Communications Chemistry最新文献_第5页

Sustainable synthesis of fine chemicals and polymers using industrial chlorine chemistry 利用工业氯化学进行精细化学品和聚合物的可持续合成。

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-11-14 DOI: 10.1038/s42004-024-01345-6

Yasuhiro Kohsaka, Daisuke Matsuura, Yoshikazu Kimura

{"title":"Sustainable synthesis of fine chemicals and polymers using industrial chlorine chemistry","authors":"Yasuhiro Kohsaka, Daisuke Matsuura, Yoshikazu Kimura","doi":"10.1038/s42004-024-01345-6","DOIUrl":"10.1038/s42004-024-01345-6","url":null,"abstract":"To achieve sustainable resource circulation, preparation of reactive species from stable compounds is unavoidable. Chlorine chemistry is an eco-friendly methodology to address this demand. Chlorine is industrially produced from sodium chloride (NaCl), an abundant natural resource in oceans. Chlorine provides various chemical products, including polymers, through chlorination and subsequent conversion reactions. In these reactions, the byproducts are usually hydrogen chloride, which is commercially utilized as hydrochloric acid and is finally neutralized to NaCl after use. Therefore, chlorine chemistry enables fine chemical production from NaCl with almost no wastage. This review provides an overview of the synthesis of fine chemicals and polymers using chlorine chemistry and discusses them from the perspective of sustainability. To achieve sustainable resource circulation, preparation of reactive species from stable compounds is needed, and chlorine chemistry is an eco-friendly approach to address this need. Here, the authors provide an overview of the synthesis of fine chemicals and polymers using chlorine chemistry, with emphasis with regards to sustainability.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-10"},"PeriodicalIF":5.9,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s42004-024-01345-6.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142616111","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

Structure confirmation, reactivity, bacterial mutagenicity and quantification of 2,2,4-tribromo-5-hydroxycyclopent-4-ene-1,3-dione in drinking water 饮用水中 2,2,4-三溴-5-羟基环戊-4-烯-1,3-二酮的结构确认、反应性、细菌诱变性和定量。

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-11-14 DOI: 10.1038/s42004-024-01356-3

Davide Ciccarelli, Ben M. J. Lancaster, D. Christopher Braddock, Matteo Calvaresi, Miroslav Mišík, Siegfried Knasmüller, Edoardo Jun Mattioli, Francesco Zerbetto, Andrew J. P. White, Tim Marczylo, Timothy W. Gant, Leon P. Barron

{"title":"Structure confirmation, reactivity, bacterial mutagenicity and quantification of 2,2,4-tribromo-5-hydroxycyclopent-4-ene-1,3-dione in drinking water","authors":"Davide Ciccarelli, Ben M. J. Lancaster, D. Christopher Braddock, Matteo Calvaresi, Miroslav Mišík, Siegfried Knasmüller, Edoardo Jun Mattioli, Francesco Zerbetto, Andrew J. P. White, Tim Marczylo, Timothy W. Gant, Leon P. Barron","doi":"10.1038/s42004-024-01356-3","DOIUrl":"10.1038/s42004-024-01356-3","url":null,"abstract":"The presence of two new disinfectant by-product (DBP) groups in the UK was recently shown using non-target analysis, halogenated-hydroxycyclopentenediones and halogenated-methanesulfonic acids. In this work, we confirmed the structure of 2,2,4-tribromo-5-hydroxycyclopent-4-ene-1,3-dione (TBHCD), and quantified it together with dibromomethanesulfonic acid at 122 ± 34 and 326 ± 157 ng L−1 on average in London’s drinking water, respectively (n = 21). We found TBHCD to be photolabile and unstable in tap water and at alkaline pH. Furthermore, spectral and computational data for TBHCD and three other halogenated-hydroxycyclopentenediones indicated they could act as a source of radicals in water and in the body. Importantly, TBHCD was calculated to have a 14.5 kcal mol−1 lower C-Br bond dissociation enthalpy than the N-Br bond of N-bromosuccinimide, a common radical substitution reagent used in organic synthesis. TBHCD was mutagenic in Salmonella/microsome assays using strains TA98, TA100 and TA102. This work reveals the unique features, activity and toxicity of trihalogenated hydroxycyclopent-4-ene-1,3-diones, prompting a need to more comprehensively assess their risks. Halogenated disinfection by-products are a recognized health risk, but unequivocal identification and monitoring of new compounds is challenging, which prevents risk assessment. Here, the authors identify and quantify 2,2,4-tribromo-5-hydroxycyclopent-4-ene-1,3-dione in London drinking water, and describe the compound’s activity and toxicity.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-11"},"PeriodicalIF":5.9,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s42004-024-01356-3.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142616105","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

