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Carbon Capture and Utilization Technology Without Carbon-Dioxide Purification and Pressurization: A Review on Its Necessity and Available Technologies HsingJung Ho, Atsushi Iizuka, and Etsuro Shibata Ind. Eng. Chem. Res., Just Accepted Manuscript • DOI: 10.1021/acs.iecr.9b01213 • Publication Date (Web): 08 May 2019 Downloaded from http://pubs.acs.org on May 9, 2019

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Industrial & Engineering Chemistry Research

Carbon Capture and Utilization Technology Without CarbonDioxide Purification and Pressurization: A Review on Its Necessity and Available Technologies Hsing-Jung Ho1, Atsushi Iizuka2,*, Etsuro Shibata2

1 Department

of Environmental Studies for Advanced Society, Graduate School of Environmental Studies, Tohoku University, Aoba-468-1 Aramaki, Aoba-ku, Sendai, Miyagi 980-0845, Japan

2 Center

for Mineral Processing and Metallurgy, Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, 2-1-1, Katahira, Aoba-ku, Sendai, Miyagi 980-8577, Japan

*E-mail: [email protected], [email protected]

Abstract: Carbon capture and utilization (CCU) has attracted increased attention as a means to mitigate and adapt to climate change. CCU technology regards CO2 as a raw material and reduces CO2 emissions. However, purity and pressurization requirements in most CCU technologies are high. Flue gas that is emitted from industries and transportation requires advanced purification and pressurization, which limits the development and decreases the feasibility of CCU application. Hence, a new approach to CCU technology without CO2 purification and pressurization is desirable. This study reviews differences between the CO2 purity and pressure of waste CO2 and feedstock CO2, reviews difficulties of CO2 purification and pressurization in recent developments of CCU, and provides several promising examples of CCU technologies without CO2 pressurization and/or purification. Various promising CCU technologies and their future research prospects are discussed. Mineral carbonation and biological conversion appear to be possible solutions as CCU technologies without CO2 purification and pressurization. For all other CCU approaches, research trials to decrease the required CO2 purity and pressure of the feedstock CO2 will be required.

1. Introduction Industry contributes to atmospheric greenhouse gas (GHG) emissions. The construction,1 cement,2 aluminum production,3 chemical,4 water,5 wood processing and power industries7 impact GHG emissions. Transportation, agriculture, residential and commercial businesses also contribute to GHG emissions through their large emission volumes.8 Various industries require effective CO2 emission reduction technologies, which can be applied to various CO2 emission

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sources. Therefore, GHG reduction is an urgent issue that must be faced and solved now or in the future. Although many alternative technologies exist related to renewable energy, low-carbon energy, nuclear power and clean-energy technology, fossil fuels will continue to be the largest global energy source over the next several decades.9 Carbon dioxide (CO2) emissions account for approximately three-quarters of GHG emissions,10 and CO2 is considered to be the main gas that causes climate change.11 To mitigate climate change, carbon capture and storage (CCS) techniques have been investigated to sequester CO2 from the atmosphere.12 In the CCS techniques, CO2 in waste streams is captured, conditioned, transported and sequestrated.13 Four options for CO2 sequestration, i.e., geological, ocean, mineralization and industrial use, have been considered. In geological storage, CO2 is introduced under cap rock for sequestration;14 and in ocean storage, CO2 injection into seawater has been considered.15 However, besides some enhanced fuel recovery processes, such as the geological sequestration option, economic problems, social acceptance, difficulty in sequestered CO2 monitoring and environmental impact are barriers to the deployment of the CCS techniques.16 Recently, the concept of carbon capture and utilization (CCU) has attracted increased attention. The purpose of CCU is to use CO2 as a feedstock for application in various ways. CO2 is regarded as an alternative feed source, which can reduce demands on natural resources and their exploitation. CCU has many applications as shown in Figure 1.17 For instance, it has been used in (1) biological conversion, (2) the food and drink industry, (3) plastics, (4) extractants, (5) refrigerants, (6) enhanced fuel recovery, (7) chemicals production, (8) mineralization, (9) fire suppression, (10) as an inert agent and (11) in miscellaneous applications. The CCU technique could yield economic income and the simultaneous reduction of CO2.18 However, various industries require CO2 purification prior to CCU, which is costly and therefore, limited to largescale industries (power generation, steelmaking and cement production industries).19 To achieve further CO2 reductions, CCU without purification is necessary. A variety of research papers and reports have dealt with a wide range of topics that are related to CCU techniques. Huaman et al.10 and Nejat et al.11 investigated the source of CO2 emitters, the range of impurities in the source gas, and their implication for use in CCU. Song et al.20 and Roh et al.21 focused on CCU process design and optimization. Von der Assen et al.22 dealt with the lifecycle assessment of CCU techniques. The detailed deployment of CCU, such as in transportation routes, network economics, pipeline financing scenarios and policy has been investigated by Edwards et al.23, Vikara et al.24 and Baik et al.25 Several reviews describe CCU techniques. Markewitz et al.26 compared several technologies for CO2 reduction by CO2 capture, storage and utilization. The energy consumption, energy supply chain and operation cost, including transportation fees for flue gas, CO2 and products and electricity generation cost have been summarized. Yuan et al.27 summarized the deployment and development of large-scale CCU processes, with a focus on CO2 conversion technologies, and


