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 CHEMICAL ENGINEERING TRANSACTIONS  
 

VOL. 39, 2014 

A publication of 

 
The Italian Association 

of Chemical Engineering 

www.aidic.it/cet 
Guest Editors: Petar Sabev Varbanov, Jiří Jaromír Klemeš, Peng Yen Liew, Jun Yow Yong  

Copyright © 2014, AIDIC Servizi S.r.l., 

ISBN 978-88-95608-30-3; ISSN 2283-9216 DOI: 10.3303/CET1439243 

 

Please cite this article as: Pérez-Fortes M., Bocin-Dumitriu A., Tzimas E., 2014, Techno-economic assessment of carbon 

utilisation potential in europe, Chemical Engineering Transactions, 39, 1453-1458  DOI:10.3303/CET1439243 

1453 

Techno-Economic Assessment of Carbon Utilisation 

Potential in Europe 

Mar Pérez-Fortes*, Andrei Bocin-Dumitriu, Evangelos Tzimas 

European Commission, Joint Research Centre, Institute for Energy and Transport, P.O. Box 2, 1755 ZG Petten, the 

Netherlands  

maria-del-mar.perez-fortes@ec.europa.eu  

The purpose of this work is to analyse different carbon capture and utilisation (CCU) options, and hence to 

identify the role of CCU on the future European energy and industrial sectors. This work carries out the 

techno-economic analyses of methanol synthesis and accelerated aqueous carbonation of waste (fly ash) 

as two differentiated options for CO2 conversion. Process flow modelling is used to evaluate the 

operational and cost performances of two conceptual designs. Calibration and validation of the models are 

completed to then assess diverse operational, economic and environmental key performance indicators 

(KPIs). The inlet CO2 and fly ash originate from a conventional power plant. The needed hydrogen for the 

methanol case is produced by water electrolysis. The work puts into relevance the differences in 

performance and costs for the two processes analysed. Future work will contemplate other CCU 

processes and a global market study in the European context that focuses on (i) current prices and 

demands for the products, and (ii) the analysis of their foreseen market evolution and price elasticity.  

1. Introduction 

The contribution of fossil fuels to the energy share is foreseen to be more important than renewables and 

nuclear power at short and medium term. Moreover, process industries like cement, iron and steel, 

aluminium, paper and pulp and refineries, have inherent CO2 emissions as a result of raw material 

conversion. In this context, carbon capture utilisation and storage (CCUS) is presented, at least, as 

medium term alternative to mitigate climate change. CCU represents a new economy for CO2, as it is used 

as raw material for other processes. This includes the synthesis of chemicals (such as methanol or formic 

acid), production of inorganic substances (like calcite, after the mineralization of CO2) and applications 

based on CO2 physico-chemical properties (for example when used in the food and beverage industry) 

(Peters et al., 2011). CO2 utilisation delays carbon emissions to the atmosphere while reducing the 

consumption of the original feedstock and avoiding the emission of other substances associated to them. 

Enhanced oil and gas recovery (EOR, EGR), as well as CO2 mineralization, result in permanent storage, 

while in the other utilisation cases, CO2 is emitted later in the product chain, i.e. when the CO2-product 

based is consumed. CCU, due to its inherent potential, is considered a complementary alternative to 

geological CO2 storage: the predicted short-term market potential by Aresta et al. (2013) is around 300 

MtCO2/y, compared to about 14,000 MtCO2/y emitted from large point sources (Boot-Handford et al., 

2014). The market for CO2 utilisation is relatively small, and future markets for CO2 will have to map and 

prioritize points of CO2 emission with utilisation opportunities, advocating for tailor-made and local 

solutions (GCCSI and PB, 2011). The different utilisation alternatives and carbon capture and storage 

(CCS), will have to work in optimum portfolios of options, i.e. different technology mix regarding the 

specific CO2 emitters, transportation and storage/use solutions of each local area analysed.  

This work analyses two carbon utilisation options: methanol synthesis and mineralization of CO2, with two 

well differentiated potentials. Methanol (CH3OH) is typically produced by the Fischer-Tropsch process, the 

catalytic conversion of syngas usually coming from steam reforming of CH4. Its current market is around 

40 Mt (produced in 2007). Future market will be larger if considering its potential as blended with gasoline, 

or converted into gasoline or diesel substitutive (dimethylether). The produced mineral considered here is 



 
1454 

 
calcite (CaCO3), that can be disposed, used in mine reclamation, in the building industry, as a polymer 

filling material, as pharmaceuticals and varnishes constituent and as raw material for optical glasses, 

among others (Peters et al., 2011).   

