Article
Chemistry, Organic
Sadhanendu Samanta, Jin Cui, Hidetoshi Noda, Takumi Watanabe, Masakatsu Shibasaki
Summary: In this study, a gram-scale syn-selective asymmetric vinylogous addition of butenolides to chromones was developed using an Al-Li-BINOL (ALB) complex catalyst. The reaction showed high diastereoselectivity with ratios up to 20:1 and enantioselectivity of 84-98% for various substrate combinations. This method is complementary to previous reports and improves selectivity for several chromones. Computational studies support the role of ALB as a bifunctional catalyst in this reaction and provide insights into the origin of the observed stereoselectivity.
JOURNAL OF ORGANIC CHEMISTRY
(2023)
Article
Chemistry, Organic
Sadhanendu Samanta, Jin Cui, Hidetoshi Noda, Takumi Watanabe, Masakatsu Shibasaki
Summary: A gram-scale syn-selective asymmetric vinylogous addition of butenolides to chromones, catalyzed by an Al-Li-BINOL (ALB) complex, was developed in this study. The diastereoselectivity reached 20:1 with 84-98% ee for various combinations of substrates. This protocol complements previous methods and improves selectivity for multiple chromones.
JOURNAL OF ORGANIC CHEMISTRY
(2023)
Article
Biochemical Research Methods
Laura Rolinger, Juergen Hubbuch, Matthias Ruedt
Summary: Monitoring the protein concentration and buffer composition during UF/DF step is crucial for biopharmaceutical production automation and real-time release testing. This study demonstrates the advantages of combining Raman spectroscopy with EKF for monitoring the UF/DF step, showing improved sensitivity and faster measurement speed.
ANALYTICAL AND BIOANALYTICAL CHEMISTRY
(2023)
Article
Engineering, Chemical
Mais Al-Attili, Carla Ferreira, Chris Price, Karen Faulds, Yi-Chieh Chen
Summary: Spatially offset Raman spectroscopy (SORS) is a subset of Raman spectroscopy used for probing subsurface compositions in non-homogenous media. In this study, a SORS probe was developed for the monitoring of pharmaceutical drying. The results showed that SORS could offer improved monitoring of pharmaceutical drying processes.
CHEMICAL ENGINEERING RESEARCH & DESIGN
(2023)
Article
Chemistry, Applied
Yuma Miyai, Anna Formosa, Cameron Armstrong, Brian Marquardt, Luke Rogers, Thomas Roper
Summary: This study discusses the implementation of PAT for real-time monitoring of intermediate and product concentrations on the PoD system, achieving a RMSEP of 2.2 mg/mL with a relative error of 2.8% for the step 2 FlowIR model and a RMSEP of 0.9 mg/mL with a relative error of 2.8% for the step 5 Raman model. These models were successfully deployed during continuous ciprofloxacin synthesis on the PoD system, demonstrating the capability of real-time prediction using PAT technology.
ORGANIC PROCESS RESEARCH & DEVELOPMENT
(2021)
Article
Biochemistry & Molecular Biology
Jessie Payne, James Cronin, Manjit Haer, Jason Krouse, William Prosperi, Katherine Drolet-Vives, Matthew Lieve, Michael Soika, Matthew Balmer, Marina Kirkitadz
Summary: The study demonstrated the suitability of in-line infrared measurements to monitor surfactant concentration in the viral vaccine drug substance during exchanges 8-15 of a 50KDa tangential flow filtration process. The preliminary multivariate model used in this work can be further optimized for manufacturing scale in-line use.
COMPUTATIONAL AND STRUCTURAL BIOTECHNOLOGY JOURNAL
(2021)
Article
Chemistry, Analytical
Lewellwyn J. Coates, Andrew Gooley, Shing Chung Lam, Boyjie Firme, Paul R. Haddad, Hans-Jurgen Wirth, Angel Diaz, Frank Riley, Brett Paull
Summary: Due to their size, conventional high performance liquid chromatographs (HPLCs) are difficult to place close to a reaction vessel within a pharmaceutical manufacturing or development site. However, a compact and modular separation system using capillary HPLC has been developed to enable co-location of an HPLC with a small-scale reactor for reaction monitoring. The compact system showed equivalent quantitative performance to an Agilent 1290 Infinity II HPLC system.