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provided some idea of the optimal design of CO2 capture processes. Sanna et al.28 and Al-Mamoori et al.18 summarized CCU acceleration methods to provide future opportunities. In this review, we focus on the requirements of CO2 purity and pressure of CO2-containing waste streams as a CCU feedstock. Most flue gas contains a large amount of impurities and the CO2 purity and pressure tend to low. However, most CCU technologies require pure and pressurized CO2 as a feedstock, which requires the installation of costly and power-consuming CO2 capture, purification, and pressurization for CO2 reduction. These requirements serve as a strict limitation, especially for moderate and small CO2 emitters for CCU technology adaptation. The feasibility of CCU implementation will be reduced by the high cost, and the CO2 capture amount may be unprofitable or lower than the amount of CO2 emissions with extensive energy consumption. On the basis of these points, the development of CCU technologies at atmospheric pressure and a low CO2 concentration is extremely important. We introduce available CCU techniques without CO2 purification and/or pressurization. For example, plastics and chemical production without CO2 pressurization and biological conversion will be discussed in detail. CCU technologies by mineralization will be introduced, including some pilot or operational plant information.

Figure 1. CCU technologies (provided by the U.S. Department of Energy's National Energy Technology Laboratory)17

2. Differences in CO2 purity and pressure between waste CO2 and feedstock CO2



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In CCU technologies for global warming mitigation, CO2 in waste streams requires conversion before use. Because of differences in CO2 purity and pressure between waste and feedstock CO2, purification and pressurization is required. In this section, CO2 purities and pressures in waste streams and those required as a feedstock in CCU technologies are summarized and compared. Major and minor impurities in waste gases are also summarized. 2.1. CO2 purities and pressures in waste streams Flue gas that is discharged from incinerators or industrial sites usually contains a large amount of impurities (NOx, SOx, H2O, O2, N2), and the CO2 purity tends to be low. Table 1 shows details of the main CO2 sources. The CO2 purity is below 40% in most flue gas sources. The highest CO2 content in flue gas is almost 85% from oxy-combustion flue gas and 70%–90% from hydrogen production plant flue gas. Because of the high CO2 content, this source has great potential for CCU technology development. The lowest CO2 content is only 3.3%. CO2 pressure from normal sources is only 1 bar. Medium CO2 emitters serve as potential CCU sources at 10%–15% of global energy related CO2 emissions and have the potential to become target sources.43 Table 1 CO2 purities and pressures in waste streams CO2 sources

CO2 (%)

Major impurities

Minor impurities

7.4%–7.7%

H2O, O2, N2.

CO, NOx

Pressure

Temper ature

1 bar

50–75°C

Power generation Gas fired flue gas29 Coal-fired flue gas30 Coal-fired flue gas31 Power plant flue gas32 320 MW coal-fired flue gas33 320 MW natural gas fired flue gas33 Power plant flue gas34 Oxy-combustion flue gas27 Oxy-combustion flue gas35 Integrated gasification combined cycle power-plant flue gas36 Industry Steelmaking plant flue gas37 Cement kiln plant flue gas38-40 Hydrogen production plant flue gas41 Gasification plant flue gas42

12.5%– 12.8% 15% 15%–20% 13.2%

N2, H2O O2, N2 N2, H2O

CO, NOx, SO2 O2

8%

N2

O2, H2O

3.3% 75%–80% 75%–86%

O2, H2O H2O H2O

NO, NO2 NOx, SOx NO, SO2

39.85%

H2, N2, CO

H2O, H2S, Ar, CH4

32.3 atm

37°C

20%

CO, N2

14%–33%

H2O, O2

H2 CO, NO, SO2

1 bar

50–75°C

70%–90%

CO

-

9.2%

N2, H2

CH4, CO

15–40 bar

40– 450°C

H2O, N2


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≈ 400 ppm

Atmosphere

N2,O2

-

1 bar

Ambient tempera ture

2.2. Required feedstock CO2 purities and pressures The CO2 content and pressure in flue gas is not sufficiently high for application of the CO2 capture technology. Table 2 shows that most CCU approaches require pure CO2 and/or a high pressure or supercritical state CO2. For example, in chemical production, the CO2 is required to be almost pure. In addition, a high CO2 pressure is required in enhanced gas/oil recovery, enhanced coal bed methane recovery, metal casting and decaffeination. In algae and mineral carbonation, CO2 purity and pressure requirements can be low. Table 3 shows the CO2 requirements. According to different requirements, CO2 could be used as a feedstock in CCU technologies. For example, in mineral carbonation, research has been conducted to use pure CO2 and to utilize flue gas directly without purification and pressurization. The difference in CO2 requirement may be attributed the differences in various target materials and designed processes. Table 2. Required feedstock CO2 purities and pressures in CCU technologies Application

