The Royal Society of Chemistry最新文献_第6页

A non-resonant Kβ valence-to-core X-ray emission approach for fluorine and oxygen differentiation in Zr compounds. Zr化合物中氟和氧分化的非共振Kβ价核x射线发射方法。

IF 3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2026-10-20 DOI: 10.1039/d6cp01440b

Christian Heinekamp, C Tufan Cakir, Ana Guilherme Buzanich, Konstantin Klementiev, Michael Roemelt, Thomas Braun, Franziska Emmerling

{"title":"A non-resonant Kβ valence-to-core X-ray emission approach for fluorine and oxygen differentiation in Zr compounds.","authors":"Christian Heinekamp, C Tufan Cakir, Ana Guilherme Buzanich, Konstantin Klementiev, Michael Roemelt, Thomas Braun, Franziska Emmerling","doi":"10.1039/d6cp01440b","DOIUrl":"https://doi.org/10.1039/d6cp01440b","url":null,"abstract":"Valence-to-core (VtC) X-ray emission spectroscopy (XES) is a powerful probe for the local electronic structure in transition-metal materials, but its potential for 4d metals such as zirconium remains largely unexplored. Here, we demonstrate that non-resonant Zr Kβ VtC XES provides quantitative descriptors that are sensitive to ligand chemistry, by probing fluorine- and oxygen-based coordination environments in well-defined and catalytically relevant Zr compounds. High-resolution X-ray emission spectra containing Zr-Kβ2 and -Kβ4 are recorded for a series of reference systems (ZrO2, ZrF4, ZrF4·H2O, ZrCl4, Zr(acac)4, Zr metal) and for Zr fluoride materials, and are analysed using quantitative line-shape parameters. Projected densities of states (PDOS) obtained from FDMNES calculations reveal that fluorine coordination enhances the Kβ″ contribution and induces characteristic changes in Kβ2 intensity and asymmetry compared to oxygen and chlorine ligands. These ligand-specific spectral signatures enable a systematic discrimination between F- and O-containing coordination spheres, even when conventional X-ray absorption or diffraction techniques provide limited contrast. This combined experimental-computational framework demonstrates that Zr Kβ VtC XES can resolve subtle ligand-dependent coordination changes in Zr-based materials, offering a general route to identify active structures in C-F bond activation and oxygen-evolution catalysis.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":" ","pages":""},"PeriodicalIF":3.0,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149222889","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Carbonic anhydrase functionalized porous bismuth metallene for selective reduction of carbon dioxide to formate. 碳酸酐酶功能化多孔金属铋选择性还原二氧化碳生成甲酸酯。

IF 4.3 2区化学

Chemical Communications Pub Date : 2026-10-20 DOI: 10.1039/d6cc04555c

Yi Wang, Liyang Shao, Xuefang Zhu, Yu Chen, Yucheng Jiang

引用次数: 0

Archaeoglobus fulgidus CbiX^S is a promiscuous chelatase with a broad substrate scope. fulgidus Archaeoglobus chixs是一种杂交螯合酶，具有广泛的底物范围。

