Angewandte Chemie International Edition最新文献_第9页

Rotation‐Coupled Guest Anions Stabilize Polymer Solid‐State Sodium‐Metal Batteries 旋转偶联客体阴离子稳定聚合物固态钠金属电池

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-15 DOI: 10.1002/anie.9801142

Yi Li, Lifeng Wang, Fangxin Ling, Ziyang Wang, Yu Shao, Weijian Gu, Zhen Li, Bin Ye, Ruiling Bai, Jialong Shen, Shuangli Yang, Yixin Hu, Hanyu Huo, Shuchen Zhang, Xianhong Rui, Yu Yao, Yan Yu

{"title":"Rotation‐Coupled Guest Anions Stabilize Polymer Solid‐State Sodium‐Metal Batteries","authors":"Yi Li, Lifeng Wang, Fangxin Ling, Ziyang Wang, Yu Shao, Weijian Gu, Zhen Li, Bin Ye, Ruiling Bai, Jialong Shen, Shuangli Yang, Yixin Hu, Hanyu Huo, Shuchen Zhang, Xianhong Rui, Yu Yao, Yan Yu","doi":"10.1002/anie.9801142","DOIUrl":"https://doi.org/10.1002/anie.9801142","url":null,"abstract":"Polymer solid‐state sodium‐metal batteries are constrained by sluggish Na + migration and unstable sodium–metal interfaces, both of which are closely associated with poorly regulated solvation chemistry. Here we report a rotation‐coupled guest‐anion strategy in a poly(vinylidene fluoride‐co‐hexafluoropropylene)‐based solid‐state electrolyte (PHSE) using Mg(OTf) 2 . Mg 2+ preferentially coordinates DMF and TFSI − , weakening Na + –TFSI − association and limiting solvent‐derived reactions at the sodium metal anode. OTf − enters the Na + solvation shell as a mobile guest anion. Its C─S rotational axis and equivalent oxygen coordination sites allow conformational rotation to synchronize with Na + hopping along polymer chains. This anchor–rotator chemistry reorganizes Na + coordination, lowers the migration barrier, and promotes an inorganic‐rich, Mg─O‐containing interphase. The optimized electrolyte enables Na 3 V 2 (PO 4 ) 3 ||Na cells to retain 94.2% capacity after 1100 cycles at 2C and supports a 94 mAh pouch cell with stable cycling. It also enables high‐voltage Na 3 V 2 (PO 4 ) 2 O 2 F||Na cells to retain 93.6% capacity after 1000 cycles at 0.5C over 2.5–4.2 V. Comparative evaluation across a total of 20 polymer electrolyte systems with varied polymer matrices and anion structures identifies anion symmetry, rotational periodicity, and finite rotational barriers as molecular criteria for designing stable polymer solid‐state sodium‐metal batteries.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"30 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149172634","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

Field‐Effect Induced Interfacial Water Restructuring Accelerates Zinc‐Catalyzed Hydrodeoxygenation 场效应诱导的界面水重组加速锌催化的加氢脱氧

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-15 DOI: 10.1002/anie.8324637

Jiaxin Li, Youwei Sheng, Nadia N. Intan, Huaiyu Chang, Haobo Li, Wan Ru Leow

{"title":"Field‐Effect Induced Interfacial Water Restructuring Accelerates Zinc‐Catalyzed Hydrodeoxygenation","authors":"Jiaxin Li, Youwei Sheng, Nadia N. Intan, Huaiyu Chang, Haobo Li, Wan Ru Leow","doi":"10.1002/anie.8324637","DOIUrl":"https://doi.org/10.1002/anie.8324637","url":null,"abstract":"The deoxygenation of biomass‐derived molecules is thermodynamically challenging yet essential for their conversion to commodity chemicals. Metallic zinc is a promising material for deoxygenation due to its strong reductive properties, but sluggish kinetics and harsh reaction conditions detract from practical application. Here, we hypothesize that zinc‐catalyzed hydrodeoxygenation could be limited by inefficient proton transport due to disordered interfacial water structure. Using the transformation of dihydroxyacetone to acetone as a model reaction, we identified the rate‐determining step to be an Eley–Rideal‐type proton‐coupled electron transfer from water to the hydroxyacetone intermediate. Applying an electric field accelerates this step by restructuring the interfacial hydrogen‐bond network and promoting direct proton transfer, thereby enabling a 10 3 ‐fold increase in surface‐area‐normalized turnover frequency and Faradaic efficiencies of 63%–70% at current densities up to 300 mA/cm 2 . These findings highlight interfacial water restructuring as a powerful lever for enhancing hydrodeoxygenation efficiency.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"11 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149172851","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