CO2 purity

Carbonated beverage44 Enhanced gas recovery45 Enhanced oil recovery46-48 Enhanced coal bed methane recovery49 Polycarbonates50 Methanol51

99% 99.9% 95%–99%

CO2 pressure 2 bar 120 bar

Total pressure

Remarks

≈ 2 bar ≈ 120 bar ≈ 90–157 bar

99%

89.6–150 bar 60–200 bar

95% 99%

1 bar 1–3 bar

≈ 1.05 bar 61–63 bar *

Methane52

99%

0.04 bar

1 bar *

Urea53

99.9%

121.6 atm

≈ 121.7 atm

Algae54

Atmospheric CO2 is utilized

-

-

Multi-stage compression

≈ 60–200 bar


Filled with 60 bar H2 for subsequent hydrogenation. *Mix gas molar feed H2:CO2:He =16:4:80 Reaction temperature: 180°C The process is in seawater and freshwater environments


Refrigerant55 Metal castings56 Decaffeination agent57-

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99% 95% 99%

70–100 bar 95 bar 300 atm

≈ 70–100 bar ≈ 100 bar ≈300 atm

6%–99.9%

0.06–150 bar

≈1–150 bar

58

Mineral carbonation5960

and atmospheric CO2 is utilized.

Reaction temperature:60– 150°C

Table 3. Category of level requirement of CO2 High (> 90%)

Low

High

Enhanced gas recovery, enhanced oil recovery, enhanced coal bed methane recovery, production of urea, decaffeination agent

Mineral carbonation

Low (around atmospheric pressure)

Carbonated beverage, production of polycarbonate, production of methanol, production of methane, refrigerant, metal castings, mineral carbonation

Mineral carbonation, algae

Purity

Pressure

3. Techniques for CO2 purification and pressurization Differences in CO2 purity and pressure between CO2 in waste streams and requirements in the abovementioned applications required the development of techniques for CO2 purification and pressurization. These techniques have some drawbacks for the development of CCU techniques. 3.1. CO2 purification techniques Because of CO2 purity requirements, various CO2 purification techniques have been developed. Several methods, such as physical adsorption,61 chemical adsorption,62 chemical absorption,63 physical absorption,64 membrane separation,65 monoethanolamine process,66 refrigeration67 and condensation67 have been investigated. Based on different impurities and different uses, different treatment methods have been used to remove varied target impurities. For example, for oxygen removal, cryogenic distillation, chemisorption of oxygen on copper and catalytic oxidation of carbon monoxide, propane, methanol, and hydrogen have been compared by Abbas et al.68 Water is also commonly found in flue streams. Dehydration can be achieved by using several


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techniques.69 Refrigeration and condensation, adsorption using silica gel and absorption using liquid desiccant have been developed in water removal.68 Based on these techniques, CO2 purity can achieve CCU technology requirements. 3.2. CO2 pressurization techniques The total pressure of the reaction gas that contains CO2 can be increased by using a pump. By increasing the total pressure, the reaction rate can be increased, and the reaction equilibrium can be moved in a desirable direction. However, pump operation to increase the gas pressure will consume excessive power, and a high-pressure reactor and pipelines will be required, which will result in expensive operation and capital cost for the CCU plant and decrease the economic feasibility of the CCU process. 3.3. Difficulties of CO2 purification and pressurization in recent developments of CCU According to the requirements of CO2 purity and pressure in CCU, CO2 purification and pressurization techniques should be integrated into the process. However, several problems will be encountered in achieving a high CO2 quality. An additional CO2 purification and pressurization plant is required.70 When the flue gas is delivered to the CCU plant from industrial sites, it must be purified and pressurized. However, the CO2 purification and pressurization plants are usually large, and may be even larger than the original CCU plant. Therefore, if we consider factors, such as land use, equipment and cost, these factors will cause difficulties in CCU development. In addition, CO2 purification and pressurization processes are expensive at almost 70%–75% of the cost of the entire process, which often causes the entire process to be uneconomic, and leads to difficulties in implementing these technologies.28 For example, the capital cost of purification and pressurization of flue gas from coal-fired power plants usually costs 42–65M€ (~47–73 million USD, 1€ = 1.12USD on 23/04/2019) and the operating cost per annum is approximately 35–43M€ (~39–48 million USD, 1€ = 1.12USD on 23/04/2019).71 Moreover, the energy input of CO2 purification and pressurization is also considerable.68,71-72 To achieve high-purity and high-pressure CO2, it is necessary to set up equipment and several unit processes, but the equipment and process operation will consume extensive energy. Based on the conversion of energy into electricity, the cost and CO2 emissions, the entire process may be unprofitable or capture less CO2 than emissions. For example, if we assume that the condition is ideal energy for the isothermal compression of an ideal gas, and the pressure is increased from 1 bar to 100 bar at 298 K, the calculated energy consumption is 72.0 kWh/t-CO2, which equates to 5.04 USD/t-CO2 if we assume a unit power generation price of 0.07 USD/kWh. Li et al.73 state that the energy penalty for CO2 purification by monoethanolamine is substantial. The thermal energy for solvent regeneration is 3.1 MJ/kg CO2 which equates to 861 kWh/t-CO2 and accounts for more than 50% of the total energy consumption. Padurean et al.74 stated that for an integrated gasification combined cycle power plant, the energy related consumption for high-concentration



