Chemistry methods : new approaches to solving problems in chemistry最新文献

Cover Picture: Analysis of Macromolecular Size Distributions in Concentrated Solutions (Chem. Methods 12/2024)

IF 6.1

Chemistry methods : new approaches to solving problems in chemistry Pub Date : 2024-12-11 DOI: 10.1002/cmtd.202481201

Dr. Sumit K. Chaturvedi, Dr. Peter Schuck

引用次数: 0

In situ X-Ray Powder Diffraction Investigation on the Development of Zeolite-Templated Carbons in FAU Zeolite 关于 FAU 沸石中沸石模板碳发展的原位 X 射线粉末衍射研究

IF 6.1

Chemistry methods : new approaches to solving problems in chemistry Pub Date : 2024-11-15 DOI: 10.1002/cmtd.202400018

Dr. Thibaud Aumond, Dr. Martin Esteves, Dr. Cristian Mocuta, Dr. Isabelle Batonneau-Gener, Dr. Julien Haines, Dr. Ricardo Faccio, Dr. Alexander Sachse

{"title":"In situ X-Ray Powder Diffraction Investigation on the Development of Zeolite-Templated Carbons in FAU Zeolite","authors":"Dr. Thibaud Aumond, Dr. Martin Esteves, Dr. Cristian Mocuta, Dr. Isabelle Batonneau-Gener, Dr. Julien Haines, Dr. Ricardo Faccio, Dr. Alexander Sachse","doi":"10.1002/cmtd.202400018","DOIUrl":"https://doi.org/10.1002/cmtd.202400018","url":null,"abstract":"A time resolved in situ X-ray powder diffraction study using synchrotron radiation allowed for describing the evolution of the zeolite FAU structure during the development of a zeolite-templated carbon (ZTC) in its porous voids. During the ZTC formation the intensity decrease of most zeolite reflections and the simultaneous rise in intensity of the 222 reflection (of null intensity in the pristine zeolite) was observed. Full pattern profile fitting by Rietveld refinement allowed for achieving a detailed description of the underlying chemistry, with coincident pore filling with carbon atoms in specific positions and framework distortion. Monitoring the intensity profiles of the 222 reflection allowed assessment of the energetics of the ZTC formation. Our results contribute to a better understanding of the phenomena involved on the atomic scale in ZTC synthesis.","PeriodicalId":72562,"journal":{"name":"Chemistry methods : new approaches to solving problems in chemistry","volume":"4 12","pages":""},"PeriodicalIF":6.1,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cmtd.202400018","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142861565","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Towards Precision Biocatalysis – Leveraging Inline NMR for Autonomous Experimentation in Flow Reactors

IF 6.1

Chemistry methods : new approaches to solving problems in chemistry Pub Date : 2024-11-15 DOI: 10.1002/cmtd.202400049

Felix Ott, Dr. Gudrun Gygli, Dr. Kersten S. Rabe, Prof. Dr. Christof M. Niemeyer

{"title":"Towards Precision Biocatalysis – Leveraging Inline NMR for Autonomous Experimentation in Flow Reactors","authors":"Felix Ott, Dr. Gudrun Gygli, Dr. Kersten S. Rabe, Prof. Dr. Christof M. Niemeyer","doi":"10.1002/cmtd.202400049","DOIUrl":"https://doi.org/10.1002/cmtd.202400049","url":null,"abstract":"Reactor automation is a transformative force for chemical processes, but the potential of reaction monitoring for machine-assisted autonomous biocatalytic reaction optimization is still largely unexplored. To address this gap, we report on automated reactor optimization for biocatalytic flow-through microreactors. For this purpose, the inline NMR analysis of an enzymatically catalyzed stereoselective reduction of a prochiral diketone was combined with a self-developed open-source analysis and control software. The algorithm is continuously fed with spectra from a benchtop NMR instrument acquired from a reaction solution from a microreactor filled with biocatalytically active materials and adjusts the flow rate of the pumps to achieve predetermined target concentrations of the product. We show that through this automated coupling of data analysis and process parameterization, for example, maximum conversion efficiency can be achieved for a given bioreactor. This work illustrates the potential of inline NMR reaction monitoring for biocatalytic processes and provides a starting point for innovation to develop automated processes for precision biocatalysis through integrated data analysis.","PeriodicalId":72562,"journal":{"name":"Chemistry methods : new approaches to solving problems in chemistry","volume":"4 12","pages":""},"PeriodicalIF":6.1,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cmtd.202400049","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142851338","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Analysis of Macromolecular Size Distributions in Concentrated Solutions

