Earth-Science Reviews 253 (2024) 104793

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Earth-Science Reviews
journal homepage: www.elsevier.com/locate/earscirev

Review Article

CO2 sequestration in subsurface geological formations: A review of trapping

mechanisms and monitoring techniques
Osama Massarweh a, Ahmad S. Abushaikha a, *
a
Division of Sustainable Development, College of Science and Engineering, Hamad Bin Khalifa University, Education City, Qatar Foundation, P.O. Box 34110, Doha,
Qatar

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

Keywords: Carbon capture and storage (CCS) in subsurface formations has emerged as a promising strategy to address global
Carbon sequestration warming. In light of this, this review aims to provide a comprehensive understanding of the mechanisms
Geological trapping involved in the geological trapping of CO2. Additionally, it aims to identify the techniques used to evaluate the
Storage reservoirs
potential for CO2 sequestration before injecting CO2 into subsurface formations and the methods used to monitor
Seismic monitoring
the progress of CO2 sequestration after injection. The review also presents future research directions based on
Atmospheric monitoring
current research trends in the field. Four principal trapping mechanisms were identified: structural, capillary
(residual), solubility, and mineral trapping. These mechanisms vary in their CO2 trapping capacity over time and
the storage security they offer. Structural trapping provides the most significant contribution to CO2 trapping,
whereas mineral trapping offers the highest storage security. In terms of monitoring and assessment, three main
approaches were identified, including seismic and borehole geophysical methods, atmospheric monitoring
methods, and laboratory-scale experiments. One of the novel aspects of this review is that it outlines the various
experimental techniques used for investigating CO2 trapping mechanisms, an area that prior reviews have not
addressed. At the laboratory level, various tests and experiments are used to study CO2 trapping characteristics.
These are categorized into petrophysical characterization, pore-scale experiments, CO2-fluid-rock interaction
experiments, and CO2 adsorption evaluation. Another novel contribution of this review is the development of a
qualitative assessment approach for the applicability of various monitoring techniques throughout the stages of
CO2 sequestration projects. This innovative approach has not been reported in the previous literature. Our review
was prepared following a scoping review methodology, ensuring the inclusion of the most recent and relevant
studies.

Recently, interest in developing carbon capture, utilization and/or

storage (CCUS) technologies has surged, aimed at eliminating CO2
1. Introduction emissions associated with fossil fuel consumption (Al-Shafi et al., 2023).
CCS has been implemented across various industrial sectors, including
1.1. Background the construction industry (Hanifa et al., 2023), energy and fuel sectors
(Massarweh et al., 2023), petroleum industry (Somoza et al., 2023),
Since the industrial revolution, there has been a significant increase chemical production (Lamberts-Van Assche et al., 2022), steel produc­
in the atmospheric concentrations of CO2 and other greenhouse gases tion (Nielsen et al., 2020), mining industry (Rausis et al., 2020), waste
(GHGs) (Chien et al., 2023; Joarder et al., 2023). A primary cause of this management (Romero-Hermida et al., 2017), and agriculture sector
increase is the excessive use of fossil fuels for energy generation globally (Zhu et al., 2021).
(Al-Ghussain, 2019; Bhattacharyya et al., 2022). The transition from One main approach for CCUS application is through CO2 sequestra­
fossil fuels to renewable energy sources has been faced with issues of tion into subsurface geological formations, which mainly include saline
unreliability, inefficiencies, high investment costs, and immature tech­ aquifers, depleted oil and gas reservoirs, unminable coal seams, and
nology, to various extents. Consequently, abandoning fossil fuels basalt formations (Jafari et al., 2017). The concept of subsurface CO2
entirely is difficult at the current time (Ghimire and Kim, 2018; Ndwali storage was initially introduced by the oil and gas industry through CO2
et al., 2020).

* Corresponding author.
E-mail address: [email protected] (A.S. Abushaikha).

https://doi.org/10.1016/j.earscirev.2024.104793
Received 8 October 2023; Received in revised form 19 April 2024; Accepted 27 April 2024
Available online 3 May 2024
0012-8252/© 2024 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/).
O. Massarweh and A.S. Abushaikha Earth-Science Reviews 253 (2024) 104793

Nomenclature MeOH Methanol

MMP Minimum miscibility pressure
Abbreviation Description MRI Magnetic resonance imaging
A Area MS Mass spectrometry
AES Atomic emission spectrophotometry MVA Monitoring, verification, and accounting
c Air parcel NC Capillary number
Cc Concentration of gas in the chamber NMR Nuclear magnetic resonance
Cc0 Concentration of gas at the outlet of the chamber OES Optical emission spectrometry
Cci Concentration of gas at the inlet of the chamber P Pressure
CCS Carbon capture and storage Pb Buoyancy pressure
CCUS Carbon capture, utilization, and/or storage Pc Capillary threshold pressure
CT Computed tomography PMMA Poly(methyl methacrylate
DMC Dimethyl carbonate PNG Pulsed neutron-gamma
DME Dimethyl ether PVC polyvinyl chloride
DSA Drop shape analyzer r Radial propagation
E Capacity coefficient R Radius of the fluid droplet
EC Eddy covariance R0 Bubble’s initial radius
EDS Energy dispersive x-ray spectroscopy Ra Rayleigh number
EGR Enhanced gas recovery RCAL Routine core analysis
EOR Enhanced oil recovery RI Resistivity index
EPPA Economic Prediction and Policy Analysis SCAL Special core analysis
Fc Flux ScCO2 Supercritical CO2
FEP Fluorinated ethylene propylene SEM Scanning electron microscopy
FRIM Fast resistivity index measurement Snwi Initial saturation of the non-wetting phase
F-T Fischer-Tropsch Snwr Residual saturation of the non-wetting phase
FWI Full waveform inversion Swiir Irreducible water saturation
g Gravitational acceleration T Temperature
GEC Global Energy and Climate t Time
GHGs Greenhouse gases TIC Total inorganic carbon
GPS Global positioning system TOC Total organic content
Gt Gigatonnes TPD Temperature-programmed desorption
h Height of the fluid column U.S. DOE United States Department of Energy
havg. Average thickness V Volume
H Heat v Vertical speed
HC Hydrocarbon VSP Vertical seismic profiling
HPMI High-pressure mercury injection W Flow rate of air
HTHP High-temperature, high-pressure XRD X-ray diffraction
IC Ion chromatography XRF X-ray fluorescence
ICP Inductively coupled plasma γ Fluid-fluid interfacial tension
IEA International Energy Agency ΔHv Heat of vaporization
IFT Interfacial tension θ Substrate wettability
IPPC International Panel on Climate Change λET Latent heat
k Permeability ρ Density
LCA Life cycle assessment ρf Density of buoyant fluid
LIF Laser-induced fluorescence ρw Density of water
M Viscosity ratio ϕ Porosity
MCO₂ Static CO₂ storage capacity

injection for enhanced oil recovery (EOR) and pressure maintenance storge safety.
operations in hydrocarbon reservoirs (Wilkinson et al., 2009). Currently, Subsurface formations have exhibited the capability to store fluids
CO2 subsurface sequestration is widely implemented in the USA and (e.g., oil, gas, and water) for millions of years. Therefore, they are
northern Europe (Stavropoulou and Laloui, 2022). Recently, many other considered suitable for storing CO2 over geological timescales. This
countries have initiated CO2 sequestration facilities to minimize CO2 storage capability is achieved because these formations have an
emissions during the energy transition period, in alignment with the impermeable caprock layer that provides a hydromechanical barrier,
objectives of the Paris Climate Agreement of 2015. Examples of these preventing buoyant CO2 from migrating to the surface of the Earth (Ali
countries include China, South Korea, Japan, New Zealand, and et al., 2022; Haq et al., 2023). Under such conditions, the capillary and
Australia (Martin-Roberts et al., 2021; Zou et al., 2021). According to viscous effects at the caprock-reservoir interface are high enough to
estimates from geological assessments, the global capacity for geological withstand the injection pressure of CO2 in the reservoir, which hinders
CO2 storage is approximately 8000 to 55,000 gigatonnes (Gt) (Kearns CO2 leakage through the caprock (Espinoza and Santamarina, 2017).
et al., 2017). This capacity is spread across various regions, as shown in Typically, CO2 is injected into reservoirs in a compressed form, either as
Fig. 1. With this large storage potential, understanding subsurface a liquid at a pressure ≥ 7.4 MPa or as a supercritical fluid with pressure
trapping mechanisms and identifying the most suitable monitoring ≥ 7.4 MPa and temperature ≥ 31.2 ◦ C. Therefore, it is recommended to
techniques is necessary for optimizing injection strategies and ensuring inject CO2 at depths exceeding 700–800 m to ensure effective storage

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O. Massarweh and A.S. Abushaikha Earth-Science Reviews 253 (2024) 104793

Fig. 1. Estimated geologic CO2 storage capacity for various regions, with lower (blue) and upper (green) estimates calculated at 0.037 and 0.26 Gt CO2/km3 of
sedimentary basin, respectively. These estimates account for onshore regions and offshore areas that are practically accessible. Data source: (Kearns et al., 2017), as
per the regions outlined by the EPPA model. (For interpretation of the references to colour in this figure legend, the reader is referred to the web version of
this article.)

Fig. 2. Illustration of the main principle of CO2 subsurface sequestration together with the curves of CO2 density (kg/m3) versus depth (m), assuming hydrostatic
conditions. The density evolution is shown: (a) at a constant temperature (T) of 25 ◦ C, and (b) at T = 15 ◦ C (surface temperature) with a 2.5 ◦ C/100 m thermal
gradient. Modified from (Stavropoulou and Laloui, 2022).

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O. Massarweh and A.S. Abushaikha Earth-Science Reviews 253 (2024) 104793

(Stavropoulou and Laloui, 2022), as illustrated in Fig. 2. ScienceDirect (to access Elsevier journals and books), SpringerLink
(for Springer publications), Wiley Online Library, the American
Chemical Society, the American Association of Petroleum Geologists
1.2. Review methodology (AAPG), the American Geophysical Union (AGU), the Royal Society
of Chemistry (RSC), and OnePetro, which is managed by the Society
This paper reviews the recent literature on CO2 sequestration in of Petroleum Engineers (SPE). Additionally, we employed Google
subsurface geological formations. In particular, it discusses the various Scholar to explore a broad spectrum of academic papers, book
mechanisms through which CO2 remains trapped underground. Addi­ chapters, and conference proceedings using the identified keywords.
tionally, it discusses the assessment and monitoring methods of CO2 The use of Boolean operators (AND, OR, NOT) played an essential
containment in subsurface formations. This paper was prepared role in refining the search results, either by narrowing down or
following a scoping review methodology, as described by (Meng et al., expanding the search scope as needed.
2022). The scoping review approach was employed to ensure compre­ 2. Screening: At this stage, the sources gathered from the searches were
hensive coverage of recent literature available on CO2 subsurface trap­ screened by thoroughly reading their titles, keywords, and abstracts
ping mechanisms and monitoring techniques. The process of conducting to eliminate those not aligning with the scope of the review.
this scoping review includes four main stages, which are detailed below 3. Eligibility: This stage involved a more detailed second-level
and outlined in Fig. 3: screening, extending our review to the results, discussion, and con­
clusions of each paper. Only studies that discussed either CO2 trap­
1. Identification: We started this stage by defining the review objec­ ping mechanisms or monitoring techniques were eligible for
tives, aiming to address an area that is not thoroughly explored in inclusion.
currently published review papers. We aimed to ensure that the 4. Inclusion and Analysis: At this stage, papers that passed the eligi­
objectives are clear, focused, feasible, and fall within the scope of the bility criteria were included, charted, and analyzed. Findings from
review, as given in Subsection 1.3 below. Then, we determined the these papers were subsequently linked to identify trends, patterns,
main keywords to effectively guide the literature search, which contradictions, conflicts, and gaps for the drawing of well-informed
mainly relate to CO2 sequestration methods, trapping mechanisms, conclusions.
and monitoring techniques. Examples of these keywords include 5. Writing: The review was carefully written, incorporating tables and
“carbon sequestration,” “geological trapping,” “storage reservoirs,” figures for visual clarity. The narrative was structured with an
“seismic monitoring,” “atmospheric monitoring,” “eddy covariance introduction, body, and conclusions, with all sources of information
(EC),” “carbon capture and storage (CCS),” “structural trapping,” being properly cited.
“residual trapping,” “capillary trapping,” “solubility trapping,”
“mineral trapping,” “water-CO2-mineral reactions,” “seismic tech­
niques,” “borehole geophysical techniques,” “laboratory-scale ex­ 1.3. Objectives, novelty, and structure of this review
periments,” “CO2-fluid-rock interactions,” “petrophysical
characterization,” “pore-scale experiments,” “laser-induced fluores­ The scope of this review is to provide an understanding of CO2
cence studies,” “CO2 adsorption evaluation,” “monitoring verifica­ trapping mechanisms and a description of monitoring techniques based
tion and accounting (MVA),” “CCS projects,” “site characterization,” on the most recent and relevant studies in the field of geological CO2
“modelling and simulation,” “microfluidic flow visualization,” and storage. This knowledge can guide researchers, field practitioners, and
others. Then, we searched for relevant sources by entering the policymakers toward the best practices to ensure environmental safety
identified keywords into various databases and platforms, such as and efficiency in carbon sequestration projects. In light of this, we have

Fig. 3. Main steps followed in the review process.

