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Recent Progress in CO2 Capture/Sequestration: A

Review
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Mazen M. Abu-Khader
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Department of Chemical Engineering, Al-Balqa Applied University, Amman, Jordan
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DOI: 10.1080/009083190933825
Recent Progress in CO2 Capture/Sequestration:

A Review
MAZEN M. ABU-KHADER
Department of Chemical Engineering
Al-Balqa Applied University
Amman, Jordan
Downloaded by [University of South Florida] at 13:43 16 April 2013
Environmental protection is a critical issue worldwide at the current time. In particu-

lar, CO2 emissions are now considered to be one of the major pollutants contributing
to global warming. The aim of this concise review is to provide a clear picture of
the present development of various capture technologies and available technology
options. In addition, this article attempts to examine recent advances in research and
developments for CO2 storage and sequestration. Finally, the article also looks at op-
portunities and challenges based on cost and engineering economics of CO2 capture
and sequestration.
Keywords CO2 capture, CO2 sequestration, CO2 storage, capturing technologies,

cost
The last 50 years has provided the strongest evidence that anthropogenic CO2 emissions
are causing significant effects on climate, and that it is becoming increasingly important
to stabilize atmospheric CO2 emissions below current levels by controlling the use of
carbonaceous fuels (IPCC, 2001). International organizations such as the United Nations
Framework Convention on Climate Change (UNFCCC) and the Intergovernmental Panel
on Climate Change (IPCC) have been formed to address this issue. Three options are
being explored to stabilize atmospheric levels of greenhouse gases (GHGs) and global
temperatures without severely and negatively impacting standard of living: (1) Reducing
energy use through improving energy efficiency, (2) switching to different fuels by either
using a lower carbon fuel, nuclear power or any of the available renewable energy sources,
and (3) employ carbon sequestration. To be successful, all three options must almost
certainly be used in concert. The most common ways to generate power from fossil fuels
are by the use of the following: (1) gas turbines that burn natural gas or light oil distillate;
(2) steam power plants that burn coal, oil or natural gas, usually at close-to atmospheric
conditions; (3) combined cycles, which is a combination of (1) and (2) where the gas
turbine exhaust heat is employed to generate steam for a steam power cycle (integrated
gasification combined cycle (IGCC)); and (4) stationary internal combustion engines.
The author would like to thank Dr. E. J. Anthony from CANMET, Energy Technology Centre
(CETC), Natural Resources Canada, for his valuable comments to improve the readability of the
manuscript.
Address correspondence to M. M. Abu-Khader, Department of Chemical Engineering, Faculty
of Engineering Technology, Al-Balqa Applied University, Box 15008, Marka, (11134) Amman,
Jordan. E-mail: mak@accessme.com
1261
1262 M. M. Abu-Khader
It should be noted that although capture and transportation of CO2 is feasible and
technically proven, further investigation regarding the reliability and safety of long-term
storage remains necessary (IPCC, 2001; Ceila and Bachu, 2002).
Recently, several short reviews were published (White et al., 2003; Freund, 2003;
Chen et al., 2003; Hill, 2003; Dijkstra and Jansen, 2004) on the capture and geologic
sequestration of CO2 generated from large point sources, i.e., fossil-fuel-fired power
gasification plants. Also, other concepts have been explored, including: the separation
and capture of CO2 from both flue gas and fuel gas using wet scrubbing technologies,
dry regenerable sorbents, membranes, cryogenics, pressure and temperature swing ad-
sorption. Also, these reviews described the existing commercial CO2 capture facilities at
electric power-generating stations based on the use of monoethanolamine, and reviewed
technologies for storage of the captured CO2 . A discussion of possible problems related
to deep injection of CO2 is presented. Cost and problems of implementation were ad-
dressed. Investigations on the technical feasibility of separating and decomposing CO2
within the context of power/energy-generation with emphasis on the combustion as-

pects of integrated CO2 -capture/power-generation advanced cycle were conducted (Ren
et al., 2002). Also, a novel method has been developed (Bolland and Undrum, 2003)
that compares power plant concepts including CO2 capturing. Instead of using extensive
thermodynamic calculations for these concepts, reaction equations for the conservation
of molecular species together with specific energy consumption numbers for the different
process sections are used to characterize the concepts with respect to fuel-to-electricity
conversion efficiency.
The findings of the first phase of The IEA Greenhouse Gas R&D work showed that
the most appropriate technology for capture of CO2 depends upon the type of power
plant and proven technology available. However, capture of CO2 adds substantially to
the cost of power generation and reduces plant efficiency. In contrast, storage of CO2 ,
e.g., in the ocean, is unproven but relatively inexpensive. There are major uncertainties
about storage, in particular long-range environmental impacts and security. Utilization
of CO2 such as making chemicals has also been considered but clearly has only limited
potential (Audus, 1997; Riemer and Ormerod, 1995; Webster, 1995).
The Japanese electric utilities and other organizations have been encouraged to de-
velop technologies that contribute to CO2 emission reduction for many years: adsorption,
absorption, membranes and cryogenic systems. Some of the key issues of CO2 recovery
technologies for large-scale application based on the experience of the Japan’s RD were
addressed (Yokoyama, 2002).
CO2 Capture and Storage

