Angewandte Chemie最新文献_第9页

Nitramine Formation via a Cryptic Non-Ribosomal Peptide Synthetase-Dependent Strategy in N-Nitroglycine Biosynthesis n-硝基甘氨酸生物合成中隐性非核糖体肽合成酶依赖策略形成硝胺

Angewandte Chemie Pub Date : 2025-05-14 DOI: 10.1002/ange.202507866

Yun Wang, Jiangtao Zhang, Dr. Ran Shi, Siyuan Zhou, Prof. Shigui Chen, Dr. Ruofei Li, Dr. Wei Huang, Prof. Hai-Yan He

{"title":"Nitramine Formation via a Cryptic Non-Ribosomal Peptide Synthetase-Dependent Strategy in N-Nitroglycine Biosynthesis","authors":"Yun Wang, Jiangtao Zhang, Dr. Ran Shi, Siyuan Zhou, Prof. Shigui Chen, Dr. Ruofei Li, Dr. Wei Huang, Prof. Hai-Yan He","doi":"10.1002/ange.202507866","DOIUrl":"https://doi.org/10.1002/ange.202507866","url":null,"abstract":"N-nitroglycine (NNG), a rare nitramine natural compound, is the only known example produced by streptomyces strains. In this study, we clarified that NNG biosynthesis originates from glycine and l-lysine and elucidated its biosynthetic gene cluster (BGC) nng. This cluster shares high homology with the recently reported BGCs of diazo compound azaserine. In vivo and in vitro results have indicated NNG biosynthetic pathway involves hydrazine and hydrazone generation, with a non-heme diiron N-oxygenase and a cytochrome P450 responsible for forming the nitramine structure. Furthermore, although NNG lacks a serine unit in the structure, its biosynthesis still requires the incorporation of a serine attached to the hydrazone intermediate by non-ribosomal peptide synthetase (NRPS), similar to the azaserine pathway, and two hydrolases are putatively involved in thioester hydrolysis and serine removal, respectively. This study, along with comparisons to azaserine biosynthesis, not only paves the way for the discovery of new nitramine and diazo compounds by genome mining but also highlights the potential for uncovering novel enzymes and chemistry involved in hydrazone oxidation.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 29","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-05-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144624634","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Hyperbranched Polymer-Based Multipath Proton Transmembrane Transport System with Redox-Switchable Characteristics for Cancer Cell Apoptosis 基于超支化聚合物的多路径质子跨膜运输系统具有氧化还原开关特性，用于癌细胞凋亡

Angewandte Chemie Pub Date : 2025-05-14 DOI: 10.1002/ange.202500986

Cong Li, Yaqi Wu, Sheng Bao, Zhengwei Xu, Jing Yan, Hui Li, Xiaoxuan Yu, Zihui Weng, Jiayun Xu, Tingting Wang, Prof. Dr. Yongfeng Zhou, Dr. Tengfei Yan, Prof. Dr. Yi Yan, Prof. Dr. Junqiu Liu

{"title":"Hyperbranched Polymer-Based Multipath Proton Transmembrane Transport System with Redox-Switchable Characteristics for Cancer Cell Apoptosis","authors":"Cong Li, Yaqi Wu, Sheng Bao, Zhengwei Xu, Jing Yan, Hui Li, Xiaoxuan Yu, Zihui Weng, Jiayun Xu, Tingting Wang, Prof. Dr. Yongfeng Zhou, Dr. Tengfei Yan, Prof. Dr. Yi Yan, Prof. Dr. Junqiu Liu","doi":"10.1002/ange.202500986","DOIUrl":"https://doi.org/10.1002/ange.202500986","url":null,"abstract":"Natural channel proteins (NCPs) enable efficient and selective transport of specific species across cellular membranes and exhibit stimulus-responsive behaviors; however, replicating these features in their artificial counterparts poses significant challenges. Here, we report a hyperbranched polymer (HBP)-derived biomimetic multipath proton transport system, H3, by a straightforward “one-pot” cationic polymerization of 3-ethyl-3-(hydroxymethyl)-oxetane. H3 efficiently transports protons while rejecting other ions and water molecules by forming multiple hydrogen bonding chains like natural proton channels. Patch clamp experiments revealed that H3 facilitates rapid proton transport (γH+ = 181 ± 4 pS) comparable to that of natural gramicidin A (γH+ = 213 ± 4 pS) and demonstrates high H+-selectivity, with PH+/PK+, PH+/PNa+, and PH+/PCl- values reaching 78.4, 233.2, and 167.8, respectively. H3-induced proton transport causes elevated lysosomal pH and mitochondrial damage, ultimately resulting in severe cancer cell apoptosis (IC50: 0.23 µM for U87MG; 1.04 µM for B16F10). Interestingly, selenide moieties-containing H3-Se exhibits an unprecedented in situ redox-switchable “ON–OFF” of proton transport by regulating its hydrophilicity. This work will contribute to a deeper understanding of the intrinsic mechanisms of NCPs and treatments for cancer and other diseases.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 29","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-05-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144624528","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Asymmetric Aziridination of Allylic Carbamates Using Ion-Paired Rhodium Complexes and Extrapolation to C─H Amination of Phenethyl Carbamates 离子对铑配合物对烯丙基氨基甲酸酯的不对称叠氮化反应及苯乙酯C─H胺化反应的外推