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O. Massarweh and A.S. Abushaikha Earth-Science Reviews 253 (2024) 104793

set the following objectives to be achieved by our review: transition period. Section 3 discusses in detail the various trapping
mechanisms associated with CO2 sequestration. Section 4 covers eval­
1. To provide readers with a clear understanding of the various CO2 uation and monitoring of CO2 sequestration, focusing on surface and
trapping mechanisms in subsurface geological formations. subsurface detection techniques. Section 5 outlines future research di­
2. To identify the current and emerging techniques used to evaluate the rections. Finally, Section 6 summarizes the review, highlighting the
potential for CO2 sequestration before CO2 injection into subsurface main findings and conclusions.
formations.
3. To identify the methods used to monitor the effectiveness and 2. Importance of CCUS during the energy transition period
progress of CO2 injection processes after the injection has taken
place. According to (IEA, 2021), there will be a continued investment in
existing and new oil and gas fields to meet the continued demand for
A number of reviews have been conducted addressing some aspects crude oil and natural gas over the forthcoming decades. For instance,
related to CO2 trapping mechanisms and monitoring techniques. For from 2031 to 2050, investment in existing oil and gas fields is antici­
example, (Ajayi et al., 2019) reviewed CO2 sequestration in geological pated to range between US$171 billion and US$255 billion, whereas
formations and main monitoring approaches. Their review provided investment in new fields will reach US$436 billion in some scenarios.
valuable information on modelling and simulation procedures used in This significant investment in oil and gas production necessitates further
estimating the storage capacity of geological formations for CO2. How­ development of CCUS technologies, aimed at eliminating CO2 emissions
ever, their discussion of some trapping mechanisms, such as structural associated with fossil fuel consumption.
trapping and capillary trapping, was limited to basic definitions and an
overview of trapping effectiveness. In addition, (Ajayi et al., 2019) did 2.1. The need for CCUS to eliminate CO2 emissions from the
not address experimental techniques for investigating CO2 trapping petrochemical industry
mechanisms, which is an essential aspect of understanding and opti­
mizing sequestration processes. (Al-Shafi et al., 2023) published a Besides being in demand as fuel sources, hydrocarbons such as oil
comprehensive review on underground gas storage systems, with a and gas will continue to be in high demand as a feedstock for many
particular focus on the storage of CO2, H2, and CH4. Their work offers an chemical processes and industries (Galadima and Muraza, 2018; Grif­
excellent discussion of the various storage systems applicable to these fiths, 2019). The production of essential petrochemical building blocks
gases. However, they did not discuss the trapping mechanisms involved relies heavily on crude oil as a raw material, resulting in significant
in gas storage. amounts of CO2 emissions. These building blocks encompass, for
(Chen et al., 2023) conducted a review discussing the interfacial example, benzene, toluene, and xylene, which are used in the production
interactions between rock, brine, and CO2, focusing on saline aquifers. of products such as synthetic rubber, appliance moldings, tires, rubber
While their review provides valuable insights into these interactions, it gloves, etc. In addition, these chemical blocks serve as solvents in the
was limited to saline aquifers without considering other geological production of agricultural sprays, coatings, and adhesives and as raw
formations such as oil fields and coal seams. (Lu et al., 2023) reviewed materials in the production of essential substances such as dimethyl
the use of low-field nuclear magnetic resonance (NMR) in the charac­ terephthalate, phthalic anhydride, isophthalic acid, and terephthalic
terization of CO2 geological storage in shale gas reservoirs. Their work acid, which are involved in polymer synthesis (Oh and In, 2015; Omran
reviews an innovative approach to characterizing reservoirs for CO2 et al., 2017).
storage. However, it is highly specific to one aspect of monitoring The production of various types of plastics also depends on petro­
techniques, suggesting the potential for other review studies to explore chemicals, such as polyethylene, polypropylene, and polyvinyl chloride
other monitoring and assessment methods. (PVC) (Comaniţă et al., 2016). These plastics are then used in many
(Raza et al., 2015) conducted a review on the relationship between industrial products, from packaging and containers to automobiles. In
CO2 injectivity and capillary trapping for CO2 storage in depleted hy­ addition, various synthetic fibers, such as polyester, nylon, and acrylic,
drocarbon reservoirs. Their review is important for understanding fac­ can be produced from petrochemicals, which are then used to make a
tors affecting CO2 storage efficiency; however, it primarily addresses broad range of textiles involved in clothing, carpets, etc. (Haji et al.,
capillary trapping without extensively covering other trapping mecha­ 2021; Pohjakallio, 2020). Lubricants such as motor and gear oil are
nisms. (Sambo et al., 2020) reviewed the role of time-lapse (4D) seismic commonly derived from crude oil (Dalbey, 2001). These lubricants are
technology in monitoring reservoir changes during CO2 sequestration. used to reduce friction, wear, and heat in industrial machinery and
Their review provided valuable information on advanced monitoring equipment, extending their lifespan and minimizing energy losses
technologies. However, a gap exists in discussing non-seismic moni­ (Pownraj and Valan Arasu, 2021). In addition, crude oil is considered
toring techniques. the primary source of bitumen, which is widely used in road construc­
Compared to previous reviews, the novelty of this work includes tion and maintenance, as well as in waterproofing and insulation (Ishag
three main aspects: Obi et al., 2022). Table 1 provides the production chain of chemical
products originating from crude oil and gas as raw materials, contrib­
1. It provides a comprehensive discussion on CO2 trapping mechanisms uting significantly to global CO2 emissions.
and monitoring techniques while maintaining a balance between
depth and breadth of coverage. 2.2. The need for diverse CCUS methods
2. It clearly outlines the various experimental techniques used for
investigating CO2 trapping mechanisms, which have not been In addition to CO2 sequestration, there are other methods used to
addressed in previous reviews. reduce CO2 atmospheric release rates at an industrial scale, which
3. It proposes a qualitative assessment approach for understanding the include biological, thermochemical, electrochemical, and photochem­
applicability of various monitoring techniques at each stage of CO2 ical methods. These methods typically focus on (1) the non-conversion
sequestration projects. This innovative approach has not been re­ utilization of CO2 (i.e., direct CO2 utilization) and (2) the conversion
ported in previous studies. of CO2 into chemical products and energy carriers (Saravanan et al.,
2021; Yaashikaa et al., 2019; Zhu et al., 2020). Some of the processes
This work is organized as follows: Section 1 introduced the review, that are used in the biological conversion of CO2 are gas fermentation,
including review background, methodology, objectives, novelty, and anaerobic fermentation, enzymatic conversion, microbial electrosyn­
structure. Section 2 discusses the importance of CCUS during the energy thesis, CO2 reduction using cyanobacteria, and CO2 conversion using

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Table 1 industrial applications.

Production chain of chemical products originating from crude oil and gas. Data
source: (Canada Energy Regulator, 2018). 3. CO2 Tapping mechanisms in subsurface formations
Stage Main products/usage

1. Raw materials Crude oil and gas A variety of chemical and physical interactions affect the accumu­
2. Feedstock Butane, naphtha, condensate, natural gas, propane, lation and retention of CO2 in subsurface formations. In this section, we
and ethane present CO2 properties and discuss the main subsurface trapping
3. Basic chemicals Propylene, ethylene, butylene, ammonia, butadiene, mechanisms that lead to CO2 immobilization over time, progressing
methanol, and aromatics: benzene, toluene, and
xylene
from structural and stratigraphic trapping to residual trapping, solubi­
4. Chemical intermediates Styrene, ethylene glycol, isobutylene, acrylonitrile, lity trapping, and lastly mineral trapping, each contributing to the
(derivatives) glycerin, and others increased security of CO2 storage.
5. Final products Industrial chemicals, paint and coatings, synthetic
rubber, explosives, resins, foams, dyes, adhesives,
plastics, synthetic fibers, and soap and detergent 3.1. Physicochemical properties of CO2 and their impacts on subsurface
6. Final uses Clothing, packaging, appliances, vehicles, CO2 flow behavior
machinery, electronics, office equipment, industrial
equipment, pharmaceuticals, personal care,
consumer products, building materials, furniture, CO2 is a chemical compound containing one carbon atom bonded to
health care, and air and space materials two oxygen atoms through covalent double bonds (Deng et al., 2020). At
ambient conditions, CO2 exists in gaseous form, as indicated in Fig. 4.
Unlike water vapor, CO2 does not undergo condensation and precipi­
algae cultivation (Kondaveeti et al., 2020). tation processes under current climate temperatures (Lacis et al., 2010).
CO2 utilization encompasses several industrial applications, such as In the atmosphere, CO2 acts as a greenhouse gas due to its ability to
enhanced oil recovery (EOR) and urea production, with yearly con­ absorb infrared radiation (Garib, 2017). CO2 can dissolve in water.
sumption rates of 70–80 Mt. CO2 and 130 Mt. CO2, respectively. Other Therefore, it affects the properties lake water, seawater, groundwater,
applications include welding, metal fabrication, beverage and food etc., by tending to lower their pH levels. This occurs as CO2 reacts with
production, fire suppression, cooling and refrigeration, and plant growth H2O, resulting in the formation of carbonic acid (H2CO3), which is
stimulation. Furthermore, CO2 is widely used in the production of characterized as a weak acid. H2CO3 then splits up into HCO−3 and H+,
building materials, polymers, chemicals, and fuels (IEA, I.E.A, 2019). lowering the pH of water. When the atmospheric levels of CO2 increase
Table 2 provides an overview of CO2 utilization approaches for due to fossil fuel consumption, for instance, the additional dissolution of
CO2 leads to ocean acidification, which is irreversible over long time­
spans (Raven et al., 2005).
Table 2
Overview of direct and indirect CO2 utilization methods, their classifications, The CO2 phase diagram, shown in Fig. 4, also indicates that CO2
and associated industrial products/processes. Based on (Rafiee et al., 2018). exists as a supercritical fluid above the critical point, where the pressure
and temperature are above 73.9 bar and 304.2 K, respectively. When
Direct/indirect Classification Examples of products/
utilization processes CO2 is injected for the purpose of sequestration, it transitions from a
liquid to a supercritical state at depths beyond 800 m in the subsurface.
Direct utilization Physical methods (CO2 - Welding medium
(CO2 is directly part stays in its molecular form, - Solvents
This occurs because temperature increases significantly with depth
of the end product) either used in pure or mixed - Refrigerants within the Earth’s crust (Bachu, 2002). In oil reservoirs and saline
forms) - Fire extinguishers aquifers, the in-situ fluids, such as oil and water, are denser than CO2. As
- Dry ice (solid form of CO2) a result, CO2 ascends to the base of the caprock, which needs to remain
- Carbonated beverages
adequately impermeable to confine the buoyant fluid (Shukla et al.,
- Urea ((NH2)2CO)
- Syngas via dry reforming 2010). Table 3 provides additional physicochemical properties of CO2.
(CO2 + CH4 → 2CO + 2H2) One primary aspect of CO2 flow and trapping is miscibility, which
Chemical methods (CO2 - Salicylic acid (C7H6O3) must be considered when studying CO2 injection processes in subsurface
molecules are broken down - Polypropylene carbonate formations. Miscibility occurs when two fluids mix totally in all pro­
and transformed into other - Formic acid (HCOOH)
compounds) - Cyclic carbonate
portions as the interface between them diminishes (i.e., the interfacial
- Cetylsalicylic acid tension (IFT) reaches zero). Therefore, the two fluids form a single-phase
- Calcium carbonate
(CaCO3)
- Enhanced gas recovery
(EGR) for additional
natural gas production
Physical methods (CO2 - EOR for additional crude
stays in its molecular form, oil production
either used in pure or mixed - Power generation using
forms) supercritical CO2 cycle
- Polyurethane (polymer
units joined by urethane
links (—NH—(C=O)—
O—)
- Methanol (MeOH,
Chemical methods (CO2 CH3OH)
molecules are broken down - Fischer-Tropsch (F-T)
and transformed into other products (e.g., high-chain
compounds) hydrocarbons)
- Dimethyl ether (DME,
Indirect utilization CH3OCH3)
(CO2 enhances a - Dimethyl carbonate
process resulting in (DMC, (CH3O)2CO)
Fig. 4. CO2 pressure-temperature phase diagram. Modified from Witkowski
a product) - Algae fuel (e.g., biodiesel)
et al. (2014).

