Article
Chemistry, Physical
Shupeng Guo, Congcong Niu, Zhongyi Ma, Jungang Wang, Bo Hou, Litao Jia, Debao Li
Summary: Introducing Ba and CN species into Co/Al2O3 catalyst can enhance the electron density on the cobalt surface, which improves the C-5(+) selectivity and C-3 o/p ratio, leading to enhanced catalytic performance in Fischer-Tropsch synthesis reaction.
Article
Energy & Fuels
Dalia Liuzzi, Francisco J. Perez-Alonso, Sergio Rojas
Summary: Ru-Co/Al2O3 and Ru-Fe/Al2O3 catalysts prepared by reduction-deposition method exhibit high activity in Fischer-Tropsch Synthesis, showing different conversion rates and product selectivity. The interaction between Ru and Co in Ru-Co/Al2O3 enhances the activity, while Ru-Fe/Al2O3 displays superior initial performance but declines over time, with less enriched products compared to Ru/Al2O3.
Article
Chemistry, Applied
Mohammad Mehrbod, Michela Martinelli, Jonathan D. Castro, Nour Alhraki, Donald C. Cronauer, A. Jeremy Kropf, Christopher L. Marshall, Gary Jacobs
Summary: Direct reduction of cobalt nitrate using alumina showed differences in reducibility and Co crystallite size compared to traditional calcination/reduction treatment. Noble metals improved cobalt oxide reducibility, especially in the final reduction step. The best performance was achieved with direct reduction of uncalcined 0.5% Pt-25%Co/Al2O3.
Article
Energy & Fuels
Shupeng Guo, Congcong Niu, Zhongyi Ma, Jungang Wang, Bo Hou, Litao Jia, Debao Li
Summary: N-doped carbon materials are being studied as a promising support for catalytic performance in Fischer-Tropsch synthesis, with efforts to overcome complex preparation methods. This study introduces a simple and harmless approach to prepare CN-modified Co/Al2O3 catalyst, showing improved reducibility and electron density on cobalt surface, leading to enhanced selectivity and TOF. This research provides a new avenue for obtaining high activity and selectivity catalysts.
Article
Energy & Fuels
Shupeng Guo, Zhongyi Ma, Jungang Wang, Bo Hou, Litao Jia, Baojun Wang, Debao Li
Summary: The synergistic promotion effect of Ru and Ba in Co/Al2O3 catalyst achieved higher CO conversion and lower CH4 selectivity, compared to unmodified or single additive modified catalyst. The influences of other alkali earth metal additives were also similar to that of Ba in promoting FTS reaction on Co-Ru catalysts.
Article
Chemistry, Physical
Xinyan Ai, Yuhua Zhang, Shuai Lyu, Chengchao Liu, Yanxi Zhao, Jinlin Li
Summary: To investigate the impact of gamma-alumina pore size on the efficiency of Co/Al2O3 catalysts in Fischer-Tropsch synthesis, ordered mesoporous alumina samples with different pore sizes were synthesized and Co/OMA catalysts were prepared. Characterization experiments were conducted and the relationship between catalyst structure and FTS performance was analyzed. The TOF and C5+ selectivity of the catalysts increased with increasing OMA pore size, while CH4 selectivity decreased. The particle size of Co3O4 in the catalysts was highly dependent on the OMA pore size, which was a crucial factor affecting catalyst performance.
Article
Chemistry, Physical
Somayeh Mansouri, Seyyed Hossein Zohdi, Hossein Atashi, Maliheh Ghofran Pakdel, Ali Akbar Mirzaei
Summary: The size of catalysts has no impact on the type of deactivation model. Smaller catalysts have a smaller deactivation constant and higher long-term stability. Larger catalyst sizes tend to accumulate carbon and heavy hydrocarbon fouling, leading to decreased specific surface area and lower catalytic activity.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2022)
Article
Chemistry, Multidisciplinary
Thitiwut Sukprom, Pooripong Somchuea, Sarannuch Sringam, Thongthai Witoon, Metta Chareonpanich, Pawin Iamprasertkun, Kajornsak Faungnawakij, Gunther Rupprechter, Anusorn Seubsai
Summary: This study investigated the direct conversion of methane (CH4) to value-added hydrocarbons (C2+) using a hybrid catalyst. The hybrid catalyst consisted of Ni/Al2O3 as the first catalyst layer to convert CH4 to carbon monoxide and K-Co/Al2O3 as the second catalyst layer to convert carbon monoxide to C2+. The hybrid catalyst exhibited effective performance at a relatively low temperature of 490 degrees C, compared to other catalysts used in methane oxidative coupling reactions. The study explored the effects of different operating conditions and found that the highest C2+ yield of 4.3% was achieved at a reactor temperature of 490 degrees C. The addition of K promoter played a crucial role in enhancing C2+ formation. The proposed mechanism for the reaction using the hybrid catalyst was described, and the stability of the catalyst was observed to be excellent during a 24-hour time-on-stream test.
