Article
Chemistry, Physical
Claudia E. Berdugo-Diaz, Yang Sik Yun, Melissa T. Manetsch, Jing Luo, David G. Barton, Xue Chen, David W. Flaherty
Summary: The direct reduction of esters to ethers offers an efficient pathway to obtain ethers from renewable intermediates. This study elucidates the reaction pathways of propyl acetate in the presence of hydrogen over Pd nanoparticles supported on high-surface area Nb2O5. The results show that esters react via three primary pathways, leading to the formation of different products. The formation of ethers is not affected by the pressure of C5H10O2 but is dependent on the pressure of H-2.
Article
Agricultural Engineering
Tang Son Nguyen, Manh Tu Le, Van Hieu Nguyen
Summary: In this work, the hydrogenolysis of benzyl phenyl ether (BPE) and real organosolv lignin feedstock using NixFey/TiN bimetallic catalysts was investigated. The bimetallic catalysts showed higher activity and selectivity compared to single-component materials, with Ni5Fe2/TiN exhibiting the best performance. XANES analysis confirmed electron transfer from Ni to Fe in Ni5Fe2/TiN, explaining its superior activity.
BIOMASS & BIOENERGY
(2023)
Article
Chemistry, Multidisciplinary
Harriet A. Stanway-Gordon, Jessica S. Graham, Michael J. Waring
Summary: DNA-encoded libraries (DELs) are a popular method for finding small molecule ligands for proteins, with a new catalytic hydrogen transfer reaction developed for efficient hydrogenolysis and hydrogenation reactions. This method shows excellent performance in multicycle synthesis and is fully compatible with DNA amplification and sequencing, enabling the synthesis of DEL sequences using orthogonal protecting groups.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Claudia E. Berdugo-Diaz, Melissa T. Manetsch, Yang Sik Yun, Jieun Lee, Jing Luo, Xue Chen, David W. Flaherty
Summary: Esters can be reduced to ethers and alcohols through C-O bond cleavage by hydrogenation and hydrogenolysis pathways on Bronsted acidic faujasite (M-FAU) supported metal nanoparticles. The rates and selectivities of each pathway are influenced by the metal identity (M=Co, Ni, Cu, Ru, Rh, Pd, and Pt). Pt-FAU catalyst exhibits propyl acetate consumption rates up to 100 times higher than other M-FAU catalysts and achieves a 34% selectivity for ethyl propyl ether. The reduction of esters appears to involve a bifunctional mechanism, with stepwise addition of H* atoms to the carbonyl to form hemiacetals on the metal sites, followed by hemiacetal diffusion to Bronsted acid sites for dehydration to ethers or decomposition to alcohol and aldehyde. The reduction rates of propyl acetate seem to be determined by H* addition to the carbonyl and C-O cleavage of hemiacetal.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Energy & Fuels
Andrew S. May, Elizabeth J. Biddinger
Summary: This study investigated the electrochemical reactions for the hydrogenation and hydrogenolysis of biomass-derived species over Cu foil catalysts. The results showed that the evaporation of MF and side reactions competed in affecting the product quality balance, with nitrogen sparging promoting MF evaporation and improving the yields of furfuryl alcohol and 2-methylfuran.
Article
Energy & Fuels
Wei Jiang, Jing-Pei Cao, Jin-Xuan Xie, Liang Zhao, Chuang Zhang, Xiao-Yan Zhao, Yun-Peng Zhao, Jian-Li Zhang
Summary: The study successfully converted lignin model compound DPE into cyclohexane using the Ru/HZSM-5 catalyst, and further investigated the reaction mechanism and structure-performance relationship.
Review
Chemistry, Physical
Zhihui Wang, Wei Zhang, Cuiqing Li, Chen Zhang
Summary: Layered double hydroxides (LDHs) are widely used in various fields due to their unique structural advantages, and are capable of synthesizing metal catalysts with high metal dispersion, tunable acid-base properties, and strong metal-support interaction. LDH-derived materials show great potential as catalysts in hydrogenation and hydrogenolysis reactions, as indicated by the rapid development in this field with over 200 papers published in the past five years. This review comprehensively discusses the applications of LDH-derived materials as catalysts in different hydrogenation and hydrogenolysis reactions, showcasing their extraordinary potentials in these reactions and their future significance.
