Article
Chemistry, Physical
Pavlo Kyriienko, Olga Larina, Dmytro Yu Balakin, Mykhailo Vorokhta, Ivan Khalakhan, Sergii A. Sergiienko, Sergiy O. Soloviev, Svitlana M. Orlyk
Summary: This paper presents the investigation of different component oxide systems in aqueous ethanol conversion into 1,3-butadiene, with a focus on the effect of lanthanum in the catalyst composition. The results show that high selectivity of 1,3-butadiene is achieved during the conversion of rectified and aqueous ethanol over the studied catalysts. The activity of the catalysts depends on the order of introducing the components, which determines the acid-base characteristics of the surface. The addition of lanthanum into Cu/Zr-Si catalysts increases their activity by forming lanthanum containing base sites that are tolerant to water. The differences in the interaction of reaction intermediates with surface Zr and La-containing sites are revealed, and the effect of water on the adsorption of carbon coke, ethoxy species, and acetaldehyde over the catalyst surface is demonstrated.
MOLECULAR CATALYSIS
(2022)
Article
Engineering, Chemical
Alexandre C. Dimian, Costin Sorin Bildea
Summary: This paper introduces a new process for manufacturing 1,3-butadiene from renewable bioethanol, and compares it with the one-stage and two-stage processes. The proposed one-stage process utilizes Hf(IV)/Zn(II) catalyst and inert gas to replicate laboratory conditions. The analysis shows that the two-stage process is currently more efficient due to the cost of compressing inert-gas rich mixtures.
CHEMICAL ENGINEERING RESEARCH & DESIGN
(2023)
Article
Chemistry, Physical
Adama A. Bojang, Ho Shing Wu
Summary: The production of 1,3-butadiene from ethanol was carried out using ash as a catalyst in combination with Zr and Mg. Different catalyst combinations were used and characterized, and the yields and selectivities of 1,3-butadiene were determined. It was found that the Ash:MgO (1:2) catalyst had the highest yield and selectivity among the tested combinations, achieving 50% yield and 83% selectivity.
Article
Chemistry, Physical
Adama A. Bojang, Ho-Shing Wu
Summary: The conversion of ethanol to 1,3-butadiene was studied using different Zr-based catalysts. The best catalyst was found to be 10% SiO2-ZrO2, which exhibited high conversion, yield, and selectivity. The composition of the catalyst plays a crucial role in the catalyst's performance and lifespan.
Article
Chemistry, Physical
Minhua Zhang, Xinyue Guan, Jianyu Zhuang, Yingzhe Yu
Summary: In this study, the structural properties of open and closed sites on Zr-beta zeolite and the mechanism of ETB reaction were investigated using density functional theory (DFT) calculations. The results showed that Zr-OH participation in the proton transfer step at open site reduced the energy barrier, making the Meerwein-Ponndorf-Verley (MPV) reaction the rate-limiting step at open site. The number of Zr-beta open sites was positively correlated with catalytic performance.
APPLIED SURFACE SCIENCE
(2022)
Article
Engineering, Chemical
Minhua Zhang, Ruishen Li, Yufei Wu, Yingzhe Yu
Summary: The study found that the MPV reaction and cross aldol condensation are more favorable on the MgO(110) surface, while cross aldol condensation is less likely to occur on the MgO(100) surface and the hydrogenation side reaction is less likely to occur on the MgO(110) surface.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2021)
Article
Chemistry, Physical
Laura A. Cramer, Avery S. Daniels, Volkan Cinar, Prashant Deshlahra, E. Charles H. Sykes
Summary: Bimetallic AgCu catalysts have shown promising applications in selective oxidation reactions. Adding a single monolayer of Ag to Cu significantly increases the selectivity for the epoxidation of 1,3-butadiene. The near-surface alloy of AgCu undergoes dynamic restructuring, enhancing oxygen dissociation on the Ag surface and improving the selectivity of the epoxidation reaction.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Applied
Minhua Zhang, Yunan Qin, Haoxi Jiang, Lingtao Wang
Summary: Hierarchical beta zeolite was prepared through protective desilication with quaternary ammonium hydroxide, and Zr-beta zeolite was prepared using the hierarchical beta zeolite. The mesoporosity of beta zeolite was successfully tuned by adjusting the length of TAAOH alkyl chain, leading to enhanced catalytic activity of Zr-beta zeolite.
