The Journal of Supercritical Fluids 132 (2018) 3–16

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The Journal of Supercritical Fluids

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Review

The CO2 economy: Review of CO2 capture and reuse technologies T

a,b,⁎ a a,b
Efthymia Ioanna Koytsoumpa , Christian Bergins , Emmanouil Kakaras
a
Mitsubishi Hitachi Power Systems Europe GmbH, Schifferstraße 80, 47059 Duisburg, Germany
b
National Technical University of Athens, Laboratory of Steam Boilers and Thermal Plants, 9 Heroon Polytechniou, Zografos 15780, Athens, Greece

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

Keywords: The continuously increasing share of Renewable Energy Sources (RES) and EU targets for CO2 reduction and
CO2 capture energy efficiency necessitate significant changes both on technical and regulatory level. Environmental chal-
CO2 utilization lenges of CO2 emissions are assessed in a review of CO2 capture and utilisation technologies, offering new
Power to methanol opportunities in CO2 economy. Commercial applications in the thermal power and industrial sector for pre and
CO2 cycles
post combustion capture as well as the potential of direct air CO2 capture are reviewed. The potential of Carbon
Capture and Utilisation (CCU) is assessed focusing on the use of CO2 for fuel as well as for combined heat and
power production. Combining CCU with energy storage as an evolutionary measure for balancing RES with
thermal power under the power to fuel concept presents high market potentials for fuel and chemical produc-
tion. Moreover, the recent progress in supercritical CO2 cycles for combined heat and power production is
reported.

1. Introduction
The European Union (EU) energy strategy for 2030 and 2050 sets
specific targets for the transition of the current European energy system
towards a low carbon energy system with decreased GreenHouse Gas
(GHG) emissions, increased energy efficiency and increased share of
Renewable Energy Sources (RES). Especially for 2030 a 40% reduction
in carbon emissions and at least a 27% EU-wide share for renewables in
primary energy consumption is foreseen. The overall electricity gen-
eration mix in EU has been following a decreasing trend over the last
few years, as a result of dwindling fossil fuel generation (mainly coal
and gas), with stagnating shares of nuclear and hydro, and a con-
tinuously increasing share of renewables. Different velocities are ob-
served in energy transition of EU Member states with Germany and
Austria to adopt more ambitious targets towards the increase of in-
stalled capacity and production of RES, while other straggle to meet EU
targets. After the 21st United Nations Climate Change Conference in
Paris in 2015, COP21 agreement sets a new benchmark − limit the rise
in global average temperature to well below 2 °C − in order to mobilise
international political response and measures to climate change. It
vindicates the EU’s early efforts and associated legislation to reduce
carbon emissions, and the thermal power industry is ready to tackle the
associated challenges. The old fleet of thermal power plants is not op-
timised for flexible operation. The existing plants are operated now at
very low part-load efficiencies, and therefore both emissions and re-
source consumption are high. So the fleet is not able to contribute to
policy goals. Simultaneously, the increasing of RES cannot be continued
without safety measures and careful considerations. Decreasing fossil
fuel- fired power plant capacity without any countermeasures en-
dangers the security of energy supply, which is challenging in an in-
dustry-based society like EU [1,2]. An insufficient network infra-
structure represents an important barrier for RES, increasing

Abbreviations: BOF, basic oxygen furnace; BTX, benzene, toluene, xylene; CAES, compressed air energy storage; CCS, carbon capture and storage; CCU, carbon capture and utilisation;
CHP, combined heat and power; DAC, direct air capture; DEA, diethanolamine; DEPG, dimethyl ether of polyethylene glycol; DGA, aminoethoxyethanol; DME, dimethyl-ether; DOE,
department of energy, US; DPA, diisopropanolamine; EJ, exajoules; EOR, enhanced oil recovery; EPPSA, European power plant suppliers association; ESA, electrical swing adsorption;
ESI, emirates steel industries; EU, European union; FQD, fuel quality directive; GHG, greenhouse gas; GJ, gigajoules; Gt/y, gigatonnes per year; HECLOT, high-efficiency calcium looping
technology; HTHP, high temperature heat pump; ICEs, internal combustion engines; IGCC, integrated gasification combined cycle; kg, kilogramms; LAES, liquid air energy storag e; LHV,
lower heating value; M100, pure methanol fuel; M15, 15% blend of methanol in gasoline fuel; M50, 50% blend of methanol in gasoline fuel; M95, 95% blend of methanol fuel; MDEA,
Methyldiethanolamine; MEA, monoethanolamine; MeOH, methanol; MHI, mitsubishi heavy industries; MJ, megajoules; MTBE, methyl tert-butyl ether; MTG, methanol-to-gasoline
process; Mtpa, million tonnes per annum; MWe, megawatt electric; MWhe, megawatthours electric; MWhth, megawatthours thermal; MWth, megawatt thermal; NMP, N-methyl-2-
pyrrolidone; OECD, organisation for economic co-operation and development; OMEs, oxy-methylene ethers; PC, propylene carbonate; PCC, post-combustion capture; PPI, pulp and paper
industry; ppm, parts per million; PSA, pressure swing adsorption; PtM, power to methanol; RED, renewable energy directive; RES, renewable energy sources; SMP, system’s market price;
SNG, substitute natural gas; SOFC, solid oxide fuel-cell; TEA, triethanolamine; TOU, time-of-use pricing; TSA, temperature swing adsorption; TTGR-BF, top gas recycle blast furnace; TVS,
temperature vacuum swing; US, United States; vol%, volume percentage; VPSA, vacuum pressure swing adsorption; VSA, vacuum swing adsorption
⁎
Corresponding author at: Mitsubishi Hitachi Power Systems Europe GmbH, Schifferstraße 80, 47059 Duisburg, Germany.
E-mail address: e_koytsoumpa@eu.mhps.com (E.I. Koytsoumpa).

