Abstract
Recent years have seen a sharp rise in CO2 emissions into the atmosphere, which has contributed to the issue of global warming. In response to this several technologies have been developed to convert CO2 into fuel. It is discovered that the employment of a solar-driven thermochemical process (S-DTCP) that transforms CO2 into fuels can increase the efficiency of the production of sustainable fuels. The process involves the reduction of metal oxide (MO) and oxidizing it with CO2 in a two-step process using concentrated solar power (CSP) at higher and lower temperatures, respectively. This study summarizes current advancements in CO2 conversion methods based on MO thermochemical cycles (ThCy), including their operating parameters, types of cycles, and working principles. It was revealed that the efficiency of the solar conversion of CO2 to fuel is not only influenced by the composition of the MO, but also by its morphology as well as the available surface area for solid/gas reactions and the diffusion length. The conversion mechanism is governed by surface reaction, which is influenced by these two parameters (diffusion length and specific surface area). Solar energy contributes to the reduction and oxidation steps by promoting reaction kinetics and heat and mass transport in the material. The information on recent advances in metal oxide-based carbon dioxide conversion into fuels will be beneficial to both the industrial and academic sectors of the economy.
1 Introduction
Fossil fuels provide a significant amount of energy (Mofijur et al., 2013a), but their ongoing usage for industrial purposes is threatening the atmosphere because of the high amounts of greenhouse gas emissions i.e. CO2 (Mofijur et al., 2013b). The impacts of greenhouse gases are widely acknowledged to be one of the fundamental causes of climate change (Langford, 2005). In order to mitigate climate change, it is necessary to minimize the emission of CO2 (Jacobson et al., 2019). Carbon dioxide is a colorless, naturally occurring gas that is made up of molecules that each have one carbon atom covalently double bonded to two oxygen. Carbon dioxide, in addition to other greenhouse gases, is a significant contributor to the ability of the earth to sustain a temperature that is suitable for human habitation (). Carbon dioxide at low concentrations has less toxicological effect. It causes the development of hypercapnia and respiratory acidosis when more than 5% are present in the atmosphere (Kettner et al., 2013). As a result of the increased effects of parasympathetic nerve activity, which is thought to be caused by interfering with the breakdown of acetylcholine by acetylcholinesterase, severe acidosis can result in a decrease in the rate of respiration (Permentier et al., 2017).
More than 10% of carbon dioxide concentrations have been shown to produce convulsions, coma, and even death (Żaba et al., 2011). Increased CO2 levels of more than 30% act quickly and can cause loss of consciousness in a matter of seconds. This might explain why sufferers of unintentional intoxication frequently do not act to fix the problem. Capturing carbon dioxide emissions at the site of emission is an appealing concept that has gained popularity in recent years and converting it into useful products such as synthetic fuels (Helal et al., 2020), with the entire cycle being powered by renewable resources such as solar irradiation (). Figure 1 presents the different S-DTCPs used to produce industrial items and fuels. In general, these processes can be divided into two categories: the creation of industrial items and the generation of fuels (Mustafa et al., 2020). Solar fuels are a particularly tempting alternative to non-renewable fossil fuels because of the availability of solar energy and the fact that the production cycle produces almost no emissions (Shahabuddin et al., 2021). The method of manufacturing solar fuels generally comprises (i) thermochemical reduction-oxidation (redox) splitting of plentiful CO2/H2O into a CO/H2 known as syngas; and (ii) hydrocarbon fuel synthesis by some well-established gas to liquid processes (e.g. Fischer–Tropsch). In contrast, the commercialisation of solar-powered syngas has not yet been realised, mostly as a result of the process’s low solar-to-fuel efficiency ().
FIGURE 1
The development of redox materials has received increased attention in recent years, intending to increase the efficiency of the technology while also making it more financially viable (Scheffe and Steinfeld, 2014). The ability of a redox material to exchange oxygen (release/absorption of O2) has a direct and proportional impact on the amount per mass of material. The use of redox materials in solar fuel production processes has proven successful in the past. Oxide minerals such as ferrites (Kodama et al., 2005; Scheffe et al., 2013a) and hercynite (; Muhich et al., 2013), and more recently ceria (; ) and perovskites (; ; ; Takacs et al., 2016), have been used successfully as redox materials (). It is evidenced that many pieces of researches are published on thermochemical splitting of CO2 but few researchers reviewed and analysed them.
Based on the aforementioned literature review, this min review aimed at summarizing the most recent works that are focused on MO-based solar thermochemical CO2 splitting to fuel. This condensed review will provide researchers updated news about the research directions in this topic and discuss it’s the technology readiness level as well as provide recent updates about scientific and industrial aspect of this technology.
2 Solar thermochemical splitting of carbon dioxide via MO-based reaction
It is possible to operate at moderate temperatures and avoid separation difficulties by dissociating CO2 in many steps, each of which makes use of metal oxides during the redox processes (Snoeckx and Bogaerts, 2017). The first phase is endothermic, and it involves the reduction of oxidized MO (MOox) to metal (M) or reduced MO (MOred) using solar thermal energy. In the second phase, the MOred is oxidised with CO2, resulting in the generation of CO. The MOox can be used again for the first step (Mustafa et al., 2020). Multiple redox cycles are known to exist that can be followed in order to separate H2O from CO2. Theoretically, these redox cycles have an efficiency of greater than 40%, according to the researchers. It is generally accepted that two-cycle classes of metal oxides, both volatile and non-volatile, should be considered (Scheffe and Steinfeld, 2014). Doping techniques are used in both types of cycles to improve the thermodynamic, kinetic, and physical properties.