Effective capture of CO2 from flue-gas streams is an essential development to permit
carbon management by sequestrating of CO2 . Hence, successful carbon management
for climate purposes requires increased understanding of carbon cycle dynamics and
improvement in the scientific capabilities available for measurement as well as for policy
needs (Dilling et al., 2003; Huston and Marland, 2003).
CO2 Capture Technologies

There are several methods for CO2 capture from gas streams such as the use of: chemical
and physical solvents, adsorption on solids, membrane, cryogenic/condensation system.
Equally, different plant configurations will require different CO2 strategies such as:
Recent Progress in CO2 Capture/Sequestration 1263
1. Post-combustion as conventional approach is going through process improvements

such as the use of advanced solvent systems, new packing material, compact
membranes and finally the use of electric swing adsorption systems (Simmonds
et al., 2003).
2. Pre-combustion de-carbonization is a new approach based on established IGCC
technology that is going through great technology improvements such as the
development of a) low maintenance cost gasifiers, and double stage gasification;
b) implementation of advanced gas turbines; c) new CO2 capture processes for
acid gas removal stage; d) the use of membranes for H2 /CO2 separation; e) the
use of auto-thermal reforming for natural gas; f) electric swing adsorption; and
g) better process integration for the overall IGCC process. A CO2 - and H2 -rich gas
can be produced through, e.g., partial oxidation (PO), methane–steam reforming
(MSR) or auto-thermal reforming, with subsequent water-gas shift (WGS). Two
relatively innovative gas turbines (GT) based power cycles with high CO2 removal
potential have been proposed and discussed (Fiaschi and Tapinassi, 2004) in terms
of exergy analysis. Where fuel de-carbonization is applied by the means of auto
thermal reforming (R-ATR) and simple reforming (R-REF), in order to convert
the primary natural gas into a highly H2 and CO2 concentrated fuel. Thus, CO2
is captured with amine chemical absorption into a specific unit and, finally, the
de-carbonized fuel is sent to the GT combustion chamber. No bottoming steam
cycle is included.
3. Oxy-fuel combustion, which is a novel approach, uses recycled CO2 to moder-
ate the temperature of combustion of fuel with oxygen. This approach has been
going through improvements in the use of air separation membrane systems and
implementation of chemical looping combustion method (CLC). Oxy-fuel pro-
cesses cover processes that employ oxygen instead of air as oxidizing agent and
they are: (a) O2 /CO2 combustion with oxygen from oxygen transport membranes
(OTM), (b) advanced zero emission power (AZEP) concept, and (c) membrane
reactor for end combustion. Practical oxy-coal combustion techniques have been
developed in order to facilitate the conversion of coal-fired utility power plants
so as to recover a CO2 rich flue gas stream for use and/or sequestration (Chui
et al., 2003).
Chemical-looping combustion (CLC) with inherent separation of CO2 is considered