2. State of the art 

Carbon utilisation options are at different levels of technological development and market maturity, and in 

particular, CO2 to produce chemicals and fuels are mostly at development phase. Methanol production is 

especially important in emerging economies, as a candidate liquid fuel to replace conventional source of 

energy. Methanol synthesis from captured CO2 is being built at a commercial scale: Iceland, Japan and 

Korea have large scale pilot plants that combine carbon dioxide and renewable hydrogen (Quadrelli et al., 

2011). Carbon Recycling International (CRI) started the operation of the first commercial demonstration 

plant, in Iceland, in 2011. There exist two catalytic routes to synthesize CH3OH: direct hydrogenation with 

H2 or CO2 conversion into CO and further hydrogenation of CO (Van-Dal and Bouallou, 2012). As 

alternative, methanol can be also produced electrochemically by CO2 reduction and H2O oxidation. The 

electrochemical conversion of CO2 can be customized to produce different products by appropriately 

selecting electrocatalysts, electrolytes and applied potential (Agarwal et al., 2011). Research is also in the 

line of mimicking photosynthesis, considering solar energy as the source for CO2 reduction with H2O in a 

compacted photo-electrochemical cell (Ampelli et al., 2011). The route considered in this work is the 

closest to the market, i.e. the catalytic route. Hydrogen for CH3OH must be provided to the process in a 

carbon-free way to reduce the life cycle CO2 emissions: H2 from water electrolysis using a renewable 

source of electricity is considered as renewable. It may be produced through alkaline or proton exchange 

membrane electrolysis (PEM), while H2 from steam electrolysis is produced via a solid electrolyser cell 

(SOEC). This last is the most efficient option, but this is currently the less developed (Redissi and 

Bouallou, 2013). Biomass, solar and wind are the most common renewable sources proposed for 

electricity supply in water electrolysis (Langè and Pellegrini, 2013): while wind is currently the most cost 

effective source among the renewable (Mignard and Pritchnard, 2008). Mineralisation of CO2 or mineral 

carbonisation mimics the natural weathering phenomenon, where natural alkaline silicate minerals and 

atmospheric CO2 react. This process has however very slow kinetics. It can be accelerated (i) if the 

concentration of CO2 is larger, (ii) if mineral has a larger reaction surface (grinding), (iii) if pressure is 

increased, and (iv) if moisture is present. Accelerated carbonation may use natural ore or alkaline solid 

waste to react with CO2 (Huijgen et al. 2006). The process can take place ex-situ, in a chemical plant after 

mining and after mineral transportation, or after residue collection; or in-situ, by injecting CO2 into 

appropriate geological formations and where the mineral matrix is not extracted from the mineral itself. Its 

main advantage is that it provides a permanent CO2 storage (Montes-Hernandez et al., 2009). 

Experimental installations have been already carried out, using different types of rocks (that must be 

grinded) or industrial waste (that may be already at a reduced particle size), like Alcoa, Skyonic and 

Calera, Novacem and Calix at pilot plant or lab scales. Accelerated carbonation tolerates different degrees 

of CO2 purity (GCCSI and PB, 2011). The conversion process selected for this work contemplates the 

utilization of fly ash from a coal power plant, which is already in a milled state.  

3. Plants modelling 

The boundaries of the current models are from “gate-to-gate”: only the carbon re-use process is modelled. 

The CO2 is captured from a power plant and then it is usually transported in a supercritical state, at 85-150 

bar and 12-44 °C (EC, 2011). Considering transportation by on-shore pipeline, according to ZEP (2011), 

the delivery pressure is 61 bar, and the delivery temperature is around 10 °C, as the approximate ambient 

ground temperature. See in Table 1 the CO2 average composition of the CO2 stream, if pre-combustion, 

post-combustion and oxy-fuel capture methods are considered. 

Table 1: CO2 average composition, from coal and gas power plant, in % by volume (EC, 2011). 

Component % by volume 

N2/O2 1.57 

H2S 0.05 

H2 0.40 

SO2 0.09 

CO 0.04 

CH4 0.34 

CO2 97.51 



 
1455 

Table 2: Size and working conditions for the selected technologies (Mineralisation: Montes-Hernández et 

al. 2009; Huijgen et al. 2006; DOE/NETL, 2013. Methanol synthesis: Van-Dal and Bouallou, 2012; Van-Dal 

and Bouallou, 2013; webpage of CRI, accessed 24.02.2014). 