Angewandte Chemie Pub Date : 2025-05-14 DOI: 10.1002/ange.202507532

Dr. Arthur R. Lit, Dr. Shotaro Takano, Christian Zachau, Ioana Băltărețu, Prof. Robert J. Phipps

{"title":"Asymmetric Aziridination of Allylic Carbamates Using Ion-Paired Rhodium Complexes and Extrapolation to C─H Amination of Phenethyl Carbamates","authors":"Dr. Arthur R. Lit, Dr. Shotaro Takano, Christian Zachau, Ioana Băltărețu, Prof. Robert J. Phipps","doi":"10.1002/ange.202507532","DOIUrl":"https://doi.org/10.1002/ange.202507532","url":null,"abstract":"Aziridination of alkenes is an important route to chiral nitrogen-containing building blocks. Here, we report that carbamate-functionalized allylic alcohols undergo highly enantioselective aziridination using achiral dimeric Rh(II, II) complexes that are ion-paired with cinchona alkaloid-derived chiral cations. The aziridine-containing products are amenable to a variety of further reactions to generate useful groupings of functionality. Furthermore, we show that the carbamate group is effective for directing highly enantioselective benzylic C─H amination when it is appended to phenethyl alcohols. Intermolecular C─H amination of phenethyl alcohol derivatives has proven highly challenging to achieve asymmetrically yet it gives rise to valuable β-amino alcohols. Both processes result in rapid access to versatile, highly enantioenriched small molecule building blocks for synthesis and highlight the effectiveness and generality of this chiral cation-based strategy for asymmetric catalysis. We report studies that probe important structural features of the chiral cation and demonstrate that the ion-paired complexes can be formed from their individual components without a separate isolation step.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 29","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-05-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202507532","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144624575","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

Inside Back Cover: First Encapsulation of Organometallic Single-Molecule Magnet into Single-Walled Carbon Nanotubes (Angew. Chem. 22/2025) 内页后盖：首次将有机金属单分子磁铁封装到单壁碳纳米管中。化学22/2025)

Angewandte Chemie Pub Date : 2025-05-13 DOI: 10.1002/ange.202510024

Haitao Zhang, Ryo Nakanishi, Takefumi Yoshida, Masahiko Nishijima, Koji Harano, Yoji Horii, Masahiro Yamashita

引用次数: 0

Inside Front Cover: Giant Birefringence Enabled by the Highly Anisotropic Linear IX2- (X=Cl, Br) Building Blocks (Angew. Chem. 27/2025) 内页封面：由高度各向异性线性IX2- (X=Cl, Br)构建块实现的巨大双折射。化学27/2025)

Angewandte Chemie Pub Date : 2025-05-13 DOI: 10.1002/ange.202509837

Chong-An Chen, Yang Li, Hongbo Huang, Congcong Jin, Bingbing Zhang, Kang Min Ok

引用次数: 0

Crystallization/Precipitation Driven Nonequilibrium Ring-Opening Polymerization of Thiovalerolactone Toward Closed-Loop Recyclable Polythioester with Excellent Barrier Properties 结晶/沉淀驱动非平衡开环聚合制备具有优异阻隔性能的闭环可回收聚硫酯