a promising technology (Ishida and Jin, 1996, 1997; Ishida et al., 1998, 2002; Jin and
Ishida, 2001, 2002; Jin et al., 1999; Lyngfelt et al., 2001). Where two interconnected
fluidized beds are used as reactors in the fuel reactor, a gaseous fuel is oxidized by
an oxygen carrier, e.g., metal oxide particles producing carbon dioxide and water. The
reduced oxygen carrier is then transported to the air reactor, where it is oxidized with
air back to its original form before it is returned to the fuel reactor. The feasibility of
using an oxygen carrier based on oxides of iron, nickel, copper, and manganese were
investigated (Cho et al., 2004; Mattisson et al., 2001; de-Diego et al., 2004). In CLC, the
critical issue of possible gas leakages was investigated in a scaled cold model: (i) from
the fuel reactor to the cyclone and to the pot-seal, (ii) from the cyclone down to the fuel
reactor, and (iii) from the pot-seal to the fuel reactor. These leakages have direct impact
on CO2 capture efficiency (Johansson et al., 2003).
Various other systems have also been evaluated such as an LNG combined-cycle
(LNG C/C), an integrated coal-gasification combined cycle (IGCC) and a molten carbon-
ate fuel cell (MCFC) (Amorelli et al., 2004) combined-cycle power-generation system
with CO2 capture and sequestration technologies. The authors illustrated that the CO2 -
emission control potentials for the LNG C/C, IGCC and MCFC are in the range 64–72%,
65–76%, and 57–68%, respectively. However, off-site power required for CO2 emission
control increases NOx and SOx emissions by as much as a factor of 1.3 to 10 (Akai
et al., 1995, 1997; Akai, 1996).
The graphical evaluation and review technique (GERT) has been used to evaluate
research and development processes of the various CO2 capture technologies having
different levels of energy efficiency (Kosugi et al., 2003).
Chemical Absorption Technology. In this technology, CO2 is captured from the flue gas
of power plants by using a chemical absorbent such as amine solutions. Heat energy is
consumed to regenerate the chemical absorbent so that the net power output of the plant
is reduced (Mimura et al., 1995; Bolland and Undrum, 1998). The chemical sorption per-
formance of various amine-enriched fly ash carbon sorbents for the capture of CO2 from
gas streams have been investigated. These sorbents were generated by the chemical treat-
ment of carbon-enriched fly ash concentrates with a 3-chloropropylamine-hydrochloride
(CPAHCL) solution at 25◦ C. The ability of similar sorbents to capture CO2 from gas
stream in the presence of moisture was also addressed (Gray et al., 2002, 2004; Breault,
2003). Amine scrubbing applied to CO2 capture has been studied by several groups
(Desideri and Paolucci, 1999; Nsakala et al., 2001). Amine solvent performance could
be improved as much as 30% by the use of mixed solvents (Chakma, 1997). The CO2
capture by aqueous 30 wt% monoethanolamine (MEA) in water through the use of the
RateFrac absorber model (Freguia and Rochelle, 2003). On the other hand, a theoretical
simulation work (Wang et al., 2004) was performed to study CO2 capture by absorption
in a hollow fiber membrane contactor through the use of three typical alkanolamine solu-
tions. This is to investigate the effects of different sorption systems, operating conditions
and membrane characteristics on the removal behavior of CO2 .
The limestones have been studied extensively to determine their ability to remove
CO2 in multiple carbonation/calcination cycles. Two systems are commonly used: a cir-
culating fluidized bed combustor (CFBC) operated in the bubbling FBC mode and a
thermogravimetric analyzer (TGA). The use of Na2 CO3 and NaCl to reactivate the lime
and enhance CO2 capture failed to do so in the FBC environment, but in the case of
NaCl, produced significant improvements in performance in the TGA after several cy-
cles, while Na2 CO3 did not improve performance in either case (Salvador et al., 2003).
The electrobalance and fixed-bed reactors were used to study the capture of CO2 from
simulated flue gas using a regenerable Na2 CO3 sorbent. CO2 capture was effective in the
temperature range of 60–70◦ C, while regeneration occurred in the range of 120–200◦ C,
depending on the partial pressure of CO2 in the regeneration gas (Liang et al., 2004). A
method for separation of CO2 from flue gases of coal-fired combustors using a dual flu-
idized bed configuration was investigated (Anthony and Wang, 2003). Experimental work
using a pilot-scale fluidized bed combustor showed that the reaction is sufficiently fast
for the fluidized bed technology to apply, and the addition of fresh limestone overcomes
the activity decay. A general design equation was developed to calculate the maximum
CO2 capture efficiency for carbonation/calcination cycle and to estimate the decay in
sorbent activity with the number of cycles (Abanades, 2002). The CaO sorbent is used
to absorb CO2 and SO2 in fluidized combustor or steam gas reformer, and is regenerated
in a calciner. In the calciner, petroleum coke is fired with pure oxygen to provide the
heat for regenerating the sorbent and give a CO2 stream for subsequent utilization or
sequestration (Wang et al., 2004).
A schematic model of ocean chemistry and transport was proposed to analyze the
geochemical consequences of a new method that involves reacting CO2 -rich power-plant
gases with seawater to produce a carbonic acid solution, which in turn is reacted on site
with carbonate mineral (e.g., limestone) to form Ca2+ and bicarbonate in solution, which
can then be released and diluted in the ocean (Caldeira and Rau, 2000).
The sorbent energy transfer system (SETS) has the potential for providing a signifi-
cant reduction in CO2 emissions from gaseous fossil fuel-fired electric power plants with
minimal loss in power generating efficiency (Yu et al., 2003).
There have been several methods to modify the Solvay process in order to make it
effective for the control of power plant CO2 emissions. The new modified process, called
the dual alkali approach, attempts to replace either or both bases, ammonia and lime, in
the Solvay process with other compounds to make CO2 capture and separation efficient
(Huang et al., 2001).
Physical Adsorption Technology. This technology captures CO2 from a boiler exhaust gas
by using the PSA (pressure swing adsorption) or PTSA (pressure and temperature swing
adsorption) method (Ohta, 1997). A nanoporous solid adsorbent was developed which
can serve as a “molecular basket” for CO2 in the condensed form. Polyethylenimine
(PEI)-modified mesoporous molecular sieve of MCM-41 type (MCM-41-PEI) has been
prepared and tested as a CO2 adsorbent (Xu et al., 2002).
Membrane Separation Technology. This technology is expected to attain a high efficiency

