Angewandte Chemie International Edition最新文献_第3页

Photocatalytic Isomerization of Stilbenes via Molecular Recognition With a Dual‐Function η 6 –Arene Catalyst 双功能η 6 -芳烃催化二苯乙烯分子识别的光催化异构化

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-17 DOI: 10.1002/anie.7628311

Yunzhi Lin, Kaifan Zhang, Hang Luo, Xinlei Zong, Bing Gu, Hang Shi

{"title":"Photocatalytic Isomerization of Stilbenes via Molecular Recognition With a Dual‐Function η 6 –Arene Catalyst","authors":"Yunzhi Lin, Kaifan Zhang, Hang Luo, Xinlei Zong, Bing Gu, Hang Shi","doi":"10.1002/anie.7628311","DOIUrl":"https://doi.org/10.1002/anie.7628311","url":null,"abstract":"Electron donor–acceptor (EDA) complexes, formed through noncovalent interactions between electron‐rich and electron‐deficient species, can undergo photoinduced charge transfer to access reactive radical intermediates. However, rapid and unproductive back electron transfer (BET) limits their synthetic utility. Herein, we report a dual‐function ( η 6 –arene)rhodium(III) catalyst that enables contra ‐thermodynamic E ‐to‐ Z isomerization of stilbenes via selective EDA complexation. In contrast to well‐studied photoisomerization reactions driven by triplet photosensitizers via intermolecular energy transfer (EnT), photoexcitation of the self‐assembled EDA complex generates a charge‐separated singlet exciplex that undergoes back electron transfer coupled with intersystem crossing to populate a localized triplet‐state olefin intermediate. The catalyst plays two pivotal roles: the metal‐bound arene scaffold enables molecular recognition of planar ( E )‐stilbenes over twisted ( Z )‐isomers through noncovalent interactions, while the heavy rhodium atom promotes ISC.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"27 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2026-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149198984","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Dimensional Reduction of Transition Metal Dichalcogenides by Oxide Insertion: Quasi‐1D Oxychalcogenide Semiconductors 通过氧化物插入降低过渡金属二硫族化合物的尺寸：准一维二硫族化合物半导体

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-17 DOI: 10.1002/anie.1906484

Ayat Tassanov, Azamat Yessengazin, Huiju Lee, Pedro R. Trinidad‐Pérez, Daniel G. Chica, Yi Xia, James M. Hodges

{"title":"Dimensional Reduction of Transition Metal Dichalcogenides by Oxide Insertion: Quasi‐1D Oxychalcogenide Semiconductors","authors":"Ayat Tassanov, Azamat Yessengazin, Huiju Lee, Pedro R. Trinidad‐Pérez, Daniel G. Chica, Yi Xia, James M. Hodges","doi":"10.1002/anie.1906484","DOIUrl":"https://doi.org/10.1002/anie.1906484","url":null,"abstract":"Heteroanionic solids offer unique levers for tuning structures and properties, but accessing multianion phase space remains challenging due to mismatches in anion reactivity. Here, we describe a new family of A 2 Hf 3 Q 6 O (A = K, Rb, Cs; Q = S, Se) oxychalcogenides, the first reported in the A─Hf─Q─O quaternary space, which are prepared by reacting HfQ 2 with the corresponding alkali carbonate (A 2 CO 3 ). The resulting structures are dimensionally reduced variants of the 1T‐HfQ 2 parent phase, where rows of O atoms insert into the transition metal dichalcogenide (TMD) layers. This yields nanometer‐wide 1D‐[Hf 3 Q 6 ] ribbons that link into step‐like sheets through distinctive Hf─O─Hf bridges, which connect heteroleptic HfQ 5 O polyhedra at the ribbon edges. UV/Vis and photoluminescence spectra reveal tunable absorption and emission features spanning 1.8–2.6 eV. Calculated band structures show direct‐gap transitions and highly dispersive bands along the [Hf 3 Q 6 ] nanoribbons, yielding effective masses more than two orders of magnitude lower than in other crystallographic directions. Charge‐density plots further illustrate quasi‐1D electronic anisotropy, showing frontier orbitals confined to the nanoribbons due to covalent Hf─Q bonding. We anticipate heteroanion‐driven dimensional reduction can be used to engineer anisotropy in semiconductors and offers new routes to synthetically challenging multianion systems.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"30 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2026-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149208495","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Topology‐Derived Closed Pores in Hard Carbon Boost Sodium‐Ion Storage 硬碳增强钠离子存储的拓扑封闭孔

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-17 DOI: 10.1002/anie.6016795

Hesheng Yu, Xinying Wang, Xi Liu, Ziheng Zhang, Daiqian Chen, Fuyong Liu, Yuping Wu, Yuanfu Chen, Jiarui He