Article
Chemistry, Physical
Yueyue Li, Ruonan Wang, Bowen Huang, Liangliang Zhang, Xuran Ma, Shikun Zhang, Zhiguo Zhu, Hongying Lu, Kaixuan Yang
Summary: This study reported an efficient catalyst for the conversion of HMF to high-value-added chemical DMF. The catalyst showed excellent stability and reusability, and achieved selective conversion of HMF by modulating the electronic structure of nickel. Furthermore, the synergy between acid-base sites and indium played a crucial role in the catalytic process.
APPLIED SURFACE SCIENCE
(2022)
Article
Chemistry, Multidisciplinary
Tobias Wagener, Lukas Lueckemeier, Constantin G. Daniliuc, Frank Glorius
Summary: This study successfully demonstrates the synthesis of sought-after, enantioenriched delta-lactams through an interrupted hydrogenation mechanism using oxazolidinone-substituted pyridines and water.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
Denise Lovison, Tobias Berghausen, Sophie R. Thomas, Jonathan Robson, Markus Drees, Christian Jandl, Alexander Poethig, Patrick Mollik, Dominik P. Halter, Walter Baratta, Angela Casini
Summary: In this study, water-soluble organometallic Ru(II) complexes were synthesized and found to act as anticancer agents by catalyzing transfer hydrogenation reactions with biomolecules. The structure-activity relationship and reaction mechanism were investigated, and the compounds were also tested for their anticancer activity in vitro.
Article
Chemistry, Multidisciplinary
Huan Wang, Weitao Wang, Xulu Jiang, Zhen-Hong He, Kuan Wang, Yang Yang, Zhao-Tie Liu, Buxing Han
Summary: In this study, a fast and self-propagated carbonization (SPC) method was proposed for the preparation of phosphorus-doped carbon (PDC) and hybrid materials. PdZr/PDC prepared by the SPC method exhibited excellent catalytic performance in the partial oxidation of benzyl alcohol to benzaldehyde and the partial hydrogenation of phenol to cyclohexanone. The method is simple, clean, and suitable for large-scale material preparation.
Article
Chemistry, Inorganic & Nuclear
Guoqi Zhang, Haisu Zeng, Quan Tang, Selin Ates, Shengping Zheng, Michelle C. Neary
Summary: A study on the regioselective epoxide ring-opening through hydroboration catalysed by a vanadium(III) dialkyl complex supported by a redox-active terpyridine ligand is reported. The effective Markovnikov hydroboration of terminal epoxides led to the synthesis of secondary alcohols in high yields, demonstrating a new catalytic application of an earth-abundant vanadium(III) complex.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Physical
Dennis Panke, German Bechthold, Thomas E. Mueller
Summary: This paper discusses the solvent effect in the catalytic depolymerization of lignin, as well as presents the results of an experimental study on the depolymerization of kraft lignin. The study finds that ruthenium and platinum catalysts, particularly Pt/C, show resilience to sulfur in kraft lignin, and methanol is a suitable solvent. The reaction conditions strongly affect the conversion of kraft lignin to lignin oil, with different catalysts showing different optimal conditions. The formation of specific products is attributed to the solubility of oligomeric lignin fragments in the solvent and the adsorption of specific groups on the catalyst surface.
Article
Chemistry, Multidisciplinary
Josanne-Dee Woodroffe, Benjamin G. Harvey
Summary: The sustainable, bio-based platform chemical 2,5-hexanedione was efficiently converted to methylcyclopentadiene through a three-step process involving intramolecular aldol condensation, catalytic chemoselective hydrogenation, and dehydration. This approach provides a new pathway for preparing high-performance fuels and polymers from sustainable feedstocks.
Review
Biochemistry & Molecular Biology
Fernando Carrillo-Hermosilla, Rafael Fernandez-Galan, Alberto Ramos, David Elorriaga
Summary: This review focuses on the organometallic chemistry of guanidinato compounds, discussing their various coordination modes, reactivity, and applications in catalysis or materials science. It is believed that these amazing ligands offer new promises in Organometallic Chemistry.
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.