CO2 capture from the exhaust gas of a power plant. The elemental technologies of the
membrane separation technologies include various kinds of CO2 separation membrane
and the vacuum pump applicable to the physical adsorption technology (Teramoto et al.,
2003). Membrane-based gas separation systems are noteworthy owing to their low energy
requirements, promising technology evolution and effective integration with power plants.
A mathematical model for membrane-based separation systems has been developed that
is able to cover the most significant membrane types and configurations (Carapellucci
and Milazzo, 2003). An efficient and selective extraction of carbon dioxide (CO2 ) at low
to medium concentration from mixed gas streams was achieved by the use of a novel
enzyme-based, facilitated transport contained liquid membrane (EBCLM) reactor (Cowan
et al., 2003).
O2 /CO2 Recirculation Boiler Technology. A power plant adopting this type of CO2 cap-
turing technology utilizes oxygen and circulated flue gas as oxidant to burn fuel. CO2 gas
can be directly captured since the flue gas consists of only CO2 and steam. This power
plant needs no de-NOx equipment (Okawa et al., 1997; Koda and Takahashi, 2002).
Series of experiments have been conducted on O2 /CO2 recycle combustion with natural
gas in air and in mixtures of oxygen and recycled flue gas (Tan et al., 2002).
Integrated Hydrogen Separation Gas Turbine Technology This technology has been pro-
posed to provide a new power generation system, and named a “hydrogen decomposed
gas turbine” system by a group in Japan, where innovative hydrogen separation mem-
branes are incorporated. There are two types of systems depending on the fuel to be
burned: LNG (liquefied natural gas) or coal (Moritsuka, 2001; Moritsuka and Koda,
2000). A survey is made of high-temperature membranes and several possible applica-
tions of membrane reactors for integration in power generation cycles with CO2 capture
(Bredesen et al., 2004). Whereas a recent work (Jordal et al., 2004) described the capture
CO2 in natural gas fired power cycles through the use of a high-temperature membrane
reactor of the methane-steam reforming type with an integrated H2 -separating membrane,
and two types of membranes were investigated: Pd membranes, which could allow for
zero-emission power cycles, and microporous membranes, the use of which means that
20% of the generated CO2 is emitted to the atmosphere.
Promising Technologies. A zero emission CO2 capture power process and plant, COOL-
ENERG (CO2 loop for energy and nature, enhanced by refrigeration and gas turbines)
was patented and thermodynamically modeled. The plant is operated by a CO2 quasi-
combined two-stage gas-turbine cycle with CH, gas burning in an O2 /recycled CO2
mixture. It uses the advanced thermal absorption technology in cogeneration of power
and cooling (Staicovici, 2002). A novel technology based on the zero CO2 emission MA-
TIANT cycle has also been developed. The optimized cycle has an efficiency of around
45% when operating on natural gas, and the system can remove the CO2 produced in the
combustion process in the liquid or supercritical state and at high pressure, without any
costly and energy consuming system like “end-of-pipe” MEA scrubbers or membranes
(Mathieu and Nihart, 1999).
Carbon-negative production is a technological opportunity based on renewable bio-
mass-based energy conversion with CO2 capture and permanent storage (BECS). Today,
most R&D and demonstration efforts concerning CO2 capture and storage technologies
are focused on achieving nearly zero emissions from fossil fuel-based systems such as, for
example, coal-fired power plants. Because BECS involves capture and storage of biotic
CO2 from renewable biomass, the technology can yield negative CO2 emissions—i.e.,
CO2 is removed from the atmosphere on a net basis (Obersteiner et al., 2001). In pulp and
paper mills with modern combined heat and power (CHP) systems. Based on recovery
boilers and biomass boilers, the overall electrical efficiencies are low. Significantly im-
proved overall energy efficiency and increased electrical efficiency could be accomplished
by the introduction of black liquor integrated gasifier with combined cycles (BLGCC),
which is, however, not a commercially available technology (Larson et al., 1999, 2000;
Maunsbach et al., 2001).
The impact of combining CO2 capture and storage with alternative systems for
biomass-based combined heat and power production (CHP) in Kraft pulp and paper
mills have been investigated, and the overall best CO2 abatement is achieved when CO2
capture is carried out within a biomass integrated gasifier with combined cycle where
the syngas undergoes a CO-shift reaction. Also, the cost of CO2 capture and storage
in pulp and paper mills depends on system configuration and the CO2 transportation
distance (Möllersten et al., 2004). Commercialized black liquor gasification (BLG), CO2
capture and reliable CO2 sequestration technologies are identified as important potential
contributors to help achieve compliance with Kyoto Protocol targets, especially in a
scenario of nuclear power closures (Möllersten et al., 2003).
CO2 Storage
Recent work overviewed (Gale, 2004) the research work that is currently underway and
provides an analysis of the current state of knowledge on geological storage of CO2 . Also,
excellent reviews of geologic storage of carbon dioxide (CO2 ) were published illustrating
that the geologic storage is an important tool for managing carbon (Bruant et al., 2002;
Freund, 2001), and other selective reviews were compiled that focus on the technical and
regulatory aspects that are most likely to be important in assessing and managing the
risks of geologic storage (Holloway, 2001; Chadwick et al., 2003). Underground storage
in porous and permeable reservoir rocks is technically feasible, and, under favorable
conditions, CO2 can be retained in underground reservoirs for millions of years (Wilson
et al., 2003; Bachu, 2001).
In the project of European Potential for Geological Storage of Carbon Dioxide from
Fossil Fuel Combustion (GESTCO), fourteen cases of actual geological situations were
selected to investigate the effective CO2 storage capacity of underground storage struc-
tures. Also, the viability of geological CO2 storage is investigated through reservoir
engineering studies, and an extensive inventory in key areas in Europe of industrial CO2
sources, potential geological storage sites (CO2 sinks) and transportation routes (Obdam
et al., 2003). Oil fields are likely to be the first category of geologic formation where car-
bon dioxide (CO2 ) is injected for sequestration on a large scale, if geologic sequestration
proves feasible. There is a need to evaluate whether an oil reservoir might be suitable
for CO2 storage, and to address a series of criteria for injection into currently producing,
