Article
Chemistry, Multidisciplinary
Sebastian Hoethker, Regine Mika, Harie Goli, Andreas Gansaeuer
Summary: We have developed a highly diastereo- and enantioselective two-step anti-Markovnikov addition of H2O to diastereomeric mixtures of trisubstituted olefins. Our method avoids the need for difficult separations by utilizing both diastereomeric olefins simultaneously in an organocatalytic syn-specific Shi-epoxidation, resulting in diastereomeric oxiranes. The observed converging behavior can be attributed to a HAT-preceding directional isomerization step, ultimately leading to high to excellent enantiomeric ratios of the final secondary alcohols.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Review
Chemistry, Physical
Ekaterina V. Pokochueva, Dudari B. Burueva, Oleg G. Salnikov, Igor V. Koptyug
Summary: HET-PHIP has attracted significant research attention in recent years, showing major prospects for applications in biomedical MRI and industrial catalytic studies, despite the current need for further improvement in NMR signal enhancements.
Article
Biology
Wayne Mitchell, Jeffrey D. Tamucci, Emery L. Ng, Shaoyi Liu, Alexander Birk, Hazel H. Szeto, Eric R. May, Andrei T. Alexandrescu, Nathan N. Alder
Summary: Mitochondria play a key role in metabolic homeostasis and their dysfunction is associated with various diseases. This study analyzed the structure-activity relationship of tetrapeptide analogs with different aromatic side chain compositions and sequence registrations. The results showed that these analogs adopt compact reverse turn conformations when bound to membranes and exhibit differences in membrane interactions. The analogs had effects on membrane surface charge and were able to penetrate cells and target mitochondria without strict requirements for side chain composition or sequence register. The analog with tryptophan side chains showed the strongest impact on membrane properties and had the highest efficacy in cell culture studies.
Article
Chemistry, Physical
Alex J. Plajer, Charlotte K. Williams
Summary: Heteronuclear complexes exhibit high catalytic activity in ring opening copolymerizations. By studying a series of trinuclear complexes, it was found that certain catalysts show high activity for specific reactions, such as CHO/CO2 ROCOP and CHO/ PA copolymerization, allowing for controlled polyether block formation. These findings can guide future catalyst design and inspire other CO2 utilization processes.
Article
Multidisciplinary Sciences
Kristiane R. Torgeson, Michael W. Clarkson, Daniele Granata, Kresten Lindorff-Larsen, Rebecca Page, Wolfgang Peti
Summary: The study reveals that residues surrounding the active site of PTP1B promote dynamically coordinated chemical reactions necessary for its function. In addition, residues distant to the active site also exhibit distinct dynamics that are correlated with its catalytic activity, allowing for different catalytic rates in this enzyme family. These findings contribute to our understanding of how conserved dynamics drive enzymatic activity and offer insights into the identification of new regulatory elements.
Article
Chemistry, Physical
Kristian Knemeyer, Jan Dirk Epping, Frederik Ruether, Christian Schulz, Benjamin Frank, Philipp Mueller, Raoul Naumann d'Alnoncourt, Matthias Driess, Frank Rosowski
Summary: The application of atomic layer deposition (ALD) in synthesizing catalysts can reveal the relationships between catalyst performance and properties, which is crucial for studying catalytic conversion processes.
Article
Chemistry, Physical
Xiaonan Hu, Yang Ye, Wenbo Dong, Yichao Huang, Mingshan Zhu
Summary: The photocatalytic behaviors among ten kinds of organic contaminants and two heterojunction photocatalysts were comparatively investigated. The photocatalysts with abundant oxygen vacancies exhibited stronger absorption capacity towards light and weaker redox ability. A quantitative evaluation of structure-activity relationships among different organic contaminants and two photocatalysts were constructed.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2022)
Article
Thermodynamics
Xu Jiang, Jun Xu, Qichen He, Cong Wang, Long Jiang, Kai Xu, Yi Wang, Sheng Su, Song Hu, Zhenyi Du, Jun Xiang
Summary: A quantification method for chemical structural heterogeneity of coal using Raman mapping technique was proposed in this study, and the heterogeneous chemical structure of coal was investigated. The results showed that the distributions of the chemical structure were highly uneven. Furthermore, the effects of chemical structural heterogeneity on pyrolysis behaviors were studied, and it was found that the heterogeneity significantly influenced the pyrolysis mechanisms and reactivity.