http://dx.doi.org/10.1016/j.supflu.2017.07.029
Received 23 January 2017; Received in revised form 21 July 2017; Accepted 23 July 2017
Available online 25 July 2017
0896-8446/ © 2017 Elsevier B.V. All rights reserved.
E.I. Koytsoumpa et al.
penetration leading to increased levels of curtailment or requiring ad-
ditional back up capacity, which can be provided by thermal power and
combinations of thermal power and energy storage. On the other hand,
the coupling of electricity markets leads to a better utilization of the
energy sources and lower electricity prices, the System’s Market Price
(SMP) reduction is a fact with profound examples that of Germany and
Spain due to the “merit order” effect. All effects of energy policy, in-
cluding rising electricity prices in the consumers’ side, might lead to
awakening of the European economies if no prompt political counter
measures are taken either by Member States or, preferably, on the EU-
level. The increasing share of intermittent RES comes with technical
and market challenges, which need to be faced with flexible thermal
plants, improved RES-technology and reactive power, a Pan-European
overlay grid, transmission technologies with improved grid monitoring,
control and effective energy storage. Although the coupling of elec-
tricity markets in Europe leads to a better utilization of the energy
sources and lower electricity prices, technical challenges need to be
faced. The technology portfolio for high RES Systems is depicted in
Fig. 1.
The main question for the future development of power industry
and electricity markets is the security of supply, the energy efficiency
and the decarbonisation. In the decarbonisation efforts and energy ef-
ficiency, the EU Commission has already set up a roadmap towards
2030 and 2050. The thermal power generation sector has already
performed considerable steps towards reduction of carbon footprint and
increase of energy conversion efficiency and is expected to have a
considerable share in the European generation mix until 2030 [1,2].
The security of supply and the market model are still under investiga-
tion. Two aspects can be highlighted here. First, taxes and policy costs
make electricity artificially expensive to end users, thus hampering
decarbonisation not only via shifting the costs to end users but also by
hindering market incentives for the necessary investments either as
capacity investments or as the deployment of storage technologies
which support both energy efficiency and avoidance of energy cur-
tailment. Secondly, today’s demand side management should be en-
riched for the future high RES system. Additional measures are con-
sidered such as integration of wholesale markets with day-ahead
market coupling and cross-border intraday and balancing electricity
markets. These measures together with grid upgrading, which requires
high investments (transmission lines), cannot currently assure and
guarantee a successful and advanced market design due to the com-
plexity of the algorithm with the combination of centralised, decen-
tralised and smart grid systems. Although price incentives (time-of-use
pricing −TOU) are provided to consumers for the reduction of their
energy self-consumption and/or moderation of their peak demand and
shift of it over time, clearly indicates that shifting the choice to single
4
The Journal of Supercritical Fluids 132 (2018) 3–16
Fig. 1. Technology portfolio in high RES systems.
consumers provides no answer to the security of supply. From the
technical point of view, the existence of dispatchable flexible and back-
up capacity in combination with energy storage technologies is the
future technology responses to secure an efficient energy transition. In
this context, dispatchable and flexible thermal power will provide pri-
marily back-up to RES and will be able to simultaneously provide pri-
mary and secondary control services, supporting grid stability and also
heat to heat grids. Capacity remuneration markets with stand-by
thermal power plants and their balancing with a cross-sectorial ap-
proach of energy shift to heat grids and storage technologies would
allow the development of regional adequacy assessments with cross-
border participation.
The need for energy storage has received significant attention with
several roadmaps to arise in European level as well as in Japan and
China, in California and US [3–7]. Energy storage technologies can be
categorized as electric to electric, electric to heat, electric to chemicals
as well as according to their installed capacity and time response ran-
ging from seasonal, to day, to hour or minute. Energy storage, when
directed to electricity grid, can provide arbitrage services, frequency
regulation, load following, voltage support, transmission and distribu-
tion services, back up reserve services with basic technologies being
represented by pumped hydro, flywheel and compressed air energy
storage (CAES) transform, Liquid Air Energy Storage (LAES) and bat-
teries. However, there is also a variety of energy storage technologies
acting as energy adsorbents and directing the end product to heat and
chemical market. Electric to heat energy storage technologies include
thermal and solar thermal storage either in large scale such as com-
bined heat and power plants, small scale decentralized heat applica-
tions or LAES technologies for heat recovery and electricity generation
in different scales. Electric to chemicals energy storage technologies or
power to fuel technologies include power to hydrogen, power to sub-
stitute natural gas (SNG), power to methanol as well as many other
derivatives directing their end products to chemical market or the
global transportation sector. Focusing on power to fuel, any fuel or
chemical requiring at least one carbon and one hydrogen molecule
enables the combination of energy storage and Carbon Capture and
Utilisation (CCU).
The present work assesses the environmental challenges of CO2
emissions as new business opportunities in a CO2 trans-sectorial
economy. A review of commercial applications in the thermal power
sector and industrial sector for pre and post combustion capture, the
potential of direct air capture as well as the potential of Carbon Capture
and Utilisation (CCU) options are presented. Among those, a special
focus on power to fuel technology is given for the conversion of CO2 to
fuels and chemicals, while the use of CO2 in supercritical cycles for
combined heat and power production is reviewed.
E.I. Koytsoumpa et al.
2. CO2 capture
Carbon dioxide can be captured from different sources according to
its partial pressure, operating conditions and composition of the gas
mixture. Higher concentrations of carbon dioxide allow relatively in-
expensive separation. Carbon dioxide can be primarily available in
every combustion process, being its main product. In thermal power
generation, including fossil fuels, biomass, municipal waste and other
waste to energy plants, carbon is captured after the combustion process
(Post-Combustion Capture-PCC). There are in general two other capture
categories: the oxyfuel combustion capture, where almost pure oxygen
is used in combustion CO2 is recirculated in the oxygen combustion
process and the pre-combustion capture [8,9]. In addition, gasification
technology, when used in Integrated Gasification Combined Cycles
(IGCC) is also included in thermal power generation, offering the op-
portunity of both post and pre- combustion capture [9]. The thermal
power sector has the biggest potential for cutting emissions, whereas
the CCS could play a decisive role. Total OECD (Organisation for Eco-
nomic Co-operation and Development) CO2 emissions in the thermal
sector accounted for 40%, while in the transportation sector for 29%.
Total OECD CO2 emissions from fuel combustion fell by 1.4% to 11.9 Gt
CO2 in 2014 compared to 2007, having remained stable in 2013, from
which oil was responsible for the largest share of CO2 emissions from
fuel combustion (40%) in 2014, followed by coal (33%) and gas (26%)
[10]. Carbon dioxide concentration in air coal combustion may vary
from 12 to 15 vol%, in natural gas combustion from 3 to 10 vol%, while
in fuel oil and biomass from 3 to 8 vol% [11]. Post Combustion capture
of flue gas streams at atmospheric pressure can be achieved by several
physical and chemical separation methods, such as absorption, mem-
branes, adsorption and cryogenic processes. There are several tech-
nologies available for post-combustion capture, which are based on
biological, physical, chemical methods and combination of those [8]. In
the present work, the commercial technologies of post- and pre- com-
bustion capture are assessed.
2.1. CO2 capture in thermal sector
Post-combustion carbon with amine solvents is the most cost ef-
fective and mature technology, which has been demonstrated at full
commercial scale [8,9,12,13]. Solubility of CO2 in solvent with high
cyclic capacity and optimum heat of absorption are required for the
energy intensive post-combustion process with low atmospheric partial
pressures of CO2 in flue gas streams. The general trend of amines in
order of loading capacity is Primary amines < Hindered amines <
Secondary amines < Tertiary amines < Diamines [13]. There is several
progress made on increasing the energy demand for these solvents
based on the use single conventional monoethanolamine with ap-
proximately 4.1 GJ per ton of CO2 captured in the 1980s. The current
commercial processes have significantly reduced the energy demand to
2.6 GJ per ton of CO2 [13]. The state of the art Mitsubishi Heavy In-
dustries (MHI) process, KM-CDR Process® developed together with
Kansai Electric Power Co., Inc., since 1990, has already been im-
plemented in 8 commercial operating plants in 2011, while this number
has been increasing. KM-CDR Process® with the developed absorption
solvent, KS-1™ has an optimum energy consumption of 2.44 MJ/kg CO2
from natural gas boiler flue gases as reported in [14], while the ad-
vantages of KS-1™, KS-2™, KS-3™ developed solvents are presented in
[15,16]. The largest commercial post-combustion capture plant in
power industry in Petra Nova Carbon Capture Project in Texas, United
States uses KM-CDR Process® by MHI as depicted in Table 1. MHI has
also operated a CO2 capture demonstration test facility with a capacity
of 500 t per day from coal derived flue gases, constructed at Southern
Company subsidiary Alabama Power’s Plant Barry in Mobile county,
Alabama, and attained a cumulative CO2 underground storage amount
of 100,000 t. MHI continues technological development for the de-
ployment of the large scale CO2 capture plants reporting an
5
The Journal of Supercritical Fluids 132 (2018) 3–16
improvement of 30 percent or more of efficiency in power generation
compared to competitor’s existing technologies with implementation of
90 percent CO2 capture, waste-heat recovery and MHI’s advanced flue-
gas treatment system [17,18]. Other commercial processes are the
Econamine FG Plus™ technology based on MEA solvent for high oxygen
content flue gases, the Hitachi H3-1 solvent with advantageous antic-
orrosion behavior and 2.4 MJ/kg CO2 energy demand for coal fired flue
gas as well as the Shell Cansolv Technology with the DC-101, DC-103
and DC-103B tertiary amine solvent (simultaneous SO2 and CO2 re-
moval) implemented in today s second largest capture plant in Sas-