CO2 capture is as follows: the power duty is 8.93 to 22.85 (MWel) the cooling agent duty is 6.81 to 210.3 (MWth) and the heating agent duty is 34.05 to 369.68 (MWth). A safety hazard assessment of CO2 purification and pressurization is critical. Comprehensive studies have focused on the risk of high-pressure and high-concentration CO2 pipelines.75-76 If pipeline security is not considered, a catastrophic release of CO2 may occur.77 The public perception of CO2 pipelines is also important, and it may not be easy to gain acceptance from the local community. Therefore, if the CCU technology can achieve a balance of process, revenue generation and reduced energy consumption, without relying on government policies and other subsidies, it can be developed globally. Based on these points, it will be important to develop CCU technology without purification and pressurization. In the following sections, CCU technology that uses pure CO2 at approximately atmospheric pressure, such as plastics production, chemicals and food production and in the drink industry, and CCU technology that uses flue gas without CO2 purification and pressurization, such as mineral carbonation and biological conversion, will be summarized.

4. CCU technology using pure CO2 under approximate atmospheric pressure Costs and energy consumption are critical in the development of a feasible CCU technology to reduce CO2. Improvements and developments of new CCU processes without pressurization or purification are trending in this field. Table 2 shows that some applications could develop CCU technology without pressurization, such as in the food and drink industry and plastics and chemical production. This approach will be discussed in detail in the following paragraph. 4.1 Plastics production The use of CO2 for polymer and polycarbonate production without CO2 pressurization has been investigated. Artz et al.78 stated that the new use of polymers to substitute energy intensive resources by CO2 offers an approach to mitigate global warming impacts in their review on CO2 conversion. In this process, several agents such as CH3OH, phenol, bisphenol-A and the intermediate formation of cyclic carbonates need to be added to help with successful CO2 conversion. Chapman et al.50 reported that captured CO2 from coal-fired power station is used to prepare the polycarbonates by using homogeneous dinuclear Zn and Mg catalysts under 1 bar CO2 pressure and 3–6 h reaction time. The results showed that polymerization catalysis can capture CO2 from flue gas for polymer synthesis. However, the production rate of polycarbonates was not mentioned in this research.50 Previously, the quality of final products (low thermal stability and poor physical properties) and energy input with higher heats and requirements for CO2 purity needed to be improved.79 However, research shows that the polycarbonate glass transition temperature and decomposition temperature can be altered. Hence, the polycarbonate


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thermal stability is improved by varying the different kinds of epoxides combined with propylene oxide in a terpolymer. In summary, the potential for use of CO2 in plastics production shows great potential for development. 4.2 Chemical production In CCU technology, one of the applications is CO2 hydrogenation to obtain methanol (MeOH):80 CO2 + 3H2 → CH3OH + H2O ΔH (300 K) = –49 kJ/mole

(1)

In the presence of Cs2CO3 as a catalyst, CO2 pressurization can be avoided, which reduces costs and increases the attractiveness of a MeOH CCU plant.51 In this case, the yield of MeOH is 78%, and the total reaction requires approximately 96 h. Although improved catalysts have been developed, the financial analysis of a MeOH CCU plant shows that the net present value (NPV) would be –1036M€ (~1165 million USD, 1€ = 1.12USD on 23/04/2019) in 20 years.81 The main variables are the investigation cost and CO2, H2 and MeOH prices. Some research has been conducted into using CO2 hydrogenation to produce methane (Eq. (2)).52 In this application, different kinds of methanation catalysts have been investigated in detail. These are based on Ni, Ru, Rh, Pd, Fe and Co. CO2 + 4H2 → CH4 + H2O ΔH (298.15 K) = –164 kJ/mole

(2)

To make the application feasible, the CO2 methanation reaction had been investigated.82 The result shows that a decrease in CO2 concentration with hydrogen will increase the conversion of CO2 to CH4. Also, methanation shows great potential for a carbon neutral economy, and should concentrate on an optimization of operating conditions and a reduction in total energy consumption. 4.3 Food and drink industry CO2 that is captured for CCU can be used to produce food. In the food and drink industry, CO2 can be used as a carbonating agent to produce soft drinks, alcoholic drinks and champagne.83 In addition, CO2 can be used as a preservative, packaging gas and solvent of flavor.83-84 The regulations of the International Society of Beverage Technologists define strict requirement for the food and drink grade of CO2.85 To obtain pure CO2 from flue gas, the plant set requires a stripper to yield a high concentration of CO2, which yields a toxicity issue.26 The use of captured CO2 without pressurization for on-site beverage supplementation can reduce CO2 transportation costs significantly. In the United States, 3.2–4.0 million metric tons of CO2 per year and 1.6–2.4 million metric tons of CO2 per year is required for food processing and carbonated beverages, respectively, in potential CO2 merchant markets.85 Therefore, promising potential exists to develop CCU technology in the food and drink industry.



