and friction between
gas molecules (Pan et al., 2021a; Tu et al., 2017). Furthermore, a
temperature rise reduces viscosity by reducing friction between
gas molecules (Pan et al., 2021a). At the same thermophysical
conditions, water viscosity (µH2 O ) is one to two orders of mag-
nitude larger than µH2 , Fig. 13(c). This also suggests that viscous
fingering is always present during H2 injection in UHS (Homsy,
1987).
6.2.3. Fluid–fluid interfacial tension
The phase boundary between immiscible fluids is determined
by the molecule types on either side of the boundary and the
intermolecular interaction between the molecules. The interfacial
tension (γFF ) between the phases is a critical feature of the phase
boundary, as it measures the amount of energy necessary to
produce more boundary surface. The experimental results for H2 -
H2 O interfacial tension (γH2 –H(2 O ) (Chow
) et al., 2018), and that for
CH4 -H2 O interfacial tension γCH4 –H2 O , and CO2 -H2 O interfacial
tension (γCO2 −H2 O ) (Pan et al., 2020) presented in Fig. 14 clearly
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Energy Reports 8 (2022) 461–499
illustrate that γFF is a function of pressure, temperature, and fluid
composition (Pan et al., 2020; Arif et al., 2016a). The relative
standard deviation (at 0.5 to 45 MPa pressure ranges) of γH2 –H2 O
for each data point reported by Chow et al. (2018) were averaged
(after 3 repeated trials) and was found to be 0.3% with standard
relative uncertainties of 0.8% and an expected combined relative
uncertainty of 95% at a confidence level of 1.7% whereas γCO2 –H2 O
and γCH4 –H2 O cases had a standard deviations of 3 mN/m after
several repetition and averaging (Pan et al., 2020).
Clearly, γH2 –H2 O is rarely affected by pressure since it remains
nearly constant as pressure rises, but it significantly decreased
as the temperature increases. When the pressure was increased
from 0.5 MPa to 45 MPa at 298 K, γH2 –H2 O dropped from 72 mN/m
to 68 mN/m. Again, when the temperature increased from 298
K to 448 K at 20 MPa, γH2 –H2 O decreased from 72 mN/m to 44
mN/m (Chow et al., 2018). For CH4 and CO2 , however, a different
pattern is observed. In the case of CH4 , γCH4 –H2 O declines equally
with pressure and temperature, whereas CO2 in the γCO2 –H2 O
system shows a substantial decrease in pressure and a moderate
increase in temperature (Pan et al., 2020; Arif et al., 2016a).
For example, at 323 K, an increase in pressure from 0.1 MPa
to 20 MPa will result in a decrease in γCH4 –H2 O from 67 mN/m
to 57 mN/m and a decrease in γCO2 –H2 O from 68 mN/m to 24
mN/m, respectively. Furthermore, assuming a constant pressure
(say, 10 MPa), γCH4 –H2 O only fell from 64 mN/m to 62 mN/m while
γCO2 –H2 O rose from 25 mN/m to 35 mN/m when the temperature
increased from 300 K to 353 K.
6.2.4. Solubility
The solubility of H2 in formation brine and other in-situ fluids
is a significant source of H2 loss in UHS, especially given their
low density (0.089 kg/m3 ) under standard conditions. The exper-
imental data in Fig. 15 demonstrates that H2 solubility varies with
pressure, temperature, and salinity. However, the behavior of H2
in an aqueous solution differs from that in a non-aqueous solution
N.S. Muhammed, B. Haq, D. Al Shehri et al. Energy Reports 8 (2022) 461–499

Fig. 14. Gas–water interfacial tension.

Source: Data obtained from Chow et al.
(2018) and Pan et al. (2020).

Fig. 15. H2 solubility at different experimental conditions.

Source: Data obtained from Alvarez et al. (1988) and Chabab
et al. (2020).

due to the varied types of oil compositions as will be discussed At ambient temperatures, H2 solubility in H2 O is much lower
herein. than at UHS temperatures. This is seen in Fig. 15(a), where H2
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N.S. Muhammed, B. Haq, D. Al Shehri et al.
Fig. 16. H2 solubility at different experimental conditions.
Source: Data obtained from Lei et al. (2016).
solubility in H2 O is 8.56 × 10−5 mole fraction at 0.678 MPa and
319 K ambient conditions. As a result, it is best to state that H2
solubility values recorded under ambient conditions are not really
a suitable representation of the reservoir due to the presence of
other fluids and hence cannot be used for UHS operations during
planning. However, H2 solubility at UHS conditions is greatly
influenced by temperature, pressure, and reservoir salinity (see
Fig. 15(a) to (c)). For example, when the pressure was increased
from 3.3 MPa to 23 MPa at 372 K, H2 solubility in 3 mol/kg NaCl
brine increased from 2.15 × 10−5 mole fraction to 1.3 × 10−3
mole fraction, Fig. 15(a); similarly, at 10.1 MPa, H2 solubility in
3 mol/kg NaCl brine increased from 6.32 × 10−4 mole fraction
to 7.03 × 10−4 mole fraction when the temperature increased
from 323 K to 373 K, Fig. 15(b). Furthermore, when the brine
salinity increased from 3 mol/kg to 5 mol/kg, H2 solubility re-
duced slightly from 9.38 × 10−4 mole fraction to 6.62 × 10−4
mole fraction at 15.1 MPa and 323 K, respectively, Fig. 15(c).
The earlier presented H2 solubility deduction is peculiar to
aqueous liquids. In the event of non-aqueous fluids such as hydro-
carbons (Kikic et al., 1980), alcohols (D’Angelo and Francesconi,
2001), white oil (Schofield et al., 1992), heavy oil (Saajanlehto
et al., 2014), diesel (Lei et al., 2016), and other solvents (Zhou
et al., 2006), H2 solubility increases with pressure (Fig. 16(a))
and temperature (Fig. 16(b)) which is qualitatively similar to that
of brine (Chabab et al., 2020). A major observation is that the
solubility of H2 in this fluid type (non-aqueous) is one magnitude
greater than that of the solubility of H2 in aqueous liquids. This,
therefore, begs the need for careful attention on H2 loss due to
dissolution in depleted oil reservoirs than in aqueous reservoirs
during UHS operation.
6.2.5. Diffusivity
Another essential component of UHS is H2 diffusivity (DH2 ),
which is used to calculate the amount of H2 lost. It describes
the amount of H2 gas that diffuses across a rock surface. As
seen in Fig. 17, it is a function of temperature, pressure, and
even fluid type. Clearly, DH2 in hydrocarbon decreased with an
increase in temperature. For example, DH2 in C4 H10 decreased
from 740 × 10−8 m2 /s to 250 × 10−8 m2 /s at 323 K, whereas
DH2 in C4 H10 decreased from 620 × 10−8 m2 /s to 220 × 10−8 m2 /s
at 298 K and the pressure increased from 0.53 MPa to 2.1 MPa
(Fig. 17(a)). A similar trend is also observed for C3 H8 , C2 H6 , and
CH4 gases (Vivian and King, 1964). Furthermore, as the number
of carbon atoms increases, DH2 in hydrocarbons drops. This is
evident as DH2 values for CH4 , C2 H6 , C3 H8 and C4 H10 at 323 K
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Energy Reports 8 (2022) 461–499
and 1.4 MPa were 650 × 10−8 m2 /s, 480 × 10−8 m2 /s, 390 × 10−8
m2 /s, and 350 × 10−8 m2 /s respectively (Vivian and King, 1964).
In the case of Fig. 17(b), DH2 in water increases with tem-
perature and pressure. For example, when the temperature was
increased from 650 K to 970 K, DH2 increased from 15.1 × 10−8
m2 /s to 219 × 10−8 m2 /s at 25 MPa (Zhao and Jin, 2019). Some
authors suggest that this is due to the effect of temperature
on molecular momentum, Brownian motion, and intermolecular
forces, which influence diffusivity (Bird, 2002). This data set leads
to the conclusion that during UHS, H2 loss by diffusion is more
important in aquifers than in hydrocarbon depleted reservoirs
because diffusivity is promoted more in the presence of water
than hydrocarbon.
6.3. Solid–fluid parameters
6.3.1. Wettability
In a three-phase system comprising of the rock matrix, the
non-aqueous (oleic) phase, as well as the aqueous (brine) phase,
the rock surface wettability is generally defined in terms of the
hydrophobicity or the aqueous phase hydrophilicity, and the in-
clination of the phase to spread on or adhere to the rock sur-
face (Yekeen et al., 2020). The wetting phase can be oil, wa-
ter (brine), or gas while the solid face is always the reservoir
rock (Yekeen et al., 2020). This phenomenon is governed by the
dynamic intermolecular force’s interaction effects (Yekeen et al.,
2020; Arif et al., 2019) that are determined between the cohesive
and adhesive forces of the different fluid phases (Yekeen et al.,
2020). In oil/gas-wet formation, the rock prefers oil/gas over
water because a substantial amount of oil/gas attaches to the rock
surface and forms residual oil/gas after water flooding, whereas
in a water-wet formation, the rock prefers water over oil/gas,
so oil/gas occupies the center of pores and pore throats (Deng
et al., 2020, 2021). Wettability plays a major role in geomaterials
(i.e., rock and minerals) and a different range of methods exist for
their characterization. This range of methods, however, depends
on the basis used for the classification as it can be grouped into
conventional and moderns (Yekeen et al., 2020), direct or indi-
rect, and quantitative or qualitative assessment methods (Yekeen
et al., 2020; Arif et al., 2019) as shown in Table 5. Compre-
hensive insights on wettability (although for rock/CO2 /brine and
rock/oil/CO2 -enriched brine systems) can be found in Yekeen
et al. (2020) and Arif et al. (2019) whereas a description of
each method in terms of advantages and limitations is presented
elsewhere (Arif et al., 2019; Iglauer et al., 2015).
N.S. Muhammed, B. Haq, D. Al Shehri et al.
Fig. 17. H2 diffusivity for (a) different hydrocarbon and (b) water.
Source: Data obtained from Vivian and King (1964) and Zhao and
Jin (2019).
Table 5
Wettability measurement classification.
Source: Modified after Arif et al. (2019).
Direct-quantitative assessment Indirect-qualitative assessment
Amott and Amott-Harvey index Wilhelmy balance method
(used in ambient condition)
U.S. Bureau of Mines; USBM Capillary rise method
(used in ambient condition)
Contact angle methods Spontaneous imbibition method
(Experimental/theoretical)
• Sessile drop Capillary pressure
• Captive bubble Relative Permeability
• 2D-micromodels Nuclear magnetic resonance (NMR)
• 3D-Micro CT (µ-CT) imaging
• Molecular dynamics (Indirect
but quantitative)
The attention of the reader is drawn towards the contact angle
(direct and quantitative) assessment method as it is the most
suitable method when pure fluids and clean cores/minerals are
used. Additionally, it can provide relatively rapid measurement
for a wide range of spectrum of operating conditions (pressure,
temperature, salinity, surface roughness, and rock surface chem-
istry) (Arif et al., 2021b). It also remains the most generally
accepted technique due to its reliability, simplicity, and versatil-
ity (Yekeen et al., 2020). However, care must be exercised dur-
ing contact angle measurements as the surface cleaning method
and surface contamination may lead to a significant bias in the
outcome. It has been reported that the presence of a minute
clay (e.g., kaolinite) in sandstone could alter the entire surface
charge (Arif et al., 2017; Kaveh et al., 2014) thereby influencing
the wettability of the sample. On this note, wettability is defined
as a fluid’s tendency to adhere to a solid (rock) surface in the
presence of other immiscible (or partially miscible) fluids and
is determined at the pore scale by the local contact angle (the
angle formed by the interface between two fluid phases with
the solid, usually measured through the denser phase) (Iglauer,
2017; Andrew et al., 2014). Wettability alteration has been largely
attributed to changes in the pore system (adsorption), which
may be due to rock–fluid interaction, fluid–fluid interactions, rock
mineralogy, and brine chemistry (Mohammed et al., 2021a,b).
Due to a variety of mineral compositions, rock surface chemistry,
and pore geometry, H2 rock wettability is distributed hetero-
geneously in the pore network of the storage rock (Scanziani
et al., 2017; Singh et al., 2016; AlRatrout et al., 2017). It is
also important for estimating storage capacity (C), H2 saturation
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Energy Reports 8 (2022) 461–499
Table 6
Rock wettability and contact angles (Iglauer et al., 2015).
Contact angle (o ) Wettability behavior
0 to 50 Strongly water wet
50 to 70 Weakly water-wet
70 to 100 Intermediate water-wet
110 to 130 Weakly oil/gas-wet
130 to 180 Strongly oil/gas-wet
(SH2 ), injectivity and withdrawal rates, and containment secu-
rity (Iglauer, 2018; Arif et al., 2016a; Øren and Bakke, 2003;
Al-Khdheeawi et al., 2018; Iglauer et al., 2015b; Al-Khdheeawi
et al., 2017). Additionally, if the wettability (contact angle) for a
given rock type is known, it can be used to perform pore-scale
modeling (micro-scale) to estimate upscaled capillary pressure
(Pc) and relative permeability (Kr ) curves (Hashemi et al., 2021a)
which can be used as input parameters for reservoir scale simu-
lations (Kunz et al., 2018; Blunt, 2017). Table 6 is a systematic
representation of the different wettability alteration behaviors
based on the contact angle ranges.
The most common experimental configurations for contact
angle measurement in the oil and gas industry for introducing
the drop of fluid on the rock substrate (depending on the drop
liquid density and the surrounding liquid phase) are sessile drop
and captive bubble. This measurement from the contact line of
the fluid–fluid interface with the rock surface is often achieved
through classic equipment such as drop shape analyzer (DSA)
and axisymmetric drop shape analyzer (ADSA). This measurement
method is usually modified as tilted plate techniques to deter-
mine both the advancing (θ a) and receding (θ r) contact angles. It
is vital to state here that in the UHS process, water receding angle
(gas advancing) is the drainage angle corresponding to water
being displaced by gas (H2 injection into the subsurface), while
water advancing angle (gas receding) is the imbibition angle
corresponding to water displacing gas (H2 withdrawal from the
subsurface) (Iglauer et al., 2021; Broseta et al., 2012).
Numerous experimental articles on contact angles measure-
ment for systems containing rock/brine/CO2 have been reported
as discussed in the reviews by Yekeen et al. (2020) and Arif et al.
(2019). However, few research articles highlight wettability data
for a rock/brine/H2 system for UHS. The major observation from
Table 7 shows that more attention has been paid to the tilted
plate sessile dynamic contact angles method whereas only one
study (as of the time of this review) conducted a static (intrinsic)
captive bubble contact angle measurement for UHS (Hashemi
N.S. Muhammed, B. Haq, D. Al Shehri et al. Energy Reports 8 (2022) 461–499

