Angewandte Chemie最新文献_第6页

Inside Front Cover: Metastable Macrocyclic Bis-Meisenheimer Adduct (Angew. Chem. 38/2025) 内页封面：亚稳态大环双-迈森海默加合物。化学38/2025)

Angewandte Chemie Pub Date : 2025-08-26 DOI: 10.1002/ange.202518392

Dr. Simon Pascal, Dr. Angélina Torres Ruiz, Aerin E. Baker, Prof. Douglas A. Vander Griend, Michel Giorgi, Aurélien Planchat, Prof. Denis Jacquemin, Dr. Olivier Siri

引用次数: 0

NitrOFF: An Engineered Fluorescent Biosensor to Illuminate Nitrate Transport in Living Cells NitrOFF：一种工程荧光生物传感器，用于照亮活细胞中硝酸盐的运输

Angewandte Chemie Pub Date : 2025-08-26 DOI: 10.1002/ange.202508058

Mariah A. Cook, Jonathan D. Smailys, Ke Ji, Shelby M. Phelps, Jasmine N. Tutol, Wantae Kim, Whitney S. Y. Ong, Weicheng Peng, Caden Maydew, Y. Jessie Zhang, Sheel C. Dodani

{"title":"NitrOFF: An Engineered Fluorescent Biosensor to Illuminate Nitrate Transport in Living Cells","authors":"Mariah A. Cook, Jonathan D. Smailys, Ke Ji, Shelby M. Phelps, Jasmine N. Tutol, Wantae Kim, Whitney S. Y. Ong, Weicheng Peng, Caden Maydew, Y. Jessie Zhang, Sheel C. Dodani","doi":"10.1002/ange.202508058","DOIUrl":"https://doi.org/10.1002/ange.202508058","url":null,"abstract":"The duality of nitrate is nowhere better exemplified than in human physiology—a detrimental pollutant but also a protective nutrient—particularly as connected to nitric oxide. Aside from limited insights into nitrate uptake and storage, foundational nitrate biology has lagged. Genetically encoded fluorescent biosensors can address this gap with real-time imaging, but such technologies for mammalian cell applications remain rare. Here, we designed and engineered a biosensor fusing the green fluorescent protein EGFP and the nitrate recognition domain NreA from Staphylococcus carnosus. Seven rounds of directed evolution and 15 mutations resulted in NitrOFF. NitrOFF has a high degree of allosteric communication between the domains reflected in a turn-off intensiometric response (Kd ≈ 9 µM). This was further reinforced by X-ray crystal structures of apo and nitrate-bound NitrOFF, which revealed a large-scale conformational rearrangement changing the relative positioning of the domains by 68.4°. This dramatic difference was triggered by the formation of a long helix at the engineered linker connecting the two domains, peeling the β7 strand off the EGFP and thus extinguishing the fluorescence upon nitrate binding. Finally, we highlighted the utility of NitrOFF to monitor exogenous nitrate uptake and modulation in the human embryonic kidney (HEK) 293 cell line.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 40","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145172032","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

Inside Front Cover: Reversing Pt/C Degradation Via Ni(OH)2-Wrapping Induced Spreading of Electric Field for Alkaline Hydrogen Evolution Reaction (Angew. Chem. 39/2025) 内页封面：通过Ni(OH)2包覆诱导电场扩散的碱性析氢反应逆转Pt/C降解（新）化学39/2025)

Angewandte Chemie Pub Date : 2025-08-26 DOI: 10.1002/ange.202518397

Yuzhu Chen, Jiajun She, Zizhun Wang, Wenwen Li, Fuxi Liu, Qing Liang, Kexin Song, Zhou Jiang, Xu Zou, Wei Zhang, Weitao Zheng

引用次数: 0

Force-Induced Ring Flipping in a Threaded Pillar[5]Arene 螺纹柱[5]Arene中力诱导的环翻转

Angewandte Chemie Pub Date : 2025-08-26 DOI: 10.1002/ange.202516485

Dr. Lei Chen, Dr. Tomás Nicolás-García, Dr. Igor Rončević, Prof. Dr. Guillaume De Bo