{"title":"Topology‐Derived Closed Pores in Hard Carbon Boost Sodium‐Ion Storage","authors":"Hesheng Yu, Xinying Wang, Xi Liu, Ziheng Zhang, Daiqian Chen, Fuyong Liu, Yuping Wu, Yuanfu Chen, Jiarui He","doi":"10.1002/anie.6016795","DOIUrl":"https://doi.org/10.1002/anie.6016795","url":null,"abstract":"The closed‐pore architecture of hard carbon governs reversible capacity, initial Coulombic efficiency (ICE), and Na‐storage kinetics, but its precise regulation and the underlying mechanism remain elusive. To address such issues, a molecular‐cavity engineering strategy is developed using cyclic molecular precursors, whose inherent cavities are preserved by low‐temperature cross‐linking, to construct topology‐derived intrinsic closed pores in hard carbon during carbonization. Using β‐cyclodextrin as a model precursor, the resulting hard carbon (β‐ICHC) delivers a reversible capacity of 410.2 mAh g −1 , an ICE of 94.7% and 99.7% capacity retention over 300 cycles. Combined theoretical and in situ/ex situ analyses reveal that intrinsic closed pores simultaneously enable high reversible capacity, high ICE, and fast Na‐storage kinetics: the intrinsic closed pores with sub‐0.35 nm electrolyte‐sieving mouths can not only serve as reversible Na‐storage spaces to increase capacity but also suppress irreversible Na + consumption to enhance ICE; the pseudo‐graphitic walls with enlarged interlayer spacing enable fast Na + transport and provide additional capacity. Furthermore, a three‐stage Na‐storage mechanism of surface/defect adsorption, closed‐pore‐wall adsorption, and closed‐pore filling is supported by the combined experimental and theoretical results. This work provides a paradigm for hard‐carbon structural design and offers new insight into sodium‐storage mechanisms.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"34 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2026-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149208504","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Inside Back Cover: Supramolecular Self-Assembly Enables Controlled Lithium Replenishment Toward High-Performance and Sustainable Regeneration of Spent LiFePO4 Batteries (Angew. Chem. Int. Ed. 43/2026) 内页后盖：超分子自组装使可控锂补充朝着高性能和可持续再生的废LiFePO4电池（新）。化学。Int。艾德。43/2026)

IF 17.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-17 Epub Date: 2026-09-28 DOI: 10.1002/anie.2026-m2509022200

Yixin Lin, Tiansheng Wang, Chaochao Gao, Jie Xu, Jiawen Chen, Zixi Lin, Guanghao Mao, Weihao Gao, Yixuan Tang, Jiaheng Zhang

引用次数: 0

SO2-Mediated 2e−, 4e−, and 6e− Reductions: Facile Access to Aryl Amines 二氧化硫介导的2e -， 4e -和6e -还原：对芳基胺的快速获取

IF 17.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-17 Epub Date: 2026-08-27 DOI: 10.1002/anie.3181079

Partha Protim Dey, Paramita Datta, Pallabi Mandal, Anex Jose, Swadhin K. Mandal

{"title":"SO2-Mediated 2e−, 4e−, and 6e− Reductions: Facile Access to Aryl Amines","authors":"Partha Protim Dey, Paramita Datta, Pallabi Mandal, Anex Jose, Swadhin K. Mandal","doi":"10.1002/anie.3181079","DOIUrl":"10.1002/anie.3181079","url":null,"abstract":"<div>\u0000 \u0000 Traditional electron-transfer catalysis frequently requires complex procedures to separate the catalyst from the reaction mixture. In contrast, a concept of a gas-mediated redox process may offer unique advantages, including its facile removal from the reaction medium. However, such a concept has remained unknown. Addressing this gap, we report the use of the SO2 gas molecule as an electron-transfer mediator by generating the sulfur dioxide radical anion (SO2•−) under ambient and chemical conditions. Such SO2•− enabled chemoselective, controlled, and scalable multi-electron reductions (2e−/2H+, 4e−/4H+, 6e−/6H+) of diverse nitrogen-containing substrates. Furthermore, the method was successfully applied to the synthesis of clinically active drugs on a multi-gram scale. Therefore, this work establishes a new paradigm in redox chemistry, demonstrating that a gas molecule can act as an electron-transfer catalyst, capable of performing reactions that typically require transition metals.\u0000 </div>","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"65 43","pages":""},"PeriodicalIF":17.6,"publicationDate":"2026-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148821661","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Development of a Potent QS‐21‐Derived Adjuvant Photoaffinity Probe: Identification of Cathepsin D as the Molecular Receptor 强效QS‐21衍生佐剂光亲和探针的开发：组织蛋白酶D作为分子受体的鉴定

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-17 DOI: 10.1002/anie.5055772

