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, Physical
Na Liu, Lin Zhang, Kangzhou Wang, Lishu Shao, Xiaoyu Guo, Yingluo He, Zhiping Wu, Peng Zhan, Guangbo Liu, Jinhu Wu, Guohui Yang, Noritatsu Tsubaki
Summary: A high-performance catalyst based on ZnZrSi oxide system was developed for the selective synthesis of butadiene from renewable aqueous ethanol. The catalyst exhibited excellent productivity and stability, with competitive ethanol conversion and butadiene selectivity.
APPLIED SURFACE SCIENCE
(2022)
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, 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
Dalibor Hradsky, Petr Machac, David Skoda, Lucie Leonova, Petr Sazama, Jana Pastvova, Dalibor Kaucky, Dalibor Vsiansky, Zdenek Moravec, Ales Styskalik
Summary: The open porosity and number of Lewis acid sites in metal silicates are key factors for high butadiene productivity from ethanol. Microporous zeolites have shown high BD yields. In this study, non-hydrolytic sol-gel (NHSG) was used to prepare micro-mesoporous zirconosilicates. The NHSG preparation provided highly homogeneous Zr dispersion in silica, resulting in increased Lewis acid site numbers and higher activity in various reactions.
APPLIED CATALYSIS A-GENERAL
(2023)
Article
Engineering, Electrical & Electronic
M. Soleimani Varaki, A. Jafari, M. Ebrahimizadeh Abrishami
Summary: Nanostructured perovskite oxides, particularly the nonstoichiometric perovskite CaMnO3-delta nanomaterial, have shown promising potential as high-performance photocatalysts under IR and visible light irradiation for CO2 photoreduction to methanol. The study demonstrated that electron photoexcitation from O-2p and Mn-3d e(g)up arrow 1 valance band to Mn-3d e(g)up arrow 2 conduction band provides the necessary radicals for CO2 reduction. This research highlights the potential of CaMnO3-delta as an active catalytic material for CO2 photoreduction to methanol under both visible and IR irradiation.
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
(2021)
Article
Chemistry, Physical
Bo Chen, Yixin Xu, Chuanye Xiong, Shane Rickard, J. Anibal Boscoboinik, De-en Jiang, Michelle Kidder, Aditya Savara
Summary: A mechanistic study was conducted on the catalytic conversion of ethanol over La0.7Sr0.3MnO3-x perovskite catalysts in the presence and absence of water. The study aimed to gain insights into the path of C-C coupling toward acetone and crotonaldehyde and to clarify the role of water in the reaction. The results provided important information on the mechanism of ethanol catalytic conversion and the formation of acetone and crotonaldehyde.
Article
Chemistry, Physical
Henrique Brasil, Albert F. B. Bittencourt, Kathlen C. E. S. Yokoo, Paulo C. D. Mendes, Lucas G. Verga, Karla F. Andriani, Richard Landers, Juarez L. F. Da Silva, Gustavo P. Valenca
Summary: This study investigated the effects of different preparation methods of HAP on catalytic activity, with microwave-treated catalyst showing the best performance. DFT results suggested that basic sites facilitate acetaldehyde formation, while the balance of acidic/basic sites contributes to C-C bond formation, consistent with experimental observations.
JOURNAL OF CATALYSIS
(2021)
Article
Chemistry, Physical
Sang-Ho Chung, Teng Li, Tuiana Shoinkhorova, Sarah Komaty, Adrian Ramirez, Ildar Mukhambetov, Edy Abou-Hamad, Genrikh Shterk, Selvedin Telalovic, Alla Dikhtiarenko, Bart Sirks, Polina Lavrik, Xinqi Tang, Bert M. Weckhuysen, Pieter C. A. Bruijnicx, Jorge Gascon, Javier Ruiz-Martinez
Summary: Wet-kneaded silica-magnesia is a benchmark catalyst for ethanol-to-butadiene Lebedev process. The formation of magnesium silicates and their properties are explained in terms of acid and base site ratios. However, the exact mechanism and reactivity of magnesium silicates have not been fully established.
