Angewandte Chemie International Edition最新文献_第4页

A Multiply and Long-Chain Branched Polyolefin with Low Density Polyethylene (LDPE)-Like Properties Containing Two Types of Functional Groups. 含有两种官能团的具有低密度聚乙烯（LDPE）类性质的多链长支化聚烯烃。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-23 DOI: 10.1002/anie.202518150

Christoph Unger,Christian Heber,Holger Schmalz,Christof Bauer,Winfried P Kretschmer,Rhett Kempe

引用次数: 0

Uphill Anion Transporters with Ultrahigh Efficiency Based on N-Heterocyclic Carbene Metal Complexes. 基于n -杂环碳金属配合物的超高效上坡阴离子转运体。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-23 DOI: 10.1002/anie.202518136

Yangyang Lin,Qin Fu,Zhuorui Kang,Yuting Zhu,Haoxuan Yuan,Changxing Ji,Boyu Zhang,Xian Kong,Peng Shi,Chao Lang

{"title":"Uphill Anion Transporters with Ultrahigh Efficiency Based on N-Heterocyclic Carbene Metal Complexes.","authors":"Yangyang Lin,Qin Fu,Zhuorui Kang,Yuting Zhu,Haoxuan Yuan,Changxing Ji,Boyu Zhang,Xian Kong,Peng Shi,Chao Lang","doi":"10.1002/anie.202518136","DOIUrl":"https://doi.org/10.1002/anie.202518136","url":null,"abstract":"Essential to the function of living systems, transmembrane ion transport in nature has inspired synthetic mimics that advance therapeutics, separations, sensing, and bioelectronics. Here, we report highly efficient and selective anion transport mediated by simple N-heterocyclic carbene (NHC) organometallic compounds. Using ruthenium (Ru) as the central metal and ion binding site, we systematically investigated seven classes of organoruthenium scaffolds and found that NHC-based Ru complexes demonstrated exceptionally high activity and selectivity. Extending the study to more metals, NHC complexes of Pd, Ag, and Cu also exhibited remarkable transport efficiency, with the iPrPh-NHC organocopper compound achieving an EC50 as low as 3.6 pM, surpassing one of the most active ion transporters, prodigiosin. Notably, NHC-based organometallic transporters leverage distinct kinetics of ligand binding and membrane diffusion to generate transmembrane potentials, and drive uphill ion transport reminiscent of proton pumps and ATPases. This work provides foundations for further development of organometallic ion transporters with high efficiency, tunable selectivity, and unique functions.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"41 1","pages":"e202518136"},"PeriodicalIF":16.6,"publicationDate":"2025-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145339317","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

Selective Electrocatalytic CO2 Reduction to Methanol: A Roadmap toward Practical Implementation. 选择性电催化二氧化碳还原为甲醇：走向实际实施的路线图。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-23 DOI: 10.1002/anie.202517916

Abdulrahman Allangawi,Xiangyun T Xiao,Xiao Ma,Mayasem Alsuhami,Mohd Adnan Khan,Rashed Aleisa,Yoji Kobayashi,Wan-Lu Li,Magnus Rueping,Jorge Gascon,Huabin Zhang

{"title":"Selective Electrocatalytic CO2 Reduction to Methanol: A Roadmap toward Practical Implementation.","authors":"Abdulrahman Allangawi,Xiangyun T Xiao,Xiao Ma,Mayasem Alsuhami,Mohd Adnan Khan,Rashed Aleisa,Yoji Kobayashi,Wan-Lu Li,Magnus Rueping,Jorge Gascon,Huabin Zhang","doi":"10.1002/anie.202517916","DOIUrl":"https://doi.org/10.1002/anie.202517916","url":null,"abstract":"Electrocatalytic CO2 reduction to methanol (MeOH) unites two urgent global needs, carbon recycling and renewable energy storage, into a single, compelling chemical transformation. According to recent techno-economic analyses, commercially competitive MeOH production (at ≈$190 per ton) can be achieved via electroreduction by meeting practical targets for current density, Faradaic efficiency (FE), and stability. Moreover, MeOH's high energy density (16 MJ L-1), substantial hydrogen content (100 g H2 per L), and low storage and transport costs further underscore its strong economic potential. Yet, the complexity of the six-electron-proton transfer (ET-PT) process that governs its formation remains intrinsically complex, with competing pathways threatening selectivity at every stage. This review critically examines current mechanistic insights, highlighting key intermediates such as CO and OCH3, and demonstrating how catalyst surfaces and reaction conditions profoundly influence pathway divergence. We highlight recent advances in catalyst development that exploit a fundamental, molecular-level understanding of intermediate stabilization to deliver unprecedented MeOH selectivity and activity. Through detailed analysis of operational parameters-including mass transport dynamics, electrolyte composition, and applied potentials-this work provides a comprehensive framework for rational catalyst development. Together, these insights converge design principles for next-generation electrocatalysts capable of selectively converting CO2-to-MeOH at scale, advancing economically viable and environmentally sustainable MeOH production.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"81 1","pages":"e202517916"},"PeriodicalIF":16.6,"publicationDate":"2025-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145351812","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