An iridium(III) complex-based luminogenic probe for high-throughput screening of hydrogen sulfide donors in living cells 基于铱（III）复合物的发光探针，用于高通量筛选活细胞中的硫化氢供体。

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-11-13 DOI: 10.1038/s42004-024-01332-x

Ke-Jia Wu, Wen Sun, Jian-Min Sun, Chang Lu, Ning Sun, Chung‐Hang Leung, Yan Li, Chun Wu

{"title":"An iridium(III) complex-based luminogenic probe for high-throughput screening of hydrogen sulfide donors in living cells","authors":"Ke-Jia Wu, Wen Sun, Jian-Min Sun, Chang Lu, Ning Sun, Chung‐Hang Leung, Yan Li, Chun Wu","doi":"10.1038/s42004-024-01332-x","DOIUrl":"10.1038/s42004-024-01332-x","url":null,"abstract":"The scarcity of suitable high-throughput screening technology for hydrogen sulfide (H2S) donors has hampered the discovery of H2S donors. In this study, a long-lived cyclometalated iridium complex was rationally designed as a mitochondria-targeted H2S probe to monitor the real-time dynamic change of H2S. By using the time-resolved emission spectroscopy (TRES) technique, an anti-interference high-throughput screening system was developed to monitor H2S in living cells with decreased false negative results. As a proof-of-concept, three natural products were identified as potential H2S donors from a natural product library using the developed TRES probe. Notably, the discovery of allicin and diallyl trisulfide demonstrated the feasibility of this screening platform, while garlic-derived allyl methyl sulfide was explored as a H2S donor candidate. The results were further validated by a commercial assay. We anticipate this high-throughput platform could facilitate the discovery of H2S donors by discriminating the endogenous interfering fluorescence from biological systems. H2S donors in living cells are essential for modulating H2S levels and have been proposed to be relevant for managing hepatic disorders, but conventional platforms to screen for H2S donors are plagued by interference by endogenous background fluorescence signals. Here, the authors develop a luminogenic probe—based on an Ir(III) complex with a 1,10-phenanthroline-5,6-dione moiety—capable of selective response to mitochondrial H2S, and set up an anti-interference high-throughput screening system capable of distinguishing target signals from complex background autofluorescence in living cells.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-7"},"PeriodicalIF":5.9,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s42004-024-01332-x.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142616101","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

Small-rotative fixed-target serial synchrotron crystallography (SR-FT-SSX) for molecular crystals 用于分子晶体的小旋转固定目标串行同步辐射晶体学（SR-FT-SSX）。

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-11-13 DOI: 10.1038/s42004-024-01360-7

Sam G. Lewis, Ben A. Coulson, Anna J. Warren, Mark R. Warren, Lauren E. Hatcher

{"title":"Small-rotative fixed-target serial synchrotron crystallography (SR-FT-SSX) for molecular crystals","authors":"Sam G. Lewis, Ben A. Coulson, Anna J. Warren, Mark R. Warren, Lauren E. Hatcher","doi":"10.1038/s42004-024-01360-7","DOIUrl":"10.1038/s42004-024-01360-7","url":null,"abstract":"The increasing availability of ultrabright Light Sources is facilitating the study of smaller crystals at faster timescales but with an increased risk of severe X-ray damage, leading to developments in multi-crystal methods such as serial crystallography (SX). SX studies on crystals with small unit cells are challenging as very few reflections are recorded in a single data image, making it difficult to determine the orientation matrix for each crystal and thus preventing the combination of the data from all crystals for structure solution. We herein present a Small-Rotative Fixed-Target Serial Synchrotron Crystallography (SR-FT-SSX) methodology, in which rotation of the serial target through a small diffraction angle $$(varphi )$$ at each crystal delivers high-quality data, facilitating ab initio unit cell determination and atomic-scale structure solution. The method is benchmarked using microcrystals of the small-molecule photoswitch sodium nitroprusside dihydrate, obtaining complete data to dmin = 0.6 Å by combining just 66 partial datasets selected against rigorous quality criteria. Multi-crystal methods such as serial crystallography can provide a complete 3D structure of the target material before radiation damage becomes significant, but the methods are challenging for small molecule crystals with small unit cells, where very few reflections are recorded in a single data image. Here, the authors present a small-rotative fixed-target serial synchrotron crystallography (SR-FT-SSX) methodology, in which rotation of the serial target through a small diffraction angle $$(varphi )$$ at each crystal delivers high-quality data, facilitating ab initio unit cell determination and atomic-scale structure solution.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-7"},"PeriodicalIF":5.9,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s42004-024-01360-7.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142616103","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