REACTION CHEMISTRY & ENGINEERING
(2023)
Article
Chemistry, Physical
Roman E. Yakovenko, Grigory B. Narochnyi, Ivan N. Zubkov, Ekaterina A. Bozhenko, Yash V. Kataria, Roman D. Svetogorov, Alexander P. Savost'yanov
Summary: This article presents a simple method for producing high-octane gasoline from CO and H-2 using a Co-Al2O3/SiO2/HZSM-5/Al2O3 hybrid catalyst. By adjusting the pressure and temperature, the content of branched hydrocarbons can be increased. The experimental batch of gasoline fraction produced under the optimized process parameters has an octane number of 78.5 units.
Article
Chemistry, Physical
Jose Antonio Diaz-Lopez, Jordi Guilera, Marti Biset-Peiro, Dan Enache, Gordon Kelly, Teresa Andreu
Summary: The technical feasibility of passivating a Co/gamma-Al2O3 catalyst using atomic layer deposition (ALD) to reduce deactivation rate during Fischer-Tropsch synthesis (FTS) was explored in this study. The results showed that 3 to 6 ALD cycles effectively reduced deactivation of the catalyst, while 10 cycles caused blockage of the active phase and a decrease in catalytic activity. This research demonstrates the potential of ALD as a method to improve catalyst stability in FTS processes.
Article
Chemistry, Physical
Tshepo Molefe, Dean Barrett, Beatriz Diaz, Roy Forbes, Neil J. Coville
Summary: This study reports on the synthesis and application of osmium nanoparticles supported on and/or encapsulated in hollow carbon spheres for Fischer-Tropsch Synthesis (FTS). It is demonstrated that the interaction between osmium and cobalt has a significant effect on the catalyst activity when loaded together. Proximity of osmium and cobalt leads to higher FTS activity and C5+ production through the primary spillover effect. This study reveals the effect of osmium on FTS catalysts for the first time.
JOURNAL OF CATALYSIS
(2023)
Review
Energy & Fuels
Da Wang, Min Zhong, Jian Xue, Zhong Wang, Xuebing Li, Bo Hou
Summary: In this review, the utilization of various catalysts and supports, including structured catalysts, high thermal conductive carbon and silicon carbide supported cobalt catalysts, and high thermal conductive Al2O3@Al support, for the improvement of heat transfer in fixed-bed reactors during cobalt-based Fischer-Tropsch synthesis (FTS) are summarized. The use of Co/Al2O3@Al catalysts in the reactor bed significantly increases the heavy hydrocarbon selectivity and shows great potential for industrial application. The review also prospects the possible technical issues and their solutions in large-scale industrial applications.
Article
Materials Science, Ceramics
Ming Hao, Peizhang Gao, Wei Liu, Baizeng Fang, Jinsheng Liang, Tingting Zhang, Youpeng Ding, Hui Zhang, Fei Wang
Summary: A novel Co/CoAl2O4/sepiolite nanocomposite was synthesized in this study, with optimal conditions identified for fabrication. The nanocomposite showed fine cobalt nanoparticles anchored on the surface of CoAl2O4, leading to higher selectivity for high-carbon hydrocarbons in Fischer-Tropsch synthesis. This work provides an effective strategy for low-cost batch fabrication of efficient cobalt-based catalysts.
CERAMICS INTERNATIONAL
(2021)
Article
Chemistry, Physical
Tobias F. Kimpel, Jin-Xun Liu, Wei Chen, Robert Pestman, Emiel J. M. Hensen
Summary: Through IR spectroscopy and DFT calculations, it has been discovered that in the Fischer-Tropsch reaction, Mn promotes a silica-supported Co catalyst with a MnO layer covering the Co surface, activating adsorbed CO through reaction with an oxygen vacancy. This results in higher activity, higher CHx coverage, increased C5+ selectivity, and decreased CH4 selectivity. Increasing pressure amplifies the selectivity differences. However, above around 4 bar, the addition of Mn decreases C5+ selectivity, possibly due to its promotion of C-O bond dissociation but not chain growth. Migration of formed monomers for chain growth on the Co surface may be hindered by high CO coverage, especially at high pressure.
JOURNAL OF CATALYSIS
(2023)
Article
Energy & Fuels
Chike George Okoye-Chine, Mahluli Moyo, Diane Hildebrandt
Summary: By varying the degree of hydrophobization of SiO2 supports, the catalytic activity of Co catalysts supported on SiO2 was enhanced, also promoting the hydrogenation of CO. It was observed that higher hydrophobicity resulted in larger cobalt clusters, decreasing the reducibility of cobalt oxides and leading to a decline in activity.