katchewan, Canada as presented in Table 1 [19–22]. Sinopec has also
developed a MEA based post-combustion capture which is used at
Shengli power plant, Dongying, Shangdong Province, China [23]. In
addition, the Alstom Chilled Ammonia Process, the Aker Clean Carbon,
the “OASE® blue” BASF process, and the Praxair amine have been de-
veloped [12,24–29]. There is a continuous research effort on the de-
velopment on more efficient solvents to reduce the energy demand to
around 2–1.1 MJ/kg CO2, on the heat integration and optimization of
the process components (eg. modifications in tower packing, optmising
water balance, installation of expanders etc) and to reduce the opera-
tional and capital costs [12,13,29,30].
According to [31], in 2016 15 large-scale CCS projects around the
world, with a CO2 capture capacity of close to 30 million tonnes per
annum (Mtpa) were in operation, while in 2017 further three large-
scale projects, all in the US, will increase the CO2 capture capacity to
35 Mtpa. It is expected that by the end of 2017, the total CO2 capture
capacity will increase to approximately 40 Mtpa with 21 projects.
Table 1 presents the three largest CCS projects in the thermal sector
incorporating post-combustion capture technologies.
2.2. CO2 capture in industry
In industry, there is a high amount of direct CO2 emissions, which
the industries have been trying to tackle with. Industrial energy con-
sumption grew to 152 exajoules (EJ) in 2013, 35% of the global total,
while chemicals and petrochemicals, cement, iron and steel, alumi-
nium, and pulp and paper industry accounted for 68% of industry
emissions [32]. CO2 emissions can vary from 20 to 30% vol dry in Iron
and Steel industry, 14–33% vol dry in cement industry, while in hy-
drogen refineries, it can be found in typical concentrations of 15–20%
vol dry [33]. There are processes such as natural gas processing, am-
monia production and other fertiliser production but also bio-ethanol
fermentation and biogas plants, where CO2 is an inherent component of
the process. [11,32]. Especially in biogas upgrading, the CO2 con-
centration reaches 40–50 vol%, which enables a pre-combustion cap-
ture and separation of CO2 and a high valuable methane rich gas. In
bioethanol and fermentation processes as well as urea/ammonia
synthesis, a nearly pure CO2 stream of around 100 vol% can be found.
[32–35].
The pre-combustion capture refers to separation of CO2 generated as
a co-product of a conversion process. In natural gas reforming and
gasification, pre-combustion is associated with the water gas shift re-
action for converting the carbon monoxide and water to carbon dioxide
and hydrogen and the removal of carbon dioxide. There are several
absorption, adsorption, membrane and cryogenic processes but ab-
sorption processes are the most widely used in commercial applications.
According to the content and composition of the treated gas different
methods for removal are applied usually also used as acid gas removal
for simultaneous separation of carbon dioxide and sulphur species.
Depending on the solvent used, the gas components can be simply
dissolved physically or are bound chemically to the solvent character-
ized as physical or chemical absorption or a mixture of those [36–38].
At low carbon dioxide content, the absorption capacities of chemical
solvents are much higher presenting higher affinity when compared
with absorption capacities of physical solvents, whereas physical sol-
vents provide better results at high partial pressures. Thermal energy
E.I. Koytsoumpa et al.
Table 1
The three largest CCS projects in thermal power sector [18–22].
Project Name Boundary Dam Carbon CCS Project–the Saskatchewan
Government is the sole owner
Project Location Saskatchewan, Canada
Industry Power generation (lignite/brown coal)
CO2 Capacity 1 million tonnes per annum (Mtpa)
CO2 Technology PCC Amine Shell Global, Cansolv technology
Start Date October 2014
Storage Aquistore project − Winnipeg and Deadwood
formations at 3.4 km/2.1 mile depth
EOR Weyburn Oil Unit − oil-bearing formation at 1.5 km/
1 mile depth
requirements for chemical solvents are much higher than those for
physical solvents due to the addition of heat through the reboiler of the
stripper column [37]. In physical solvents, the loading capacity of the
solvents is in a virtual linear dependency between the partial pressure
of the component to be removed and the solvent loading according to
Henry’s law, allowing its regeneration by pressure throttling. The dis-
solution of carbon dioxide in the physical liquid solvent is attributed to
the van der Waals or electrostatic interaction and is optimal at high
pressure and low temperature [37,38]. Depending on the presence of
sulphur species, the regeneration of the physical solvent might also
demand heat for the reboiler duties [39–41]. Two stage processes are
also used for the chemical solvents such as the HiPure Process [42].
Among the physical processes, solvents such as DEPG (Dimethyl Ether
of Polyethylene Glycol), MeOH (Methanol), NMP (N-Methyl-2-Pyrroli-
done) and PC (Propylene Carbonate) are used. The state of the art
processes are Selexol®, Rectisol®, Purisol®, Morphysorb®, Fluor® [37–42].
Among chemical solvents, primary amines such as monoethanolamine
(MEA), secondary amines Diethanolamine (DEA), Aminoethoxyethanol
(DGA) and Diisopropanolamine (DPA) and tertiary amines such as
Triethanolamine (TEA) and Methyldiethanolamine (MDEA), Ucarsol® as
well as alternatives to amines such as hot potassium carbonate are used.
Among hot potassium carbonate processes, Benfield®, Catacarb®,
Giammarco-Vetgrocoke® and Vacasulf® processes exist. In addition,
mixtures of chemical solvents or physical and chemical solvents can be
also used such as in commercial solvents OASE® (aMDEA®), Amisol®,
Sulfinol-D® and Sulfinol-M®. Flexsorb® also uses hindered amines
[37–43]. The composition of the treated gas, the selected operating
process parameters of the scrubbing technologies as well as their stages
and heat integration may present significant differences in the energy
demand. In [37], an energy penalty of 7.64–14% is reported for natural
gas pre-combustion technology based on commercial CO2 separation
systems. Minimum electricity demand as reported in [36] for DEPG and
MeOH solvents at 97% CO2 capture without pre-compression from coal
steam gasification at 20 bar is around 0.3 MJ/kg CO2, while in [39] and
[40] for DEPG without considering CO2 compression and at 90% CO2
capture from coal gasification at 35 bar an electric demand of around
0.16 MJ/kg CO2 is reported. For the heat demands for DEPG around
0.12 and 0.29 MJ/kg CO2 is reported respectively in [39] and [40]. For
potassium carbonate and MDEA at 97% CO2 capture from coal steam
gasification at 20 bar, a heat duty of 1.99 and 1.77 MJ/kg CO2 and an
electricity consumption of around 0.05 MJ/kg CO2 is reported in [36].
Due to the wide field of applications and the diversity of conditions, no
further review on the energy demand is presented.
Chemical and petrochemical industry generates as basis olefins (C2-
C4) such as ethylene, propylene, generally obtained from hydrocarbon
feedstocks using steam cracking, aromatics (C6-C8) such as benzene,
toluene, xylene (BTX), generated using steam cracking of catalytic re-
forming which are further processed into a wide range of plastics,
The Journal of Supercritical Fluids 132 (2018) 3–16
Petra Nova Carbon Capture Project Sinopec Shengli Power Plant CCS Project
Texas, United States Shengli power plant, Dongying, Shangdong
Province, China
Power generation − pulverized coal boiler (sub- Power generation − pulverized coal boiler
bituminous coal)
1.4 million tonnes per annum (Mtpa) today 40,000 t per annum of CO2, Scale up to: 1
million tonnes per annum.
PCC KM-CDR amine scrubbing CO2 developed by PCC SINOPEC
MHI and KEPCO
2016 2010–2017
No No
Frio Formation (sandstone) 1640–2066 m/ Injection is at 3 Km depth into the Shengli oil
5000–6300 feet below ground surface field in the Yellow River delta.
rubbers, resins, solvents and other petrochemical products, and also
synthesis gas based chemicals such as ammonia, methanol, hydrogen,
carbon black, sulphur etc. For the production of synthesis gas based
chemicals as well as for hydrogen production, pre-combustion capture
is often used after water gas shift reaction which moderates the hy-
drogen to carbon ratio for the subsequent synthesis [36–38]. According
to [31], among the operating commercial CCS projects, the majority has
found application in natural gas processing, fertiliser and hydrogen
production implementing pre-combustion technologies. The initial vo-
lume fraction in syngas derived via solid fuel gasification may vary
according to the fuel, the stoichiometric ratio, the operating pressure
and temperature and the oxidation agent but typical values are in the
range of 5–30 vol dry% before the water gas shift reaction [36,44–47].
Natural gas reforming is conventionally performed via steam reforming,
partial oxidation, autothermal reforming, dry reforming of methane,
but also via combined reforming of methane, reforming with mem-
brane, tri-reforming of Methane. In dry reforming, waste carbon di-
oxide is used to reform natural gas to syngas with a low H2/CO ratio
(≈1.0) which can be preferentially used for production of liquid hy-
drocarbons in Fischer-Tropsch and DME synthesis with the aim of re-
duction in thermal energy consumption required by steam generation
[48]. In ethylene production from gaseous, liquid or other feedstocks,
carbon dioxide is reduced down to 2 ppm and hydrogen sulfide is re-
moved simultaneously from the cracked gas by acid gas removal sys-
tems (such absorption in caustic wash and regenerative alkanolamines
solvents) in order to avoid formation of ice and hydrates in the sub-
sequent fractionation steps. In steam crackers, depending on the raw
feedstock 1–1.6 ton of CO2 per ton of ethylene is produced, while in
comparison to bioethanol derived ethylene, CO2 emission per ton of
ethylene are lower by 60% [49]. In Canada, Shell, on behalf of the
Athabasca Oil Sands Project venture is capturing more than 1 million
tonnes of CO2 per year using ADIP®-X process. The Scotford upgrader
turns thick heavy oil from the oil sands bitumen into synthetic crude for
further refining to gasoline and jet fuel cell using hydrogen to upgrade
to lighter oil from the Scotford oil sands bitumen. This is the largest
capture and storage project in oil industry operating since 2015 redu-
cing Scotford plant’s direct CO2 emissions by up to 35% [50,51]. In the
Tomakomai project, CO2 capture with amine scrubbing is operating at
an oil refinery, which produces high purity hydrogen for hydrotreating
via PSA system. The PSA offgas, contains H2, CH4, CO and a large
amount of CO2 in 44–59% volume. This is Japan’s first CCS project
capturing 100.000 tonnes of CO2 per year lead by Japan CCS Co. Ltd
which group of major companies with expertise in CCS-related fields,
including electric power, petroleum, oil development, and plant en-
gineering [52]. The Gorgon project has started operation in 2016 cap-
turing CO2 from the Gorgon Field gas (14% vol CO2) and the Jansz-Io
field gas (0.15% CO2) in order to be separated from the natural gas
stream prior to further gas processing and liquefaction. This is the
6
E.I. Koytsoumpa et al. The Journal of Supercritical Fluids 132 (2018) 3–16