Chromatin inspired bio-condensation between biomass DNA and guanosine monophosphate produces all-nucleic hydrogel as a hydrotropic drug carrier 受染色质启发，生物质 DNA 与单磷酸鸟苷之间的生物缩合产生了全核苷水凝胶，可作为亲水性药物载体

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-11-12 DOI: 10.1038/s42004-024-01353-6

Suryakamal Sarma, Neha Thakur, Nidhi Varshney, Hem Chandra Jha, Tridib K. Sarma

{"title":"Chromatin inspired bio-condensation between biomass DNA and guanosine monophosphate produces all-nucleic hydrogel as a hydrotropic drug carrier","authors":"Suryakamal Sarma, Neha Thakur, Nidhi Varshney, Hem Chandra Jha, Tridib K. Sarma","doi":"10.1038/s42004-024-01353-6","DOIUrl":"10.1038/s42004-024-01353-6","url":null,"abstract":"The integration of biomolecules into supramolecular nanostructures forms the basis of the natural world. Naturally occurring liquid-liquid phase separation resulting in biomolecular condensates has inspired the formation of biomolecule-based smart materials with multi-dimensional applications. A non-covalent bio-condensation between biomass DNA and guanosine monophosphate (GMP) has been described, mimicking chromatin folding and creating a unique “all-nucleic” DNA-GMP condensates. These condensates initiate the formation of G-quadruplex-based superstructures, assembling into super-helical fibres driven by synergistic hydrogen bonding and stacking, which have been thoroughly investigated. This simple, one-step method for the bio-condensation of biomass DNA leads to an “all-nucleic” hydrogel with higher-order self-assembly and excellent mechanical properties. While most of the reported DNA based biomaterials, including hydrogels, require precisely sequenced and molecularly architectured DNA building blocks, we have developed a simple, universal, and facile bio-condensation method that utilizes biomass DNA acquired from any bio-resource to fabricate DNA hydrogels. The hydrogel efficiently encapsulates and sustains the release of both hydrophilic and hydrophobic drugs, demonstrating its competency as a drug carrier. We believe this energy-efficient and low-cost method represents a new technique for using biomass DNA as building blocks for the next generation of soft materials. Biomolecular condensates provide a useful platform for a range of applications. Here, the authors describe a non-covalent bio-condensation between biomass DNA and guanosine monophosphate, mimicking chromatin folding and creating an all-nucleic hydrogel as a carrier for both hydrophobic and hydrophilic drugs.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-13"},"PeriodicalIF":5.9,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s42004-024-01353-6.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142600839","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

Environment-sensitive turn-on fluorescent probe enables live cell imaging of myeloperoxidase activity during NETosis 环境敏感型开启荧光探针可对母细胞瘤形成过程中髓过氧化物酶的活性进行活细胞成像

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-11-12 DOI: 10.1038/s42004-024-01338-5

Enebie Ramos Cáceres, Lotte Kemperman, Kimberly M. Bonger

{"title":"Environment-sensitive turn-on fluorescent probe enables live cell imaging of myeloperoxidase activity during NETosis","authors":"Enebie Ramos Cáceres, Lotte Kemperman, Kimberly M. Bonger","doi":"10.1038/s42004-024-01338-5","DOIUrl":"10.1038/s42004-024-01338-5","url":null,"abstract":"Myeloperoxidase (MPO) plays an important role in the immune response of human neutrophils and has been implicated in autoimmune conditions, cardiovascular disorders, and neurodegeneration. Current methods to detect MPO activity rely on the detection of HOCl using activatable probes or require challenging experimental procedures. Therefore, these tools provide limited information about the dynamics and localization of MPO in complex molecular processes such as NETosis in real time. In this study, we report a ‘’turn-on” activity-based probe that fluoresces exclusively upon binding to MPO, exhibits minimal background fluorescence in buffered aqueous media, and is blocked by MPO inhibitors. Our probe facilitates real-time imaging of direct MPO activity in human neutrophils and HL-60-derived granulocytes during NETosis under wash-free conditions. Furthermore, it allows for the discrimination between different triggers of NETosis in human neutrophils. These findings hold promise for advancing our understanding of the role of MPO in immune responses and inflammatory conditions. Myeloperoxidase (MPO) plays an important role in the innate immune response of human neutrophils and has been implicated in various diseases, but current methods to detect MPO provide limited information about its dynamics and localization in complex molecular processes. Here, the authors develop an activity-based probe that fluoresces exclusively upon binding to MPO, enabling real-time imaging of direct intracellular MPO activity in human neutrophils and HL-60-derived granulocytes during NETosis under wash-free conditions.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-7"},"PeriodicalIF":5.9,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s42004-024-01338-5.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142600840","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

Liquid-liquid crystalline phase separation of spider silk proteins 蜘蛛丝蛋白质的液-液结晶相分离

