Catalysis on Stable Molecules (CO2, CO, CH4, N2, NH3) Activation and Their Transformation, 2nd Edition

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

Deadline for manuscript submissions: closed (29 February 2024) | Viewed by 5824

Special Issue Editor


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Guest Editor
1. Department of Chemical Engineering, Ajou University, Suwon 16499, Republic of Korea
2. Department of Energy Systems Research, Ajou University, Suwon 16499, Republic of Korea
Interests: C1 chemistry; methane activation; biomass conversion; CO oxidation; methanation
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Special Issue Information

Dear Colleagues,

This issue is a continuation of the previous successful Special Issue “Catalysis on Stable Molecules (CO2, CO, CH4, N2, NH3) Activation and Their Transformation”.

C1 gases, including CO, CO2, and CH4, can be a starting material for the synthesis of value-added chemicals via several catalytic pathways. In addition to C1 gas, N2 and NH3 are also important building blocks for cc chemicals. In this Special Issue of Catalysts, recent research works on the activation and catalytic conversion of these stable molecules will be disclosed. The scope of this Special Issue of Catalysts encompasses all aspects of catalyst research on these stable molecules, from theoretical calculation to catalyst screening, for homogeneous and/or heterogeneous catalysts.

Prof. Dr. Eun Duck Park
Guest Editor

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Keywords

  • CO2 activation
  • CO2 conversion
  • CO2 hydrogenation
  • dry reforming of methane, methane activation
  • methane conversion
  • amination
  • ammonia decomposition
  • N2 activation
  • ammonia synthesis
  • carbonylation
  • hydroformylation
  • CO hydrogenation

Published Papers (5 papers)