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Table 3 1994; Czernichowski-Lauriol et al., 2006; Gunter et al., 1996).

Main physicochemical properties of CO2. Data source: (Green and Southard, CO2 dissolution in porewater results in a pH decrease, leading to
2019). complex mineralogical reactions that occur in reservoir rock, fractures,
Property Value and caprock. These reactions, which result from interrelated thermo­
Molecular weight 44.01 g/mol
dynamic, kinetic, flow, and transport phenomena, can modify rock
Triple-point temperature 216.6 K (− 56.55 ◦ C) permeability and porosity, thereby impeding CO2 injection or facili­
Triple-point pressure 5.18 bar tating CO2 migration out of the storage region. For instance, CO2
Vapor pressure of liquid CO2 at 216.6 K (− 56.55 ◦ C) 5.18 bar injectivity might be increased due to the rapid dissolution of calcite in
Vapor pressure of liquid CO2 at 304.2 K (31.05 ◦ C) 73.84 bar
the proximity of the injection well. Conversely, flow pathways might be
Density of liquid CO2 at 216.6 K (− 56.55 ◦ C) 26.828 mol/dm3
Density of liquid CO2 at 304.2 K (31.05 ◦ C) 10.5600 mol/dm3 blocked due to rapid mineral precipitation, impeding the movement of
Heat of vaporization (ΔHv) of liquid CO2 at 216.6 K 1.52020 × 107 J/ CO2. Similarly, mineral dissolution in the caprock might create flow
(− 56.55 ◦ C) kmol pathways aiding CO2 migration, while a self-sealing phenomenon might
Heat of vaporization (ΔHv) of liquid CO2 at 304.2 K 0 J/kmol also occur, aiding CO2 containment. Such geochemical reactions are
(31.05 ◦ C)
Thermal conductivity of liquid CO2 at 216.6 K (− 56.55 ◦ C) 0.1769 W/(m•K)
highly reservoir-specific, depending on pressure and temperature (P-T)
Thermal conductivity of liquid CO2 at 300 K (26.85 ◦ C) 0.0754 W/(m•K) conditions, fluid chemistry, and rock mineralogy. These reactions are
Henry’s constant at 298.15 K (25 ◦ C) 1656.66 bar also highly time-dependent because of the different reaction kinetics.
Solubility in water at 293.15 K (20 ◦ C) and 1.013 bar 0.1688 g/100 cm3 Therefore, the geochemical changes affecting the petrophysical prop­
Solubility in water at 303.15 K (30 ◦ C) and 1.013 bar 0.1257 g/100 cm3
erties of reservoir rock, fractures, and caprock need to be evaluated, as
they significantly affect the storage longevity and security (Carroll et al.,
fluid (Karkevandi-Talkhooncheh et al., 2017). Under geological 2009; Czernichowski-Lauriol et al., 2006; Gunter et al., 1997; Michael
sequestration conditions, at depths exceeding 1000 m, CO2 and water et al., 2010).
(brine) are usually immiscible (Kuo et al., 2010). This immiscibility Upon the injection of CO2 in a subsurface reservoir, it forms a
means that CO2, upon injection, can migrate away from the injection site gaseous zone (or a bubble) surrounding the injection well (Fig. 5), dis­
due to its buoyancy and mobility relative to the brine (Sarris et al., placing the mobile water and/or oil both horizontally and vertically
2014). As a result, in the absence of hydrocarbons (e.g., oil and gas), CO2 within the injection region. As CO2 contacts the formation brine, CO2-
migration in subsurface reservoirs is governed by multiphase flow water interactions take place, initiating geochemical trapping processes.
physics (Kuo et al., 2010). The injection of CO2 will displace pore water In addition to these, there are other key processes involved in CO2
as CO2 migrates due to buoyancy and pressure gradients. With time, trapping within subsurface environments, as discussed in this section.
reservoir water starts to imbibe back into pore spaces following the
migration of the CO2 plume, leaving small, isolated CO2 blobs held in 3.3. Structural and stratigraphic trapping
place by capillary forces (Krevor et al., 2015).
On the other hand, CO2 and hydrocarbon fluids can be miscible Various subsurface geological features can physically preclude the
depending on the reservoir pressure. If the reservoir pressure is above lateral and upward migration of subsurface fluids. As shown in Fig. 6,
the minimum miscibility pressure (MMP), then CO2 and hydrocarbons subsurface formations resulting from geological deformations, such as
are miscible. In this case, CO2 tends to displace large amounts of the faults, may present a physical barrier against the free movement of CO2
existing fluids. Upon the continuation of the injection process, CO2 will toward the Earth’s surface. In addition to these, large-scale folds
occupy most of the pore spaces. In the immiscible case, more quantities comprising low permeability caprocks (i.e., seals) can prevent the
of the existing fluids are bypassed during CO2 injection compared to the migration of gaseous and supercritical CO2. Moreover, barriers pre­
miscible case. In most hydrocarbon reservoirs, the displacement process venting fluid movement can be naturally created through depositional
encompasses both miscible and immiscible mechanisms due to the and diagenetic processes, lending further support to the containment of
presence of hydrocarbons and water in the same pore space (Massarweh CO2 within specific reservoirs (He et al., 2016).
and Abushaikha, 2022; Skauge and Sorbie, 2014). Under immiscible In a fault system, structural trapping of fluids occurs due to a fault
conditions, the fluid saturation distribution and CO2 plume evolution intersecting a dipping zone of the reservoir, requiring both a sealing
are mainly governed by multiphase flow (Kopp et al., 2009; Sambo et al., caprock and a highly impermeable matrix within the fault structure
2020). (Szulczewski et al., 2013). According to (R. J. Knipe, 1997), there are
five main types of fault seals contributing to the structural storage of
reservoir fluids:
3.2. Role of CO2-water-rock geochemical interactions in controlling CO2
trapping mechanisms 1. Cataclastic fault rocks: These are formed from pure sandstones with
low clay content because of fracturing and frictional sliding of rock
The degree of interaction between CO2, porewater (i.e., formation grains, leading to a reduction in rock grain sizes and porosity. These
brine), and reservoir minerals may beneficially or deleteriously influ­ seals are typically categorized into deformation bands and granula­
ence CO2 injection processes, storage capacity, sealing effectiveness, and tion seams.
long-term stability and safety. In subsurface formations, CO2 can be 2. Juxtaposition seals: These seals are formed when a fault juxtaposes
trapped under different mechanisms, such as physical trapping, solubi­ lithologies or rock types of distinct capillary entry pressure and
lity trapping, ionic trapping, and mineral/chemical trapping. Physical permeability properties, such as shales and sandstones.
trapping typically involves supercritical CO2 bubbles captured inside the 3. Cement seals: These are formed due to mineral precipitation occur­
reservoir’s pore structure. In solubility trapping, CO2 dissolves in the ring within the fault zone, filling the pore spaces and blocking fluid
formation brine, contributing to chemical reactions occurring between flow.
CO2 and reservoir minerals. This, in turn, results in pH buffering, which 4. Phyllosilicate/framework fault rocks: These are created when a fault
enhances the extent of solubility trapping by forming dissolved bicar­ structure deforms impure sandstones containing sand grains
bonate ions (HCO−3 ) and complexes, a process referred to as ionic trap­ (framework grains) and clay minerals (phyllosilicates). This defor­
ping. In mineral trapping, dissolved CO2 may react with non‑carbonate mation process creates low-permeability regions within the fault
minerals that are rich in calcium (Ca), magnesium (Mg), or iron (Fe), region.
leading to the mineral immobilization of CO2 for extended geological
time periods in the form of solid carbonate precipitates (Bachu et al.,

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O. Massarweh and A.S. Abushaikha Earth-Science Reviews 253 (2024) 104793

Fig. 5. Variations in CO2 plume (gray) according to different permeability characteristics: (a) homogeneous low-permeability storage formation, (b) homogeneous
high-permeability storage formation, (c) homogeneous high-permeability media in a sloping aquifer, (d) heterogeneous permeability featuring continuous layers of
shale, and (e) heterogeneous permeability characterized by discontinuous lenses of shale. The injection interval situated in the lower half of the subsurface formation
is denoted by the black bar. Modified from (Espinet et al., 2013).

5. Clay smears: These are created when the faulting process deforms encompasses an impermeable seal of fine-grained rock, such as
clay units along the fault zone, which results in the formation of a mudstone or shale (Chen et al., 2011; Szulczewski et al., 2013). The
low-permeability clay layer along the plane of the fault. second type includes domes. These are convex-upward structures with a
cross-sectional geometry that can be circular or elliptical (Kuo et al.,
Similar to fault systems, folds represent primary geological features 2011; Scheffers et al., 2015).
with the capability of structural storage of CO2. Folds are mainly formed In structural trapping, CO2 injection leads to high pressure near the
by the deformation of ductile rock, resulting from compression stresses injection well, which then spreads and decreases over time. Peak pres­
induced by tectonic activity (Ju et al., 2022). The process of rock sures are always highest near the well, indicating a potential risk to its
deformation is strongly affected by subsurface temperature and litho­ structural integrity. Therefore, a caprock must exhibit low permeability
static pressures. When the temperature is low, rock deformation tends to to prevent long-term CO2 leakage. Additionally, it should have high
be brittle. Contrarily, high temperatures coupled with adequate compressive and tensile strengths to withstand changes in stress during
confining pressure result in ductile deformation, leading to the forma­ and after the injection process (Sarris et al., 2020; Sarris and Gravanis,
tion of fold-like structures. Furthermore, rock deformation behavior is 2019). The effectiveness of a caprock as a “barrier to flow” is determined
influenced by rock characteristics such as mineral composition, mineral by an essential property known as capillary threshold pressure. In two-
distribution, grain size, grain size distribution, degree of crystallinity, fluid systems, the flow of the non-wetting fluid through the pore space is
porosity, permeability, and the presence of interstitial fluids and their controlled by the surface tension between the two fluids. Therefore,
chemical composition (Gomez-Rivas et al., 2020). Two primary types of work (energy) is needed to disrupt the fluid-fluid interface, allowing for
folds can be used for CO2 storage. The first type includes anticlines, fluid flow. This energy is usually represented by the concept of capillary
which mostly have an upward convex shape, creating natural traps for threshold pressure (Pc), as given in Eq. 1 (Yielding, 2015):
fluids in sedimentary rocks. Typically, an anticline structure

