Angewandte Chemie International Edition最新文献_第8页

Carbon and Oxygen Double Defects Enhanced Ru-based Catalyst for Ammonia Decomposition

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-03-27 DOI: 10.1002/anie.202501898

Likang Lv, Peiqi Chu, Tong Han, Yunpeng Jiang, Zhiwei Wang, Yuxi Liu, Hongxing Dai, Lu Wei, Jiguang Deng

{"title":"Carbon and Oxygen Double Defects Enhanced Ru-based Catalyst for Ammonia Decomposition","authors":"Likang Lv, Peiqi Chu, Tong Han, Yunpeng Jiang, Zhiwei Wang, Yuxi Liu, Hongxing Dai, Lu Wei, Jiguang Deng","doi":"10.1002/anie.202501898","DOIUrl":"https://doi.org/10.1002/anie.202501898","url":null,"abstract":"Although ammonia is widely recognized as one of the most promising candidates for hydrogen storage and transformation, the catalytic mechanisms involved in ammonia decomposition remain insufficiently understood, and the stability of catalysts continues to present significant challenges. In this study, Ru/CeO2-CNTs catalysts with double defect sites were synthesized by a straightforward method, achieving an outstanding hydrogen production rate of 2,230 mmol/gRu/min at 500 °C, outperforming most Ru-based catalysts. Experimental characterization and theoretical calculations revealed that the CeO2-CNT interface promotes the formation of oxygen vacancies (Ov) and carbon defects (Cd) through carbon-oxygen interactions. These defects enhance electron transfer from the support to Ru nanoparticles (NPs), modulate NH3 adsorption and activation, as well as the recombination and desorption of adsorbed N species (N*). Moreover, the coating of CeO2 significantly improved the stability of CNTs, which weakens undesired reaction under high temperature and hydrogen-rich conditions. The study introduced a rational design strategy that enhance the multiple elementary stages of the NH3 decomposition by constructing double defect sites, and offering new insights into the design of efficient and durable catalysts under harsh environment.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"17 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143713796","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

Interweaved Nanofiber Anode Coating Based on Covalent Organic Frameworks for High-Performance Lithium-Metal Batteries

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-03-27 DOI: 10.1002/anie.202505626

Huifen Zhuang, Can Guo, Wenhai Feng, Liwen Wang, Zixi Zheng, Qi Li, Haifu Zhang, Yifa Chen, Ya-Qian Lan

{"title":"Interweaved Nanofiber Anode Coating Based on Covalent Organic Frameworks for High-Performance Lithium-Metal Batteries","authors":"Huifen Zhuang, Can Guo, Wenhai Feng, Liwen Wang, Zixi Zheng, Qi Li, Haifu Zhang, Yifa Chen, Ya-Qian Lan","doi":"10.1002/anie.202505626","DOIUrl":"https://doi.org/10.1002/anie.202505626","url":null,"abstract":"High-rate lithium-metal batteries call for unique interfacial structures of anode with interfacial compatibility, facilitated lithium insertion/extraction and dendrite suppression properties to meet the growing high-rate demand. Here, we develop an interweaved porous coating based on a kind of covalent organic framework (ODH-Cu3-COF) based helical nanofibers through the assembly of non-linear oxalyldihydrazide unit and rigid Cu3 unit. The interweaved helical nanofibers network with well-arranged polar groups (i.e. C=N, -CO-NH- and pyrazole groups) could serve as nuclei sites to achieve fast Li+ insertion/extraction and dendrite suppression in high-rate conditions. Benefiting from the advantages of interface design, the resultant ODH-Cu3-COF modified anode improves the Coulombic efficiency (97.5%, 120 cycles at 5 mA cm-2) and showcases a stable lifespan (1000 h at 2 mA cm-2 and 2 mAh cm-2) in symmetric cell. Moreover, the high-rate property of ODH-Cu3-COF@Li||LFP full cell presents an excellent cycling stability (900 cycles at 5 C) in commercial carbonate electrolyte. Theoretical calculations reveal that lithiophilic ODH-Cu3-COF has high Li affinity to reduce the nucleation barrier and achieve fast desolvation process in interface to promote the lifespan of high-rate lithium-metal batteries.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"54 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723897","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 Front Cover: Enantioselective Synthesis of Chiral Ferrocenyl Aminoalcohols: Simultaneous Induction of Multiple Types of Chirality by a Rhodium-Catalyzed Asymmetric Ring-Opening Strategy

