Chemistry methods : new approaches to solving problems in chemistry最新文献_第6页

Revealing the Mechanism and Kinetics of Fe5C2 Formation From Ferrous Oxalate under CO2 Fischer-Tropsch Conditions Using Time-Resolved In Situ X-Ray Absorption Spectroscopy 用时间分辨原位x射线吸收光谱法揭示CO2费托条件下草酸亚铁生成Fe5C2的机理和动力学

IF 3.6

Chemistry methods : new approaches to solving problems in chemistry Pub Date : 2025-03-16 DOI: 10.1002/cmtd.202400058

Dr. Elizaveta A. Fedorova, Dr. Aleksandr Fedorov, Dr. Dmitry E. Doronkin, Dr. David Linke, Dr. Christoph Kubis, Prof. Dr. Angelika Brückner, Prof. Dr. Evgenii V. Kondratenko

{"title":"Revealing the Mechanism and Kinetics of Fe5C2 Formation From Ferrous Oxalate under CO2 Fischer-Tropsch Conditions Using Time-Resolved In Situ X-Ray Absorption Spectroscopy","authors":"Dr. Elizaveta A. Fedorova, Dr. Aleksandr Fedorov, Dr. Dmitry E. Doronkin, Dr. David Linke, Dr. Christoph Kubis, Prof. Dr. Angelika Brückner, Prof. Dr. Evgenii V. Kondratenko","doi":"10.1002/cmtd.202400058","DOIUrl":"10.1002/cmtd.202400058","url":null,"abstract":"The fundamentals of in situ formation of iron carbides are required for the tailored design of Fe-based catalysts for the efficient conversion of CO2 to higher hydrocarbons. Herein, time-resolved in situ X-ray absorption spectroscopy has been used to elucidate the mechanism of the formation of Fe5C2 from ferrous oxalate (FeC2O4) at 350 °C using a H2/CO=3 reaction feed. Regardless of the kind of alkali metal promoter and reaction pressure (1 or 7.5 bar), FeC2O4 is first decomposed to FeO followed by the conversion of the latter to Fe5C2. Further insights into the above transformations were derived by kinetic analysis using a Johnson–Mehl–Avrami–Erofeev–Kolmogorov model and kinetics-constrained neural ordinary differential equations method. Both approaches revealed that the formation of FeO at 1 bar follows a nucleation mechanism, while a diffusion mechanism has a higher contribution at 7.5 bar. The latter mechanism is valid for the conversion of FeO to Fe5C2 at both pressures. Alkali metal promoters were found to accelerate the rate of Fe5C2 formation. This rate decreases with increasing total pressure due to the stabilization of FeO.","PeriodicalId":72562,"journal":{"name":"Chemistry methods : new approaches to solving problems in chemistry","volume":"5 5","pages":""},"PeriodicalIF":3.6,"publicationDate":"2025-03-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cmtd.202400058","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143944820","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: Sodium-Potassium Competition as a Tool for Chemoselective Cucurbit[n]uril-Xenon Host–Guest Complexation in Imaging Applications (Chem. Methods 3/2025) 封面图：钠钾竞争作为化学选择性瓜素[n]铀-氙主-客体络合在成像中的应用方法3/2025)

IF 3.6

Chemistry methods : new approaches to solving problems in chemistry Pub Date : 2025-03-10 DOI: 10.1002/cmtd.202580301

Dr. Katarzyna Dziubińska-Kühn, Dr. Guzel Musabirova, Sophie Effertz, Prof. Jörg Matysik, Prof. Renaud Blaise Jolivet

{"title":"Cover Picture: Sodium-Potassium Competition as a Tool for Chemoselective Cucurbit[n]uril-Xenon Host–Guest Complexation in Imaging Applications (Chem. Methods 3/2025)","authors":"Dr. Katarzyna Dziubińska-Kühn, Dr. Guzel Musabirova, Sophie Effertz, Prof. Jörg Matysik, Prof. Renaud Blaise Jolivet","doi":"10.1002/cmtd.202580301","DOIUrl":"10.1002/cmtd.202580301","url":null,"abstract":"The Front Cover illustrates that by paw-holding, wild sea otters ensure they stay together and do not drift apart in their sleep. This comes from a concept of no herd member being left behind. If the experimental conditions are met, the same phenomenon is observed in the study by Renaud Blaise Jolivet and co-workers, where K+ ions and cage molecules interact in the solution, forming species with significantly higher Xe encapsulation rates. The preferential caging of Xe by CB[6]-alkali pairs is seen as an analogy to the paw-holding-based social gathering of sea otters. For more details, see the Research Article by Renaud Blaise Jolivet and co-workers (DOI: 10.1002/cmtd.202400033).\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":"5 3","pages":""},"PeriodicalIF":3.6,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cmtd.202580301","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143581788","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}