Rational Engineering of a Pseudaminic Acid Synthase Enzyme Enables Access to a 3-Fluoro Sugar with Motility Inhibition in Bacterial Pathogens. 假胺合酶的合理工程使细菌病原体获得具有运动抑制作用的3-氟糖。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-23 DOI: 10.1002/anie.202515851

James M Jeffries,Abigail J Walklett,Natasha E Hatton,Bartosz Kowalski,Tessa Keenan,Lickson Munjoma,Richard Haigh,Christopher D Bayliss,Gavin H Thomas,Martin A Fascione

{"title":"Rational Engineering of a Pseudaminic Acid Synthase Enzyme Enables Access to a 3-Fluoro Sugar with Motility Inhibition in Bacterial Pathogens.","authors":"James M Jeffries,Abigail J Walklett,Natasha E Hatton,Bartosz Kowalski,Tessa Keenan,Lickson Munjoma,Richard Haigh,Christopher D Bayliss,Gavin H Thomas,Martin A Fascione","doi":"10.1002/anie.202515851","DOIUrl":"https://doi.org/10.1002/anie.202515851","url":null,"abstract":"We report the rational engineering of a pseudaminic acid synthase (PseI), which enables the first synthesis of a 3-fluorinated pseudaminic acid sugar (3-(eq)-F-Pse5Ac7Ac), potentially establishing a new class of metabolic inhibitors targeting bacterial glycosylation. Pseudaminic acids are ⍺-keto acid sugars essential for O-glycosylation of flagellin in pathogens such as Campylobacter jejuni, where they are critical for motility and virulence. By introducing rational mutations in the PseI active site, we achieve enhanced turnover with unnatural 3-fluoro-phosphoenolpyruvate, facilitating a scalable chemoenzymatic synthesis of the fluorinated sugar. Subsequent treatment of C. jejuni with 3-(eq)-F-Pse5Ac7Ac resulted in a significant, time-dependent reduction in motility, and in vitro studies demonstrated bacterial CMP-pseudaminic acid synthetase enzymes (PseF) can process the fluoro sugar to afford CMP-3-(eq)-F-Pse5Ac7Ac, potentially implicating the fluorinated pseudaminic acid or its glycosyltransferase CMP-donor as an anti-motilin in vivo. This study demonstrates, for the first time, that fluorinated pseudaminic acids can impair bacterial motility, paving the way for anti-virulence strategies in pathogenic bacteria. This anti-motilin approach offers a promising alternative to traditional antibiotics, addressing the urgent need for novel strategies to combat antimicrobial resistance, and could be extended to other bacterial ⍺-keto acid sugars.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"20 1","pages":"e202515851"},"PeriodicalIF":16.6,"publicationDate":"2025-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145351813","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

Pd(II)/PIDA-Enabled Migratory Triple Functionalization of Terminal Alkenes via a 1,2-C/Pd(IV) Dyotropic Rearrangement. 通过1,2- c /Pd（IV）异向重排，Pd(II)/ pida使末端烯烃迁移三重功能化。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-23 DOI: 10.1002/anie.202518735

Chen-Xu Liu,Qian Wang,Jieping Zhu

引用次数: 0

Deciphering Ball Milling Mechanochemistry via Molecular Simulations of Collision-Driven and Liquid-Assisted Reactivity. 通过碰撞驱动和液体辅助反应的分子模拟来解读球磨机械化学。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-23 DOI: 10.1002/anie.202505263

Rupam Gayen,Leonarda Vugrin,Zehua Zhang,György Hantal,Ivan Halasz,Ana-Sunčana Smith