Abhijit Saha, Alba Mosteiro‐Couso, Adrián Plata, Carlo Pifferi, Priscila Tonon‐Baschirotto, Iker Oyenarte, June Ereño‐Orbea, Mikel Azkargorta, Félix Elortza, Juan Anguita, Alberto Fernández‐Tejada

{"title":"Development of a Potent QS‐21‐Derived Adjuvant Photoaffinity Probe: Identification of Cathepsin D as the Molecular Receptor","authors":"Abhijit Saha, Alba Mosteiro‐Couso, Adrián Plata, Carlo Pifferi, Priscila Tonon‐Baschirotto, Iker Oyenarte, June Ereño‐Orbea, Mikel Azkargorta, Félix Elortza, Juan Anguita, Alberto Fernández‐Tejada","doi":"10.1002/anie.5055772","DOIUrl":"https://doi.org/10.1002/anie.5055772","url":null,"abstract":"The saponin natural product QS‐21 is a potent immunological adjuvant used in human vaccines to enhance the immune response but suffers from scarcity, instability, and dose‐limiting toxicity, precluding its advancement as a stand‐alone adjuvant. Further, putative cellular receptor(s) and its molecular mechanisms of action are unknown, which has prevented the rational design of saponin adjuvants, emphasizing the need for discovering these receptors and elucidating mechanisms. Herein, we have developed novel saponin photoaffinity probes for molecular target identification, merging synthetic chemistry, photoaffinity labeling, and chemical proteomics. One of these potent adjuvants generated superior antibody responses to QS‐21 with less toxicity and enabled identification of Cathepsin D (CatD) as the selective receptor driving saponin adjuvant effects. Binding to surface‐exposed CatD, lipid raft interactions, and lysosomal acidification were shown to be key for CatD‐mediated saponin‐induced immune activation, whereas neither photocrosslinking nor apparent binding was observed in comparative experiments with other lysosomal cathepsins, confirming the specificity of the interaction. These studies highlight the promise of this saponin probe as a potent vaccine adjuvant, unveiling CatD as the molecular target. This breakthrough sets the stage for elucidating the precise mechanisms of saponin immunopotentiation, facilitating rational adjuvant design and development of optimized adjuvant–antigen combinations for future vaccines.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"10 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2026-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149208503","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Regulating What We Cannot Yet Measure? A Scientific Perspective on Polymeric PFASs, Total Fluorine, and the PFAS Fluorine Gap 监管我们还无法衡量的东西？聚合物全氟化合物、全氟化合物和全氟化合物氟差距的科学观点

IF 17.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-17 Epub Date: 2026-09-10 DOI: 10.1002/anie.6774558

Jörg Feldmann, Raquel Gonzalez de Vega, Viktoria Müller

{"title":"Regulating What We Cannot Yet Measure? A Scientific Perspective on Polymeric PFASs, Total Fluorine, and the PFAS Fluorine Gap","authors":"Jörg Feldmann, Raquel Gonzalez de Vega, Viktoria Müller","doi":"10.1002/anie.6774558","DOIUrl":"10.1002/anie.6774558","url":null,"abstract":"<div>\u0000 \u0000 Class-based regulation of per- and polyfluoroalkyl substances (PFASs) requires analytical metrics that are both scientifically meaningful and operationally enforceable. The proposed EU REACH restriction uses total fluorine (TF), extractable or adsorbable organic fluorine (EOF/AOF), targeted PFAS analysis, and non-target analysis as complementary lines of evidence. We argue that these approaches are valuable, but they do not measure the same chemical quantity. While TF is a useful conservative gatekeeper for fluorinated materials, it cannot distinguish between polymeric PFASs, inorganic fluorine, volatile precursors, or fluorinated substances that may or may not fall within broad PFAS definitions. This limitation is especially important for polymeric PFASs, including both backbone fluoropolymers and side-chain fluorinated polymers, which can be non-extractable, particulate, or transformable into mobile precursors such as fluorotelomer alcohols. We propose an analytical decision tree that separates bulk fluorine screening, extractable fractions, volatile and semi-volatile PFASs, polymeric and particulate PFASs, and structurally confirmed molecular PFASs. Such an operational framework would preserve the regulatory value of fluorine screening while avoiding overinterpretation of any single metric as “PFAS content”. PFAS content should be assessed by what is there not by what can easily be measured.\u0000 </div>","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"65 43","pages":""},"PeriodicalIF":17.6,"publicationDate":"2026-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148915264","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Enthalpy-Entropy Molecular Design of Gel Polymer Electrolytes for Regulating Solvation Chemistry in Lithium–Sulfur Batteries 调节锂硫电池溶剂化化学的凝胶聚合物电解质的焓熵分子设计

IF 17.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-17 Epub Date: 2026-08-17 DOI: 10.1002/anie.7695165

Zirui Guo, Zihui Song, Runyue Mao, Naiwen Hu, Chang Su, Shuo Zhuo, Xigao Jian, Fangyuan Hu

