Article
Chemistry, Physical
Gema Blanco-Brieva, Frederique Desmedt, Pierre Miquel, Jose M. Campos-Martin, Jose L. G. Fierro
Summary: The direct synthesis of hydrogen peroxide using a palladium catalytic system on silica was studied without the use of acid and halide promoters. Several bromide substituents were utilized in the catalyst synthesis. Characterization of the catalysts revealed the presence of only palladium (II) species, with the Pd/Br ratio affecting hydrogen peroxide yield and selectivity.
Article
Chemistry, Multidisciplinary
David Kovacic, Richard J. Lewis, Caitlin M. Crombie, David J. Morgan, Thomas E. Davies, Angeles Lopez-Martin, Tian Qin, Christopher S. Allen, Jennifer. K. Edwards, Liwei Chen, Martin Skov Skjoth-Rasmussen, Xi Liu, Graham J. Hutchings
Summary: In this study, the promotive effect of Au and Sn incorporation into Pd nanoparticles was evaluated for the direct synthesis of H2O2. The introduction of secondary metal modifiers significantly enhanced the catalytic performance, with the incorporation of Sn improving Pd dispersion. The optimal PdSn catalyst achieved comparable H2O2 selectivities to state-of-the-art materials.
Article
Engineering, Environmental
Zaiyong Yang, Zengxi Wei, Shunxin Zhou, Bo Bao, Shuangliang Zhao, Fuzhong Gong
Summary: This study reports a new continuous DSHP process by constructing a feasible microreactor upon microfluidic chip under ambient condition, which achieved continuous production of H2O2 with high concentration. The study provides a promising on-site route to produce H2O2 in a green, safe yet ready-to-use process.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Multidisciplinary Sciences
Hong-chao Li, Qiang Wan, Congcong Du, Jiafei Zhao, Fumin Li, Ying Zhang, Yanping Zheng, Mingshu Chen, Kelvin H. L. Zhang, Jianyu Huang, Gang Fu, Sen Lin, Xiaoqing Huang, Haifeng Xiong
Summary: This study develops a two-step approach to prepare PdSn nanowire catalysts, which exhibit superior reactivity and high producibility in the synthesis of H2O2.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Aoxue Huang, Roxanna S. Delima, Yongwook Kim, Eric W. Lees, Fraser G. L. Parlane, David J. Dvorak, Michael B. Rooney, Ryan P. Jansonius, Arthur G. Fink, Zishuai Zhang, Curtis P. Berlinguette
Summary: This study reports a method for direct hydrogenation of O(2) gas to form H2O2 using a membrane reactor without H-2 gas. Hydrogen is obtained from water source and the reactor is powered by electricity. The concentration of H(2)O(2) can be increased about 8 times by optimizing the ratio of methanol-to-water in the chemical chamber and through catalyst design. The study also demonstrates the sensitivity of H(2)O(2) concentration to its decomposition rate, which can be minimized using AuPd alloy catalysts.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Jiawei Zhao, Xiaotong Zhang, Jiajia Xu, Wei Tang, Zhong Lin Wang, Feng Ru Fan
Summary: Researchers have discovered a new method to synthesize hydrogen peroxide (H2O2) by contact charging a two-phase interface, yielding stable and high production of H2O2 under room temperature and normal pressure. This finding provides an efficient way for H2O2 preparation and may encourage further exploration of contact-electrification-induced chemistry processes.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Applied
Xuan Tin Tran, Viet Le Nam Vo, Young-Min Chung
Summary: In this study, FePd catalysts supported on graphite were prepared through fast microwave-irradiated carbon nanotube growth and metal reduction, effectively solving the problem of low H2O2 yield in direct synthesis. The use of different carbon sources significantly affected the geometric and electronic characteristics of Pd on the carbon surface, and therefore influenced the catalytic activity for the DSHP reaction.
