Angewandte Chemie最新文献_第10页

Inside Back Cover: Flexibility-Aided Orientational Self-Sorting and Transformations of Bioactive Homochiral Cuboctahedron Pd12L16 (Angew. Chem. 37/2025) 内后盖：生物活性同手性立方面体Pd12L16的柔性辅助取向自分类和转化（新）。化学37/2025)

Angewandte Chemie Pub Date : 2025-08-21 DOI: 10.1002/ange.202517790

Subhasis Chattopadhyay, Robin Durník, Dr. Anniina Kiesilä, Dr. Elina Kalenius, Dr. Juha M. Linnanto, Assoc.Prof. Pavel Babica, Dr. Jan Kuta, Prof.Dr. Radek Marek, Dr. Ondřej Jurček

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Photocatalytic Synthesis of Unprotected Sulfonimidamides and Their Application in Photochemical Nitrene Transfer Reactions 无保护磺胺类化合物的光催化合成及其在光化学亚硝基转移反应中的应用

Angewandte Chemie Pub Date : 2025-08-21 DOI: 10.1002/ange.202509870

Ivan Sliusarevskyi, Jordan Diaz, Sudip Senapati, Ben J. Ebel, Nico J. Linnartz, Prof. Dr. Iris M. Oppel, Dr. Claire Empel, Prof. Dr. Philip Wai Hong Chan, Prof. Dr. Rene M. Koenigs

{"title":"Photocatalytic Synthesis of Unprotected Sulfonimidamides and Their Application in Photochemical Nitrene Transfer Reactions","authors":"Ivan Sliusarevskyi, Jordan Diaz, Sudip Senapati, Ben J. Ebel, Nico J. Linnartz, Prof. Dr. Iris M. Oppel, Dr. Claire Empel, Prof. Dr. Philip Wai Hong Chan, Prof. Dr. Rene M. Koenigs","doi":"10.1002/ange.202509870","DOIUrl":"10.1002/ange.202509870","url":null,"abstract":"The selective incorporation of nitrogen into organic molecules remains a central challenge in modern synthetic chemistry, particularly when aiming to access complex, functionalized scaffolds under mild and sustainable conditions. In this report, we describe a photocatalytic method that employs hydroxylamine-derived nitrene precursors and unprotected sulfinamides under mild conditions, enabling efficient nitrene transfer without the need for stoichiometric amounts of an oxidant. The resulting unprotected sulfonimidamides serve not only as target compounds but also as versatile intermediates for further nitrene-transfer reactions, affording complex sulfur–nitrogen-rich frameworks. Mechanistic studies support a photoinduced single-electron transfer process involving a reactant complex between the photocatalyst and nitrene precursor. This work establishes a general and modular platform for accessing challenging architectures based on sulfonimidamides, expanding the toolkit for late-stage functionalization and heteroatom-rich molecule construction.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 39","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-08-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202509870","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145129207","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}

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Bioorthogonal In Situ Formation of AIE Luminogens for Imaging Disease Progression via Sigmoidal Signal Amplification 通过s型信号放大成像疾病进展的AIE发光原的生物正交原位形成

Angewandte Chemie Pub Date : 2025-08-21 DOI: 10.1002/ange.202511705

Xinyu Yu, Xirui Liu, Prof. Hongbao Sun, Tianruo Shen, Yingqiao Deng, Prof. Haiyan Ren, Peixuan Zou, Prof. Yongxiang Zheng, Prof. Peihong Xiao, Prof. Qiyong Gong, Prof. Meng Qin, Prof. Xiaogang Liu, Prof. Haoxing Wu