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or outside structural and stratigraphic closures. Capillary trapping re­

quires the fluid to be the nonwetting phase in the reservoir system
(Hermanrud et al., 2009; Krevor et al., 2015). Unlike structural trapping,
the effectiveness of capillary trapping does not depend on the integrity
of the caprock (Saadatpoor et al., 2010). Fig. 7 presents the extent of
capillary trapping of CO2 following its injection below an impermeable
layer of rock.
Residual trapping of CO2 is affected by the characteristics of the
drainage (brine displacement by CO2) and imbibition (CO2 displacement
by brine) processes. During drainage, CO2 is initially pumped into the
brine-saturated reservoir rock until reaching the irreducible water
saturation and maximum CO2 saturation. Once irreducible water satu­
ration is reached, the imbibition cycle begins. During imbibition, brine
flows back into the pores until the relative permeability of CO2 is
reduced to zero. However, the presence of an irreducible water satura­
tion condition within the pore space of reservoir rock limits the available
space for CO2 storage. This means that conditions with lower irreducible
water saturation result in higher saturation of trapped CO2. The inter­
action between the wetting phase (e.g., brine) and the non-wetting
phase (e.g., CO2) in the rock pores follows the relationship Sw + Snw
= 1, where Sw and Snw represent the saturations of the wetting and non-
wetting phases, respectively. This interaction affects both the reservoir’s
capillary pressure and the relative permeability of each phase, which is
evaluated at their respective residual saturations (Li et al., 2017).
Several parameters determine the quantity of residual CO2 that is
trapped due to the capillary effect. These parameters include rock type,
wettability conditions, pore aspect ratio, pore geometry, hysteresis, and
the existence of impurities within the CO2 gas stream. Further param­
eters include CO2 viscosity, interfacial tension, and the initial saturation
of the oil and gas phases. Furthermore, the residual saturation of CO2
Fig. 6. Cases of structural trapping of CO2: (a) by a subsurface fault structure may be affected by formation porosity, pore pressure, flow rate, gravity
and (b) by an overlying impermeable seal rock in a fold system. number, capillary number, and coordination number. For instance, in
consolidated formations, the decrease in porosity leads to an increase in
2γ.cos θ the residual saturation of CO2 (Raza et al., 2015).
Pc = (1) (Alyafei and Blunt, 2016) studied a relationship between the initial
R
saturation of the non-wetting phase (Snwi) and its capillary trapping in
where γ is the fluid-fluid interfacial tension, θ is the substrate wettability water-wet porous media. It was found that residual saturation of the
in the two-fluid system, and R is the radius of the fluid droplet being non-wetting phase (Snwr) increases with the increase in Snwi. However,
pushed through the narrow spaces (pore-throats) in rocks. Therefore, the study by (Alyafei and Blunt, 2016) was limited to carbonate media
since there is an abrupt decrease in the radius of the pore throats when with a high calcite composition under specific temperature conditions.
moving from reservoir rock to caprock, the capillary threshold pressure Therefore, it may not fully capture the complexity of reservoir rocks.
will increase abruptly. Thus, future work in this field needs to investigate capillary trapping
The presence of capillary threshold pressure will halt buoyant fluids, under varied wettability and temperature conditions and across diverse
such as CO2, at the reservoir-caprock interface. This will lead to fluid rock compositions. (Tanino and Blunt, 2012) examined the capillary
accumulation beneath the caprock, inducing a buoyancy pressure (Pb), trapping of the non-wetting phase in carbonate and sandstone cores. It
as expressed in Eq. 2 (Yielding, 2015): was observed that Snwr decreases with the increase in porosity, regard­
( ) less of the rock type for given porosity values. It was also observed that
Pb = ρw –ρf .g.h (2) the extent of capillary trapping is not significantly affected by intra-
aggregate and intraparticle microporosity. It should be indicated,
where ρw and ρf represent the densities of water and the buoyant fluid,
however, that (Tanino and Blunt, 2012) conducted their experiments at
respectively, h denotes the height of the fluid column trapped beneath
ambient temperature and pressure. These conditions may not accurately
the caprock, and g denotes the gravitational acceleration. It can be
represent the high-pressure, high-temperature conditions found in sub­
inferred from Eq. 1 and Eq. 2 that CO2 remains safely stored as long as Pb
surface geological formations targeted for CO2 storage. Therefore,
< Pc. However, when Pb exceeds Pc (i.e., h exceeds hmax), the buoyancy
further work in this area is recommended. In an analytical study, (Blunt,
effect will force CO2 through the pore throats of the caprock. This will
2022) examined the effect of Ostwald ripening on the capillary trapping
lead to CO2 leakage toward the surface strata. Therefore, it is essential to
of gases stored in subsurface reservoirs. It was shown that Ostwald
continuously monitor the evolution of the CO2 column height
ripening plays an important role in the evolution of the gas configura­
throughout the sequestration processes to ensure effective structural
tion within porous media, redistributing gas ganglia. This, in turn, leads
trapping (Yielding, 2015).
to the establishment of a new state of gravity-capillary equilibrium. In
this case, the gas is trapped and confined to a narrow layer located
3.4. Capillary (residual) trapping of CO2 beneath a mobile gas region in the storage reservoir. One limitation of
the study by (Blunt, 2022) is that it ignored mineralization, which could
Capillary trapping occurs when the buoyancy of CO2 is not sufficient play an important role in the long-term sequestration of CO2. Moreover,
to surpass the capillary entry pressure within the pore throats of the the study assumed the aqueous phase was not flowing; therefore,
reservoir rock, preventing its entry into adjacent upper pores. This convective dissolution was not investigated. Additionally, it was
subsequently enables CO2 storage at high saturations at locations below assumed that small concentration gradients had no effect on reaction

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Fig. 7. Capillary (residual) trapping of CO2 subsurface formations. Modified from (Krevor et al., 2015).

rates. Such assumptions present areas for further investigation in future 3.5. Solubility trapping of CO2
studies.
To study CO2 capillary trapping, (Akbarabadi and Piri, 2013) con­ Upon injection into a subsurface reservoir, part of the injected CO2
ducted 30 steady- and unsteady-state draining and imbibition experi­ dissolves in the reservoir brine in the form of different species, such as
ments in Nugget and Berea sandstones of various permeabilities. They CO2−3 (aq), HCO3 (aq), and CO2 (aq), preventing any CO2 leakage as a
−

showed that ~49–83% of the initial CO2 saturation could be trapped in discrete phase. In this context, the notation CO2 (aq) represents the total
rock due to capillary trapping. The study reported by (Akbarabadi and amount of the electrically neutral dissolved forms of CO2 in water,
Piri, 2013) is valuable for determining the initial and residual CO2 including H2CO3 (aq). The kinetics of CO2 dissolution vary depending on
saturation levels achievable under laboratory conditions. However, the different factors. CO2 dissolution in the form of CO2 (aq) is relatively fast
use of these results to predict long-term, field-scale CO2 storage capacity compared to the formation of HCO−3 , which is affected by the rate of
and behavior can be challenging due to the complexity of subsurface release of cations (e.g., K+, Na+, and Ca2+) through mineral dissolution.
reservoirs. Factors such as high heterogeneity, fractures, and varying This release of cations helps neutralize H2CO3, enabling further disso­
rock types contribute to this complexity and should be considered in ciation to occur. Additionally, the extent of CO2 dissolution in the
future research. (Ni et al., 2019) carried out a study involving core reservoir brine may be affected by factors such as reservoir permeability
flooding experiments on nine sandstone core samples of various het­ and porosity, CO2 flow rate within the reservoir, and the effective
erogeneities. It was found that the residual trapping of CO2 increases as diffusion coefficients of the species under reaction (Balashov et al.,
the degree of rock heterogeneity increases, whereas it decreases with an 2013). In addition to that, the solubility of CO2 is influenced by brine
increase in porosity. The experimental results reported by (Ni et al., salinity and reservoir temperature. As the salinity and temperature in­
2019) reveal the potential impact of reservoir petrophysical properties crease, CO2 solubility decreases. Furthermore, at the initial interaction
on the capillary trapping capacity in sandstone formations. However, between CO2 and reservoir brine, the rate of CO2 dissolution is rapid.
applying these results to actual field conditions and other rock types However, once the reservoir brine becomes saturated with CO2, the
requires further research. This involves conducting more core-flooding dissolution rate drops significantly, which is subsequently controlled by
experiments with varying rock types to increase the accuracy of the diffusion and convection processes. The following chemical reaction
models used for predicting CO2 trapping in subsurface formations. A (Eq. 3) represents the dissolution of CO2 in reservoir brine (Benson et al.,
further in-depth discussion on the experimental aspects of evaluating 2005):
and monitoring CO2 trapping is presented later in this review.
CO2 (g) + H2 O ↔ H2 CO3 ↔ HCO3 − + H+ ↔ CO3 2− + 2H+ (3)
CO2 dissolving in the aqueous phase produces a weak acid that reacts
with Na and K basic silicates or with Ca, Mg, and Fe carbonate/silicate

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O. Massarweh and A.S. Abushaikha Earth-Science Reviews 253 (2024) 104793

minerals in the reservoir. This results in the formation of bicarbonate lithologies under consideration. These reactions are also affected by the
ions (HCO−3 ) according to the following reaction (Eq. 4) (Benson et al., pH, reservoir pressure, reservoir temperature, and ionic concentration of
2005): the different involved species. When large quantities of dry supercritical
CO2 (scCO2) flow through the reservoir, direct contact may occur be­
3 K − feldspar + 2H2 O + 2CO2 ↔ Muscovite + 6 Quartz + 2 K+ + 2HCO3 −
tween the rock and dry scCO2, leading to slow mineral dissolution.
(4) Subsequently, significant mineral trapping may occur over long
It is worth mentioning that the time required for the occurrence of geological periods (Schaef et al., 2011; Zhang and Song, 2014). As
CO2-mineral reactions varies depending on the type of reservoir mineral shown in Fig. 8, the various trapping mechanisms provide different
involved, taking days for certain carbonate minerals and hundreds to extents of storage security. Among these mechanisms, mineral trapping
thousands of years for silicate minerals. Solubility trapping offers two offers the most secure form of CO2 storage. However, the kinetics of
main benefits with regard to CO2 subsurface storage. Firstly, as CO2 mineral trapping processes are slow, extending over centuries to
dissolves in reservoir brine, it is no longer present as a separate phase, millennia.
which eliminates the buoyancy effects that drive CO2 upward. Secondly,
the aqueous solubility of CO2 contributes to the formation of ionic 4. Evaluation and monitoring of CO2 trapping in CCS projects
species, leading to a pH decrease, where a fraction of the dissolved CO2
is converted into stable mineral forms, such as carbonate minerals (Metz CCS projects typically involve a sequence of iterative steps aimed at
et al., 2005). assessing the feasibility and effectiveness of geological CO2 sequestra­
tion operations, encompassing activities such as site characterization,
3.6. Mineral trapping of CO2 modelling and simulation, risk assessment, and MVA (monitoring,
verification, and accounting), as shown in Fig. 9. This section presents
Mineral trapping is related to solubility trapping. Mineral trapping current and emerging methods used to evaluate the potential for CO2
occurs when the CO2 dissolved during solubility trapping changes into sequestration before CO2 is injected into subsurface formations. Addi­
stable mineral forms through reactions with organic and mineral ma­ tionally, it discusses the methods used to monitor the effectiveness and
terials existing in the subsurface environment (Mat Razali et al., 2022). progress of CO2 injection processes after the injection has occurred. It is
Examples of common mineral reactions are given in Table 4. While some noteworthy that these methods are often interrelated; therefore, it is
of these reactions may increase the tendency for CO2 trapping, such as important to discuss them together.
the reactions resulting in the formation of carbonate minerals, others
might be deleterious, leading to further CO2 migration (Zhang and Song, 4.1. Seismic and borehole geophysical techniques for CO2 trapping
2014). monitoring
Mineral reactions can be described as competing processes that are
highly influenced by the mineralogy, structure, and hydrogeology of the Seismic studies are used as a robust tool for evaluating and moni­
toring geophysical sequestration/trapping of CO2 within subsurface
Table 4 structures. Geophysical monitoring is employed at different stages of
Common water-CO2-mineral reactions in subsurface reservoirs (Espinoza et al., CO2 sequestration projects. First, prior to CO2 injection, baseline (pre-
2011). injection) monitoring is carried out to collect site-specific data, allowing
for predicting geological and geochemical trends during the potential
Minerals Reaction equations Remarks
CO2 injection (Ma et al., 2016; Myrttinen et al., 2012). Then, injection
• Rate of reaction = 1.26 ×
monitoring is performed during the actual CO2 injection. Next, after the
10− 14 mol.m− 2 s− 1.
• SiO2(s) + 2H2O ↔ H4SiO4
• There is no change in quartz
Silicates ↔ H+ + H3SiO−4 ↔ H+ +
solubility as the
H2SiO2−4
concentration of dissolved
CO2 increases.
• Rate of reaction for calcite =
1.6–3.2 × 10− 5 mol.m− 2 s− 1.
• CaCO3(s) + H+ ↔ Ca2+ +
• Solubility is influenced by
HCO−3 (Keq = 101.85)
temperature, pressure, ionic
• CaCO3(s) + CO2 + H2O ↔
concentration, salinity, and
Ca2+ + 2HCO−3 (Keq =
Carbonates pH.
10–4.5)
• The rate of dissolution is
• CaCO3(s) + H2O ↔ Ca2+ +
rapid. However, the total
HCO−3 + OH− (Keq =
amount of reaction is small.
10–8.48)
• It leads to a pH range of 3 to
5.
• Slower than carbonates.
• Rate of reaction for Kaolinite
= 10− 14 − 10− 15 mol.m− 2
s− 1.
• Rate of reaction for
Anorthite = 1.2 × 10− 5 mol.
• Kaolinite: Al2Si2O5(OH)4
3+ m− 2 s− 1.
(s) + 6H ↔ 2Al
+
+
• Rate of reaction for
2H4SiO4 + H2O (Keq =
Oligoclase = 1.2 × 10− 8 mol.
Aluminosilicates 103.8)
m− 2 s− 1.
• Anorthite: CaAl2Si2O8(s) +
• Rate of reaction for Albite =
8H+ ↔ Ca2+ + 2Al3+ +
3.6 × 10− 9 mol.m− 2 s− 1.
2H4SiO4 (Keq = 1021.7)
• It comprises feldspars, clays,
and micas.
• It yields a higher quantity of
dissolved cations compared
to carbonate.
Fig. 8. Performance of various CO2 trapping mechanisms. Modified from
• It leads to a pH of up to 8
(Benson et al., 2005).