The basic equations for this cycle are:
Deepak and Banerjee presented literature that analysis the thermal efficiency of the ThCy on iron and Ceria under different conditions. It was concluded that the thermal efficiency in the temperature range 600–2300 ranged from 35 to 70% without any heat recovery. The global sun-to H2 efficiencies for iron and zinc oxide are estimated to be within the ranges at 43–65.2% and 31.6–61.8%, respectively. The variations in the thermal efficiencies were related to the considerations of the optical efficiency of the heliostat field and the thermal efficiency of the reactor. For ceria-based solar ThCy was determined to be in the range of 20.2%–29.5% without heat recovery and increase to 50% with heat recovery A second law analysis was used to examine the exergy efficiency of the ceria-based ThCy as 23% and 26% for reactors operating temperature of 2300 K and 2600 K, respectively
2.1 Solar thermochemical splitting of carbon dioxide via ceria-based redox reactions
Ceria (CeO2)-based ThCy may be able to store intermittent and diluted solar energy by generating chemical fuels. Many researchers have experimented with and reported the performance of ceria-based ThCy. For example, Hathaway, Bala Chandran, Gladen, Chase, Davidson (Hathaway et al., 2016) et al. studied a 4.4 kW solar receiver/reactor’s ability to split CO2 through the isothermal CeO2 thermochemical redox cycle in the course of steady-state operation within a high-flux solar simulator. At 1750K, a steady-periodic operation took place where 360 ml min−1 of CO generated more than 45 redox cycles in a continuous flow. A 95% of the sensible heat derived from process gases was recovered. Without considering the energy costs of N2 production, the solar-to-fuel efficiency was 1.64%. N2 is used as a sweep gas for reduction. Including the solar energy needed for N2 production through cryogenic separation, the solar-to-fuel efficiency was found to be 0.72%. A conclusion was reached that splitting CO2 or water, following the isothermal approach, via a thermochemical MO redox cycle does not show prospects for development. There are certain thermodynamic limitations in this cycle and other issues like the inability to increase reactor efficiency beyond 2%.
Lin, Samson, Wismer, Grolimund, Alxneit, Wokaun (Lin et al., 2016) investigated the dual-phase Zn that was modified by ceria synthesized via coprecipitation to be used as a redox material to thermochemically split H2O and CO2. In the first few cycles, it was observed that the materials showed a significant increase in the productivity of H2 and CO. There was a correlation between the increased productivity in the initial cycles and a considerable loss of Zn during the sublimation of ZnO. His observation suggests that the secondary ZnO phase in Zn-modified ceria expressed a negative effect on its thermochemical activity.
Nair, Abanades (Nair and Abanades, 2016a) studied the combination of methane being partially oxidized with the splitting of H2O and CO2 set in solar thermal conditions. CO2 and H2O were split by CeO2 by utilizing concentrated solar energy. The reaction temperatures were varying from 900 to 1100 °C. This experiment took place inside a solar-powered thermogravimetric system and results showed close reaction orders of both CO2-induced oxidation of CeO2−δ and CH4-induced reduction with corresponding activation energies, 36 and 109 kJ mol−1. A comparison of the outcomes was noted down with the ones acquired from surfactant-induced self-assembly and hydrothermal templating. The material synthesis that occurred via hydrothermal and self-assembly methods had high reaction rates and stability on cycling. MgO promoted CeO2 resulted in a higher rate of reduction and highest nonstoichiometric (δ = 0.431) when reduction occurred at a temperature of 1000°C. Results about the amount of evolved CO implied that reoxidation is almost complete as it came out to be the highest (δ = 0.402). For thermal reduction of ceria, the obtained nonstoichiometric and consequent fuel effectivity were 10 times more than the values that were reported. Some studies were performed in solar reactor prototypes to enable partial ceria reduction in the presence of methane. Subsequently, oxidation with ceria was promoted by H2O/CO2. MgO and Al2O3 took place and were experimented with under packed bed conditions. This was put into comparison with commercial ceria based on the production of syngas. MgO promoted CeO2 showed remarkable augmentation in the system efficiency.
Haeussler, Abanades, Julbe, Jouannaux, Cartoixa (Haeussler et al., 2020) designed, constructed and experimented with a new solar reactor that is monolithic and has compatibility with ceria redox reactions when the solar radiation is concentrated. The ceria redox material is built as structures that are porous and reticulated with controlled cell sizes and gradients, 10–60 pores per inch (ppi). These features allow effective volumetric solar radiation absorption and microscale interconnected porosity. This system helps increase efficiency in solid-gas reactions. The effect of functioning conditions like the type of oxidizing gas, pressure and reduction and oxidation temperatures on reactor performance was examined. When the temperature for reduction was increased or the pressure was decreased, the yields of fuel production and ceria reduction extent improved (up to 341 µmol/g). Decreasing CO: CO2, by raising the total inlet gas flow rate, or increasing inlet CO2 concentration resulted in an improved rate of oxidation by as far as 9.3 ml/g/min. The observed fuel production rates surpassed the maximum of the previously recorded values 8 times more utilizing the ceria porous foams that were manufactured to be highly reactive that underwent cycling between 900°C and 1400°C. In 100% of CO2, oxidation took place upon dynamic cooling. A mean H2/CO production of ∼280 Ncm (Langford, 2005)/cycle was attained where 64 cycles were performed, where solar-to-fuel efficiency reached ∼7.5% with significant performance stability of the material.
