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Catalysts
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Chemical Looping for Catalysis
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Chemical Looping for Catalysis

A special issue of Catalysts (ISSN 2073-4344).

Deadline for manuscript submissions: closed (15 October 2021) | Viewed by 44038

Special Issue Editor

Prof. Dr. Vladimir Galvita

E-Mail Website
Guest Editor
Laboratory for Chemical Technology, Universiteit Gent, Ghent, Belgium
Interests: catalysis; chemical kinetics; chemical looping
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Chemical looping is one of several emerging technologies capable of low emission with applications in the production of heat, fuels, chemicals, and electricity. The flexibility of chemical looping results from the fact that a single reaction is separated into two sub-reactions, coupled through the oxygen carrier material, thus opening up a wide parameter space for design and optimization of reactor feed and process operation. It is noteworthy that over the full cycle, the “oxygen carrier” undergoes the same cyclic reduction–oxidation as a catalyst as in the well-established Mars–van Krevelen mechanism and fulfils the same function as a catalyst, i.e., it facilitates the reaction without being formed or consumed. This principle should be fundamentally applicable to any catalytic reaction if suitable carriers or conditions are found that allow transport of the desired functional group. The product separation that is inherent to this technology can have a significant impact in the future on a broad range of chemical processes, leading to higher efficiency and ‘greener’ chemistry.

The aim of this Special Issue is to cover promising recent research and novel trends in the field of chemical looping applications for performing catalytic reactions (selective oxidation, reforming, dehydrogenation, etc.). Reactions could run in liquid or gas phase, employing a range of different catalysts and materials with various oxidants. A key component for the development of novel chemical looping processes is the design of suitable materials. Chemical looping involves many aspects of materials science, including synthesis, reactivity, and mechanical properties, flow stability and contact mechanics, as well as gas–solid reaction engineering. Studies offering material design would also be of great interest.

Prof. Dr. Vladimir Galvita
Guest Editor

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Keywords

  • product separation
  • hybrid looping
  • carrier material
  • selective oxidation
  • energy storage
  • carbon capture and utilization
  • CO2 transformation
  • sorption-enhanced
  • equilibrium shift

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Published Papers (6 papers)