world's largest operating sequestration project in gas industry capturing

Capture capacity (Mtpa) 3.4–4 million tonnes CO2 per year using ADIP®-X [53]. In Coffeyville
project, 1 million tonnes per annum (Mtpa) are captured using the
Selexol process at a petroleum coke-based nitrogen fertiliser production
process at Kansas, US. Synthetic gas is produced from the petroleum

0.3–0.6
1.2–1.4
3.4–4.0
coke gasification, from which ammonia and urea ammonium nitrate
1.3
0.7

0.9

0.7
8.4

0.9

0.8
0.8
(UAN) fertilisers are subsequently synthesised. The capture CO2 after
7

1
1

1
1

1
3
compression and dehydration is injected into the North Burbank Unit
(natural gas processing)

(natural gas processing)

(natural gas processing)

(natural gas processing)

(natural gas processing)

(natural gas processing)

(natural gas processing)

(natural gas processing)

(natural gas processing)

for enhanced Oil Recovery. In the Enid project in Oklahoma US, am-
monia, liquid fertiliser and Urea are produced providing a high purity
CO2 using Selexol process which is dehydrated, compressed and
(gasification)

(gasification)
transported for enhanced Oil Recovery in a capacity of 680,000 t of CO2
per annum [54]. An overview of the largest CCS projects in the in-
dustrial sector according to [54] is presented in Table 2.
Among the three leading technologies in Steel Industry, Basic
Pre-combustion capture

Pre-combustion capture
Pre-combustion capture
Pre-combustion capture
Pre-combustion capture
Pre-combustion capture

Pre-combustion capture
Pre-combustion capture

Pre-combustion capture

Pre-combustion capture

Pre-combustion capture
Oxygen Furnaces (BOF) with Blast Furnace (BF) shares the 69% of
Industrial Separation

Industrial Separation
Industrial Separation

Industrial Separation

Industrial Separation
Industrial Separation
Industrial Separation

Industrial Separation
worldwide steel production and will remain dominant as it is the most
cost-effective route of virgin ore steel production for high added value
Capture type

products. Other technologies are FINEX® and COREX® processes, the

smelting reduction (SR), coal based Direct Iron Reduction (DRI) and gas
based DRI (Midrex, HYL/Energiron). Worldwide, there are few pilot
scale facilities using CO2 capture in Steel Industry (HYL/Energiron)
[55]. In 2003, the World Steel Association launched the ‘CO2 Break-
Iron and Steel Production
Natural Gas Processing

Natural Gas Processing

Natural Gas Processing

Natural Gas Processing

Natural Gas Processing

Natural Gas Processing

Natural Gas Processing

Natural Gas Processing

Natural Gas Processing

Synthetic Natural Gas

through Programs’, with research and development being done in the

Hydrogen Production

Hydrogen Production

Chemical Production
Fertiliser Production

Fertiliser Production

Fertiliser Production

Power Generation

EU (ultra-low CO2 steelmaking, or ULCOS I and ULCOS II), in the US, in

Canada, in South America, in Japan (Course 50), in Korea, China and
Oil Refining

Taiwan, and Australia [55–57]. Blast Furnace Technology is directly

Industry

connected with the use of coal which is processed in the coke plant,
while studies on substituting coke in a certain extend via pulverized
coal or natural gas or even oil, tar, biomass and waste plastics have
Operation date

been performed. In ULCOS BF, Top Gas Recycle Blast Furnace (TGR-
BF), the Hisarna technology (combination of a hot cyclone and bath
smelter HIsarna based on HIsmelt process), the direct reduction process
1972
1982
1986
1996
2000
2008
2010
2013
2013
2013
2013
2015
2015
2016
2017
2017
2017
2017
2017

ULCORED as well as two electrolysis variants ULCOWIN and ULCO-

LYSIS were investigated. The TGR-BF involves the replacement of host
United Arab Emirates

blast with oxygen and the recycle of top gas with the CO2 removal. The
technologies for CO2 removal involve Pressure Swing Adsorption (PSA),
Vacuum Pressure Swing Adsorption (VPSA) and amines. The total en-
United States
United States
United States

United States
United States
United States
United States

United States
United States
Saudi Arabia

ergy demand required including compression work as reported in [55]

Australia
Location

Norway

Norway
Canada

Canada

Canada
Canada

is 1.12, 1.05 and 3.81 MJ/kg CO2 for Pressure Swing Adsorption (PSA),
Brazil

Vacuum Pressure Swing Adsorption (VPSA) and amines respectively.

The world’s first commercial carbon-capture steel project, the Al Rey-
Alberta Carbon Trunk Line (“ACTL”) with North West Sturgeon Refinery CO2 Stream

adah − Masdar Abu/Dhabi National Oil Company project, has started

operation in Abu Dhabi. Amine scrubbing is used to capture CO2 from
an off stream from the Emirates Steel Industries (ESI) Factory with a
capacity of 0.8 million tonnes per annum. After compression and de-
hydration at Al Reyadah, it is injected into onshore oil fields for en-
hanced oil recovery [38,54].
Alberta Carbon Trunk Line (“ACTL”) with Agrium CO2 Stream

CO2 is a by-product of the cement manufacturing process as the raw

material (limestone) used in cement manufacturing accounts for
Great Plains Synfuel Plant and Weyburn-Midale Project

roughly two thirds of the total CO2 emitted from the cement plant. The
Illinois Industrial Carbon Capture and Storage Project
Petrobras Santos Basin Pre-Salt Oil Field CCS Project
Air Products Steam Methane Reformer EOR Project

other third derives from the combustion of fossil fuels to obtain the heat
required for the limestone decomposition process [58]. Pre-combustion,
The largest CCS projects in industrial sector [54].

Uthmaniyah CO2-EOR Demonstration Project

post-combustion and direct capture as well as oxyfuel are currently

Gorgon Carbon Dioxide Injection Project

being considered [59–62]. Pre-combustion is related to new integrated

gasification technologies for produce syngas production and hydrogen
Shute Creek Gas Processing Facility

firing in the cement kiln without CO2 capture from the calcination
Enid Fertilizer CO2-EOR Project

Kemper County Energy Facility

process. On the other hand, post-combustion capture has many retro-

Val Verde Natural Gas Plants

Coffeyville Gasification Plant

Sleipner CO2 Storage Project

Snøhvit CO2 Storage Project

ffitting options with lower costs and higher emission reduction, while
Abu Dhabi CCS Project

the replacement with new highly efficient power plants is also a con-
Lost Cabin Gas Plant

sidered configuration [61]. Pure oxygen combustion in oxyfuel requires

major modifications to burner design, kiln, and new plant configuration
Century Plant
Project name

[59–62]. In [61], a categorization according to the technology readi-

ness level has been made for 5 different technologies, with post-com-
Table 2

Quest

bustion capture to has the highest level due to its existing applications
in thermal power industry. Post- combustion capture in cement