Table 7
Recent works of literature on contact angle measurement for rock/brine/H2 systems.
Substrate Fluids Gases Methods Surface roughness P & T conditions Remarks Wettability Refs.
Kaolinite, Illite and Brine, 20 wt % H2 , CO2 , Ar, N2, Tilted plate Nil 5 to 20 MPa, 333K θ a (dynamic) Strongly water-wet Al-Yaseri et al.
Montmorillonite NaCl and 1 wt % and He. increases with P (2021)
clays. KCl for all clays
Basaltic rock Brine of 2.2 M H2 , CO2 , N2, and Tilted plate RMS = 210 nm 5 to 20 MPa, 323K θ a (dynamic) Strongly water-wet Al-Yaseri and Jha
ionic strength He. increases with P (2021)
Berea and Brine with NaCl H2 Captive-Bubble Pa = 0.030 mm 2 to 10 MPa, θ (intrinsic/static) Water-wet Hashemi et al.
Bentheimer and synthetic sea Bentheimer, 293–323 K was not affected (2021b)
sandstone water Pa = 0.025 mm by P & T
Berea
Quartz and aged Brine, 10 wt% NaCl H2 Tilted plate RMS = 1–2 nm 0.1–25 MPa, θ (dynamic) Water-wet to Iglauer et al.
Quartz, in acid (before aging) 296–343 K increases with P & intermediate-wet (2021)
RMS = T
160–330 nm (after
aging)
Quartz and aged Brine, 10 wt% NaCl H2 Tilted plate RMS = 1–2 nm 0.1–25 MPa, 323 K θ (dynamic) Strongly water-wet Ali et al. (2021b)
Quartz, in acid (before aging) increases with P to intermediate-wet
RMS =
160–330 nm (after
aging)
Mica and aged Brine, 10 wt% NaCl H2 Tilted plate RMS = 1 nm 0.1–25 MPa, θ (dynamic) both Weakly-water wet Ali et al. (2021a)
Mica, in acid 308–343 K increased/decreased to intermediate-wet
with P & T based
on the acid
concentrations

a Young’s equation (see Eq. (3)) was used to determine (θ ) after measuring θ and θ contact angles.
a r