IF 3.3 3区化学

Dalton Transactions Pub Date : 2026-10-20 DOI: 10.1039/d6dt01532h

Bruce S Lickey, Matthew D Liptak

{"title":"Archaeoglobus fulgidus CbiXS is a promiscuous chelatase with a broad substrate scope.","authors":"Bruce S Lickey, Matthew D Liptak","doi":"10.1039/d6dt01532h","DOIUrl":"10.1039/d6dt01532h","url":null,"abstract":"Organisms biosynthesize square planar metal tetrapyrrole cofactors containing Mg, Fe, Co, and Ni using chelatase enzymes, which selectively insert the correct metal into a specific organic ligand. Archaeoglobus fulgidus CbiXS has been proposed to be an \"ancestral\" chelatase enzyme; in this work we have evaluated its substrate scope to ascertain whether this enzyme is a promising starting point for synthetic chelatase design. Size-exclusion chromatography revealed that CbiXS is a tetramer in solution regardless of the metalation state of the enzyme, in contrast to the dimeric structure of the nickel chelatase CfbA. Reaction conditions that minimize enzyme-free metal insertion into tetrapyrroles were determined, which revealed that many of the in vitro activity assays reported in the literature for chelatase enzymes may be plagued by non-enzymatic metal insertion. Under these conditions that minimize uncatalyzed metal insertion, CbiXS was observed to catalyze metal insertion for six different combinations of metal and tetrapyrrole. Based upon the turnover numbers of these reactions, CbiXS is most effective at catalyzing metal insertion for reactants similar to its native substrates: cobalt and sirohydrochlorin. Kinetic analysis for reactions with varying substrate concentrations revealed that CbiXS may be substrate-inhibited for non-native substrates. In addition, the kinetic data identifies metal-ligand bond formation as the rate-limiting step of the enzyme. Due to its broad substrate scope, CbiXS is an encouraging starting point for synthetic chelatase design that could yield non-natural metal tetrapyrroles for use in the biotechnology sector.","PeriodicalId":71,"journal":{"name":"Dalton Transactions","volume":" ","pages":"14614-14624"},"PeriodicalIF":3.3,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149101105","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Prevention of IED threats: a non-destructive and multiparametric detection of pre-blast explosive residues in fabrics using confocal Raman microscopy. 预防简易爆炸装置威胁：使用共聚焦拉曼显微镜对织物中爆炸前残留物的非破坏性和多参数检测。

IF 3 3区化学

Analytical Methods Pub Date : 2026-10-20 DOI: 10.1039/d5ay00685f

Giuseppina Gullifa, Flavia Iezzi, Antonietta Lombardozzi, Maria Cristina Pigro, Daniela Panetta, Alessandro Ruscitti, Chiara Albertini, Stefano Materazzi, Roberta Risoluti

{"title":"Prevention of IED threats: a non-destructive and multiparametric detection of pre-blast explosive residues in fabrics using confocal Raman microscopy.","authors":"Giuseppina Gullifa, Flavia Iezzi, Antonietta Lombardozzi, Maria Cristina Pigro, Daniela Panetta, Alessandro Ruscitti, Chiara Albertini, Stefano Materazzi, Roberta Risoluti","doi":"10.1039/d5ay00685f","DOIUrl":"https://doi.org/10.1039/d5ay00685f","url":null,"abstract":"Improvised explosive devices (IEDs) are widespread among criminal and terrorist cells since such organizations are more and more capable of creating evermore powerful and easily concealable explosive devices. This makes their detection not only challenging but also crucial to prevent bomb attacks. In particular, textiles are often a source of evidence of contamination as a consequence of manipulating explosives. This work proposes a novel, rapid and accurate confocal Raman microscopy method for the detection and identification of pre-blast explosive residues related to the handling, packaging, and carriage of explosive devices. Raman spectra were collected from explosive residues of TNT, TATP, PETN, Pyrodex, RDX, and ANFO trapped in different types of fibers (natural/synthetic, dyed/undyed) in order to evaluate the spectroscopic response in conditions that are as realistic as possible and to quantify the interfering effect of the substrate. The results demonstrated that all the investigated explosives were correctly identified with 100% accuracy, showing no sample thermodegradation or interfering contributions related to the textile substrate. This innovative approach permits the simultaneous detection of the most common explosives involved in IEDs by a fast, accurate and non-destructive platform able to be used as confirmatory analysis and to provide timely support for forensic investigation for homeland security.","PeriodicalId":64,"journal":{"name":"Analytical Methods","volume":" ","pages":""},"PeriodicalIF":3.0,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149226690","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

PIDA/ammonium carbamate-mediated oxidative ring opening of indolizines to form pyridine-based acrylonitriles. PIDA/氨基甲酸铵介导吲哚嘧啶氧化开环生成吡啶基丙烯腈。

