Recent advances in CO2 hydrogenation to value-added products — Current challenges and future directions

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Abstract

Climate change, global warming, fossil fuel depletion and rising fuel prices have created great incentives to seek alternative fuel production technologies. CO2 transformation to value-added products using renewable H2 has proven to be an emerging solution to enable this goal. In this regard, three different promising processes, namely methane, methanol and hydrocarbon synthesis via CO2 hydrogenation are thoroughly discussed. In addition, the influential factors affecting process efficiencies such as catalyst design and mechanistic insight, operating conditions as well as reactor types are investigated, with key pathways that dictate catalyst activity and selectivity of the most promising materials described. Furthermore, a brief overview of the reactor configuration and its crucial role in the improving process viability is analyzed. Accordingly, fixed-bed, fluidized-bed, annular and spherical reactors along with H2O/H2 perm-selective membrane reactors are disscussed for hydrocarbon production. In addition, different reactor configurations are compared to assess the best one that is adjustable depending on the reaction mechanism. Consequently, a corrugated-wall dual-type membrane reactor is proposed as an emerging alternative for CO2 hydrogenation to value-added products.

Introduction

The combustion of fossil fuels (coal, oil and natural gas) to generate energy results in huge amounts of greenhouse gas (GHG) emissions to the atmosphere, typically in CO2 form [1], [2], [3], [4]. In 2018, approximately 33 gigatonnes of CO2 emissions [5], resulted in a considerable increase in the atmospheric CO2 concentration from 280 ppm to 410 ppm. Production of sustainable and clean energy as a necessity for future consumption requires energy-efficient and advanced technologies [6], [7], [8]. In addition, increasing the use of renewable energy and valorization of different raw materials are necessary. In this regard, carbon capture and storage (CCS) as well as carbon capture and utilization (CCU) are hypothesized to play important roles [9], [10], [11], [12], [13], [14], [15]. These technologies offer significant benefits for reducing carbon emissions, with the latter promoting a circular economy, through encouraging industrial symbiosis from industry with large CO2 footprints, and providing renewable energy storage. This is consistent with the European policy with the goal of reducing 40 % of GHG emissions by 2030 compared to 1990 levels [16,17]. Indeed, CO2 storage and use to produce various chemicals play a significant role in achieving this objective.

CCS plays an important role in the reduction of GHG emissions along with climate change mitigation in the future. CCU is another attractive approach; but, compared to total CO2 production the market for the utilization of recovered CO2 is rather small (11%–17%) [18]. However, CCU results in the production of valuable fuels and chemicals in addition to the reduction of CO2 emissions compared to CCS [19]. CCUS is the integration of CCU and CCS that may be able to effectively exploit the benefits of the corresponding approaches, via increasing both economic and environmental incentives [20]. In this regard, CO2 is a key component to decrease fossil consumption via transforming to valuable chemicals while ensuring the energy efficiency of a process. Moreover, CO2 conversion to feedstocks for the chemical/petrochemical industry can be an efficient method for the renewable energy contribution in the chemical chain [21], [22], [23], [24], [25], [26], [27].

Many studies have been devoted to the utilization of CO2 as an available waste resource in terms of a cheap raw material [28], [29], [30], [31], [32]. CO2 can be supplied via the integration with various chemical plants. For instance, emissions of ammonia plants can be recovered for the simultaneous production of methanol and ammonia. The cement industry as well as iron and steel plants are other CO2 sources [33]. In addition, much attention should be paid to industrial and municipal wastes as potential CO2 sources [34,35]. Therefore, studying and disseminating knowledge about fuels and chemical production via capturing CO2 from other processes is of paramount significance. However, social acceptance is very low about this issue and some skepticism regarding long term ecological advantages exist [36]. Centi et al. [21] and Olah et al. [37] proposed three different pathways for CO2 utilization to produce various compounds comprising methanol and dimethyl ether (DME). As shown in Scheme 1, the main products of CO2 activation and transformation are methane, methanol, DME and hydrocarbons (olefins/ LPG/ gasoline/aromatic) [38]. Using excess renewable energy from wind and solar, the “Power-to-Fuel” strategy has attracted much attention and CO2 hydrogenation forms a core of this technology when coupled with CO2 capture and renewable H2 production from electrolysis. Accordingly, CO2 hydrogenation is extensively investigated in scientific literature for providing a direct pathway to produce various chemicals as fuels or feeds in other processes [39], [40], [41], [42], [43], [44], [45]. Catalytic hydrogenation is the most mature and promising technology in this regard [46]. Different catalysts catalyze CO2 hydrogenation to various products as depicted in Scheme 2 [47].

