Recent Advances in Catalytic CO2 Conversion for Value-Added Chemical Production

A special issue of Catalysts (ISSN 2073-4344). This special issue belongs to the section "Environmental Catalysis".

Deadline for manuscript submissions: closed (10 March 2022) | Viewed by 27225

Special Issue Editors

Korea Institute of Science and Technology, Korea University, Seoul, Korea
Interests: CO2 hydrogenation; electrochemical CO2 reduction; Process systems engineering; optimization; Machine learning; Bayesian optimization

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Guest Editor
Korea Institute of Science and Technology (KIST), Seoul, Korea
Interests: electrocatalysts; water splitting; CO2 reduction; in-situ/operando analysis (XAFS, NEXAFS, Raman, ICP-MS)

Special Issue Information

Dear Colleagues,

The atmospheric CO2 concentration reached 410 ppm in 2018 as identified by the Mauna Loa observatory, and its increasing rate has been accelerated up to an annual increase of 2.87 ppm year-1 which is ca. 100 times faster than the level at the end of the last ice age. A lot of issues about climate change including global warming, ocean acidification, and ecosystem destruction, caused by greenhouse gas emissions have led to the Paris Agreement in which many countries submitted their targets for mitigating carbon emission. A recent projection on climate change suggests that warming can be kept below 1.5 °C (compared to the pre-industrial level) with a probability of more than 50% even if existing CO2-emitting infrastructures will be used until their lifetime, while delaying necessary actions significantly reduces the probability.

Catalytic CO2 conversion is a promising option for mitigating greenhouse gases while maintaining the economic feasibility of chemical production processes. Catalytic CO2 conversion may include 1) thermochemical catalytic CO2 conversion, 2) electrochemical CO2 reduction, and 3) biological CO2 capture and conversion. Amongst them, several research topics such as CO2 hydrogenation and electrochemical CO2 reduction processes are highlighted for the practical application of value-added chemical production as large-scale demonstration projects have successfully demonstrated the economic feasibility of CO2 utilization. This Special Issue on catalytic CO2 conversion will present an overview of currently applied techniques for CO2 conversion, focusing on their advantages, and disadvantages and on the main challenges facing their large-scale application.

Guest Editor

Prof. Dr. Hyung-Suk, Oh

Prof. Dr. Ung Lee

Keywords

  • Carbon dioxide
  • Heterogeneous catalysis
  • Photocatalysis
  • Electrocatalysis
  • Biocatalysis
  • Techno-economic analysis
  • Life cycle assessment

Published Papers (6 papers)

