Communications Chemistry最新文献_第6页

Women in chemistry: Q&A with Professor Tricia Breen Carmichael 化学界的女性特里西娅-布林-卡迈克尔教授问答

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-10-01 DOI: 10.1038/s42004-024-01287-z

引用次数: 0

Supramolecular fibrillation in coacervates and other confined systems towards biomimetic function 在共聚物和其他封闭系统中实现超分子纤化，从而实现生物仿生功能

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-09-30 DOI: 10.1038/s42004-024-01308-x

Adrian Sanchez-Fernandez, Ignacio Insua, Javier Montenegro

{"title":"Supramolecular fibrillation in coacervates and other confined systems towards biomimetic function","authors":"Adrian Sanchez-Fernandez, Ignacio Insua, Javier Montenegro","doi":"10.1038/s42004-024-01308-x","DOIUrl":"10.1038/s42004-024-01308-x","url":null,"abstract":"As in natural cytoskeletons, the cooperative assembly of fibrillar networks can be hosted inside compartments to engineer biomimetic functions, such as mechanical actuation, transport, and reaction templating. Coacervates impose an optimal liquid-liquid phase separation within the aqueous continuum, functioning as membrane-less compartments that can organise such self-assembling processes as well as the exchange of information with their environment. Furthermore, biological fibrillation can often be controlled or assisted by intracellular compartments. Thus, the reconstitution of analogues of natural filaments in simplified artificial compartments, such as coacervates, offer a suitable model to unravel, mimic, and potentially exploit cellular functions. This perspective summarises the latest developments towards assembling fibrillar networks under confinement inside coacervates and related compartments, including a selection of examples ranging from biological to fully synthetic monomers. Comparative analysis between coacervates, lipid vesicles, and droplet emulsions showcases the interplay between supramolecular fibres and the boundaries of the corresponding compartment. Combining inspiration from natural systems and the custom properties of tailored synthetic fibrillators, rational monomer and compartment design will contribute towards engineering increasingly complex and more realistic artificial protocells. The bottom-up reconstitution of natural filaments within simplified artificial cellular compartments, such as coacervates, offer a model to study, mimic, and potentially exploit cellular functions. Here, the authors summarize the latest developments towards assembling confined fibrillar networks inside coacervates and related compartments, including a selection of examples ranging from biological to fully synthetic building blocks.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-11"},"PeriodicalIF":5.9,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s42004-024-01308-x.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142329477","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Structural phase transition in NH₄F under extreme pressure conditions 极压条件下 NH₄F 的结构相变

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-09-30 DOI: 10.1038/s42004-024-01309-w

Umbertoluca Ranieri, Christophe Bellin, Lewis J. Conway, Richard Gaal, John S. Loveday, Andreas Hermann, Abhay Shukla, Livia E. Bove

{"title":"Structural phase transition in NH₄F under extreme pressure conditions","authors":"Umbertoluca Ranieri, Christophe Bellin, Lewis J. Conway, Richard Gaal, John S. Loveday, Andreas Hermann, Abhay Shukla, Livia E. Bove","doi":"10.1038/s42004-024-01309-w","DOIUrl":"10.1038/s42004-024-01309-w","url":null,"abstract":"Ammonium fluoride (NH₄F) exhibits a variety of crystalline phases depending on temperature and pressure. By employing Raman spectroscopy and synchrotron X-ray diffraction beyond megabar pressures (up to 140 GPa), we have here observed a novel dense solid phase of NH₄F, characterised by the tetragonal P4/nmm structure also observed in other ammonium halides under less extreme pressure conditions, typically a few GPa. Using detailed ab-initio calculations and reevaluating earlier theoretical models pertaining to other ammonium halides, we examine the microscopic mechanisms underlying the transition from the low-pressure cubic phase (P-43m) to the newly identified high-pressure tetragonal phase (P4/nmm). Notably, NH₄F exhibits distinctive properties compared to its counterparts, resulting in a significantly broader pressure range over which this transition unfolds, facilitating the identification of its various stages. Our analysis points to a synergistic interplay driving the transition to the P4/nmm phase, which we name phase VIII. At intermediate pressures (around 40 GPa), a displacive transition of fluorine ions initiates a tetragonal distortion of the cubic phase. Subsequently, at higher pressures (around 115 GPa), every second ammonium ion undergoes a rotational shift, adopting an anti-tetrahedral arrangement. This coupled effect orchestrates the transition process, leading to the formation of the tetragonal phase. Solid ammonium fluoride has fascinating structural similarities with water ice, despite its ionic character. Here, the authors investigate NH4F at room temperature and high pressure, and report a new tetragonal phase formed through displacive transition of fluorine ions and subsequent rotation of ammonium ions in ‘antiferromagnetic’ units at ~115 GPa, which is unlike any form of ice.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-8"},"PeriodicalIF":5.9,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s42004-024-01309-w.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142329456","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Women in chemistry: Q&A with Professor Hongjing Dou 化学界的女性窦红静教授问答