IF 2.8 3区化学

Organic & Biomolecular Chemistry Pub Date : 2026-10-20 DOI: 10.1039/d6ob01337f

Rohit Kumar, Avanish Yadav, Vijay Kumar, Anupam Ghosh, Deepak K Sharma

引用次数: 0

Regioselective copper-catalyzed domino synthesis of 7-iodobenzo[d]oxazoles as potential ER_β ligands. 区域选择性铜催化7-碘苯并[d]恶唑作为潜在ERβ配体的多米诺合成。

IF 2.8 3区化学

Organic & Biomolecular Chemistry Pub Date : 2026-10-20 DOI: 10.1039/d6ob01200k

Walid K Al-Jammal, Raed M Al-Zoubi, Sally R Al-Zoubi, Mohanad Shkoor, Abbas Khan, Abdelali Agouni, Ameera Al-Jabiry, Robert McDonald

{"title":"Regioselective copper-catalyzed domino synthesis of 7-iodobenzo[d]oxazoles as potential ERβ ligands.","authors":"Walid K Al-Jammal, Raed M Al-Zoubi, Sally R Al-Zoubi, Mohanad Shkoor, Abbas Khan, Abdelali Agouni, Ameera Al-Jabiry, Robert McDonald","doi":"10.1039/d6ob01200k","DOIUrl":"https://doi.org/10.1039/d6ob01200k","url":null,"abstract":"7-Halogenated benzoxazoles are a recurring motif in preclinical ligands for the estrogen receptor β (ERβ) and in other oxazole-based pharmacophores, yet selective and direct access to the 7-halo regiochemistry is not well served by classical condensation routes or by existing copper-catalyzed arylation methods. Here we report that 5-substituted 1,2,3-triiodobenzenes undergo a regioselective copper-catalyzed domino C-N/C-O arylation with primary amides to deliver 7-iodobenzoxazoles. Substrate-screening conditions implement the cascade as two in situ steps executed in a one-pot procedure. Across twenty substrate combinations explored under the two-stage protocol, yields reached up to 98% and the regiochemistry of the 7-iodo product was confirmed unambiguously by single-crystal X-ray diffraction of 7m. The reaction tolerates gram-scale execution (82% at 2.06 mmol). Using this methodology, human β-estrogen receptor 1 (7c) (AstraZeneca patent (WO2002051821)) is prepared in only one step with excellent regioselectivity and isolated yield. A subset of the 7-iodobenzoxazoles was evaluated in silico against the ERβ ligand-binding domain by convolutional-neural-network-guided and diffusion-based docking (GNINA and DiffDock), followed by 200 ns AMBER22 molecular dynamics and MM/GBSA free-energy calculations; 7g and 7e emerged as candidate scaffolds with MM/GBSA ΔGtotal values of -31.2 and -28.6 kcal mol-1, respectively, and reproducible binding poses centred on a conserved Met336 anchor.","PeriodicalId":96,"journal":{"name":"Organic & Biomolecular Chemistry","volume":" ","pages":""},"PeriodicalIF":2.8,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149226699","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Emergence of active foams in a minimal cognitive flocking model. 最小认知群集模型中活性泡沫的出现。