MICROPOROUS AND MESOPOROUS MATERIALS
(2021)
Article
Engineering, Environmental
Cheng Liu, Iran Li, Linlin Wu, Zhongfeng Geng
Summary: The kinetics of 1,3-butadiene synthesis from ethanol and acetaldehyde over ZrO2-MgO-SiO2 catalyst were studied, showing that the aldol condensation step followed the Langmuir-Hinshelwood mechanism. The obtained kinetics models were verified under different conditions, suggesting their validity for practical applications.
CHEMICAL ENGINEERING JOURNAL
(2021)
Article
Chemistry, Applied
Kangzhou Wang, Na Liu, Qingxiang Ma, Yugo Kawabata, Fan Wang, Weizhe Gao, Baizhang Zhang, Xiaoyu Guo, Yingluo He, Guohui Yang, Noritatsu Tsubaki
Summary: The efficient synthesis of butadiene from aqueous ethanol was achieved over a series of x%LaZnZr/Si-beta multifunctional catalysts prepared by wet impregnation method. The introduction of La species improved the physicochemical properties and catalytic performance of the ZnZr/Si-beta catalyst. The La species enhanced the main reaction of aldol condensation and inhibited ethanol dehydration, resulting in higher butadiene selectivity and ethanol conversion.
Article
Chemistry, Applied
Houqian Li, Jifeng Pang, Nicholas R. Jaegers, Libor Kovarik, Mark Engelhard, Anthony W. Savoy, Jianzhi Hu, Junming Sun, Yong Wang
Summary: The Ag-O-Si interfaces significantly enhanced the dehydrogenation of ethanol, while the Zr-O-Si interfaces promoted the condensation of acetaldehyde, leading to a high yield of 1,3-butadiene through the synergistic effects of these interfaces.
JOURNAL OF ENERGY CHEMISTRY
(2021)
Article
Environmental Sciences
Jun Nakamura, Sujey Carro, Avram Gold, Zhenfa Zhang
Summary: The study found that 3,4-epoxybutane-1,2-diol (EBD) and its analogs exhibited high toxicity in cells lacking FANC genes, possibly transformed into bifunctional epoxy aldehyde, forming intrastrand cross-links. This finding is important in understanding the mechanisms by which EBD may cause leukemia and lymphoma in humans.
Article
Chemistry, Physical
Astrid Boje, William E. Taifan, Henrik Strom, Tomas Bucko, Jonas Baltrusaitis, Anders Hellman
Summary: This study employs first-principles and microkinetic analysis to investigate the kinetic process of ethanol conversion to 1,3-butadiene, revealing that the dehydration pathway is less active for 1,3-butadiene and identifying rate-determining states in the dehydrogenation, dehydration, and condensation steps.
CATALYSIS SCIENCE & TECHNOLOGY
(2021)
Article
Chemistry, Physical
Yingzhe Yu, Hai Chen, Yantao Hu, Minhua Zhang
Summary: Density functional theory was used to investigate the transition states and energy barriers of side reactions of Aldol condensation on MgO(1 0 0) and MgO(1 1 0) surfaces. The results showed different formation mechanisms of acetone on different crystal planes of MgO, while ethoxyethanol formation reaction had higher activity on both surfaces. Comparing the energy barriers and reaction heats, it was found that the side reactions are more likely to occur on the MgO(1 0 0) surface in terms of kinetics and thermodynamics.