depleted, or inactive reservoirs, taking into consideration aspects such as reservoir depth,
storage capacity, water and oil volumes in place, formation thickness, and permeability
(Kovscek, 2002). The existing information on the adaptation of geological reservoirs for
natural gas storage can assist the development of CO2 storage. There is currently little
information in the public domain on leakage from reservoirs.
The economics of major technologies and practices under development for CO2
storage and sink enhancement were compared, including options for storing captured
CO2 from various geological sites, as well as the enhancement of biological sinks such
as forests and croplands (Bock et al., 2003).
An experimental investigation looked at the absorption of CO2 into C-60-C-70 binary
solids at room temperature using a commercially available autoclave. The study concluded
that no trace of CO2 storage was detected for pure C-70, and that the stability of CO2
trapped in solid fullerenes (C-60) is explained in terms of geometrical considerations
based on hard-sphere packing at octahedral sites (Takahashi and Yamazaki, 2003).
A new technology called acid gas re-injection has emerged over the past ten years
in Canada as an effective way of ensuring that acid gases are not emitted into the atmo-
sphere. This technology involves compressing the acid gas and injecting it into a suitable
underground zone, similar to deep well disposal of produced water. This technology
represents an innovative CO2 storage opportunity (Wong et al., 2003).
CO2 Sequestration
Current technologies for CO2 sequestration include: disposal of CO2 in deep oceans; de-
pleted oil and gas fields (Bossie-Codreanu et al., 2003); deep saline formations (aquifers);
and recovery of enhanced oil, gas, and coal-bed methane. However, the current cost for
the utilization of these types of technologies has proven to be too expensive. Conse-
quently, reducing the cost for the capture of CO2 will be a critical step in the overall
carbon management program (DOE, 1993). Geological sequestration of CO2 is immedi-
ately available and technologically feasible means of reducing CO2 emissions, which is
particularly suited to landlocked sedimentary basins (Bachu, 2000, 2002; Kuuskraa and
Pekot, 2003). Warm sedimentary basins are less favorable for CO2 sequestration than
cold basins because of reduced capacity in terms of CO2 mass, and because of higher
CO2 buoyancy, which drives the upward CO2 migration (Bachu, 2003).
The Natural Analogues for the Storage of CO2 in the Geological Environment
(NASCENT) project is studying several natural European CO2 accumulations (Pearce
et al., 2003). The importance of these accumulations is that they offer the potential to
understand the long-term geological processes involved in CO2 sequestration. By identi-
fying the effects of CO2 on rock properties, such as changes in permeability and porosity
or rock strength, models can be verified against empirical data.
Two recent technical reviews (Voormeij and Simandl, 2004; Yamasaki, 2003) ad-
dressed the geological, ocean, and mineral CO2 sequestration options. These reviews
covered the following methods: storage in oil and gas reservoirs (Bachu and Shaw,
2003; Shaw and Bachu, 2002; Wilson et al., 2001), in deep coal seams, in deep saline
aquifers (Bachu and Adams, 2003), in deep ocean, in salt caverns, and mineral car-
bonation (Goldberg and Walters, 2003; Maroto-Valer et al., 2003). Also, it discussed
weaknesses and strengths of each of these methods. Engineering and economic assess-
ments were conducted (Gupta et al., 2003; Shimada et al., 2003) to review the status
of existing technologies that could be used to sequester CO2 , develop a preliminary en-
gineering concept to accomplish the required operations, estimate capital and operating
costs for sequestration systems under various design conditions, and outline regulatory
and project implementation aspects.
The deep ocean (Lee et al., 2003; Song, 2003; Brewer et al., 2000, 2003; Warzinski
et al., 2000) is one of only a few possible CO2 disposal options (others are depleted
oil and gas wells or deep, confined aquifers) and is a prime candidate because the deep
ocean is vast and highly unsaturated in CO2 . Understanding the phase behavior and
formation kinetics of CO2 hydrate is essential for developing the sequestration process
of CO2 into the deep ocean and its feasibility (Lee et al., 2002). A new method has
been developed named gas lift advanced dissolution (GLAD) system, which utilizes a
gas-lift pump system that dissolves the low purity CO2 into seawater at a relatively
shallow depth of 200–300 m and then transports CO2 -rich seawater to a depth greater
than 1000 m (Kosugi et al., 2001; Saito et al., 2000).
Several modes of CO2 injection have been identified in the literature, and the most
feasible initial options will likely involve a release of liquid CO2 at intermediate depths
of 1000 to 1500 m (Adams et al., 1995). Process modeling of CO2 injection into depleted
natural gas reservoirs offers the potential to sequester while simultaneously enhancing
CH4 recovery (Oldenburg et al., 2001). To evaluate the efficiency of the ocean in retaining
purposefully sequestered CO2 , eight ocean modeling groups made a set of standard
injection simulations, and at 3000-m injection, all models showed 85% efficient (Orr et al.,
2001, 2003). Also, a semi-analytical model (Saripalli and McGrail, 2002) to simulate the
deep well injection of CO2 for geological sequestration has been developed. It is simple
and easy to use modeling tools to assess the performance of a deep well operation during
and after injection. The direct injection of industrial CO2 emissions into the mid-water
oceanic column below 500 m depth has been reviewed (Ametistova et al., 2002). Such
a process is a potential candidate for switching atmospheric carbon emissions directly
to long-term sequestration. Fundamental and applied studies on injection of CO2 into
geologic formations are being conducted within the integrated collaborative technology,
development program for CO2 sequestration in geologic formations in the United States
by the Department of Energy R&D (Klara et al., 2003). The effectiveness of injection into
the ocean of CO2 produced from the use of fossil fuels is also being investigated using a
coupled climate-carbon cycle model (Harvey, 2003), and radiocarbon as a good predictor
is used to estimate the effectiveness of carbon sequestration by direct injection (Caldeira
et al., 2002). The dilution processes of CO2 were investigated near injection points in the
deep ocean to evaluate the biological impacts of the ocean sequestration of CO2 (Sato
and Sato, 2002). It is important to establish science-based regulatory framework for CO2
injection. The Environmental Protection Agency (EPA) Underground Injection Control