Riaz, Ali, Enge, Tsuzuki, Lowe, Lipiski (Riaz et al., 2020) investigated the effects of the concentrations of two elements, V and Ce, in vanadia–ceria multiphase systems for the generation of synthesis gas through the splitting of CO2 and H2O following thermochemical redox cycles of splitting that had methane partial oxidation reactions integrated with it. The concentration range varied from 0 to 100% each. Prepared oxygen carriers’ oxidation is executed by separate and sequential splitting reactions of CO2 and H2O. Pure CeO2 showed the lowest oxygen exchange capacities while pure V2O5 showed the highest. Pure CeO2 also exhibited the lowest performance of syngas production whereas pure V2O5 showed the highest. The systems involving mixed-oxide showed a balanced neutral performance where the oxygen exchange capacity was recorded to be 5 times higher than what pure CeO2 shows when the length of methane cracking was decreased. Having 25% V added to CeO2 resulted in a CeVO4 and CeO2 optimum mixture for the improved splitting of CO2 and H2O. When the concentration of V is high, the formation of cyclic carbide and oxidation are consequent to a syngas yield that is greater than pure CeO2. The synthesis methods used in preparation of ceria based material is presented in Table 1.
TABLE 1
| Synthesis approach | Cycles | Reduction temperature (°C) | Average O2 released (µmol/g) | Re-oxidation temperature (°C) | Average H2 produced (µmol/g) | Average CO produced (µmol/g) | Reference |
|---|---|---|---|---|---|---|---|
| Commercial | 1 | 2000 | − | 550 | 3254 | − | |
| Combustion | 12 | 1500 | 49.55 | 1000 | 33.9 | − | Kaneko et al. (2008) |
| Commercial | 1 | 1600 | 263.4 | 800 | 526 | − | |
| 500 | 1500 | 133.9 | 800 | 267 | − | ||
| Commercial | 4 | 1581-1624 | 96.4 | 900 | − | 175 | |
| 4 | 1622-1640 | 118.3 | 900 | 188.9 | − | ||
| Co-precipitation | 3 | 1400 | 50 | 1000-1200 | − | 100 | Meng et al. (2011) |
| 3 | 1400 | 70 | 1000-1200 | − | − | ||
| Polymerized complex | 4 | 1500 | 27 | 500 | − | − | Le Gal et al. (2011) |
| Polymerized complex | 9 | 1500 | 79.1 | 500 | 142.4 | − | Petkovich et al. (2011) |
| Commercial | 10 | 1494-1582 | 67.9 | 927 | 98.66 | 41 | Lapp et al. (2012) |
| Commercial | 1 | 1597 | 100.8 | − | − | 203 | |
| Auto- combustion | 22 | 1500 | 55.8 | 1500 | 87.5 | − | |
| Commercial | 2 | 1400 | 80 | 1050 | 120 | − | Hao et al. (2013) |
| Hydrothermal | 1 | 1500 | 254.5 | 800 | − | 348 | Kang et al. (2014) |
| Electrospinning | 10 | 1200 | − | 800 | − | 18 | Scheffe et al. (2013c) |
| 50 vol% pore-forming agent | 20 | 1500 | − | 1000 | − | 199.6 | |
| 30 vol% pore-forming agent | 1 | 1574 | 112.5 | − | − | 224 | |
| Complex polymerization | 9 | 1500 | 69.2 | 500 | − | − | |
| Commercial Replication | 1 | 1547 | 97.3 | − | − | 196.9 | Marxer et al. (2015) |
| Commercial | 2 | 1500 | 130 | 1000 | − | 240 | Zhao et al. (2016) |
| Commercial | 3 | 1400 | 30 | 1000 | − | 60 | Zhao et al. (2016) |
| Co-precipitation | 4 | 1290 | − | 1000 | 50 | − | |
| 4 | 1400 | − | 1000 | − | 90 |
Experimental findings reported in case of CeO2 based solar thermochemical H2O/CO2 splitting cycles. Reprinted with permission.
It can be seen that both binary and ternary MOs containing Ce and other metals at different compositions can be utilized in ThCy. Table 2 illustrates the O2 and H2/CO productivities of binary and ternary ceria-based composites in multiple solar ThCys. It was discovered that adding some dopants increased the ceria-based material’s reactivity and thermal stability through a number of ThCyas.
