Angewandte Chemie International Edition最新文献_第10页

Mechanistic Insights into the Dissolution Relay for Deep Progression of Active Sites Toward Efficient and Ultralong-Life Energy Storage. 活性位点向高效超长寿命能量储存方向深入发展的溶解接力机理研究。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-07-23 DOI: 10.1002/anie.202510365

Mingming Sun,Wei Guo,Jinxin Wang,Yu Xu,Qiuyu Zhang

{"title":"Mechanistic Insights into the Dissolution Relay for Deep Progression of Active Sites Toward Efficient and Ultralong-Life Energy Storage.","authors":"Mingming Sun,Wei Guo,Jinxin Wang,Yu Xu,Qiuyu Zhang","doi":"10.1002/anie.202510365","DOIUrl":"https://doi.org/10.1002/anie.202510365","url":null,"abstract":"Transition metal (oxy)hydroxides serve as efficient aqueous cathode materials but suffer from the challenge of structure degradation during long-term cycling applications. Achieving an ultralong service life, e.g., beyond 100 000 cycles, is highly desired for aqueous energy storage, which necessitates the precise cognition and modulation of the surface/interface microenvironment with prolonged cycling conditions. Herein, to address this issue, we for the first time engineer the competitive bonding and the electrochemical deep progression of NiCoCu medium-entropy hydroxides. The theoretical and experiment results indicate that Cu is prone to leaching from the medium-entropy hydroxides with cycling, which elevates the d/p-band centers to activate the lattice oxygen and Co atoms, triggering a Cu/Co dual-cation dissolution relay phenomenon. As-incorporated Co vacancies favor the β-to-γ phase transformation of the reconstructed structure, accompanied by the coordination oscillation and the production of ultrafine (∼1.9 nm) nanodomains with improved kinetics and stability. Consequently, capacity retention of 1485 C g-1 was achieved after 150 000 cycles for the reconstructed electrodes, which is superior to many state-of-the-art NiCo-based materials. This work elucidates the potential of the coordination reorganization and deep progression of the reaction microenvironment to break the performance limit of energy storage and beyond.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"678 1","pages":"e202510365"},"PeriodicalIF":16.6,"publicationDate":"2025-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144684258","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

General Base‐Free Suzuki‐Miyaura Cross‐Coupling Reaction via Electrophilic Substitution Transmetalation 亲电取代转金属的一般无碱Suzuki - Miyaura交叉偶联反应

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-07-22 DOI: 10.1002/anie.202512496

Meng Zhang, Jing‐Ran Shan, Yuke Xie, Lanen Wei, Haigen Xiong, Ge‐Ning Xie, Ting Qi, Qinqin Shi, K. N. Houk, Hui Huang

引用次数: 0

1,4‐Dearomatization of Pyridines and Quinolines Enabled by the Carbodication Lewis Acid 碳化路易斯酸催化吡啶和喹啉类化合物的1,4 -脱芳化反应

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-07-22 DOI: 10.1002/anie.202510385

Xiaofeng Huang, Qiu Shi, Guoyin Lai, Wenbo H. Liu

引用次数: 0

The Design of Interfacial Organic‐Riched Phase by Molecular Interlocking for Stable Zn Anodes 用分子联锁设计稳定锌阳极界面富有机相

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-07-22 DOI: 10.1002/anie.202512032