 Renewable methanol Mineral carbonation 

Plant size 1,300 (t of product/d) 14,400 (kg/h of fly ash) 

Pressure (bar) 75.7 (Reaction) and 1.1 (Distillation)  20 (Reaction) 

Temperature (°C) 210  (Adiabatic reactor) 30 (Isothermal reactor) 

Mass flow of CO2 (kg/h) 80,500 464 (Stoichiometric) 

Mass flow of reactants (kg/h) 10,977 (Stoichiometric H2) 216,000 of H2O (L/S=15 kg/kg)  

The models performed in this preliminary approach use CO2 at a 100 % of purity, assuming a further 

process of purification after its transportation, whose modelling is beyond the scope of the current work. It 

is assumed that no by-products are produced. The employment of renewable sources for the provision of 

electricity in the water electrolysis process to produce H2 is not taken into account: the electricity 

production (i.e. the CO2 emissions) is from a pulverised coal power plant. Specifically for the case of 

aqueous carbonation, it is supposed that the conversion at large scale and with a continuous reactor, 

behaves as the experimental batch reactor used as reference. See in Table 2 the most representative 

average size, input data and working conditions for the selected plants. The models have been 

implemented in a process flow modeller. Thermodynamics properties are calculated with the property 

packages Redlich-Kwong-Soave and NRTL for low and high pressure sections in methanol synthesis, 

respectively, and Peng-Robinson for CO2 mineralisation. The needed rules of thumb and costs 

expressions for conceptual design dimensioning and costs evaluation are from Towler and Sinnott, 2013. 

3.1 Methanol production 
The process simulated uses CO2 already purified in combination with H2 from water electrolysis, that 

consumes 4.8 kWhel/Nm
3
 of H2 produced (Van-Dal and Bouallou, 2013). It is assumed that the plant 

produces 1,300 t/d of methanol. Therefore, according to the efficiency reported in Van-Dal and Bouallou, 

2013, the corresponding inlet CO2 stream is of 80,500 kg/h. Inlet H2 correspond to the stoichiometric 

amount of H2, according to the governing Eq(1): 

                    (1) 

                (2) 

Eq(2) occurs in parallel reducing the amount of CO2 converted into CH3OH. The resulting water stream 

can be potentially recycled to the CO2 capture plant to provide the needed water for the conversion of CO 

into CO2, or used for electrolysis. Doped metal oxides are usually used as catalysts for Eq(1). The 

implemented kinetics correspond to those using the catalyst Cu/ZnO/Al2O3: specific reaction rates 

expressions can be found in Van-Dal and Bouallou (2013), and they follow the Langmuir-Hinshelwood-

Hougen-Watson model.  

See in Figure 1 a simplified block diagram of the model. CO2 is entering from the capture plant at 1.1 bar. 

H2 is coming from the electrolysis process at 30 bar. Both streams are at 25 °C. They are compressed 

separately until 78 bar. The CO2 compressor is multistage according to the same Pi/Pi-1 ratio for each 

stage, along with (Pn/Po)
1/n 

close to 2.5, where Pn and Po are the initial and final pressures, respectively. 

Therefore, three stages have resulted for CO2 and one stage compressor for H2. Then, the mixture of both 

streams is heated up until the temperature of the methanol reactor (210 °C): this is an adiabatic fixed bed 

reactor simulated by a kinetic plug-flow reactor. Reactor dimensions have been calculated for the case 

study described in Van-Dal and Bouallou, 2013 and taken into account the amount (44,500 kg) and density 

(1,775 kg/m
3
) of the utilised catalyst, resulting in a diameter of 2.13 m and a height of 8.5 m. Final height is 

7.9 m for the inlet conditions of the current case study, to maintain the same conversion. HE1 heats up the 

mixture of CO2 and H2 while cooling down the appropriate amount of products resulting in the methanol 

reactor (from 286.5 °C until 92 °C). The conditioning system adapts the mainly CH3OH and water stream 

to 35 °C and 73.4 bar. The heat exchanger is integrated downstream with HE2 and the reboiler heating 

needs. Flash1 separates the mixture, with a vapour fraction of 0.904. CO2 recycling injects the resulting 

CO2 stream into the inlet mixture of CO2 and H2. COMP3 increases the pressure again until 78 bar. Then, 

the distillation column that separates methanol and water has as inlet conditions 80 °C and 1.1 bar. Flash2 

separates any vapour fraction before methanol purification. The detailed model for the distillation column 

counts with 57 stages, a reflux ratio of 1.2, and a bottoms-to-feed ratio of 0.4, in mole basis. Feed stream 

is on stage 44. Further purification is obtained with the following COMP4 and HE3, finally delivering 