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5. CCU technology using flue gas without CO2 purification and pressurization CCU technology that uses flue gas without CO2 purification and pressurization will be discussed in detail. Based on the disadvantage and difficulties that were introduced in previous paragraphs, CO2 utilization without purification and pressurization appears very promising. We focus on these points in this section. 5.1 Mineral carbonation Previously, because of the slow reaction rate and poor carbonation efficiency, most people did not discuss mineral carbonation specifically.62 However, interest in this topic has increased, because the products in this method are stable carbonates, which improves public perception, acceptance and economic benefits, which is lacking in current CCS.86 Rapid developments, optimization of the process reaction rate and efficiency and the costs of power consumption have decreased to make mineral carbonation processes available. In mineral carbonation, alkaline rock and/or wastes can be reacted with CO2 to yield carbonates as final products. alkaline rock/wastes + CO2 → carbonate (CaCO3/MgCO3) + residue

(3)

Figure 287 shows that ΔGº > 0 when CO2 reacts with the most materials, which results in the entire reaction requiring a supply of large amounts of energy and high-purity, high-pressure CO2. The Gibbs energy change of 100 kJ/mole in Figure 2 corresponds to 631 kWh/t-CO2 and can be converted to 44.2 USD/t-CO2 (0.07 USD/kWh). When CO2 reacts with alkaline rock or alkaline wastes, it will yield carbonates, such as CaCO3 and MgCO3, and the ΔGº of the reaction is negative and is much smaller than other reactions to ensure that the reaction that uses flue gas without purification and pressurization becomes available. Therefore, this reaction has several advantages. (A) Spontaneous reaction, which can make the reaction proceed with a relatively small amount of energy. (B) The product is more stable than other CCU technology applications and has many industrial applications. (C) This process has a relatively huge potential. Compared with other application products, the market size of CaCO3 is huge.88 Therefore, this process is not limited by market demand. In other words, mineral carbonation is a promising technology in CCU. Based on these advantages, mineral carbonation has great potential for development.


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Figure 2. Standard Gibbs free energy of formation for CO2 and related molecules.87 5.1.1 Source Table 4 summarizes the possible target materials. Several alkaline rocks can be used as target materials, such as olivine, wollastonite, serpentine and phlogopite. In natural rocks, chemical compounds usually exist as silicates. Alkaline wastes, such as waste cement powder, waste concrete, fly ash and bottom ash can also be used in mineral carbonation. Because these materials contain Ca and Mg, it is possible to obtain carbonates by their reaction with CO2, which reduces CO2 and landfill costs of wastes, and is effective for environment improvement. The ratio of Si content to Ca and Mg is important in terms of the amount of reactive free Ca/Mg that is unbound in the silica tetrahedra network structure; a higher Ca/Mg content to Si means a higher free Ca/Mg content. Seawater could also be used in CCU because it contains Ca and Mg. Because seawater already contains CO32- and HCO3-, the amount of newly fixed CO2 may be reduced; but, in this case, the best advantage is an unlimited source of Ca and Mg and huge potential for CO2 capture.105 Different alkaline rocks and wastes have different chemical compositions. Therefore, in mineral carbonation, direct and indirect carbonation without CO2 purification and pressurization can be achieved to great effect. Table 4. Summary of typical elemental compositions for alkaline minerals and wastes used for CCU Chemical compositions (mass%) Alkaline rocks/wastes

Ca

Mg

Si

Al

Fe


Minerals/chemical compound information


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Olivine89 Wollastonite89 Phlogopite89 Serpentine90 Waste-concrete powder91 Waste concrete92

0.9 29.2 0.8 N/A

25.7 0.1 12.3 27.1

24.7 13.5 21.6 20.1

N/A N/A N/A N/A

11.5 0.6 7.1 4.3

32.3

N/A

11.5

2.9

N/A

18.0

0.2

25.6

1.2

1.0

Concrete sludge93

12.3

N/A

1.5

0.3

1.3

Cement kiln dust94

24.6

1.2

6.2

1.8

2.0

Circulating fluid bed fly ash95

20.3

1.2

12.9

16.9

1.2

Coal combustion fly ash96

3.6

N/A

19.3

14.6

2.3

34.5

1.0

3.1

2.1

0.6

11.6

1.6

23.0

4.0

5.3

59.4

0.2

0.2

0.1

0.01

23.2

N/A

0.3

0.2

0.2

CaSO4·2H2O

36.2

6.2

8.3

0.6

12.8

Calcium silicates

Ladle slag102

30.2

9.0

7.0

11.8

0.6

Electric arc furnace slag102 Blast furnace slag103 Pulverized firing oil shale ash102