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-11-12 DOI: 10.1038/s42004-024-01357-2

Michael Landreh, Hannah Osterholz, Gefei Chen, Stefan D. Knight, Anna Rising, Axel Leppert

{"title":"Liquid-liquid crystalline phase separation of spider silk proteins","authors":"Michael Landreh, Hannah Osterholz, Gefei Chen, Stefan D. Knight, Anna Rising, Axel Leppert","doi":"10.1038/s42004-024-01357-2","DOIUrl":"10.1038/s42004-024-01357-2","url":null,"abstract":"Liquid-liquid phase separation (LLPS) of proteins can be considered an intermediate solubility regime between disperse solutions and solid fibers. While LLPS has been described for several pathogenic amyloids, recent evidence suggests that it is similarly relevant for functional amyloids. Here, we review the evidence that links spider silk proteins (spidroins) and LLPS and its role in the spinning process. Major ampullate spidroins undergo LLPS mediated by stickers and spacers in their repeat regions. During spinning, the spidroins droplets shift from liquid to crystalline states. Shear force, altered ion composition, and pH changes cause micelle-like spidroin assemblies to form an increasingly ordered liquid-crystalline phase. Interactions between polyalanine regions in the repeat regions ultimately yield the characteristic β-crystalline structure of mature dragline silk fibers. Based on these findings, we hypothesize that liquid-liquid crystalline phase separation (LLCPS) can describe the molecular and macroscopic features of the phase transitions of major ampullate spidroins during spinning and speculate whether other silk types may use a similar mechanism to convert from liquid dope to solid fiber. Liquid-liquid phase separation (LLPS) of proteins can be considered an intermediate solubility regime between disperse solutions and solid fibers, relevant to both pathogenic and functional amyloids. Here, the authors review the evidence that links spider silk proteins (spidroins) and LLPS and its role in the spinning process.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-8"},"PeriodicalIF":5.9,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s42004-024-01357-2.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142600845","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

DigFrag as a digital fragmentation method used for artificial intelligence-based drug design DigFrag 作为一种数字碎裂方法，用于基于人工智能的药物设计

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-11-11 DOI: 10.1038/s42004-024-01346-5

Ruoqi Yang, Hao Zhou, Fan Wang, Guangfu Yang

{"title":"DigFrag as a digital fragmentation method used for artificial intelligence-based drug design","authors":"Ruoqi Yang, Hao Zhou, Fan Wang, Guangfu Yang","doi":"10.1038/s42004-024-01346-5","DOIUrl":"10.1038/s42004-024-01346-5","url":null,"abstract":"Fragment-Based Drug Design (FBDD) plays a pivotal role in the field of drug discovery and development. The construction of high-quality fragment libraries is a critical step in FBDD. Conventional fragmentation approaches often rely on rigid rules and chemical intuition, limiting their adaptability to diverse molecular structures. The rapid development of Artificial Intelligence (AI) technology offers a transformative opportunity to rethink traditional methods. Here, we present DigFrag, a digital fragmentation method that highlights important substructures by focusing locally within the molecular graph. In addition, we feed the fragments segmented by machine intelligence and human expertise into the deep generative model to compare the preference for data from different sources. Experimental results show that the structural diversity of fragments segmented by DigFrag is higher, and more desirable compounds are generated based on these fragments. These results also demonstrate that data generated based on AI methods may be more suitable for AI models. Moreover, a user-friendly platform called MolFrag ( https://dpai.ccnu.edu.cn/MolFrag/ ) is developed based on various fragmentation techniques to support molecular segmentation. Fragment-based drug design plays a pivotal role in the field of drug discovery and development, however, the construction of high-quality fragment libraries is a critical but challenging step. Here, the authors develop DigFrag, a digital fragmentation method based on the graph attention mechanism, showing higher structural diversity of the fragments and higher applicability to artificial intelligence-based drug design.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-9"},"PeriodicalIF":5.9,"publicationDate":"2024-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s42004-024-01346-5.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142599026","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

Pivotal role of 99Tc NMR spectroscopy in solid-state and molecular chemistry 99Tc NMR 光谱在固态和分子化学中的关键作用

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-11-11 DOI: 10.1038/s42004-024-01349-2

Vitaly V. Kuznetsov, Frederic Poineau, Konstantin E. German, Elena A. Filatova

引用次数: 0

On the interfacial phenomena at the Li7La3Zr2O12 (LLZO)/Li interface 关于 Li7La3Zr2O12 (LLZO)/Li 界面的界面现象

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-11-09 DOI: 10.1038/s42004-024-01350-9

Kostiantyn V. Kravchyk, Huanyu Zhang, Maksym V. Kovalenko

引用次数: 0