{"title":"Bioorthogonal In Situ Formation of AIE Luminogens for Imaging Disease Progression via Sigmoidal Signal Amplification","authors":"Xinyu Yu, Xirui Liu, Prof. Hongbao Sun, Tianruo Shen, Yingqiao Deng, Prof. Haiyan Ren, Peixuan Zou, Prof. Yongxiang Zheng, Prof. Peihong Xiao, Prof. Qiyong Gong, Prof. Meng Qin, Prof. Xiaogang Liu, Prof. Haoxing Wu","doi":"10.1002/ange.202511705","DOIUrl":"https://doi.org/10.1002/ange.202511705","url":null,"abstract":"Aggregation-induced emission (AIE) luminogens are promising tools for biological imaging, yet their utility is often limited by nonspecific aggregation and elevated background fluorescence. Here, we present a bioorthogonal in situ formation strategy that enables precise, organelle-specific activation of AIEgens within live cells. This system employs a dual-lock mechanism—combining tetrazine quenching and twisted intramolecular charge shuttle (TICS) dynamics—to maintain an ultra-low fluorescence background in the precursor state, even under aggregating conditions. Upon bioorthogonal reactions and molecular aggregation, the resulting AIEgens exhibit tunable emission peaks ranging from 605 to 665 nm, large Stokes shifts (up to 201 nm), and an exceptional fluorescence enhancement (up to 1033-fold). Their high biocompatibility and spatial precision allow for multiplexed, simultaneous labeling of intracellular targets. Compared to conventional fluorogenic and bioorthogonal probes, these AIEgens exhibit a sigmoidal amplification response, enabling the sensitive discrimination of subtle biomarker expression differences and the effective identification of injured cells during disease progression. This strategy significantly enhances the specificity and sensitivity of live-cell imaging, expands the functional utility of AIE luminogens, and offers a versatile platform for high-resolution, multiplexed bioimaging in biomedical research and diagnostics.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 40","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-08-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145171994","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

Outside Front Cover: Conditional Stabilization of the Hypoxia-Inducible Factor HIF1α: Photoswitchable Stapled Peptides Prevent Elongin BC–Mediated Degradation (Angew. Chem. 36/2025) 外封面：缺氧诱导因子HIF1α的条件稳定：光开关钉接肽防止长链蛋白bc介导的降解（新）。化学36/2025)

Angewandte Chemie Pub Date : 2025-08-21 DOI: 10.1002/ange.202517898

Dr. Van Tuan Trinh, Dr. Sabrina Fischer, Dr. Lei Zhang, Dr. Heiko Geisler, Belen Pardo, Dr. Robert Liefke, Dr. Frank Abendroth, Prof.Dr. Olalla Vázquez

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Ensemble of Active Acid Sites on Amorphous Silica–Alumina Surfaces for Catalytic Cracking 无定形二氧化硅-氧化铝表面活性酸位系综催化裂化

Angewandte Chemie Pub Date : 2025-08-21 DOI: 10.1002/ange.202506711

Dr. Kaustubh J. Sawant, Dr. David Stockwell, Dr. Anthony Debellis, Lucas Dorazio, Prof. Philippe Sautet

{"title":"Ensemble of Active Acid Sites on Amorphous Silica–Alumina Surfaces for Catalytic Cracking","authors":"Dr. Kaustubh J. Sawant, Dr. David Stockwell, Dr. Anthony Debellis, Lucas Dorazio, Prof. Philippe Sautet","doi":"10.1002/ange.202506711","DOIUrl":"https://doi.org/10.1002/ange.202506711","url":null,"abstract":"Amorphous silica–alumina are critical materials in catalysis, particularly for fluid catalytic cracking (FCC). However, the atomic scale understanding of the active sites has been challenging, because of the nonuniform atomic distribution and the material's amorphous nature. Here, we use density functional theory (DFT), machine learning potentials and sampling methods to investigate the relationship between structure and acidity in silica-modified alumina. Under FCC conditions, we predict an ensemble of acid sites with diverse local structures and a spectrum of acid strengths, including zeolite-like bridging Brønsted acid sites (BAS) and pseudo-bridging silanol BAS. This distribution is influenced by surface structure, Si coverage, and extent of hydroxylation, shaped by synthesis methods and reaction conditions. Experiments using a model Si-stabilized alumina catalyst confirm that Brønsted acidity increases with Si content, peaking at an optimal value before declining. These insights provide a foundation for designing efficient solid acid catalysts for industrial applications.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 38","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-08-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145062558","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}

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Accelerated Porosity Screening Using a Multichannel Colorimetric Array 使用多通道比色阵列加速孔隙度筛选

Angewandte Chemie Pub Date : 2025-08-21 DOI: 10.1002/ange.202510400

Yushu Han, Dr. Isaiah Borne, Dr. Biplab Dutta, Rob Clowes, Dr. Hang Qu, Dr. Alex James, Dr. Charlotte E. Boott, Dr. Marc A. Little, Prof. Andrew I. Cooper