{"title":"Force-Induced Ring Flipping in a Threaded Pillar[5]Arene","authors":"Dr. Lei Chen, Dr. Tomás Nicolás-García, Dr. Igor Rončević, Prof. Dr. Guillaume De Bo","doi":"10.1002/ange.202516485","DOIUrl":"https://doi.org/10.1002/ange.202516485","url":null,"abstract":"Pillar[n]arenes are popular macrocycles used in various supramolecular systems and materials due to their unique host–guest properties and ease of synthesis. Their pillar shape originates from the cyclic arrangement of methylene-bridged hydroquinone groups. They usually exist in one of two conformations where all the hydroquinone rings are oriented in the same direction (left or right), which is the source of their planar chirality. However, the controlled formation of pillar[n]arenes with intermediate conformations, for example, where only one ring is inverted, remains a challenge. Here we show how mechanical force can be used to reach this elusive conformation via the force-induced flipping of a single hydroquinone ring in a pillar[5]arene-based rotaxane. We show that the flipping motion can be controlled with the shape of the stopper and the axle, as well as with the nature of the pillar[5]arene substituents. This flipping behavior acts as a mechanical damper by slowing the scission of the polymer under tension. These results show how mechanical force can be used to access synthetically challenging supramolecular architectures, and we anticipate that this new dampening mechanism will prove useful in the formation of tougher materials.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 41","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202516485","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145230704","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

Frontispiece: Reduction of CO2 Accompanying ATP Synthesis in Polydopamine Microreactors Covered by Lipid Bilayers with ATPase 前言：ATP酶脂质双层覆盖的聚多巴胺微反应器中伴随ATP合成的CO2减少

Angewandte Chemie Pub Date : 2025-08-25 DOI: 10.1002/ange.202583502

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Outside Front Cover: Thermodynamics of Water Displacement from Binding Sites and its Contributions to Supramolecular and Biomolecular Affinity (Angew. Chem. 35/2025) 外封面：水从结合位点位移的热力学及其对超分子和生物分子亲和力的贡献（新）。化学35/2025)

Angewandte Chemie Pub Date : 2025-08-25 DOI: 10.1002/ange.202516888

Dr. Jeffry Setiadi, Priv.-Doz. Dr. Frank Biedermann, Prof. Dr. Werner M. Nau, Prof. Dr. Michael K. Gilson

引用次数: 0

A Fluorogenic Hydrazino-Pictet–Spengler Reaction in Live Cells 活细胞中的荧光肼-皮塞特-斯宾格勒反应

Angewandte Chemie Pub Date : 2025-08-25 DOI: 10.1002/ange.202510959

Kaleena Basran, Prof. Nathan W. Luedtke

{"title":"A Fluorogenic Hydrazino-Pictet–Spengler Reaction in Live Cells","authors":"Kaleena Basran, Prof. Nathan W. Luedtke","doi":"10.1002/ange.202510959","DOIUrl":"https://doi.org/10.1002/ange.202510959","url":null,"abstract":"Lipid peroxidation generates diverse aldehydic lipids associated with oxidative stress and signaling, yet methodologies capable of their detection in live cells are currently lacking. Here, we report a fluorogenic hydrazino-Pictet–Spengler (HIPS) probe for lipidic aldehydes “FLipA-HIPS” that generates bright, wash-free fluorescent reaction products in vitro and in cellulo. FLipA-HIPS is essentially nonfluorescent but reacts with aldehydes to give an environmentally sensitive fluorophore with a higher quantum yield in SDS micelles as compared to aqueous buffer alone. FLipA-HIPS reacts with lipidic aldehydes to give 10- to 25-fold higher fluorescence intensities than reactions containing either short-chain aliphatic or aromatic aldehydes in aqueous buffer. Confocal microscopy shows that live cells pretreated with potassium bromate or the aldehydic phospholipid “POVPC” display rapid and selective FLipA-HIPS staining that co-localizes with the endoplasmic reticulum (ER), consistent with the ER's known role in accumulating lipidic aldehydes. These results demonstrate that HIPS reactions can exhibit useful fluorogenic properties for aldehyde biosensing applications in live cells.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 40","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-08-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202510959","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145172025","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

Carbon Dioxide Capture and Functionalization from a Molecular Ti(III) Oxo Anion 分子Ti（III）氧阴离子的二氧化碳捕获和功能化