et al., 2021b). This could be attributed to the effect of image
processing as spreading and diffusion of the brine into the porous
hydrophilic substrate may be challenging when using sessile
drops (Hashemi et al., 2021b; Prydatko et al., 2018). The only
contact angle measurement via 3D µ-CT is that by Jha et al.
(2021) where a pore-scale investigation on sandstone substrate
was reported.
The data presented in Fig. 18 represent the works of Ali et al.
(2021a), Al-Yaseri and Jha (2021), Iglauer et al. (2021) and Al-
Yaseri et al. (2021). As seen in Al-Yaseri et al. (2021) and Al-Yaseri
and Jha (2021), at approximately similar experimental conditions
(pressure and temperature) the rock/brine/H2 wettability on clay
minerals (kaolinite, illite, and montmorillonite) and basaltic rock
calculated via the Young’s equation, increased with pressure at a
constant temperature. The overall wetting states of the clay/rock
minerals indicate strongly water-wet as the θl is below 40◦ .
Specifically, at 5 MPa and 333 K, the calculated θl for kaolinite, il-
lite and montmorillonite were 13.4◦ , 16.3◦ and 19.8◦ respectively.
The same trend is also observed for other pressure conditions
(10 MPa, 15 MPa, and 20 MPa) in terms of increasing contact
angles with respect to the clay minerals. Based on the nature of
the clay minerals, montmorillonite exhibited higher contact angle
than illite while kaolinite showed lowest implying that, kaolinite
(a 1:1) clay mineral is the most water wet. However, Basaltic
rocks measurement in the work of Al-Yaseri and Jha (2021) at
5 MPa and 323 K was 9.88◦ as compared to the other injected
gas (i.e., CO2 , N2 , and He). While all minerals exhibited a strongly
water-wet state, it can be suggested that in the presence of H2 ,
residual and capillary trapping in their pores will be high under
their storage condition, and as such, high containment security
can be achieved in such formation for an extended period of H2
injection (Al-Yaseri and Jha, 2021; Al-Yaseri et al., 2021).
In Iglauer’s work, Iglauer et al. (2021) on Pristine quartz, both
θ a and θ r increased with pressure and temperature. Specifically,
when the pressure increased from 5 MPa to 25 MPa at 296 K, θ
a increased from 7.5◦ to 28.8◦ whereas θ r increased from 6.1◦
to 24.6◦ . Similarly, at 343 K when the pressure increased from 5
MPa to 25 MPa, θ a again increased from 27.2◦ to 48.3◦ while θ r
increased from 24.4◦ to 44.1◦ respectively. A general observation
is a fact that all measured contact angles had greater values than
those for clay and basaltic rocks except at 296 K and 323 k. This
thus indicates that clay and basaltic can be used a barriers to
improve storage security. Ali et al. (2021a) also observed similar
behavior in terms of increase in θ a and θ r with pressure (for
mica substrates), however, an opposite observation with tem-
perature is recorded as θ a and θ r increased with decrease in
480
temperature. For instance, when the pressure increased from 5
MPa to 20 MPa, at 308 K, θ a and θ r simultaneously increased
from 30.8◦ to 64.6◦ and 26.1◦ to 58.4◦ respectively, whereas, at
constant pressure (i.e., 20 MPa), θ a increased from 39.6◦ to 64.6◦
while θ r increased from 34.1◦ to 58.4◦ when the temperature
decreased from 343 K to 308 K. The only experimental work
which neither increased with pressure, temperature and salinity
is that by Hashemi et al. (2021b) where static contact angle (θ s)
was measured. Though averagely, all the repeated experimental
θ s in the presence and absence of brine were different (for both
Berea and Bentheimer sandstone), they, however, fall within the
same value range of 21.1◦ to 43◦ , as such, no meaningful correla-
tion between parameters was established. The non-conformance,
however, was attributed to the measurement method, sample
preparation, and experimental conditions.
The effect of acid concentration categorically is presented in
the works of Ali et al. (2021a,b) and Iglauer et al. (2021). A
general trend is the fact that acid concentration plays a major role
in mimicking the reservoir condition thus, wettability alteration
could be affected depending on the type of rock samples and
the reservoir conditions. In the case of Iglauer et al. (2021) and
Ali et al. (2021b) who used the same experimental conditions,
an approximately similar wettability outcome was noticed as
presented in Table 7. Specifically, Iglauers’s (Iglauer et al., 2021)
works indicate that H2 wettability of pure and aged stearic acid
quartz surface changes from strongly water-wet to intermediate
water wet under different acid conditions and increased thermo-
physical conditions. This study was later confirmed by Ali et al.
(2021b) using a representative and realistic geological scenario
where a mixture of organic acid exists in the reservoir. The
overall outcome shows that the pristine rock sample which was
inherently water wet turned intermediate water-wet when the
substrate was aged in an organic acid having a longer alkyl chain.
Further studies conducted by Ali et al. (2021a) on mica substrate
confirm that rock sample and acid concentration also affect wet-
tability where it was reported that mica tends to become weakly
water-wet at higher temperatures, lower pressures, and very low
stearic acid concentration. Though, it turned intermediate-wet at
higher pressures, lower temperatures, and increasing stearic acid
concentrations suggesting that the structural H2 trapping capac-
ities in geological formations and sealing potentials of caprock
highly depend on the specific thermo-physical condition (Ali
et al., 2021a).
Contact angle measurement as seen in the study is scarce, and
the only direct and quantitative 3D µ-CT study is that by Jha
et al. (2021). The overall H2 and brine saturation at slow injec-
tion rate (0.01 ml/min, equivalent to 5 PV) were approximately
N.S. Muhammed, B. Haq, D. Al Shehri et al.
Fig. 18. Experimental data for rock/brine/H2 at different conditions.
Source: Data obtained from Ali et al. (2021a), Al-Yaseri and Jha
(2021), Iglauer et al. (2021) and Al-Yaseri et al. (2021).
65% and 35% of the rock’s pore volume, respectively. As seen in
Fig. 19, H2 gas location after injection is predominantly occupied
in the larger pores whereas brine remains in the smaller pore,
pore throats, and corners points of the block after injection. This
behavior according to the authors indicates a capillary-dominated
flow (Singh et al., 2019). Additionally, Fig. 19 also proves the in-
herent wetting state of a sandstone core in the presence of H2 gas
as it can be seen at the curvature of the grain meniscus that, sand-
stone is vehemently water wet. Other information that can be
deduced from the 2D segmented image is the difference between
the brine phases at initial and residual H2 saturations. Approx-
imately 41% H2 saturation was observed after brine flooding
indicating that the residual saturation of H2 remained signifi-
cantly high in the sandstone pores thus, this medium can be used
for potential long-term storage.
As a conclusion, Table 7 shows a general agreement on the
influence of pressure when tilted plate techniques are used for
dynamic contact angle measurement (in sandstones, clays, and
even basaltic rock type) as compared to captive bubble which
reported a static contact angle for sandstones (Benthaimer and
Berea). However, other factors are believed to influence the ef-
fect of wettability including temperature and formation brine.
Besides, experimental artifacts such as surface cleaning process,
fluid equilibration, and surface contamination cannot be over-
looked (Arif et al., 2019). Another influencing factor that is in-
trinsic to the rock property is the surface roughness which can
be measured via Atomic Force Microscopy (AFM) that is evaluated
experimentally, either in root mean square (RMS) roughness (Ali
et al., 2021a), Pa factor — defined as the arithmetic mean of the
absolute ordinate height values with a sampling length (Hashemi
et al., 2021b), and roughness ratio rs, which is the ratio of the
total surface area to a flat projection of that surface (Tudek et al.,
2017).
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Energy Reports 8 (2022) 461–499
6.3.2. Solid–fluid interfacial tension
solid–fluid interfacial tension (γSF ) is a vital component that
influences the distribution and migration of H2 in the subsur-
face (Arif et al., 2016b; Pan et al., 2021b). Theoretically, Young–
Laplace equation; Eq. (3) is used to represent the relationship
between rock (solid) wettability (contact angle measurements)
and solid–fluid interfacial tension (γSF ). It is a function of the
interplay of the three interfacial tensions (rock/H2 , rock/brine and
brine/H2 ) as expressed by Young’s equation (Arif et al., 2016b).
γrock−H2 − γrock−H2 O
cos θ = (3)
γH2 −H2 O
Where γrock−H2 , γrock−H2 O , and γH2 −H2 O denote solid/H2 , solid/water,
and H2 /water interfacial tensions, respectively. To assess the
wettability dependence on the interfacial interactions, the quan-
tification of γSF is obtained via semi-empirical methods due to
the absence of experimental techniques to reliably measure the
parameter (Pan et al., 2020; Arif et al., 2016b; Pan et al., 2021b).
Presently, the work by Pan et al. (2021b) on ‘‘Rock–fluid inter-
facial tension at subsurface conditions: Implications for H2 , CO2 ,
and natural gas geo-storage’’ so far is the only reported literature
that discusses the rock–fluid interfacial tension for H2 .
The rock–gas interfacial tension is a function of pressure,
temperature, and acid content, as shown in Fig. 20. According to
the experimental results, the rock-H2 IFT (γrock−H2 ), rock-CO2 IFT
(γrock−CO2 ), and rock-CH4 IFT (γrock−CH4 ), dropped with pressure
and temperature for cleaned quartz Fig. 20(a)), and the γrock−H2
and γrock−CO2 reduced similarly for basaltic rock Fig. 20(b)). For
γrock−H2 , the clean quartz IFT dropped by 11 mN/m (from 102
mN/m to 91 mN/m) at 323 K when the pressure increased from
5 MPa to 25 MPa, but it reduced by 9 mN/m (from 92 mN/m to
83 mN/m) at 20 MPa when the temperature increased from 323
K to 343 K. Similar trend for both pressure and temperature is
observed for that of γrock−CO2 , and γrock−CH4 for clean quartz as
well as γrock−H2 , and γrock−CO2 for basaltic rock (Pan et al., 2021b).
The aforementioned behavior is mostly due to the gas type
because any rise in pressure and reduction in temperature for a
N.S. Muhammed, B. Haq, D. Al Shehri et al. Energy Reports 8 (2022) 461–499

Fig. 19. H2 and brine phases at (a) initial H2 saturation, and (b) residual H2 saturation (Jha et al., 2021). (For interpretation of color in this figure legend, the reader
is referred to the web version of this article).

Fig. 20. Rock–gas IFT for (a) clean quartz and (b) basaltic rock, against pressure; and (c) aged quartz gas-IFT against concentration, at 323 K.
Source: Data obtained from Pan et al. (2021b).

specific gas type would result in a general increase in gas density
and rock intermolecular forces (Pan et al., 2019; Al-Yaseri et al.,
2016), thus, lowering the γrock–gas correspondingly (Pan et al.,
2020). The gas density follows the order H2 < CH4 < CO2 for a
variety of gas types under the same thermophysical conditions. As
a result, the order of γrock–gas will be γrock−H2 > γrock−CH4 > γrock−CO2
correspondingly. This sequence is consistent, and it also supports
the findings of Abdulelah et al. (2021).
482
At constant pressure and temperature, γrock−H2 and γrock−CO2
decreases with the increase in stearic acid concentration, as seen
in Fig. 20(c). For example, at 323 K and 25 MPa, the γrock−H2
dropped from 85 mN/m to 72 mN/m, while the γrock−CO2 de-
creased from 16 mN/m to 10 mN/m when the acid concentration
increased from 1 × 10−9 mol/L to 1 × 10−2 mol/L. Because pristine
quartz, as stated by Pan et al. (2021a) and Iglauer et al. (2021),
does not exist in the reservoir, stearic acid aged quartz H2 IFT is
N.S. Muhammed, B. Haq, D. Al Shehri et al.
Fig. 21. Capillary pressure for the H2 /CO2 water sandstone systems.
Source: Data obtained from Abdoulghafour et al. (2020), Pini et al.
(2012) and Yekta et al. (2018a).
recommended for determining the link between rock and fluid
wettability in UHS operations (Ali et al., 2021b).
6.3.3. Capillary pressure
The pressure between two immiscible fluids in a thin tube, re-
sulting from the interactions of forces between the fluids and the
tube’s solid walls (see Eq. (4)), is known as capillary pressure (Pc).
It is a key aspect in the study of multiphase fluid flow in porous
media, and its capillary forces are frequently the determining
factor (Iglauer, 2017).
2γ cos θ
Pc = (4)
r phase (since θa will be far greater than 100◦ , see Fig. 22). As an
Where Pc , γ , θ , and r denote the capillary pressure, IFT, contact
angle, and radius of the largest pore respectively.
Pc is usually combined with relative permeability curves (both
as a function of water saturation) to evaluate fluid movement,
pore-scale fluid configurations, and the general flow geome-
try (Al-Khdheeawi et al., 2018; Luboń and Tarkowski, 2020).
During H2 injection in porous media, the brine originally present
in the aquifer or hydrocarbon reservoir formation is replaced by
H2 . As a result, the H2 moves to the reservoir top and remains at
the caprock (seal) because of the effect of gravity segregation (Zi-
var et al., 2021). The pressure required to displace this brine is
the Pc, and thus it is more favorable in UHS operation to have a
high H2 saturation (SH2 ) or low water saturation (Sw ) which will
result into a larger storage capacity in the rock pores.
Capillary pressure against water saturation experimental data
for CO2 -water sandstone systems have been reported in the lit-
erature (Abdoulghafour et al., 2020; Pini et al., 2012), however,
only the work by Yekta et al. (2018a) illustrated the data set for
the H2 -water sandstone system. For comparison purposes, both
CO2 and H2 data are plotted in Fig. 21 where it can be seen that
both the effect of pressure and temperature were insignificant for
the H2 -water system because both data set almost overlapped.
Specifically, Sw increased from 17% to 32% when Pc decreased
from 110 KPa to 61 KPa at 5.5 MPa and 293 K, but Sw increased
from 19% to 42% (at 10 MPa and 318 K) when Pc decreased from
81 KPa to 51 KPa. However, Pc for CO2 -water systems at different
UHS conditions for pressure and temperatures (9 MP, 298 K; 9
MPa, 323 K; and 10 MPa, 323 K) had significant influence.
To determine the surface tension and contact angle for the
H2 -water sandstone system for the entire water saturation range,
the authors combined (through fitting) both capillary pressure
483
Energy Reports 8 (2022) 461–499
Fig. 22. Relationship between receding θr and advancing θa contact angles as
a function of intrinsic θi contact angle (Hashemi et al., 2021a). *Denotes the
θr = 12o and θa = 85o benchmark data by Hashemi et al..
data obtained via modified semi-dynamic technique with mer-
cury injection measurement and thereafter, surface tension and
contact angle of 51 mN/m and 21.56◦ (at 5.5 MPa, 20 ◦ C shallow
condition) and 46 mN/m and 34.9◦ (at 10 MPa, 45 ◦ C, deeper
condition) respectively were determined for both potential UHS
scenarios (Yekta et al., 2018a). However, while the core flood
has been performed at primary drainage condition (i.e., initial
H2 injection), the obtained water receding contact angles (θr =
21.5o for shallow, and θr = 34.9o for deep) when evaluated on
the modified Morrow curve to get the representative advancing
angles does not fully represent the case of H2 as the non-wetting
extension, after tracing the modified Morrow hysteresis curve by
Hashemi et al. (2021a), it was found that, once θr is ∼≥ 12o ,
the corresponding advancing angle will always be greater than 90
(i.e., θa > 90o ) which is very unlikely to be realistic (for primary
drainage condition) as the rock sample is still considered as H2 -
wet. Therefore, to fully achieve a non-wetting state (which was
intended by the primary drainage study of Yekta et al., 2018a),
θa was set to 85o using the same experimental data and the pore
network model result indicate a consistent trend with the exper-
imental study of Yekta et al. (2018a) for both shallow and deep
reservoir conditions implying that further pore-scale modeling
can be performed to quantify the crucial reservoir-scale functions
of Pc and Kr and their dependencies on fluid and reservoir rock
conditions.
After benchmarking with the experimental data, Hashemi
et al. further conducted a rigorous sensitivity analysis to study the
hysteresis behavior appropriately during primary drainage (initial
H2 injection), secondary imbibition (H2 withdrawal), and sec-
ondary drainage (H2 re-injection), for cyclic H2 transport (Hashemi
et al., 2021a). Additionally, the impact of fluid and rock properties
on the upscaled functions was analyzed. Results indicated that
while maintaining the brine as the wetting phase and H2 as the
non-wetting phase, both Pc and Kr were observed to be sensitive
to wettability changes (i.e., contact angle). Also, they noted that
the amount of trapped H2 in the grid blocks largely depends
on rock characteristics and wettability (contact angle) and is
independent of the number of cycles. The overall study highlights
that if the contact angle for a particular rock sample is known, it
can be used to perform pore-scale modeling to obtain upscaled Pc
and Kr curves which are vital because they can be used as input
for reservoir scale in a multiphase flow study. Clearly, the work
N.S. Muhammed, B. Haq, D. Al Shehri et al. Energy Reports 8 (2022) 461–499