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-03-27 DOI: 10.1002/anie.202505856

Takamu Isoda, Komei Jimba, Kyohei Kawashima, Takahiro Nishinoiri, Seiji Mori, Akihiro Tsurusaki, Ken Kamikawa

引用次数: 0

Decoding Variants of Pyrite, Arsenopyrite and Marcasite Using an Electron Counting Rule

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-03-27 DOI: 10.1002/anie.202502322

Dirk Johrendt, Kristian Witthaut, Sandra Kreiner

{"title":"Decoding Variants of Pyrite, Arsenopyrite and Marcasite Using an Electron Counting Rule","authors":"Dirk Johrendt, Kristian Witthaut, Sandra Kreiner","doi":"10.1002/anie.202502322","DOIUrl":"https://doi.org/10.1002/anie.202502322","url":null,"abstract":"Pyrite, Marcasite and Arsenopyrite are of significant historical and contemporary interest. Compounds adopting these structure types are extensively studied for their crystallographic properties and potential applications in energy storage and conversion. Despite numerous investigations since the 1970s, understanding the chemical behaviour of Pyrite, Marcasite, and Arsenopyrite remains limited. This study proposes a new structure determining electron (SDE) rule to systematise these compounds without relying on formal charge assignments. The SDE rule predicts structure types based on the distribution of non-localised electrons around transition metals, providing a clear framework for identifying and categorising related compounds. We observe good agreement with literature data and furthermore synthesised nine new compounds within the Pt/Ir-Ge-As/Sb systems, demonstrating the applicability of SDE. Our findings reveal that these new compounds have layer configurations of Pyrite (P), Marcasite (M) and Arsenopyrite (A), enhancing our understanding of their chemical diversity. This work not only categorises existing compounds, but also paves the way for future exploration of new materials, highlighting the greater structural potential of P, M, A-related compounds beyond traditional frameworks. Preliminary results indicate that the type of layers influences physical properties, such as electrical conductivity, warranting further investigation into the relationship between structure and function in these compounds.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"16 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143713795","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

Outside Back Cover: Boosting C─O Bond Cleavage and Reverse Water-Gas Shift Activity via Enriched in-plane Sulfur Vacancies in Single-Layer Molybdenum Disulfide

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-03-27 DOI: 10.1002/anie.202506409

Zhiyuan Zheng, Xin Shang, Weijue Wang, Xiaofeng Yang, Xiong Su, Yanqiang Huang

引用次数: 0

Biomimetic Adhesion/Detachment using Layered Polymers with Light‐induced Rapid Shape Changes

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-03-27 DOI: 10.1002/anie.202503748

Youfeng Yue, Yasuo Norikane, Eiji Nishibori

{"title":"Biomimetic Adhesion/Detachment using Layered Polymers with Light‐induced Rapid Shape Changes","authors":"Youfeng Yue, Yasuo Norikane, Eiji Nishibori","doi":"10.1002/anie.202503748","DOIUrl":"https://doi.org/10.1002/anie.202503748","url":null,"abstract":"Geckos achieve rapid and efficient adhesion and detachment on various surfaces within milliseconds due to the hierarchically structured fibrillar architecture of their toe pads. Extensive research has focused on developing adhesive materials that mimic these micro‐nano structures. However, no conventional adhesives have matched the performance of their natural counterparts, which are both non‐degrading and self‐cleaning. Here, we develop a chemically crosslinked polymer film with a nanoscale layered structure that exhibits high‐speed‐switching of mechanical motions (expansion and contraction) in both forward and reverse directions through controlled ultraviolet (UV) irradiation. Under UV light on/off switching, the film shows reversable shape changes in the direction perpendicular to the molecular alignment. These photoresponsive molecular movements in the film is demonstrated for remote control in a smart adhesion system with rapid responsiveness and high reproducibility. The films respond to UV light to release picked‐up objects and immediately regain their adhesion when the UV light ceases. Additionally, we propose the working principles and mechanisms of these reusable adhesive films, providing new insights into the development of smart soft materials. The material's rapid deformation, high responsiveness, and flexibility make it a promising candidate for light‐controlled object transport and remote‐controlled robotics.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"125 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143713308","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