APPLIED SURFACE SCIENCE
(2021)
Article
Chemistry, Multidisciplinary
Qi-Chen Wei, Ya Chen, Zhao Wang, Da-Zhuang Yu, Wei-Hao Wang, Jian-Quan Li, Li-Hua Chen, Yu Li, Bao-Lian Su
Summary: A light-assisted semi-hydrogenation process using water as the hydrogen atom source and in situ photocatalysis was developed, showing excellent catalytic performance and selectivity for 1,3-butadiene semi-hydrogenation at ambient temperature. This H-2-free process has the potential to bring advancements in industrial hydrogenation technology in terms of economic and safe operations.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Physical
Pavlo Kyriienko, Olga Larina, Dmytro Yu Balakin, Anatolii O. Stetsuk, Yurii M. Nychiporuk, Sergiy O. Soloviev, Svitlana M. Orlyk
Summary: A series of ZnO/MgO-SiO2 systems with different MgO:SiO2 ratios were studied for their catalytic performance in 1,3-butadiene production, showing that water presence can decrease C-C coupling products but hydrated sites remain active in the reaction. High 1,3-butadiene selectivity was achieved with MgO:SiO2 ratios of (1:1) and (3:1) in the catalysts.
APPLIED CATALYSIS A-GENERAL
(2021)
Article
Chemistry, Physical
Pavlo Kyriienko, Olga Larina, Dmytro Yu Balakin, Sergiy O. Soloviev, Svitlana M. Orlyk
Summary: Copper and silver have a promoting effect on the catalytic performance of MgO-SiO2 oxide systems in the ethanol-to-butadiene process. The modification of MgO-SiO2 with copper and silver increases the yields by forming active sites for ethanol dehydrogenation and aldol-croton condensation reactions.
Article
Chemistry, Physical
Pavlo Kyriienko, Olga Larina, Dmytro Yu Balakin, Mykhailo Vorokhta, Ivan Khalakhan, Sergii A. Sergiienko, Sergiy O. Soloviev, Svitlana M. Orlyk
Summary: This paper presents the investigation of different component oxide systems in aqueous ethanol conversion into 1,3-butadiene, with a focus on the effect of lanthanum in the catalyst composition. The results show that high selectivity of 1,3-butadiene is achieved during the conversion of rectified and aqueous ethanol over the studied catalysts. The activity of the catalysts depends on the order of introducing the components, which determines the acid-base characteristics of the surface. The addition of lanthanum into Cu/Zr-Si catalysts increases their activity by forming lanthanum containing base sites that are tolerant to water. The differences in the interaction of reaction intermediates with surface Zr and La-containing sites are revealed, and the effect of water on the adsorption of carbon coke, ethoxy species, and acetaldehyde over the catalyst surface is demonstrated.
MOLECULAR CATALYSIS
(2022)
Article
Engineering, Chemical
Gaukhar Yergazieva, Nursaya Makayeva, Zhanna Shaimerden, Sergiy Soloviev, Moldir Telbayeva, Erzhan Akkazin, Fariza Ahmetova
Summary: This article discusses the decomposition of methane on monometallic and bimetallic catalysts in a certain temperature range. The results show that the bimetallic catalyst is more active in the methane decomposition to hydrogen. Various physicochemical methods were used to explain the enhanced catalytic activity of the bimetallic catalyst.
BULLETIN OF CHEMICAL REACTION ENGINEERING AND CATALYSIS
(2022)
Article
Chemistry, Multidisciplinary
G. Yergaziyeva, N. Makayeva, A. Abdisattar, M. Yeleuov, S. Soloviev, M. Anissova, A. Taurbekov, K. Dossumov, E. Akkazin, C. Daulbayev
Summary: In this study, Ni-foam and Ni-Fe composites obtained by the electrochemical method were used as catalysts for methane decomposition. The Ni-Fe150 catalyst showed high catalytic activity and stability at high temperatures.