by Hashemi et al. (2021a) confirms that the contact angle in the

cyclic storage transport system in UHS is hysteric.
Several physical effects also occur during gas injection in the
subsurface such as fingering (contrast in mobilities), and gravity
override (density differences between the two fluids), and solu-
bility and dissolution. These effects are most common when gas
is injected into formations that are strongly water-wet, weakly
water-wet, or intermediately water-wet, where the formation
brine spontaneously imbibes the rock and displaces the injected
gas (Hu et al., 2018). This process breaks the H2 plume during
propagation into a discontinuous clustered H2 phase and the
associated capillary fingering effect increases the storage capac-
ity for H2 (Iglauer and Wülling, 2016; Tanino and Blunt, 2013).
This principle of capillary entrapment (where sequestered CO2
is trapped at the pore scale by capillary forces as a residual
phase) is a significant storage mechanism in CGS (Kalam et al.,
2020; Akbarabadi and Piri, 2013). Usually, the buoyant gases
(e.g., CH4 , CO2 , H2 ) are stored by an impermeable seal layer
Fig. 23. Relative permeability for the H2 water system.
termed caprock (Busch et al., 2008; Wollenweber et al., 2010)
Source: Data obtained from Yekta et al. (2018a).
which are generally porous with a very low permeability (Song
and Zhang, 2013). As a result, the capillary entry pressure in
addition to the very small pores in the caprock reduces the ability
of the buoyant gas to percolate thus high storage capacity is 6.3.4. Relative permeability
achieved. Relative permeability (kr ) is the ratio of the effective perme-
However, UHS operations require multiple injection and with- ability (ke ) to the base permeability (kbase ). As a point of note, ke is
drawal cycles depending on the demand (Tarkowski, 2019), as a the permeability of one fluid in a multi-fluid system, i.e., perme-
result, the trapped residual H2 saturation must be minimized to ability to a fluid when its saturation is less than 100%, whereas
address the splitting of the H2 plume so that larger H2 clusters depending on the system, kbase could be (i) absolute permeability,
can be re-mobilized more easily during H2 withdrawal (Tanino (ii) effective permeability of one of the phases at irreducible water
and Blunt, 2013; Herring et al., 2016). To address this, the buoy- saturation, (Swir ), or (iii) dry air absolute permeability at atmo-
ancy pressure (PB ) therefore must be greater than the entry spheric pressure. kr is a vital parameter in reservoir pore space
capillary pressure (Pce ) to overcome the counter acting capillary calculation in the multiphase flow of fluids. It is also a function
forces (Iglauer et al., 2015b). For instance, assuming both the
of pore size distribution, wettability, and saturation (Burnside and
formation brine and H2 exist as a continuous phase, the PB can
Naylor, 2014; Juanes et al., 2006; Ruprecht et al., 2014; Krevor
be expressed as Eq. (5).
et al., 2012).
PB = ρbrine − ρH2 gh = ∆ρ gh
( )
(5) Information on kr for the H2 -water system is still lacking in the
open literature. However, the study by Yekta et al. using steady-
Where ∆ρ = ρbrine − ρH2 , whereas ρbrine , ρH2 , g, and h repre-
state core flooding experiments for a sandstone core (porosity
sent brine density, H2 density, the gravitational constant, and H2
column height which is permanently immobilized beneath the — 19.5% and permeability — 44 mD) provided insight on H2
caprock respectively. Eq. (4) is modified to Eq. (6) assuming the behavior during UHS. Clearly, Fig. 23 shows that at 293 K and
rock pore network is a perfect cylinder with a cross-sectional 5.5 MPa, relative permeability for H2 (kr −H2 ) increased from 0
area, as: to 0.04 when Sw decreased from 90% to 40%: whereas at 318 K
and 10 MPa UHS conditions, kr −H2 again increased from 0 to 0.03
2γ(H2 −brine) cos θ
P ce = (6) when Sw decreased from 81% to 40%. It was concluded that the
r low kr −H2 obtained reflects on the pore capacity for H2 to flow
Where γ(H2 −brine) is the IFT between H2 and the formation brine. in a sandstone. This effect was attributed to the heterogeneity of
At equilibrium, both the capillary pressure and buoyancy pres- the sandstone used for the experiment (Yekta et al., 2018a).
sure become equal (Iglauer, 2017), thus the maximum column Out of the influencing properties (Pc, kr , θ , and γ ) used to
height can be determined as expressed in Eq. (7). access fluid–fluid and rock–fluid interactions in a UHS, the effect
2γ(H2 −brine) cos θ of kr and Pc is the two major sources that affect storage efficiency
hmax = (7)
r ρbrine − ρH2 g through the increase in H2 loss (Zivar et al., 2021). As for the kr , it
( )
can behave as a function of saturation depending on the history
In a recent study, it was documented that hmax varies with storage of the system. This process: also known as hysterics is observed
depth as other factors (γ , θ , and ∆ρ ) significantly vary with depth during drainage operation where a non-wetting phase (e.g., H2 ) is
in CGS conditions (Iglauer, 2018). However, a lower depth barrier
injected to increase the gas saturation in the reservoir. Afterward,
exists below which CO2 cannot be stored permanently through
an imbibition process is accompanied by the withdrawal of gas to
structural trapping because, at approximately 15,000 m depth,
reduce the gas saturation. Each of these processes (drainage and
density reversal occurs, and since CO2 is heavier than brine, it
imbibition) has a different trapping system for H2 thus accounts
spontaneously sinks deep into the reservoir due to gravitational
forces (Span and Wagner, 1996). Based on this hypothesis, the for the difference in the kr , curves. The same principle applies
maximum storage depth for H2 in UHS settings was investi- to Pc during fluid flow in the porous media as it shows the
gated (Iglauer, 2021). It was found that an optimum storage depth different behaviors of drainage and imbibition during a storage
for H2 exists at a depth of 1100 m, at which a maximum of operation. Pc controls the fluid distribution in the pore space and
H2 can be stored. Though, H2 will always be buoyant due to its since it is path-dependent (Raeesi et al., 2014), different cycles
high volatility in a geologic reservoir (Leachman et al., 2009). or loops (hysteresis) are observed for the drainage (H2 injection)
These experimental investigations confirm that besides CO2 , Pc and imbibition (H2 withdrawal). An example of such hysteresis
can be applied to determine structural trapping for H2 and thus is presented in Fig. 24, and for detail insight, refer to Hashemi
containment security and storage capacity. et al.’s (2021a) work discussed in the previous section.
484
N.S. Muhammed, B. Haq, D. Al Shehri et al.
Fig. 24. Capillary pressure hysteresis for H2 -water system.
Source: Adapted and redrawn from Carden and Paterson
(1979).
6.3.5. Mobility ratio
Mobility ratio (M) is defined as the unstable displacement of
a more viscous fluid by a less viscous fluid (Muhammed et al.,
2020; Hagemann, 2018; Massarweh and Abushaikha, 2021). It can
also represent the product of ka and kr divided by fluid viscosity
(µ) (Pan et al., 2021a). The displacing fluid (less viscous) is the
H2 in this case whereas the displaced fluid (more viscous) is the
water. This phenomenon is evaluated using the mobility ratio as
represented in Eq. (9).
( )
ka ×kr1
µ1
M= ( ) (8)
ka ×kr2
µ2
kr1 µ2
M=
kr2 µ1
where kr1 is the relative permeability of the displacing fluid
at the average saturation behind the displacement front, kr2 is
the relative permeability of the displaced fluid at the average
saturation ahead of the displacement front and µ1 and µ2 are
the respective viscosities for the displacing and displaced fluid.
In general, it is accepted that mobility ratios <1 result in a stable
displacement, whereas mobility ratios >1 become unstable, and
viscous fingering occurs in the displacement front (Hagemann,
2018). This will result in low H2 sweep efficiency and inefficient
displacement of formation brine (Berg and Ott, 2012).
Paterson performed an experimental study to investigate the
effect of H2 fingering. The outcome showed that fingering could
result in huge H2 loss. The major contributing factor is the rate of
gas injection because of the early breakthrough and high mobility
associated with the gas (Paterson, 1983). The H2 loss due to
injection rate is significant as it affects the stability of the fluid
front. An unstable front is created by a higher injection rate,
which eventually affects the boundary between the pre-existing
fluid and H2 . To characterize this parameter (injection rate), a
capillary number (Nc) equation is employed. This equation is a di-
mensionless group widely used to evaluate the efficiency of fluid
displacement in porous media. It is defined as the ratio between
viscous and capillary forces as shown in Eq. (10) (Khosravi et al.,
2014; Rezk et al., 2019; Zivar and Pourafshary, 2019).
ϑµ
Nc =
σ chemical reactions (Pan et al., 2021a).
Where Nc , ϑ , µ, and σ represent the capillary number, Darcy’s
velocity, the viscosity of the displacing fluid, and the IFT, respec-
tively. As an illustration, a comparison between the H2 and CH4
Energy Reports 8 (2022) 461–499
water systems is presented by studying the viscous and capillary
forces. If a constant Darcy velocity (injection rate) is assumed, less
sweep efficiency will be observed in H2 as compared to methane-
based on its lower viscosity. As a result, there is less room for H2
