Review
Chemistry, Multidisciplinary
Allison M. Arinaga, Morgan C. Ziegelski, Tobin J. Marks
Summary: Research on the catalytic oxidative coupling of methane (OCM) using alternative oxidants such as N2O, CO2, and S-2 is still in its early stages, with unique advantages and challenges compared to oxygen (O-2) as the oxidant. This area has not been extensively reviewed, despite the renewed interest in OCM due to the abundance of shale gas resources.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
Sora Ishioka, Aya Fujiwara, Sunao Nakanowatari, Lauren Takahashi, Toshiaki Taniike, Keisuke Takahashi
Summary: This study utilizes machine learning and catalyst big data to design catalyst descriptors for representing catalytic activities. Experiments confirm the accuracy of the proposed catalyst descriptors and demonstrate that these physical quantities can be used as alternative descriptors for designing heterogeneous catalysts.
Article
Chemistry, Applied
Jordy Ramos-Yataco, Justin Notestein
Summary: The oxidative coupling of methane (OCM) is a direct method for upgrading methane to higher value hydrocarbons using an oxidant. While there has been extensive research on the initial coupling reactions to form ethylene, there has been less focus on further molecular weight growth to C3+ species. This study investigates the OCM activity and production of C3+ using different catalysts, including the A2WO4-MnOx/SiO2 family. The results show that C3+ formation is a gas-phase radical process, and ethylene co-feeds can enhance it under certain reactor conditions.
Article
Chemistry, Physical
Fubo Gu, Xuetao Qin, Liu Pang, Ri Zhang, Mi Peng, Yao Xu, Song Hong, Jinglin Xie, Meng Wang, Dongmei Han, Dequan Xiao, Guangsheng Guo, Xiayan Wang, Zhihua Wang, Ding Ma
Summary: Direct oxidation of methane into value-added liquid chemicals utilizing rhodium dispersed on ZSM-5 catalysts under mild conditions shows high selectivity and efficiency. Increasing acidity over the catalyst improves methane conversion and formic acid selectivity, with activation of C-H bonds even at room temperature.
Article
Energy & Fuels
Shican Jiang, Weixiao Ding, Kun Zhao, Zhen Huang, Guoqiang Wei, Yanyan Feng, Yijv Lv, Fang He
Summary: This study successfully utilized Na-doped LaMnO3 as redox catalysts to convert methane into C-2 products, achieving higher performance in oxidative coupling reaction. The incorporation of Na enhanced the redox properties of the catalyst, promoting the formation of C-2 hydrocarbons, with 019Na-LaMnO3 demonstrating the best results among all samples.
Article
Engineering, Chemical
Hasan Ozdemir, Ecem Ciftcioglu, M. A. Faruk Oksuzomer
Summary: La2O3 and La2O2CO3 catalysts with different morphologies were synthesized and tested for the oxidative coupling of methane. La2O3 catalysts were sensitive and La2O2CO3 catalysts were stable under atmospheric conditions. The surface oxygen type, surface area, and basicity were found to be important factors influencing the activity and selectivity of the catalysts.
CHEMICAL ENGINEERING SCIENCE
(2023)
Article
Chemistry, Physical
Lien Thi Do, Jae-Wook Choi, Dong Jin Suh, Chun-Jae Yoo, Hyunjoo Lee, Jeong-Myeong Ha
Summary: The oxidative coupling of methane using hybrid catalysts containing BaTiO3 perovskite and Mn-Na2WO4 exhibited high activity and selectivity at low temperature by improving oxygen-supplying ability and methane activation ability of the catalysts. This was achieved through the insertion of Mn into BaTiO3 and the formation of NaxMn(Ti) O-2, and the stable interaction between WO(4)(2-) anions and the catalysts.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2021)
Article
Chemistry, Multidisciplinary
Sagar Sourav, Yixiao Wang, Daniyal Kiani, Jonas Baltrusaitis, Rebecca R. Fushimi, Israel E. Wachs
Summary: The study showed that the crystalline Na2WO4 active phase is unstable under OCM reaction conditions, partially transforming into thermally stable surface Na-WOx sites. These sites are responsible for selectively activating CH4 and over-oxidizing CHy.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Energy & Fuels
Na Sun, Jiayu Zhang, Lixia Ling, Pengyu Niu, Riguang Zhang, Litao Jia, Debao Li, Baojun Wang
Summary: Lanthanum oxide (La2O3) catalyst is a promising system for the oxidative coupling of methane (OCM) reaction, but its low activity for methane dissociation limits its widespread use. Low-value dopants, such as Mg and Li, can enhance the methane conversion activity on La2O3 catalysts. This study investigated the mechanism and catalytic performance of OCM reaction on Mg-doped and Li-doped La2O3 catalysts using a combination of DFT and experimental methods. The results showed that Mg and Li doping significantly improved CH4 dissociation activity and C2H4 selectivity on the La2O3(0 0 1) surface. Mg-doped La2O3 catalyst exhibited the best catalytic performance, while Li-doped La2O3 showed poorer performance due to the loss of doped Li during the OCM process. The study also explored the OCM reaction cycle and the mechanism of action of oxygen species on Mg-doped La2O3(0 0 1).