Article
Chemistry, Analytical
Qiu-Yue Cheng, Ting Wang, Jun Hu, Hong-Yuan Chen, Jing-Juan Xu
Summary: Visible-light-mediated heterogeneous photocatalysis is a promising method for organic transformations. However, accurately detecting and identifying photogenerated species, especially short-lived radical intermediates, remains challenging. In this work, a hybrid ion emitter integrated with a pico-liter heterogeneous photocatalytic reactor was developed for the rapid identification of transient radical intermediates produced under visible-light irradiation. This novel coupling device provides a powerful tool for exploring complex heterogeneous photochemical processes and their ultrafast initial transformations.
ANALYTICAL CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Arianna Brandolese, David H. Lamparelli, Miquel A. . Pericas, Arjan W. Kleij
Summary: A commercially available Lipase B from Candida antarctica immobilized onto a macroporous support (Novozym 435) was used as a benign oxidant for the epoxidation of various biorenewable terpenes in the presence of H2O2. The epoxidation protocol was explored under both heterogeneous batch and continuous flow conditions. The catalyst showed good recyclability under batch conditions for 10 cycles and could be used for more than 30 hours under continuous flow operation. This sustainable flow epoxidation allows for the production of gram quantities of terpene epoxides and the post-functionalization of biobased polymers.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2023)
Article
Chemistry, Multidisciplinary
Jinn-Kye Lee, Shuyang Wu, Pei Chong Lim, Zhengyang Zhang
Summary: This study presents a facile approach to visualize the in situ formation of copper and oxygen vacancies on the surface of Cu2O under ambient condition. The results reveal significant heterogeneity in the rate of defect formation at different facets, and the location of defect formation changes during the photocorrosion process.
Article
Spectroscopy
Polina Skvortsova, Yuliya Valiullina, Natalia Baranova, Dzhigangir Faizullin, Yuriy Zuev, Elena Ermakova
Summary: Amphibians are a natural source of a variety of peptides with functional activities, which can be characterized using a complex of spectroscopic methods. The structure and functional activity of megin-1, a peptide isolated from amphibian skin, were studied using NMR, FTIR, CD, and UV-spectroscopy. Thermodynamic characteristics of peptide transformation and its antibacterial, antimycotic, and protease inhibitory activities were analyzed.
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
(2022)
Article
Chemistry, Applied
Guojun Lv, Yan Chen, Xuyang Zou, Jiangzhang Wang, Tao Wang, Fumin Wang, Xubin Zhang
Summary: In this study, vanadium-titanium doped MFI zeolite was synthesized and its synergistic catalytic effect in the epoxidation of 1-hexene and cyclohexene was investigated. The simultaneous incorporation of vanadium and titanium induced the partial charge transformation of titanium (IV) into titanium (III), leading to improved catalytic performance. Additionally, the dual insertion of vanadium and titanium increased the number of Lewis acid sites and external surface area, further enhancing the synergistic catalytic effect. The prepared VTS(0.15) zeolite exhibited high catalytic activity and good reusability.
MICROPOROUS AND MESOPOROUS MATERIALS
(2022)
Review
Chemistry, Physical
Mona Abdelgaid, Giannis Mpourmpakis
Summary: This article discusses the importance of heterogeneous catalysts in industrial chemical transformations, with a focus on metal oxides as catalysts and the application of computational chemistry in catalyst discovery. Through structure-activity relationships, promising catalytic materials can be rapidly predicted to guide experimental research. The article also provides detailed insights into the applications of oxides in industrial reactions such as methane activation and conversion, alkane dehydrogenation, and alcohol dehydration.