Article
Chemistry, Applied
Nuria Garcia-Moncada, Lole Jurado, L. Marcela Martinez-Tejada, Francisca Romero-Sarria, Jose Antonio Odriozola
Summary: The study synthesized a highly efficient water-gas-shift catalyst by mixing proton conductors Mo-Eu-Zr mixed oxide systems with a conventional Pt/CeO2/Al2O3 catalyst. The designed catalyst is able to reach equilibrium conversion at medium temperatures and the mechanism of proton conductors enhances catalytic activity.
Article
Chemistry, Multidisciplinary
Francisco M. Baena-Moreno, Miriam Gonzalez-Castano, Juan Carlos Navarro de Miguel, Kamal U. M. Miah, Ralf Ossenbrink, Jose Antonio Odriozola, Harvey Arellano-Garcia
Summary: The study evaluates the influence of metal substrate geometry on the CO2 methanation reaction, showing the advantages of 3D complex geometries over traditional honeycomb structures, leading to a potential 14% improvement in CO2 conversion under various conditions.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2021)
Article
Chemistry, Multidisciplinary
Tomas R. Reina, Miriam Gonzalez-Castano, Victor Lopez-Flores, L. T. Marcela Martinez, Andrea Zitolo, Svetlana Ivanova, Wenquian Xu, Miguel Angel Centeno, Jose A. Rodriguez, Jose Antonio Odriozola
Summary: In this study, it was demonstrated using in situ X-ray absorption spectroscopy that both Au and Pt remain unoxidized during the water-gas shift (WGS) reaction, with significant differences in their dynamics under WGS atmospheres. While Pt undergoes restructuring into metallic particles, Au nanoparticles experience particle splitting and agglomeration processes, maintaining a zero oxidation state throughout the reaction.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Luis F. Bobadilla, Lola Azancot, Svetlana Ivanova, Juan J. Delgado, Francisca Romero-Sarria, Miguel A. Centeno, Anne-Cecile Roger, Jose A. Odriozola
Summary: The study on methanol adsorption over supported NiSn Nps and analogous NiSn catalyst provided insights into the hydrogen production mechanism from methanol steam reforming, identifying important intermediate species and reaction sites, and elucidating a plausible reaction mechanism. Additionally, it was demonstrated that DME is a secondary product generated by condensation of methoxides in an acid-catalyzed reaction over alumina support.
Article
Chemistry, Physical
L. F. Bobadilla, A. Munoz-Murillo, J. Gandara-Loe, A. Perez, O. H. Laguna, T. L. M. Martinez, A. Penkova, M. A. Centeno, J. A. Odriozola
Summary: This study focuses on the development of efficient catalysts for selective CO methanation in practical conditions. The results show that Rh significantly enhances the activity and selectivity, while Pt has a negative effect. These findings suggest that RuRh-based catalysts could be important for treating industrial-volume streams.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2023)
Article
Engineering, Chemical
Baldassarre Venezia, David C. Morris, Asterios Gavriilidis
Summary: A unique Taylor-vortex membrane reactor (TVMR) design for continuous gas-liquid reactions is presented, which showed improved performance compared to an unbaffled reactor. The reactor design restricts the annular cross section and divides it into multiple mixing zones.
Article
Chemistry, Physical
Lole Jurado, Jerome Esvan, Ligia A. A. Luque-Alvarez, Luis F. F. Bobadilla, Jose A. Odriozola, Sergio Posada-Perez, Albert Poater, Aleix Comas-Vives, M. Rosa Axet
Summary: Rhodium-catalysed hydroformylation is an effective tool for both bulk and fine-chemical synthesis, but its major drawbacks are metal leaching and catalyst recycling. Single-atom catalysts have emerged as a powerful solution to combine the advantages of homogeneous and heterogeneous catalysts. In this study, we demonstrate that Rh atoms anchored on graphitic carbon nitride are robust catalysts for the hydroformylation reaction of styrene.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Multidisciplinary
Loukia-Pantzechroula Merkouri, Juan Luis Martin-Espejo, Luis Francisco Bobadilla, Jose Antonio Odriozola, Melis Seher Duyar, Tomas Ramirez Reina
Summary: In recent years, CO2 emissions in the atmosphere have been increasing rapidly, leading to global warming. CO2 methanation reaction is seen as a solution for this problem by converting CO2 into synthetic natural gas, or CH4. NiRu/CeAl and NiRu/CeZr have demonstrated promising activity for CO2 methanation, with NiRu/CeAl achieving near-equilibrium conversion at 350 degrees C with 100% CH4 selectivity. By adding potassium as an adsorbent, the CO2 adsorption capability of NiRu/CeAl was enhanced, allowing it to function as a dual-function material for CO2 capture and utilization, producing 0.264 mol of CH4/kg of sample from captured CO2. Time-resolved operando DRIFTS-MS measurements provided insights into the process mechanism, showing that CO2 was captured on basic sites and dissociated on metallic sites, resulting in the production of methane through two different pathways. This study highlights the potential of designing advanced dual-function materials by adding an adsorbent to an effective NiRu methanation catalyst.