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Integrating Flow Chemistry With Electrospray Ionization Mass Spectrometry 将流动化学与电喷雾离子化质谱技术相结合

IF 3.6

Chemistry methods : new approaches to solving problems in chemistry Pub Date : 2025-03-03 DOI: 10.1002/cmtd.202400036

Quentin Duez

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Correlative Characterizations Reveal the Structure-Bonding-Property Relationship at a Local Scale 相关表征揭示了局部尺度上的结构-键合-性质关系

IF 3.6

Chemistry methods : new approaches to solving problems in chemistry Pub Date : 2025-03-02 DOI: 10.1002/cmtd.202500009

Huaide Zhang, Yiming Zhou, Chongjian Zhou, Matthias Wuttig, Yuan Yu

{"title":"Correlative Characterizations Reveal the Structure-Bonding-Property Relationship at a Local Scale","authors":"Huaide Zhang, Yiming Zhou, Chongjian Zhou, Matthias Wuttig, Yuan Yu","doi":"10.1002/cmtd.202500009","DOIUrl":"10.1002/cmtd.202500009","url":null,"abstract":"Grain boundaries (GBs) play an important role in the mechanical and functional properties of polycrystalline materials. For charge carrier transport, GBs can either decrease or even increase the electrical conductivity, depending on the local atomic arrangements at the GB. Yet, uncovering the “one-to-one correlation” between structures and properties is non-trivial. This work demonstrates an advanced approach that combines multiple in-situ and ex-situ techniques to investigate the structural, chemical, and transport properties of individual GBs. Advanced characterization and processing techniques such as electron backscatter diffraction and focused ion beam allow us to site specifically “lift out” individual GBs from the polycrystalline bulk. Combined with semiconductor fabrication protocols such as electron beam lithography and deposition to prepare a measurement circuit, we can obtain the electrical properties of the microscale lamella. Moreover, the chemical composition and bonding mechanism of the same GB can be determined by atom probe tomography. An example of PbS shows that the high-angle GB strongly reduces carrier mobility due to the existence of a potential barrier and the local collapse of metavalent bonding.","PeriodicalId":72562,"journal":{"name":"Chemistry methods : new approaches to solving problems in chemistry","volume":"5 9","pages":""},"PeriodicalIF":3.6,"publicationDate":"2025-03-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/cmtd.202500009","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144998724","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}

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SLIC-SABRE at Microtesla Fields Enables High Levels of Nuclear Spin Polarization Without Magnetic Shielding SLIC-SABRE在微特斯拉磁场下实现高水平的核自旋极化而不需要磁屏蔽

IF 3.6

Chemistry methods : new approaches to solving problems in chemistry Pub Date : 2025-02-21 DOI: 10.1002/cmtd.202400060

Vitaly P. Kozinenko, Alexey S. Kiryutin, Alexandra V. Yurkovskaya

{"title":"SLIC-SABRE at Microtesla Fields Enables High Levels of Nuclear Spin Polarization Without Magnetic Shielding","authors":"Vitaly P. Kozinenko, Alexey S. Kiryutin, Alexandra V. Yurkovskaya","doi":"10.1002/cmtd.202400060","DOIUrl":"10.1002/cmtd.202400060","url":null,"abstract":"Employing nuclear spin hyperpolarization to enhance NMR sensitivity opens new horizons for metabolic studies and chemical reaction monitoring. Among the hyperpolarization techniques, Signal Amplification by Reversible Exchange (SABRE) is prominent for its ability to transfer spin order from parahydrogen to target nuclei, especially 13C and 15N, without the chemical modification of the substrate under study. Despite its power, existing implementations of SABRE require expensive equipment like radiofrequency (RF) hardware and magnetic shielding. This paper demonstrates the SLIC-SABRE (Spin Lock Induced Crossing SABRE) method at low magnetic fields as a low-cost and efficient technique for achieving high 15N polarization using a simple setup, consisting only of a small set of magnetic coils driven by a desktop PC sound card. The method yields from 5 up to 17 % polarization across various SABRE-active molecules, outperforming the conventional SABRE-SHEATH (SABRE in SHield Enables Alignment Transfer to Heteronuclei) approach and significantly enhancing the accessibility of hyperpolarization techniques.","PeriodicalId":72562,"journal":{"name":"Chemistry methods : new approaches to solving problems in chemistry","volume":"5 5","pages":""},"PeriodicalIF":3.6,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cmtd.202400060","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143944961","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}