{"title":"Deciphering Ball Milling Mechanochemistry via Molecular Simulations of Collision-Driven and Liquid-Assisted Reactivity.","authors":"Rupam Gayen,Leonarda Vugrin,Zehua Zhang,György Hantal,Ivan Halasz,Ana-Sunčana Smith","doi":"10.1002/anie.202505263","DOIUrl":"https://doi.org/10.1002/anie.202505263","url":null,"abstract":"Mechanochemistry by ball milling proceeds through a series of discrete, high-energy collisions between milling balls and the sample, yet the molecular-level processes that govern the resulting chemical and physical transformations remain poorly understood. In this study, we develop a molecular dynamics simulation protocol to investigate a model mechanochemical reaction between potassium chloride (KCl) and 18-crown-6 ether, both under dry conditions and in the presence of water as a liquid additive. Our simulations reveal that the reaction is initiated by collision-induced fragmentation of the KCl crystal into individual ions. This process occurs when the absorbed energy per ion pair during a collision exceeds the crystal's cohesion energy. We further show that the addition of a small amount of water facilitates the formation of complexes between potassium ions and 18-crown-6 molecules. However, excessive water content stabilizes the reactants instead, thereby suppressing complex formation. These findings highlight a non-linear relationship between liquid additive concentration and the reaction outcome. Our approach offers a molecular-level perspective on mechanochemical reactivity, providing valuable insights that could guide the rational optimization of milling conditions-particularly the targeted selection and dosing of liquid additives-to improve reaction efficiency.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"105 1","pages":"e202505263"},"PeriodicalIF":16.6,"publicationDate":"2025-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145351798","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

Cost-Effective Scalable Production of Ultra-Stable Alkyl MOF Featuring Single-Molecule C3H6 Trap for Record Capture of Trace C3H6 from C2H4. 具有单分子C3H6陷阱的超稳定烷基MOF的成本效益可扩展生产，用于记录从C2H4中捕获痕量C3H6。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-23 DOI: 10.1002/anie.202515496

Miao Chang,Zitong Wang,Ruihan Wang,Minghui Liu,Yujie Wang,Dahuan Liu

{"title":"Cost-Effective Scalable Production of Ultra-Stable Alkyl MOF Featuring Single-Molecule C3H6 Trap for Record Capture of Trace C3H6 from C2H4.","authors":"Miao Chang,Zitong Wang,Ruihan Wang,Minghui Liu,Yujie Wang,Dahuan Liu","doi":"10.1002/anie.202515496","DOIUrl":"https://doi.org/10.1002/anie.202515496","url":null,"abstract":"Highly efficient capture of trace C3H6 from C2H4 by physisorbents remains an enormous challenge to combine top-rank separation performance with excellent stability and economical scalability. We, herein, built a single-molecule C3H6 trap that bears an opposite series of oxygen and dense alkyl groups distributed in an ultramicroporous [Al(OH)(trans-CDC)] (Al-CDC, trans-H2CDC = trans-1,4-cyclohexanedicarboxylic acid). The ultra-stable trap with well-matched pore size and pore chemistry enables a record uptake (40.8 cm3(STP) g-1) at ultralow concentration, Henry coefficient (12685.5 cm3(STP) g-1 bar-1), initial adsorption heat difference (27.2 kJ mol-1), adsorption kinetic (0.49 min-1) and kinetic selectivity (3.1) for C3H6 with one of the highest initial C3H6 adsorption heats (50.5 kJ mol-1) and selectivity (16.3), establishing a novel benchmark for capture of trace C3H6. The C3H6 adsorption mechanism is deciphered to be thermodynamically driven owing to the synergism of multiple hydrogen-bonding and van der Waals (vdW) forces. Breakthrough tests validate that Al-CDC owns a record C2H4 productivity (≥99.999%) of 410.5 cm3(STP) g-1 for trace C3H6 capture with excellent reproducibility. The cost-effective scalable production with the cheapest cost (508.9 $ kg-1) and highest space-time yield (4564.8 kg m-3 day-1) and shaping of Al-CDC is realized with unaffected structural property and capture performance.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"50 1","pages":"e202515496"},"PeriodicalIF":16.6,"publicationDate":"2025-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145351809","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

The Weakened Super-Exchange Interaction Realizes the Direct Regeneration of Spent Lithium-lon Battery Cathodes. 弱化的超交换相互作用实现了废旧锂离子电池阴极的直接再生。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-23 DOI: 10.1002/anie.202520448

Yuan-Meng Li,Yujia He,Kai Jia,Haojie Dong,Xin-Yu Zhang,Hao Qin,Ling-Jiao Hu,Hao Zhang,Zhao-Kun Guan,Si-Fan Chen,Mengting Liu,Bing Xiao,Shujiang Ding,Kai Xi,Peng-Fei Wang