ANALYTICA CHIMICA ACTA
(2023)
Article
Chemistry, Analytical
Yujing Zuo, Zhiming Gou, Minggang Tian, Jingting Zhan, Weiying Lin
Summary: Rapid response is an important goal in fluorescence analysis technology, but it is often uncontrollable due to the limitations of the response mechanism and detection targets. In this study, a novel catalyst PNL-Br was synthesized and successfully incorporated into fluorescence analysis, showing a higher catalytic potential in thiol-Michael addition reactions. Notably, PNL-Br was an efficient catalyst for dithiothreitol (DTT) detection by fluorescence analysis, which was the first example of a catalysis system for fluorescent probe detection reactions.
SENSORS AND ACTUATORS B-CHEMICAL
(2023)
Article
Chemistry, Applied
Haifeng Yu, Jian Mo, Xuemin Niu, Dashuang Luo, Guangbo Che
Summary: Switchable synthesis of 3-alkenyl succinimides and maleimides was achieved by adjusting reaction conditions. The Michael addition reaction of alpha-oxo ketene dithioacetals and maleimides using CH3SO3H in DCE at 120 degrees C resulted in 40-90% yields of 3-alkenyl succinimides. The oxidative cross-coupling reaction of alpha-oxo ketene dithioacetals with maleimides using Pd(OAc)(2) in DMF at 20 degrees C yielded 40-80% yields of 3-alkenyl maleimides. The method can be scaled up to gram scale without the need for directing groups on the substrates.
ADVANCED SYNTHESIS & CATALYSIS
(2023)
Article
Automation & Control Systems
Michel Thiel, Nicolas Sauwen, Tastiana Khamiakova, Tor Maes, Bernadette Govaerts
Summary: This paper introduces a practical framework based on different dimension-reduction and calibration methods for tracking chemical experiments organized in batches, aiming to visualize and interpret chemical reaction kinetics in real time or off-line, and predict chemical component concentrations over time. Results show that NMF and MCR provide better interpretability for chemical reactions compared to PCA, and unsupervised methods such as PCA, NMF or MCR can be used to predict concentrations of chemical compounds continuously with good precision and interpretability.
CHEMOMETRICS AND INTELLIGENT LABORATORY SYSTEMS
(2021)
Article
Chemistry, Organic
Huangdi Feng, Futao Peng, Hui Xi, Ling Zhong, Liliang Huang
Summary: The study presents a simple method for synthesizing propargylamines, with high yields achieved by controlling the loading of amines to increase selectivity.
ASIAN JOURNAL OF ORGANIC CHEMISTRY
(2021)
Article
Chemistry, Physical
Meirong Zeng, Chen-Lin Liu, Kevin R. Wilson
Summary: During the examination of the reaction between chlorine atoms and alkenes in the presence of Cl-2, we observed a significant increase in reactivity and the dominance of chlorinated reaction products, even under high O-2 conditions. These findings suggest a multiphase catalytic coupling between free radical oxidation and electrophilic Cl-2 addition, with the production of oxygenated reaction intermediates acting as gas-liquid phase-transfer catalysts (gl-PTCs) to enhance electrophilic addition. This work demonstrates the importance of reimagining multiphase reaction schemes of aerosols for understanding catalytic reaction mechanisms.
JOURNAL OF PHYSICAL CHEMISTRY A
(2022)
Article
Chemistry, Applied
Hamidulla B. Tukhtaev, Stanislav I. Bezzubov, Elena A. Tarasenko, Mikhail Ya. Melnikov, Konstantin L. Ivanov, Ekaterina M. Budynina
Summary: A new method was developed for the design of diastereodivergent approach to phosphazenopyrrolines by switching step order within a cascade process. The strategy relies on the multifaceted roles of phosphazene intermediates in cascade transformation, providing a stereodivergent route to synthesize biorelevant compounds with different stereoisomers.
ADVANCED SYNTHESIS & CATALYSIS
(2021)
Article
Biotechnology & Applied Microbiology
David Heinrich Mueller, Carsten Flake, Thorsten Brands, Hans-Juergen Koss
Summary: In order to improve the productivity and quality of bioprocess, it is important to monitor critical process parameters in real time. Raman spectroscopy is a commonly used PAT tool for in-situ and non-invasive monitoring of substrate, metabolite, and product concentrations. However, robust statistical modeling is required for evaluation of the bioprocess Raman spectra. In this study, we successfully demonstrated that Indirect Hard Modeling (IHM) is an alternative approach to statistical models with significantly lower calibration effort for monitoring a glucose to ethanol fermentation process using Raman spectroscopy.