Min Yang, Yanan Zhang, Qingjie Li, Xiao Wang, Buyu Ma, Zhiqiang Niu

{"title":"The Design of Interfacial Organic‐Riched Phase by Molecular Interlocking for Stable Zn Anodes","authors":"Min Yang, Yanan Zhang, Qingjie Li, Xiao Wang, Buyu Ma, Zhiqiang Niu","doi":"10.1002/anie.202512032","DOIUrl":"https://doi.org/10.1002/anie.202512032","url":null,"abstract":"Rechargeable aqueous zinc‐ion batteries (ZIBs) are promising energy storage devices due to their high safety and environmental friendliness. However, they suffer from some issues in Zn anodes, including dendrites, hydrogen evolution reaction, and byproducts. Herein, an organic‐riched phase (ORP) layer was constructed on Zn anode by introducing sodium anthraquinone‐1‐sulfonate (AQS) into the aqueous electrolyte with ethylene glycol (EG). In such an electrolyte, the zincophilic ‐SO3− groups of AQS molecules preferentially adsorb on Zn anodes, and stable chemical bonds are achieved between them. After that, the low‐polarity and hydrophobic anthraquinone group in the AQS layer tends to repel H2O molecules. Simultaneously, more AQS and EG molecules are attracted and migrate toward AQS layer due to polar compatibility, constructing the AQS/EG‐riched layer on the Zn anode by the interlocking effect among them. When Zn2+ solvated structures migrate through the ORP layer on Zn anode surface, AQS and EG molecules enter Zn2+ solvated structures, and thus, the solvated H2O molecules are removed. As a result, hydrogen evolution and side reactions were significantly suppressed, and the Coulombic efficiency of Zn anodes during plating/stripping process reached 99.56%. To illustrate the feasibility of the ORP layer, Zn||V2O5 full cells were assembled and exhibited superior cycling performance.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"25 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144677763","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

Monodisperse Regulation of Self‐Assembled Monolayer Via Dipole Molecules for Efficient Perovskite Solar Cells 高效钙钛矿太阳能电池中偶极子分子自组装单层的单分散调控

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-07-22 DOI: 10.1002/anie.202512660

Zhinan Zhang, Yinghao Xu, Sifan Chen, Wenbo Li, Shaofu Wang, Chuan Peng, Shengjie Du, Sixiong Li, Xingzhong Zhao, Ti Wang, Zhenhua Yu

{"title":"Monodisperse Regulation of Self‐Assembled Monolayer Via Dipole Molecules for Efficient Perovskite Solar Cells","authors":"Zhinan Zhang, Yinghao Xu, Sifan Chen, Wenbo Li, Shaofu Wang, Chuan Peng, Shengjie Du, Sixiong Li, Xingzhong Zhao, Ti Wang, Zhenhua Yu","doi":"10.1002/anie.202512660","DOIUrl":"https://doi.org/10.1002/anie.202512660","url":null,"abstract":"The application of self‐assembled monolayers (SAMs) significantly drives the enhancement in the efficiency of perovskite solar cell (PSC). However, the transition mechanism of SAM molecules from colloidal solutions to films remains unclear. Herein, we systematically investigate the SAM precursor solutions and the crystallization quality of the resulting SAM and perovskite films. Fibrous micelles of about 460 nm are found in the pristine SAMs solution, leading to nonuniform and low coverage distribution of films. Strong dipole molecules are employed to establish supramolecular interactions with SAMs, enabling the formation of highly monodisperse cubic micelles in solution (160 nm) and uniform SAM films. The contact at buried interface is determined by the balance between dipole moment and steric hindrance. Consequently, the regulated SAMs based inverted PSCs (0.09 cm2) and mini‐module (aperture area of 14.40 cm2) achieves efficiency of 26.58% (certificated 25.81%) and 22.95%, respectively. The optimized devices retain more than 96.30% of the initial efficiency for 5,100 h under the ISOS‐D‐1 condition with a linear fitting extrapolation to T90 of 11,259 h and 98.30% efficiency for 2,660 h under the ISOS‐L‐2 condition. This work highlights the great potential of SAMs micelle regulation for achieving efficient and stable PSC.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"17 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144677766","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

Ligand Type Guided Keto‐Arylation Enables Modular Total Synthesis of Polycyclic CBS Xanthones 配体型引导酮芳基化实现多环CBS香酮的模块化全合成

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-07-22 DOI: 10.1002/anie.202513532

Jonas W. Meringdal, Vivienne Prangenberg, Tim Treiber, Andreas J. Schneider, Leon Honsdorf, Dirk Menche

引用次数: 0

Scalable Synthesis of Stable Hydrogen‐Bonded Organic Framework for Efficient Hexafluoroethane Purification 高效净化六氟乙烷的稳定氢键有机骨架的可扩展合成