Article
Chemistry, Multidisciplinary
Seiji Ogo, Takeshi Yatabe, Tamon Tome, Riko Takenaka, Yoshihito Shiota, Kenji Kato
Summary: In this study, a homogeneous catalyst is used to synthesize hydrogen peroxide using H2 and O2 in water, eliminating the need for flammable H2/O2 mixtures and cocatalysts. The catalyst is capable of extracting electrons from H2, storing them for the reduction of O2, and then converting the reduced oxygen to H2O2. The catalyst exhibits the highest turnover number (TON) among all homogeneous catalysts.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Seiji Ogo, Takeshi Yatabe, Tamon Tome, Riko Takenaka, Yoshihito Shiota, Kenji Kato
Summary: This paper reports a method for the synthesis of H2O2 using a homogeneous catalyst in water, using only H2 and O2 without flammable mixtures or cocatalysts. The catalyst can remove electrons from H2, store them for the reduction of O2, and allow the protonation of the reduced oxygen to form H2O2. The turnover number (TON) is 910 under an H2/O2 (95/5) atmosphere (1.9 MPa) for 12 hours at 23 degrees C, which is the highest among any homogeneous catalysts. Furthermore, a reaction mechanism based on two crystal structures is proposed.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Roberto Calmanti, Maurizio Selva, Alvise Perosa
Summary: Tungstate catalysts are commonly used for olefin epoxidation reactions, but their catalytic activity for CO2 insertion in epoxides has recently been discovered. A new catalytic tandem process was developed for directly converting olefins into cyclic organic carbonates (COCs) using an ammonium tungstate ionic liquid catalyst. This process showed high efficiency and selectivity in converting 1-decene into decene carbonate without the need for intermediate work-up.
Article
Chemistry, Physical
Ole Reinsdorf, Kari Eranen, Tapio Salmi
Summary: In this study, a combination of transient methods in a laboratory-scale trickle bed reactor and attenuated total reflection (ATR)-infrared spectroscopy was used to investigate the reaction mechanism of direct synthesis of hydrogen peroxide (DSHP) on a commercial 5%Pd/C catalyst with water and methanol as solvents. The results showed an oscillatory pattern with the appearance of methoxy and hydroxymethyl species before peroxide species after switching from water to methanol. Based on the specific position and intensities of these species over time, an enhanced reaction scheme for DSHP in methanol was proposed, wherein methanol can form hydroxymethyl species that act as co-catalysts to reduce absorbed oxygen species.
Article
Chemistry, Physical
Zhu Jin, Yifeng Liu, Liang Wang, Chengtao Wang, Zhiyi Wu, Qiuyan Zhu, Lingxiang Wang, Feng-Shou Xiao
Summary: In this study, AuPd nanoparticles fixed within aluminosilicate zeolite crystals were used as catalysts for the direct synthesis of H2O2 in aqueous solution. The zeolite-assisted proton transfer process catalyzed the oxygen hydrogenation to form H2O2, leading to high productivity and selectivity of H2O2 in water. The findings highlight the potential of zeolite fixed structures for designing efficient catalysts in H2O2 synthesis.
Article
Chemistry, Physical
Lyudmila B. Belykh, Nikita I. Skripov, Tatyana P. Sterenchuk, Elena A. Milenkaya, Tatyana A. Kornaukhova, Fedor K. Schmidt
Summary: The behavior of palladium-phosphorus catalysts on a Na-ZSM-5 zeolite support in the direct synthesis of hydrogen peroxide under mild conditions was studied. Elemental phosphorus was found to enhance the activity and selectivity of Pd catalysts for H2O2 synthesis. The P:Pd ratio showed a direct relationship with the catalysts' activity. The influence of phosphorus on the properties of palladium catalysts in side reactions and the chemical and phase composition of Pd-P particles were investigated.
APPLIED CATALYSIS A-GENERAL
(2023)
Article
Chemistry, Analytical
Fanny Girard-Sahun, Pauline Lefrancois, Vasilica Badets, Stephane Arbault, Franck Clement
Summary: This study aims to detect the in situ production of reactive oxygen and nitrogen species (RONS), specifically superoxide anion (O-2(center dot-)), in aqueous buffer solutions exposed to cold atmospheric plasmas (CAPs). The production and accumulation of RONS in the liquids were found to depend on the plasma composition, with N-2-based shieldings providing the highest concentrations of superoxide. The study provides valuable insights into the interactions between CAPs and physiological solutions for biomedical applications.
ANALYTICAL CHEMISTRY
(2022)
Article
Chemistry, Applied
Min Woo Lee, Deok Yeon Jo, Geun-Ho Han, Kwan-Young Lee
Summary: The study observed that the hydrogen peroxide selectivity of Pd/SiO2 and PdBrx/SiO2 catalysts increased with the bromine content. Density functional theory calculations confirmed that the adsorption of bromine adjusted the reaction barrier on the Pd catalyst surface, improving the selectivity of hydrogen peroxide.