7
E.I. Koytsoumpa et al.
industry has a considerable advantage compared to the thermal power
sector due to the higher CO2 concentration of 14–33% [62]. The pilot
plant in Brevik, Norway with different capture technologies is the most
developed project in cement industry [61]. The main infrastructure
includes amine scrubbing from Aker Solutions, whereas Alstom’s re-
generative carbonate cycle and sorbents from the Research Institute
Triangle and Membrane technology have been developed [58]. In ad-
dition, the High-Efficiency Calcium Looping Technology (HECLOT)
capture project by the Industrial Technology Research Institute
(Taiwan) and Taiwan Cement is in operation capturing 1 ton CO2 per
hour [63], while Skyonic has an operational pilot facility in San An-
tonio, Texas, US. Capitol SkyMine is expected to capture 75,000 tonnes
annually from the coal-fired Capitol Aggregates Cement plant and uti-
lising the CO2 towards the production of hydrochloric acid, baking soda
(sodium bicarbonate) and bleach. The SkyMine® process claims a 30%
energy reduction compared to amine-based CO2 capture [64].
In pulp and paper industry, mechanical mills and integrated Kraft
mills are commonly used. Kraft mills in Europe have the highest share
of European PPI emissions and thus the Kraft PPI plants and thus the
largest potential for capture of CO2. Emissions can arise from the bark
boiler, the black liquor and from the lime kiln, thus it can be biogenic or
not depending on the fuels used [65]. Depending on the installation,
CO2 emissions from pulp and paper mills are scattered around the site
in several stacks, but emissions from the recovery boiler are usually
considered with concentrations varying from 10 to 20 vol% [66]. The
advantage of capture in Kraft mills is the biogenic emissions from the
recovery boiler [66] considering post-combustion technologies, while
pre-combustion can be used in the gasification of the black liquor
[67,68].
2.3. Direct CO2 capture from air
Carbon dioxide is also available in air with concentration in the
range of 399 ppm in 2015 according to [69]. Although the low con-
centration of CO2 in air requires the treatment of high volumes, there
has been several interest [70]. Direct carbon dioxide (DAC) absorption
from atmospheric air has been investigated since half a century [71,72]
and has been applied in cryogenic oxygen separation plants, space craft,
and submarines [73]. DAC can be achieved with organic capture, with
production of metal carbonates and with the use of sorbents
Organic carbon reduction with organisms, which naturally capture
CO2 through photosynthesis, is fundamentally limited to one-time re-
ductions. Alternative solutions such as ocean flora creating plankton
has also been investigated with limited success [74]. Steel slag and
waste concrete with calcium and magnesium oxides, have also been
suggested as air carbon sequestration materials forming solid carbo-
nates [74,75]. According to [75], the total annual production of con-
crete and steel could capture less than 1% of U.S. emissions. For larger
quantities, regenerative materials are investigated for direct air capture.
Fans driving air counter-currently through convective towers and
packed scrubbing towers with sodium hydroxide solutions have been
suggested for the direct carbon dioxide absorption from atmospheric air
[76–78]. In [79], spray towers have also been suggested. The main
principal is the absorption of CO2 into a solution of sodium hydroxide
and its conversion to an aqueous solution of sodium hydroxide and
sodium carbonate focusing on optimum conditions at the contact of the
components. However, the sodium carbonate has to be regenerated in a
closed loop process and converted again into sodium hydroxide, via the
causticization processes using lime. In [77] the capture ratio is only
50% capture rate based on CO2 concentration of 380 ppm in air. In [80]
and [81], a comparison of air capture and post combustion capture is
made. In [80], for a capture ratio of 25% for both processes the cross
sectional area required for air is higher by a factor of 3.6, while the
amount of air processed would be over 1000 times that of flue gas
capture for an equivalent amount of CO2. This provides an indication on
the capital costs and energy requirements. Respectively in [81], the
8
The Journal of Supercritical Fluids 132 (2018) 3–16
DAC reference plant with a capacity of 1 MtCO2 annually or equivalent
to a 150 MWe supercritical power plant based on a scheme published by
[78], requires around 330 absorbers, resulting in a total absorber cross
section of 37,000 m2. Comparing the energy demand, the afore men-
tioned process, requires a minimum thermodynamic energy limit of
179 kJ/mol CO2 for the conversion of calcium carbonate to lime and
109.4 kJ/mol CO2 for the conversion of sodium carbonate to sodium
hydroxide [82]. In [81], the net thermal energy requirement for the
DAC plant is estimated at 6.1 GJ for each ton of CO2 captured, which
means that combusting natural gas with 75% thermal efficiency for
providing high temperature heat results in a total thermal energy input
of 8.1 GJ per ton of CO2 captured. In addition, the total electricity re-
quirement is also reported in [81] equal to 1.78 GJ per ton of CO2
captured. However, the authors in [82] suggest the regeneration of
NaOH via direct causticization using titanate. They report that half of
the energy is required, as the heat requirement of the proposed process
is equal to 135 kJ/mol and similar to MEA requirements. In [83], en-
ergy requirements as high as 500–800 KJ/mol CO2 are reported.
Adsorption technology for CO2 capture receives more and more
attention due to its potential of lower energy consumption.
Temperature swing adsorption (TSA), temperature-vacuum swing
(TVS), pressure swing adsorption (PSA), vacuum swing adsorption
(VSA), and electrical swing adsorption (ESA) are considered for treat-
ment of feed gases with various CO2 concentrations [84]. As the ad-
sorption material plays a key role, a lot of research is going on different
materials with zeolites, metal-organic frameworks (MOFs), amine
modified adsorbents to receive significant attention. DAC with ad-
sorption of CO2 has also been investigated. The adsorption capacity of
carbon-based materials and MOFs is strongly pressure dependent and
decreases with at low partial pressures as the CO2 concentration in air
[85]. The adsorption capacity of activated carbons is low, while the
presence of water highly influences the selectivity of zeolites [86]. The
combination of chemical and physical adsorption in amine functiona-
lized mesoporous supports has received several attention for DAC
[84–91]. In [89], the specific energy requirements of the TVS adsorp-
tion process studied vary according to the air relative humidity and are
estimated to be 12.5 kJ/mol CO2 of mechanical work and between 493
and 640 kJ/mol CO2 of heat for operation below 100 °C. In [90], cap-
ture ratios of 90% and 99% purity are reported. In [91], the authors
have tested amine-grafted mesoporous adsorbents and reported the
formation of urea groups which decreased the adsorption capacity due
to thermal desorption. New startups such as Climeworks, Global Ther-
mostat and Carbon Engineering have been emerged deploying air CO2
capture technologies [92–94].
3. CO2 utilisation
Carbon Capture and Utilisation (CCU) explores the use of carbon
dioxide in applications other than storage. Carbon dioxide is already
used in a variety of sectors and processes as presented in Table 3.
Especially the enhanced oil and gas recovery has the highest potential
for near term CCS in specific areas [95]. Although, it imposes geo-
graphical constrains the same as the storage sites which are not viable
for all CO2 emitters, thus other options are investigated [96]. The
European Commission has launched several relevant calls within Hor-
izon 2020 (SPIRE, BIOTEC, LCE 25, NMBP 19 and 20) to support re-
search on CO2 utilisation as a viable approach for sustainable produc-
tion of fuels, chemicals and intermediates [97]. Several European
initiatives have been started to develop CO2 reuse technologies [98],
while in US the Department of Energy support also the research within
the Carbon Use and Reuse technology areas [96]. Utilization of CO2
finds applications in the chemical, oil and power sector, in the food,
pharmaceutical sector, in pulp and paper industry, in steel industry as
well as other uses. Its use can be categorized to resource recovery (e.g.
Enhanced Oil and Gas Recovery, Enhanced Coal-Bed Methane Re-
covery), captive (process integrated) using CO2 as an intermediate
E.I. Koytsoumpa et al. The Journal of Supercritical Fluids 132 (2018) 3–16