BIOTECHNOLOGY AND BIOENGINEERING
(2023)
Article
Chemistry, Organic
Michal Kopyt, Michal Tryniszewski, Michal Barbasiewicz, Piotr Kwiatkowski
Summary: Enantioselective Michael addition under high-pressure conditions is an efficient method to synthesize chiral cyclohexanes.
Review
Chemistry, Applied
Qingyue Wang, King Lun Yeung, Miguel A. Banares
Review
Chemistry, Applied
Li Chen Kao, Wen Chen Kan, Rosa Maria Martin-Aranda, Maria Olga Guerrero-Perez, Miguel A. Banares, Sofia Ya Hsuan Liou
Article
Chemistry, Physical
Yuxin Li, Wei Han, Ruixuan Wang, Lu-Tao Weng, Ana Serrano-Lotina, Miguel A. Banares, Qingyue Wang, King Lun Yeung
APPLIED CATALYSIS B-ENVIRONMENTAL
(2020)
Article
Engineering, Chemical
M. Olga Guerrero-Perez, Gregory S. Patience, Miguel A. Banares
Summary: Raman scattering is an inelastic interaction that exchanges energy in the region of molecular vibrational transitions, highly sensitive to nanocrystals. With the advent of powerful lasers in the 1970s, Raman technology began to be routinely applied in research.
CANADIAN JOURNAL OF CHEMICAL ENGINEERING
(2021)
Article
Chemistry, Multidisciplinary
Qingyue Wang, Yuxin Li, Ana Serrano-Lotina, Wei Han, Raquel Portela, Ruixuan Wang, Miguel A. Banares, King Lun Yeung
Summary: A unique 1D nanostructure of Pt@CeO2-BDC was prepared for toluene oxidation, facilitating the stepwise oxidation of toluene to CO2 and H2O. The presence of Pt clusters on the catalyst surface promoted the adsorption of toluene and reaction activation.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Editorial Material
Chemistry, Multidisciplinary
Iseult Lynch, Antreas Afantitis, Dario Greco, Maria Dusinska, Miguel A. Banares, Georgia Melagraki
Article
Chemistry, Applied
J. J. Ternero-Hidalgo, M. Daturi, G. Clet, P. Bazin, M. A. Banares, R. Portela, M. O. Guerrero-Perez, J. Rodriguez-Mirasol, T. Cordero
Summary: Simultaneous operando Raman and transmission FTIR spectroscopic measurements were used to study the structure-activity relationships of V-Zr-O catalysts during propane oxidative dehydrogenation. The combination of both spectroscopies allowed the identification of reaction intermediates and provided structural information about the catalyst. The results suggested a Mars-van Krevelen mechanism and showed higher activity of bridging oxygen sites than terminal V--O bonds.
Article
Chemistry, Physical
Carlos A. Ortiz-Bravo, Santiago J. A. Figueroa, Raquel Portela, Carlos A. Chagas, Miguel A. Banares, Fabio Souza Toniolo
Summary: The performance of the Mn-Na2WO4/SiO2 catalyst for oxidative coupling of methane (OCM) has been attributed to crystalline phases that are not present at reaction temperatures. The evolution of W and Mn sites structure was monitored, showing phase transitions and changes in bond order with temperature. Steady-state experiments demonstrated that Mn3+ sites are more active in methane activation.
JOURNAL OF CATALYSIS
(2022)
Article
Chemistry, Physical
Maria Victoria Toledo, Carla Jose, Carlos R. Llerena Suster, Sebastian E. Collins, Raquel Portela, Miguel A. Banares, Laura E. Briand
Summary: In this study, the esterification of rac-ibuprofen and rac-ketoprofen with glycerol using Novozym(R) 435 as the catalyst was investigated, showing different conversion rates and selectivities under various molar ratios. Molecular level analysis confirmed the reaction progress, and the interaction between CALB and ibuprofen was found to impact the structure of the lipase, potentially improving catalytic performance.