storage because less water is swept when H2 is injected.
In addition to gas injection rate, viscous fingering is initi-
ated due to differences in viscosity, density, and surface tension
forces (Berg and Ott, 2012; Phukan et al., 2020; Al-Abri et al.,
2012; Yip et al., 2013). Following the enhanced oil recovery (EOR)
method with an emphasis on mobility study, viscous fingering
can result in a poor vertical and horizontal sweep within the
porous media (Massarweh and Abushaikha, 2021; Diersch, 2014).
As a result, a larger contact area is formed between the injected
H2 gas and the water, thereby increasing the chance of H2 disso-
lution due to gas diffusion. Furthermore, the H2 interaction with
the rock could affect its purity during withdrawal (Zivar et al.,
2021; Tarkowski, 2019).
6.3.6. Adsorption–desorption
Gas adsorption–desorption mechanisms are a popular solid–
liquid technique used in characterizing flow in porous media.
Adsorption denotes the adhesion of ions, atoms, or molecules
from a gas/liquid or dissolved solid to a surface, whereas des-
orption entails the removal of the adsorbed substances under
high temperature and pressure. These phenomena take place in
micropores with the mesopores or macropores providing storage
for the free gas and tortuous paths for gas transport (Afagwu
et al., 2021a,b). These processes have received significant atten-
tion in CO2 , CH4 (Zhang et al., 2016c; Wang et al., 2018; Zhou
et al., 2019),
( and) N2 (Liu et al., 2019). Currently, H2 adsorption
capacity AH2 studies remain scarce as only few publications
point towards them (Iglauer et al., 2021a; Bardelli et al., 2014;
López-Chávez et al., 2020; Didier et al., 2012).
Notwithstanding, AH2 between a raw clay (composition: 17 wt%
illites, 2.6 wt% kaolinite, 2 wt% chlorites, 20 wt% carbonate,
22 wt% quartz, and 5 wt% other) and purified clay (void of Fe,
(9) Mn, and carbonate with approximately clay content of 80%) was
investigated by Bardelli et al. (2014) as shown in Fig. 25. Clearly,
AH2 is a function of surface area, pressure, and temperature. For
example, at 363 K and 46 m2 /g surface area, AH2 increased from
0.125 mmol/g to 0.61 mmol/g as pressure increased from 0.4 MPa
to 4 MPa for the raw clay, whereas at 363 K and 84 m2 /g surface
area, AH2 increased from 0.065 mmol/g to 1.23 mmol/g as the
pressure increased from 0.4 MPa to 5.5 MPa for the purified clay.
This means that at greater pressures and larger surface areas, AH2
is higher. A significant finding for both clay samples was that
AH2 remained consistent after saturation (did not increase further
with pressure). Similar outcome is reported for CO2 (Hui et al.,
2019) and CH4 (Wang et al., 2016), indicating the similarity of
some gases during the adsorption and desorption process.
As also illustrated in Fig. 25, the temperature effect in H2
adsorption shows that at constant pressure (e.g., 6 MPa), a slight
increase (from 0.53 mmol/g to 0.62 mmol/g) for raw clay was
observed as the temperature increased from 301 K to 363 K
respectively. This could be attributed to the presence of iron in
the clay sample, which reacts faster with H2 at elevated tem-
peratures (Didier et al., 2012; Chen et al., 2011; Guan et al.,
2018). However, a similar trend was also reported for the puri-
fied clay sample (from 0.93 mmol/g to 1.23 mmol/g) when the
temperature increased from 301 K to 363 K at constant pressure
(i.e., 6 MPa). Therefore, to reduce the uncertainties on AH2 , more
investigation is required for iron-free clay minerals to serve as
a benchmark as the adsorption process usually overlaps with
(10)
Again, H2 adsorption on a synthetic dry sodium montmoril-
lonite type-clay and Callovo-Oxfordian clay rock using gas chro-
matography were studied by Didier et al. (2012). After the dry
485
N.S. Muhammed, B. Haq, D. Al Shehri et al.
Fig. 25. H2 adsorption capacity for clay rocks (Bardelli et al., 2014).
clay samples reacted with H2 at 0.045 MPa and 363 K, they
observed that 0.11 wt% of H2 was adsorbed for an exposure time
of 30 to 45 days (in the case of synthetic sodium montmorillonite
clay) whereas no reduction was observed with Callovo-Oxfordian
at the experimental conditions. They attributed the changes (H2
adsorption) to the presence of Fe (III) ions in the synthetic sodium
montmorillonite clay whereas Callovo-Oxfordian clay only con-
tained smectite/illite and calcite minerals as such the clay rock
seems to be geochemically stable against the presence of H2 at
such UHS experimental conditions (Didier et al., 2012). Similarly,
López-Chávez et al. (2020) studied H2 adsorption on calcite rock
oil fields via molecular dynamic simulation. The authors high-
lighted that about 0.42 wt% of H2 was adsorbed on the calcite
rock surface at 0.1 MPa and 400 to 600 K oil field conditions.
In a recent study, Iglauer et al. (2021a) experimentally investi-
gated the effect of H2 adsorption on sub-bituminous coal located
in Collie, Western Australia. The group reported that substantial
amounts of H2 (0.23709 moles H2 /kg coal) via adsorption can
be stored even at moderate pressure (3.3 MPa) and tempera-
ture (303 K). Also, when enhanced at higher pressures (14.3
MPa) and temperature (318 K), a higher amount of H2 (0.60183
moles H2 /kg coal) could be stored. Furthermore, the outcome
was compared with CGS conditions, and it was documented that
similar
( ) behavior was recorded as both H2 adsorption capacity
AH2 and adsorbed CO2 adsorption capacity (ACO2 ) increases with
pressure until adsorption saturation was attained. However, the
temperature was observed to influence AH2 more than ACO2 at the
same thermo-physical condition. The change (i.e., a smaller value
of AH2 as compared to the large value of ACO2 ) was attributed
to the different quadrupole moments, since it was established
that CO2 has a quadrupole moment nearly ten times bigger than
H2 (Iglauer et al., 2021a).
7. Hydrogen reaction in the subsurface environments
Understanding the potential reactions of injected H2 with
pre-existing minerals, gases, ions, microorganisms, and other sub-
stances is critical as it is required for safe (to reduce the risk
of leakage) and successful operations (to avoid H2 conversion or
reduction in its purity). The generation and or consumption re-
action process for H2 in the subsurface can be grouped as abiotic
(non-living components such as water, rock minerals, and gases)
and biotic (living components such as bacteria) reactions (Pan-
filov, 2016; Gregory et al., 2019). The contributions of each of
486
Energy Reports 8 (2022) 461–499
these processes to the gaseous composition of the subsurface
will depend on the environment. For instance, the subsurface is
often characterized by combinations of factors such as elevated
temperature, high salt concentrations, and high pressure, reduced
void space, and limited nutrient availability (Thaysen et al., 2021).
Abiotic processes are inorganic reactions between the reser-
voir rock, in-situ brine, and injected H2 that could alter the
petrophysical reservoir performance (porosity, permeability, pore
structure, and composition) and the geo-mechanical stability of
the rock (Yekta et al., 2018b; Truche et al., 2013). It can operate
over a wider range of temperatures (over 600 ◦ C) which does
not represent typical UHS conditions (Zivar et al., 2021). Since
abiotic H2 generation occurs at high temperatures and involves
radiation, it may inhibit microbial life close to the reservoir vicin-
ity. However, at a lower source of heat or radiation and farther
away from such vicinity, this H2 could become available for
microorganisms’ consumption and as such, biotic environments
are likely to promote H2 removal or consumption. Reactions of
this form (biotic processes) are mainly facilitated by the activities
of biochemicals such as microorganisms in the reservoir (Bagnoud
et al., 2016; Jacops et al., 2015). Most microorganisms in nature
grow in biofilms attached to surfaces in the form of aggregated
microbial cells embedded in a secreted matrix of extracellular
polymeric substances (Dopffel et al., 2021; Thaysen et al., 2021;
Yin et al., 2019). Even small amounts of biofilm can reduce pore
throat sizes and increase the flow-path tortuosity, thus, resulting
in a significant decrease in permeability (Coombs et al., 2010).
In the subsurface, unlike CO2 which undergoes acid–base re-
actions through carbonic acid formation (Adamczyk et al., 2009;
Iglauer, 2011), H2 reactions are essentially reduction–oxidation
(redox) (Truche et al., 2013; Reitenbach et al., 2015). A com-
prehensive insight on H2 generation and consumption processes
is presented elsewhere (Thaysen et al., 2021; Gregory et al.,
2019). While both abiotic and biotic constitute generation and
consumption of H2 , abiotic, however, is often ascribed to H2
generation while biotic depicts H2 consumption. In the context
of UHS studies, the four main microbial processes (biotic) with
implications for H2 geo-storage are presented in Fig. 26, which are
briefly discussed below. Their metabolic reactions differ by the
used electron acceptor. These processes (methanogenesis, aceto-
genesis, sulfate reduction, and iron (III) reduction) have assisted
in H2 consumption and applied to all types of UHS (caverns and
porous media). It is vital to state herein that, water production
from sulfate and iron (III) reduction bacteria, is twice as much
water per unit mass of H2 for methanogenesis, and acetogen-
esis (Panfilov, 2016). A summary of studies on UHS microbial
activities is presented in Table 8.