Modular Synthesis of Bridge‐Disubstituted Bicyclo[3.1.1]heptanes via Stereoselective Difunctionalization of Tricyclo[4.1.0.0 2 , 7 ]heptane 三环[4.1.0.0 2,7]庚烷立体选择性双官能化桥-二取代双环[3.1.1]庚烷的模块化合成

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-15 DOI: 10.1002/anie.9614011

Zhenda Fu, Yufei Zhou, Xiaowen Gu, Xueping Hu, Yingzi Li, Wei‐Qiao Deng, Xingwei Li, Songjie Yu

{"title":"Modular Synthesis of Bridge‐Disubstituted Bicyclo[3.1.1]heptanes via Stereoselective Difunctionalization of Tricyclo[4.1.0.0 2 , 7 ]heptane","authors":"Zhenda Fu, Yufei Zhou, Xiaowen Gu, Xueping Hu, Yingzi Li, Wei‐Qiao Deng, Xingwei Li, Songjie Yu","doi":"10.1002/anie.9614011","DOIUrl":"https://doi.org/10.1002/anie.9614011","url":null,"abstract":"Scaffolds with flexible bond exit vectors are essential in bioisosteric design, enabling adaptive molecular recognition of conformationally dynamic targets, and fine‐tuning key physicochemical properties. Despite this potential, current benzene bioisosteres based on bicyclo[n.1.1]alkanes are confined to three‐dimensional scaffolds with fixed exit vectors at their rigid bridgehead positions. As a critical piece for mimicking substituted arenes, the development of C(sp 3 )‐enriched bioisosteres bearing two flexible vectors has been thwarted by the lack of stereoselective synthetic routes. Herein, we report a photochemical nickel‐catalyzed selective 1,7‐difunctionalization of tricyclo[4.1.0.0 2,7 ]heptane using readily available organohalides. This sequential protocol generates previously elusive anti ‐stereoselective 6,7‐difunctionalized bicyclo[3.1.1]heptanes with high stereocontrol, broad coupling‐partner scope, and built‐in handles for post‐functionalization. Biological assays and computational modeling on drug analogues demonstrate the bioisosteric potential of these dual‐flexible‐vector bicyclo[3.1.1]heptane scaffolds. This methodology unlocks previously unexplored chemical space with broad implications for drug discovery and beyond.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"410 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149173012","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

Potential-Gated Spin Crossover Triggers Fe─N─C Catalyst Demetallation 电位门控自旋交叉触发Fe─N─C催化剂脱金属

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-15 DOI: 10.1002/anie.8986276

Haobo Li,Xinwei Wang,Bohan Cao,Fubo Tian,Zhiyao Duan

引用次数: 0

4,9,13,18-Tetraazateropyrenes: Synthesis, Cross-Locked Saddle Packing and Unique Geometry Reorganization 4,9,13,18-四氮杂蒽：合成、交锁鞍形填料及独特几何结构重组

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-15 DOI: 10.1002/anie.4825806

Yan Kou,Yi Han,Mengjiao Wu,Lingfei Hu,Wei Yuan,Yulan Chen

引用次数: 0

Positional Isomerism Reveals Intrinsic Decoupling of Structural Relaxation and Vibrational Frequency in MR‐TADF Emitters 位置异构揭示了MR - TADF发射体结构弛豫和振动频率的内在解耦

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-15 DOI: 10.1002/anie.2538716

Xiaojuan Song, Yangyang Xin, Xiaoning Li, Xiyun Ye, Yujun Xie, Yuewei Zhang, Lian Duan, Ben Zhong Tang, Zhen Li