CH3OH at atmospheric pressure and 20 °C. The ΔP considered in all heat exchangers take is of 0.2-0.3 

bar. Compressors consider a mechanical efficiency of 0.8. If not mentioned the integration of streams, the  



 
1456 

 

 

Figure 1: Simplified simulation flowsheet of methanol synthesis produced from captured CO2 and H2 from 

water electrolysis (own source and model based on Van-Dal and Bouallou, 2012) 

heat exchanged is with water at 1.1 bar and 25 °C. The electricity provided by the coal power plant adds 

803 tCO2/GWh (DOE/NETL, 2013) to the overall CO2 balance.  

Reactor simplification: The results of the kinetic methanol reactor for different flowrates have been 

analysed in order to simplify its implementation. By adjusting the amount of methanol synthesized, it is 

possible to replace the kinetic reactor by an equilibrium reactor at the temperature Treactor + 13.85 °C, with 

an error of +/-3-5% in composition and temperature. 

3.2 Accelerated aqueous carbonation of fly ash 
The process receives the CO2 already purified and the fly ash from the baghouse of a 550 MW e pulverised 

coal power plant (DOE/NETL, 2013). It is assumed that the plant utilises the fly ash collected in the 

abovementioned power plant: 14,400 kg/h. The inlet amount of CO2 is 464 kg/h, according to the 

stoichiometry of Eq(3) and Eq(4):  

                 (3) 

                        (4) 

Where, CaO is a 4.1 % on a mass basis; being the rest of the components 50 % of SiO2, 30 % of Al2O3, 

and 15.9 % of Fe2O3 (Montes-Hernandez et al., 2009). The resulting water stream, that now is not recycled 

to form the slurry, can be used for other heating/cooling purposes (T = 40 °C), or potentially recycled to the 

CO2 capture plant to provide the needed water for the water gas shift reactor. Fly ash, further grinded (if 

needed) and suspended in water, reacts in the carbonation reactor according to a pseudo-second-order 

kinetic model, dependent on CO2 concentration, for Eq(4) (Montes-Hernandez et al., 2009).  

See in Figure 2 a schematic block diagram of the model. CO2 is entering from the capture plant, and fly 

ash is entering from the same power plant, at 1.1 bar and 25 °C. H2O is also entering at the same 

conditions of P and T, with a corresponding flowrate of 15 times the flowrate of fly ash, according to the 

ratio liquid / solid (L/S=15kg/kg) (Huijgen at al., 2006). CO2 is compressed until at least 20 bar, that is the 

 

Figure 2: Simplified simulation flowsheet of accelerated and aqueous carbonation of fly ash from a coal 

power plant - own source and model based on Huijgen at al. (2006) and Montes-Hernandez et al.(2009) 

Methanol

 Electricity

H2O

O2

H2

WATER 

HYDROLYSIS

H2 

CO2

COMP2

Methanol 

reactor

Conditioning 

system

Purge

Residual 

gases

Distillation 

column

H2O

METHANOL SYNTHESIS 

COMP1

HE1

COND

REB

Flash1 

Flash2 

COMP3

HE2

HE3

COMP4

Flash3 

ACCELERATED AQUEOUS CARBONATION OF FLY ASH

H2O

Fly ash

CO2
COMP1

Pump
Carbonation 

reactor

CO2 

Recycles

Crusher

Filter

CaCO3 - rich 

fly ash

H2O 

(Purge)H2O 

HE1
HE2

HE1-HE2

COMP2

Flash1

Flash2

Purge 2
Purge 1



 
1457 

inlet pressure of the carbonation reactor. A multistage compressor (with two stages) is used, analogously 

to the previous model. Fly ash slurry is pumped at the same pressure. Fly ash is previously grinded until a 

maximum of 40 μm (Bond working index = 12 kWh/t). HE1-HE2 cools down the liquid product of the 

carbonation reactor reaching 40 °C and 17.9 bar, while conditioning the reactor inlet stream (if needed). 