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-07-22 DOI: 10.1002/anie.202513398

Zhenyu Ji, Yunzhe Zhou, Rajamani Krishna, Maochun Hong, Mingyan Wu

{"title":"Scalable Synthesis of Stable Hydrogen‐Bonded Organic Framework for Efficient Hexafluoroethane Purification","authors":"Zhenyu Ji, Yunzhe Zhou, Rajamani Krishna, Maochun Hong, Mingyan Wu","doi":"10.1002/anie.202513398","DOIUrl":"https://doi.org/10.1002/anie.202513398","url":null,"abstract":"Developing stable, efficient and easily scalably‐synthesized adsorbents for removal of hydrofluoroethanes to obtain high purity hexafluoroethane (C2F6) is of great importance to the electronics industry. Herein, we report a hydrogen‐bonded organic framework (HOF‐TDBB) which exhibits statically as well as dynamically preferential hydrofluoroethanes (CF3CH2F and CF3CHF2) adsorption and achieves efficient one‐step C2F6 purification from CF3CH2F/CF3CHF2/C2F6 mixture. At 298 K, 11.7 mol kg−1 of high‐purity C2F6 can be obtained by HOF‐TDBB from 5/5/90 CF3CH2F/CF3CHF2/C2F6 mixture. Additionally, excellent stability endows HOF‐TDBB with good separation ability under various harsh conditions. For example, the separation performance can be well maintained within the dozens of consecutive separation experiments. Even at 338 K, 5.7 mol kg−1 of pure C2F6 can also be collected. More importantly, this material can be rapidly synthesized with a large scale by simple rotary evaporation. Combined with excellent separation performance, high stability and scalable synthesis, HOF‐TDBB has unlocked its great potential in this challenging industrial separation.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"52 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144677850","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

Carbon Dots‐Induced Hydrogen‐Bonding Traps in RHO Zeolite: Mechanistic Insights and Superior Flue Gas Separation Performance RHO沸石中碳点诱导的氢键陷阱：机理见解和卓越的烟气分离性能

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-07-22 DOI: 10.1002/anie.202509087

Yining Yang, Yida Zhou, Siyu Zong, Shiyu Zhou, Jiyang Li

{"title":"Carbon Dots‐Induced Hydrogen‐Bonding Traps in RHO Zeolite: Mechanistic Insights and Superior Flue Gas Separation Performance","authors":"Yining Yang, Yida Zhou, Siyu Zong, Shiyu Zhou, Jiyang Li","doi":"10.1002/anie.202509087","DOIUrl":"https://doi.org/10.1002/anie.202509087","url":null,"abstract":"Zeolites stand out as promising materials for flue gas separation, however, it poses a significant challenge to conduct pore interior modifications to improve the separation performance. Herein, we present a novel strategy for constructing hydrogen‐bonding traps in a small‐pore RHO zeolite by embedding carbon dots (CDs), thereby to regulate pore microenvironment and enhance the separation ability of CO2/N2. The incorporation of CDs into the RHO zeolite is realized via a straightforward calcination process, which endows the zeolite with the defect sites rich in hydroxyl groups that easily form hydrogen bonds with CDs. Along with 1H‐1H DQ‐SQ experiments, in situ FTIR and DFT calculations, the unique hydrogen‐bonding traps are unraveled, which can selectively capture and concentrate CO2. As a result, the CDs‐containing zeolite (R‐500) showcases exceptional performance in terms of both CO2 adsorption (90.40 cm3 g−1 at 298K and 1 bar) and CO2/N2 (15/85) separation (IAST selectivity of 1063.6). Strikingly, a superior CO2 adsorption with a capacity of 42.9 cm3 g−1 is achieved in the dynamic separation process (CO2/N2 15/85). The facile synthesis and impressive separation performance of R‐500 provides a promising solution for industrial scale CO2/N2 separation in flue gas.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"33 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144678212","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

Electro‐responsive Tri‐state Switch in Supramolecular Circuits 超分子电路中的电响应三态开关

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-07-22 DOI: 10.1002/anie.202511115