19.225.8 29.0

6.4

15.118.6 15.9

2.810.0 5.0

1.92.0 0.6

36.6

3.0

10.2

2.8

2.8

Bauxite residue104

1.8

0.05

10.2

10.7

19.0

Air pollution control fly ash from municipal solid waste incinerator97 Municipal solid waste incinerator bottom ash98 Paper mill waste99 Flue gas desulfurization gypsum100 Linz–Donawitz converter steel slag101

11.4

5.1.2 Temperature and pressure requirements


Mg2SiO4 CaSiO3 KMg₃AlSi₃O₁₀(OH)₂ Mg3Si2O5(OH)4 Hydrated cement and aggregates: calcium silicate hydrates and Ca(OH)2 etc. Hydrated cement: calcium silicate hydrates and Ca(OH)2 etc. *Composition in slurry state CaO, MgO Amorphous aluminosilicate glass matrix (SixAlyOz) and recrystallized minerals including CaO Chalco-aluminosilicate glass phase, mullite, quartz, and lime etc. N/A in ref. 94 *The main carbonation reaction occurs with portlandite (Ca(OH)2) Ca(OH)2, CaCO3 and Ca10(PO4)6(OH)2

Ca2SiO4, Ca12Al14O33, Ca2MgSi2O7 and MgO Ca–Mg-silicates and Mg–Fesilicates Amorphous calcium silicate CaO, Ca(OH)2, CaSiO3, Ca2SiO4, Ca3Mg(SiO4)2 *Effective contents for CCU are Na2O and Ca content in the form of katoite (Ca3Al2(SiO4)(OH)8)

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In mineral carbonation, different processing conditions exist according to different possible sources. Figure 3 summarizes the conditions for natural rocks,115-122 red gypsums,111-114 fly ashes,96,106-110 steel slags123-131 and waste concretes.92,132-141 The temperature and pressure requirements of natural rocks are higher than other target materials. Hence, this provides a good opportunity to use wastes as raw materials based on their reactive properties. However, owing to the slow mineral carbonation reaction rate, a long reaction time is usually required.62 Therefore, the reaction temperature may be altered depending on the application requirements. Because the ΔGº of the mineral carbonation is smaller than 0, the reaction is spontaneous, and waste concretes, red gypsums and steel slags can react at atmospheric pressure and normal temperature. In this range, CO2 does not need to be purified, and therefore, it can be used directly from flue gas.

Figure 3. Carbonation reaction conditions in mineral carbonation for each waste. 5.1.3 Research activities Detailed summaries of CCU by mineral carbonation have been introduced in recent reviews;62,142143 thus, typical research activities for mineral carbonation with a lower CO purity and pressure 2 are introduced in the section. The main research directions are direct carbonation by using active wastes for a longer time, and indirect carbonation under mild conditions by using intermediates with their effective regeneration methods. Ghacham et al.132 investigated the direct carbonation of waste concrete and anorthosite tailings in gas–solid–liquid and gas–solid routes by cement plant flue gas that contains 18.2% CO2. The results showed that waste concrete is more reactive than anorthosite tailings, and 34.6% of the introduced CO2 is converted into carbonate after 15 min of contact with the gas without chemical additives and at a relatively low gas pressure. Han et al.104 investigated direct carbonation using bauxite residue at atmospheric pressure and temperature with different CO2 concentrations of