TABLE 2
| Dopant concentration | Synthesis approach | Cycles | Reduction temperature (°C) | Average O2 released (µmol/g) | Re-oxidation temperature (°C) | Average H2 produced (µmol/g) | Average CO produced (µmol/g) | Reference |
|---|---|---|---|---|---|---|---|---|
| 10% Mn | Combustion | 1 | 1500 | 80 | 1000 | 168.3 | − | Roeb et al. (2012) |
| 10% Ni | Combustion | 1 | 1500 | 115.2 | 1000 | 121.8 | - | |
| 10% Cu | Combustion | 1 | 1500 | 69.6 | 1000 | 43.8 | - | |
| 10% Fe | Combustion | 4 | 1400 | 59.4 | 1000 | 100.9 | - | |
| 11% Fe | Combustion | 11 | 1400 | 58.03 | 1000 | 89 | - | |
| 75% Zr | Co-precipitation | 4 | 1400 | − | 1100 | 26 | - | Kaneko and Tamaura, (2009) |
| 1 | 1400 | − | 1100 | − | 158.5 | |||
| 50% Si | Co-melting | 1 | 1500 | 1110 | 530 | 1500-1940 | − | Miller et al. (2008) |
| 50% Ti | Co-melting | 1 | 1400 | 1000 | 630 | 1560-1740 | − | |
| 50% Fe | Co-melting | 1 | 1400-1500 | 1000 | 500 | 600 | − | |
| 50% Nb | Co-melting | 1 | 700 | 840 | 500 | 820 | − | |
| 5% Ni | Combustion | 8 | 1400 | 62.5 | 1000 | 89 | − | |
| 15% Sm | Commercial | 53 | − | − | 700 | 343.8 | − | |
| 10% Ni | Wetness impregnation | 11 | − | − | 500 | 151.8 | 10.3 | |
| 15% Sm | ||||||||
| 25% Zr | Pechini | 2 | 1450 | 110 | 950 | 130 | − | Le Gal and Abanades, (2011) |
| 25% Zr | Co-precipitation | 2 | 1400 | 180 | 1050 | 320 | − | Kaneko et al. (2011) |
| 25% Zr | Pechini | 3 | 1400 | 140 | 1000-1200 | − | 200 | Meng et al. (2011) |
| 3 | 1400 | 220 | 1000-1200 | 380 | − | |||
| 20% Zr | Polymerized complex | 4 | 1500 | 129.5 | 500 | − | − | Le Gal et al. (2011) |
| 10% Mg | Polymerized complex | 9 | 1500 | 88.4 | 500 | 173.9 | − | Petkovich et al. (2011) |
| 10% Sc | Polymerized complex | 9 | 1500 | 98.7 | 500 | 181 | − | |
| 10% Hf | Polymerized complex | 9 | 1500 | 132 | 500 | 200.9 | − | |
| 10% Pr | Combustion | 1 | 1500 | 104 | 750 | 177 | − | |
| 2.5% Li | Polymerized complex | 9 | 1500 | 1300 | 500 | 2400 | − | Le Gal and Abanades, (2012) |
| 10% Ta | Co-precipitation | 1 | 1450 | − | 1040 | 140 | − | |
| 25% Ta | Co-precipitation | 2 | 1400 | − | 1050 | 70 | − | |
| 10% La | Co-precipitation | 3 | 1400 | 60-100 | 1000-1200 | 120-140 | − | |
| 10% Sm | Co-precipitation | 2 | 1400 | 60 | 1050 | 110 | − | |
| 10% Gd | Co-precipitation | 2 | 1400 | 60 | 1050 | 100 | − | |
| 25% Zr | Co-precipitation | 2 | 1400 | 170 | 1050 | 270 | − | |
| 23% Zr | Co-precipitation | 2 | 1400 | 140 | 1050 | 260 | − | |
| 2% La | ||||||||
| 23% Zr | Co-precipitation | 2 | 1400 | 150 | 1050 | 240 | − | |
| 2% Y | ||||||||
| 25% Zr | Co-precipitation | 2 | 1400 | 190 | 1050 | 280 | − | |
| 1% Gd | ||||||||
| 25% Zr | Co-precipitation | 2 | 1450 | 140 | 950 | − | 120 | |
| 10% Zr | Co-precipitation | 2 | 1400 | 90 | 1050 | − | 120 | |
| 25% Zr | Pechini | 3 | 1400 | 120-180 | 1000-1200 | − | 140-240 | |
| 54% Zr | Commercial | 2 | 1400 | 230 | 1050 | 390 | − | Hao et al. (2013) |
| 50% Zr | Co-precipitation | 2 | 1400 | 230 | 1050 | 370 | − | |
| 37% Zr | Pechini | 2 | 1400 | 210 | 1050 | 370 | − | |
| 24% Zr | Pechini | 2 | 1400 | 190 | 1050 | 340 | − | |
| 1% Gd | ||||||||
| 40% Zr | Commercial | 2 | 1300 | 150 | 1050 | 290 | − | |
| 15% Zr | Auto-combustion | 4 | 1400 | 160 | 900 | − | 310 | Scheffe et al. (2013d) |
| 15% Zr | Auto-combustion | 100 | 1400 | 100-150 | 900 | − | 200-280 | |
| 20% Zr | Co-precipitation | 2 | 1400 | 116 | 1100 | − | 192.42 | Meng and Tamaura, (2014) |
| 10% Ni | Co-precipitation | 2 | 1400 | 158.5 | 1100 | − | 135.7 | |
| 20% Zr | ||||||||
| 10% Fe | Co-precipitation | 2 | 1400 | 184.4 | 1100 | − | 165.2 | |
| 20% Zr | ||||||||
| 10% Mg | Co-precipitation | 2 | 1400 | 140 | 1100 | − | 241.5 | |
| 20% Zr | ||||||||
| 10% Mn | Co-precipitation | 2 | 1400 | 249 | 1100 | − | 102.2 | |
| 20% Zr | ||||||||
| 2% Mg | Co-precipitation | 2 | 1400 | 296.9 | 1100 | − | 282.1 | |
| 20% Zr | ||||||||
| 10% Hf | Polymerized complex | 5 | 1500 | 137.9 | 500 | 255.3 | − | Jiang et al. (2014) |
| 10% Pr | ||||||||
| 20% Ti | Co-precipitation | 1 | 1400 | 589 | 900 | − | 53.6 | Kang et al. (2014) |
| 25% Hf | Hydrothermal | 1 | 1400 | 321.4 | 1000 | − | 111.6 | |