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measurements provide information on the composition and micro­

structure of the rock matrix and the distribution of pore fluids. These
measurements facilitate the determination of material types based on
density and strength characteristics (Glover, 2000). Downhole pressure
measurements are utilized to define reservoir boundaries, determine
average reservoir properties, and monitor reservoir response during
injection processes (Jackson et al., 2024; Sakai et al., 2024). Pressure
transients taken at a single depth can be employed in CCS for both site
characterization and monitoring (Jenkins et al., 2024; Nagao et al.,
2024). Research indicates that pressure in injection and monitoring
wells responds rapidly to variations in CO2 injection. When CO2 reaches
the monitoring well and displaces the brine beneath the packer, a sharp
increase in pressure is observed (Strandli and Benson, 2013).
In addition to monitoring CO2 plume evolution, it is important to
monitor CO2 leakage from CO2 sequestration sites. An effective method
for this is shallow groundwater monitoring, which assesses the impact of
CO2 leakage on groundwater quality. According to (Keating et al., 2010,
2013), shallow groundwater monitoring usually involves conducting
field observations, collecting samples, and performing subsequent lab­
oratory analyses to identify geochemical changes induced by elevated
CO2 levels. Field-scale reactive-transport simulations are then developed
to predict scenarios where CO2 leakage might occur and assess its impact
on groundwater chemistry. These simulations use data derived from
experimental analyses of water samples, focusing on variables such as
Fig. 9. Illustration of iterative and interconnected elements of typical CO2 pH levels, trace element mobility, and overall water quality changes
sequestration projects. Modified from (Gorecki et al., 2012).
resulting from the interaction between CO2 and shallow groundwater.
The integration of field data and modelling ensures that any changes in
injection phase, the storage site is sealed, where post-closure monitoring groundwater quality are detected early and managed effectively, thus
is implemented over long time periods, aiming to evaluate the safety and preventing environmental risks associated with CO2 leakage in CCS
security of CO2 storage. During the post-closure stage, seismic moni­ projects. In addition to groundwater monitoring, it is essential to
toring emerges as the most effective method to assess the effectiveness of monitor the surrounding atmosphere near CO2 sequestration sites. In
CO2 sequestration (Ma et al., 2016). this regard, Subsection 4.2 discusses the different methods and systems
Seismic monitoring employs various techniques that are based on 4D used for atmospheric monitoring of CO2 storage.
(four-dimensional) seismic technology (Sambo et al., 2020). Examples
of these techniques include 4D–3C (4-dimensional and 3-component) 4.2. Atmospheric monitoring methods for CO2 storage
seismic methods, 4D-3C-VSP (4-dimensional, 3-component vertical
seismic profiling), 4D–9C (4-dimensional and 9-component) seismic There is a growing public concern over the potential for CO2
techniques, cross-well seismic tomography, and passive seismic moni­ migration from subsurface CO2 storage sites to the atmosphere. Atmo­
toring (Bjorn N. P. Paulsson, 2006; Hovorka et al., 2006; Ma et al., 2016; spheric monitoring tools are used to check for any leakage following CO2
Verdon et al., 2010; Yamamoto et al., 2004). injection into subsurface formations (Ajayi et al., 2019; Zahid et al.,
4D time-lapse seismic monitoring is a process that takes a long period 2011). Due to the quick spreading and dilution of the leaked CO2 into
of time. During this process, variations in travel time and amplitude the surrounding atmosphere, these tools need to be highly sensitive,
within the reservoir are recorded and then compared to baseline (pre- detecting minute fluctuations in atmospheric CO2 concentrations. To
injection) seismic data. Subsequently, the horizontal and vertical evo­ increase their detection effectiveness, atmospheric monitoring tools are
lution of the CO2 plume is estimated using seismic data processing (Al typically deployed at potential CO2 leakage points (Plasynski et al.,
Hosni et al., 2016; Eiken et al., 2011; White, 2013). Recently, several 2011). Usually, atmospheric monitoring of CO2 storage involves the
projects have successfully used 4D seismic technologies to monitor CO2 utilization of various methods and systems, such as optical sensors (Sun
sequestration in Australia, Canada, the European Union, Norway, and et al., 2021), atmospheric tracers (Watson and Sullivan, 2012), eddy
the United States. Globally, most CO2 sequestration projects use seismic covariance devices (Jiemin Wang et al., 2015), advanced leak detection
studies, such as baseline seismic monitoring and seismic surveys, to systems (Plasynski et al., 2011), and flux champers (Myers et al., 2020).
evaluate the suitability of prospective storage sites (Ma et al., 2016). Table 6 provides an overview of the main methods and systems utilized
Borehole geophysical monitoring techniques are also used to assess for atmospheric monitoring of geologically stored CO2.
geological CO2 trapping in subsurface reservoirs. For instance, time- Flux chambers are commonly used to monitor the CO2 flowing to­
lapse well logging is implemented to monitor the saturation of CO2, ward the atmosphere from source areas that are <1 m2. Depending on
oil, and water during miscible CO2 injection for EOR purposes, utilizing the chamber type, the flux (Fc) is calculated in two different ways
neutron and induction resistivity logs (Xue et al., 2006). An overview of (Leuning et al., 2008). In flow-through chambers, Eq. 5 is used:
the application of seismic and borehole geophysical methods for moni­
toring CO2 trapping is provided in Table 5. FC =
W
(Cc0 –Cci ) (5)
Sonic logging is one of the well logging tools used to monitor sub­ A
surface changes resulting from CO2 injection as CO2 replaces formation
where W is the flow rate of air, A is the chamber’s basal area, and (Cc0 –
fluids (e.g., water) (Ajo-Franklin et al., 2013; Freifeld et al., 2009; Xue
Cci) is the difference in the concentration of gas between the outlet and
et al., 2006). Sonic logs measure the travel time of elastic waves, pri­
inlet of the chamber. On the other hand, in accumulation chambers, Eq.
marily P-waves and S-waves, through geological formations to deter­
6 is used:
mine wave velocity. Data from sonic logging are used to identify various
geological features, including formation porosity, facies, fractures, V ∂Cc
FC = (6)
compaction, over-pressures, and source rocks. Furthermore, sonic A ∂t

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Table 5
Case studies on field application of seismic and borehole geophysical methods for monitoring CO2 trapping.
Reference Formation Formation/site remarks Main CO2 monitoring Main findings
technique(s)

- Midale Marly dolostone (ϕavg. = 27%, k

= 1–50 mD) and Midale Vuggy
limestone (ϕavg. = 10%, k = 10–300 - The CO2 plume could be tracked seismically.
mD). - Time-lapse signal was not significantly affected
- Weyburn Field, - Impermeable seal of Midale Evaporite - 3D time-lapse seismic by changes in the reservoir pressure.
(White, 2013)
Saskatchewan, Canada (anhydrite, ϕ = 0.2%, k = 0.01–0.4 μD). monitoring. - The detected seismic response due to CO2
- Reservoir pore pressures = ~14 MPa injection was affected by the injection schemes
(upon discovery). and lateral heterogeneity.
- Reservoir pressure during waterflooding
= 8–19 MPa.
- Sandstone formation.
- Depth of the injection interval = - Inverted acoustic impedance values strongly
- Tuscaloosa Formation - 3D time-lapse seismic
(Zhang et al., 3012–3142 m. agree with measurements from well logging
at Cranfield, monitoring
2013) - ϕavg. of the gas cap and oil zone is pertaining to CO2 saturations, providing high-
Mississippi, USA - Well logging.
~20%. resolution images of the CO2 plume.
- kavg. = 280 mD.
- 2D and 3D VSP seismic
- Deep depleted gas reservoir surrounded - Seismic monitoring could be effectively used to
(Urosevic et al., monitoring.
- Naylor Field, Australia by complex fault system. monitor and verify the storage of CO2 in depleted
2010) - Time-lapse 3D surface
- The reservoir is thin and heterogeneous. gas reservoirs.
seismic monitoring.
- The decrease in P-wave velocity indicated the
distribution of CO2 in the vicinity of the injection
(Saito et al., - Nagaoka test site, - Onshore aquifer. - Time-lapse cross-well well.
2006) Japan - Thin permeable sandstone layer. seismic tomography. - Seismic tomography is an effective method to
monitor the progress of CO2 geological
sequestration.
- Gas accumulating within sand layers (~ - FWI could be used to quantify free CO2 in
- Seismic monitoring of CO2
(Queißer and - Sleipner Field, North 10 m). subsurface sequestration.
utilizing time-lapse 2D full
Singh, 2010) Sea, Norway - The seal against buoyant CO2 comprises - Saline aquifers could be used as natural reservoirs
waveform inversion (FWI).
shale beds of several meters. for the storage of CO2.
- Saline aquifer (620–650 m depth)
- 3D time-lapse seismic - Field data can be used to monitor the distribution
- Sandstone porous media.
monitoring. of the injected CO2.
- Extreme permeability and porosity
- Pulsed neutron-gamma - Time-lapse seismic measurements, petrophysical
(Ivanova et al., - Stuttgart Formation, heterogeneity.
(PNG) well logging. experiments, and PNG measurements can be used
2012) Ketzin, Germany - The top seal of the formation is the
- Petrophysical laboratory to quantify the amounts of injected CO2 into the
Triassic Weser Formation, which
experiments on core formation and determine the saturation values of
consists mainly of clayey siltstone, a
samples. CO2.
thick anhydrite layer, and mudstone.
- Sandstone porous media.
- Reservoir depth ranges from 1409 m to - Seismic monitoring and well logging may be used
(Ma et al.,
1661 m. to study reservoir heterogeneities, detect CO2
2013) - Jingbian Field, North of - 4D seismic monitoring.
- ϕ = 9–13%. plume behavior, assess borehole integrity,
(Ma et al., Shaanxi, China - Time-lapse well logging.
- k = 0.5–3.5 mD. identify CO2 leakage, determine the best injection
2014)
- Reservoir temperature = 40 ◦ C. schemes, and evaluate the efficiency of CO2-EOR.
- Reservoir pressure = 12 MPa.
- Wireline logging/sampling provided subsurface
- Carboniferous sandstone reservoir. characteristics, which were used in geochemical
- Wireline logging/sampling.
- Reservoir depth ranges from 1850 m to and geomechanical modelling.
(Mathieson - In Salah site, Krechba, - Repeat 3D seismic
1950 m. - Repeat 3d seismic was used to study subsurface
et al., 2011) Algeria monitoring.
- ϕ = 10–18%. characteristics and CO2 plume migration.
- Microseismic.
- kavg. = 10 mD. - Microseismic was used to monitor CO2 leakage
and caprock integrity.
- High-resolution images of CO2 distribution could
- Sealed saline aquifer that is part of a be obtained by measuring the P-wave velocity.
(Daley et al., - Frio formation, sandstone formation. - Cross-well and VSP seismic - The extent of the CO2 plume from a monitoring
2008) Houston, Texas, USA - Downhole pressure = 15 MPa. monitoring. well in three directions could be estimated from
- Downhole temperature = 55 ◦ C. the change in the amplitude of the seismic
reflection induced by CO2 injection.
- Bottom-hole pressure
- Time-lapse well logging could be used to evaluate
monitoring.
the progress of residual and solubility trapping of
- Formation pressure
CO2.
monitoring.
- CO2 could be safely stored in sandstone porous
- Nagaoka test site, - Neutron logging yields
(Mito and Xue, - Saline aquifer. media.
Pleistocene Haizume porosity data.
2011) - Sandstone porous media. - Well logging could be used to monitor the
formation, Japan - Sonic logging acquires P-
draining process.
and S-wave velocity.
- The draining process continued to take place
- Induction logging acquires
during the CO2 injection stage and during the
data on formation
early post-injection phase.
resistivity.
- Sandstones (ϕ = 25%–35%, k = - PNLs could be used to monitor changes in CO2
- Bell Creek oil field,
(Braunberger 150–1175 mD). - Time-lapse pulsed-neutron and oil saturation within the reservoir.
southeastern Montana,
et al., 2014) - Initial reservoir pressure = 1200 psi logs (PNLs) - Time-lapse monitoring was successfully used to
USA
(8.27 MPa) study the movement of the CO2 plume within the
(continued on next page)

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Table 5 (continued )
Reference Formation Formation/site remarks Main CO2 monitoring Main findings
technique(s)

reservoir. In addition, it could be used to evaluate

flow boundaries, storage potential, and sweep
efficiency.