1%, 14% and 100%. Short-term (24–48 h) and long-term (55 days) batch experiments with atmospheric CO2 were tested. The estimated maximum CO2 sequestration was ~0.083 g CO2/g bauxite residue. The reaction will be much smaller as field treatment does not allow for a thorough mixing and results in a delayed reaction rate. The Ca addition method can improve the efficiency. Kodama et al.144 proposed a two-step indirect mineralization process to convert slag with a recyclable reaction solution by using NH4Cl. In this research, 13% CO2 gas was used to precipitate CaCO3 and regenerate NH4Cl solution at 80°C. The energy consumption of this process is estimated to be 300 kWh/t-CO2. Wang et al145-146 designed an indirect carbonation process by using serpentine and the addition of ammonium salts. The total process is composed of several steps. In the first step, serpentine is dissolved by NH4HSO4 in 1 h. Then, impurities are removed via a pH-swing method by NH3 addition. Magnesium carbonate is precipitated by NH4HCO3 addition from CO2 absorption from flue gas by NH3 solution at 80°C and 30 min. (NH4)2SO4 as the remaining aqueous solution can be recovered by evaporation and heated to regenerate NH3 and NH4HSO4. They also investigated direct utilization of gaseous CO2 in flue gas to MgCO3 precipitation.146 Although the total pressure reached as high as 20 bar, they tested direct utilization of flue gas with different concentrations of CO2 (5%, 15%, 25%) in the presence of SOx and NOx at 80–140°C for 3 h. SOx and NOx could be removed to some extent by MgCO3 carbonation. Shuto et al.91,147 designed indirect carbonation by using waste concrete powder (byproduct of aggregate recycling from demolished concrete) as the raw material under atmospheric pressure and reaction with flue gas without CO2 purification. An innovative technique, bipolar membrane electrodialysis (BMED), was used to regenerate acid and alkali used in the process. A prerequisite for extracting the maximum amount of calcium requires acid and/or alkali agent use instead of water. However, chemical consumption costs influence the feasibility of the CCU. Moreover, the agents must be treated, which increases the process cost. BMED, which can regenerate alkali and acid solutions, will be used to achieve zero chemical consumption. In this process, calcium extraction is achieved by acid agents and any concentration of CO2 from the flue gas is captured by the alkali agent. After carbonate precipitation, the salt solution will be treated by BMED to regenerate alkali and acid solutions. Based on this innovative technique and idea, Shuto et al. designed a promising process with a leaching reaction time of 40 min, carbonate precipitation of 30 min and a BMED of 120 min. Vanderzee et al.148 investigated mineral carbonation using waste concrete via BMED. The result showed that 100% calcium can be leached from hydrochloric acid, and impurity removal can be achieved in the alkaline addition part. Finally, calcium carbonate can be obtained and agent regeneration can be conducted by BMED. 5.1.4 Business operation technologies Some mineral carbonation business processes have been used globally. All processes cannot be achieved without CO2 purification and pressurization as summarized in Table 5. Target materials, such as concrete sludge, thermal wastes, cement, concrete materials, coal fly ashes and concrete masonry have been used. Carbon 8 Aggregates Ltd.,149 Solidia Technologies Inc.,150


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Kajima Corporation, The Chugoku Electric Power, Denki Kagaku Kogyo Kabushiki Kaisha151-152 and Carboncure Technologies Inc.153 treated the relevant materials as mineral carbonation targets. Through mineral carbonation, construction materials are obtained as products and CO2 reduction is achieved. Carbon 8 Aggregates Ltd.149 used carbonation conditions of 100% CO2, 2 bar and 72 h. Solidia Technologies Inc.150 achieved the carbonation of calcium silicate cement within 145 h while curing at 30°C with 10% CO2 gas. Kajima Corporation, The Chugoku Electric Power and Denki Kagaku Kogyo Kabushiki Kaisha151-152 used flue gas from a thermal power plant directly for concrete material (mixture of water, cement, aggregates, special additives and coalfired fly ash) curing. CO2 gas 15%–20% was used at 40°C with a curing time of approximately 2 weeks.151 Carboncure Technologies153 supplied pure CO2 to produce concrete at atmospheric pressure and room temperature. Nippon Concrete Industry Co. Ltd.154-159 developed concrete sludge as a source to obtain calcium carbonates and phosphorus adsorbent (PAdeCS). The process in Figure 493 shows that boiler gas with a CO2 concentration of 6%–13% was used directly. The main equipment was a calcium extraction reactor, filter press, CaCO3 crystallization reactor and a hammer crusher. This process can be operated under atmospheric pressure and at an ordinate temperature without any chemical addition, and without generating secondary wastes. The process water can be used repeatedly. The by-product, PAdeCS, is developed to remove phosphorus from aqueous solution, neutralize acid mine drainage or acidic hot spring water and remove blue–green algae in closed water systems. Table 5. Summary of current business operation technologies of mineral carbonation Name

Target materials Thermal waste

Final product

Application

Remarks

Carbon8 Aggregate (C8Agg)

Solidia Technologies, Inc. 150

Cement

Solidia cement, Solidia concrete

Blocks, precast concrete, ready-mix concrete, screed. Construction materials

Kajima Corporation, The Chugoku Electric Power and Denki Kagaku Kogyo Kabushiki Kaisha151-152

Concrete materials, coal fly ashes.

CO2 storage under infrastructure by concrete materials (CO2 SUICOM)

Suitable for use with fiber reinforcement, good consistent quality, good reliability of supply, low shrinkage, low density, CO2 reduction, binder addition required Increased durability, streamlined secondary processing, near-zero waste, lower water consumption, expense reduction, CO2 reduction CO2 reduction, reduced cement usage, high durability

Carbon 8 Aggregates Ltd.149

Concrete curbs, fence block, precast concrete



CarbonCure Technologies Inc. 153 Nippon Concrete Industry Co. Ltd.