7.1. Methanogenesis
Methanogenesis is the biological generation of methane. It oc-
curs in the presence of hydrogenotrophic methanogens (archaea)
microorganisms which use CO2 as the electric acceptor in optimal
conditions (9 MPa and 303 K to 313 K) in the subsurface. This
process is called Sabatier’s reaction (Panfilov, 2016). It can also
occur at a higher temperature (1073 K) in the presence of a
nickel catalyzer (Panfilov, 2016). Three groups of methanogens
are usually found including Methanobacteriales, Methanococcales,
and Methanomicrobiales (Panfilov, 2016). The most common H2
conversion to methane due to methanogens is the Labodice town
gas storage aquifer project earlier reported (Kruck et al., 2013;
Šmigáň et al., 1990). A typical reaction for methanogenesis is
given by Eq. (11). Methane from such processes usually has
high purity. Additionally, it is easy to store and transport and
its combustion emit few pollutants compared to oil and coal
combustion (Burkhardt and Busch, 2013).
4H2 + CO2 ↔ CH4 + 2H2 O (11)
N.S. Muhammed, B. Haq, D. Al Shehri et al.
Fig. 26. Types of hydrogenotrophic bacteria in UHS (Panfilov, 2016).
7.2. Acetogenesis
As for acetogenesis, the microbes also use H2 and CO2 for their
metabolism via the conversion of acetate to acetic acid as shown
in the following reaction (Gregory et al., 2019; Rabii et al., 2019;
Pichler, 2013) (see Eq. (12)).
4H2 + 2CO2 ↔ CH3 COOH + 2H2 O
The acetate production is usually slow in acidic aqueous aquifers
and depleted hydrocarbon reservoirs where a high prevalence
for salinity conditions exists (Jaafar et al., 2009; Bagaria et al.,
2013). Although reactions between the injected H2 and the hy-
drocarbons (e.g., C2 H6 + H2 ↔ 2CH4 ) may occur, which could
lead to H2 loss eventually (Carden and Paterson, 1979; Truche
et al., 2013). Common acetogens include Clostridium thermoau-
totrophicum, Clostridium aceticum, Butyribacterium methylotroph-
icum, Sporomusa sphaeroides, Sporomusa ovata, Acetogenium kivui,
Acetobacterium woodii, and other species (Panfilov, 2016).
7.3. Sulfate-reduction
In the case of sulfate-reduction reactions, the archaea mi-
croorganism are bacteria that produce hydrogen sulfide (H2 S)
after the consumption of H2 in the presence of sulfate-reducing
ions as displayed in the reaction (Eq. (13)). This type of reac-
tion occurs mostly in hydrocarbon reservoirs where incompatible
water is injected during flooding because of the activity of the
sulfate-reducing ions (Cavallaro et al., 2005; Ligthelm et al., 1991).
Optimally, the reaction temperature is around 311 K (Bernardez
et al., 2013), however, a higher temperature up to 383 K is also
reported (Machel, 2001; Jorgensen et al., 1992).
2
5H2 + SO−
4 ↔ H2 S + 4H2 O
The case study of the water incompatibilities is that reported
by Cavallaro et al. where an increase in H2 S production was
observed after water flooding in Las Hera-Cerro Grande oilfield in
Argentina (Cavallaro et al., 2005). H2 S production (a highly toxic
substance) in the sub-surface poses’ significant threat to the in-
jection and production facilities and since the product comes with
water, it could reduce the H2 storage capacity by an increase in
water saturation at the outlet during H2 withdrawal (Carden and
Paterson, 1979). Similar to acetate production reaction, sulfate
reduction should be slower in an acidic aqueous and depleted
hydrocarbon reservoir where high salinity exists (Jaafar et al.,
2009; Bagaria et al., 2013).
Energy Reports 8 (2022) 461–499
7.4. Iron-reduction
Iron (III) reducing bacteria use metabolic reaction in UHS.
The process of this reaction where iron (III) oxide (ferric ox-
ide) consumes H2 is shown in Eq. (14)). Iron-reducers can be
heterotrophic (that use organic carbon as food) or autotrophic
(12) (those bacteria that can synthesize their food) (Porsch et al.,
2009). It also leads to water production after reacting with the
rock minerals hence reducing the H2 storage capacity since high
Sw will be achieved (Gregory et al., 2019; Pichler, 2013; Porsch
et al., 2009). Some common iron-reducing bacteria are Geobacter
metallireducens and Shewanella putrefaciens (Panfilov, 2016).
H2 + 3FeIII II
2 O3 ↔ 2Fe3 O4 + H2 O (14)
Besides the rock mineral (solid–fluid) interactions, iron-reducing
bacteria can also induce in-situ reactions with the occupying
fluids and the minerals (fluid–fluid) leading to precipitation and
mineral dissolution. Although, this reaction rate, largely depends
on the reservoir conditions (including temperature, pressure, bac-
teria ions, and the pre-existing minerals). The primary effect of
such a reaction is the potential damage that might be caused
to the reservoir porosity and permeability, which could affect
the containment security (Shabani and Zivar, 2020). It is well
established that UHS is advantageous over other storage tech-
niques due to its security (Lemieux et al., 2019), however, mineral
precipitation and/or dissolution if not addressed, can alter the
efficiency of the UHS operations. For example, when the pre-
cipitation rate (which can occur both at the reservoir and cap
rocks level) is less than the dissolution rate, the caprock integrity
becomes compromised and the chance of H2 loss via leaking is in-
(13) creased due to porosity and permeability enhancement whereas,
if greater than the dissolution rate, the caprock integrity might
still be intact but the porosity and permeability near the well-
bore region might be jeopardized thus reducing the ultimate
injection and withdrawal rate of the UHS operation (Zivar et al.,
2021; Shabani and Zivar, 2020).
8. Modeling perspective of the UHS
Multiphase flow properties in subsurface reservoirs can be
predicted by several methods including laboratory measurements
and numerical simulations. Experiments are expensive and time-
consuming, and they can only be used on a small number of
487
N.S. Muhammed, B. Haq, D. Al Shehri et al.
Table 8
Selected H2 reaction studies.
Author (s) Objective(s)
Panfilov et al. (2006) Hydrodynamics of H2 mixtures
with other gases as well as
bacteria effects
Ebigbo et al. (2013) Pore-scale study of the effect
of microorganisms
(methanogens, acetogens, and
acetotrophs)
Amid et al. (2016) Investigated possible reactions
between H2 and the mineral
components of the reservoir
Hagemann et al. (2016) Impact of H2 on the
hydrodynamic and
bio-chemical behavior during
Hydrogenization of
underground storage of natural
gas
Hemme and Berk (2018) Effect of microbial actions in
depleted gas
Thaysen et al. (2021) Investigated the potential
effects of H2 consumption in
42 depleted oil and gas
reservoirs (UK case study)
samples and situations. To allow for a larger range of research
and sensitivity analysis, numerical modeling and simulations are
essential to supplement laboratory experiments. These are done
to either address the controlling parameters such as physical,
geo-hydraulic, geochemical, biochemical, and mineralogical pro-
cesses during UHS. Through an integrated study of the above
processes, numerous questions involving which of these factors
488
Methodology
• Monod’s model
• Mathematical model
• Numerical analysis
• Coupled pore-scale modeling
• biofilm model
• viscous-fluid model
• Biological study
• chemical study
• Growth and decay modeling
using Monod, Moser, and
Panfilov models
• Biochemical model
• Microbial growth rate
• Microbial growth calculation
• Cell-specific H2 consumption
estimation
• H2 consumption calculation
affect the reservoir and fluid properties within the storage zone,
what happens when a new gas (H2 in this case) is injected into the
native gas initially present in the reservoir during injection and
withdrawal cycles and most importantly, the governing parame-
ters that affect the dynamics of the fluid is determined. A sum-
mary of recent works concerning those controlling parameters is
presented in Table 9.
Energy Reports 8 (2022) 461–499
Remarks
• Transport phenomenon is
influenced by the activity of
the methanogens
• Bacterial activity leads to the
transformation of a part of H2
and CO2 (cushion gas) into CH4
and H2 O.
• Methanogenic growth rates
depend on biomass presence
and the available residual
water saturated with the
biomass.
• Conversion of the films was
highly dependent on the
amount of residual water
• Sulfur-containing
assemblages were considered
as a potential threat to the site
• About 3.7% of H2 was lost
due to methane presence and
biomass over the storage
period
• Biological loss due to residual
CO2 conversion was limited
even in CaCO3 dissolution
• The presence of H2 S was
reported as a potential
challenge in the field
• The amount of microbes
present determines the extent
of partial transformation of the
injected H2 into CH4 and H2 O
• Microbial growth function
selection has an important
influence on the outcome
• Loss of H2 by bacterial
consumption was imminent
• Losses due to methanogens
(CO2 ) and sulfate reduction
(SO24− ) effect between the
reservoir and top caprock as
well as reservoir and bottom
seal were different due to
other presiding mineral
presence over a long time
• Provided detailed
multi-dimensional information
on microbial growth control
• Noted that temperature,
salinity, and pressure impact
more on the microbe’s growth
in the subsurface.
• Some fields were reported
sterile concerning temperature
while some fields can sustain
all the microbial processes
studied
• H2 consumption was
reported negligible as
compared to the percentage of
the stored H2
N.S. Muhammed, B. Haq, D. Al Shehri et al. Energy Reports 8 (2022) 461–499