CO2 hydrogenation when the H2/CO2 ratio is equal to 4 [48,49], results in CH4 formation through the Sabatier reaction (R1) [21]. The Sabatier reaction is well known, but its application as an appropriate route for CO2 utilization is hindered due to the large H2 consumption, lower energy per unit volume and difficulties in storage compared with oxygenates (methanol, DME).CO2+4H2CH4+2H2OΔH298K=164.63kJ/mol

Methanol is one of the main raw materials in chemical/petrochemical industries owing to its extensive applications as solvent, energy source (e.g., as fuel, or in mixture with gasoline) and chemical feedstocks (e.g., for the production of methyl methacrylate, dimethyl carbonate, chloromethane, acetic acid, formaldehyde, methylamines, dimethyl terephthalate, and methyl tertiary butyl ether, etc.) [50], [51], [52]. In addition, methanol can be used for the production of ethylene and propylene via methanol-to-olefin (MTO) processes [53,54]. In recent years, methanol production from CO2 has gained much attention owing to the proposition of the so-called “Power-to-Fuel” concept [48,49], which is driven by availability of cost effective renewable energy. Direct methanol production through CO2 hydrogenation is represented in (R2) [55]:CO2+3H2CH3OH+H2OΔH298K=49.5kJ/mol

However, the traditional route for methanol production is the gas to methanol process, where CO is obtained from CO2 via the reverse water gas shift (RWGS) reaction and transformed to methanol as presented in (R3) and (R4) [56,57]:CO2+H2CO+H2OΔH298K=+41.2kJ/molCO+2H2CH3OHΔH298K=90.7kJ/mol

Many efforts to synthesize effective catalysts along with designing advanced reactors for CO2 hydrogenation have made it a competitive technology with industrial methanol synthesis from syngas. The required H2/CO2 ratio for methanol production should be 3 [58]. Considering energy and safety aspects, using H2 to produce methanol from CO2, i.e., for a direct methanol fuel cell, is more appropriate compared to reversible H2 storage as formic acid for use in PEM fuel cells. In addition, methanol-based fuel cells were found to comprise the greatest portion of the methanol market [21,59].

Methanol can also be converted to DME, a colorless environmentally friendly ether, which is not corrosive or toxic, and can be employed as a clean fuel and chemical building block for the production of valuable materials such as light olefins (ethylene and propylene) [60]. In addition, chlorofluorocarbon species in aerosols can be replaced by DME [61]. Moreover, DME can be used to produce alkyl aromatics as a hydrogen source in fuel cells. Besides, DME acts as an important intermediate for methyl acetate and dimethyl sulfate production [62]. DME can be produced via catalytic methanol dehydration (R5) based on either Langmuir-Hinshelwood [63] or Eley-Rideal [64] mechanisms, wherein both DME and water are reported to act as inhibitors during reaction [65].2CH3OHCH3OCH3+H2OΔH298K=23.4kJ/mol

Ethanol production from carbon dioxide has received less attention [66,67], despite the interest in recent decades in employing ethanol as both fuel [68] and feedstock for the production of numerous chemicals [69]. Ethanol can also increase the octane number of petrol and decrease CO and particulate matter emissions. Direct ethanol synthesis proceeds according to (R6) [48,49] and has low selectivity toward C2+ alcohols and low conversions even at high pressures.2C+12O2+3H2C2H5OHΔH298K=277.7kJ/mol

The reaction is believed to proceed through two steps comprising RWGS (R3) and CO hydrogenation (R7) [66]:2CO+4H2C2H5OH+H2OΔH298K=255.6kJ/mol

CO2 conversion to CO occurs at high temperatures (a CO2 conversion of about 48% can be obtained at 575 °C) owing to the endothermicity of the RWGS reaction. Another pathway for ethanol production is through DME transformation as reported by Atsonios et al. [48,49]. At first, carbon dioxide and hydrogen react to form methanol according to (R2–R4) and then methanol is dehydrated to DME via (R5). DME is then transformed into methyl acetate as an intermediate in (R8), which is then hydrogenated to ethanol as represented in (R9):CH3OCH3+COCH3COOCH3ΔH298K=114.16kJ/molCH3COOCH3+2H2CH3OH+C2H5OHΔH298K=30.3kJ/mol