Table 3 up to 300 Mtpa in [95]), the urea production, the polymer processing as
State of the art carbon dioxide utilization [75–80]. well as in fuel and chemical synthesis such as renewable methanol,
formic acid. The cement sector has also a great uptake potential of up to
Sector Process/Product Potential
300 Mtpa in [95,104], In the food sector, a medium potential exists
Chemical and Oil Enhanced Oil Recovery High basically for beverage carbonation, packaging, decaffeination and
Enhanced Gas Recovery horticulture.
Enhanced Coal bed Methane Recovery
In the power sector, if supercritical CO2 cycles are not only limited
Stimulation/Fracturing of oil and gas
Urea production to today’s existing applications of geothermal plants and heatpumps, a
Polymer Processing broad market is to be expected for future potential applications ranging
Chemicals and Fuels (Methanol, methane, from nuclear, coal, biomass and natural gas, waste incinerator plants as
CO, fertilisers etc and derivatives) well as in small combined heat and power applications [95,96,99–101].
Food Beverage Carbonation Medium
In the present work, a focus is made on the CO2 utilisation related to the
Coffee Decaffeination
Wine production power sector focusing on chemical and fuel synthesis via power to fuel
Food processing technology and on using CO2 in supercritical cycles.
Food preservation
Food packaging (Modified or controlled
3.1. CO2 utilization and energy storage under power to fuel technologies
atmosphere packaging)
Dry Ice Production
Horticulture (greenhouses) Power to fuel refers to Power to gas, either hydrogen or SNG or in
Refrigeration the production of other liquid fuels such as methanol, dimethyl-ether
Mineralisation Calcium and Magnesium carbonate for use in Medium (DME), oxy-methylene ethers (OMEs), other chemicals and derivatives.
cement
As a mean of energy storage, the electrolyser technology simulta-
Baking soda
CO2 concrete curing neously converts water to hydrogen via use of electricity and also
Bauxite residue treatment (red mud) provides grid balancing services. Although the electrolyser technology
Power Heat pumps Low-Medium of alkaline electrolysers is mature, the lack of existing infrastructure
Working medium in other CO2 cycles
and its capital intensity as well as safety issues are prohibiting its wide
Energy crops Algae cultivation (biomass production via Medium
photosynthesis)
use for power to hydrogen applications. The combination of CO2 uti-
Pharmacheutical Inerting Low lisation and energy storage is realized under Power to Fuel technology,
Chemical synthesis where captured CO2 and the produced hydrogen are mixed and com-
Supercritical Fluid Extraction pressed before inserted in catalytic reactors [105]. Power to SNG in-
Product transportation
cludes the production of methane in catalytic reactors [11]. The prices
Pulp and Paper pH reduction during Washing Low
Steel Injection to metal casting Low of fossil natural gas prohibit the merge of electricity market with nat-
Bottom stiring agent in BOF furnaces ural gas market as a high utilisation factor reflect operation in high
Chilling medium electricity prices mitigating the elevated costs to the end product [105].
Hardening sand cores and moulds
Methanol production via the use of carbon dioxide and hydrogen
Other Electronics (in printed circuit manufacture) Low
Pneumatics (working medium in hand tools
produced via water electrolysis has been demonstrated at the produc-
and equipment) tion plant of 4000 tons of methanol from CO2 per year, George Olah
Welding (shield gas) plant at Svartsengi, Iceland, built and operated by Carbon Recycling
Fire extinguishers, fire suspension International. The process for the conversion was described before
Flavors, Fragnaces
[104] and can reach conversion efficiencies of > 60% from electricity
Blanket Products
Aerosol can Propelant to CO2 derived methanol lower heating value depending on the appli-
Inert gas cation. The integration of the methanol technology with a power plant
Soda ash production for glass industry and flexible operation will be further demonstrated in an ongoing EU
Dry gas cleaning funded project, MefCO2 (Grant agreement 637016) [105]. The wide
Water treatment
Refrigerant gas
application of power to methanol (PtM) technology in power, chemical
and steel industry and its high potential of use in large automotive
market contributes to CO2 emission reduction and offers grid balancing
product in the manufacturing chain without external sources and the services. A large-scale commercial methanol plant connected to the
non-captive or merchant use [95,96,99–101]. As reported in [95], the grid, able to produce 50,000 to 100,000 t/annum methanol (based on
order of magnitude for CO2 reuse is very pertinent with the global non 8500 full load hours) requires thermal energy of 1.01 MWhth/ton
captive consumption to be estimated at approximately 80 Mtpa, while methanol and electric energy of 9.74 MWhe/ton methanol based on
only urea production in the global captive consumption reaches alkaline electrolyser with an efficiency from an Alternating to Direct
113 Mtpa. The worldwide urea production required 112–120 Mtpa CO2 Current of 4.4 kWhe/Nm3 of H2 produced. If the heat is provided from a
and was estimated to grow up to 176 Mt by 2016 as given in [102,103]. power or Combined Heat and Power (CHP) plant, the corresponding
CO2 utilisation has an estimated potential of at least 3.7 Gigatonnes per amount of electricity not produced but consumed as heat for covering
year (Gt/y), which is equal to about 10% of the world’s current annual. the thermal demands of the CO2 Capture is 0.15 MWhe/ton methanol
It is expected to produce revenues coupled with favourable CCS projects (based on 15% losses at the specific heat extraction conditions for
in developing economies, releasing some of the pressure on the energy covering the thermal demands of the CO2 Capture). The total energy
costs and abatement and aiming at value-added products that create demand in units of electrical energy is therefore 9.89 MWhe/ton me-
jobs and economic benefits [99]. In [104], CO2 utilisation potential has thanol. The configuration of the existing power plant and the PtM plant
been evaluated at around 300 Mtpa. The Global CO2 Initiative presents is shown in Fig. 2. Integration with power or CHP plants can involve
an annual market on CO2-based products of 0.8–1.1 trillion dollars via only extraction of flue gas and provision of heat extracted from the
using over 10% of annual global CO2 emissions. steam cycle in order to cover the reboiler needs of post-combustion
The highest potential and market size for CO2 utilisation is identi- capture. The techno-economics of this scale are highly influenced by a)
fied in the chemical and oil industry, with the Enhanced Oil Recovery the final methanol price as well as by b) regulations concerning elec-
(EOR) to have the greatest potential for non captive demand (estimated tricity market, c) fuel and chemical market and specifically by d) the
Renewable Energy Directive (RED) and e) Fuel Quality Directive (FQD)