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Research

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18 pages, 38887 KiB  
Article
Development of V-Based Oxygen Carriers for Chemical Looping Oxidative Dehydrogenation of Propane
by Tianwei Wu, Qingbo Yu, Kun Wang and Martin van Sint Annaland
Catalysts 2021, 11(1), 119; https://doi.org/10.3390/catal11010119 - 15 Jan 2021
Cited by 10 | Viewed by 2762
Abstract
Two different preparation methods, viz. incipient impregnation and mechanical mixing, have been used to prepare V-based oxygen carriers with different V loadings for chemical looping oxidative dehydrogenation of propane. The effect of the preparation method, V loading, and reaction temperature on the performance [...] Read more.
Two different preparation methods, viz. incipient impregnation and mechanical mixing, have been used to prepare V-based oxygen carriers with different V loadings for chemical looping oxidative dehydrogenation of propane. The effect of the preparation method, V loading, and reaction temperature on the performance of these oxygen carriers have been measured and discussed. It was found that the VOx species can be well distributed on the support when the V loading is low (5 wt.% and 10 wt.%), but they may become aggregated at higher loadings. For oxygen carriers with a higher V loading, the oxygen transport capacity of the oxygen carrier, propane conversion and COx selectivities increase, while the propylene selectivity decreases. With a V-loading of 10 wt.%, the maximum propylene yield was achieved. The VOx species were better distributed over the support when applying the impregnation method; however, at higher V loadings the V-based oxygen carriers prepared by mechanical mixing showed a larger oxygen transport capacity. The oxygen carriers prepared by impregnation showed a better performance for the oxidative dehydrogenation of propane (ODHP) and re-oxidation reactions compared to oxygen carriers prepared by mechanical mixing. Higher reaction temperatures are favorable for the re-oxidation reaction, but unfavorable for the propylene production. Full article
(This article belongs to the Special Issue Chemical Looping for Catalysis)
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16 pages, 5798 KiB  
Article
Solar-Driven Chemical Looping Methane Reforming Using ZnO Oxygen Carrier for Syngas and Zn Production in a Cavity-Type Solar Reactor
by Srirat Chuayboon and Stéphane Abanades
Catalysts 2020, 10(11), 1356; https://doi.org/10.3390/catal10111356 - 21 Nov 2020
Cited by 7 | Viewed by 2618
Abstract
Converting sunlight into chemical fuels and metal commodities, via solar thermochemical conversion processes, is an attractive prospect for the long-term storage of renewable energy. In this study, the combined methane reforming and ZnO reduction in a single reaction for co-production of hydrogen-rich syngas [...] Read more.
Converting sunlight into chemical fuels and metal commodities, via solar thermochemical conversion processes, is an attractive prospect for the long-term storage of renewable energy. In this study, the combined methane reforming and ZnO reduction in a single reaction for co-production of hydrogen-rich syngas and metallic Zn was demonstrated in a flexible solar thermochemical reactor prototype, driven by highly concentrated sunlight. Using solar energy as the process heat source in chemical-looping methane reforming with the ZnO/Zn oxygen carrier is a means to reduce the dependence on conventional energy resources and to reduce emissions of CO2 and other pollutants, while upgrading the calorific value of the feedstock for the production of energy-intensive and high-value chemical fuels and materials. On-sun experiments were carried out with different operating parameters including operating temperatures (800–1000 °C), inlet methane flow-rates (0.1–0.4 NL/min), and inlet ZnO feeding-rates (0.5–1.0 g/min) both in batch and continuous modes under reduced (0.15 and 0.45 bar) and atmospheric pressures (0.90 bar), thereby demonstrating solar reactor flexibility and reliability. As a result, increasing the temperature promoted net ZnO conversion at the expense of favored methane cracking reaction, which can be lowered by decreasing pressure to vacuum conditions. Diminishing total pressure improved the net ZnO conversion but favored CO2 yield due to insufficient gas residence time. Rising ZnO feeding rate under a constant over-stoichiometric CH4/ZnO molar ratio of 1.5 enhanced ZnO and methane consumption rates, which promoted Zn and syngas yields. However, an excessively high ZnO feeding rate may be detrimental, as ZnO could accumulate when the ZnO feeding rate is higher than the ZnO consumption rate. In comparison, continuous operation demonstrated greater performance regarding higher ZnO conversion (XZnO) and lower methane cracking than batch operation. High-purity metallic Zn with a well-crystallized structure and of micrometric size was produced from both batch and continuous tests under vacuum and atmospheric pressures, demonstrating suitable reactor performance for the solar thermochemical methane-driven ZnO reduction process. The produced Zn metal can be further re-oxidized with H2O or CO2 in an exothermic reaction to produce pure H2 or CO by chemical-looping. Full article
(This article belongs to the Special Issue Chemical Looping for Catalysis)
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Review