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Natural and Artificial Aging Methods For Silver Mock-ups In Recent Conservation And Heritage Studies: A Short Review 近年来保护和遗产研究中银质模型的自然和人工老化方法综述

IF 3.6

Chemistry methods : new approaches to solving problems in chemistry Pub Date : 2025-02-19 DOI: 10.1002/cmtd.202400055

Dr. Qing Wu, Han Zhou, Prof. Loïc Bertrand, Prof. Maartje Stols-Witlox, Prof. Laura Brambilla, Prof. Edith Joseph

{"title":"Natural and Artificial Aging Methods For Silver Mock-ups In Recent Conservation And Heritage Studies: A Short Review","authors":"Dr. Qing Wu, Han Zhou, Prof. Loïc Bertrand, Prof. Maartje Stols-Witlox, Prof. Laura Brambilla, Prof. Edith Joseph","doi":"10.1002/cmtd.202400055","DOIUrl":"10.1002/cmtd.202400055","url":null,"abstract":"Silver has been widely used for art and heritage objects throughout history, due to its excellent ductility, malleability and brilliant metallic lustre. However, silver objects tarnish over time and must be regularly treated to maintain their appearance. In conservation and heritage studies, naturally or artificially aged silver mock-ups are often used to simulate the tarnishing conditions of valuable historical silver objects. Over the last few decades, many research groups have proposed different aging protocols. In this paper, we reviewed the silver aging protocols employed in recent studies in the field. Although the chemistry-based aging methods are most widely used, issues regarding alterations of the tarnish stratigraphy and negative influences on environment and operator safety should not be neglected. This review aims to provide important references for conservators, scientists and researchers to select safe and suitable aging methods for building their own mock-up systems, and to encourage the development of more sustainable aging protocols for future conservation of historical silver objects.","PeriodicalId":72562,"journal":{"name":"Chemistry methods : new approaches to solving problems in chemistry","volume":"5 5","pages":""},"PeriodicalIF":3.6,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cmtd.202400055","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143945035","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}

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Graphene Oxide-Cyclopentylamine (GO-d-CP) Liquid Crystals as a Novel Alignment Medium for Anisotropic NMR with Analyte Recovery 氧化石墨烯-环戊胺（GO-d-CP）液晶作为分析物回收的各向异性核磁共振新取向介质

IF 3.6

Chemistry methods : new approaches to solving problems in chemistry Pub Date : 2025-02-14 DOI: 10.1002/cmtd.202400039

Sandesh Chickmagalur Jatheendranath, Akhi Das, Sudhindra H Deshpande, Nilamoni Nath, Walter Maier, Verena Streitferdt, Udaya Kiran Marelli

{"title":"Graphene Oxide-Cyclopentylamine (GO-d-CP) Liquid Crystals as a Novel Alignment Medium for Anisotropic NMR with Analyte Recovery","authors":"Sandesh Chickmagalur Jatheendranath, Akhi Das, Sudhindra H Deshpande, Nilamoni Nath, Walter Maier, Verena Streitferdt, Udaya Kiran Marelli","doi":"10.1002/cmtd.202400039","DOIUrl":"10.1002/cmtd.202400039","url":null,"abstract":"In this study, we present graphene oxide derivatized with cyclopentylamine (GO-d-CP) as a DMSO-compatible liquid crystal alignment medium that is free from any background NMR signal for application in anisotropic NMR. This novel alignment medium facilitates optimal isotropic and anisotropic conditions within a single sample preparation, controlled by sonication, thereby enabling the measurement of anisotropic NMR parameters- residual dipolar couplings (RDC) and residual chemical shift anisotropy (RCSA). GO-d-CP offers several advantages, including ease of synthesis, isolation of solid GO-d-CP as a stable non-hygroscopic material, and maintenance of the anisotropic state stability >30 days, allowing for prolonged and repetitive experiments. Notably, post the analysis it allows for easy recovery of valuable analytes as well as GO-d-CP for reuse, enabling the routine application of anisotropic NMR in structural analysis of small molecules. We demonstrate its efficacy by analyzing the relative stereochemistry of four compounds - estrone, santonin, griseofulvin, and cinmethylin - using anisotropic NMR data.","PeriodicalId":72562,"journal":{"name":"Chemistry methods : new approaches to solving problems in chemistry","volume":"5 4","pages":""},"PeriodicalIF":3.6,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cmtd.202400039","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143793481","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}

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Continuous Titration Based Method for Rapid In-Solution Analysis of Non-Covalent Interactions 基于连续滴定的非共价相互作用快速溶液分析方法

IF 3.6

Chemistry methods : new approaches to solving problems in chemistry Pub Date : 2025-02-14 DOI: 10.1002/cmtd.202400059