CO2 can be hydrogenated to hydrocarbons through both direct and indirect pathways, e.g. by producing synthesis gas and/or methanol as an intermediate. [70], [71], [72], [73]. The indirect path can be accomplished in a single-stage reactor using hybrid catalysts or in multi-stage reactors to conduct multi-step transformations simultaneously (R3) along with (R10 to R11) [74].nCO+2nH2CnH2n+nH2OAlkeneproductionnCO+(2n+1)H2CnH2n+2+nH2OAlkaneproductionnCO2+3nH2(CH2)n+nH2ODirectCO2hydrogenation

The direct transformation (R12) occurs analogous to the Fischer-Tropsch (FT) reaction where CO2 and H2 are considered as feed. Generally, hydrocarbon production from CO2 requires more energy and H2 consumption and comprise more reaction steps with respect to the production of oxygenates and is not considered as a favorable method of fuel production [75]. Nevertheless, other reasons such as better infrastructure integration and growth in the market may justify this path. Thus, an integrated life-cycle and techno-economic analysis are essential to analyze different possibilities. In fact, direct hydrocarbon production using CO2 hydrogenation, which includes RWGS and FT reactions is one of the most significant applications of CCU (Scheme 1) [38].

In this context, hydrogen is required for the activation and transformation of CO2 to value-added fuels and chemicals. H2 has the ability to activate CO2, owing to exhibiting high energy density, which is a thermodynamically stable molecule [76,77]. Steam methane reforming, syngas, coke oven gas and chlorine alkali plants can be used as hydrogen sources in hydrogenation reactions [78]. Various hydrogen sources are presented in Scheme 3. However, future investigations should be devoted to finding alternative sources of H2 to guarantee process economics (approximately 65% of costs are ascribed to the electrolyzer) [79], [80], [81], [82]. In addition, hydrogen production technologies should have a zero carbon footprint to meet GHG mitigation targets.

Today, the most common method of H2 production is steam methane reforming, which results in CO formation along with hydrogen (R13). Further reaction of CO with H2O can lead to hydrogen generation according to (R14).CH4+H2O3H2+COΔH298K=+205.8kJ/molH2O+COH2+CO2ΔH298K=41.2kJ/mol

These emissions can be minimized via autothermal reforming where oxygen is used along with H2O (R15) in the reactor at high temperatures (> 727 °C). However, further optimization concerning the H2/CO ratio, catalyst activity and its deactivation are required to achieve eco-friendly process standards.CxHyOz+O2+H2OH2+CO+CO2+CnHm+tar

Another route for hydrogen generation is the utilization of biomass in gasification, pyrolysis and liquefaction processes [84], [85], [86]. Biomass gasification is more beneficial with respect to conventional coal gasification since biomass is naturally renewable. Combining biomass and coal gasification can minimize CO2 production and subsequently reduces negative environmental consequences [87]. Ethanol, glycerol, bio-liquids and bio-oils can be used as biomass sources. However, problems regarding feed quality, seasonal availability and regional dependencies should be solved as well as economic issues. Consequently, improved technologies with reduced catalyst deactivation as well as fewer carbon emissions require development.

One of the promising H2 generation methods, to produce high purity hydrogen without further separation costs, is water electrolysis (R16). Industrial electrolysis plants can produce hydrogen with about 50-70 % efficiency. However, the main issue of this process is to achieve electricity production with low cost and low carbon emission. Therefore, fossil fuels should be substituted by renewable energies such as solar or wind in electricity generation plants to mitigate the CO2 formation [88], [89], [90]. The mentioned energies are climate dependent, which should be considered in designing sustainable operation.2H2O2H2+O2ΔHSTP=+237kJ/mol

Solar energy can also be used for H2O splitting to H2 and O2 in the presence of catalysts exhibiting special electronic structures (photo-semiconductor) or some microorganisms [91]. However, this process is still far from commercial implementation due to low efficiency, low durability and high oxidation-resistant catalysts. As a whole, due to no CO2 byproduct, water electrolysis seems to be the most appropriate source of H2 production if CO2-free sources can be used for the required electricity generation [92].