Table 9
Summary of literature works on UHS modeling studies.
Author(s) Objectives Software tool(s) Storage duration Storage medium Injected gas Adopted Major findings (s)
approach(s)
Pfeiffer and Investigated the Eclipse 300 Short term Existing Rhaetian N2 and H2 • Peng–Robinson • Simulation shows
Bauer hypothetical behavior anticlinal structure EOS for property that storage can
(2015) of subsurface porous based on saline modeling supply about 20%
media H2 storage site aquifer model demand for electrical
using numerical energy for 1 week
simulation • An optimized
injection scheme can
further improve the
storage performance
Hagemann Mathematical Open-source code Short term Aquifer H2 and CH4 • Selective • Injection rate
et al. (2015) modeling of unstable DuMux technology controls gravitational
transport (gas rising, • Darcy’s law and viscosity forces
lateral spreading, and • Brooks Corey displacements
hydrodynamics) in • Box-method • Gas rise and
UHS leakage is delayed by
storing H2 in a
stratified manner
through selective
technology
• The lateral extent
of the barriers
significantly influence
gas rising and also
depends on gas type

Amid et al. Seasonal storage of PHREEQC Short term Depleted gas H2 • Volumetric • The facility could
(2016) H2 by comparing the (geochemical analysis store about 42% of
respective capacities modeling) • Chemical the energy capacity
and deliverability in a stability study supplied
UK storage facility • Leakage study • H2 loss due to
dissolution and
diffusion could be
reduced to < 0.1%

Feldmann Investigated the Open-source code Long term Depleted gas H2, CO2 , CH4 , and • Peaceman’s • Good UHS potential
et al. (2016) effect of gas mixing, DuMux (flow H2 O model • H2 storage in
seasonal injection and transport process) • Selective stratified aquifers
production cycles, and COMSOL technology limits gas loss due to
and hydrodynamics Multiphysics • conventional lateral spreading or
of UHS (numerically cell-centered finite viscous fingering
simulate gas volume method beyond the spill point
displacement • Molecular • Selective
front) diffusion technology
• Mechanical implementation is
dispersion considered a good
way of H2 production
• Native fluid
displacement
efficiency depends on
the extent of gravity
override and viscous
fingering
Pfeiffer Numerical simulation Eclipse 300 Short term Existing Rhaetian H2 and N2 • Penge Robinson • H2 storage was
et al. (2016) and geophysical anticlinal structure EOS found to increase
monitoring of a based on Saline • gravity modeling with cycle numbers
synthetic, aquifer model • facies modeling as more H2 was
heterogeneous field • P-wave velocity available at the final
site for UHS model storage cycle
• petrophysical • Detailed
rock model multi-dimensional
• Gassmann fluid information for UHS
substitution model was presented in this
• seismic study
mapping, flow
simulation model
• geoelectric
resistivity model

(continued on next page)

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N.S. Muhammed, B. Haq, D. Al Shehri et al. Energy Reports 8 (2022) 461–499

Table 9 (continued).
Author(s) Objectives Software tool(s) Storage duration Storage medium Injected gas Adopted Major findings (s)
approach(s)
Hagemann Studied the effect of Open-source code - Depleted gas H2 and CH4 • Darcy’s, law • The importance of
et al. (2016) H2 hydrodynamics for DuMux • Fick’s law injection rate was
effective comparison • Brooks Corey emphasized, and it
between natural gas • Mathematical showed that a high
and depleted gas model injection rate leads to
reservoir • Hydro-dynamical an unstable and
model lateral finger
spreading below the
caprock
• Observed that
lateral fingers are
more pronounced in
UHS than in storage
of natural gas

Pfeiffer H2 storage in Eclipse 300 Short term Existing Rhaetian H2 and N2 • Penge Robinson • Storage is mainly
et al. (2017) heterogeneous anticlinal structure EOS limited by the
sandstone effects of based on Saline • facies modeling achievable extraction
dimensioning and aquifer model rates.
induced hydraulics • This study provides
detailed information
on how
heterogeneous
parameter
distribution affects
storage efficiency

Sainz-Garcia Assessment of COMSOL Long term Saline aquifer H2+ CH4 • 3D multiphase • A maximum H2
et al. (2017) feasible strategies for Multiphysics model recovery ratio of 78%,
seasonal underground • Darcy’s law was achieved
H2 storage • Brooks Corey • No viscous
fingering
• Steeply dipping
structures can store
H2 gas without
cushion gas, though it
is prone to up coning
• H2 is best
recovered if several
shallow extraction
wells are located
beneath the caprock

Pfeiffer and To compare Eclipse 300 Short term Existing Rhaetian H2 and N2 • Analytical • This study can
Bauer simulations of H2 anticlinal structure averaging methods provide detailed
(2018) storage in a based on Saline multi-dimensional
sandstone formation aquifer model information on the
using heterogeneous applicability of spatial
and homogeneous averaging methods
flow property models for approximating
storage characteristics
Hemme and To identify potential PHREEQC Long term Depleted gas H2 • one-dimensional • Observed losses
Berk (2018) risks during storage (geochemical reactive mass due to diffusion
modeling) transport (1DRMT) through the cap tock
• Monod model • Storage time,
pressure,
temperature, kinetic
rate, and stored gas
composition
significantly influence
the overall loss

(continued on next page)

9. Economics of UHS
As part of the effort to promote the H2 economy, UHS, as re-
viewed, has promising potential due to its significant impact over
the years. However, to fully achieve this vision, it is imperative to
discuss the economic viability of the UHS process. Clearly, UHS is
advantageous in terms of security containment (Lemieux et al.,
2019), capacity (Lemieux et al., 2019; Tarkowski and Czapowski,
490
2018), duration (Tarkowski, 2019), and high economic viabil-
ity (Michalski et al., 2017). However, the financial aspect span
over capture cost, transportation cost, storage/withdrawal cost,
and monitoring cost (Taylor et al., 1986) which if not carefully
decided, can affect the overall storage process.
In petroleum economics, capital cost (CAPEX) and operating
cost (OPEX) are the major costings used to determine the prof-
itability of any financial assets. Thus, relating it to UHS, Taylor
N.S. Muhammed, B. Haq, D. Al Shehri et al. Energy Reports 8 (2022) 461–499

Table 9 (continued).
Author(s) Objectives Software tool(s) Storage duration Storage medium Injected gas Adopted Major findings (s)
approach(s)
Hassan- Multi-step Geochemist Short and long Depleted gas H2 + CH4 mixture • Equilibrium • The kinetic batch
nayebi et al. geochemical study of workbench (GWB) term modeling model shows that H2
(2019) fluid–rock • Primary kinetic interactions with
interactions using batch modeling minerals require time
equilibrium and • Final kinetic scales much larger
kinetic batch batch modeling than a typical H2
simulations in • storage cycle
Molasse, Basin, Upper • Interactions among
Austria H2 and brine
components are
recognized to be
more relevant within
the storage cycle of
H2
• Observed pyrite
reduction into
pyrrhotite
significantly increased
the reservoir pH and
further led to H2 -loss.

Luboń and Evaluation of the PetraSim-TOUGH2 Long term Aquifer H2 • Isothermal • Up coning was
Tarkowski viability of seasonal assumption reported as the major
(2020) (cyclic) H2 storage • Multi-phase issue in the aquifer
flow modeling • The percentage
• Geothermal recovery of H2
modeling increased with
withdrawal cycles
• Water management
is considered a
potential
environmental
challenge

Lysyy et al. Seasonal H2 storage Eclipse 100 Long term Depleted oil and H2 and CH4 • History • Annual H2 delivery
(2021) evaluation gas field matching of ∼ 400 million Sm3
• Storage was achieved
initialization • 87% of H2 was
• Cyclic operation recovered
• Prolonged • Injection of 30% H2
withdrawal with gas mixture
investigation resulted in fluctuation
Case studies in H2 delivery
• Dipping structure
was considered as
not a good H2
storage candidate

Heinemann A comprehensive Petrel Long term Depleted gas H2 • One injection • Cushion gas is an
et al. investigation on the GEM and production important component
(2021b) role of cushion gas well assumption for exploiting the
for H2 injection and • SRK EOS used total capacity of an
production for H2 property H2 storage site
modeling • Cushion gas to
• Peaceman’s working gas capacity
model was used in depends on geological
GEM for reservoir parameters including
flow rate storage reservoir
depth, anticline
structure, and
reservoir permeability