Article
Chemistry, Inorganic & Nuclear
Rupam Sen, Sudipta De, Antonio M. dos Santos, Livia B. L. Escobar, Paula Cristina Brandao, Filipe A. Almeida A. Paz, Mario S. Reis, Zhi Lin
Summary: A novel triazole bridged cobalt fluorophosphate coordination polymer has been synthesized and characterized. The compound consists of Co-5 clusters that build the whole framework, with all cobalt centers in octahedral geometry. The compound shows antiferromagnetic interactions among the Co(II) ions and exhibits high catalytic activity in the conversion of olefins to their corresponding epoxides, with a selectivity of up to 65% and high TON numbers.
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Vitaly L. Sushkevich, Rene Verel, Jeroen A. van Bokhoven
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2020)
Article
Chemistry, Physical
Vladimir Paunovic, Sharon Mitchell, Rene Verel, Sung Sik Lee, Javier Perez-Ramirez
JOURNAL OF PHYSICAL CHEMISTRY C
(2020)
Article
Chemistry, Physical
Manouchehr Nadjafi, Paula M. Abdala, Rene Verel, Davood Hosseini, Olga Safonova, Alexey Fedorov, Christoph R. Mueller
Article
Chemistry, Multidisciplinary
Laura Piveteau, Marcel Aebli, Nuri Yazdani, Marthe Millen, Lukas Korosec, Franziska Krieg, Bogdan M. Benin, Viktoriia Morad, Christophe Piveteau, Toni Shiroka, Aleix Comas-Vives, Christophe Coperet, Aaron M. Lindenberg, Vanessa Wood, Rene Verel, Maksym Kovalenko
ACS CENTRAL SCIENCE
(2020)
Article
Chemistry, Physical
Pedro Castro-Fernandez, Maria Blanco, Rene Verel, Elena Willinger, Alexey Fedorov, Paula M. Abdala, Christoph R. Mueller
JOURNAL OF PHYSICAL CHEMISTRY C
(2020)
Article
Chemistry, Multidisciplinary
Pascal Jurt, Anne Sofie Abels, Juan Jose Gamboa-Carballo, Israel Fernandez, Gregoire Le Corre, Marcel Aebli, Matthew G. Baker, Frederik Eiler, Fabian Mueller, Michael Worle, Rene Verel, Sebastien Gauthier, Monica Trincado, Thomas L. Gianetti, Hansjorg Grutzmacher
Summary: A bimetallic Rh-I-Pt-II complex with a specially designed multidentate phosphine olefin ligand can catalytically detoxify nitrogen oxides, forming water and N-2 as benign products at room temperature. Investigation into the conversion process revealed the generation of a hyponitrite (N2O22-) complex as an intermediate, shedding light on a possible reaction mechanism.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
Manouchehr Nadjafi, Agnieszka M. Kierzkowska, Andac Armutlulu, Rene Verel, Alexey Fedorov, Paula M. Abdala, Christoph R. Mueller
Summary: In this study, the catalytic activity for propane dehydrogenation (PDH) of Zn-based Al2O3 catalysts was correlated with their structure and structural evolution. Four-tetrahedral Zn sites near Al sites in the zinc aluminate spinel phase were found to be more active and selective in PDH compared to the supported ZnO wurtzite phase. ZnO/Al2O3 catalyst exhibited 77% selectivity to propene, but experienced irreversible activity loss due to Zn depletion on the surface after repeated PDH and air-regeneration cycles.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Soil Science
Timothy McLaren, Rene Verel, Emmanuel Frossard
Summary: In this study, the composition of soil organic phosphorus (Po) was examined using solution P-31 nuclear magnetic resonance (NMR) spectroscopy. The results showed that soil phosphomonoesters in large molecular weight fractions consist of multiple components with varying linewidth.
SOIL SCIENCE SOCIETY OF AMERICA JOURNAL
(2022)
Article
Chemistry, Physical
Mikalai A. Artsiusheuski, Rene Verel, Jeroen A. van Bokhoven, Vitaly L. Sushkevich
Summary: Direct methane conversion to methanol via chemical looping using copper-exchanged zeolites is a highly researched area, where different zeolite topologies and copper species structures can influence the nature of reaction products. The structure of copper active sites in zeolites strongly determines the type and relative fraction of formed products, leading to opportunities for tuning material properties for optimal performance. Multiple pathways of methane transformation over copper-exchanged zeolites have been identified, showing potential for further development in this field.