(UIC) program has extensive experience in regulating the injection of mainly liquid wastes
into geologic formations. A review has been complied (Tsang et al., 2002) on the current
UIC regulations, injection-well classification scheme and monitoring requirements, and
identification of the unique factors related to the physical and chemical processes in the
subsurface associated with CO2 injection.
The kinetic modeling of CO2 sequestration reactions (Zerai et al., 2003) and their
implications for CO2 sequestration in deep-saline aquifers were studied by conducting
experimental CO2 -saturated brine-rock interactions at elevated temperature and pressure
(Rosenbauer and Koksalan, 2003). High-pressure injection of CO2 into these deep aquifers
was simulated by reaction path modeling, and the results indicate that this is a feasible
method to reduce the inputs of anthropogenic CO2 into the atmosphere (Cipolli et al., 2004).
A novel, externally controlled microreaction system has been developed (Wolf et al.,
2004) to provide the first in situ observations of the reaction processes that control
CO2 sequestration via mineral carbonation. The system offers pressure (up to 20 MPa),
temperature (up to 250◦ C), and activity control suitable for investigating a variety of
fluid-fluid and fluid-solid interactions of environmental interest.
Coupling a low-temperature once-through methanol synthesis process (Mahajan and
Goland, 2003) with CO2 sequestration technology would provide an option for integrated
gasification combined cycle (IGCC) power plants to address the CO2 mitigation issue and
also create the capability to utilize methanol as a peak-shaving fuel. The potential of this
approach is considered in light of the recent advances in CO2 sequestration technologies.
A pressure-swing adsorption process, which uses zeolite 13X as an adsorbent to
recover and sequester carbon dioxide from mixture gas (nitrogen and carbon dioxide), is
investigated through dynamic simulation and optimization (Ko et al., 2003).
The development of a CO2 scrubber that uses an enzyme to reduce CO2 emissions
is a viable option (Bond et al., 2001). The enzyme, carbonic anhydrase, is the biological
catalyst that accelerates the rate of CO2 hydration for subsequent fixation into stable
mineral carbonates.
A decision support system has been developed to evaluate the technical and econom-
ical feasibility of CO2 storage in the subsurface. With this system, CO2 sequestration
systems can be defined, consisting of a selection of CO2 sources and sinks and a pipeline
route (Egberts et al., 2003).
There has been proposed strategy that utilizes an innovative application of chemical
processes to convert CO2 , NOx and SOx emissions into valuable fertilizers (mainly,
NH4 HCO3 ) that can enhance sequestration of CO2 into soil and subsoil earth layers,
reduce NO3 -contamination of groundwater and stimulate photosynthetic fixation of CO2
from the atmosphere. If this technology is developed, it could contribute importantly to
global CO2 sequestration and clean air protection (Lee and Li, 2003).
A risk and consequence assessment methodology for carbon sequestration projects
was developed using a typical injection field as the source of hazard, and leaking CO2
fluxes as the key measures of risk and consequence to humans, animals, biota, property,
agriculture, and water resources (Saripalli et al., 2003). An assessment and valuation
have been reported on the environmental impacts arising from the full fuel cycles of a
natural gas combined cycle (NGCC) plant featuring CO2 separation and disposal to a
disused gas well, an integrated gasification combined cycle (IGCC) plant featuring CO2
separation and disposal to the deep ocean, and finally a pulverized fuel plant with flue
gas desulphurization (PF + FGD) with CO2 capture by a managed forest at a site remote
from the power plant (Holland et al., 1995).
CO2 Cost and Policy Control