Article
Chemistry, Physical
Fangliang Li, Binli Wang, Xiao Chen, Hongjun Fan, Xueming Yang, Qing Guo
Summary: The study shows that the R-TiO2(100)-(1 x 1) surface exhibits high reactivity and selectivity for aldol condensation of unbranched aldehydes at room temperature. The low energy barriers for enolization and dehydration reactions, along with stable adsorption of intermediates, contribute to the surface's efficiency in forming crotonaldehyde. The exclusive selectivity of (E)-crotonaldehyde formation is attributed to the adsorption configuration of CH3CHO and surface structure of R-TiO2(100)(1 x 1).
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Chemistry, Multidisciplinary
Jachym Muck, Jaroslav Kocik, Karel Frolich, Josef Simek, Martina Michalkova, Martin Hajek
Summary: The conversion of ethanol into petrochemicals using a Mg-Fe mixed oxide catalyst modified with a second transition metal was studied. The effects of the second transition metal on both the catalyst itself and the reaction products were investigated. It was found that Ni and Cu enhanced the ethanol conversion and promoted the yield of ethyl acetate and higher alcohols. Additionally, the long-term stability of all catalysts was tested.
Article
Physics, Atomic, Molecular & Chemical
Shu-Xuan Dang, Han-Xuan Liu, Tao Ban, Xin Gao, Zheng-Qing Huang, Dong-Yuan Yang, Chun-Ran Chang
Summary: In this study, the mechanism of one-step conversion of ethanol to butadiene over ZnY/BEA catalyst was investigated using density functional theory (DFT) calculations. It was found that ethanol dehydrogenation preferred to proceed on the Zn site, while aldol condensation to produce butadiene preferred to occur on the Y site. Based on this mechanism, Zn-Y/BEA was identified as the most optimal catalyst for this reaction.
CHINESE JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Multidisciplinary
Al-Shaimaa M. Essehaity, Dalia R. Abd ElHafiz, Delvin Aman, Sara Mikhail, Yasser K. Abdel-Monem
Summary: The study focused on acrolein production from bio-alcohols methanol and ethanol mixtures using AMnO(3) perovskite catalysts doped with Ba and/or Sr. The BaSrMnO3 sample showed the highest catalytic performance, achieving an acrolein selectivity of 62% under specific conditions. The increase in acrolein production was attributed to the high C-C coupling tendency of BaSrMnO3 due to metal substitution, enhancing the aldol condensation reaction.
Article
Chemistry, Physical
Ruiyi Yan, Zhaopo Lv, Hongguo Tang, Yinge Bai, Mengyue Li, Yuchao Li
Summary: The study utilized diethylammonium acetate as a catalyst to achieve a high conversion rate of 99.9% from propionaldehyde to methacrolein, with a selectivity of 97.4%. Isotopic tracing experiments and decreasing the reaction temperature were used to propose a possible reaction mechanism.
Article
Multidisciplinary Sciences
Shima Nasri, Mohammad Bayat, Fatemeh Rostami Miankooshki
Summary: A novel multi-component reaction was developed for the synthesis of diverse spiro-imidazo pyridine-indene derivatives. The reaction involved heterocyclic ketene aminals reacting with bindone, using malononitrile as a promoter or as one of the precursors. The convenient one-pot operation, high substrate diversity, and presence of active sites in the synthesized products are attractive features of this approach.
SCIENTIFIC REPORTS
(2022)
Article
Chemistry, Physical
Dien-Thien To, Yu-Chia Chiang, Jyh-Fu Lee, Chi-Liang Chen, Yu-Chuan Lin
Summary: An active and stable Co catalyst decorated by N species was developed and applied in the hydrogenation of levulinic acid to gamma-valerolactone. The doped N species improved the concentration of Co delta+ with strong Lewis acidity, enhancing the activity of Co-based catalysts derived from CoPS.
Article
Energy & Fuels
Elbert Halim, Cheng-Pao Lee, Wei-Cheng Wang, Jhe-Kai Lin, Yu-Chuan Lin
Summary: This study investigates the role of single-metal-loaded SAPO-11-based catalysts in producing renewable jet fuel. Among the metals tested, nickel-loaded SAPO-11 showed the highest conversion rate, with Ni/SAPO-11(CA) displaying higher selectivity towards the carbon chain length of jet fuel compared to Ni/SAPO-11. Operating conditions such as temperature, pressure, and H-2-to-feedstock ratio were optimized using the Taguchi method, resulting in a high conversion rate to HRJ with a favorable isomer-to-normal alkane ratio.
