Article
Chemistry, Applied
Lucas L. R. Vono, Cornelia Broicher, Karine Philippot, Liane M. Rossi
Summary: The large-scale production of biomass-derived fuels generates lignocellulosic residues that can be further converted into bio-derived value-added chemicals, with a focus on the selective hydrogenation of phenol as a model compound. Different nanoparticles (NPs) of Pd, Ru and Rh immobilized on modified silica-based supports showed varying selectivity towards cyclohexanone and cyclohexanol, with titania-containing supports enhancing selectivity.
Article
Multidisciplinary Sciences
Guanhua Cheng, Wei Zhang, Andreas Jentys, Erika E. Ember, Oliver Y. Gutierrez, Yue Liu, Johannes A. Lercher
Summary: This study demonstrates the significant role of the self-established open circuit potential (OCP) in stabilizing cationic intermediates and transition states, as well as enhancing reaction rates in catalytic reactions.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Organic
Xiaohan Li, Ruchita R. Thakore, Balaram S. Takale, Fabrice Gallou, Bruce H. Lipshutz
Summary: Commercially available Pd/C catalyst with only 0.4 mol % Pd loading can be used for nitro group reductions. The reaction can be carried out using silane or a hydrogen balloon, resulting in high yields of desired amines. Both the catalyst and surfactant can be recycled without loss of reactivity.
Article
Chemistry, Physical
Heng Xia, Hongzi Tan, Hongyou Cui, Feng Song, Yuan Zhang, Rongrong Zhao, Zhe-Ning Chen, Weiming Yi, Zhihe Li
Summary: The selectivity of hydrogenation of phenol to cyclohexane or cyclohexanol over Pd/NaY catalyst can be achieved by regulating the solvent polarity. The solvent polarity greatly influences the reaction mechanism and product selectivity, as well as the adsorption manner of phenol in the catalyst.
CATALYSIS SCIENCE & TECHNOLOGY
(2021)
Article
Chemistry, Physical
Robert Bavisotto, Sree Pradipta Roy, Nicholas Hopper, Wilfred T. Tysoe
Summary: We investigated the influence of hydrogen pressure on the selectivity of furfural hydrogenation on palladium. Our findings show that at low hydrogen pressures, decarbonylation products are formed, while at higher pressures, 2-methyl furan is produced. This change in selectivity is attributed to the effect of co-adsorbed hydrogen on the orientation of furfural adsorbed on the surface. The results obtained from studying the hydrogenation of furfural on a Pd(111) single crystal support this postulate.
JOURNAL OF CATALYSIS
(2023)
Article
Chemistry, Multidisciplinary
Sif T. Linde, Vasco Corti, Vibeke H. Lauridsen, Johannes N. Lamhauge, Karl Anker Jorgensen, Nomaan M. Rezayee
Summary: This article presents a method for obtaining a versatile chiral biaryl structure through C-H halogenation reactions using high-valent Pd catalysis and chiral transient directing groups. The method is scalable, moisture and air insensitive, and in some cases, requires low Pd-loadings of only 1 mol%. Chiral mono-brominated, dibrominated, and bromochloro biaryls can be prepared in high yield and excellent stereoselectivity, serving as building blocks for various reactions with orthogonal synthetic handles.
Article
Multidisciplinary Sciences
Zhongzhe Wei, Zijiang Zhao, Chenglong Qiu, Songtao Huang, Zihao Yao, Mingxuan Wang, Yi Chen, Yue Lin, Xing Zhong, Xiaonian Li, Jianguo Wang
Summary: This study presents an efficient galvanic replacement strategy to load Pd metallenes on Nb2C MXenes at room temperature. The Pd metallenes have a chair structure of six-membered ring with a coordination number of Pd as low as 3. The strategy exhibits outstanding catalytic activity and selectivity in the semihydrogenation of alkynes.
NATURE COMMUNICATIONS
(2023)
Article
Multidisciplinary Sciences
Chiheng Chu, Dahong Huang, Srishti Gupta, Seunghyun Weon, Junfeng Niu, Eli Stavitski, Christopher Muhich, Jae-Hong Kim
Summary: Research shows that neighboring Pd single atom catalysts can maintain their high selectivity and greatly enhance the activity for hydrogenation of carbon-halogen bonds through cooperative interactions between adjacent atoms. This promising hydrogenation performance presents a new approach for manipulating the activity and selectivity of single atom catalysts.