The valve expands the product till atmospheric pressure for separation. If necessary, CO2 can be recycled 

at two points of the flowsheet (in units flash1 and flash2, after reaction and expansion). A centrifuge filter, 

working at 1,200 rpm is selected to separate solids and liquids. The carbonation reactor has been divided 

into two reactors for modelling purposes: one stoichiometric reactor that reaches the complete conversion 

of CaO into Ca(OH)2 (Eq(3)) and a kinetic reactor with the following preliminary adaptation of the kinetic 

rate expression described in Montes-Hernandez et al. 2009, taking into account that the volume of reaction 

is 1 dm
3
: rateCaCO3[mol/m

3
s] = 0.4877*(0.032-[CaCO3]). The whole ΔP is of 1.5 bar. Again, the ΔP 

considered in all heat exchangers is between 0.2-0.3 bar. Compressors have a mechanical efficiency of 

0.8. If not mentioned the integration of streams, the heat exchanged is with water at 1.1 bar and 25 °C. A 

coal power plant releases 803 tCO2/GWh (DOE/NETL, 2013).  

Reactor simplification: The reactor has been replaced by a stoichiometric reactor that calculates the 

consumed moles of CO2 according to the behaviour observed in Montes-Hernandez et al. (2009): the 

carbonation efficiency CaO-CaCO3 is approximately 82 %. Therefore, the reactor calculates the nCaCO3 = 

nCa(OH)2 [mol/h] = 0.82*mCaO [kg/h] / 56.077. This carbonation efficiency has been checked at different 

larger rates than experimental, and the error is around +/-0.5-1 % compared to the results obtained with 

the kinetic reactor. 

4. Results  

The results, represented as a list of key performance indicators (KPI) for both processes, are shown in 

Table 3. (i) Product purity refers to the % on a mass basis of CH3OH and CaCO3 in the product stream for 

both processes. (ii) The % of CO2 converted in the reactor is a ratio between the outlet/inlet molar flow.  

(iii) The CO2 recycled and converted expresses the percentage of CO2 that is not released of the system, 

i.e. the CO2 that has been used or recycled. (iv) The selectivity is only expressed for the methanol reactor, 

since two different reactions using CO2 are taking place; on the contrary, in mineral carbonation only the 

mineralization reaction is considered in the reactor. (v) Heat duty and (vi) electricity duty expresses the 

utility needs per ton of CO2 used. (vii) CO2 emissions in CO2 emissions per ton of CO2 used, refers to the 

emissions corresponding to outlet streams from the two processes described, plus the CO2 released due 

to the production of the electricity need. And finally, the (viii) CAPEX is the total investment required per 

ton of CO2 used, following Hand’s method. It includes the total cost of purchase, offsites design and 

engineering and contingency items. This approach corresponds to a preliminary estimate, so the accuracy 

is typically +/- 30 %. The estimated costs, as a starting value, assume that the only material used is carbon 

steel. For the estimation of heat exchangers costs, heat interchange with water or steam is assumed 

(Towler and Sinnott, 2013). Even if the purpose of this work is not to compare the two CCU options among 

them, since different needs are satisfied by the two differentiated processes, is it important to remark that 

mineralisation is more advantageous in terms of electricity needed and relative CO2 emissions, while 

methanol production is cheaper in relative terms, and more efficient, in general. Its absolute CAPEX is 118 

MEUR, while the absolute CAPEX for mineralisation is 20 MEUR. 

Table 3: List of KPIs evaluated for each methanol synthesis and carbon mineralisation.   

KPIs Renewable methanol Mineral carbonation 

Product purity (%wt)  88 (of CH3OH) 6 (of CaCO3) 

CO2 converted in the reactor (%) 27 17 

Total CO2 recycled and converted (%) 94 82 

Selectivity 33.7 - 

Heat duty (MWh/tCO2used) 1.47 (cooling needs) 1.57 (cooling) , 8.18 (heating) 

Electricity requirement 

(MWh/tCO2used) 
8.08 1.28 

CO2 emissions (tCO2/tCO2used) 6.5 (0.3 without electrolysis) 1.3 

CAPEX (MEUR2010/(tCO2used/h)) 1.56 53.4 

 



 
1458 

 
5. Conclusions 

The analysis presented in this work considers methanol production and accelerated aqueous carbonation 

of fly ash for carbon re-use. The two conceptual designs, at realistic scales, have been simulated in order 

to obtain the needed mass and energy balances to evaluate the KPIs. This paper describes the 

methodology followed and that will be also applied for studying other CCU technologies, with the final 

purpose of performing a global market study that focuses on (i) current prices and demands for the CO2 

products, and (ii) the analysis of their foreseen market evolution and price elasticity. The study aims to 

indicate the most sustainable ways to convert CO2 and analyse the role of CCU in the whole CCUS 

context. Further this work may also help on prioritizing support and/or RD&D funding to enable the 

commercialisation of the selected CCU technologies.  

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