Article
Materials Science, Multidisciplinary
M. Safdar, M. Gonzalez-Castano, A. Penkova, M. A. Centeno, J. A. Odriozola, H. Arellano-Garcia
Summary: This study investigates the impact of Ni-supported YMn1-xAlxO3 catalysts on the CO2 methanation reaction. The results show the importance of the support nature and the improvement in redox behavior achieved through Al-incorporation.
APPLIED MATERIALS TODAY
(2022)
Article
Energy & Fuels
M. Gonzalez-Castano, J. Gonzalez-Arias, L. F. Bobadilla, E. Ruiz-Lopez, J. A. Odriozola, H. Arellano-Garcia
Summary: Promoting catalytic performance by incorporating alkali has been effective for several reactions, but controversial outcomes have been reported for synthetic natural gas production. This study examines Ni catalysts for CO2 and CO methanation reactions. In-situ DRIFTS spectroscopy reveals similar reaction intermediates for all evaluated systems, suggesting a reaction mechanism involving formate decomposition and hydrogenation of linear carbonyl species. The enhanced CO2 methanation rates of NiFe/Al and NiFeK/Al systems are attributed to promoted formate decomposition, while differences in catalyst performance for CO methanation are associated with the concentration of linear carbonyl species. Interestingly, the incorporation of K in the NiFeK/Al system worsens CO methanation rates.
Article
Chemistry, Physical
S. Carrasco-Ruiz, Q. Zhang, J. Gandara-Loe, L. Pastor-Perez, J. A. Odriozola, T. R. Reina, L. F. Bobadilla
Summary: Dry reforming of methane is a promising catalytic route for converting biogas into syngas. The study has developed a highly stable bimetallic catalyst that prevents coke formation and deactivation, offering a promising solution for biogas upgrading.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2023)
Article
Chemistry, Applied
L. A. Luque-Alvarez, M. Serrano-Cruz, M. Gonzalez-Castano, L. F. Bobadilla, J. A. Odriozola
Summary: Methanol carbonylation was studied over Cu-exchanged zeolitic materials with different topologies: Cu@MOR, Cu@FER, and Cu@ZSM-5. Acid strength was found to be influenced by the framework topology as supported by NH3-TPD results. Pore size and distribution were found to affect catalytic performance, with Cu@FER showing higher methanol conversion due to the presence of Bronsted acid sites and redox centres. Selectivity for acetic acid, methyl acetate, and DME production was determined by the specific channel structure in each material. The reaction mechanism was elucidated using operando DRIFTS-MS and involved methanol adsorption and dehydration on acidic Bronsted sites, with CO activation occurring over Cu+ species.
MICROPOROUS AND MESOPOROUS MATERIALS
(2023)
Review
Chemistry, Physical
Muhammad Asif Nawaz, Ruben Blay-Roger, Maria Saif, Fanhui Meng, J. Gonzalez-Arias, Baoji Miao, Luis F. Bobadilla, Tomas Ramirez-Reina, J. A. Odriozola
Summary: This study summarizes the prospective analysis of nitrogen-based energy carriers, focusing on the renewable synthesis, conversion, and utilization of ammonia. It provides an effective approach for achieving zero carbon emission and paves the way for the development of nitrogen-based energy technologies.
Article
Chemistry, Physical
Loukia-Pantzechroula Merkouri, Juan Luis Martin-Espejo, Luis F. Bobadilla, Jose Antonio Odriozola, Anna Penkova, Tomas Ramirez Reina, Melis S. Duyar
Summary: Time-resolved operando DRIFTS-MS technique was used to reveal the CO2 capture and conversion mechanisms of NiRuNa/CeAl dual-functional material in CO2 methanation, reverse water-gas shift, and dry reforming of methane. CO2 was mainly captured in the form of carbonyls and bidentate carbonates, and a spillover mechanism was employed to obtain the desired products.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Physical
L. A. Luque-Alvarez, J. Gonzalez-Arias, F. Romero-Sarria, T. R. Reina, L. F. Bobadilla, J. A. Odriozola
Summary: Currently, the production of acetic acid through the carbonylation reaction of methanol has limitations, leading to the exploration of alternative methods using heterogeneous catalysts. This study investigates the methanol carbonylation reaction over a Cu-H-MOR catalyst and proposes a reaction mechanism based on the catalytic behavior and performance of the catalyst. The results provide insights into the reaction mechanism and the involvement of acid and redox centers.
CATALYSIS SCIENCE & TECHNOLOGY
(2024)