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Research

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21 pages, 2293 KiB  
Article
Implementation of Formic Acid as a Liquid Organic Hydrogen Carrier (LOHC): Techno-Economic Analysis and Life Cycle Assessment of Formic Acid Produced via CO2 Utilization
by Changsoo Kim, Younggeun Lee, Kyeongsu Kim and Ung Lee
Catalysts 2022, 12(10), 1113; https://doi.org/10.3390/catal12101113 - 26 Sep 2022
Cited by 20 | Viewed by 4010
Abstract
To meet the global climate goals agreed upon regarding the Paris Agreement, governments and institutions around the world are investigating various technologies to reduce carbon emissions and achieve a net-negative energy system. To this end, integrated solutions that incorporate carbon utilization processes, as [...] Read more.
To meet the global climate goals agreed upon regarding the Paris Agreement, governments and institutions around the world are investigating various technologies to reduce carbon emissions and achieve a net-negative energy system. To this end, integrated solutions that incorporate carbon utilization processes, as well as promote the transition of the fossil fuel-based energy system to carbon-free systems, such as the hydrogen economy, are required. One of the possible pathways is to utilize CO2 as the base chemical for producing a liquid organic hydrogen carrier (LOHC), using CO2 as a mediating chemical for delivering H2 to the site of usage since gaseous and liquid H2 retain transportation and storage problems. Formic acid is a probable candidate considering its high volumetric H2 capacity and low toxicity. While previous studies have shown that formic acid is less competitive as an LOHC candidate compared to other chemicals, such as methanol or toluene, the results were based on out-of-date process schemes. Recently, advances have been made in the formic acid production and dehydrogenation processes, and an analysis regarding the recent process configurations could deem formic acid as a feasible option for LOHC. In this study, the potential for using formic acid as an LOHC is evaluated, with respect to the state-of-the-art formic acid production schemes, including the use of heterogeneous catalysts during thermocatalytic and electrochemical formic acid production from CO2. Assuming a hydrogen distribution system using formic acid as the LOHC, each of the production, transportation, dehydrogenation, and CO2 recycle sections are separately modeled and evaluated by means of techno-economic analysis (TEA) and life cycle assessment (LCA). Realistic scenarios for hydrogen distribution are established considering the different transportation and CO2 recovery options; then, the separate scenarios are compared to the results of a liquefied hydrogen distribution scenario. TEA results showed that, while the LOHC system incorporating the thermocatalytic CO2 hydrogenation to formic acid is more expensive than liquefied H2 distribution, the electrochemical CO2 reduction to formic acid system reduces the H2 distribution cost by 12%. Breakdown of the cost compositions revealed that reduction of steam usage for thermocatalytic processes in the future can make the LOHC system based on thermocatalytic CO2 hydrogenation to formic acid to be competitive with liquefied H2 distribution if the production cost could be reduced by 23% and 32%, according to the dehydrogenation mode selected. Using formic acid as a LOHC was shown to be less competitive compared to liquefied H2 delivery in terms of LCA, but producing formic acid via electrochemical CO2 reduction was shown to retain the lowest global warming potential among the considered options. Full article
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15 pages, 7207 KiB  
Article
Development of Pilot-Scale CO2 Methanation Using Pellet-Type Catalysts for CO2 Recycling in Sewage Treatment Plants and Its Validation through Computational Fluid Dynamics (CFD) Modeling
by Jeongyoon Ahn, Heysuk Kim, Yeonhee Ro, Jintae Kim, Woojin Chung and Soonwoong Chang
Catalysts 2021, 11(8), 1005; https://doi.org/10.3390/catal11081005 - 20 Aug 2021
Cited by 6 | Viewed by 3146
Abstract
In this study, a pilot-scale reactor was designed and compared using computational fluid dynamics (CFD) for a high-efficiency CO2 methanation reaction. The trends of the CO2 methanation catalyst efficiency at a pilot or industrial scale could be lower than those measured [...] Read more.
In this study, a pilot-scale reactor was designed and compared using computational fluid dynamics (CFD) for a high-efficiency CO2 methanation reaction. The trends of the CO2 methanation catalyst efficiency at a pilot or industrial scale could be lower than those measured at the laboratory scale, owing to the flow of fluid characteristics. Therefore, the CO2 methanation reactor was designed based on the results of the CFD analysis to minimize the above phenomenon. Ni–Ce–Zr was used to manufacture a CO2 methanation catalyst in the form of pellets. The catalyst successfully produced about 43.3 Nm3/d of methane from the reactor. This result shows that CO2 methanation, which is known as an exothermic reaction, was stable at the pilot scale. It is believed that the self-supply of energy will be possible when this CO2 methanation technology is applied to industrial processes generating large amounts of CO2 and H2 from by-product gases. Full article
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14 pages, 1881 KiB  
Article
Techno-Economic and Environmental Analysis for Direct Catalytic Conversion of CO2 to Methanol and Liquid/High-Calorie-SNG Fuels
by Tesfalem Aregawi Atsbha, Taeksang Yoon, Byung-Hoon Yoo and Chul-Jin Lee
Catalysts 2021, 11(6), 687; https://doi.org/10.3390/catal11060687 - 29 May 2021
Cited by 12 | Viewed by 4470
Abstract
Catalytic hydrogenation of CO2 has great potential to significantly reduce CO2 and contribute to green economy by converting CO2 into a variety of useful products. The goal of this study is to assess and compare the techno-economic and environmental measures [...] Read more.
Catalytic hydrogenation of CO2 has great potential to significantly reduce CO2 and contribute to green economy by converting CO2 into a variety of useful products. The goal of this study is to assess and compare the techno-economic and environmental measures of CO2 catalytic conversion to methanol and Fischer–Tropsch-based fuels. More specifically, two separate process models were developed using a process modeler: direct catalytic conversion of CO2 to Fischer–Tropsch-based liquid fuel/high-calorie SNG and direct catalytic conversion of CO2 to methanol. The unit production cost for each process was analyzed and compared to conventional liquid fuel and methanol production processes. CO2 emissions for each process were assessed in terms of global warming potential. The cost and environmental analyses results of each process were used to compare and contrast both routes in terms of economic feasibility and environmental friendliness. The results of both the processes indicated that the total CO2 emissions were significantly reduced compared with their respective conventional processes. Full article
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12 pages, 1872 KiB  
Article
Catalytic Hydrogenation of Carbon Dioxide over Magnetic Nanoparticles: Modification in Fixed-Bed Reactor
by Mehnaz Bibi, Rasheed Ullah, Muhammad Sadiq, Saima Sadiq, Idrees Khan, Khalid Saeed, Muhammad Abid Zia, Zaffar Iqbal, Inam Ullah, Zahoor Iqbal and Shahbaz Ahmad
Catalysts 2021, 11(5), 592; https://doi.org/10.3390/catal11050592 - 3 May 2021
Cited by 13 | Viewed by 3283
Abstract
A specific finger-projected fixed-bed reactor (FPFBR) was designed to efficiently utilize magnetic nanoparticles (MnFe2O4/Bi-MnFe2O4) for a model reaction (hydrogenation of a greenhouse gas, CO2, to valuable products: VPs). Coprecipitation method, with desired modification [...] Read more.
A specific finger-projected fixed-bed reactor (FPFBR) was designed to efficiently utilize magnetic nanoparticles (MnFe2O4/Bi-MnFe2O4) for a model reaction (hydrogenation of a greenhouse gas, CO2, to valuable products: VPs). Coprecipitation method, with desired modification was used for the preparation of magnetic nanoparticles (MNPs) with controlled shape and size. Eighteen fingers in a single chamber were designed in the fixed-bed reactor’s skeleton; each finger worked as an independent reaction core. Controlled flow of hydrogen and CO2 was continuously provided to preheated reaction cores (catalyst beds) from saturator. One of the major products methanol {(%: Conv, 22/Sel 61)} among VPs was identified and quantified by GC. The efficiency of self-designed reactor was 74% for the direct catalytic hydrogenation of CO2 to valuable organic products. Full article
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13 pages, 3598 KiB  
Article
Effects of Alkali Metals on Nickel/Alumina Catalyzed Ethanol Dry Reforming
by Se-Won Park, Dongseok Lee, Seung-Ik Kim, Young Jin Kim, Ji Hoon Park, Iljeong Heo, Tae Sun Chang and Jin Hee Lee
Catalysts 2021, 11(2), 260; https://doi.org/10.3390/catal11020260 - 15 Feb 2021
Cited by 7 | Viewed by 2915
Abstract
Although ethanol dry reforming is an attractive carbon utilization technology, problems of severe coke formation and low catalytic activity should be solved for realization of the technology. We demonstrate the effects of alkali metal additives (lithium, sodium, and potassium) on nickel catalyzed ethanol [...] Read more.
Although ethanol dry reforming is an attractive carbon utilization technology, problems of severe coke formation and low catalytic activity should be solved for realization of the technology. We demonstrate the effects of alkali metal additives (lithium, sodium, and potassium) on nickel catalyzed ethanol dry reforming. Potassium doped nickel catalyst (Ni/K2O-Al2O3) showed enhanced catalytic activity and durability in ethanol dry reforming. Thermogravimetric analysis (TGA) showed that Ni/K2O-Al2O3 had a high resistance to coke formation. The amounts of coke formed on Ni/K2O-Al2O3 were 1/3 lower than the amounts of coke formed on Ni/Al2O3. The total coke quantities were closely correlated to the number of basic sites of the nickel catalysts. Raman spectroscopy and transmission electron microscopy analyses revealed that the alkali metals control the coke formation on the catalysts. Full article
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Review