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Research

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13 pages, 4423 KiB  
Article
Investigating the Catalytic Deactivation of a Pd Catalyst during the Continuous Hydrogenation of CO2 into Formate Using a Trickle-Bed Reactor
by Kwangho Park, Kyung Rok Lee, Sunghee Ahn, Hongjin Park, Seokyeong Moon, Sungho Yoon and Kwang-Deog Jung
Catalysts 2024, 14(3), 187; https://doi.org/10.3390/catal14030187 - 09 Mar 2024
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Abstract
The practical application of formic acid production through the hydrogenation of CO2 has garnered significant attention in efforts to tackle the challenges associated with (1) achieving net-zero production of formic acid as a chemical feedstock and (2) improving hydrogen storage and transport. [...] Read more.
The practical application of formic acid production through the hydrogenation of CO2 has garnered significant attention in efforts to tackle the challenges associated with (1) achieving net-zero production of formic acid as a chemical feedstock and (2) improving hydrogen storage and transport. This study focuses on demonstrating the continuous operation of a trickle bed reactor for converting CO2 into formate using palladium on activated carbon (Pd/AC). Optimal temperature conditions were investigated through a dynamic operation for 24 h, achieving the maximum productivity of 2140 mmolFA·gPdsurf.−1·h−1 at 150 °C and 8 MPa, with an H2/CO2 ratio of 1:1; however, catalyst deactivation was observed in the process. Stability tests performed under continuous operation at 120 °C and 8 MPa with an H2/CO2 ratio of 1:1 indicated a gradual decline in productivity, culminating in a 20% reduction after 20 h. A comprehensive analysis comparing fresh and spent catalysts revealed that the diminished catalytic activity at elevated temperatures was attributed to the partial sintering and leaching of Pd nanoparticles during the hydrogenation process. These findings offer insights for the future development of novel Pd-based catalyst systems suitable for continuous hydrogenation processes. Full article
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11 pages, 2128 KiB  
Article
Organocatalysts for the Synthesis of Cyclic Carbonates under the Conditions of Ambient Temperature and Atmospheric CO2 Pressure
by Yeongju Seong, Sanghun Lee, Seungyeon Cho, Yoseph Kim and Youngjo Kim
Catalysts 2024, 14(1), 90; https://doi.org/10.3390/catal14010090 - 22 Jan 2024
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Abstract
2–(1H–1,2,4–Triazol–3–yl)phenol (CAT–1) was used as an organocatalyst for the coupling reaction of CO2 and epoxides at an ambient temperature and atmospheric CO2 pressure (1 bar). This compound has a structure in which a hydrogen bond donor, a [...] Read more.
2–(1H–1,2,4–Triazol–3–yl)phenol (CAT–1) was used as an organocatalyst for the coupling reaction of CO2 and epoxides at an ambient temperature and atmospheric CO2 pressure (1 bar). This compound has a structure in which a hydrogen bond donor, a hydrogen bond acceptor, and another hydrogen bond donor are adjacent in sequence in a molecule. The binary catalytic system of CAT–1/nBu4NI showed TON = 19.2 and TOF = 1.60 h−1 under 1 bar CO2 at room temperature within 12 h using 2–butyloxirane. Surprisingly, the activity of CAT–1, in which phenol and 1H–1,2,4–triazole are chemically linked, showed a much greater synergistic effect than when simply mixing the same amount of phenol and 1H–1,2,4–triazole under the same reaction conditions. In addition, our system showed a broad terminal and internal epoxide substrate scope. Full article
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21 pages, 5083 KiB  
Article
Comparative Study of Supported Ni and Co Catalysts Prepared Using the All-in-One Method in the Hydrogenation of CO2: Effects of Using (Poly)Vinyl Alcohol (PVA) as an Additive
by Luisa F. Navarrete, María Atienza-Martínez, Inés Reyero, José Carlos Urroz, Oihana Amorrortu, Oihane Sanz, Mario Montes, Siby I. Garcés, Fernando Bimbela and Luis M. Gandía
Catalysts 2024, 14(1), 47; https://doi.org/10.3390/catal14010047 - 10 Jan 2024
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Abstract
Two series of Ni and Co catalysts supported onto La-Al2O3 were prepared and the CO2 hydrogenation reactions investigated. The catalytic performance was evaluated in terms of the evolution with the reaction temperature of the CO2 conversion and product [...] Read more.
Two series of Ni and Co catalysts supported onto La-Al2O3 were prepared and the CO2 hydrogenation reactions investigated. The catalytic performance was evaluated in terms of the evolution with the reaction temperature of the CO2 conversion and product (CH4 and CO) yields, as well as specific activities (TOF) and apparent activation energies. CH4 was the favored product over both metals while the TOF for CH4 formation was about three times higher for Ni than Co at 240–265 °C. Metallic particle size effects were found, with the TOF for CH4 formation decreasing over both Ni and Co as the mean metallic size decreased. In contrast, the TOF for CO formation tended to increase at a decreasing particle size for the catalysts with the smallest Ni particle sizes. The apparent activation energies for Ni and Co were very similar and significantly decreased to values of 73–79 kJ/mol when the metallic dispersion increased. The catalysts were prepared using the all-in-one method, resulting in (poly)vinyl alcohol (PVA) being a key additive that allowed us to enhance the dispersion of Ni and Co to give very effective catalysts. This comparative study joins the few existing ones in the literature in which catalysts based on these metals operated under strictly the same reaction conditions. Full article
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11 pages, 3475 KiB  
Article
Cu and Cu-Fe Bi-Metal Nanoparticles Encapsulated in Hollow S-1 Zeolite for Reverse Water Gas Shift Reaction
by Rui Hu, Tianye Wang, Hongwei Li, Yuan Zhu, Yifan Wang, Fuli Wen, Enhui Xing, Yu Wu and Zhijian Da
Catalysts 2023, 13(7), 1037; https://doi.org/10.3390/catal13071037 - 26 Jun 2023
Cited by 1 | Viewed by 1046
Abstract
The hollow hierarchical structure Cu@S and CuFe0.5@S catalysts were successfully synthesized through the “dissolution-recrystallization” (D-R) method for the reverse water gas shift reaction (RWGS). The encapsulated catalysts had a hierarchical porous structure and better dispersion of Cu particles than the Cu-S [...] Read more.
The hollow hierarchical structure Cu@S and CuFe0.5@S catalysts were successfully synthesized through the “dissolution-recrystallization” (D-R) method for the reverse water gas shift reaction (RWGS). The encapsulated catalysts had a hierarchical porous structure and better dispersion of Cu particles than the Cu-S and CuFe0.5-S samples prepared via the conventional impregnation method. Furthermore, CuFe0.5-S and CuFe0.5@S catalysts showed higher CO2 conversion and 100% selectivity of CO at the entire temperature range investigated in this work compared to the monometallic catalysts Cu-S and Cu@S. Interestingly, the reaction activity of all the samples increased according to the sequence: CuFe0.5@S > CuFe0.5-S > Cu@S > Cu-S at 400–550 °C under atmospheric pressure. These results indicate that the higher dispersion of encapsulation structure and the enhanced surface basicity derived from the addition of Fe play crucial roles in enhancing the catalytic performance of Cu-based catalysts in the RWGS reaction. Full article
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Review

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25 pages, 3341 KiB  
Review
Low-Temperature Electrochemical Oxidation of Methane into Alcohols
by Adeel Mehmood, Sang Youn Chae and Eun Duck Park
Catalysts 2024, 14(1), 58; https://doi.org/10.3390/catal14010058 - 12 Jan 2024
Cited by 1 | Viewed by 1218
Abstract
The direct oxidation of methane to methanol is considered challenging due to the intrinsically low reactivity of the C–H bond of methane and the formation of a large number of unstable intermediates (methanol, formaldehyde, and formic acid) relative to the yield of methane. [...] Read more.
The direct oxidation of methane to methanol is considered challenging due to the intrinsically low reactivity of the C–H bond of methane and the formation of a large number of unstable intermediates (methanol, formaldehyde, and formic acid) relative to the yield of methane. However, promising advances have recently been reported in this area based on the use of electrochemical systems that differ from traditional thermal catalysis. In this review, the recent advances in direct and indirect electrochemical methane conversion with homogeneous catalysts are reviewed and discussed, especially under low-temperature conditions. Finally, the limitations of the current electrochemical methane conversion technology and future research directions are discussed. Full article
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