Article
Multidisciplinary Sciences
Rosa M. Coco-Martin, Cristina Andres-Iglesias, Girish K. Srivastava, Javier Lagos-Rodriguez, Miguel Ruiz-Tevah, Mario R. Diaz-Cardenas, Ivan Fernandez-Bueno, Juan Garcia-Serna, Maria T. Garcia-Gutierrez, Alfredo Garcia-Layana, J. Carlos Pastor
Summary: The study reported cases of acute intraocular toxicity caused by MEROCTANE commercialized by a Turkish company, highlighting the cytotoxic effects and presence of highly toxic contaminants. While perfluorocarbon liquids are useful tools for intraocular surgery, measures must be implemented to ensure product safety based on both chemical and cytotoxicity analysis for every batch, and medical staff should report suspected cases to the respective National Agencies.
SCIENTIFIC REPORTS
(2021)
Article
Green & Sustainable Science & Technology
Marta Ramos-Andres, Beatriz Aguilera-Torre, Juan Garcia-Serna
Summary: The study focused on the valorization of discarded carrot pulp through hydrothermal treatment, extracting free sugars, hemicellulose, and pectin. The flow-through extraction method allowed for the obtainment of high molecular weight fractions, enabling further applications.
JOURNAL OF CLEANER PRODUCTION
(2021)
Article
Chemistry, Applied
Filippo Buttignol, Alberto Garbujo, Pierdomenico Biasi, Daniel Rentsch, Oliver Kroecher, Davide Ferri
Summary: This study investigates the effect of an alumina-based binder on the structure of a commercial Fe-ZSM-5 catalyst. The results show that the binder improves the catalyst's dispersion of Fe species, framework Al content, and acidity, while reducing Fe agglomeration and framework Al migration.
Article
Engineering, Chemical
Tapio Salmi, Vincenzo Russo, Adriana Aguilera, Pasi Tolvanen, Johan Warna, Martino Di Serio, Riccardo Tesser, Tommaso Cogliano, Sebastien Leveneur, Kari Eranen
Summary: A rigorous mathematical model was developed for a complex liquid-liquid-solid system in a batch reactor, particularly applicable for the indirect epoxidation process of vegetable oils. The model takes into account reaction kinetics and intra- and interfacial mass transfer effects. The model was tested with a generic example, demonstrating the applicability of multiphase models in epoxidation processes.
Article
Engineering, Chemical
German Araujo-Barahona, Kari Eranen, Jay Pee Ona, Dmitry Murzin, Juan Garcia-Serna, Tapio Salmi
Summary: This study focuses on the development and application of a solid foam catalyst based on ruthenium nanoparticles supported on active carbon. Kinetic experiments were conducted to investigate the hydrogenation performance of the catalyst on two sugars at different temperatures and hydrogen pressures. The results showed high selectivities and conversions of the sugars to sugar alcohols, and the ratio of the sugar mixture also affected the reaction rate and catalyst behavior.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2022)
Article
Engineering, Chemical
Ali Najarnezhadmashhadi, Catarina G. Braz, Vincenzo Russo, Kari Eranen, Henrique A. Matos, Tapio Salmi
Summary: This study developed an advanced three-phase model for a trickle bed reactor with solid foam packings. The model considers the effects of axial, radial, and catalyst layers, and includes most individual terms like internal diffusion, gas-liquid and liquid-solid mass transfer, and kinetics. Sensitivity analysis was conducted to study the effects of kinetic parameters and operation conditions on reaction conversions.
Article
Chemistry, Applied
Juan Garcia-Serna, Raul Pinero-Hernanz, Desiree Duran-Martin
Summary: This paper emphasizes the importance of catalysis in chemical processes, presenting twelve methodological best practices in catalyst design and conception, along with application examples.
Article
Engineering, Chemical
German Araujo Barahona, Kari Eranen, Dmitry Murzin, Juan Garcia Serna, Tapio Salmi
Summary: This study demonstrates the capability of ruthenium-based solid foam catalysts in the hydrogenation of monomeric sugars. The research proposes reaction mechanisms and kinetic models based on plausible surface reactions, providing a new approach for the selective hydrogenation of various sugars to sugar alcohols.