Table 6
Overview of different methods and systems used for atmospheric monitoring of CO2 storage. Modified from (Srivastava et al., 2008).
Monitoring Description Advantages Challenges
method/system

- Moderate costs
- A method that is based on the measurement of atmospheric - Mature technology.
Atmospheric eddy - Necessitates specialized equipment and
flux, aimed to determine the atmospheric concentrations of - High accuracy of data.
covariance data processing.
CO2 at given heights above the Earth’s surface - Allows for continuous operation.
- “Signal to noise” challenge
- Capable of covering large areas.
Advanced leak - Monitoring is carried out by terrestrial vehicles or aircraft - Portable - Maintaining repeatability under
detection utilizing sensitive three-gas detectors (CO2, CH4, and total - The use of multiple gases allows for the variable seasonality and during diurnal
systems HC) and GPS mapping technology. acquisition of process-related information, variations is a key challenge.
facilitating the interpretation of changes.
- Inexpensive compared to other techniques.
- Portable
- Detecting CO2 leakage above ambient
- Incorporate mature and new technologies,
CO2 detectors - CO2 sensors utilized continuously or intermittently in air levels of CO2 is challenging.
providing diverse options.
- “Signal to noise” challenge
- Used in confined spaces to ensure worker
safety.
- Open-path devices that utilize laser technology to produce
- High accuracy - High cost
Laser systems a beam according to the wavelength absorbed by CO2
- Wide spatial coverage range. - “Signal to noise” challenge
molecules, covering many meters.
- Relatively inexpensive
- A device utilized to measure soil CO2 flux, providing data
Flux accumulation - Mature technology. - Limited to instantaneous
that can be correlated with soil gas geochemical
chamber - A quick and effective tool for measuring soil measurements and small areas.
characterization.
CO2 flux at a defined area.

where V is the chamber’s volume, A is the chamber’s basal area, (∂Cc/∂t) control, batteries, wireless communication systems, and embedded
the rate of change in the concentration of gas in the chamber. computers for system control. Fig. 10 shows a schematic of a flux
Modern flux chambers typically contain electronic components for chamber that was installed at the Otway CO2 Sequestration Project in
system control. They are also equipped with different sensors for Australia. In that project, a flux chamber system was utilized to
monitoring humidity, pressure, and temperature. In addition, modern continuously measure CO2 flux at a depth of ~1.3 m, providing more
flux chambers contain sensors for measuring CO2 concentrations over sensitive and useful data compared to single-point measurements of CO2
wide ranges (e.g., 2000 ppm to 200,000 ppm), GPS receivers for time concentrations. Furthermore, the system was found to be effective for
monitoring near-surface CO2 concentrations, considering public regu­
lations that aim to protect the environment from CO2 seepage resulting
from subsurface CO2 sequestration sites (Bernardo and Vries, 2011).
One main challenge with the use of flux chambers for measuring
near-surface CO2 concentration is the variability in background con­
centration resulting from changes in soil moisture and temperature,
atmospheric variations in temperature, pressure, and wind speed,
diurnal variations, and the influences of biological activities, including
photosynthesis, leaf and root respiration, and microbial processes
(Hirsch et al., 2004; Loisy et al., 2013; Al Makky et al., 2017; Velasco
et al., 2021). Therefore, to accurately measure CO2 leakage, the mea­
surement process needs to be properly designed to account for natural
CO2 sources and sinks (Leuning et al., 2008).
While flux chambers are used for measuring local near-surface CO2
flux, eddy covariance (EC) systems are used to measure surface fluxes
over large spatial extents (Cortis et al., 2008; Jones et al., 2014;
McDaniel et al., 2017). These systems are used to measure atmospheric
fluxes of CO2, water vapor (H2O), latent heat (λET), and sensible heat
(H), which are transferred in the atmosphere in the form of rotating
eddies of various sizes, resulting from atmospheric turbulences
(Babaeian and Tuller, 2023). Physically, the EC method quantifies the
molecules ascending and descending in the atmosphere and their travel
speed over time. Mathematically, the EC method employs a covariance
between the vertical velocity measurements, the upward and downward
Fig. 10. Schematic of a flux chamber installed at Otway CO2 geo-sequestration motions of air, and the concentration of the specific gas/entity under
site in Australia. Modified from (Bernardo and Vries, 2011).

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O. Massarweh and A.S. Abushaikha Earth-Science Reviews 253 (2024) 104793

Fig. 11. Illustration of the fundamental concept behind the measurement procedure used in the eddy covariance (EC) method. Modified from (Burba, 2013).

study (Baldocchi, 2014; Dupont et al., 2021; Li et al., 2021).

Table 7
Fig. 11 illustrates the fundamental measurement concept of the EC
Factors affecting the accuracy and resolution of CO2 flux maps produced
method. At a given moment (time1), air parcel c1 is moved down by
employing the EC method.
eddy1 at the speed v1. Then, at time2, at the same point, air parcel c2 is
moved up by eddy2 at the speed v2. Each of these air parcels is charac­ Factors Comments References

terized by its distinct humidity, temperature, gas concentration, etc. Atmospheric - Several components affect CO2 (Grace et al., 1996;
Upon measuring the characteristics of each air parcel at the vertical conditions flux measurements, such as: Man et al., 2021;
• Atmospheric CO2 Rebmann et al., 2018)
speed (v), the vertical upward and downward fluxes of humidity, tem­
concentration
perature, and gas concentrations can be determined. For instance, if at • Wind speed and direction
time1, three CO2 molecules moved upward, and at time2, only two CO2 • Precipitation
molecules moved downward, then the direction of the net flux is upward • Temperature
with a quantity of one CO2 molecule (Burba, 2013). • Radiation
Surface heterogeneity - Several components affect CO2 (Lees et al., 2018)
Recently, the EC method has been employed by major entities, such and terrain flux measurements, such as:
as the U.S. Department of Energy (DOE) and the International Panel on complexity • Vegetation
Climate Change (IPPC). This included detecting and quantifying CO2 • Soil type
leakage from CCS sites as a part of storage efficiency evaluation. Modern • Topography and terrain
features
EC stations can now be automatically utilized to measure CO2 emissions
Measurement height - The measurement height (Velasco and Roth,
from storage areas directly. The emission values are typically reported as significantly affects CO2 2010)
CO2 gas (volume or weight) per unit area per unit time (Burba et al., concentrations, sources, and
2013). sinks.
In a study reported by (Koopmans et al., 2021), eddy covariance was Instrumentation - The accuracy of measurements (Baldocchi et al.,
can be affected by the quality 1996)
employed to quantify sub-seafloor CO2 emissions resulting from and configuration of EC
controlled CO2 injection into the North Sea. This was achieved by instruments.
measuring water velocity and pH as influenced by CO2 injection at rates Length of averaging - Random sampling errors are (Baldocchi, 2003)
ranging from 5.7 to 143 kg/day at a depth of three meters below the periods reduced when CO2 flux
measurements are averaged
seafloor. Prior to CO2 injection, the proton flux resulting from the nat­
over longer periods (e.g., days
ural mineralization of organic matter in the benthic zone of the sea was to a year).
quantified, indicating a flux value of 7.6 ± 3.3 mmol /(m2⋅day) of dis­ Number of EC stations - As the number of EC stations (Lewicki and Hilley,
solved inorganic carbon. Upon injecting CO2 at the lowest injection rate, increases, the resolution of the 2012)
the proton flux due to the dissolution of CO2 was 20 times higher than CO2 flux map improves;
however, this leads to
the naturally occurring proton flux. At the highest injection rate, while
increased monitoring costs.
accounting for the kinetics of the carbonate system, the emitted CO2 Data processing - Different post-field data pro­ (Massman and Lee,
represented 73 ± 13% of the injected CO2. However, neglecting the approach cessing approaches can influ­ 2002; Mauder and
kinetics, the calculated emitted CO2 was 1/5 of that amount. Based on ence eddy covariance flux Foken, 2006)
estimates.
that, the study by (Koopmans et al., 2021) highlights that pH eddy
Spatial distribution of - EC stations need to be (Post et al., 2015;
covariance can quantify small natural and abiotic seafloor CO2 emis­ EC stations distributed appropriately to Zhuang et al., 2022)
sions, which is highly important for monitoring CO2 sequestration in capture the spatial variability
offshore geological formations. of CO2 fluxes.
Several factors affect the accuracy and resolution of the CO2 flux
maps produced using the EC method, as detailed in Table 7. These fac­
variations in gas concentrations at a high frequency to obtain accurate
tors include atmospheric conditions, surface heterogeneity, terrain
flux estimates utilizing the EC method, especially in turbulent condi­
complexity, measurement height, and instrumentation. Additionally,
tions. This is usually achieved using ultrasonic anemometers and high-
these factors include the data processing approach, the number of EC
frequency gas analyzers. Additionally, flux data must include informa­
stations, and the distribution of the EC stations relative to the source of
tion on surrounding environmental conditions, such as radiation,
the leakage signal (Aubinet et al., 2012; Baldocchi et al., 1996; Goulden
moisture, air pressure, and air temperature, which are required to cor­
et al., 1996; Lewicki and Hilley, 2012; Massman and Lee, 2002; Ver­
rect the measured fluxes precisely.
oustraete et al., 2002; Wang et al., 2010). According to (Rebmann et al.,
2018), the wind speed needs to be measured simultaneously with the