| 15% La | Hydrothermal | 1 | 1500 | 321.4 | 800 | − | 272 | |
| 25% Zr | Combustion | 1 | 1400 | 290.2 | 900 | − | 473.2 | |
| 20% Sn | Combustion | 1 | 1400 | 500 | − | − | − | |
| 15% Sm | Hydrothermal | 1 | 1500 | 169.4 | − | − | − | |
| 15% Y | Hydrothermal | 1 | 1500 | 174 | − | − | − | |
| 10% Mg | Hydrothermal | 3 | 1400 | 135.7 | 1100 | − | 232.6 | Jiang et al. (2014) |
| 20% Zr | ||||||||
| 5% Ca | Hydrothermal | 3 | 1400 | 160 | 1100 | − | 282.5 | |
| 20% Zr | ||||||||
| 5% Mg | Hydrothermal | 2 | 1200 | 60.7 | 1000 | − | 107 | |
| 20% Zr | ||||||||
| 5% Ca | Hydrothermal | 2 | 1200 | 70.1 | 1000 | − | 137.0 | |
| 20% Zr | ||||||||
| 10% Zr | Electrospinning | 10 | 1140 | − | 740 | − | 71.4 | Scheffe et al. (2013c) |
| 2.5% Zr | Electrospinning | 108 | 1400 | − | 800 | − | 178 | |
| 10% Dy | Complex polymerization | 9 | 1500 | 48.2 | 500 | − | − | |
| 10% Y | Complex polymerization | 9 | 1500 | 51.3 | 500 | − | − | |
| 10% Sc | Complex polymerization | 9 | 1500 | 83 | 500 | − | − | |
| 10% Zr | Complex polymerization | 9 | 1500 | 108.9 | 500 | − | − | |
| 10% Hf | Complex polymerization | 9 | 1500 | 137 | 500 | − | − | |
| 15% Zr | Auto-combustion | 4 | 1400 | 160 | 900 | − | 310 | |
| 2.5% Sm | Auto-combustion | 4 | 1400 | 150 | 900 | − | 300 | |
| 15% Zr | ||||||||
| 2.5% Y | Auto-combustion | 4 | 1400 | 140 | 900 | − | 260 | |
| 15% Zr | ||||||||
| 2.5% La | Auto-combustion | 4 | 1400 | 140 | 900 | − | 270 | |
| 15% Zr | ||||||||
| 2.5% Gd | Auto-combustion | 4 | 1400 | 140 | 900 | − | 270 | |
| 15% Zr | ||||||||
| 10% Zr | Solid state reaction | 2 | 1500 | 160 | 1000 | − | 330 | Zhao et al. (2016) |
| 20% Hf | Solid state reaction | 2 | 1500 | 230 | 1000 | − | 390 | |
| 2% Li | Solid state reaction | 2 | 1500 | 170 | 1000 | − | 340 | |
| 9.8% Hf | ||||||||
| 50% Zr | Co-precipitation | 3 | 1400 | 140 | 1000 | − | 270 | Zhao et al. (2016) |
| 2% Pr | Co-precipitation | 3 | 1400 | 140 | 1000 | − | 290 | |
| 8% La | ||||||||
| 50% Zr | ||||||||
| 50% Fe | Sol-gel | 8 | 1400 | 70 | 1000 | − | 120 | |
| 5% Zr | Co-precipitation | 4 | 1400 | 120 | 1000 | − | 170 | |
| 5% Hf | ||||||||
| 5% Zr | Co-precipitation | 20 | 1400 | 110 | 1000 | − | 160- | |
| 5% Hf | ||||||||
| 20% Zn | Co-precipitation | 4 | 1290 | − | 1000 | 20−60 | ||
| 4 | 1400 | − | 1000 | − | 60-110 | |||
| 1% Rh | Co-precipitation | 6 | 1400 | 74 | 500 | 130 | − | |
| 59 | 1400 | 80 | 500 | 150 | − | |||
| 11 | 1500 | 120 | 500 | 200 | − | |||
| 50% Mg | Solid solution | 3 | 1000 | 1850 | 1000 | − | 1720 | |
| 50% Al | Solid solution | 3 | 1000 | 1130 | 1000 | − | 1100 |
Experimental findings reported in case of doped ceria based solar thermochemical H2O/CO2 splitting cycles. Reprinted with permission from Bhosale et al. (2019)
2.2 Solar thermochemical splitting of carbon dioxide via perovskite-based redox reactions
Perovskites have the capability of providing high production of O2 at temperatures that are comparatively high (). Additionally, they can integrate reduction oxidation that demands energy (Sastre et al., 2017a). The cation found in the M site determines the redox properties of perovskites. It is denoted by ABO3−δ and falls in the category of nonstoichiometric oxides (Mustafa et al., 2020). There has not been much investigation into these oxides to reduce metals in thermochemical cycles (). The cation sites, A and B, are where the replacement of dopants can take place. This makes material configurations notably larger inside perovskites relative to ceria. Research related to thermodynamics that involved oxygen non-stoichiometry data evaluation and extracting entropies and enthalpies have proven lanthanum strontium manganite perovskites’ (indicated by La1-xSrxMnO3−δ) capability in augmenting oxygen exchange capacity relative to pure ceria (Scheffe et al., 2013b). It has been experimentally confirmed that even though the extent of reduction is notably higher, oxidation is thermodynamically less viable and this causes oxidation to be incomplete. Nevertheless, total CO generation from the decomposition of CO2 continues to be significantly higher in contrast to ceria.