INTERNATIONAL JOURNAL OF ENERGY RESEARCH
(2022)
Article
Chemistry, Physical
Cheng-Chia Li, Chou-Hsun Hsieh, Yu-Chuan Lin
Summary: Ni catalysts obtained by carbothermal reduction exhibit excellent performance in the hydrogenation of levulinic acid, with high stability and GVL productivity.
MOLECULAR CATALYSIS
(2022)
Article
Engineering, Environmental
Mahmoud Kamal Hussien, Amr Sabbah, Mohammad Qorbani, Mohamed Hammad Elsayed, Putikam Raghunath, Tsai-Yu Lin, Shaham Quadir, Hong-Yi Wang, Heng-Liang Wu, Der-Lii M. Tzou, Ming-Chang Lin, Po-Wen Chung, Ho-Hsiu Chou, Li-Chyong Chen, Kuei-Hsien Chen
Summary: This study presents a green method for synthesizing a metal free modified g-C3N4 photocatalyst, achieving high efficiency in gas-phase CO2 reduction and hydrogen generation without the need for any cocatalyst. This work provides a new avenue for exploring rational modifications of g-C3N4 nanosheets for efficient clean energy production.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Chemistry, Multidisciplinary
Shih-Hao Wang, Rathinam Raja, Chuen-Yo Hsiow, Farheen Khurshid, Hau-Ren Yang, Po-Wen Chung, Yu-Ying Lai, Ru-Jong Jeng, Leeyih Wang
Summary: This work demonstrates the efficient catalytic conversion of CO2 to CO using a fullerene derivative, DTBT-C-60, as a photocatalyst, which exhibits excellent solar absorption and durable catalytic activity.
Article
Chemistry, Physical
Korawich Trangwachirachai, Chin-Han Chen, Ai-Lin Huang, Jyh-Fu Lee, Chi-Liang Chen, Yu-Chuan Lin
Summary: Co-pyrolyzing gallium nitrate hydrate and melamine, melem, or g-C3N4 generates gallium nitride (GaN) for the conversion of methane to acetonitrile (AcCN). The solid-state-pyrolysis-made GaN catalysts exhibited better activity than commercial GaN. Among the as-prepared catalysts, GaN made by using g-C3N4 with a N/Ga ratio of 2 (i.e., GaN-(C3N4)-(2)) showed the highest initial methane conversion and AcCN productivity.
CATALYSIS SCIENCE & TECHNOLOGY
(2022)
Article
Chemistry, Physical
Warot Prasanseang, Kittisak Choojun, Yingyot Poo-arporn, Ai-Lin Huang, Yu-Chuan Lin, Tawan Sooknoi
Summary: In this study, copper phyllosilicate was utilized as a bifunctional catalyst to convert methyl palmitate into long-chain alpha-olefins, achieving high conversion and selectivity.
APPLIED CATALYSIS A-GENERAL
(2022)
Article
Nanoscience & Nanotechnology
Raju Kumar, Cheng-Chia Li, Chia-Hui Wu, Tai-Wei Tzeng, Der-Lii M. Tzou, Yu-Chuan Lin, Po-Wen Chung
Summary: We have demonstrated that the surface nature of nanoscale hydrotalcite-derived oxide (HTO) can be controlled simply by adding amorphous silica during material preparation. This modification leads to the formation of ternary Mg, Al, and Si interfaces and enhances the chemically accessible aluminum (Al3+tetra) as acidic sites. The modified HTO/SiO2-X catalyst shows different catalytic performance in the ethanol condensation reaction, with HTO promoting 1-butanol production and HTO/SiO2-5 favoring 1,3-butadiene production. This difference in catalytic performance can be attributed to the redistribution of acidic and basic sites upon the newly formed ternary interfaces.
ACS APPLIED NANO MATERIALS
(2022)
Article
Energy & Fuels
Min-Yee Choo, Lee Eng Oi, Yu-Chuan Lin, Tau Chuan Ling, Eng-Poh Ng, Wei-Hsin Chen, Chin Kui Cheng, Joon Ching Juan
Summary: Energy is essential in the 21st century, with most of it being supplied by fossil fuels. However, the environmental and sustainability issues associated with burning fossil fuels have led to the production of biofuels. In this study, two synthesis strategies were used to address the diffusion limitation of conventional zeolite Y, resulting in the preparation of hierarchical nanosized zeolite Y. The best hierarchical nanosized zeolite Y (MY0.15) showed good deoxygenation performance and reusability under H-2 free conditions.