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15 pages, 1204 KiB  
Review
Catalytic Dehydrogenation of Ethane: A Mini Review of Recent Advances and Perspective of Chemical Looping Technology
by Danis Fairuzov, Ilias Gerzeliev, Anton Maximov and Evgeny Naranov
Catalysts 2021, 11(7), 833; https://doi.org/10.3390/catal11070833 - 9 Jul 2021
Cited by 38 | Viewed by 10334
Abstract
Dehydrogenation processes play an important role in the petrochemical industry. High selectivity towards olefins is usually hindered by numerous side reactions in a conventional cracking/pyrolysis technology. Herein, we show recent studies devoted to selective ethylene production via oxidative and non-oxidative reactions. This review [...] Read more.
Dehydrogenation processes play an important role in the petrochemical industry. High selectivity towards olefins is usually hindered by numerous side reactions in a conventional cracking/pyrolysis technology. Herein, we show recent studies devoted to selective ethylene production via oxidative and non-oxidative reactions. This review summarizes the progress that has been achieved with ethane conversion in terms of the process effectivity. Briefly, steam cracking, catalytic dehydrogenation, oxidative dehydrogenation (with CO2/O2), membrane technology, and chemical looping are reviewed. Full article
(This article belongs to the Special Issue Chemical Looping for Catalysis)
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21 pages, 5995 KiB  
Review
Intensification of Chemical Looping Processes by Catalyst Assistance and Combination
by Hilde Poelman and Vladimir V. Galvita
Catalysts 2021, 11(2), 266; https://doi.org/10.3390/catal11020266 - 17 Feb 2021
Cited by 10 | Viewed by 3930
Abstract
Chemical looping can be considered a technology platform, which refers to one common basic concept that can be used for various applications. Compared with a traditional catalytic process, the chemical looping concept allows fuels’ conversion and products’ separation without extra processes. In addition, [...] Read more.
Chemical looping can be considered a technology platform, which refers to one common basic concept that can be used for various applications. Compared with a traditional catalytic process, the chemical looping concept allows fuels’ conversion and products’ separation without extra processes. In addition, the chemical looping technology has another major advantage: combinability, which enables the integration of different reactions into one process, leading to intensification. This review collects various important state-of-the-art examples, such as integration of chemical looping and catalytic processes. Hereby, we demonstrate that chemical looping can in principle be implemented for any catalytic reaction or at least assist in existing processes, provided that the targeted functional group is transferrable by means of suitable carriers. Full article
(This article belongs to the Special Issue Chemical Looping for Catalysis)
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64 pages, 9135 KiB  
Review
Development of Stable Oxygen Carrier Materials for Chemical Looping Processes—A Review
by Yoran De Vos, Marijke Jacobs, Pascal Van Der Voort, Isabel Van Driessche, Frans Snijkers and An Verberckmoes
Catalysts 2020, 10(8), 926; https://doi.org/10.3390/catal10080926 - 12 Aug 2020
Cited by 79 | Viewed by 9654
Abstract
This review aims to give more understanding of the selection and development of oxygen carrier materials for chemical looping. Chemical looping, a rising star in chemical technologies, is capable of low CO2 emissions with applications in the production of energy and chemicals. [...] Read more.
This review aims to give more understanding of the selection and development of oxygen carrier materials for chemical looping. Chemical looping, a rising star in chemical technologies, is capable of low CO2 emissions with applications in the production of energy and chemicals. A key issue in the further development of chemical looping processes and its introduction to the industry is the selection and further development of an appropriate oxygen carrier (OC) material. This solid oxygen carrier material supplies the stoichiometric oxygen needed for the various chemical processes. Its reactivity, cost, toxicity, thermal stability, attrition resistance, and chemical stability are critical selection criteria for developing suitable oxygen carrier materials. To develop oxygen carriers with optimal properties and long-term stability, one must consider the employed reactor configuration and the aim of the chemical looping process, as well as the thermodynamic properties of the active phases, their interaction with the used support material, long-term stability, internal ionic migration, and the advantages and limits of the employed synthesis methods. This review, therefore, aims to give more understanding into all aforementioned aspects to facilitate further research and development of chemical looping technology. Full article
(This article belongs to the Special Issue Chemical Looping for Catalysis)
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26 pages, 6837 KiB  
Review
Approaches for Selective Oxidation of Methane to Methanol
by Richa Sharma, Hilde Poelman, Guy B. Marin and Vladimir V. Galvita
Catalysts 2020, 10(2), 194; https://doi.org/10.3390/catal10020194 - 6 Feb 2020
Cited by 39 | Viewed by 13185
Abstract
Methane activation chemistry, despite being widely reported in literature, remains to date a subject of debate. The challenges in this reaction are not limited to methane activation but extend to stabilization of the intermediate species. The low C-H dissociation energy of intermediates vs. [...] Read more.
Methane activation chemistry, despite being widely reported in literature, remains to date a subject of debate. The challenges in this reaction are not limited to methane activation but extend to stabilization of the intermediate species. The low C-H dissociation energy of intermediates vs. reactants leads to CO2 formation. For selective oxidation, nature presents methane monooxygenase as a benchmark. This enzyme selectively consumes methane by breaking it down into methanol. To assemble an active site similar to monooxygenase, the literature reports Cu-ZSM-5, Fe-ZSM-5, and Cu-MOR, using zeolites and systems like CeO2/Cu2O/Cu. However, the trade-off between methane activation and methanol selectivity remains a challenge. Density functional theory (DFT) calculations and spectroscopic studies indicate catalyst reducibility, oxygen mobility, and water as co-feed as primary factors that can assist in enabling higher selectivity. The use of chemical looping can further improve selectivity. However, in all systems, improvements in productivity per cycle are required in order to meet the economical/industrial standards. Full article
(This article belongs to the Special Issue Chemical Looping for Catalysis)
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