IF 2.9 3区化学

Soft Matter Pub Date : 2026-10-20 DOI: 10.1039/d6sm00751a

Aryan Dwivedi, Diganta Bhaskar, Anil Kumar Dasanna

{"title":"Emergence of active foams in a minimal cognitive flocking model.","authors":"Aryan Dwivedi, Diganta Bhaskar, Anil Kumar Dasanna","doi":"10.1039/d6sm00751a","DOIUrl":"https://doi.org/10.1039/d6sm00751a","url":null,"abstract":"We investigate a minimal visual perception-driven model of self-propelled particles that interact through purely position-based cohesive steering within a finite vision cone, in the absence of velocity alignment and physical volume exclusion. Building on a previously proposed minimal cognitive model, we extend the interaction range from the previously studied short-range and distance-independent limits to an intermediate regime, enabling a systematic investigation of how a finite vision range influences collective behavior. We find that this regime exhibits a rich state diagram that combines characteristics of both limiting cases while giving rise to qualitatively new collective states. Besides the gas, nematic-band, and polar file states, we uncover the emergence of active foams - system-spanning fractal-like networks sustained by dynamically evolving particle streams. These structures arise solely from non-reciprocal vision-based interactions and are absent in both the short and long vision-range limits. For larger vision angles, the system self-organizes into a variety of aggregate morphologies, including condensates, rings, and multi-twist filaments, revealing a strong interplay between interaction range and anisotropic perception in shaping collective organization.","PeriodicalId":103,"journal":{"name":"Soft Matter","volume":" ","pages":""},"PeriodicalIF":2.9,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149226731","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Metal-free synthesis of primary amides from aldehydes using hydroxylamine-O-sulfonic acid. 用羟胺-邻磺酸从醛类合成伯胺的无金属研究。

IF 2.8 3区化学

Organic & Biomolecular Chemistry Pub Date : 2026-10-20 DOI: 10.1039/d6ob01347c

Shivam Bhargav, Jawahar L Jat

引用次数: 0

Mechanism of the dehydrogenation of Mg(BH₄)₂·THF_0.25 to Mg(B₁₀H₁₀): role of the THF solvate. Mg(BH4)2·THF0.25脱氢生成Mg（B10H10）的机理：THF溶剂的作用

IF 3.3 3区化学

Dalton Transactions Pub Date : 2026-10-20 DOI: 10.1039/d6dt02098d

McKinley A Prager, Sunil Shrestha, Phuong Q H Nyugen, Natalie McNurlin, Stephen Kim, Craig M Jensen

{"title":"Mechanism of the dehydrogenation of Mg(BH4)2·THF0.25 to Mg(B10H10): role of the THF solvate.","authors":"McKinley A Prager, Sunil Shrestha, Phuong Q H Nyugen, Natalie McNurlin, Stephen Kim, Craig M Jensen","doi":"10.1039/d6dt02098d","DOIUrl":"10.1039/d6dt02098d","url":null,"abstract":"Dehydrogenation of Mg(BH4)2·THFx (1·THF) at 180 °C has been previously found to produce primarily a mixture of Mg(B3H8)2 (2) and Mg(B10H10) (3). It has now been found that dehydrogenation under a H2 back pressure of 20 bar suppresses the formation of 2 and results in very high (>95%) selectivity for 3. The production of 3 is not inhibited by hydrogen pressure. This demonstrates that the reaction pathway leading to its formation does not involve reversible, rate limiting H2 elimination and is divergent from the pathway leading to 2. Unlike the pathway leading to the formation of 2, the dehydrogenation of 1·THF to 3 is irreversible under moderate conditions. Concurrent with the dehydrogenation reaction, THF is slowly converted to Mg(OBun)2, curtailing the production 3. However, the dehydrogenation process is revived by addition of a fresh aloquate of THF to the reaction mixtures. It is hypothesized that THF enables the production of 3 by stabilizing the key intermediate, [B2H5]- and by the low melting point (<100 °C) of 1·THF which allows long-range diffusion of borane anions at much lower energies than those required for their transport in the solid-state.","PeriodicalId":71,"journal":{"name":"Dalton Transactions","volume":" ","pages":"14521-14525"},"PeriodicalIF":3.3,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149101060","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

A biphenyl-bridged bis(cyclen) cyclophane: Ag(I)-induced conformational reorganization and successive Ag(I) binding. 联苯桥接双（环）环烷：Ag(I)诱导的构象重组和连续的Ag(I)结合。

IF 3.3 3区化学

Dalton Transactions Pub Date : 2026-10-20 DOI: 10.1039/d6dt02170k

Hiroki Horita, Eunji Lee, Mari Ikeda, Shunsuke Kuwahara, Yoichi Habata

引用次数: 0