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-09-30 DOI: 10.1038/s42004-024-01307-y

引用次数: 0

Biosynthesis of iron-chelating terramides A-C and their role in Aspergillus terreus infection 铁螯合萜酰胺 A-C 的生物合成及其在赤霉菌感染中的作用

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-09-30 DOI: 10.1038/s42004-024-01311-2

Yi Han, Yaojie Guo, Nan Zhang, Fan Xu, Jarukitt Limwachiranon, Zhenzhen Xiong, Liru Xu, Xu-Ming Mao, Daniel H. Scharf

{"title":"Biosynthesis of iron-chelating terramides A-C and their role in Aspergillus terreus infection","authors":"Yi Han, Yaojie Guo, Nan Zhang, Fan Xu, Jarukitt Limwachiranon, Zhenzhen Xiong, Liru Xu, Xu-Ming Mao, Daniel H. Scharf","doi":"10.1038/s42004-024-01311-2","DOIUrl":"10.1038/s42004-024-01311-2","url":null,"abstract":"Fungal natural products from various species often feature hydroxamic acid motifs that have the ability to chelate iron. These compounds have an array of medicinally and ecologically relevant activities. Through genome mining, gene deletion in the host Aspergillus terreus, and heterologous expression experiments, this study has revealed that a nonribosomal peptide synthetase (NRPS) TamA and a specialized cytochrome P450 monooxygenase TamB catalyze the sequential biosynthetic reactions in the formation of terramides A-C, a series of diketopiperazines (DKPs) with hydroxamic acid motifs. Feeding experiments showed that TamB catalyzes an unprecedented di-hydroxylation of the amide nitrogens in the diketopiperazine core. This tailoring reaction led to the formation of two bidentate iron-binding sites per molecule with an unusual iron-binding stoichiometry. The structure of the terramide A-Fe complex was characterized by liquid chromatography-mass spectrometry (LC-MS), Fourier transform infrared spectroscopy (FT-IR), Raman spectroscopy and electron paramagnetic resonance spectroscopy (EPR). Antimicrobial assays showed that the iron-binding motifs are crucial for the activity against bacteria and fungi. Murine infection experiments indicated that terramide production is crucial for the virulence of A. terreus and could be a potential antifungal drug target. Terramides A-C are produced by Aspergillus terreus and feature hydroxamic acid motifs in diketopiperazines to chelate iron; however, their biosynthesis is not fully understood. Here, the authors probe the function of two key enzymes TamA and TamB and propose the biosynthesis of terramides A-C as well as their function in the virulence of A. terreus.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-10"},"PeriodicalIF":5.9,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s42004-024-01311-2.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142329467","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

The molecular picture of the local environment in a stable model coacervate 稳定模型凝聚态局部环境的分子图谱

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-09-30 DOI: 10.1038/s42004-024-01304-1

Atanu Baksi, Hasan Zerze, Aman Agrawal, Alamgir Karim, Gül H. Zerze

{"title":"The molecular picture of the local environment in a stable model coacervate","authors":"Atanu Baksi, Hasan Zerze, Aman Agrawal, Alamgir Karim, Gül H. Zerze","doi":"10.1038/s42004-024-01304-1","DOIUrl":"10.1038/s42004-024-01304-1","url":null,"abstract":"Complex coacervates play essential roles in various biological processes and applications. Although substantial progress has been made in understanding the molecular interactions driving complex coacervation, the mechanisms stabilizing coacervates against coalescence remain experimentally challenging and not fully elucidated. We recently showed that polydiallyldimethylammonium chloride (PDDA) and adenosine triphosphate (ATP) coacervates stabilize upon their transfer to deionized (DI) water. Here, we perform molecular dynamics simulations of PDDA-ATP coacervates in supernatant and DI water, to understand the ion dynamics and structure within stable coacervates. We found that transferring the coacervates to DI water results in an immediate ejection of a significant fraction of small ions (Na+ and Cl−) from the surface of the coacervates to DI water. We also observed a notable reduction in the mobility of these counterions in coacervates when in DI water, both in the cluster-forming and slab simulations, together with a lowered displacement of PDDA and ATP. These results suggest that the initial ejection of the ions from the coacervates in DI water may induce an interfacial skin layer formation, inhibiting further mobility of ions in the skin layer. Transferring coacervates based on polydiallyldimethylammonium chloride and adenosine triphosphate into deionized water has been experimentally demonstrated to stabilize them against coalescence. Here, molecular modeling and simulations are used to study the coacervation and stabilization of the relevant polyelectrolyte mixture, systematically investigating the structural and dynamic properties that lead to stability.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-11"},"PeriodicalIF":5.9,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s42004-024-01304-1.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142329463","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

On-surface synthesis of porous graphene nanoribbons mediated by phenyl migration 苯基迁移介导的多孔石墨烯纳米带的表面合成

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-09-29 DOI: 10.1038/s42004-024-01284-2