IF 6.1

Chemistry methods : new approaches to solving problems in chemistry Pub Date : 2024-11-12 DOI: 10.1002/cmtd.202400035

Dr. Sumit K. Chaturvedi, Dr. Peter Schuck

{"title":"Analysis of Macromolecular Size Distributions in Concentrated Solutions","authors":"Dr. Sumit K. Chaturvedi, Dr. Peter Schuck","doi":"10.1002/cmtd.202400035","DOIUrl":"https://doi.org/10.1002/cmtd.202400035","url":null,"abstract":"The solution state of macromolecules in concentrated solutions impacts fields ranging from cell biology, to colloid chemistry and engineering of protein pharmaceuticals. Dependent on the interplay between repulsive and weakly attractive forces, proteins may exhibit oligomerization, aggregation, crystallization, liquid-liquid phase separation, or the formation of multiprotein complexes. The particle size-distribution is a key characteristic, but difficult to determine when interparticle distances are on the order of their size and macromolecular motion is coupled through hydrodynamic interactions. Here we extend sedimentation velocity analytical ultracentrifugation to measure macromolecular size distributions under these conditions: We apply results from statistical fluid mechanics for the concentration-dependence of hindered settling and diffusion, embedded in a mean-field approximation that can resolve coupled sedimentation and diffusion processes of different sized species given experimental sedimentation data. This is combined with a description of transient optical aberrations from lensing in the refractive index gradients associated with sedimentation boundaries (Wiener skewing). We demonstrate this approach in the application to protein solutions with macromolecular volume fractions up to ≈10 %, for example, resolving monomers and dimers of albumin at 140 mg/ml. This enables size-distribution analysis of proteins at concentrations of therapeutic antibody formations and close to physiological concentration in serum and cells.","PeriodicalId":72562,"journal":{"name":"Chemistry methods : new approaches to solving problems in chemistry","volume":"4 12","pages":""},"PeriodicalIF":6.1,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cmtd.202400035","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142851468","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Cover Picture: Video Documented Upscaled Synthesis of Salts of the Parent Carbaborate Ion [CB11H12]−, its Undecafluorinated Form [CHB11F11]− and Useful Starting Materials for its Introduction (Chem. Methods 11/2024) 封面图片：通过视频记录硼酸根离子[CB11H12]-母体、其未十氟化形式[CHB11F11]-的盐类及其有用起始材料的放大合成（化学方法 11/2024）

IF 6.1

Chemistry methods : new approaches to solving problems in chemistry Pub Date : 2024-11-11 DOI: 10.1002/cmtd.202481101

Jan Kulenkampff, Christian Armbruster, Johanna Drolshagen, Celine Regnat, Tina Wienold, Luisa Spari, Jana Fix, Tabea Sterbak, Dr. Harald Scherer, Prof. Dr. Ingo Krossing

{"title":"Cover Picture: Video Documented Upscaled Synthesis of Salts of the Parent Carbaborate Ion [CB11H12]−, its Undecafluorinated Form [CHB11F11]− and Useful Starting Materials for its Introduction (Chem. Methods 11/2024)","authors":"Jan Kulenkampff, Christian Armbruster, Johanna Drolshagen, Celine Regnat, Tina Wienold, Luisa Spari, Jana Fix, Tabea Sterbak, Dr. Harald Scherer, Prof. Dr. Ingo Krossing","doi":"10.1002/cmtd.202481101","DOIUrl":"https://doi.org/10.1002/cmtd.202481101","url":null,"abstract":"The Front Cover shows the molecular structure of the undecafluorinated carbaborate anion [CHB11F11]−, as well as its precursor [CB11H12]− and the starting material [BH4]−. Detailed synthetic protocols for the synthesis of [CB11H12]− and [CHB11F11]− in large scales are provided by Ingo Krossing and co-workers in their Research Article. To facilitate the reproduction of the preparation of these compounds, the synthesis has been filmed and instructive videos are provided with the publication. Starting from the [CHB11F11]− anion, the authors tested its chemical properties and synthesized its trityl ([Ph3C]+) as well as its silver salt ([Ag(odfb)2]+) and used them for a representative hydrosilylation reaction, as well as the oxidation of ferrocene and the ‘magic blue’ amine N(4-C6H4Br)3. More information can be found in the Research Article by I. Krossing and co-workers (DOI: 10.1002/cmtd.202400011).\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture>\u0000 </div>\u0000 </figure>\u0000 ","PeriodicalId":72562,"journal":{"name":"Chemistry methods : new approaches to solving problems in chemistry","volume":"4 11","pages":""},"PeriodicalIF":6.1,"publicationDate":"2024-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cmtd.202481101","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142665965","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Direct Spectroscopic Confirmation of the Oxygen-Centered Diradical Character of the Tetraoxidorhenium(VII) Cation [Re(O)4]+