Readymix concrete, concrete masonry Concrete sludge

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Enhanced concrete

Construction industry

CO2 reduction, increased compressive strength performance, increased durability

PAdeCS

Environmental purification agents

CO2 reduction, neutralization of acidic drainage, good absorption ability, great sterilization

93,154-159

Figure 4. Overall process in pilot-scale plant.93 5.2 Biological conversion In biological conversion, two main points of focus are carbon fixation pathways and organisms. Diverse organisms have different carbon fixation pathways based on their growth characteristics, thermal stability, types of metabolites produced and tolerance to inhibitors.160 For example, algae are the most widely known biological application in CCU technology. CO2 is dissolved into the sea and can be used to grow algae. Algae are widely distributed, fast growing and have a rapid CO2 uptake.161 Also, they are available for genetic modification.162-163 Hence, algae have great potential for CCU technology development. The carbon fixation pathway is the Calvin–Benson–Bassham cycle and the key CO2 fixating reaction occurs as in the following reaction equation:160 Ribulose-1,5-bisphosphate + CO2 + H2O → 2 × 3-phosphoglycerate

(4)

Cyanobacteria have been noticed in this field. The carbon fixation pathway of cyanobacteria also occurs by the Calvin–Benson–Bassham cycle. Some occurrence of calcifying cyanobacteria exists in alkaline seas globally.164 Calcification can provide a protective shield against high light exposure, enhance nutrient uptake, provide toxic levels of intracellular calcium and increase CO2


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uptake. Some research has focused on cyanobacteria calcification to improve their properties in CCU, and is classified as a biomineralization process.164-165 Jansson mentioned that “cyanobacterial calcification are stromatolites and whitings, very fast, large-scale precipitations of fine-grained CaCO3 together with organic compounds.”164 The research trend of this topic has focused on calcification to define the specific conditions and applications and to focus on clarifying reactions, such as nucleation, phase transition and crystallization in biomineralization. This application could use gas sources from municipal solid waste incineration, small coal-fired power plants and CO2 emitting industries.164 A promising CCU technology is microalgae use to produce biofuels.161,166 Advantages of this technology are greater production yields, available land areas, a reduction in atmospheric CO2 emissions, and a reduced competition for land.161 Weyer et al.167 indicated that the theoretical calculated maximum annual oil production from algae was 354,000 liters per hectare per year; the best case observed in their experiments ranged from 40,700 to 53,200 liters per hectare per year (which corresponds to 4.07 × 10-3 to 5.32 × 10-3 m3/m2/year). Anjos et al.168 stated that the CO2 biofixation rate of Chlorella vulgaris reached 2.22 g/L/day with low CO2-concentration flue gas (6.5% CO2). Microalgae can capture light for conversion to energy, which results in a higher photosynthetic efficiency compared with land plants.169 Microalgae can also produce biohydrogen and biogas as products.166 This application can be achieved with wastewater because of the large amounts of nutrients in the water.170 Some researchers have studied the behavior of microalgae in different conditions, such as natural waterbodies, wastewater, open pond systems and high concentrations of nitrogen and organics,170 and also investigated different microalgae types that grow in different environments, such as CO2-enriched gas streams,171 waste heat172 and waste glycerol.173 Many researchers have demonstrated that biological conversion through CO2 capture by microalgae is available and possible. However, few global companies use this approach. The most important challenge is the cost of operation, which becomes an impediment to process commercialization.163 Therefore, biological conversion that uses microalgae has allowed researchers to develop the by-product value to make the process beneficial.160 The genetic and metabolic engineering of microalgae has been developed recently and allows this technology to achieve a high potential for process feasibility. The technological development of metabolics and the gene changing of microalgae is attractive, and detailed metabolic studies of different major algal lineages are necessary.

Conclusions This study reviews CCU technologies without CO2 pressurization and/or purification. We focused initially on the differences between CO2 purity and pressure of waste CO2 and feedstock CO2. We have summarized several main CO2 sources in detail. The CO2 purity is below 40% in most flue gas sources. Most CCU technologies require pure CO2 and a high pressure. Therefore, most CCU technologies usually require purification and pressurization. However, purification and pressurization in CCU technologies obstructs developments in CCU technology. Disadvantages



include the requirement of an additional CO2 purification and pressurization plant, the high expense and the large energy input for CO2 purification and pressurization processes, and the processes are almost 70%–75% of the cost of the entire process and require critical land use, equipment, and energy input. Hence, this study reviews CCU technologies without CO2 pressurization and/or purification. A promising solution includes mineral carbonation and biological conversion. In mineral carbonation, direct carbonation with active wastes is possible, and the increase in maximum CO2 sequestration and carbonation rate are future research directions. Indirect carbonation by using recyclable ammonium salt systems and the BMED system can achieve great results and effective regeneration. The optimized regeneration system and a more detailed cost estimate are future research prospects. To study the feasibility, a demonstration of direct and indirect carbonation that uses actual waste gas that contains a greater amount of impurities is needed. In biological conversion, microalgae provide competitive merits to produce biofuels from flue gas and atmospheric CO2. The genetic and metabolic engineering of microalgae and the development of several products, such as biohydrogen and biogas, make this technology potentially feasible. For all other CCU approaches, research trials to decrease the required CO2 purity and pressure of the feedstock CO2 will be needed. In summary, CCU technology without CO2 purification and pressurization provides prospective opportunities in various CO2 emitters to reduce future CO2 emissions.

Acknowledgements We thank Laura Kuhar, PhD, from Edanz Group (www.edanzediting.com/ac) for editing a draft of this manuscript.

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