Perovskites are considered to be potential redox materials for fuel synthesis via thermo-electrochemical means Ezbiri, Takacs, Stolz, Lungthok, Steinfeld, Michalsky (). For designing perovskites that constitute balanced redox energetics for the thermochemical splitting of CO2, electronic structure computations predict lattice oxygen vacancy activities as well as the stability of a representative range of perovskites against phase changes of crystals and deleterious carbonate formation (Rafique et al., 2022). The range of free energy calculated for isothermal and temperature-swing redox cycles is used for illustrating systematic changes in the characteristics of these materials when they have specific metal cations doped with them.
Mulmi, Chen, Hassan, Marco, Berry, Sharif, Slater, Roberts, Adams, Thangadurai (Mulmi et al., 2017) examined the usage of perovskite oxides that are nonstoichiometric, (Ba2Ca0.66Nb1.34−xFexO6−δ (BCNF) (0 ≤ x ≤ 1)), for the purpose of splitting CO2 into C, CO, and O2 at increased temperatures. Double perovskite-type BCNF’s chemical stability is exhibited by powder X-ray diffraction after exposure to CO2 of 2000 ppm in Ar at a temperature of 700°C. All members of x ≤ 0.66 BCNF express great chemical stability despite being in conditions at 700 °C temperature and pure CO2. The creation of solid carbon upon being exposed to CO2 was confirmed through scanning electron microscopy along with Raman spectroscopy, DFT analyses, temperature-programmed oxidation (TPO) and mass spectroscopy (MS), and energy-dispersive X-ray. As Fe increases, more solid carbon is produced in BCNF. In the Mössbauer spectroscopy of the as-prepared BCNF, Fe3+, Fe4+ and Fe5+ were found. When exposed to Ar, a constituent Fe that has higher valence undergoes reduction to Fe3+ followed by Fe3+ enhanced CO2 reduction being oxidized. The overall outcomes of BCNFs displayed redox activity at much lesser temperatures if put into comparison with state-of-the-art ceria for reducing CO2. Thus, it can be seen that there is a possibility of putting them into use in fuel technologies that are powered by renewable sources.
Sastre, Carrillo, Serrano, Pizarro, Coronado (Sastre et al., 2017b) proposed mixed oxides with perovskite structure as an alternate material for solar fuel generation through thermochemical redox cycles. The system La0.6Sr0.4Mn1−xAlxO3 (x = 0–0.8) was chosen for this study as it has the required features: thermal stability that is high and rapid oxidation kinetics. The ratio of Al/Mn and its impact on the redox properties were also looked into. After characterization through thermogravimetric analysis, the five oxides samples having varying Al amounts verified the high redox capacity. They also verified the favourable behaviour of these materials in consecutive cycles. According to the results, consequent of reduction at temperature 1300 °C in the inert atmosphere, there is a release of up to 0.32 mmol g−1 of O2. A reaction test of 10 cycles confirmed that for long-term operations, perovskites are viable. Based on observations, when the content of Al was increased, the reduction extent became enhanced. However, the oxidation degree is maximal for constitutions that are close to x = 0.5 and showed 0.318 mmol g−1 O2 delivery (δ = 0.132). After the selection of the constitutions having potentially better redox properties, further reactions were operated in a fixed bed reactor that is of lab scale. For CO formation, CO2 was injected in the oxidation step at 900°C. Perovskite La0.6Sr0.4Mn0.6Al0.4O3 showed interesting results where the reduction extent was 0.266 mmol g−1. However, CO generation is comparatively notably lower with the value being 0.114 mmol g−1.
Ramos, Maiti, Daza, Kuhn, Bhethanabotla (Ramos et al., 2019) assert that perovskite oxides in the category of type ABO3 have proven significant potential for thermochemical CO2 conversion at low temperature using the reverse water gas shift chemical looping (RWGS-CL) process. Transition metals on the ‘B’ site of these perovskite oxides are responsible for adjusting the material properties necessary for the effective conversion of CO2. The functions of Fe, Mn and Co in LaBO3 were explored using an integrated approach of both theory and experiment. Ab-initio density functional theory (DFT) simulations were used for investigating the intrinsic oxygen vacancy generation features and electronic charge distribution of these materials. Properties that are microscale including conversion yield of CO2 and crystallite size were explored by experiments. A comparative analysis is performed to differentiate the material properties influencing the stability and improved CO2 conversion process using perovskites that are plentiful in Fe, in contrast to Mn and Co-rich phases.
Parvanian, Salimijazi, Shabaninejad, Troitzsch, Kreider, Lipiński, Saadatfar (Parvanian et al., 2020) explored the redox functioning ability of porous ceramics having a coating of perovskite designing different forms of architecture. Fabrication of reticulated porous ceramics (RPCs) in three varying pore sizes was done for representing structures and pore sizes of a wide range. The pore sizes were 5, 12, and 75 ppi. The perovskite matter is composed of lanthanum manganite. After its synthesis, the perovskite material underwent Ca and Al doping via Pechini method. Implementing a method involving deep coating, the surface of RPC substrates underwent modifications and got a thin-film coating with ∼15 μm thickness. The CO2 conversion performance of the materials that were formed was evaluated in a gold-image IR furnace. For an in-depth investigation of features pertaining to bulk and surface, an X-ray micro-computed tomography along with SEM/EDX was employed during the investigation. According to findings, 12 ppi, which is the intermediate pore size, reaches the highest perovskite loading and shows a high level of coating uniformity and connectivity. The highest CO generation for 75 ppi was observed after CO2 conversion tests. Inside the furnace, the severe conditions, along with the flow of gaseous phases make the RPCs shrink to 23% of their original length. This alters the pore phase and eliminates minute pores thus decreasing the overall specific surface area. The findings also revealed a major mechanism that causes the CO2 conversion to stop where the coating layer of perovskite shifts its position into the matrix of the RPC frame.