Article
Chemistry, Physical
Yu-Chuan Lin, Chou-Hsun Hsieh
Summary: This study investigates the use of Co-based catalysts derived from different materials including CoAl-layered double hydroxide (LDH), LDH/melamine, LDH/activated carbon, and LDH/g-C3N4 in the hydrogenation of gamma-valerolactone into 1,4-pentanediol. The CoAl-LDH/g-C3N4 catalyst showed improved turnover frequency due to its higher concentrations of strong Bronsted acid, Lewis acid, and Lewis base sites.
CATALYSIS SURVEYS FROM ASIA
(2023)
Article
Chemistry, Physical
Bo-Yan Chen, Galina Dobele, Ance Plavniece, Aleksandrs Volperts, Loreta Tamasauskaite-Tamasiunaite, Eugenijus Norkus, Chi-Liang Chen, Yu-Chuan Lin
Summary: K-doped FeCx catalysts derived from the carbothermal reduction of the Fe-chitosan complex were investigated for the hydrogenation of CO2 to light olefins. Catalyst characterization and performance evaluation revealed a correlation between the physicochemical properties of the catalysts and their catalytic activities. Mechanistic studies identified various carbonate and formate species as intermediates involved in C2-6= synthesis. The most active catalyst, FeK@CS-(0.5)-py, exhibited the highest space-time yield of C-2-6(-) (13.7 mu mol(C2-6=)/g(Fe)/s).
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2023)
Article
Chemistry, Physical
Dien-Thien To, Joon Ching Juan, Meng-Hsuan Tsai, Chia-Hsin Wang, Chih-Wen Pao, Chi-Liang Chen, Yu-Chuan Lin
Summary: FeCx catalysts were synthesized by co-pyrolyzing iron nitrate with various CN sources. The Fe-d-C3N4-(0.3)-Py catalyst exhibited the highest CO2 conversion, olefin yield, and olefin STY, attributed to its high surface FeCx concentration. A correlation between surface FeCx and hydrocarbon/olefin STY was established.
CATALYSIS SURVEYS FROM ASIA
(2023)
Article
Chemistry, Physical
Hepsiba Niruba Catherine, Zhi-Ting Liu, Chan-Yi Lin, Po-Wen Chung, Shun Tsunekawa, Shawn D. Lin, Masaaki Yoshida, Chechia Hu
Summary: In this study, potassium chloride (KCl)-incorporated graphitic carbon nitride (g-C3N4, CN) with enhanced Lewis basicity and varying amounts of N-vacancies and pyridinic-N was synthesized for carbon dioxide (CO2) capture. The CN11 sample showed higher CO2 adsorption capacity compared to other template-free carbon materials due to its abundance of pyridinic-N and high surface area. Spectroscopic analysis confirmed the presence of pyridinic-N and Lewis basic sites on the CN sample, which contributed to the enhanced CO2 adsorption. This work provides insights into the CO2 adsorption mechanism and identifies CN11 as a promising candidate for CO2 capture and storage.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
K. Trangwachirachai, A. -l. Huang, H. -K. Chen, C. -L. Chen, J. -F. Lee, H. -K. Tian, Y. -C. Lin
Summary: The reduction of GaN using different carriers was investigated and tested for methane conversion to acetonitrile. The highest ammonia and ACN productivities were obtained using 5 wt% GaN on HZ. The N-Ga interaction was weakened due to the presence of a neighboring Bronsted acid, and rejuvenation of activity could be achieved through a renitridation step. The (001) side surface of GaN was found to be important in the conversion of methane to ACN.
MATERIALS TODAY CHEMISTRY
(2023)
Review
Chemistry, Inorganic & Nuclear
Korawich Trangwachirachai, Yu-Chuan Lin
Summary: This review surveys the processes of transforming light hydrocarbons to nitriles, discusses the developments in nitrile synthesis from alkanes, and addresses the existing challenges and plausible solutions.
DALTON TRANSACTIONS
(2023)