Article
Chemistry, Physical
Yixiao Wang, Sagar Sourav, Jason P. Malizia, Brooklyne Thompson, Bingwen Wang, M. Ross Kunz, Eranda Nikolla, Rebecca Fushimi
Summary: This study investigates the role of individual oxide phases and their combinations in supported Mn-Na2WO4 /SiO2 catalysts for oxidative coupling of methane (OCM). It is found that Mn plays an important role in promoting gas phase oxygen activation, while NaOx/SiO2 and WOx/SiO2 are relatively inert. The supported catalyst combining Na and W in the form of Na2WO4 shows enhanced gas-phase oxygen activation and methane activation. However, excessive Mn content leads to nonselective OCM pathways.
Article
Chemistry, Physical
JeongHyun Cho, Dahye Kwon, Inchan Yang, Suna An, Ji Chul Jung
Summary: The addition of Ca as a promoter significantly influences the catalytic activity of MgO in oxidative coupling of methane by affecting oxygen vacancies and the basicity of surface lattice oxygen, leading to increased methane conversion and ethylene production.
MOLECULAR CATALYSIS
(2021)
Article
Chemistry, Applied
P. Saychu, M. Thanasiriruk, C. Khajonvittayakul, R. Viratikul, V. Tongnan, M. Hartley, S. Wongsakulphasatch, N. Laosiripojana, U. W. Hartley
Summary: The NaCl-Mn2O3/SiO2 catalyst showed the best performance in the OCM reaction, with high methane conversion and C-2 selectivity. However, slight deactivation was observed due to the decomposition of NaCl, leading to a decrease in chloride content and carbon formation. Na2WO4-Mn2O3/SiO2 exhibited good stability and no coke deposition, suggesting high surface oxygen content in Na2WO4.
Article
Chemistry, Applied
Roman Petrov, Sergey Reshetnikov, Yuliya Ivanova
Summary: A 7-step kinetic model of oxidative coupling of methane (OCM) on the SrO-La2O3 catalyst was developed and validated with experimental data, showing high accuracy in predicting the reaction. Compared to other models, the developed model demonstrated better agreement between experimental results and predictions.
FUEL PROCESSING TECHNOLOGY
(2021)
Article
Chemistry, Applied
Zixiao Liu, Sichao Cheng, Emily Schulman, Weiqi Chen, Dionisios G. Vlachos, Yuying Shu, Dat T. Tran, Dongxia Liu
Summary: This study prepared a vitreous silica-supported iron (Fe/SiO2-V) catalyst by fusion of quartz silica and fayalite, and investigated its physicochemical properties and performance in direct non-oxidative methane coupling (NMC). Compared to cristobalite support, the vitreous silica support with disordered Si-O bonds and structural defects enabled better iron dispersion and more vital metal-support interaction. The Fe/SiO2-V catalyst exhibited a shorter induction period in methane activation and produced less coke during NMC.
Article
Chemistry, Physical
Duanxing Li, Shintaro Yoshida, Bhavin Siritanaratkul, Angel T. Garcia-Esparza, Dimosthenis Sokaras, Hirohito Ogasawara, Kazuhiro Takanabe
Summary: The study investigated the oxidative coupling of methane over a K2WO4/SiO2 catalyst, finding that the addition of H2O increased CH4 conversion rate and C2 selectivity. The presence of K2O2 and KO2 species at high temperatures was shown to catalyze H2O activation for OH radical generation, contributing to the OCM reaction.