Angewandte Chemie Pub Date : 2025-08-25 DOI: 10.1002/ange.202511532

Samuel S. Veroneau, Jacob S. Mohar, Mrinal Bhunia, Hannah Farber, Alexander L. Laughlin, Robert W. Voland, Alexandra Bacon, Michael R. Gau, Kyle M. Lancaster, Daniel J. Mindiola

{"title":"Carbon Dioxide Capture and Functionalization from a Molecular Ti(III) Oxo Anion","authors":"Samuel S. Veroneau, Jacob S. Mohar, Mrinal Bhunia, Hannah Farber, Alexander L. Laughlin, Robert W. Voland, Alexandra Bacon, Michael R. Gau, Kyle M. Lancaster, Daniel J. Mindiola","doi":"10.1002/ange.202511532","DOIUrl":"https://doi.org/10.1002/ange.202511532","url":null,"abstract":"Carbon dioxide capture and functionalization sequesters carbon dioxide in more robust products and offers a viable route to reducing greenhouse gas emissions. We present herein a unique molecular TiIII oxo anion that reversibly binds CO2 to allow both its sequestration and functionalization. The reduction of [(PN)2Ti═O] (1) [PN = (2-PiiPr2-4-methylphenyl)(mesityl)amide] with KC8 and 2.2.2-cryptand (crypt) resulted in formation of [K(crypt)][(PN)2Ti═O] (2), which was fully characterized and shown to contain a Ti-centered radical. Complex 2 reacts with Al(CH3)3 to form [K(crypt)][(PN)2Ti{O(Al(CH3)3}] (3), which can be independently prepared from [K(crypt)][(PN)2Ti(OCP)] and Al(CH3)3. Whereas 1 does not react with CO2, 2 rapidly captures the gas (1 atm, 25 °C) to produce a TiIII carbonate [K(crypt)][(PN)2Ti(κ2-O2C═O)] (4). Chemical and electrochemical oxidation of 4 releases CO2 to regenerate 1 while a soluble organic carbonate [Me3SiOC(O)OSiMe3, Me = CH3] is obtained from reaction of 4 with ClSiMe3.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 40","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-08-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202511532","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145172026","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

Molecular Afterglow of Lophine-Based Luminophore and Its Imaging Applications 洛芬基发光团的分子余辉及其成像应用

Angewandte Chemie Pub Date : 2025-08-25 DOI: 10.1002/ange.202507174

Jun Yang, Yusheng Yang, Huizhe Wang, Steven H. Liang, Chongzhao Ran

{"title":"Molecular Afterglow of Lophine-Based Luminophore and Its Imaging Applications","authors":"Jun Yang, Yusheng Yang, Huizhe Wang, Steven H. Liang, Chongzhao Ran","doi":"10.1002/ange.202507174","DOIUrl":"https://doi.org/10.1002/ange.202507174","url":null,"abstract":"Lophine, the first chemiluminescent compound discovered in history, has rarely been applied for in vivo imaging since its discovery in 1877. In this report, we demonstrate that lophine's chemiluminescence emission could be significantly enhanced by caging the imidazole moiety via molecular afterglow mechanism. Notably, our study revealed a rare superoxide anion-mediated luminescence. Our novel probes JIMI-11 and JIMI-12 could be used for in vivo mouse imaging. Compared to its uncaged form JIMI-6, JIMI-11 exhibited a significant enhancement (126-fold) in vitro and a 190-fold higher emission signal in vivo. JIMI-11 selectively accumulates in white adipose tissues (WAT) and can be used to monitor changes in WAT mass in a mouse model of type-1 diabetes. Additionally, it can assess the therapeutic effects of Semaglutide in a mouse model of diet-induced obesity. Lastly, we designed JIMI-12 with a reactive oxygen/nitrogen species (ROS/RNS) responsive moiety as the caging group and demonstrated its utility for in vivo imaging of ROS in a lipopolysaccharide (LPS)-induced inflammatory mouse model. Our studies suggest that re-designing lophine-based probes could unlock their potential for both in vitro and in vivo applications. The ability to switch from chemiluminescence to molecular afterglow introduces a novel approach to designing imaging probes.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 41","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-08-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145230810","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

Optical Force Monitoring in Polymeric Materials with a Coumarin-Based Mechanophore 基于香豆素的机械团在高分子材料中的光力监测

Angewandte Chemie Pub Date : 2025-08-25 DOI: 10.1002/ange.202513283

Yang Li, Jess M. Clough

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