{"title":"Accelerated Porosity Screening Using a Multichannel Colorimetric Array","authors":"Yushu Han, Dr. Isaiah Borne, Dr. Biplab Dutta, Rob Clowes, Dr. Hang Qu, Dr. Alex James, Dr. Charlotte E. Boott, Dr. Marc A. Little, Prof. Andrew I. Cooper","doi":"10.1002/ange.202510400","DOIUrl":"https://doi.org/10.1002/ange.202510400","url":null,"abstract":"Porous materials are important for many technologies, but the measurement of porosity by gas adsorption isotherms is slow, taking around one day per sample using a single-port gas sorption analyzer, even when using a “quick” analysis method with relatively few data points. With the increased use of automated platforms for material generation, porosity analysis is now frequently the bottleneck in the discovery of new porous materials. Here, we present a semiautomated pre-screening strategy that uses dye adsorption to create a colorimetric array that is combined with computer vision analysis for porosity screening. By using a six-dye multichannel array and a defined porosity threshold, our method rapidly screened 50 candidate materials that spanned molecular solids, polymers, and metal–organic frameworks. The method showed a 98–100% classification accuracy compared with gas uptake measurements. While this method is more qualitative than quantitative, it is more than 30 times faster than conventional gas sorption measurements, and it has the scope to be made much faster with greater parallelization and automation. This makes this colorimetric method suitable for pre-screening arrays of materials to choose samples that merit more detailed conventional porosity analysis.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 40","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-08-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202510400","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145171997","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

Fe-Triazolate Metal–Organic Frameworks as Water Oxidation Catalysts with Dual Photoanode Functionality 具有双光阳极功能的三氮酸铁金属-有机骨架水氧化催化剂

Angewandte Chemie Pub Date : 2025-08-21 DOI: 10.1002/ange.202513556

Jully Patel, Naduvile Purayil Dileep, Vladimir Bondar, Priya Gopal, Anton V. Sinitskiy, Sergei Savikhin, Yulia Pushkar

{"title":"Fe-Triazolate Metal–Organic Frameworks as Water Oxidation Catalysts with Dual Photoanode Functionality","authors":"Jully Patel, Naduvile Purayil Dileep, Vladimir Bondar, Priya Gopal, Anton V. Sinitskiy, Sergei Savikhin, Yulia Pushkar","doi":"10.1002/ange.202513556","DOIUrl":"https://doi.org/10.1002/ange.202513556","url":null,"abstract":"Artificial photosynthesis is an emerging technology that achieves renewable fuels, such as hydrogen, from sunlight. Its realization depends on finding highly active and stable catalysts of water splitting and photoactive materials for light absorption. To be scalable, these should contain only abundant elements. Here, for the first time, Fe-triazolate (Fe(ta)2) and its metal substituted derivatives (Fe-Metal(ta)2) Metal-organic frameworks (MOFs) are characterized as new dual-function materials for photo-absorption and water oxidation catalysis in acidic media. The materials were studied by a range of structural, spectroscopic, and computational density functional theory (DFT) techniques. Fe(ta)2 and Fe-Mn(ta)2 were found to be highly active and stable in chemical and photochemical water oxidation, and in addition function as photoanodes, with photo-electrocatalytic currents (∼2.00 x 10−3 Acm−2 at + 1.4 V vs. Ag/AgCl) at pH = 1. The possibility of a unique catalytic mechanism where O─O bond formation is possible from the coupling of two adjacent FeIV = O fragments was demonstrated by DFT analysis. Thus, Fe-triazolate MOF has been established as a new, stable, scalable, versatile, and efficient platform for sustainable energy conversion in the realm of artificial photosynthesis.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 40","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-08-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202513556","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145171999","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}

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SuFEx-Enabled Polypeptide: Creating Diversified Properties with Minimal Preset Conditions SuFEx-Enabled多肽：用最小的预设条件创建多样化的属性

Angewandte Chemie Pub Date : 2025-08-21 DOI: 10.1002/ange.202504496

Ying Liu, Yajie Chen, Xue-Ao Mei, Shengwen Duan, Yugang Bai

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Non-Fused Conjugated Alkylfluorene Bridged Naphthalimides Cathode Interlayer Enables Low-Noise Near-Infrared Organic Photodiodes 非熔融共轭烷基芴桥接萘酰亚胺阴极中间层实现低噪声近红外有机光电二极管