Article
Chemistry, Physical
Ekaterina Ponomareva, Marco-Antonio Lopez-Martinez, Daan Wiggere, Maria V. Morales, Ignacio Melian-Cabrera
APPLIED CATALYSIS A-GENERAL
(2019)
Article
Chemistry, Physical
Yu A. Gordienko, V. Lomonosov, E. A. Ponomareva, M. Yu Sinev, A. Bukhtiyarov, Z. S. Vinokurov
RUSSIAN JOURNAL OF PHYSICAL CHEMISTRY A
(2019)
Article
Engineering, Environmental
Vladimir Lomonosov, Yury Gordienko, Ekaterina Ponomareva, Mikhail Sinev
CHEMICAL ENGINEERING JOURNAL
(2019)
Article
Physics, Atomic, Molecular & Chemical
E. A. Lagunova, Yu. D. Ivakin, M. Yu. Sinev, D. P. Shashkin, Z. T. Fattakhova, Yu. A. Gordienko
RUSSIAN JOURNAL OF PHYSICAL CHEMISTRY B
(2020)
Article
Physics, Atomic, Molecular & Chemical
E. A. Lagunova, Yu. D. Ivakin, M. Yu. Sinev, D. P. Shashkin, Yu. A. Gordienko, Z. T. Fattakhova
RUSSIAN JOURNAL OF PHYSICAL CHEMISTRY B
(2020)
Article
Physics, Atomic, Molecular & Chemical
M. Yu. Sinev, Yu. D. Ivakin, D. P. Shashkin, Z. T. Fattakhova, E. A. Ponomareva, Yu. A. Gordienko, V. Yu. Bychkov
RUSSIAN JOURNAL OF PHYSICAL CHEMISTRY B
(2020)
Article
Physics, Atomic, Molecular & Chemical
P. R. Vasyutin, E. A. Lagunova, M. Yu. Sinev, Yu. D. Ivakin, Yu. A. Gordienko, D. P. Shashkin
Summary: The effect of synthesis method on the structure and composition formation of lanthanum oxide compounds deposited on porous alumina composites is studied. The morphology of porous alumina influences the formation of various compounds during thermal treatment, with more intense processes observed in water fluid treatment due to increased mobility of structural elements in a hydrated state. The hydration of initial aluminum oxide limits the formation of LaAlO3 aluminate, which is more significant in the case of gamma-modification. Variation in treatment sequence and conditions allows the obtainment of composites with different morphologies and oxide compounds.
RUSSIAN JOURNAL OF PHYSICAL CHEMISTRY B
(2022)
Article
Physics, Atomic, Molecular & Chemical
P. R. Vasyutin, Yu. A. Gordienko, M. Yu. Sinev, Yu. D. Ivakin, E. A. Lagunova
Summary: The formation of mixed oxides in the Al2O3-MO (M = Mg, Ca, Sr, Ba) systems by heat treatment and treatment with water fluids (WFs) is studied. It is shown that mainly MAl2O4 aluminates are formed during the high-temperature treatment, sometimes with an admixture of aluminates of a different composition. Pretreatment in WF leads to more complex composition due to dehydration and partial structuring. Addition of ammonia to WF stimulates the formation of double oxides, likely through alkaline hydrolysis.
RUSSIAN JOURNAL OF PHYSICAL CHEMISTRY B
(2022)
Article
Chemistry, Multidisciplinary
Vladimir Lomonosov, Thomas M. R. Wayman, Elizabeth R. Hopper, Yurii P. Ivanov, Giorgio Divitini, Emilie Ringe
Summary: Bimetallic Pd-Mg nanoparticles were synthesized and studied for their catalytic and photocatalytic properties in selective hydrogenation of acetylene. The Mg-Pd structures consist of metallic Mg and sustain plasmon resonances. Even without light excitation, the Pd-Mg nanostructures exhibit excellent catalytic activity. With laser excitation, the reaction rate increases and the activation energy decreases, indicating a catalytic behavior affected by plasmon excitation. The coupling between Mg's plasmonic and Pd's catalytic properties paves the way for sustainable catalytic structures for selective hydrogenation processes.