Article
Chemistry, Multidisciplinary
K. V. Valihura, O. V. Larina, S. O. Soloviev
Summary: The redox and acid-base properties of MgO-Al2O3 systems have been controlled by incorporating bifunctional additives of molybdates and tungstates during synthesis. Doping with Mo and W compounds enhances the activity of Mg-Al-oxide catalysts and the selectivity of 1-butanol formation in ethanol condensation process, attributed to the increased concentration of ethanol dehydrogenation and acetaldehyde aldol condensation sites.
THEORETICAL AND EXPERIMENTAL CHEMISTRY
(2023)
Article
Chemistry, Physical
Svitlana Orlyk, Pavlo Kyriienko, Andriy Kapran, Valeriy Chedryk, Dmytro Balakin, Jacek Gurgul, Malgorzata Zimowska, Yannick Millot, Stanislaw Dzwigaj
Summary: The research focused on the influence of BEA zeolite dealumination on the acid-base characteristics and catalytic performance of Zn-BEA compositions in propane dehydrogenation with CO2. The catalyst samples were prepared through a two-step post-synthesis procedure and characterized using various techniques. Full dealumination led to the formation of a mesoporous structure and decrease in acidity, resulting in enhanced selectivity and yield of propene. The results highlighted the advantages of using Zn-BEA catalysts in the presence of CO2 for producing the target olefin.
Article
Chemistry, Multidisciplinary
S. O. Soloviev, G. R. Kosmambetova, P. I. Kyriienko, D. E. Samoilenko, Y. P. Kurylets
Summary: NiO-Al2O3 and Co3O4 oxide catalysts modified with palladium and oxides of rare earth metals (Ce and La) and formed on structured cordierite supports were investigated for methane oxidation. It was found that the addition of cerium and lanthanum oxides to cobalt-containing catalysts allowed methane oxidation to proceed without CO formation even at low O2/CH4 ratios. The addition of CeO2 promoted dispersion of Co3O4, increased oxygen vacancies, and prevented agglomeration of the catalyst's active phase. Palladium modification enhanced the activity of the Co3O4-CeO2/cordierite catalyst by increasing surface oxygen mobility through interphase interaction with cobalt oxides and ceria.
THEORETICAL AND EXPERIMENTAL CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
S. M. Orlyk, V. I. Chedryk, S. O. Soloviev, O. D. Vasylyev
Summary: Research has shown that modified nickel composites based on stabilized zirconia exhibit high catalytic activity and stability as anode materials for solid oxide fuel cells (SOFC) in the oxidative reforming of alkanes, such as tri-reforming of methane and steam- (oxygen) reforming of butane. Modification of Ni-10Sc1CeSZ composite with Cu and CeO2 enhances its resistance to carbonization, while doping with platinum or palladium (0.1 wt.%) improves its resistance to H2S poisoning. Structured Ni-(CeO2, La2O3)-Al2O3/cordierite catalysts demonstrate high activity and stability in the oxidative reforming of C-1-C-3 alkanes into syngas and can be effectively integrated with an external processor in SOFC systems. Bench tests of the fuel cell show acceptable electrical characteristics.
THEORETICAL AND EXPERIMENTAL CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
O. Larina, P. Kyriienko, O. Morozov, T. Obushenko, N. M. Tolstopalova, S. O. Soloviev
Summary: This study investigates the effect of alkali metal ions (Na+ or K+) on the acid-base and catalytic properties of Zn-Mg(Zr)Si oxide systems during the production of 1,3-butadiene from ethanol. The findings show that modifying Zn-MgSi oxide systems can increase the selectivity of 1,3-butadiene (at temperatures >= 670 K) by reducing the number of by-product formation sites. In the composition of Zn-ZrSi oxide systems, the addition of alkali metal cation leads to a decrease in ethene and diethyl ether selectivity due to the reduction of strong acid sites that are active in the ethanol dehydration reaction.
THEORETICAL AND EXPERIMENTAL CHEMISTRY
(2022)