9
E.I. Koytsoumpa et al.
Fig. 2. Power to Fuel integrated in thermal plants.
for non-biological sources. Both the original RED and FQD set ambi-
tious targets on the decarbonisation of the transport sector which put
pressure on the fuel market to fulfil the stricter sustainability criteria on
a scale that matches fossil fuels. Therefore, low carbon electricity
should be used for the production of the low carbon fuel.
On the other hand industrial must-run CHP plants in industry and
connected to heating grids suffer from decreased demand for electricity
while they have to burn by-products like off-gases from steel industry or
wood waste from wood and pulp and paper industry and/or have to
deliver steam or heat to industry and the heating grids. In such cases,
optimum boundary conditions exist for implementation of power to fuel
as except from the available CO2, the necessary infrastructure also ex-
ists such as heat source/sink and connections to the grid. If other low
carbon electricity is available, the heat export can be increased by using
electrolyser waste heat and a high temperature heat pump (HTHP) for
steam production increasing the efficiency [106]. This way must-run
power plants can create new business by providing methanol and in
parallel enable more renewables to be installed and/or avoid curtail-
ment in conjunction with new transmission lines and optimally de-
signed grid upgrades. Additional advantages arise from the sales of grid
services, nearby consumers of oxygen like steel-industry. In Fig. 3, the
integration of power to fuel technology −focusing on methanol pro-
duction- in CHP systems for future applications is presented.
Although methanol is already used for fuel blending, for Methyl tert-
butyl ether (MTBE) production for biodiesel production, other path-
ways for the introduction of low carbon fuel are available such as the
conversion of methanol to drop-in fuels. Drop-in fuels can be used pure
or can be blended with gasoline for use in existing internal combustion
engines (ICEs). Examples are oxygenates like dimethyl-ether (DME) and
Fig. 3. Power to Fuel integrated in CHP systems.
10
The Journal of Supercritical Fluids 132 (2018) 3–16
oxy-methylene ethers (OME) [107]. DME can easily be manufactured
from methanol with proven technology, but is not liquid at ambient
temperature and therefore requires a separate distribution infra-
structure with pressurised tanks. OME production processes are still
under development. The methanol-to-gasoline process (MTG) on the
other hand is well developed and used in large scale but as also men-
tioned for OME-, it has lower overall efficiency than direct use of me-
thanol or DME [107–110].
Direct methanol use as blend with high methanol content 50–85%,
in ICEs is possible in flex-fuel engines or as M100 (pure methanol) in
dedicated methanol engines. After fleet tests of methanol cars in Europe
and the US [111] in the 80s triggered by the oil crisis, the R & D ac-
tivities slowed down in a phase of low oil prices. Having urgent need
today for the reduction of emissions in the transport sector new activ-
ities are started for methanol as a clean alternative [105]. Due to the
absence of carbon–carbon bonds in the methanol molecule, soot for-
mation is avoided, resulting in virtually zero values. The absence of
sulphur in the fuel leads to inherently zero sulphur emissions from pure
methanol combustion. The lower flame temperature of methanol also
results in inherently lower NOx emissions. Even at higher compression
rates enabled by methanol’s wider knock limits and allowing highest
ICE efficiency, lower levels of NOx emissions are achievable compared
to gasoline [112]. In Europe, a 3% blend of methanol in gasoline is
standardized for SP95 gasoline in DIN EN228. Some countries in-
centivise blending or use of low carbon methanol in biodiesel produc-
tion, and in the UK no road taxes are applied to M95 (95% methanol).
Australia has a similar initiative with reduced road taxes for methanol.
In Sweden, unblended methanol is also utilised as zero sulphur marine
fuel. China has sold a 15% blend of methanol in gasoline (M15) as
E.I. Koytsoumpa et al.
automobile fuel in several provinces and fleet tested 100% methanol
(M100) in eleven major cities. In Iceland, Carbon Recycling Interna-
tional has conducted fleet testing of at 50:50 blend of methanol and
gasoline (M50) in flexible fuel vehicles from Ford and is now testing
M100 with vehicles from Chinese automobile manufacturer Geely
[106,113].
In future fuel cell cars based on methanol can enable the highest
well-to-wheel efficiencies compared to all other synthetic fuels with
Ballard, SFC Energy and Serenergy to have already commercialized the
technology. Serenergy in Denmark is delivering methanol fuel cell
systems as range extenders for electric cars [114,115]. Nissan started
testing of bio-ethanol fuel cell (Solid Oxide Fuel-Cell, SOFC) cars in
2016 [116].
Although the final value of the carbon footprint reduction depends
on the specific application and the CO2 footprint of the electricity used,
there are several aspects of environmental protection and economic
benefits associated with PtM. Carbon dioxide is captured and reused for
replacing fossil fuels and their respective emissions from exploration,
transport and processing reducing NOx, SOx and soot emissions in the
transportation sector as well as the energy dependency in Europe in a
sustainable and economic way.
3.2. CO2 as working medium
Waste heat streams are generated mainly by exhaust gases in boi-
lers, ICES, kilns, furnaces, ovens, turbines, engines, and other equip-
ment in the thermal and process industry, as well as in mines and other
sites including residential sites [117]. The EU Energy Efficiency Di-
rective includes a comprehensive assessment of the national potential of
cogeneration and district heating and cooling in each EU member state.
According to 2012, a target of 20% energy efficiency target by 2020,
while since November 2016, an update was proposed for a target of
30% energy efficiency target by 2020 [118]. Waste heat can be utilized
to produce electricity (waste heat to power) or mechanical work, to
produce warm water or steam increasing the energy efficiency. The
economic feasibility for waste heat recovery declines as the tempera-
ture and flow rate decline. Thermodynamic cycles such as Rankine,
steam Rankine cycle (SRC), organic Rankine cycle (ORC), Kalina cycle,
and supercritical carbon dioxide (CO2) cycle are used [117].
Another application of CO2 is its use as a working fluid in cycle
processes. Carbon dioxide has been used as a working medium in
transcritical and supercritical processes. In transcritical processes, CO2
has been used in refrigeration and heat pumps in commercial scale with
increasing market in households and industry applications. A review of
different transcritical cycles and applications is presented in [119].
Especially domestic scale CO2 heat pumps have found many applica-
tions in the water heating industry because of their ability to deliver
significantly more heat for the same amount of electricity compared to
traditional electric storage water heaters installations. The market share
of CO2 as a natural refrigerant was 35% in 2012, with Japan to have
established a mature market with Ecocute system [120,121]. According
to [122], the ESA30-25 CO2 refrigerant heat pump water heater has
achieved the industry’s highest COP of 4.3 for a 30 kW application.
Modular heat pump units can be assembled together to reach higher
scales. In industrial heat supply, today’s heat pumps can produce hot air
up to a temperature of 120 °C and steam up to 165 °C replacing boilers
in many industrial processes [123].
3.3. Supercritical CO2 brayton cycles
In supercritical processes, CO2 has been used in supercritical CO2
Brayton cycles for producing electricity in industrial medium scale
applications. Different pilot plant systems are being tested in the US,
Japan and Korea [124]. Echogen and Dresser Rand have commercia-
lized the technology developing a compact system with a maximum net
electricity output of 8 MWel and a process efficiency up to 30% [125].
11
The Journal of Supercritical Fluids 132 (2018) 3–16
NET Power is commercializing a new thermodynamic cycle, the Allam
Cycle, named for its lead inventor, Rodney Allam- using a high-pres-
sure, highly recuperative, oxyfuel, supercritical CO2 cycle with in-
corporated CO2 capture. NET Power, CB & I, Toshiba, and Exelon have
partnered to develop a 50MWth NET Power demo plant in La Porte,
Texas which is expected to be completed in 2017. NET Power is aiming
at the design and development of plants with an electrical power output
of 295 MWel until 2022 and efficiency of 58.9% [126,127]. In [128],
supercritical CO2 cycle system of 10 MWe with upscaling potential to
33 MWe using GE’s prototype CO2 turbine claim to reach efficiency of
50% at 700 °C. The use of CO2 in supercritical Brayton cycles has
considerable advantages related to the high density of supercritical CO2
which results in smaller and compact equipment sizes. Except its sta-
bility and relative inertness, non-toxicity, abundance and its low cost,
its compressibility factor around the critical point decreases resulting in
lower pressure ratios in the cycle and less energy consumption
[124,129].
The critical parameters for CO2 reaching the supercritical region of
state are a pressure of 7.38 MPa and a temperature of 30.98 °C [129].
The basic design of supercritical CO2 Brayton Cycle in closed system
includes the compression step, a heating source where enthalpy in-
crease is realized via a heat exchanger, a turbine for pressure reduction
and simultaneous power generation and a cooler for heat rejection.
There are many different configurations to the basic cycle. A selection is
presented in Fig. 4. The most efficient layout depends on the specific
conditions of the heat source as well as the required power and heat
demand. A comparison of numerous process layouts is presented in
[124] and in the literature presented in Table 4 [129–153]. In
[124,129,139], the recompression supercritical Brayton Cycle config-
uration has presented the highest efficiency.
The highest theoretical efficiencies have been reported with the
following conditions at the inlet of the turbine: a temperature of 700 °C
and pressure of 20 MPa with an efficiency of 53% [129,138], a tem-
perature of 620 °C and pressure of 20 MPa with an efficiency of 52.4%
[144], a temperature of 700 °C and optimal pressure ratio of 4.4 with an
efficiency of 52.1% [139] and a temperature of 750 °C and pressure of
20 MPa with an efficiency of 52% [150]. The difference in the results is
attributed to the configuration used and the assumptions made on the
isentropic and mechanical efficiencies of the compressor and turbine,
on the temperature approach, effectiveness and pressure losses in the
heat exchangers and recuperators and on the cooling temperature. Se-
lected isentropic efficiencies for the compressor are in the range of 80%
[129], 85% [138,145], 86%, [131], 87% [149], 88% [124], 89%
[141,142,144,147].
Moreover, selected isentropic efficiencies for the turbine are in the
range of 90% [131,138,143,145], 92% [124], and 93%
[141,142,144,147]. Indicatively the effectiveness for the recuperators
is in the range of 86–95% [124,129–153]. More research is required for
testing the power production, the efficiency of its machinery compo-
nent and rotor dynamics, the fluid properties also in mixtures, the
material corrosion and stresses at higher pressure and temperatures and
the design of heat exchangers [129,151]. It has to be mentioned that
there is a lot of research and development required to achieve the
theoretical efficiencies as also the pilot facilities presented in [124] are
still on the research stage for achieving the targeted efficiencies.
However, a process with an electrical power output of more than 10
MWel is necessary to determine the challenges and opportunities that
are related to this technology [124]. The current research efforts are
summarized in Table 5 according to the application, heat source and
scale [154].
As reported in [137], the Department of Energy (DOE) Gen-IV S-
CO2 Research Program, there are different sizes and applications in-
vestigated. In nuclear applications, direct or indirect applications in
temperature ranges of 350–700 °C and scales of 10–300 MWe are in-
vestigated. In fossil fuel thermal power, indirect applications in tem-
perature ranges of 550–900 °C and scales of 300–600 MWe and direct
E.I. Koytsoumpa et al. The Journal of Supercritical Fluids 132 (2018) 3–16

Fig. 4. Supercitical Brayton Cycle Configurations.

Table 4
Efficiencies reported in the literature for different applications.