Article
Chemistry, Multidisciplinary
Vladimir Lomonosov, Jeremie Asselin, Emilie Ringe
Summary: The study reveals a pronounced effect of solvent on the reaction kinetics of metallic nanoparticles in the reduction of 4-NiP, with alcohols leading to a dramatic decrease in reaction rate. However, increasing borohydride concentration or reaction temperature can noticeably improve the reduction rate.
REACTION CHEMISTRY & ENGINEERING
(2022)
Article
Chemistry, Physical
V. I. Lomonosov, M. Yu. Sinev
Summary: This study analyzes the validity of using kinetic scheme reduction procedures to compare kinetic models and values of kinetic parameters, as well as the peculiarities of gas-phase reaction development and approaches to selecting kinetic parameters of elementary steps. It has been shown that kinetic models developed based on the independence of kinetic parameters principle may have low predictive power, and there are limitations in using reduction procedures to analyze complex process mechanisms.
KINETICS AND CATALYSIS
(2021)
Article
Chemistry, Applied
Qingyuan Zheng, Jack H. Williams, Scott Elgersma, Mick D. Mantle, Andrew J. Sederman, G. Leendert Bezemer, Constant M. Guedon, Lynn F. Gladden
Summary: In this study, a pilot-scale fixed-bed reactor compatible with NMR/MRI was developed for Fischer-Tropsch synthesis. Multiple magnetic resonance techniques were applied to quantitatively characterize different product species within catalyst pellets, providing valuable information for catalyst and reactor optimization.
Article
Chemistry, Applied
Lisa Ramisch, Sebastian Pfaff, Sabrina M. Gericke, Edvin Lundgren, Johan Zetterberg
Summary: We present a combination of optical operando techniques that allow simultaneous measurement of adsorbed species on catalyst surfaces, monitoring of surface oxide formation, and imaging of the gas phase above the catalyst surface. The experimental setup was validated by studying CO oxidation on Pd(100) at different pressures, revealing the effects of pressure on the heterogeneous catalytic reaction.
Article
Chemistry, Applied
Marta Paniagua, Gabriel Morales, Juan A. Melero, Daniel Garcia-Salgado
Summary: The influence of common impurities in levulinic acid on the catalytic performance of different acid catalysts for bio-jet fuel production was studied. It was found that furfural had the greatest detrimental effect on catalyst performance, while propyl-sulfonic acid-modified SBA-15 and sulfonic acid resin Amberlyst-70 showed good regeneration ability.
Article
Chemistry, Applied
Jesus Tapiador, Pedro Leo, Guillermo Calleja, Gisela Orcajo
Summary: This study presents a new MOF material, Zn-URJC-13, with acid and basic sites, permanent porosity, and high affinity to CO2 molecules. The Zn-URJC-13 catalyst exhibits efficient performance in CO2 cycloaddition reactions and can be reused multiple times.
Article
Chemistry, Applied
Dan Zhao, Vita A. Kondratenko, Dmitry E. Doronkin, Shanlei Han, Jan-Dierk Grunwaldt, Uwe Rodemerck, David Linke, Evgenii V. Kondratenko
Summary: This study demonstrates the potential of cheap and commercially available Zr or Ti-based supports and ZnO to serve as active and selective catalysts for propane dehydrogenation (PDH). The catalytically active species formed in situ under PDH conditions consist of isolated ZnOx. ZnOx on the surface of LaZrOx shows the highest rate of propene formation.
Article
Chemistry, Applied
Hanbyeol Kim, Jung Rae Kim, Young-Kwon Park, Jeong-Myeong Ha, Jungho Jae
Summary: In this study, metal phosphates were used as catalysts for biomass conversion to produce sustainable aromatics through DielsAlder cycloaddition reactions. The effects of synthesis method, activation method, and P/Ti molar ratio on the structure and acid properties of titanium phosphate catalysts were systematically studied. The mesoporous titanium phosphate catalyst synthesized by hydrothermal method at 180℃ for 12 h followed by ethanol refluxing at 60℃ for 24 h at a molar P/Ti ratio of 1 showed the highest surface area and acid site density.