{"title":"Enthalpy-Entropy Molecular Design of Gel Polymer Electrolytes for Regulating Solvation Chemistry in Lithium–Sulfur Batteries","authors":"Zirui Guo, Zihui Song, Runyue Mao, Naiwen Hu, Chang Su, Shuo Zhuo, Xigao Jian, Fangyuan Hu","doi":"10.1002/anie.7695165","DOIUrl":"10.1002/anie.7695165","url":null,"abstract":"<div>\u0000 \u0000 Gel polymer electrolytes (GPEs) show great promise in lithium–sulfur (Li–S) batteries, but their practical application is limited by the high enthalpy of Li+ desolvation and the slow conversion rate of polysulfides, which disrupt the redox pathway and accelerate capacity decay. Here, we propose an enthalpy-entropy molecular design strategy to integrate these processes into a unified electrolyte system. By regulating the solvation structures of Li+ and polysulfides, we can both restrict available reaction pathways and control the coordination environment of polysulfides within the solvation structure. By modulating the solvation structure, we reduce the desolvation enthalpy of both Li+ and polysulfides, thereby promoting uniform nucleation of Li2S. This pioneering design enables the resulting GPE with an ionic conductivity of up to 1.21 mS cm−1 at 22°C and a Li+ transference number of 0.82, the resulting Li||Li symmetric cell can cycle stably for over 2250 h. Consequently, the cell exhibits an ultralow capacity fading rate of 0.043% per cycle over 1000 cycles at 2C and remained functional when assembled into a 1.8 Ah pouch-cell (403.7 Wh kg−1). This study highlights the crucial role of enthalpy-entropy molecular design strategies in GPEs.\u0000 </div>","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"65 43","pages":""},"PeriodicalIF":17.6,"publicationDate":"2026-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148729248","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Günther Jung (1937–2026): A Pioneer of Molecular Immunology 格<s:1>纳尔·荣格（1937-2026）：分子免疫学的先驱

IF 17.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-17 Epub Date: 2026-09-16 DOI: 10.1002/anie.2797694

Annette Beck-Sickinger, Roderich D. Süssmuth, Karl-Heinz Wiesmüller

引用次数: 0

Dynamic Soft‐Confinement via Hydrogen‐Bonded Organic Frameworks Reshapes C–C Coupling Interfacial Chemistry at Bi 1 –Bi 2 Sites 通过氢键有机框架的动态软约束重塑bi1 - bi2位点的C-C耦合界面化学

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-17 DOI: 10.1002/anie.5407135

Zhiwei Shao, Caichao Ye, Jun Xiong, Xiaojing Bi, Xuhao Yang, Wei Jiang, Jun Di

{"title":"Dynamic Soft‐Confinement via Hydrogen‐Bonded Organic Frameworks Reshapes C–C Coupling Interfacial Chemistry at Bi 1 –Bi 2 Sites","authors":"Zhiwei Shao, Caichao Ye, Jun Xiong, Xiaojing Bi, Xuhao Yang, Wei Jiang, Jun Di","doi":"10.1002/anie.5407135","DOIUrl":"https://doi.org/10.1002/anie.5407135","url":null,"abstract":"The core bottleneck in photocatalytic CO 2 reduction toward multi‐carbon oxygenates lies in the thermodynamic‐kinetic dual limitations of the C–C coupling step. Conventional strategies have focused on intrinsic electronic structure optimization of active sites while overlooking the critical influence of the reaction microenvironment on coupling probability. Herein, we propose a dynamic soft‐confinement catalytic strategy by in situ constructing a disordered hydrogen‐bonded organic framework (HOF) layer on Bi 3 O 4 Br surfaces, thereby establishing an HOF/Bi 3 O 4 Br integrated photocatalytic system. The introduction of HOF not only induces the formation of asymmetric Bi 1 –Bi 2 coupling sites but also establishes a dynamic hydrogen‐bonding microenvironment surrounding them. This microenvironment enhances CO 2 coverage near the coupling sites by constructing a persistent carbon source enrichment layer. Simultaneously, the interfacial polarization field promotes exciton dissociation and directs electron transport toward the Bi 1 –Bi 2 sites. Furthermore, the reconfigurable hydrogen bonds impose orientational soft confinement on *CO intermediates, guiding them into spatial configurations favorable for *OCCO bond formation. This soft‐hard synergistic interfacial design enables 0.7HOF/Bi 3 O 4 Br to achieve a CH 3 COOH production rate of 325.12 µmol g −1 h −1 with 98.81% product selectivity under sacrificial agent‐free conditions. This work demonstrates that dynamic microenvironment programming around active sites constitutes a critical pathway for overcoming the photocatalytic C–C coupling bottleneck.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"8 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2026-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149198982","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0