IF 6.1

Chemistry methods : new approaches to solving problems in chemistry Pub Date : 2024-10-25 DOI: 10.1002/cmtd.202400023

Mayara da Silva Santos, Dr. Robert Medel, Simon Kruse, Max Flach, Olesya S. Ablyasova, Martin Timm, Prof. Dr. Bernd von Issendorff, Dr. Konstantin Hirsch, Dr. Vicente Zamudio-Bayer, Prof. Dr. Sebastian Riedel, Prof. Dr. J. Tobias Lau

{"title":"Direct Spectroscopic Confirmation of the Oxygen-Centered Diradical Character of the Tetraoxidorhenium(VII) Cation [Re(O)4]+","authors":"Mayara da Silva Santos, Dr. Robert Medel, Simon Kruse, Max Flach, Olesya S. Ablyasova, Martin Timm, Prof. Dr. Bernd von Issendorff, Dr. Konstantin Hirsch, Dr. Vicente Zamudio-Bayer, Prof. Dr. Sebastian Riedel, Prof. Dr. J. Tobias Lau","doi":"10.1002/cmtd.202400023","DOIUrl":"https://doi.org/10.1002/cmtd.202400023","url":null,"abstract":"Mononuclear inorganic diradical species are scarce. Here, we confirm, via X-ray absorption spectroscopy in the gas phase combined with computational studies, the oxygen-centered diradical character of the tetraoxidorhenium(VII) cation. A dioxido-superoxido isomer, close in energy to the diradical, is also found, where rhenium appears in its rare oxidation state of +6. Addition of one or two hydrogen atoms to [Re,O4]+ forms hydroxido ligands, and strongly disfavors isomers with any oxygen-oxygen bond. This adds spectroscopic characterization of the rhenium oxidation state and the nature of ligands to the known ability of [Re,O4]+ to perform two consecutive hydrogen-atom abstraction reactions from methane, and demonstrates that pentaatomic [Re,O4]+ combines a metal center in its highest oxidation state with two oxygen-centered radical ligands in a highly reactive species.","PeriodicalId":72562,"journal":{"name":"Chemistry methods : new approaches to solving problems in chemistry","volume":"4 12","pages":""},"PeriodicalIF":6.1,"publicationDate":"2024-10-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cmtd.202400023","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142851578","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Video Documented Upscaled Synthesis of Salts of the Parent Carbaborate Ion [CB11H12]−, its Undecafluorinated Form [CHB11F11]− and Useful Starting Materials for its Introduction 通过视频记录硼酸根离子[CB11H12]-母盐、其未十氟化形式[CHB11F11]-及其有用起始材料的放大合成过程

IF 6.1

Chemistry methods : new approaches to solving problems in chemistry Pub Date : 2024-10-21 DOI: 10.1002/cmtd.202400011

Jan Kulenkampff, Christian Armbruster, Johanna Drolshagen, Celine Regnat, Tina Wienold, Luisa Spari, Jana Fix, Tabea Sterbak, Dr. Harald Scherer, Prof. Dr. Ingo Krossing

{"title":"Video Documented Upscaled Synthesis of Salts of the Parent Carbaborate Ion [CB11H12]−, its Undecafluorinated Form [CHB11F11]− and Useful Starting Materials for its Introduction","authors":"Jan Kulenkampff, Christian Armbruster, Johanna Drolshagen, Celine Regnat, Tina Wienold, Luisa Spari, Jana Fix, Tabea Sterbak, Dr. Harald Scherer, Prof. Dr. Ingo Krossing","doi":"10.1002/cmtd.202400011","DOIUrl":"https://doi.org/10.1002/cmtd.202400011","url":null,"abstract":"In this work, we present our improved protocols for the single batch syntheses of approximately 32 g of [NHMe3][CB11H12] and 10 g of Na[CHB11F11] as well as salt metathesis reactions, granting access to useful starting materials to introduce the [CHB11F11]− anion. This includes the trityl cation [Ph3C]+ and the bis-1,2-difluorobenzene-silver(I)-complex [Ag(odfb)2]+, as well as some applications of the shown compounds. The described methodology allows the synthesis of large amounts of both the [CB11H12]− and the [CHB11F11]− anion and therefore making them accessible for further reactions. To facilitate the reproducibility, we present video tutorials of the synthetic steps towards Na[CHB11F11].","PeriodicalId":72562,"journal":{"name":"Chemistry methods : new approaches to solving problems in chemistry","volume":"4 11","pages":""},"PeriodicalIF":6.1,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cmtd.202400011","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142666104","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