MOLECULAR CATALYSIS
(2021)
Article
Multidisciplinary Sciences
Alba Tamargo, Natalia Molinero, Julian J. Reinosa, Victor Alcolea-Rodriguez, Raquel Portela, Miguel A. Banares, Jose F. Fernandez, M. Victoria Moreno-Arribas
Summary: Microplastics are a recognized global problem due to their presence in natural environments and the food chain. This study found that microplastics not only have an impact on human microbiota, but also undergo biotransformation in the gastrointestinal tract. The researchers observed that microplastics alter the composition of the human colonic microbial community, and hypothesized that some members of the microbiota adhere to the surface of microplastics, promoting the formation of biofilms. Considering the increasing exposure to microplastics in consumer products, it is important to investigate the effects of plastics on gut microbiome functionality and their potential degradation by intestinal bacteria.
SCIENTIFIC REPORTS
(2022)
Review
Instruments & Instrumentation
Afroditi Ntziouni, James Thomson, Ioannis Xiarchos, Xiang Li, Miguel A. Banares, Costas Charitidis, Raquel Portela, Enrique Lozano Diz
Summary: This review analyzes the standards, guides, and practices related to Raman spectroscopy. The standardization work is mainly dominated by American institutions, with the pharmaceutical industry being the major user of Raman spectroscopy. However, the current standardization landscape is incomplete and needs to be modernized according to recent technological advancements. Active involvement from the Raman community is crucial for this modernization process.
APPLIED SPECTROSCOPY
(2022)
Review
Chemistry, Multidisciplinary
Houeida Issa Hamoud, Lukasz Wolski, Ilia Pankin, Miguel A. Banares, Marco Daturi, Mohamad El-Roz
Summary: This article discusses the identification and quantification methods of the steps involved in photocatalysis, as well as the use of in situ/operando techniques to study reactant activation/conversion and mass transfer. The application of these techniques helps to better understand the mechanism of photocatalysis and improve reaction efficiency and catalyst design.
TOPICS IN CURRENT CHEMISTRY
(2022)
Review
Nanoscience & Nanotechnology
Ewelina Wyrzykowska, Alicja Mikolajczyk, Iseult Lynch, Nina Jeliazkova, Nikolay Kochev, Haralambos Sarimveis, Philip Doganis, Pantelis Karatzas, Antreas Afantitis, Georgia Melagraki, Angela Serra, Dario Greco, Julia Subbotina, Vladimir Lobaskin, Miguel A. Banares, Eugenia Valsami-Jones, Karolina Jagiello, Tomasz Puzyn
Summary: This Review discusses the importance of a comprehensive system for defining nanomaterial descriptors in enabling a safe-and-sustainable-by-design concept for engineered nanomaterials. The unique nanoscale properties of engineered nanomaterials can pose risks to human health and the environment, making it crucial to design new nanomaterials with safety and sustainability in mind. Physicochemical characteristics, such as chemical composition and size, play a key role in the biological activity of nanomaterials, and nanodescriptors can be used to optimize their functionality and minimize health and environmental hazards. The successful integration of experimental data and computational models is essential for the safe adoption of nanomaterials on a large scale.
NATURE NANOTECHNOLOGY
(2022)
Article
Chemistry, Physical
Ana Serrano-Lotina, Karen Cruz, Miguel A. Banares, Marco Daturi, Pedro Avila
Summary: Bimetallic shaped catalysts were prepared by wet equilibrium impregnation, where MnO2 was the main component and a second metal oxide (Co, Fe and Ce oxides) was added. The Ce-promoted catalyst showed the highest catalytic activity in the selective reduction of NOx with NH3 (88% NO conversion at 170 degrees C) due to its ability to adsorb NOx even in the presence of water. However, the Fe-promoted catalyst exhibited lower NOx conversion with NH3-SCR in the presence of water (65% NO conversion at 170 degrees C) due to the absence of NOx adsorbed species.
APPLIED SURFACE SCIENCE
(2023)
Article
Chemistry, Applied
M. Olga Guerrero-Perez, Olga B. Lapina, Soren B. Rasmussen, Miguel A. Banares
Summary: Nanoscaled-VPO catalysts were prepared on an alumina support to achieve high surface-to-volume ratio of the active phase. Surface species transformations were studied using these nanoscaled catalysts, with minimized signal from the bulk. The chemical environment and oxidation state of the species were determined by NMR, ESR, and XANES spectroscopies. The results optimized V + P coverage and V/P molar ratio to minimize isolated vanadium oxide species and maximize V4+ concentration. The distribution of phosphorus islands greatly influenced the structure of the catalytic material for the desired partial oxidation reaction.
TOPICS IN CATALYSIS
(2023)
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.