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4.3. Experimental techniques for investigating CO2 trapping mechanisms micro-computed tomography (micro-CT) (Soong et al., 2014; Zhang
et al., 2019), and Laser-induced fluorescence (De et al., 2021; Zhang
4.3.1. Petrophysical characterization et al., 2020).
Petrophysics is the scientific study of rock properties and the in­
teractions between rock and fluids (aqueous solutions, gases, and liquid 4.3.2.1. Microfluidic flow visualization. In a notable study conducted by
hydrocarbons) (Sikiru, 2021; Tiab and Donaldson, 2016). Petrophysical (Sell et al., 2013), CO2 diffusivity was evaluated following a microfluidic
data is essential to estimate CO2 storage potential and simulate and approach aimed at predicting CO2 security in subsurface storage. In that
monitor CO2 injection, flow, and storage in subsurface reservoirs (Har­ experimental study, microfluidic chips were prepared from PMMA (poly
bert et al., 2016; Liu and Grana, 2020). Petrophysical data is commonly (methyl methacrylate)). The chips were composed of two pieces, each
obtained using routine core analysis (RCAL) and special core analysis measuring 25 × 25 × 3 mm in dimension. A schematic of the flow
(SCAL). RCAL involves the evaluation of rock porosity, rock perme­ process in the microfluidic system is presented in Fig. 12. Firstly, the
ability, grain density, and fluid saturation. SCAL, on the other hand, chip is filled with a fluorescent solution to visualize the flow. Then, with
examines properties such as relative permeability, wettability, capillary the purge valve open, pure CO2 begins to flow into the chip. The flow
pressure, and electrical properties (Alyafei, 2021; Worden et al., 2018). process through the fluidic resistor forces the CO2 and liquid out through
According to (AlRassas et al., 2022), the static CO2 storage capacity the purge valve. Upon closing the purge valve, the confining pressure
(MCO2 ) in Mt. units can be estimated using the following equation (Eq. immobilizes the interfaces. During this procedure, the diffusion process
7): is visualized utilizing a fluorescence microscope at the specified
location.
MCO2 = φ × havg. × A × E × ρCO2 × B × (1–Swiir ) (7)
The microfluidic flow visualization approach demonstrated by (Sell
et al., 2013) provides some advantages for the study of CO2 diffusivity.
where φ is the porosity (%) of the injection site, havg. is the average
Microfluidic chips allow for studying the effects of salinity and pressure
thickness (m) of the layer, A is the trap area (m2), E is the capacity co­
efficient, ρCO2 is the density (kg/m3) of CO2, B is the formation volume on the diffusion coefficient using microliter samples, which can be
completed within a few minutes. Furthermore, this approach signifi­
factor (m3/m3), and Swiir is the irreducible water saturation (%).
(Fleury et al., 2013) introduced a rapid yet efficient workflow of cantly enhances the precision of diffusion studies. These microfluidic
chips are designed to isolate the diffusion process from the convective
experiments for evaluating the petrophysical properties of reservoir rock
(clayey sandstone) and caprock of a saline aquifer located at the Ketzin effects by three main design features. First, the chips are oriented hor­
izontally; therefore, the gravity acts perpendicular to the density
site, Germany. The storage aquifer, which is part of the Triassic Stuttgart
formation, is situated onshore and is targeted for CO2 storage. Table 8 gradient and the diffusion direction. Second, the Rayleigh number (Ra)
for such microfluidic systems is maintained well below the critical Ra,
presents a series of experiments employed in the petrophysical investi­
gation for CO2 storage detailed in the study by (Fleury et al., 2013). For thus preventing free convection. Third, the design is such that the
capillary pressure within the microchannels is high, thereby allowing
field application, the experimental results from laboratory studies
similar to that of (Fleury et al., 2013) need to be combined with field-
scale models and data from actual CO2 injection and monitoring activ­
ities at injection sites. In addition, these studies need to be enhanced by
other experiments that examine the effects of geochemical interactions
on the mechanical integrity of reservoir rock and caprock. Such in­
teractions can significantly affect both the tensile and compressive
strengths of rock, potentially causing stress-induced fractures. These
fractures can alter the permeability and leakage behavior of geological
formations.

4.3.2. Pore-scale experiments

A variety of approaches are used to characterize the flow behavior of
CO2 and its trapping mechanisms in subsurface porous media at the
pore-scale level. These approaches include, for instance, microfluidic
flow visualization (Cao et al., 2015; Tirapu-Azpiroz et al., 2022), mag­
netic resonance imaging (MRI) (Jiang et al., 2017; Teng et al., 2022),

Table 8
Main experimental workflow employed in petrophysical investigation for CO2
Storage. Based on: (Fleury et al., 2013).
Property studied Experimental technique

Rock heterogeneity - CT scan characterization

Pore entry size
- High-pressure mercury injection (HPMI)
distribution
Porosity - Nuclear magnetic resonance (NMR)
- Conductivity measurement utilizing a face-to-face two-
Formation factor
electrode system
Resistivity index (RI) - Fast resistivity index measurement (FRIM)
Centrifuge capillary
- Automated centrifuge experiments
pressure
Relative permeability - Automated centrifuge experiments
- The steady-state method
Caprock permeability
- The pulse decay method
- The standard method
Caprock entry pressure
- The dynamic method
Fig. 12. CO2 flow process in a microfluidic system. Modified from (Sell
Caprock diffusion - Deuterium tracer technique
et al., 2013).

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O. Massarweh and A.S. Abushaikha Earth-Science Reviews 253 (2024) 104793

the interfacial body forces to be neglected. It should be indicated, min. In miscible flow (r > 0.8 ml/min), the intensity of the MR signal
however, that the experiments reported by (Sell et al., 2013) were decreased steadily regardless of the injection rate, which could be
conducted within temperature and pressure conditions that may not attributed to miscibility between water and supercritical CO2 at the start
fully represent those found in subsurface sequestration sites. Addition­ of CO2 injection. MRI images also revealed the occurrence of CO2
ally, the study focuses mainly on the effects of NaCl salinity, neglecting channeling (fingering) more prominently in porous media of lower
the effects of other dissolved ions that are typically present in reservoir permeability. (Jiang et al., 2017) reported that increasing particle sizes
brines. Therefore, additional research is needed to address these results in a decrease in capillary forces due to an increase in the
shortcomings. permeability of the porous medium. They also reported that the flow
The use of CO2 foam is an approach aimed at increasing the sub­ patterns of CO2, including viscous fingering, capillary fingering, and
surface storage efficiency of anthropogenic CO2 (Chaturvedi and stable displacement, vary depending on the viscosity ratio (M) of the two
Sharma, 2021; Jones et al., 2022). As such, (Gizzatov et al., 2021) uti­ fluids and capillary number (NC). It is important to note that using
lized microfluidic systems to rapidly evaluate and screen various sur­ quartz beads as porous media to represent actual reservoir rock consti­
factants based on their ability to produce CO2 foam at reservoir tutes a major limitation of the study conducted by (Jiang et al., 2017).
conditions, including pressure, temperature, and salinity. The micro­ This is because actual reservoir rocks, such as sandstones, usually
fluidic systems were manufactured to simulate the pore structure of display a variety of porosity, permeability, mineral composition, and
reservoir rock, withstanding a temperature of 100 ◦ C and a pressure of pore structure characteristics. Hence, for a more accurate depiction of
13.8 MPa. During the microfluidic experiments, pressure and flow CO2 flow under reservoir conditions, it is recommended to use actual
behavior were monitored. In addition, visual observation allowed for a reservoir core samples.
quantitative evaluation of the half-life time of CO2 foam. According to MRI can also be used to evaluate the capillary trapping of CO2 in
(Gizzatov et al., 2021), the use of microfluidic systems offers several rock. In a study reported by (Teng et al., 2022), MRI was used to study
advantages for studying CO2 flow behavior for storage purposes. These water imbibition and CO2 drainage in carbonate and sandstone rocks in
systems provide a safe, rapid, and cost-effective means for screening different scenarios. It was found that the amount of capillary trapping
chemicals for CO2 sequestration operations. In addition, they can be depends on the pore structure and injection rate. (Suekane et al., 2006)
used to predict formation damage resulting from deposition and pre­ used MRI technology to visually capture the distribution of CO2 injected
cipitation of solids occurring during CO2 injection. It should be indi­ into water-saturated porous media at supercritical conditions. The
cated, however, that (Gizzatov et al., 2021) did not provide a method for porous media used in the experimental work included Berea sandstone
quantifying or modelling CO2 sequestration based on the data obtained and glass beads. The results showed that measuring the intensity of the
from microfluidic experiments. Therefore, future studies are recom­ MR signal could effectively be used to determine CO2-water distribution
mended to focus on integrating microfluidic experimental data with in porous media. The MRI method also allowed for determining the
reservoir simulation models. The development of a direct correlation capillary dispersion rate and Darcy velocities of the phases, assisting
between this microfluidic CO2 flow visualization and CO2 sequestration reservoir simulation. Furthermore, it facilitated the examination of CO2
performance in geological formations is an area of research that deserves migration induced by buoyancy effects that significantly influence CO2
further study. physical trapping. However, (Suekane et al., 2006) indicated that due to
Microfluidic systems can also be used to study calcite dissolution the limitations of their pumping system, they were only able to capture
occurring during CO2 sequestration processes and gas/oil recovery op­ the distribution of each phase in the core at a single flow rate. As a result,
erations. In a study reported by (Song et al., 2014), microfluidic chan­ their study was limited to local Darcy velocity and capillary dispersion
nels were created through a novel approach, utilizing a naturally rate function. To address this limitation, (Suekane et al., 2006) recom­
occurring calcite crystal substrate. This approach offers several advan­ mended that later studies measure the in-situ saturation profiles at
tages. A major advantage is replicating the exact rock chemistry, a various CO2 injection flow rates.
feature that does not exist in conventional microfluidic models. A
further advantage is observing real-time changes in rock pores, which 4.3.2.3. Micro-CT scanning. Similar to MRI, micro-CT scanning is
can be challenging in core flooding systems. (Song et al., 2014) could widely employed to evaluate the pore-scale effects of CO2 injected for
visually capture the formation of CO2 bubbles resulting from carbonate- sequestration purposes (Kweon and Deo, 2017; Santarosa et al., 2013;
acid interactions in the system. Additionally, they could visualize the Van Stappen et al., 2018; Yang et al., 2021). (Zhang et al., 2019) utilized
change in the width of the microchannels due to dissolution processes. micro-CT scanning to capture 3-D microstructure variations due to
The approach presented by (Song et al., 2014) is effective for transparent ScCO2 injection into anthracite coal samples. Initially, it was visually
crystalline substrates, such as calcite crystals. The transparent nature of observed that CO2 injection leads to rapid coal swelling, resulting in
calcite, which has a trigonal-rhombohedral structure, allows for optical microfracture closure and permeability reduction. With continuous CO2
observation methods, including microfluidic flow visualization. How­ injection, wormhole features appeared, which led to permeability
ever, applying this approach to substrates with amorphous components, rebound. This phenomenon was attributed to mineral dissolution and
such as those containing amorphous silica (i.e., opal), can be challenging hydrocarbon mobilization, both of which are characterized by relatively
due to their opaque properties. A solution for this challenge could be the slower reaction kinetics. The characterization of microstructural evo­
development of alternative imaging techniques that do not rely on lution in high-rank coals (anthracite) due to supercritical CO2 injection
transparency for visualization. For instance, future research could focus was the main focus of the study conducted by (Zhang et al., 2019), which
on developing X-ray-based microfluidic systems to study microfluidic addressed a gap in the current literature. Future studies are needed,
flow in opaque or amorphous substrates. however, to assess microstructure variations in other types or ranks of
coal. This is important given the potential for varied interactions be­
4.3.2.2. Magnetic resonance imaging (MRI). Similar to microfluidic tween CO2 and coal depending on the coal rank. In a study conducted by
visualization, MRI can be used to characterize the flow of CO2 on a pore- (Liu et al., 2022), micro-CT scanning was utilized to study the effects of
scale level. For instance, (Jiang et al., 2017) used MRI to investigate the CO2 flooding on coal cleat permeability in anthracite coal samples, as
miscible and immiscible water displacement by CO2 in porous media depicted in Fig. 13 (a). In situ micro-CT scanning revealed that upon CO2
composed mainly of quartz glass beads. In the immiscible flow, occur­ flooding, the aperture size of micro cleats gradually decreased and then
ring at low injection rates (r < 0.8 ml/min), the intensity of the MR increased, depending on CO2 injection pressure (1 to 4 MPa), which was
signal increased because of the dissolution of CO2. The dissolution attributed to adsorption-swelling effects. The variations in the aperture
phenomenon became less visible after increasing the flow rate to 0.8 ml/ sizes of the micro-cleat network of coal affected the permeability

17
O. Massarweh and A.S. Abushaikha Earth-Science Reviews 253 (2024) 104793

Fig. 13. Understanding the intricacies of CO2 flow in coal: (a) depiction of an anisotropic coal sample containing cleats, and (b) permeability anisotropy (%) vs. CO2
injection pressure. Modified from (Liu et al., 2022).