Philipp Willmer, Adam C. Hundahl, Rodolphe Marie, Henrik Jensen

{"title":"Continuous Titration Based Method for Rapid In-Solution Analysis of Non-Covalent Interactions","authors":"Philipp Willmer, Adam C. Hundahl, Rodolphe Marie, Henrik Jensen","doi":"10.1002/cmtd.202400059","DOIUrl":"10.1002/cmtd.202400059","url":null,"abstract":"Development of new drugs typically involves the identification and validation of molecular inhibitors or promotors of endogenous biological processes. The identification of ligands that can bind the target of interest is typically achieved by screening large libraries of small molecules, using analytical methods that only provide yes/no answers. These methods are only qualitative and often associated with unacceptable amounts of false positives and negatives. Quantitative methods are in general more accurate but time intensive. This is mainly due to repeating measurements of a dilution series in order to generate a titration curve and measure the dissociation constant (Kd). In this work, we introduce Continuous Titration Based Spectral Related Intensity Change (cSPRING), that combines Taylor dispersion analysis (TDA) with ratiometric fluorescence detection to measure a Kd in a single experiment. cSPRING is an in-solution method that reduces the sample preparation time 8-fold and requires only nanograms of protein. We show a good agreement of cSPRING with other quantitative methods for three well-known protein-small molecule interactions with binding affinities ranging from the low nanomolar to high micromolar. In addition, we show that cSPRING is able to measure binding affinities in under a minute, highlighting its efficiency and potential for screening applications.","PeriodicalId":72562,"journal":{"name":"Chemistry methods : new approaches to solving problems in chemistry","volume":"5 5","pages":""},"PeriodicalIF":3.6,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cmtd.202400059","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143944745","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}

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Exploring Bonding in Bioinorganic Chemistry: Ab Initio Valence Bond Calculations of Iron(II)-CO and Iron(IV)-Oxo Units in Cytochrome P450 under Oriented External Electric Fields 探索生物无机化学中的化学键：定向外电场作用下细胞色素P450中铁(II)-CO和铁(IV)-氧基的从头算价键计算

IF 3.6

Chemistry methods : new approaches to solving problems in chemistry Pub Date : 2025-02-14 DOI: 10.1002/cmtd.202400090

Enhua Zhang, Hajime Hirao

{"title":"Exploring Bonding in Bioinorganic Chemistry: Ab Initio Valence Bond Calculations of Iron(II)-CO and Iron(IV)-Oxo Units in Cytochrome P450 under Oriented External Electric Fields","authors":"Enhua Zhang, Hajime Hirao","doi":"10.1002/cmtd.202400090","DOIUrl":"10.1002/cmtd.202400090","url":null,"abstract":"We performed ab initio valence bond (VB) calculations under oriented external electric fields (OEEFs) to explore the bonding nature of iron(II)-CO and iron(IV)-oxo units in cytochrome P450 enzymes (P450s). By utilizing ligand-free models and analyzing changes in electronic structures under OEEFs, we gained insights into how ligands influence the iron center in realistic environments. Our findings revealed that ligand effects in P450s, exerted by the proximal and equatorial ligands, align with an electric field of approximately −0.125 to −0.100 au along the bond axis (Fz). Additionally, the proximal thiolate ligand alone corresponds to a weaker field, with Fz values around −0.060 to −0.050 au. Negative Fz values enhanced π backdonation while suppressing σ donation in iron(II)-CO, whereas positive Fz values exhibited the opposite trend. Furthermore, negative Fz values significantly stabilized VB structures with higher oxidation states of Fe in iron(IV)-oxo. In the absence of OEEFs, the oxidation state of Fe in iron(IV)-oxo is predominantly Fe(II). However, under negative Fz values, VB structures with Fe(III) character become considerably more stable. These findings underscore the significant influence of external electric fields – and by extension, ligands – on the electronic properties of metal-containing bioinorganic systems.","PeriodicalId":72562,"journal":{"name":"Chemistry methods : new approaches to solving problems in chemistry","volume":"5 8","pages":""},"PeriodicalIF":3.6,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/cmtd.202400090","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144869314","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}

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Cover Picture: All-in-One Portable Electrochemical Strips for Drug Release, Delivery and Monitoring (Chem. Methods 2/2025) 封面图片：用于药物释放、传递和监测的多功能便携式电化学试纸条。方法2/2025)

IF 3.6

Chemistry methods : new approaches to solving problems in chemistry Pub Date : 2025-02-10 DOI: 10.1002/cmtd.202580201

Sima Singh, Mohga Khater, Ada Raucci, Ovidio Catanzano, Fabiana Quaglia, Stefano Cinti

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