Article
Chemistry, Applied
Yasin Khani, Sumin Pyo, Kwang-Eun Jeong, Chul-Ung Kim, Moonis Ali Khan, Byong-Hun Jeon, Kun-Yi Andrew Lin, Siyoung Q. Choi, Young-Kwon Park
Summary: A protonated form of Zeolite Socony Mobil-5 (H-ZSM-5) catalyst was synthesized through a hydrothermal method using different sources of silica. The effect of loading the catalyst with yttrium, samarium, and gadolinium on the acidic properties was investigated. Among the metal-loaded catalysts, the Sm/LHZ catalyst showed the best performance in the methanol to propylene conversion due to its high amount of weak and intermediate acid sites, while the Gd-LHZ catalyst increased the selectivity towards ethane and propane.
Article
Chemistry, Applied
Michael Franc, Ivana Cisarova, Jan Vesely
Summary: The present study investigates an enantioselective cyclization of enals with imidazolone derivatives catalyzed by a combination of achiral Pd(0) complex and chiral secondary amine. Corresponding spirocyclic imidazolones were produced in high yields with moderate diastereoselectivity and excellent enantioselectivity. The developed co-operative catalytic methodology provides a highly substituted spirocyclic scaffold with four stereogenic centers under mild conditions.
Article
Chemistry, Applied
Mauro Alvarez, Jennifer Cueto, David P. Serrano, Pablo Marin, Salvador Ordonez
Summary: This study focuses on improving the formulation and preparation methods of catalysts for the production of dimethyl carbonate. By using suitable catalyst preparation methods and copper salt precursors, the researchers successfully produced catalysts with optimal performance for dimethyl carbonate formation.
Article
Chemistry, Applied
Claudia J. Keijzer, Luc C. J. Smulders, Dennie Wezendonk, Jan Willem de Rijk, Petra E. de Jongh
Summary: This study investigates the catalytic behavior of alpha-alumina supported silver catalysts in the presence of chloride. It is found that the particle size of silver can affect the selectivity of the catalyst, but different strategies lead to different results. In this size range, the selectivity of ethylene oxide is correlated to the Ag : Al2O3 surface ratio.
Article
Chemistry, Applied
Takeshi Aihara, Wataru Aoki, Michikazu Hara, Keigo Kamata
Summary: The development of acid-base bifunctional catalysts is important for promoting specific chemical transformations. In this study, Ti-based perovskite oxides were synthesized and used as catalysts for two C-C bond-forming reactions (cyanosilylation and Knoevenagel condensation). The highly pure SrTiO3 nanoparticles with a high specific surface area exhibited the highest catalytic performance, and could be easily recovered and reused.
Article
Chemistry, Applied
Olga Gorlova, Petra Pribylova, Eliska Vyskocilova, Katerina Peroutkova, Jan Kohout, Iva Paterova
Summary: This study investigates the Baeyer-Villiger oxidation of beta-cyclocitral using tin-modified mixed oxides as catalysts. The optimal reaction conditions and the effects of various factors on the reaction course and selectivity were determined. The results show that tin-modified mixed oxides exhibit high activity and selectivity in the oxidation reaction.
Article
Chemistry, Applied
M. I. Avila, M. M. Alonso-Doncel, L. Briones, G. Gomez-Pozuelo, J. M. Escola, D. P. Serrano, A. Peral, J. A. Botas
Summary: The catalytic fast pyrolysis of lignin using ion-exchanged zeolite catalysts showed significant improvements in bio-oil quality and the production of aromatic hydrocarbons and oxygenated compounds.
Article
Chemistry, Applied
Enrico Catizzone, Giorgia Ferrarelli, Paolo Bruno, Girolamo Giordano, Massimo Migliori
Summary: The acid-catalysed alcohol conversion reaction is a promising route for de-fossilization strategies. Research on pure alcohol conversion and simultaneous dehydration of mixed alcohols have shown different product compositions, with the type and distribution of acid sites affecting the reaction mechanism.
Article
Chemistry, Applied
Alireza Ranjbari, Juho Kim, Jihee Yu, Jiyun Kim, Mireu Park, Nayoung Kim, Kristof Demeestere, Philippe M. Heynderickx
Summary: This study investigated a novel kinetic model for the adsorption and photocatalytic degradation of methyl orange using commercial ZnO and reduced ZnO photocatalysts. The results provided new insights into the interaction of catalysts with molecules of different charges and compared with a previous study on methylene blue. The presence of oxygen vacancies in ZnO and their effects on adsorption and photocatalytic degradation were analyzed, and the photocatalytic degradation rate of reduced ZnO was found to increase significantly.