et al. enumerated categorically that compressor (based on op-
erating units’ requirement) cost, foundation cost, transformer
erection and installation cost, electricity (circuit breaker) cost,
monitoring (cooling/heating, ventilation, lighting, the alarm just
to name a few) cost, gas holding (based on storage capacity)
cost, and the cost of wellhead construction are the major CAPEX
required. In addition to the highlighted cost, additional costing in-
volving excavation (drilling cost), reinforcement cost, lagoon cost
(for disposal of the withdrawn brine), plugs, surface works, and
handling equipment cost are required for cavern development
since caverns are more construction intensive than aquifers and
491
depleted hydrocarbon reservoir whom are already built and are
geology dependent (Taylor et al., 1986; Lindblom, 1985).
Embrittlement cost due to H2 interaction with surface and
subsurface facilities during transportation is another important
economic aspect that must be considered when designing a viable
UHS operation. Materials resistant to corrosion and rusting are
required to alleviate the effect of mechanical or physicochem-
ical failure due to cracking (Ugarte and Salehi, 2021). Also, it
was reported that embrittlement is more pronounced in UHS
as compared to natural gas storage thus, more attention is re-
quired (Kruck et al., 2013). In the case of operating cost, Taylor
N.S. Muhammed, B. Haq, D. Al Shehri et al.
Fig. 27. Notable challenges to UHS.
Source:
(https://youtu.be/2VqAeYU22n0).
et al. enumerated the cost of H2 generation power, cooling, la-
bor and utilities, supervision/administration, and other overhead
costs such as cushion gas requirements for pressure maintenance
of the stored gas (Taylor et al., 1986). Clearly, the cost of cooling
and power is regarded as OPEX since it is a continuous effect that
may be incurred additionally if the UHS operations take more
than expected due to natural occurrences.
Some researchers have made efforts to evaluate the economics
of UHS potential storage sites based on the above CAPEX and
OPEX costing reported by Taylor et al. (1986). The aim of this
review in terms of economics is to provide the reader with
the basic component used to ensure the economic viability of
potential H2 storage operation. Therefore, detailed insight and
data for cost analysis and economics of different UHS processes
can be found in other publications (Lord et al., 2014; Michalski
et al., 2017; Iordache et al., 2014; Le Duigou et al., 2017).
10. Prospects and challenges
The selection and use of clean fuels and energy sources can be
envisaged as the most intriguing challenge for the future of the
environment and society (Fig. 27). The flexibility in production
from a variety of feedstocks such as fossil fuels up to renewable
energy sources makes H2 an ideal candidate for becoming the
best solution as a fuel and energy carrier (Holladay et al., 2009;
Nikolaidis and Poullikkas, 2017; Muhich et al., 2016). Out of all
the storage techniques for H2 , UHS has received greater attention
as seen in the up rise in publications. As a new technology frontier
targeted towards reducing GHGs emissions through providing a
net-zero or carbon-free ecosystem, UHS techniques among others
are not without some challenges as the experience on this tech-
nology are scarce. In addition, besides the difficulty associated
with the potential sites (including geological, engineering, and
economics), other intriguing factors such as legal and societal
interplay contributes to its entire success (Kabuth et al., 2017).
Though some of these factors (finances, governmental policies,
engineering, legal and social) are adjustable whereas some are
rigid (geology-related). It, therefore, becomes essential to ensure
all these mentioned criteria are put into perspective for an effec-
tive UHS operation. Some of the potential challenges based on the
reviewed storage means are enumerated.
• Geology-related implication without penitence is the most
challenging, and therefore, it must be addressed first when
selecting any potential site for UHS operation. In this regard,
caverns are considered the best option due to their easy
Energy Reports 8 (2022) 461–499
Modified after
access, fairly absence of microbial activities, and the ability
to withstand high reservoir conditions (pressure and tem-
perature) but are limited in number. Depleted hydrocarbon
reservoirs (oil and gas) are second while aquifer is third due
to the un-identified challenges inherent in aquifer reservoirs
compared to depleted reservoirs that are already tested
(caprock integrity) and explored. Such challenges include
the cushion gas quantification which is the second require-
ment in any UGS operation after the injected working gas
(e.g., H2 , CO2 , or CH4 ). For example, 33% for H2 and 50% for
CH4 cushion gas have been reported in a depleted hydro-
carbon reservoir whereas 33%–66% for H2 and 80% for CH4
is documented for aquifer (Bai et al., 2014).
• Information on the depth and storage capacity of the po-
tential site is vital as it can affect the entire UHS operation.
Although depth may not be as critical as the volume, it is
important during the planning and design stage (to save
the team of drilling deep) since the density and viscosity
of H2 have no considerable change with depth (Zivar et al.,
2021). In contrast, storage capacity is significant, and it
informs the decision stage (during planning and execution)
because caverns are known to have a low storage capacity
as compared to porous media storage techniques (aquifer
and depleted hydrocarbon reservoir), which have high ca-
pacity in addition to the excellent porosity and permeability.
A reservoir with good permeability will promote efficient
injection and withdrawal of H2 .
• Understanding the fluid–fluid and solid–fluid interactions in
reservoir geology help to plan for an efficient UHS process.
In this case, the salt cavern is preferable compared to porous
media since reaction seldom takes place in them. However,
a special class of archaea (microbes) that are temperature
loving (thermophilic), and salt-loving (anaerobic, barophilic,
and halophilic) might precipitate into different forms during
H2 consumption. As for porous media, the rock type, bacte-
ria, ions in the water, and pre-existing fluid are significant
because of the abiotic and biotic reactions that may occur
at different stages. Clearly, the aquifer, in this case, is the
safest since the in-situ fluid is only water/brine. On the other
hand, when considering a depleted hydrocarbon reservoir,
the inherent hydrocarbon fluid in the reservoir can add
more complications.
• Seismic activities are an important safety concern relating to
UHS because they could compromise the integrity of storage
structures (e.g., the fracturing of caprock or caverns). There-
fore, potential UHS sites must ensure seismic hazard maps
492
N.S. Muhammed, B. Haq, D. Al Shehri et al.
are available especially at field scale operation to ensure the
storage process is void of any potential seismic activities
that might occur within the location (Lemieux et al., 2019).
The effect of neglecting this factor might be a catastrophe
that might even result in loss of life.
• Again, flammability is also important during the selection
of UHS sites. Aquifer — due to the absence of oxygen can-
not create any ignition (thus forming a flammable mixture
can be avoided) compared to depleted hydrocarbon reser-
voir. Also, improved monitoring procedures are required to
ensure that the H2 can be stored safely.
As a concluding remark, it is vital to state that various experts
agree upon the vision that the future energy economy will be
mainly based on H2 (probably in combination with electricity).
The pathway for the transition from current energy economies
to an H2 economy is paved with many scientific, technological,
and economical drawbacks, and to fully accomplish this future,
several transitional and gradual steps will be required. The most
significant milestones for the H2 pathway must be mainly based
on the intensification of awareness, research, and development
programs in analyzing and investigating the opportunities and
challenges.
11. Lessons learned and recommendations
This review provided a robust but concise overview of the
potential application of geological formations for UHS to achieve
a large-scale H2 economy. Extensive discussions on the applicable
sites for UHS have been presented with the systematic approach
used in site selection and identification. Attention has also been
given extensively to each corner of the hydrodynamics influ-
encing parameters affecting UHS operations ranging from solid,
liquid, and solid–liquid interactions. In addition, reaction per-
spectives, modeling studies, and challenges have been presented.
Based on this study, the learning outcome is summarized below.
• Salt caverns (with a lesser cushion gas percentage) among
other geological options is used to conduct UHS study due
to their short-term storage and ease of cyclicities (injec-
tion/withdrawal) during peak demand for H2 whereas porous
media (aquifer and depleted reservoirs) are used for an ex-
tensive and longer storage period. The aquifer is often used
as case studies for porous media due to the nature of the
in-situ fluid present which makes computation and analysis
less complex compared to depleted deposits, especially oil
reservoirs.
• The use of cushion gas depends on the target and application
of the potential UHS projects as each gas i.e., N2 , CO2 , and
CH4 reported in this review plays a major role in the purity
of H2 during underground storage since each gas exhibit
different mixing and dilution profile when combined with
H2 .
• Recent methodologies have adopted a machine learning ap-
proach in predicting various properties for potential geolog-
ical candidates used for UHS study thus, a wider spectrum
of computation can be conducted within a short period with
a high-efficiency rate. Though, it also depends on the type
of models as each outcome is different.
• Out of the research areas for UHS, hydrodynamics and ge-
omechanics have received more attention based on the ease
in comparison between other related gases (i.e., CH4 and
CO2 ) to infer the behavior of H2 during storage.
• Geomechanics and hydrodynamics (solid, fluid, and solid–
fluid) interactions show that H2 leakage (losses) is mostly
affected by H2 diffusion/precipitation with rock minerals
and microbial activities such as sulfate-reducing bacteria,
methanogens, and acetogens.
493
Energy Reports 8 (2022) 461–499
• The reviewed data on contact angle showed similar behavior
of H2 with rock and different mineral types in terms of
increase in pressure. However, acid concentration in the
reservoir may alter such a trend as wettability may be in-
creased or decreased. Additionally, the difference in wetting
properties can be attributed to the influence of mineralogy,
rock heterogeneity, as well as petrophysical properties of
rock surface.
• Challenges on geological sites for UHS are numerous, how-
ever, site selection is considered the most significant be-
cause it can generally preserve the economic balance of the
potential UHS projects.
Even though UHS has been demonstrated to be feasible, further
research and up-scaled pilot projects are needed. Thus, con-
clusions drawn from this study may not be used categorically
to emphasize the direct behavior of UHS operation, since this
novel energy carrier, is still in its infancy hence, more research
and development targeted towards a sustained H2 economy is
essential. Based on this study, the following knowledge gaps are
recommended.
• It has been discussed that σeffective affects both ka and φeffective .
Notwithstanding, the response of σeffective on φeffective is gen-
erally smaller than that of ka (Hu et al., 2020; Dong et al.,
2010), hence investigating the effect of σeffective on φeffective at
reservoir conditions before large scale UHS application and
that between σeffective and kr is highly essential.
• H2 diffusivity can be related to viscosity using the Ein-
(where D, µ, r, T and kB
kB T
stein relationship, D = 6πµ r
represent diffusion coefficient, viscosity, particle spherical
radius, temperature, and Boltzmann’s constant respectively).
However, the absence of H2 viscosity and diffusivity data at
the same thermo-physical conditions makes it difficult, thus
experimenting or modeling such behavior is recommended.
• Generally, the magnitude of gas flow (H2 ) in porous media
varies with the size and interconnected compartment and
since Darcy’s law is valid for macropores, it is highly sug-
gested that H2 transport in micro and mesopores be studied
further assuming different pore geometries.
• So far, the solubility (Chabab et al., 2020) and diffusiv-
ity (Vivian and King, 1964) of H2 were reported for only
bulk liquid phases neglecting the fact that gas dissolution
and diffusion can occur in the micro and nanopores of the
reservoir pore network (Afagwu et al., 2021a; Yang et al.,
2021). Therefore, investigating the quantity of solubility and
diffusivity of H2 in such pore networks for different porous
media is suggested for future studies.
• The physicochemical interactions of H2 with solid surfaces
on wettability are interesting to explore. While the
rock/brine/H2 wettability has been studied as seen in recent
observation such as sandstones (Hashemi et al., 2021b;
Iglauer et al., 2021; Ali et al., 2021b), basalt (Al-Yaseri
and Jha, 2021), and clay minerals (Ali et al., 2021a; Al-
Yaseri et al., 2021), further investigation on chemical active
surfaces such as carbonate and their proxy minerals to
effectively study the behavior of H2 -wettability on large
scale is welcomed.
• Hydrogen loss due to microbial activities especially based
methanogens, acetogens, and sulfate reduction should be
investigated further as they are the most contributing mi-
crobes (Thaysen et al., 2021).
Declaration of competing interest
The authors declare that they have no known competing finan-
cial interests or personal relationships that could have appeared
to influence the work reported in this paper.
N.S. Muhammed, B. Haq, D. Al Shehri et al.
Acknowledgment
The authors appreciate the College of Petroleum Engineer-
ing and Geoscience (CPG) at King Fahd University of Petroleum
and Minerals (KFUPM) for providing unrestricted access to vast
academic resources which made this work possible. The corre-
sponding author would like to thank the College of Petroleum and
Geosciences at KFUPM for providing the Start-Up Fund - SF19005.
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