Min Tan, Xueyan Zhao, Zhibin Zhao, Adila Adijiang, Haibo Shu, Lichuan Chen, Zhiqiang Fan, Dong Xiang

{"title":"Electro‐responsive Tri‐state Switch in Supramolecular Circuits","authors":"Min Tan, Xueyan Zhao, Zhibin Zhao, Adila Adijiang, Haibo Shu, Lichuan Chen, Zhiqiang Fan, Dong Xiang","doi":"10.1002/anie.202511115","DOIUrl":"https://doi.org/10.1002/anie.202511115","url":null,"abstract":"Efficiently manipulating charge transport at the molecular level is critical to developing multifunctional and responsive molecular electronic devices. Here, we report the first electroresponsive tristate switch in a supramolecular circuit, overcoming the binary limitation and enabling richer logic encoding, governed solely by a bias voltage (electric field). At low electric fields, p‐phenylenediamine (PPD) molecules exhibit a high‐conductance state, which transitions successively to two distinct low‐conductance states as the external electric field strength increases. This precise control of supramolecular junctions through electric field manipulation achieved an on/off ratio GH/GL of ∼1.25×103, which is one of the largest values reported to date. Flicker noise analysis and density functional theory calculations reveal the intrinsic mechanism for the observation, i.e., electric field promoting the formation of trimer supramolecular junctions leads to the striking on/off ratio. These findings provide new insights into the design of molecular circuits with tunable conductance, paving a way for the design of molecular computation, memory devices, and sensors.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"53 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144678213","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

Intercalation Chemistry Awakens Transition Metal Hydroxide for Boosted and Sustained Electrocatalytic Sulfion Oxidation 插层化学唤醒过渡金属氢氧化物促进和持续电催化硫氧化

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-07-22 DOI: 10.1002/anie.202511402

Fengli Li, Wai Kwong NG, Wei Qiao, Yuting Yang, Xiaogang Li, Baojuan Xi, Yu Yu, Jingyun Fang, Ping Li, Shenglin Xiong

{"title":"Intercalation Chemistry Awakens Transition Metal Hydroxide for Boosted and Sustained Electrocatalytic Sulfion Oxidation","authors":"Fengli Li, Wai Kwong NG, Wei Qiao, Yuting Yang, Xiaogang Li, Baojuan Xi, Yu Yu, Jingyun Fang, Ping Li, Shenglin Xiong","doi":"10.1002/anie.202511402","DOIUrl":"https://doi.org/10.1002/anie.202511402","url":null,"abstract":"Electrocatalytic sulfion oxidation reaction (SOR) is a sustainable approach to treat sulfion‐rich sewage for S recovery. Transition metal hydroxide (TMOH), utilized in various electrocatalysis, yet is clumsy in SOR due to overstrong adsorption toward S‐containing intermediates from unsuitable electronic structure. Herein we report, for the first time, that the SOR performance of TMOH can be awakened by intercalation chemistry. Take Co(OH)2 as a proof‐of‐concept demonstration, MoO42− intercalated Co(OH)2 2D nanosheet array is engineered, and presents remarkably enhanced SOR behavior with an ultralow potential of 0.29 V versus RHE to attain 100 mA cm−2, a record Tafel slope of 27.7 mV dec−1, and stable operation for 192 h without appreciable deterioration. The experimental and theoretical studies unveil that MoO42−‐intercalated nanoarray is advantageous for active site exposure, and boosting mass transport with enhanced sulfion enrichment and superhydrophilicity. Impressively, MoO42− intercalation can manipulate electronic structure of Co(OH)2 with downshift of d‐band center, thereby weakening binding strength with HS− and S8, and decreasing the |ΔGs*|, eventually enhancing both activity and stability. Notably, such intercalation wake‐up strategy for the SOR is general and can be extended to other oxometallate intercalated TMOH systems. This contribution provides a new paradigm to evoke TMOH for SOR electrocatalysis via elegant intercalation tactic.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"14 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144677849","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