{"title":"Positional Isomerism Reveals Intrinsic Decoupling of Structural Relaxation and Vibrational Frequency in MR‐TADF Emitters","authors":"Xiaojuan Song, Yangyang Xin, Xiaoning Li, Xiyun Ye, Yujun Xie, Yuewei Zhang, Lian Duan, Ben Zhong Tang, Zhen Li","doi":"10.1002/anie.2538716","DOIUrl":"https://doi.org/10.1002/anie.2538716","url":null,"abstract":"The pursuit of high‐color‐purity organic light‐emitting diodes (OLEDs) has spurred the development of multiple resonance (MR) emitters. Yet a long‐standing assumption in the field holds that minimizing excited‐state structural displacement (Δ Q ) is essential for achieving narrow emission bandwidth. Here we challenge this notion by demonstrating that Δ Q and molecular vibrational frequency ( ω ) act as independent, rather than coupled, determinants of the emission full width at half maximum (FWHM). Through systematic ortho ( o DB‐BN), meta ( m DB‐BN), and para ( p DB‐BN) positional isomerism of a sterically bulky dimesitylboryl acceptor on an archetypal MR scaffold, we reveal that small Δ Q reduces the Stokes shift but does not guarantee narrow FWHM; instead, low ω emerges as the decisive factor. The meta‐substituted isomer, despite exhibiting the smallest Δ Q , displays the broadest FWHM owing to a prominent low‐frequency torsional vibration. Conversely, the ortho ‐ and para ‐isomers retain ultranarrow emission despite pronounced molecular distortion. The resulting OLEDs achieve excellent external quantum efficiencies of up to 33.3% with suppressed roll‐off, and pDB‐BN delivers a remarkable luminance of 109 600 cd m −2 . This work provides an alternative perspective on the design of narrowband emitters, suggesting that controlling vibrational coupling, in addition to minimizing structural displacement, is a valuable consideration in molecular engineering.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"232 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149172892","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

O‐B‐O Positional Isomerism and Matrix Synergy in Arylboronic Ester‐Modified Naphthalene: A Strategic Approach for Enhanced Organic Phosphorescence and Time‐Resolved Multilevel Information Encryption 芳香硼酯修饰萘的O - B - O位置异构和基质协同作用：增强有机磷光和时间分辨多级信息加密的策略方法

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-15 DOI: 10.1002/anie.5272666

Zhenjie Zhou, Qiang Feng, Jianhua Liu, Hui‐min Xu, Tian Wang, Wang Zuo, Junxi Liao, Sijie Xie, Qiang Cheng, Dianyuan Wang, Jianguo Wang, Huanan Huang

{"title":"O‐B‐O Positional Isomerism and Matrix Synergy in Arylboronic Ester‐Modified Naphthalene: A Strategic Approach for Enhanced Organic Phosphorescence and Time‐Resolved Multilevel Information Encryption","authors":"Zhenjie Zhou, Qiang Feng, Jianhua Liu, Hui‐min Xu, Tian Wang, Wang Zuo, Junxi Liao, Sijie Xie, Qiang Cheng, Dianyuan Wang, Jianguo Wang, Huanan Huang","doi":"10.1002/anie.5272666","DOIUrl":"https://doi.org/10.1002/anie.5272666","url":null,"abstract":"Organic room‐temperature phosphorescence (RTP) materials have attracted widespread attention for their potential in both fundamental research and advanced technologies, owing to their unique long‐lived luminescence characteristics. However, their development is hampered by issues such as low triplet exciton generation efficiency, oxygen quenching, and nonradiative decay in organic molecules. In this study, we propose an effective strategy to modulate polymer‐confined arylboronate RTP via positional isomerization. Two naphthyl isomers with O‐B‐O units, 2‐phenylnaphtho[2,3‐d][1,3,2]dioxaborole (2,3‐NPB) and 2‐phenylnaphtho[1,8‐de][1,3,2]dioxaborinine (1,8‐NPB), were synthesized. Interestingly, despite their identical chemical compositions, they display distinctly different performances in poly(vinyl alcohol) (PVA) films: 2,3‐NPB@PVA exhibits a phosphorescence lifetime of 867 ms and a photoluminescence quantum yield of 38.5%, whereas 1,8‐NPB@PVA delivers corresponding values of 765 ms and 12.2%. Experiments and calculations confirm that O‐B‐O positional isomerism alters aromaticity, geometry, and electrostatic potentials, thus modulating the competition between triplet exciton evolution and nonradiative decay. The good film‐forming ability, flexibility, and processability of PVA confer deformation tolerance, indicating potential in flexible anti‐counterfeiting and secure information storage. This work not only achieves precise triplet‐state control in purely organic boron‐based phosphors, but also elucidates structure‐property relationship (O‐B‐O positional isomerism‐microstructure‐triplet evolution‐matrix synergy), offering a concise design route for high‐performance RTP materials.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"10 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149172895","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

Bimetallic Metal-Acetylide Frameworks for Highly Selective and Durable H2O2 Electrosynthesis 高选择性和耐用H2O2电合成的双金属金属-乙酰基醚框架

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-15 DOI: 10.1002/anie.2288856