Takalkar, Bhosale, AlMomani, Rashid, Qiblawey, Saleh Saad, Khraisheh, Kumar, Gupta, Shende (Takalkar et al., 2021) investigated La (1-x) SrxMnO3 (LSM) perovskites and their redox reactivity in the context of splitting CO2. Synthesis of LSM perovskites took place following the solution combustion synthesis (SCS) technique. This technique used glycine as a reducing agent. Many types of analytical approaches are used to characterize the structural properties of LSM perovskites. In three sets, thermogravimetric thermal reduction (TR) and CS cycles are conducted to acquire an estimation of the amount of O2 released (nO2) and CO yielded (nCO) by an individual lanthanum strontium manganite perovskite. The sets are in one, three and ten cycles. Higher nO2 by each LSM perovskite is released than the nCO that releases nO2 during the first cycle. The nO2 is lessened, and each LSM perovskite’s re-oxidation capacity is enhanced from cycle one to cycle three. Considering the average nO2 and nCOfrom cycle 2-cycle 10, the perovskites La0.30Sr0.70Mn0.99O2.982 (342.1 μmol of CO/g. cycle) and La0.60Sr0.41Mn0.99O2.993 (214.8 μmol of O2/g·cycle) have been found to reach the top highest redox reactivity. LSM perovskites, excluding La0.88Sr0.11Mn1.00O2.980, have a record of having a very high redox activity than the CeO2 material.
There are a large number of studies that are based on perovskite-based redox reactions as presented in Table 3 in the supplementary documents. It was concluded that although perovskite-based redox reactions can accommodate a wide range of oxygen, the high vacancy formation associated with re-oxidation stem imped the reaction and generated low ratio of CO/H2. There for a compromises between maximal achievable oxygen and fuel generation yield should be optimized, which can be controlled by perovskite formulation.
TABLE 3
| Material | Synthesis method | Experimental conditions | O2Production | H2/CO | Reference |
|---|---|---|---|---|---|
| La0.7Sr0.3Mn0.7Cr0.3O3 | Modified Pechini | Reduction: 1350°C under N2 Oxidation: H2O between 50 and 84%; 1000°C during 60 min | ∼98 | ∼107 | Gokon et al. (2019) |
| LaFe0.75Co0.25O3 | Solid-state | Reduction: 1300°C under Ar Oxidation: 50% CO2 in Ar at 1000°C | 59 | 117 | Nair Mahesh and Abanades, (2018) |
| LaCoO3 | Solid-state | Reduction: 1300°C under Ar Oxidation: 50% CO2 in Ar at 1000°C | 369 | 123 | |
| Ba0.5Sr0.5FeO3 | Solid-state | Reduction: 1000°C under Ar Oxidation: 50% CO2 in Ar at 1000°C | 582 | 136 | |
| La0.6Sr0.4Co0.2Cr0.8O3 | Pechini | Reduction: 1200°C under Ar Oxidation: 50% CO2 in Ar at 800°C | − | 157 | |
| La0.4Ca0.6Mn0.6Al0.4O3 | Modified Pechini | Reduction: 1400°C under Ar Oxidation: 40% H2O in Ar at 1000°C | 231 | 429 | Wang et al. (2017a) |
| BaCe0.25Mn0.75O3 | Modified Pechini | Reduction: 1350°C under Ar Oxidation: 40% H2O in Ar at 1000°C | − | 135 | |
| La0.5Sr0.5MnO3 | Solid-state | Reduction: 1400°C under Ar Oxidation: H2O at 1000°C | 298 | 195 | |
| La0.35Sr0.75MnO3 | Commercial powder | Reduction: 1400°C under Ar Oxidation: H2O at 1050°C | 166 | 124 | |
| La0.5Ca0.5MnO3 | Solid-state | Reduction: 1400°C under Ar Oxidation: 50% CO2 at 1050°C | 311 | 210 | |
| La0.5Ba0.5MnO3 | Solid-state | Reduction: 1400°C under Ar Oxidation: 50% CO2 at 1050°C | 203 | 185 | |
| La0.5Sr0.5Mn0.4Al0.6O3 | Pechini | Reduction: 1400°C under Ar Oxidation: 50% CO2 at 1050°C | 246 | 279 | |
| La0.5Sr0.5Mn0.83Mg0.17O3 | Solid-state | Reduction: 1400°C under Ar Oxidation: 50% CO2 at 1050°C | 214 | 209 | |
| La0.5Sr0.5MnO3 | Pechini | Reduction: 1400°C under Ar Oxidation: 50% CO2 at 1050°C | 256 | 256 | Nair and Abanades, (2016b) |
| Y0.5Sr0.5MnO3 | Pechini | Reduction: 1400°C under Ar Oxidation: 50% CO2 at 1050°C | 539 | 101 | |
| La0.6Sr0.4Mn0.6Al0.4O3 | Modified Pechini | Reduction: 1400°C under Ar Oxidation: 40% CO2 at 1000°C | − | 307 | McDaniel et al. (2013) |
| La0.6Ca0.4Mn0.6Al0.4O3 | Modified Pechini | Reduction: 1240°C under Ar Oxidation: 50% CO2 at 850°C | 165 | 230 | |
| La0.6Sr0.4Mn0.6Al0.4O3 | Modified Pechini | Reduction: 1240°C under Ar Oxidation: 50% CO2 at 850°C | 190 | 245 | |
| La0.6Ca0.4Mn0.8Ga0.2O3 | Modified Pechini | Reduction: 1300°C Oxidation: H2O at 900°C | 212 | 401 | Wang et al. (2017b) |
| La0.5Sr0.5Mn0.95Sc0.05O3 | − | Reduction: 1400°C under Ar Oxidation: 40% CO2 at 1100°C | 417 | 545 | |
| La0.6Sr0.4Mn0.8Fe0.2O3 | Modified Pechini | Reduction: 1350°C under N2 Oxidation: CO2 at 1000°C | 286 | 329 | Luciani et al. (2018) |
| La0.6Sr0.4CoO3 | Modified Pechini | Reduction: 1300°C Oxidation: 40% H2O at 900°C | 718 | 514 | Wang et al. (2018a) |
| La0.6Ca0.4CoO3 | Modified Pechini | Reduction: 1300°C Oxidation: 40% H2O at 900°C | 715 | 587 | Wang et al. (2018b) |
| Y0.5Ca0.5MnO3 | Solid state | Reduction: 1400°C Oxidation: CO2 at 1100°C | 573 | 671 |
Summary of the thermochemical cycles based on perovskites studies. Reprinted with permission from Bhosale et al. (2019)
Challenges for solar thermochemical processes
The challenges connected to various solar thermochemical processes can be summarized as follow:
1 The primary disadvantage of using perovskites is typically the insufficient re-oxidation yield brought on by low kinetics and low thermodynamic driving forces. Tuning the redox properties to maximize fuel production is possible thanks to the wide range of perovskite formulations that are possible and the discovery of novel materials.