FSscore: A Personalized Machine Learning-Based Synthetic Feasibility Score FSscore：基于机器学习的个性化合成可行性评分

IF 6.1

Chemistry methods : new approaches to solving problems in chemistry Pub Date : 2024-10-18 DOI: 10.1002/cmtd.202400024

Rebecca M. Neeser, Prof. Bruno Correia, Prof. Philippe Schwaller

{"title":"FSscore: A Personalized Machine Learning-Based Synthetic Feasibility Score","authors":"Rebecca M. Neeser, Prof. Bruno Correia, Prof. Philippe Schwaller","doi":"10.1002/cmtd.202400024","DOIUrl":"https://doi.org/10.1002/cmtd.202400024","url":null,"abstract":"Determining whether a molecule can be synthesized is crucial in chemistry and drug discovery, as it guides experimental prioritization and molecule ranking in de novo design tasks. Existing scoring approaches to assess synthetic feasibility struggle to extrapolate to new chemical spaces or fail to discriminate based on subtle differences such as chirality. This work addresses these limitations by introducing the Focused Synthesizability score (FSscore), which uses machine learning to rank structures based on their relative ease of synthesis. First, a baseline trained on an extensive set of reactant-product pairs is established, which is then refined with expert human feedback tailored to specific chemical spaces. This targeted fine-tuning improves performance on these chemical scopes, enabling more accurate differentiation between molecules that are hard and easy to synthesize. The FSscore showcases how a human-in-the-loop framework can be utilized to optimize the assessment of synthetic feasibility for various chemical applications.","PeriodicalId":72562,"journal":{"name":"Chemistry methods : new approaches to solving problems in chemistry","volume":"4 11","pages":""},"PeriodicalIF":6.1,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cmtd.202400024","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142666060","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

High-Pressure Cell for In Situ Grazing Incidence XAS Characterization of Model Catalysts on Planar Supports 用于平面载体上模型催化剂原位放牧入射 XAS 表征的高压样品室

IF 6.1

Chemistry methods : new approaches to solving problems in chemistry Pub Date : 2024-10-18 DOI: 10.1002/cmtd.202400014

Sumant Phadke, João Coroa, Imran Abbas, Dr. Jinlong Yin, Dr. Didier Grandjean, Prof. Dr. Ewald Janssens, Dr. Olga V. Safonova

{"title":"High-Pressure Cell for In Situ Grazing Incidence XAS Characterization of Model Catalysts on Planar Supports","authors":"Sumant Phadke, João Coroa, Imran Abbas, Dr. Jinlong Yin, Dr. Didier Grandjean, Prof. Dr. Ewald Janssens, Dr. Olga V. Safonova","doi":"10.1002/cmtd.202400014","DOIUrl":"https://doi.org/10.1002/cmtd.202400014","url":null,"abstract":"The growing interest in physically deposited model catalysts for uncovering complex structure-activity relationships is spurred by the possibility of depositing nanoparticles of precise atomic structure and composition using cluster-beam sources. However, the limitations accompanying these synthesis techniques, such as low deposition rates and flat sample geometry, present a challenge for in situ structural characterization using bulk-sensitive methods, such as X-ray absorption spectroscopy (XAS), especially at elevated pressures (1–100 bar). To overcome this challenge, we constructed an in situ XAS cell operating in a grazing incidence (GI) geometry. The GIXAS cell was used to investigate the structure of cluster-beam-generated Pd and Au0.3Ag0.7 nanoparticles under CO2-to-methanol hydrogenation conditions (230 °C, 20 bar, CO2:H2=1 : 3). These nanoparticles, with metal loading of 0.96–10 μg cm−2, demonstrated stability and resistance to sintering upon activation in H2 at 120 °C and catalytic conditions, revealed by in situ XAS. The promising results from our work will help bridge the gap in the investigation of model catalytic materials produced by gas-phase cluster deposition at industrially relevant pressures and temperatures, which is vital for a mechanistic understanding of catalytic processes.","PeriodicalId":72562,"journal":{"name":"Chemistry methods : new approaches to solving problems in chemistry","volume":"4 11","pages":""},"PeriodicalIF":6.1,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cmtd.202400014","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142666059","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Cover Feature: (Chem. Methods 10/2024) 封面专题：（化学方法 10/2024）

IF 6.1

Chemistry methods : new approaches to solving problems in chemistry Pub Date : 2024-10-07 DOI: 10.1002/cmtd.202481001

引用次数: 0