Article
Soil Science
Jolanda E. Reusser, Federica Tamburini, Andrew L. Neal, Rene Verel, Emmanuel Frossard
Summary: This study elucidates the chemical nature of increasing molecular size organic phosphorus (Porg) in soil extracts using gel-filtration size exclusion chromatography (SEC) and solution 31P nuclear magnetic resonance (NMR) spectroscopy. The results show that organic P is present across the entire molecular size range and comprises multiple components of varying NMR peak line width. Additionally, the stabilisation of inositol hexakisphosphates (IP6) in soils is associated with the organic phase.
Article
Chemistry, Multidisciplinary
Alexander V. Yakimov, Manoj Ravi, Rene Verel, Vitaly L. Sushkevich, Jeroen A. van Bokhoven, Christophe Coperet
Summary: This study investigates the structures of Brosted acid sites and Lewis acid sites in Zeolite and their interactions with pyridine using NMR spectroscopy and DFT modeling. The study reveals the temperature-dependent variations of the structures and emphasizes the importance of considering temperature effects in obtaining accurate structural assessments.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Multidisciplinary Sciences
Daniil Salionov, Olesya O. Semivrazhskaya, Nicola P. M. Casati, Marco Ranocchiari, Sasa Bjelic, Rene Verel, Jeroen A. van Bokhoven, Vitaly L. Sushkevich
Summary: Metal-organic frameworks (MOFs) with their vast structural and chemical diversity hold great potential for designing materials with tailored properties. However, the synthesis of MOFs remains challenging due to a lack of understanding of their formation mechanisms. This study presents a detailed molecular-level mechanism for the formation of MIL-53(Al), shedding light on the complexity of MOF crystallization chemistry.
NATURE COMMUNICATIONS
(2022)
Article
Soil Science
Jolanda E. Reusser, Alessandro Piccolo, Giovanni Vinci, Claudia Savarese, Silvana Cangemi, Vincenza Cozzolino, Rene Verel, Emmanuel Frossard, Timothy I. McLaren
Summary: We investigated the composition of organic phosphorus (Porg) in different soil organic matter (SOM) fractions using sequential chemical fractionation (SCF) procedure combined with nuclear magnetic resonance (NMR) spectroscopy. The SCF procedure extracted a higher amount of Porg compared to a single-step extraction. Approximately 38% of the extracted Porg was in the form of unresolved Porg pool, represented by broad signals in the phosphomonoester region of NMR spectra. The SCF revealed the recovery of phosphomonoesters in different SOM fractions, with a portion closely associated with the soil mineral phase. The extractability of inositol phosphates (IP) was also increased using the SCF procedure.
Article
Chemistry, Inorganic & Nuclear
Anne Sofie Abels, Frederik Eiler, Gregoire Le Corre, Pascal Jurt, Michael Worle, Rene Verel, Zoltan Benko, Hansjorg Grutzmacher
Summary: A series of stable group 6 metal complexes with 2,4,6-oxy functionalised 1,3,5-triphosphinines as ligands were synthesized, resulting in the formation of [M{P3C3(OX)(3)}(CO)(3)] compounds (M = Cr(0), Mo(0), W(0); X = H, SitBuPh(2), B(ipc)(2)]. The triphosphinines coordinate in an eta(6)-binding mode via the 6 pi-system of the ring. The ligand properties can be tuned by changing the substituent on the oxygen centre, and the order of pi-electron accepting properties is P3C3(OH)(3) < P3C3((OSiBuPh2)-Bu-t)(3) < P3C3(OB(ipc)(2))(3).
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Physical
Antonio J. Martin, Florentine L. P. Veenstra, James Luthi, Rene Verel, Javier Perez-Ramirez
Summary: Nitrogen electroreduction shows potential in reducing fossil energy requirements for fertilizer production, but efficient catalysts are still needed. This article introduces guidelines for using UV-vis spectroscopy and ion-selective electrodes for initial catalyst screening, highlighting the importance of 1H-NMR for confirming the catalytic origin of ammonia. The study also presents a protocol for making 1H-NMR quantification more accessible, allowing for qualitative and quantitative analyses in a timely manner.