NATURE COMMUNICATIONS
(2021)
Article
Multidisciplinary Sciences
Jia Yu, Peng Zhang, Lulu Li, Kailang Li, Gong Zhang, Jia Liu, Tuo Wang, Zhi-Jian Zhao, Jinlong Gong
Summary: This paper describes a strategy of balancing the active sites for the generation and dimerization of ketyl intermediates by constructing bimetallic Pd/Cu electrocatalysts with tunable surface coverage of Pd, achieving high Faradaic efficiency and production rate of hydrobenzoin. Experimental and theoretical results show that Pd promotes the generation of ketyl intermediates, while Cu enhances their dimerization. The balance between these two sites facilitates the coupling of benzaldehyde towards hydrobenzoin.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Organic
Jordi Ballesteros-Soberanas, Marta Mon, Antonio Leyva-Perez
Summary: This study demonstrates the synthesis of 1,4-enediols enriched in one diastereoisomer through the classical Pd-catalyzed semi-hydrogenation reaction using readily available 1,4-diacetylenic diols. The semi-hydrogenation reaction concurrently involves the desymmetrization of the meso/racemic form of the enediol. Additionally, it is found that these products can completely inactivate the Pd catalyst when added to H-2 in advance (only before H-2). These findings not only provide a straightforward method for the production of 1,4-enediols enriched in one diastereoisomer using classical catalysis but also offer a means to inhibit H-2 dissociation on Pd nanoparticles.
ORGANIC & BIOMOLECULAR CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Anton Kudashev, Olivier Baudoin
Summary: A ligand-controlled site-selective C(sp(3))-H arylation of heteroaromatic ketones has been developed using Pd catalysis, with selective reactions occurring at the alpha- or beta-position of the ketone side-chain. Addition of a pyridone ligand enables switching from alpha- to beta-arylation. The alpha-arylation process demonstrates broad scope and high site- and chemoselectivity, while the beta-arylation is more limited, with mechanistic investigations suggesting different pathways for the two processes.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Physical
Xiang Li, He Li, Chunzhi Li, Maodi Wang, Qihua Yang
Summary: By changing the carbon chain length of side oxyalkyl groups, two COFs with moderate and strong surface hydrophobicity were prepared. Pd NPs were successfully loaded on the two COFs, and the electron donating from imine linkage to Pd NPs was evidenced by XPS characterizations. Compared with commercial Pd/C, Pd/COF showed higher TOF in the hydrogenation of nitrobenzene, which was attributed to the electron rich Pd, hydrophobic surface, and crystalline structure of COFs. Pd NPs on COFs with strong hydrophobicity were more active than those on COFs with moderate hydrophilicity in the hydrogenation of moderate lipophilic nitro compounds. However, the reversed tendency was observed for the hydrogenation of moderate hydrophilic p-amino-nitrobenzene. The modulation of COFs' surface wettability provides an efficient strategy to improve the catalytic performance of supported metal NPs.
Article
Chemistry, Physical
Pengchao Chen, Kaijie Li, Peijian Yan, Junyou Wang, Shenghu Zhou
Summary: In this study, Pd-FexOy@HMSNs nanoparticles were successfully synthesized with different Pd/Fe ratios, showing significantly enhanced catalytic performance for the reduction of nitroarenes. The improved catalytic activity can be attributed to the synergistic effect of Pd and FexOy as well as the confinement effect of functional nanoparticles inside the hollow cavities.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Chemistry, Inorganic & Nuclear
Taolian Guo, Yi Huang, Nannan Zhang, Tian Chen, Chao Wang, Xing Xing, Zhenda Lu, Lili Wen
Summary: This study demonstrates that the catalytic activity of Pt NPs in nanocomposites can be controlled by modulating the microchemical environment using ultrathin NMOFs as supports. The catalytic activity of the nanocomposites towards liquid-phase hydrogenation shows a significant difference, with Pt@NMOF-Ni exhibiting the highest activity. Increasing the amount of Ni2+ nodes in the carriers can improve the catalytic activity. X-ray photoelectron spectroscopy and density functional theory calculations confirm the distinct electron interactions between Pt NPs and NMOFs as the possible origin of the difference in catalytic activity.
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Physical
Zhengyan Qu, Yucheng Liu, Yanhua Shao, Jiuxuan Zhang, Hong Jiang, Rizhi Chen
Summary: Activated carbon supports obtained from different sources were used for the synthesis of Pd/C catalysts in phenol hydrogenation. The results showed that the Pd/C catalyst using activated carbon derived from wood exhibited superior catalytic activity compared to those using activated carbon derived from coconut shell and coal. The enhanced activity of Pd/C-W was attributed to its larger surface area, higher surface N and O contents, more surface defects, and abundant acidic and alkaline sites.
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.