There have been several recent studies of energy technologies to reduce greenhouse gas
emissions that address the opportunities and challenges based on cost and engineering
economics of CO2 capture and sequestration (Biggs et al., 2001; Brown et al., 1998;
Grubler et al., 1999; Herzog and Vukmirovic, 1999; Hirsh, 1999; Keith and Morgan,
2001; Nawaz and Ruby, 2001; Rubin et al., 2001; Simbeck, 2001; Singh et al, 2002; Wong
et al., 2000). Energy savings and carbon sequestration, including CO2 capture/storage and
enhancement of natural carbon sinks, can be highly beneficial, although it is suggested
that both economic and climatic feedbacks could nullify part of the gains achieved, and
that substantial R&D is needed to improve available technology and to lower the cost
(Jean-Baptiste and Ducroux, 2003a, 2003b).
The Norwegian experience on “engineering cost evaluations” for capture of car-
bon dioxide (CO2 ) from thermal power plant emissions is developed by investigating a
possible commercial application for CO2 -sequestration (Hustad, 2001).

An investigation was conducted to determine under what conditions microalgal-
based CO2 capture from flue gases is economically attractive (Olaizola, 2003). When
using a hybrid coal integrated gasification combined-cycle (IGCC) system, consisting of
a gasifier, a shift reactor and a membrane separator, the energy and cost analysis show
that CO removal in this hybrid IGCC scheme is technically feasible (Kaldis et al., 2004).
Various technical and economical aspects for CO2 capture in small size cogeneration
plants were analyzed (Desideri and Corbelli, 1998). The CO2 budget, or an “equivalent
CO2 ” budget, was quantified and associated with each of the individual energy-cycle
steps, in addition to process design capital and operating costs for CO2 -capture tech-
nologies combined with integrated gasification combined-cycle (IGCC) power systems,
CO2 transportation, and options for the long-term sequestration of CO2 (Doctor et al.,
1997). Also, the CO2 -capturing power generation systems that use solar thermal energy
and gasified coal as the input energy were evaluated (Pak and Kosugi, 2002).
A method of full-fuel-cycle analysis was developed which made up from the “pri-
vate costs” of owning and operating a power station together with the “external costs”
representing its environmental impact (Audus and Freund, 1997; Hu et al., 2004).
Various frameworks for computing mitigation costs and a simplified model of electric
sector planning were developed. The extent to which carbon capture and sequestration
(CCS) technologies might lower the cost of CO2 control in competitive electric markets
will depend on how they displace existing generating units in a system’s dispatch order, as
well as on their competitiveness with abatement alternatives (Johnson and Keith, 2001).
Despite conservative assumptions about cost, CCS units are seen to provide significant
reductions in baseload CO2 emissions at a carbon price below 100$/tC. Also, the ability
to retrofit coal plants for post-combustion CO2 capture is not seen to lower the overall
cost of CO2 abatement (Johnson and Keith, 2004).
Efficient and economical CO2 capture technologies are available for the retrofit of
modern pulverised coal fired power plants. One option is to separate CO2 from the
products of combustion using conventional approaches such as amine scrubbing. An
emerging alternative, commonly known as O2 /CO2 recycle combustion, involves burning
the coal with oxygen in an atmosphere of recycled flue gas. These technologies consume
significant amounts of energy to capture, purify and compress the CO2 for subsequent
sequestration, which make them expensive options. A techno-economic comparison study
was conducted (Singh et al., 2003), and showed that the CO2 capture cost for the MEA
case is 3.3¢/kWh. For the O2 /CO2 case, the CO2 capture cost is lower at 2.4¢/kWh.
These capture costs represent an approximate increase of 20–30% in current electricity
prices (Singh et al., 2001). The CO2 capture system, based on a shift reaction and phys-
ical absorption, in combination with underground or oceanic carbon storage, could be
attractive. Costs are estimated to amount to 10.3–18.8 US$/t CO2 , depending on the iron
production process (Gielen, 2003). Sets of data and comparisons of absorption perfor-
mance and energy requirement for regeneration of various chemical solvents including
monoethanolamine (MEA), diethanolamine (DEA), and methyldiethanolamine (MDEA)