Angewandte Chemie Pub Date : 2025-08-21 DOI: 10.1002/ange.202514390

Yueyue Wang, Minming Yan, Shunyu Wang, Danni Chen, Qilin Zhang, Yi Su, Dongwen Zou, Meili Xu, Hong Chen, Hong Meng

{"title":"Non-Fused Conjugated Alkylfluorene Bridged Naphthalimides Cathode Interlayer Enables Low-Noise Near-Infrared Organic Photodiodes","authors":"Yueyue Wang, Minming Yan, Shunyu Wang, Danni Chen, Qilin Zhang, Yi Su, Dongwen Zou, Meili Xu, Hong Chen, Hong Meng","doi":"10.1002/ange.202514390","DOIUrl":"https://doi.org/10.1002/ange.202514390","url":null,"abstract":"The cathode interface layers (CILs) play a crucial role in enhancing the performance of organic photodiodes (OPDs). However, the poor film formation, the tendency of orientation and aggregation, and contact in the interface of the bulk heterojunction (BHJ)/CILs/electrode increase the dark current, leading to a limitation of light detection. In this study, we designed and synthesized a nonfused conjugated small molecule (FNA) with dioctyl fluorene (F) as the π-bridge and N-dimethylaminopropyl-1,8-naphthalimide (NA) as terminal groups. As the CIL, it significantly modifies the interfaces of BHJ/CILs/electrode and minimizes dark current density (Jd). Using PTB7-Th:IEICO-4F as the BHJ, FNA-based OPDs achieve a remarkably low Jd of 1.12 × 10−8 A cm−2 (at −0.5 V) and a peak specific detectivity of 8.23 × 1012 Jones (940 nm), outperforming conventional devices with PDINN as CIL. These improvements are attributed to lower Jd by modified interfacial contact and increased photoresponse by reducing depletion region width in FNA-based photodiodes. Furthermore, uniform photoresponse in 5 × 5 OPD pixel arrays further validates its potential for imaging applications.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 41","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-08-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145230782","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}

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Divergent Synthesis of ΔAA-Peptides Using a Bioorthogonal pro-Amino Acid and Aqueous Flavin Photocatalyst: Green Light Enhances Catalyst Performance and Product Selectivity 使用生物正交前氨基酸和黄素光催化剂的发散合成ΔAA-Peptides：绿光增强催化剂性能和产物选择性

Angewandte Chemie Pub Date : 2025-08-21 DOI: 10.1002/ange.202511832

Pei-Hsuan Chen, Steven Bloom

{"title":"Divergent Synthesis of ΔAA-Peptides Using a Bioorthogonal pro-Amino Acid and Aqueous Flavin Photocatalyst: Green Light Enhances Catalyst Performance and Product Selectivity","authors":"Pei-Hsuan Chen, Steven Bloom","doi":"10.1002/ange.202511832","DOIUrl":"10.1002/ange.202511832","url":null,"abstract":"Dehydroamino acids (ΔAAs) are vital building blocks in the design and optimization of peptide drugs. The exact olefin geometry, side chain chemotype, and ancillary β-carbon substituents play a significant role. Unfortunately, general approaches to install these motifs into peptides are lacking, complicated by the instability of unsaturated residues during traditional amide-bond coupling and failure of divergent protocols, such as oxidative Heck and Horner–Wadsworth–Emmons, to accommodate a complete range of substrate classes. Herein, we conceive and interrogate an original bioorthogonal reagent, β-sulfonyldehydroamino acid (ΔSulf), that can be site-specifically encoded into standard peptides through solid- or liquid-phase synthesis. When combined with an aqueous flavin photocatalyst, myriad boronic acids and 525 nm light—a more biologically benign portion of the flavin visible absorption spectra that has not previously been exploited for flavin photoredox catalysis,—this latent residue becomes one of several (Z)-ΔAA variants (aromatic, heteroaromatic, aliphatic) via stereoretentive radical conjugate addition and β-scission. The importance of green light is established through mechanistic studies showing that it tempers radical formation and discourages flavin-catalyzed isomerization, controlling product selectivity. We apply our original reagent and catalytic platform in a brief medicinal chemistry campaign to discover tetrapeptides that modulate Aβ42 aggregation for the treatment of Alzheimer's disease.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 39","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-08-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145129208","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