2 It is crucial to continue making progress in the discovery and characterization of new, higher-performing redox materials that also meet the criteria for desirable thermodynamics, quick reaction kinetics, and crystallographic stability under thermochemical cycling.]
3 The cost projections for ThCy vary greatly and future cost projections are very difficult to make because they depend on a lot of arbitrary and incorrect assumptions. Therefore, well defined cost analysis is required
4 When producing fuel using a flammable redox material like zinc oxide, the dissociation reaction necessitates a very high temperature, which poses problems for the reactor’s materials. It has been noted that a sizable amount of zinc recombines with oxygen during the quench process to form zinc oxide, reducing the process’ overall effectiveness. To avoid zinc recombination with oxygen, rapid quenching with fine zinc particles is recommended.
5 Recombination is dealt with by non-volatile redox materials like ceria and iron. However, sintering, where the particle size increases after a few cycles of operation and lowers overall hydrogen yield, is a problem with ferrite-based cycles.
3 Conclusion
The conversion of CO2 into fuels and chemicals is a potential alternative strategy for addressing both energy and climate change issues simultaneously. There are several technologies available for converting CO2 into fuel, each of which faces its own set of obstacles when it comes to implementation in the field. A great deal has been accomplished in solar thermochemical technology, and it has emerged as a viable option for harnessing concentrated solar power. Because it makes direct use of solar energy, this technique is both highly beneficial and advantageous when compared to other energy utilisation methods. In industrial applications (i.e. electricity generation), CO2 and H2O reduction, concentrated solar energy is increasingly being used. However, even though the thermochemical splitting of CO2 and H2O through metal oxides is thermodynamically feasible, further research on achieving higher efficiency is still recommended.
Statements
Author contributions
ZR: Writing original draft; MM: Writing original draft; SA: Writing original draft; AC: Review and editing; FA: Review and editing.
Conflict of interest
The authors declare that the research was conducted in the absence of any commercial or financial relationships that could be construed as a potential conflict of interest.
Publisher’s note
All claims expressed in this article are solely those of the authors and do not necessarily represent those of their affiliated organizations, or those of the publisher, the editors and the reviewers. Any product that may be evaluated in this article, or claim that may be made by its manufacturer, is not guaranteed or endorsed by the publisher.
Abbreviations
CO2, Carbon Dioxide; CO, Carbon monoxide; H2, Hydrogen; ZnO, Zinc oxide; CeO2, Ceria Oxide; TPO, Temperature-Programmed Oxidation; MS, MassSpectroscopy; SCS, Solution Combustion Synthesis; TR, Thermal Reduction.
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Summary
Keywords
thermochemical splitting, ceria, perovskites, carbon dioxide emission, climate change
Citation
Rony ZI, Mofijur M, Ahmed SF, Kabir Z, Chowdhury AA and Almomani F (2022) Recent advances in the solar thermochemical splitting of carbon dioxide into synthetic fuels. Front. Energy Res. 10:982269. doi: 10.3389/fenrg.2022.982269
Received
30 June 2022
Accepted
06 September 2022
Published
03 October 2022
Volume
10 - 2022
Edited by
M.A. Mujtaba, University of Engineering and Technology, Pakistan
Reviewed by
Fahad Noor, University of Engineering and Technology, Pakistan
Manzoore Elahi Soudagar, Chandigarh University, India
Muhammad Amjad, University of Engineering and Technology, Pakistan
Updates
Copyright
© 2022 Rony, Mofijur, Ahmed, Kabir, Chowdhury and Almomani.
This is an open-access article distributed under the terms of the Creative Commons Attribution License (CC BY). The use, distribution or reproduction in other forums is permitted, provided the original author(s) and the copyright owner(s) are credited and that the original publication in this journal is cited, in accordance with accepted academic practice. No use, distribution or reproduction is permitted which does not comply with these terms.
*Correspondence: Fares Almomani, falmomani@qu.edu.qa
This article was submitted to Bioenergy and Biofuels, a section of the journal Frontiers in Energy Research
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