have been provided (Veawab et al., 2003), and the information obtained with respect
to absorption and regeneration has been used to establish the strategy for analyzing the
associated capital and operating costs.
A comprehensive economic study has been carried out on CO2 recovery plants in
the Middle East area for the purpose of enhanced oil recovery (EOR) based on various
parameters which included (i) the capacity of the CO2 recovery unit, (ii) the utility cost,
(iii) the pipeline cost, and (iv) any other operational requirements. The study showed that
CO2 recovery and compression costs from boilers are estimated to be between 0.83 and
1.15 US$/MSCF (16 to 22 US$/ton), which is equivalent to the expected CO2 trading
price in Europe (Iijima and Kamijo, 2003).
The BEAP model and its use for the analysis of biomass policies for CO2 emis-
sion reduction considers competing land use, trade and leakage effects, and competing
emission reduction strategies. Bioelectricity does not gain a significant market share in
case competing CO2 -free electricity options such as CO2 capture and sequestration and
nuclear are considered. To some extent, trade in agricultural food products such as beef
and cereals will be affected by CO2 policies (Gielen et al., 2003). Several bioenergy
processing options were compared based on the specific cost of reduction. The largest
and most long-term sustainable CO2 reduction would be achieved by refining the woody
biomass to fuel pellets for coal substitution, which has been done in Sweden (Wahlund
et al., 2004).
Performance and cost models of an amine (MEA)-based CO2 absorption system for
post-combustion flue gas applications have been developed and integrated with an existing
power plant modeling framework that includes multi-pollutant control technologies for
other regulated emissions. The CO2 avoidance cost for retrofit systems was found to be
generally higher for new plants, mainly because of the higher energy penalty resulting
from less efficient heat integration as well as site-specific difficulties typically encountered
in retrofit applications (Rao and Rubin, 2002).
Conclusion
It is clear that there is no single unique solution for CO2 emissions. Integrating several
technology options may provide the optimum solution for such a complex problem where
the removal of CO2 may cause an increase in other types of gaseous pollutants such as
NOx and SOx . Therefore, there is a great need for further research and developed to
improve CO2 capture technologies and energy saving to lower the cost. Also, further
investigation regarding the reliability and safety of long-term storage remains necessary.
More risk assessment studies are required to look closely at all the possible migration
paths for CO2 from the reservoirs and then develop a detailed understanding of each
migration pathway so that the relative risks of each can be evaluated and compared.
After the Rio summit in 1992, there have been great efforts in developing the proper
scientific understanding of global warming. However, even though many nations adopted
strategies to limit emissions, initially through improved energy efficiency and changes in
fuels, the reality is that the overall cost for real implantation are still likely to be high.
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On: 16 April 2013, At: 13:43

Energy Sources, Part A: Recovery, Utilization, and

Recent Progress in CO2 Capture/Sequestration: A

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Recent Progress in CO2 Capture/Sequestration:

Environmental protection is a critical issue worldwide at the current time. In particu-

Keywords CO2 capture, CO2 sequestration, CO2 storage, capturing technologies,

within the context of power/energy-generation with emphasis on the combustion as-

CO2 Capture and Storage

CO2 Capture Technologies

1. Post-combustion as conventional approach is going through process improvements

Chemical-looping combustion (CLC) with inherent separation of CO2 is considered

Membrane Separation Technology. This technology is expected to attain a high efficiency

injection. The Environmental Protection Agency (EPA) Underground Injection Control

CO2 Cost and Policy Control

possible commercial application for CO2 -sequestration (Hustad, 2001).

Basis. Cambridge: Cambridge University Press.

Technologies, Vols. I and II, Proceedings, 339–344.

Challenges for the Future 912:226–234.

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