César Moreno, Xabier Diaz de Cerio, Maria Tenorio, Fei Gao, Manuel Vilas-Varela, Ane Sarasola, Diego Peña, Aran Garcia-Lekue, Aitor Mugarza

{"title":"On-surface synthesis of porous graphene nanoribbons mediated by phenyl migration","authors":"César Moreno, Xabier Diaz de Cerio, Maria Tenorio, Fei Gao, Manuel Vilas-Varela, Ane Sarasola, Diego Peña, Aran Garcia-Lekue, Aitor Mugarza","doi":"10.1038/s42004-024-01284-2","DOIUrl":"10.1038/s42004-024-01284-2","url":null,"abstract":"Advancements in the on-surface synthesis of atomically precise graphene nanostructures are propelled by the introduction of innovative precursor designs and reaction types. Until now, the latter has been confined to cross-coupling and cyclization reactions that involve the cleavage of specific atoms or groups. In this article, we elucidate how the migration of phenyl substituents attached to graphene nanoribbons can be harnessed to generate arrays of [18]-annulene pores at the edges of the nanostructures. This sequential pathway is revealed through a comprehensive study employing bond-resolved scanning tunneling microscopy and ab-initio computational techniques. The yield of pore formation is maximized by anchoring the graphene nanoribbons at steps of vicinal surfaces, underscoring the potential of these substrates to guide reaction paths. Our study introduces a new reaction to the on-surface synthesis toolbox along with a sequential route, altogether enabling the extension of this strategy towards the formation of other porous nanostructures. The on-surface synthesis of graphene nanoribbons typically relies on Ullmann polymerization followed by an internal cyclodehydrogenation. Here, following these two steps, the authors expand the synthetic protocol by adding controlled phenyl migration and intraribbon aryl-aryl dehydrogenative coupling to afford graphene nanoribbons with periodic arrays of [18]annulene pores at the edges.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-7"},"PeriodicalIF":5.9,"publicationDate":"2024-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s42004-024-01284-2.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142329453","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Photoaging enhances the leaching of di(2-ethylhexyl) phthalate and transformation products from polyvinyl chloride microplastics into aquatic environments 光照增强了聚氯乙烯微塑料中邻苯二甲酸二（2-乙基己基）酯和转化产物在水生环境中的沥滤作用

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-09-27 DOI: 10.1038/s42004-024-01310-3

Charlotte Henkel, Thorsten Hüffer, Ruoting Peng, Xiaoyu Gao, Subhasis Ghoshal, Thilo Hofmann

{"title":"Photoaging enhances the leaching of di(2-ethylhexyl) phthalate and transformation products from polyvinyl chloride microplastics into aquatic environments","authors":"Charlotte Henkel, Thorsten Hüffer, Ruoting Peng, Xiaoyu Gao, Subhasis Ghoshal, Thilo Hofmann","doi":"10.1038/s42004-024-01310-3","DOIUrl":"10.1038/s42004-024-01310-3","url":null,"abstract":"Increasing chemical pollution is a threat to sustainable water resources worldwide. Plastics and harmful additives released from plastics add to this burden and might pose a risk to aquatic organisms, and human health. Phthalates, which are common plasticizers and endocrine-disrupting chemicals, are released from polyvinyl chloride (PVC) microplastics and are a cause of concern. Therefore, the leaching kinetics of additives, including the influence of environmental weathering, are key to assessing exposure concentrations but remain largely unknown. We show that photoaging strongly enhances the leaching rates of di(2-ethylhexyl) phthalate (DEHP) by a factor of 1.5, and newly-formed harmful transformation products, such as mono(2-ethylhexyl) phthalate (MEHP), phthalic acid, and phthalic anhydride from PVC microplastics into the aquatic environment. Leaching half-lives of DEHP reduced from 449 years for pristine PVC to 121 years for photoaged PVC. Aqueous boundary layer diffusion (ABLD) is the limiting mass transfer process for the release of DEHP from pristine and photoaged PVC microplastics. The leaching of transformation products is limited by intraparticle diffusion (IPD). The calculated mass transfer rates can be used to predict exposure concentrations of harmful additives in the aquatic environment. The environmental weathering of plastics and the leaching kinetics of additives are key to assessing exposure concentrations. Here, the authors show that photoaging enhances the leaching rate of the common additive di(2-ethylhexyl) phthalate (DEHP) by a factor of 1.5, and newly-formed harmful transformation products, such as mono(2-ethylhexyl) phthalate (MEHP), phthalic acid, and phthalic anhydride, are released from PVC microplastics into the aquatic environment.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-10"},"PeriodicalIF":5.9,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s42004-024-01310-3.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142328598","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Women in chemistry: Q&A with Dr Ritika Gautam-Singh 化学界的女性与 Ritika Gautam-Singh 博士的问答

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-09-25 DOI: 10.1038/s42004-024-01302-3

引用次数: 0

Women in chemistry: Q&A with Professor Hyunjoo Lee 化学界的女性与 Hyunjoo Lee 教授的问答

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-09-25 DOI: 10.1038/s42004-024-01291-3

引用次数: 0