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30 pages, 5825 KiB  
Review
Towards the Large-Scale Electrochemical Reduction of Carbon Dioxide
by Subin Park, Devina Thasia Wijaya, Jonggeol Na and Chan Woo Lee
Catalysts 2021, 11(2), 253; https://doi.org/10.3390/catal11020253 - 13 Feb 2021
Cited by 45 | Viewed by 8272
Abstract
The severe increase in the CO2 concentration is a causative factor of global warming, which accelerates the destruction of ecosystems. The massive utilization of CO2 for value-added chemical production is a key to commercialization to guarantee both economic feasibility and negative [...] Read more.
The severe increase in the CO2 concentration is a causative factor of global warming, which accelerates the destruction of ecosystems. The massive utilization of CO2 for value-added chemical production is a key to commercialization to guarantee both economic feasibility and negative carbon emission. Although the electrochemical reduction of CO2 is one of the most promising technologies, there are remaining challenges for large-scale production. Herein, an overview of these limitations is provided in terms of devices, processes, and catalysts. Further, the economic feasibility of the technology is described in terms of individual processes such as reactions and separation. Additionally, for the practical implementation of the electrochemical CO2 conversion technology, stable electrocatalytic performances need to be addressed in terms of current density, Faradaic efficiency, and overpotential. Hence, the present review also covers the known degradation behaviors and mechanisms of electrocatalysts and electrodes during electrolysis. Furthermore, strategic approaches for overcoming the stability issues are introduced based on recent reports from various research areas involved in the electrocatalytic conversion. Full article
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