A recent review by Jiang et al. [93] addresses CO2 hydrogenation to methanol in terms of catalyst design, mechanistic and kinetic studies as well as reactor design and optimization. In addition, Zhong et al. [94] studied the thermodynamic challenges and catalyst development of this process along with industrial reactor development, while Nie et al. [95] focused on recent advances in catalytic materials and mechanistic insight for the production of alcohols and hydrocarbons. However, the significance of choosing the appropriate reactor configuration along with mechanistic considerations have not been addressed for the mentioned processes.

Accordingly, kinetic modeling of CO2 hydrogenation to hydrocarbons was investigated [96] and the kinetic parameters of the simultaneous RWGS and FT reactions were evaluated through an artificial bee colony (ABC) algorithm considering mass and heat transport in a fixed-bed catalytic reactor [97]. This study systematically investigates three different processes, namely methane, methanol and hydrocarbon synthesis via hydrogenation of CO2. The effects of catalyst and mechanism, operating conditions as well as reactor type on CO2 hydrogenation are investigated. Additionally, a comprehensive outline about reactor configurations as the most significant parameter on process enhancement is provided. Moreover, by taking account of the current literature, the differenct configurations of the reactor based on the reaction mechanisms are discussed. Lastly, a corrugated-wall dual-type membrane reactor is proposed as a promising alternative for CO2 hydrogenation to value-added products.

Section snippets

Methanation

CO2 hydrogenation to methane (Sabatier reaction) is an exothermic reaction, which has been developed in 1902 [98], [99], [100]. This reaction is significant for closed loop CO2 cycling where CO2 from contained spaces are recycled to fuel for combustion. Literature reported effects of catalyst development and mechanistic studies, operating conditions and reactor configuration are presented in the following sections.

Methanol synthesis

Methanol is an alternative fuel, a common solvent, and a starting material in the chemical industry. Indeed, CO can be replaced with CO2 as a potent route for utilization of CO2 in methanol production [243], [244], [245], [246], [247], [248], [249], [250] as represented in (R2).

From a thermodynamic aspect, temperature reduction or pressure elevation could favor methanol synthesis. There is evidence that improved reaction temperature (higher than 240 °C) facilitates CO2 activation and synthesis

Hydrocarbons synthesis

The transformation of CO2 to light alkanes and alkenes comprises two indirect pathways: modified Fischer-Tropsch (MFT) process, and methanol-mediated route. In the MFT process, CO2 hydrogenation results in CO formation (RWGS) and further hydrogenation of CO (FT) leads in the formation of hydrocarbons [457]. However, in the second route, methanol is the product of CO2 hydrogenation, which is converted to hydrocarbons via further hydrogenation. Obviously, different active sites are required in

Discussion and perspectives

As described in this review, the hydrogenation of CO2 was a powerful and feasible process for CO2 utilization. However, CO2 is chemically stable and thermodynamically unfavorable, which indicates some limitations on its conversion and utilization. Almost all previous studies aiming to inspect factors affecting the fuel and chemical production efficiency through CO2 hydrogenation that were performed experimentally. High reaction heat, multi reaction systems and sensitive catalysts make CO2

Conclusions

As the main greenhouse gas, CO2 increase in the atmosphere is mostly considered to be responsible for climate change and global warming, CO2 transformation to fuels and chemicals would be helpful to circulate carbon in order to diminish the greenhouse effect. Methane, methanol and HCs can be exploited as fuel substitutes, emerging energy storage media and raw materials of petrochemical products. Thus, CO2 hydrogenation can efficiently decrease the CO2 accumulation and diminish the greenhouse

Declaration of Competing Interest

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Acknowledgements

This research has been supported by the NRDI Fund (TKP2020 NC, Grtant No. BME-NCS) based on the charter of bloster issued by the NRDI office under the auspices of the Ministry for Innovation and Technology. SLS acknowledges the support of the US Department of Energy, Office of Basic Energy Sciences, Division of Chemical, Biological and Geological Sciences under grant DE-FG02-86ER13622.A000.

Dr. Samrand Saeidi, is a visiting researcher at the Institute of Energy and Process Systems Engineering, TU-Braunschweig. He holds Master's and PhD awards in Applied Chemistry, Material Science, Chemical Engineering and Mechanical Engineering. Combining these backgrounds, he successfully commercialized novel ideas on smart adsorbents applied in wood and paper industry. He has authored 27 refereed journal publications (H-index 14, 1100 cites), and worked extensively with industry. His research

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