anisotropy in the coal samples, as shown in Fig. 13 (b). fluid-rock interactions. The main objective of these experiments is to
determine the chemical, mineralogical, physical, and morphological
4.3.2.4. Laser-induced fluorescence. The dissolution of CO2 gas bubbles alterations expected to occur at the reservoir level upon CO2 injection
in a confined configuration is a phenomenon of interest in geophysics (Busch et al., 2023; Chen et al., 2023; Khosravi et al., 2023; Simmons
and CO2 sequestration applications. In the laboratory, a confined et al., 2023; Wang et al., 2023b). Table 9 provides common experi­
configuration can be physically represented by a Hele-Shaw cell, and in mental techniques that are used to study CO2-fluid-rock interactions.
this case, the dissolution phenomenon is typically investigated utilizing
laser-induced fluorescence (LIF). In a study conducted by (Peñas-López 4.3.4. CO2 adsorption experiments
et al., 2017), planar LIF applied over a horizontal Hele-Shaw cell was CO2 can be physically adsorbed onto rock due to electrostatic and
used to examine the dissolution of CO2 in air-saturated water, which is van der Waals forces, which significantly affects the CO2 storage ca­
driven by the diffusion process. It was found the radial propagation of an pacity of subsurface formations (Guang et al., 2023; Liu et al., 2019a;
isoconcentration front, represented as rf(t), changes over time according Petrovic et al., 2022). Due to its importance, CO2 adsorption is studied
to the following relation (Eq. 8): experimentally to determine the adsorption capacity of different rocks.
√̅ This is typically described through adsorption isotherms. Adsorption
rf –R0 ∝ t (8) characteristics determined through adsorption experiments are neces­
sary for modelling CO2 flow and transport in subsurface porous media
where t is time and R0 is the bubble’s initial radius.
(Eliebid et al., 2018). Several experimental methods are used to study
In a study reported by (Brouzet et al., 2022), planar LIF was
CO2 adsorption characteristics of mineral surfaces. These include, for
employed in examining the convective dissolution of CO2 injected into a
instance, gravimetric (Abdulkareem et al., 2020; Hui et al., 2019),
3-D porous medium composed of granular materials, including fluori­
manometric (Masum et al., 2023; Sadasivam et al., 2022), volumetric
nated ethylene propylene (FEP), silica, and PMMA grains. The refractive
(Fakher and Imqam, 2020; Wang et al., 2021), chromatographic (Gas­
index matching was employed to cancel the refraction of light at the
parik et al., 2014; Xie et al., 2022), and temperature-programmed
solid-liquid interface, which allowed for clear visualization of the
desorption (TPD) methods (Jeong et al., 2023; Wang et al., 2023a).
diffusion concentration field in CO2 flow. Additionally, various other
studies have also utilized LIF for examining CO2 flow in porous media,
indicating its widespread application in this area of research (De et al., 4.4. Selection of CO2 monitoring techniques effective for studying CO2
2021; Jia et al., 2020; Kuhn and Jensen, 2012; Vreme et al., 2016; Zhang trapping mechanisms
et al., 2020). It should be noted, however, that applying laboratory
findings from LIF experiments to actual CO2 sequestration in subsurface Evaluation of CO2 trapping is essential to determine the feasibility
reservoirs might present challenges. This limitation primarily arises and effectiveness of CO2 sequestration projects. This part of the review
when the experimental conditions do not fully capture the complex provides a qualitative assessment of the effectiveness of different eval­
heterogeneities of subsurface reservoirs. In many cases, LIF experiments uation/monitoring techniques for studying the various CO2 trapping
are conducted under highly controlled conditions with artificial porous mechanisms, as shown in Fig. 14. This assessment is a general overview
media that do not accurately represent the natural reservoir rock in based on the reviewed literature. Fig. 14 considers two situations: (a)
terms of porosity, permeability, mineral composition, and pore structure pre-injection estimation/evaluation of CO2 trapping and (b) post-
characteristics. injection monitoring of CO2 trapping.
Prior to CO2 injection, seismic methods, such as 4D seismic, are
4.3.3. CO2-fluid-rock interaction experiments highly effective for evaluating large-scale structural-stratigraphic trap­
Several experimental techniques are used to investigate the in­ ping potential. This is because seismic methods can identify suitable
teractions occurring between CO2, brine, and rock, which pertain to CO2 storage sites and examine the reservoir geology over large spatial ex­
trapping. Commonly, these interactions are examined by focusing on tents. However, seismic methods are less capable of predicting solubil­
four aspects: rock analysis, fluid analysis, fluid-fluid interactions, and ity, capillary, and mineral trapping. Following CO2 injection, seismic

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Table 9
Experimental studies on CO2-fluid-rock interactions pertaining to CO2 trapping.
Reference Targeted Rock type Analysis category Property/parameter evaluated Experimental technique(s)
sequestration
formation

- Mineralogical composition of rock - XRD (X-ray diffraction)

- Rock analysis - XRF (X-ray fluorescence)
- Chemical composition of rock
- EMP (electron microprobe)
- SEM-EDS (scanning electron
- Change in rock morphology due to
(Wang et al., - Lithic sandstone microscopy coupled with energy
- Deep coal seams CO2-brine exposure
2016) - Calcareous mudstone dispersive x-ray spectroscopy)
- Fluid-rock
- ICP-MS (inductively coupled plasma
interactions
mass spectrometry)
- Mineral dissolution due to CO2
- IC (ion chromatography)
- pH and alkalinity measurements
- Rock analysis - Mineralogical composition of rock - XRD analysis
- Solubility measurement in a high-
- Fluid-fluid
- CO2 solubility in brine temperature, high-pressure (HTHP)
interactions
reactor
(Tan et al., - Rock wettability alteration due to CO2-
- Oil field - Carbonate rock - Optical contact angle measurement
2022) brine exposure
- Fluid-rock - Change in the surface morphology of
- SEM
interactions rock due to CO2-brine exposure
- Reactivity measurement in an HTHP
- CO2-brine rock chemical reactions
reactor
- Change in rock mineralogy due to CO2-
- XRD analysis
brine-rock reactions
- Rock analysis and
- Change in porosity and permeability - Nitrogen gas porosimetry-
fluid-rock
due to CO2-brine-rock reactions. permeametry measurement
(Azin et al., - Deep saline - Carbonate rock (pure interactions
- Change in the surface morphology due
2015) aquifer dolomite) - SEM
to CO2-brine-rock reactions
- Fluid analysis and - Change in the chemical composition of - ICP-optical emission spectrometry
fluid-rock formation brine prior to and after CO2 (ICP-OES) on solutions sampled
interactions injection. during flooding experiments
- Rock analysis - Rock mineralogy - XRD analysis
- Change in the chemical composition
- Fluid analysis and
and pH of brine due to CO2-brine-rock - ICP-MS on solutions sampled from an
fluid-rock
(Liu et al., - Deep saline reactions, aiming to investigate HTHP reactor
- Sandstone rock interactions
2019b) aquifer mineral dissolution.
- Rock analysis and - Change in the mineral morphology,
fluid-rock resulting from CO2-brine-rock - SEM
interactions interaction.
- Change in pressure.
- Change in the amounts of produced
- Fluid analysis and fluids. - CO2 flooding brine–rock experiments
fluid-rock - Change in brine chemistry, including combined with ICP-atomic emission
interactions pH, alkalinity, ionic chemical spectrophotometry (ICP-AES)
composition, mineral saturation, and
total inorganic carbon (TIC).
(Yu et al., - Change in the mineral composition of
- Oil field - Feldspathic sandstones
2012) core samples due to CO2-brine-rock - XRD analysis
reactions.
- Rock analysis and - Change in the mineral morphology,
fluid-rock resulting from CO2-brine-rock - SEM-EDS
interactions interaction.
- Change in rock porosity and air
- Helium porosimetry measurement
permeability due to CO2-brine-rock
- Air permeametry measurement
reactions.
- Change in the chemical composition
- Fluid analysis and - ICP-AES and ICP-MS on aqueous so­
and pH of brine due to CO2-brine-rock
fluid-rock lutions sampled from a high-pressure
reactions.
(Rosenbauer interactions reactor
- Aquifer - Tholeiitic basaltic rock - CO2 uptake
et al., 2012)
- Rock analysis and
fluid-rock - Mineral precipitation - XRD and SEM analyses
interactions
- Rock analysis - Organic matter within the rock - Total organic content (TOC) analysis
- Clays (quartz, feldspar,
- Rock wettability alteration due to CO2 - Contact angle measurement using a
(Gholami illite/smectite, illite/
- Shales - Fluid-rock exposure in a static reactor drop shape analyzer (DSA)
et al., 2021) mica, kaolinite, and
interactions - Mineralogical alteration after CO2
chlorite) - XRD and SEM analyses
exposure in a static reactor

methods are effective in monitoring the physical evolution of a CO2 can provide important data on all trapping mechanisms.
plume relevant to structural, capillary, and solubility trapping. Borehole Atmospheric methods have a limited role in evaluating the storage
logging can produce high-resolution data about the region surrounding capabilities of CO2 sequestration sites. Nevertheless, they play a main
the injection well, providing essential information used for estimating role in detecting CO2 leakage, which is mostly relevant to structural,
structural-stratigraphic trapping. After CO2 injection, borehole logging capillary, and solubility trapping. Petrophysical characterization and

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O. Massarweh and A.S. Abushaikha Earth-Science Reviews 253 (2024) 104793

Fig. 14. Effectiveness of evaluation/monitoring techniques for CO2 trapping mechanisms: (a) prior to CO2 injection and (b) following CO2 injection.

pore-scale experiments are essential for examining rock properties, 6. Summary and conclusions
which are used to determine the potential for structural, capillary, and
mineral trapping before CO2 injection. However, these experiments This review provided an understanding of the various trapping
require extensive lab work, making them resource-intensive and less mechanisms relevant to CO2 sequestration in subsurface reservoirs.
efficient in monitoring temporal changes occurring after CO2 injection. These mechanisms include structural-stratigraphic, capillary (residual),
CO2-fluid-rock interaction experiments are highly effective in solubility, and mineral trapping. Each of the trapping mechanisms is
studying possible mineralogical alterations related to mineral trapping. characterized by its own trapping performance, with structural trapping
They are also effective in predicting solubility and capillary trapping. providing the most storage contribution over time and mineral trapping
However, like petrophysical characterization and pore-scale experi­ providing the highest storage security. Furthermore, this review dis­
ments, CO2 -fluid-rock interaction experiments demand rigorous labo­ cussed the main evaluation and monitoring approaches that are used in
ratory investigation, making them less efficient for post-injection the pre-injection and post-injection stages of CO2 sequestration projects.
monitoring of CO2 trapping. CO2 adsorption experiments are very These approaches aim to estimate the amounts of CO2 that can be stored
effective in understanding how CO2 might be adsorbed onto the rock in subsurface formations and evaluate the safety and security of CO2
surface, which is necessary for predicting mineral trapping. However, storage. Different approaches were presented, including seismic and
these experiments are not commonly employed in monitoring CO2 borehole geophysical techniques, atmospheric monitoring methods, and
trapping following CO2 subsurface injection. laboratory scale experiments. We expect our review to be important for
researchers, field practitioners, and policymakers by providing guidance
5. Future directions on field and laboratory methods for investigating and assessing CO2
subsurface trapping. It also proposes an innovative qualitative approach
As the field of geological CO2 sequestration rapidly expands, the for selecting appropriate monitoring techniques across the various
development of a robust framework for selecting efficient monitoring stages of CO2 sequestration projects.
techniques has become increasingly necessary. Future research should Seismic and borehole geophysical approaches encompass a variety of
focus on a detailed analysis and comparison of various monitoring techniques, such as 4D seismic technology, 4D–3C, 4D-3C-VSP,
techniques in terms of cost, effectiveness, time scale, and appropriate 4D–9C, cross-well seismic tomography, passive seismic monitoring,
application scenarios for CO₂ sequestration projects. and time-lapse well logging. Such techniques are highly effective for
Based recent research trends, we identified four primary areas for evaluating/monitoring structural trapping over large areas. Atmo­
future investigation and development in geological CO2 storage: (1) spheric methods, on the other hand, are not commonly used in the pre-
advanced CO2 monitoring techniques; (2) improved reservoir charac­ injection stage; however, they are highly valuable in monitoring the CO2
terization for CO2 storage; (3) integration of CO2 storage with CO2-based release into the atmosphere from subsurface sources in the post-
EOR; and (4) examination of caprock integrity. Details on these research injection stage. On a laboratory scale, various tests and experiments
directions are provided in Table 10. are used to examine CO2 trapping characteristics. These tests are

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O. Massarweh and A.S. Abushaikha Earth-Science Reviews 253 (2024) 104793

Table 10 Data availability

Recent research directions in CO2 storage.
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