{"title":"The Weakened Super-Exchange Interaction Realizes the Direct Regeneration of Spent Lithium-lon Battery Cathodes.","authors":"Yuan-Meng Li,Yujia He,Kai Jia,Haojie Dong,Xin-Yu Zhang,Hao Qin,Ling-Jiao Hu,Hao Zhang,Zhao-Kun Guan,Si-Fan Chen,Mengting Liu,Bing Xiao,Shujiang Ding,Kai Xi,Peng-Fei Wang","doi":"10.1002/anie.202520448","DOIUrl":"https://doi.org/10.1002/anie.202520448","url":null,"abstract":"The direct regeneration of cathodes is an effective technique to address resource waste and environmental pollution caused by spent lithium-ion batteries (LIBs). However, Li+ migration within the rock-salt phase of degraded LiNi0.5Co0.2Mn0.3O2 cathodes follows an energetically unfavorable 2-transition metal (2-TM) transport pathway (tetrahedral sites between face-sharing octahedra), creating a kinetic barrier that fundamentally limits direct regeneration. A Na-based molten salt pretreatment is applied to introduce Na atoms into the unoccupied tetrahedral sites of the rock-salt phase, which alters the electronic state distribution of bridged oxygen anions and reduces super-exchange interactions between TM atoms in adjacent layers, thereby triggering a phase transformation from rock-salt to targeted layered structure. Consequently, the Li+ migration pathway shifts from a high-energy 2-TM route to a more favorable low-barrier 1-TM route, enabling efficient lithiation and complete restoration of the cathode. The regenerated materials exhibit high structural uniformity and excellent electrochemical performance, achieving 78% capacity retention after 500 cycles. This study provides an insightful perspective on direct LIB recycling by regulating super-exchange interactions within the degraded cathode structures.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"101 1","pages":"e202520448"},"PeriodicalIF":16.6,"publicationDate":"2025-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145339320","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

From Oxygen to Tellurium: The Impact of the Chalcogen on Nucleophilicities and Basicities of Isochalcogenourea Catalysts. 从氧到碲：硫对异硫脲催化剂亲核性和碱度的影响。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-23 DOI: 10.1002/anie.202514865

Lotte Stockhammer,Kevin Kasten,Andreas Eitzinger,Lukas S Vogl,Magdalena Piringer,David Weinzierl,Armin R Ofial,Andrew D Smith,Mario Waser

{"title":"From Oxygen to Tellurium: The Impact of the Chalcogen on Nucleophilicities and Basicities of Isochalcogenourea Catalysts.","authors":"Lotte Stockhammer,Kevin Kasten,Andreas Eitzinger,Lukas S Vogl,Magdalena Piringer,David Weinzierl,Armin R Ofial,Andrew D Smith,Mario Waser","doi":"10.1002/anie.202514865","DOIUrl":"https://doi.org/10.1002/anie.202514865","url":null,"abstract":"Isochalcogenoureas (IChU) embedded in bi- or tricyclic ring systems have proven to be versatile Lewis base/nucleophilic catalysts that activate a wide range of electrophilic substrates for organocatalytic transformations. Ring size, variation of substituents, and the choice of the chalcogen atom affect the efficiency of IChU catalysis in a complex way. To gain a systematic insight into the key parameters that influence reactivity, 14 IChUs covering the fundamental motifs of these structural variations were selected and analyzed by a combination of kinetic, thermodynamic, and quantum-chemical methods. Two previously unknown tricyclic isotellurourea catalysts were synthesized to facilitate a comparison of all naturally abundant chalcogens (O, S, Se, and Te) in the IChU structure. Furthermore, their reactivity on the Mayr nucleophilicity scale as well as their Brønsted and Lewis basicities were determined in polar organic solvents under standardized conditions. Catalyst performance was assessed in two alcohol acylation reactions and in allenoate activation. The low electronegativity of tellurium gave rise to superior nucleophilicity and Lewis basicity of the isotelluroureas when compared to O-, S-, or Se-containing IChUs. Embedding tellurium in IChU structures thus provides a novel handle to influence and fine-tune the effectiveness of IChU organocatalysis.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"45 1","pages":"e202514865"},"PeriodicalIF":16.6,"publicationDate":"2025-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145339321","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

Surface-Decoupled Altitudinal and Azimuthal Triptycene-Fused Tetrapodal Molecular Motors. 表面解耦的垂直和方位三叶草熔合四足分子马达。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-23 DOI: 10.1002/anie.202513922

Kateřina Bezděková,Lukáš Severa,Eva Kaletová,Katarina Majerová Varga,Milan Mašát,Liang-Ting Wu,Jyh-Chiang Jiang,Ivana Císařová,Jiří Kaleta

引用次数: 0