CHEMICAL ENGINEERING SCIENCE
(2022)
Article
Chemistry, Physical
Atte Aho, Narendra Kumar, Kari Eranen, Paivi Maki-Arvela, Tapio Salmi, Markus Peurla, Ilari Angervo, Jukka Hietala, Dmitry Yu. Murzin
Summary: Methyl levulinate was selectively formed from glucose and methanol over a copper modified Beta zeolite bifunctional catalyst at 180 degrees C under argon atmosphere. The copper modification significantly changed the distribution of acid sites on the zeolite, leading to higher selectivity towards methyl levulinate. Metal modification of Beta zeolite with Sn and Zn did not perform as well as Cu in the formation of methyl levulinate during glucose transformation.
REACTION KINETICS MECHANISMS AND CATALYSIS
(2022)
Article
Engineering, Chemical
Ananias Medina, Javier Ibanez, Pasi Tolvanen, Cesar de Araujo Filho, Tapio Salmi
Summary: Recent studies have provided new information on glycerol hydrochlorination in the presence of carboxylic acids as homogeneous catalysts, showing that a portion of the carboxylic acid is esterified in some steps of the reaction mechanism. Inspired by this observation and the previously proposed mechanism for glycerol hydrochlorination, new kinetic equations were derived. These equations take into account the fraction of catalyst present in the form of esters and epoxides, explaining the initial zero-order kinetics with respect to glycerol.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2022)
Article
Engineering, Chemical
Wilhelm Wikstrom, Adriana Freites Aguilera, Pasi Tolvanen, Robert Lassfolk, Ananias Medina, Kari Eranen, Tapio Salmi
Summary: Biolubricants, plasticizers, bio-based rigid foams, and non-isocyanate polyurethanes can be produced in a green way from epoxidized fatty acids. The direct epoxidation of fatty acids in the presence of an immobilized enzyme allows for high conversion and low concentration of byproducts. The use of semibatch operation results in improved product yield.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2023)
Article
Biochemistry & Molecular Biology
Izabela Kurzydym, Alberto Garbujo, Pierdomenico Biasi, Izabela Czekaj
Summary: Transition-metal-modified zeolites have attracted great interest among scientists recently. Ab initio calculations based on density functional theory were conducted using the Perdew-Burke-Ernzerhof (PBE) functional for exchange and correlation. Cluster models of ZSM-5 zeolites with adsorbed Fe particles on aluminum were used. The adsorption of three iron adsorbates (Fe, FeO, and FeOH) within the pores of the zeolite was investigated with different aluminum arrangements. The analysis of DOS diagram and molecular orbitals revealed the insulating or conducting nature of the systems, which significantly affects their catalytic activity.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2023)
Article
Chemistry, Multidisciplinary
Maryam Hmoudah, Michele Emanuele Fortunato, Rosanna Paparo, Marco Trifuoggi, Amjad El-Qanni, Riccardo Tesser, Dmitry Yu. Murzin, Tapio Salmi, Vincenzo Russo, Martino Di Serio
Summary: The adsorption efficiency of commercial activated carbon toward ibuprofen (IBU) was studied using the adsorption dynamic intraparticle model (ADIM). A realistic model was proposed to quantitatively describe the influence of operation parameters on adsorption kinetics and thermodynamics. Thermodynamic data was successfully interpreted with the Freundlich isotherm, revealing an endothermic adsorption mechanism. The system was dominated by intraparticle diffusion and the obtained parameters will be used for process scaling by designing adsorption columns.
Article
Chemistry, Multidisciplinary
Matias Alvear, Marie-Louis Reich, Kari Era''nen, Stefan Haase, Dmitry Yu. Murzin, Tapio Salmi
Summary: Epoxidation of butane isomers (1-butene and isobutene) on a commercial titanium silicate catalyst (TS-1) was studied in a trickle bed reactor using the transient step response technique. The study revealed different dynamics of product formation between the isomers. The molecular structure of the isomers impacted both the transient and stationary states of the system, with 1-butene displaying a dynamic behavior and isobutene behaving similarly to ethene and propene.
Article
Engineering, Environmental
Marta Ramos-Andres, Sergio Diaz-Cesteros, Natasha Majithia, Juan Garcia-Serna
Summary: This research successfully extracted hemicellulose and pectin biopolymers of different molecular weights from discarded carrots, and purified and separated them using techniques like ultrafiltration and diafiltration, making them suitable for producing biodegradable films and other products.
CHEMICAL ENGINEERING JOURNAL
(2022)