Angewandte Chemie Pub Date : 2025-05-13 DOI: 10.1002/ange.202505104

Weijie Pei, Yiming Liu, Qin Yan, Kunlun Yuan, Sai Li, Prof. Yong Shen, Prof. Zhibo Li

引用次数: 0

Inside Back Cover: Photocatalytic Nitrogen Reduction for Ammonia Synthesis Accelerated by Overcoming Photo-Dember Effect (Angew. Chem. 26/2025) 内页后盖：克服光记忆效应加速氨合成的光催化氮还原。化学26/2025)

Angewandte Chemie Pub Date : 2025-05-13 DOI: 10.1002/ange.202509838

Peishen Li, Yixuan Gao, Alistair G. L. Borthwick, Panpan Li, Huixuan Zhang, Fangyuan Chen, Long Chen, Fan Li, Wen Liu

引用次数: 0

Intracellular Polymerization Induced Self-Assembly and Gold Nanocomposite Synthesis in Living Bacteria 活细菌胞内聚合诱导的自组装和金纳米复合材料的合成

Angewandte Chemie Pub Date : 2025-05-13 DOI: 10.1002/ange.202504936

Shiling Zhang, Jinying Yang, Jinyan Luo, Jiao Zhang, Mianqi Huang, Kui Tan, Prof. Gaojian Chen, Prof. Qi Xing, Prof. Hang Fai Kwok, Prof. Zhuojun Dai, Prof. Jin Geng

引用次数: 0

Outside Back Cover: Data–Knowledge-Dual-Driven Electrolyte Design for Fast-Charging Lithium Ion Batteries (Angew. Chem. 24/2025) 外后盖：数据-知识-双驱动电解液设计的快速充电锂离子电池(新。化学24/2025)

Angewandte Chemie Pub Date : 2025-05-13 DOI: 10.1002/ange.202510008

i Yang, Nan Yao, Yu-Chen Gao, Xiang Chen, Yu-Xin Huang, Shuo Zhang, Han-Bing Zhu, Lei Xu, Yu-Xing Yao, Shi-Jie Yang, Zheng Liao, Zeheng Li, Xue-Fei Wen, Peng Wu, Ting-Lu Song, Jin-Hao Yao, Jiang-Kui Hu, Chong Yan, Jia-Qi Huang, Qiang Zhang

引用次数: 0

Bridging Nano to Micron: Architectural Engineering of Supramolecular Bottlebrushes for Extensively Tunable Structures and Photonics 桥接纳米到微米：广泛可调结构和光子学的超分子瓶刷的建筑工程

Angewandte Chemie Pub Date : 2025-05-13 DOI: 10.1002/ange.202503633

Dezhi Liu, Dr. Zhenli Zhang, Yuxia Zhang, Prof. Dr. Yuesheng Li, Prof. Dr. Dong-Po Song

{"title":"Bridging Nano to Micron: Architectural Engineering of Supramolecular Bottlebrushes for Extensively Tunable Structures and Photonics","authors":"Dezhi Liu, Dr. Zhenli Zhang, Yuxia Zhang, Prof. Dr. Yuesheng Li, Prof. Dr. Dong-Po Song","doi":"10.1002/ange.202503633","DOIUrl":"https://doi.org/10.1002/ange.202503633","url":null,"abstract":"Supramolecular bottlebrush block copolymers (BBCPs) offer greater architectural adaptability than covalent BBCPs. However, the dynamic nature of non-covalent interactions hinders precise control over their chain architecture, resulting in poorly controlled self-assembly, unpredictable morphologies, and limited utility. Herein, we introduce a novel molecular design for amphiphilic supramolecular BBCPs that overcomes key challenges in the field. The resulting materials exhibit superior thermodynamic stability in weakly polar solvents. This enables the first demonstration of well-controlled self-assembly of supramolecular surfactants within a complex emulsion system, leading to the formation of photonic supraballs with homogenous porous structures. Critically, precise chain architectural engineering enables pore diameter tuning over an unprecedented nanometer-to-micrometer range (67 nm–1.92 µm), significantly surpassing the maximum domain sizes achievable with self-assembled covalent BBCPs. This extends the photonic bandgap into the mid-wave infrared range, paving the way for next-generation materials with potential applications in thermal management.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 29","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-05-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144624438","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0