Ref. Temperature (°C) Pressure Efficiency A (Thermal) % Efficiency B (System) %

109 550 20 MPa 46 theoritical

109 550 20 MPa 45.3 calculated
109 650 20 MPa 50
109 700 20 MPa 53
110 520 10 to 15 MPa 35 to 40 33.42
110 520 18 to 25 MPa > 40 35.14
110 520 25 to 30 MPa > 40 35.3
111 580 8 and 34 MPa 38
111 700 8 and 34 MPa 42
112 675 3.2/10 MPa 44.5
113 732 26,5 48 40
114 600 25–30 MPa 51
115 800 12 MPa 50
116 555 20 MPa 41%
117 600–700 20 MPa 50–53
118 538 43
118 700 50
118 800 54
119 700 ratio 4.4 52.1
119 700 ratio 4.5 46.8
120 < 750 40–50
121 550–850 25 MPa < 56%
122 550–900 25 MPa 47.9–60.5
123 516.15–579–650 40.88–41.56–33.65 MPa 41.35–45.15–49.42
124 550–850 15–40 MPa 41–58
124 620 20 MPa 41.9
124 620 20 MPa 42.1
124 620 20 MPa 46.8
124 620 20 MPa 47.1
124 620 30 MPa 52.4 47.8
125 550 20 MPa 44.18/28.34 36
126 650 7.5 MPa 35.1
127 400 17.5 MPa 36.69
128 550 25 MPa 43.6
128 550 25 MPa 45.7
129 620 20–35 MPa 47.4–50.8
129 620 35 MPa . 41.4
129 700 35 MPa 44.5
130 550 22 MPa 39.59
130 550 22 MPa 42.67–43.72
131 750 20 MPa 52 40
132 650 20 MPa 43.4
133 540/300 21/20 MPa 39.44

12
E.I. Koytsoumpa et al. The Journal of Supercritical Fluids 132 (2018) 3–16

Table 5
Research efforts according to different applications, heat sources and scales [132].

Heat Source Quality Technology/ Heat Source Turbine Inlet Turbine Inlet Pressure Ratio SCO2 Cycle Net Cycle Power Output
Investigator Temperature (°C) Pressure (MPa) Efficiency

High Grade (> 500 °C) PWR PFBC 700 20.68 2.6 49.9% (cycle) 38.3% (plant)
NREL Solar Power Tower 700 22 2.6 38.30% 5–10 MWe
Sandia Gas Fast Reactor 650 20 2.7 45–50% 200 MWth
EPRI Coal-fired boiler 600 7.58 2–4 – 400–800 MWe
KAIST Small Modular Water 550 20 2.6 40% 330 MWth
Cooled Reactor
KAIST Sodium Fast Reactor 550 20 2.08–2.64 44.02–46.65% 264.1–279.9 MWe
Sandia Immersion Heaters 536 13.98 1.81 – 52.8 kWe
Barber-Nichols Unspecified 400–650 22 2 – 12.2 MWe
Intermediate Grade Abengola Solar Parabolic 500 40 2.7 25% (power) 65% (thermal)
(200 °C–500 °C) Concepts NREC Gas Turbine Exhaust 480 24.65 2.75 40–50% (Improvement over GT
20–24%)
Kumar Concentrated Solar 480 19.8 7.5 32.14% 5.6 kWe
Thermal
Univ. of Seville Molten Carbonate 375 21.6 3 39.90% 583.6 kWe
Fuel Cell (MCFC)
Echogen Waste Heat 200–540
Low Grade (< 200 °C) Oak Ridge/Univ. Geothermal/Waste 120 30 5 16.5 –
S. Fla Heat/Solar

applications in temperature ranges of 1100–1500 °C and scales of
300–600 M are investigated. In addition, concentrated solar power
applications with temperature range of 500–1000 °C and scales of
10–100 MWe, waste heat recovery in the temperature range of
230–650 °C and scales of 1–10 MWe as well as geothermal applications
in ranges of 100–3000 °C and scales of 1–50 MWe [137]. A direct cycle
is the most efficient approach as additional losses associated with the
primary loop are eliminated and indirect cycles have a complicated
plant layout and cost increase. However, direct cycles impose limita-
tions on the range of applicability of the cycle and there is also a focus
on replacing the steam cycle [117]. In the thermal power sector, su-
percritical CO2 Brayton cycles have been investigated mainly in
[144,145] and [148] but also in [152] and [153]. In [144], the coupled
coal power plant exhibits a net efficiency in the range of 47.8 ± 0.1%-
LHV (Lower Heating Value) efficiency compared to the state of the art
steam Rankine cycle in coal power plants of 45.4%-LHV based effi-
ciency and they suggest further improvements for reaching a net effi-
ciency of 48.8%-LHV based ± 0.1. A recompression cycle with different
recompression and reheating stages, a turbine inlet temperature of
620 °C and 30 MPa pressure was used. The researchers assumed a pinch
of 6 K in the cycle recuperators, a pinch of 30 K in the air-gas heat
exchanger, a compressors isentropic efficiency of 89%, a turbine isen-
tropic efficiency of 93%, an alternator/motor electrical efficiency of
99.6% and a mechanical efficiency of 98.5%. In [145], the cascaded
configuration with a supercritical CO2 part flow topping cycle and a
simple supercritical CO2 bottoming cycle coupled with a counter-cur-
rent radiative-convective biomass boiler has been investigated. Gross
efficiency in the range of 30–36% was achieved with air preheating and
a turbine inlet temperature of 550 °C and pressure of 20 MPa assuming
a temperature difference with the flue gases of 50 °C. The researchers
assumed an effectiveness of 90 and 95% in the low and high tem-
perature recuperators, a compressors isentropic efficiency of 90%, a
turbine isentropic efficiency of 90%, and a mechanical efficiency of
98%. The researchers claim that the maximum of 36% is 4.7%-points
higher than that of the simple cascaded system using the same boiler
design. In [148], the author presents the combination of supercritical
Brayton cycle with recompression and reheating stages into a coal fired
power plant with two different carbon capture systems that deliver the
make-up CO2 for the cycle. The net efficiency of the plant without the
carbon capture and supercritical conditions at the inlet of the turbine of
300 bar and 620 °C is 50.3% LHV based, which is 4% points above the
efficiency of a state of the art hard coal power plant. The net plant
efficiency with MEA-based carbon capture and CO2 compression to
110 bar was calculated to 41.3% LHV based. It is reported that via in-
creasing the turbine inlet temperature at 700 °C, the total net plant
efficiency with carbon capture and compression is increased to 44.5%
eliminating the energy penalty imposed by CO2 capture in the net
power generation from coal power plants. In [152], a net efficiency in
the range of 43.4% is calculated for a combination of oil and natural gas
boilers with a split flow with two turbines and intercooling supercritical
Brayton cycle configuration and turbine inlet temperature of 650 °C and
20 MPa pressure. The researchers assumed an average recuperation
effectiveness of 93%, a compressors isentropic efficiency of 88%, a
turbine isentropic efficiency of 93% and a mechanical efficiency of
98%. In [153], the researchers have tried to estimate the different
combined heat and power efficiencies in different loads and different
combinations of supercritical Brayton cycle. They claim that the cas-
caded supercritical CO2 CHP plant with the higher cycle working at
540 °C and 21 Mpa and the lower cycle working at 300 °C and 20 MPa
can achieve net efficiencies of 39.44% compared to the conventional
CHP configuration with an efficiency of 37.97% Their efficiency results
reported have some inconsistencies.
4. Conclusions
The future energy system has to assure the grid stability, to secure
heat and electricity supply in the power and industrial sector, to in-
tegrate highly efficient and environmental friendly technologies. The
operation of the thermal fleet harmonised together with the fluctuating
renewable energy sources and energy storage is a necessity. The flex-
ibility, the efficiency and emission reduction of thermal plants needs to
be addressed taking into consideration an integrated system of the
power and industrial sector in a CO2 circular economy. In the present
paper, CO2 emissions and capture technologies from different industries
were reviewed with the focus on commercial applications. Several
commercial projects prove that CO2 capture has successfully managed
to reach a high technology readiness level. However, the incentives for
a wide implementation of the technology in the thermal and industry
sector are still missing. CO2 utilisation could be the bringing gap for the
deployment and geographical constraints of capture technologies based
on boosting legislative schemes. A general review for CO2 utilisation
applications has been presented in the present work. Among different
applications, the power to fuel technologies and supercritical CO2 cy-
cles have been assessed focusing on the thermal sector but having also
applications in the process industry. An integrated Industry System
between thermal power, energy intensive industries and the renewable

13
E.I. Koytsoumpa et al.
electricity sector supports decarbonisation of three sectors, electricity,
heat and transportation transforming the European Market.
Acknowledgements
The authors would like to acknowledge Philipp Moormann for his
contribution to the literature review for CO2 Cycles which is included in
the present work. The authors would like to acknowledge the EU
Commission for the financial support of the MefCO2 Project −Synthesis
of methanol from captured carbon dioxide using surplus electricity”
which is funded under the EU funded SPIRE2–2014: Adaptable in-
dustrial processes allowing the use of renewables as flexible feedstock
for chemical and energy applications −Horizon 2020 with the Grant
agreement no: 637016.
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