Lifen Chen,Qixiao Lu,Linli Xu,Lawrence Yoon Suk Lee,Wai-Yeung Wong

引用次数: 0

Efficient Bipolar Hydrogen Peroxide Production Through Photoelectrochemistry 利用光电化学高效生产双极过氧化氢

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-15 DOI: 10.1002/anie.3694210

Bo Yang, Shijie Ren, Rui‐Ting Gao, Yang Yang, Mu Xiao, Limin Wu, Lei Wang

{"title":"Efficient Bipolar Hydrogen Peroxide Production Through Photoelectrochemistry","authors":"Bo Yang, Shijie Ren, Rui‐Ting Gao, Yang Yang, Mu Xiao, Limin Wu, Lei Wang","doi":"10.1002/anie.3694210","DOIUrl":"https://doi.org/10.1002/anie.3694210","url":null,"abstract":"Hydrogen peroxide (H 2 O 2 ) is a crucial environmentally benign oxidant. Photoanodes in bias‐free photoelectrochemical (PEC) systems suffer from poor H 2 O 2 selectivity at low potentials, limiting the efficiency of bipolar H 2 O 2 production. Herein, we report a rare‐earth ytterbium oxide (YbO x ) modified BiVO 4 /WO 3 photoanode for efficient PEC water oxidation to H 2 O 2 . The optimized photoanode achieves a photocurrent density of 4.83 mA cm −2 at 1.23 V RHE , an H 2 O 2 Faradaic efficiency (FE) of over 80% across the potential range of 0.6–1.8 V RHE , and a peak FE of 90.4% at 1.6 V RHE . Yb 3+ Lewis acid sites suppress the competitive four‐electron oxygen evolution reaction by forming Yb‐hydroxyl complexes, while YbO x enhances charge transfer and reduces interfacial resistance. Importantly, when coupled with a FeZnWMnYb high‐entropy amorphous oxide cathode for the two‐electron oxygen reduction reaction, the bias‐free tandem cell achieves ∼160% bipolar H 2 O 2 FE. Scaling the photoelectrode to 20 cm 2 under 0.7 suns illumination yields an H 2 O 2 production rate of 3.03 mmol L −1 h −1 . This work demonstrates a viable strategy for large‐scale solar‐driven H 2 O 2 synthesis for environmental applications.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"11 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149172633","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

Proximity‐Induced Protein Deglycosylation by Endogenous O‐GlcNAcase 内源性O - GlcNAcase近距离诱导的蛋白去糖基化

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-15 DOI: 10.1002/anie.1827729

Haixing Xu, Bowen Ma, Yunpeng Huang, Jialin Liu, Billy Wai‐Lung Ng

{"title":"Proximity‐Induced Protein Deglycosylation by Endogenous O‐GlcNAcase","authors":"Haixing Xu, Bowen Ma, Yunpeng Huang, Jialin Liu, Billy Wai‐Lung Ng","doi":"10.1002/anie.1827729","DOIUrl":"https://doi.org/10.1002/anie.1827729","url":null,"abstract":"O‐GlcNAcylation is an important post‐translational modification that regulates numerous cellular processes, yet tools enabling selective removal of O‐GlcNAc from individual proteins via endogenous O‐GlcNAcase (OGA) in living cells remain limited. Here, we report De‐O‐GlcNAcylation‐targeting chimeras (DOGTACs), a chemically induced proximity strategy that selectively reduces O‐GlcNAc from target proteins by recruiting endogenous OGA. Initial designs incorporating potent competitive OGA inhibitors efficiently engaged OGA but failed to induce de‐O‐GlcNAcylation, revealing that catalytic competence is essential for productive proximity‐driven editing. By attenuating inhibitor potency while retaining OGA engagement, we developed optimized DOGTACs that promote concentration‐ and time‐dependent, target‐specific de‐O‐GlcNAcylation in living cells without perturbing global O‐GlcNAc levels. Furthermore, we successfully applied DOGTAC to additional target proteins including FKBP12 F36V fused proteins and endogenous CK2α across different cell lines. Besides, we found DOGTAC (R)‐C4 treatment could reduce the stability of FKBP12 F36V fused‐NUP98‐KDM5A in cells. Collectively, this work established attenuated competitive inhibitors as recruitment modules for catalytic enzyme engagement and a novel strategy, DOGTAC, for targeted de‐O‐GlcNAcylation via endogenous OGA recruitment in living cells.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"21 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149172969","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