Preparation of thermally and photochemically immobilized N-type conjugated polymer films via quantitative backbone editing

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-03-27 DOI: 10.1002/anie.202505608

Charlotte Rapley, Adam V. Marsh, Edgar Gutierrez-Fernandez, Mohamad Insan Nugraha, Flurin Eisner, Martina Rimmele, Jaime Martín, Thomas D. Anthopoulos, Martin Heeney

{"title":"Preparation of thermally and photochemically immobilized N-type conjugated polymer films via quantitative backbone editing","authors":"Charlotte Rapley, Adam V. Marsh, Edgar Gutierrez-Fernandez, Mohamad Insan Nugraha, Flurin Eisner, Martina Rimmele, Jaime Martín, Thomas D. Anthopoulos, Martin Heeney","doi":"10.1002/anie.202505608","DOIUrl":"https://doi.org/10.1002/anie.202505608","url":null,"abstract":"We report a series of n-type conjugated polymers based on PNDI-TfBTT and PNDIV-TfBTT backbones constructed from electron-deficient naphthalene diimide (NDI) and fluorinated benzothiadiazole (fBT) units, with PNDIV-TfBTT incorporating a vinylene spacer. Quantitative post-polymerisation modification (PPM) via nucleophilic substitution replaced the fBT fluorine with thioether side chains, optionally containing azide groups. Thioether substitution improved solubility, while subtly changing the ordering of polymer films. Azide incorporation enabled both thermal and photochemical crosslinking, yielding insoluble and immobile films that retained good electron transport; although UV crosslinking initially reduced mobility, subsequent thermal annealing largely restored crystallinity and performance. This work underscores the utility of precise backbone editing to fine-tune the electronic and morphological properties of n-type polymers, offering new avenues for the fabrication of stable, patterned active layers in advanced organic electronic devices.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"35 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143713797","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

Enhancing the Stability of Aqueous Membrane-Free Flow Batteries: Insights into Interphase Processes

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-03-27 DOI: 10.1002/anie.202424650

Rebeca Marcilla, paula navalpotro, carla santana santos, antonio Martínez-Bejarano, murilo alcantara, vanesa muñoz-Perales, santiago Ibañez, Nomnotho Jiyane, Catarina Neves, ruben rubio-presa, thomas quast, Joao Coutinho, wolfgang Schuhmann

{"title":"Enhancing the Stability of Aqueous Membrane-Free Flow Batteries: Insights into Interphase Processes","authors":"Rebeca Marcilla, paula navalpotro, carla santana santos, antonio Martínez-Bejarano, murilo alcantara, vanesa muñoz-Perales, santiago Ibañez, Nomnotho Jiyane, Catarina Neves, ruben rubio-presa, thomas quast, Joao Coutinho, wolfgang Schuhmann","doi":"10.1002/anie.202424650","DOIUrl":"https://doi.org/10.1002/anie.202424650","url":null,"abstract":"Membrane-free flow batteries using immiscible electrolytes aim to overcome limitations of conventional redox flow batteries by eliminating expensive ion-selective membranes. However, they face challenges including low power density due to the transport constraints in immiscible electrolytes, the need for high partitioned stable compatible active species, and the overlooked self-discharge interphase phenomena that reduces coulombic efficiency. We present a novel aqueous biphasic system based on two salts improving electrolyte ionic conductivity and viscosity. Potassium ferrocyanide (K4[Fe(CN)6]) and sulfonated viologen ((SPr2)V) species were examined computationally and experimentally demonstrating effective species separation in all oxidation states, achieving a tenfold higher concentration in their electrolyte. The mutual compatibility and stability of these species enabled unprecedented scanning electrochemical microscopy (SECM) analysis of the interphase revealing insights like species concentration gradients and crossover. The enhanced electrolyte properties expanded the open-circuit voltage to 1.1 V and improved mass transport, enabling power densities being 3.5 times higher than previous examples. The battery achieved 80.2% energy efficiency at C/2 rate and under flowing conditions it maintained stable performance over a month (400 cycles) at high states of charge. This work presents an innovative aqueous membrane-free flow battery that avoids parasitic reactions, enabling detailed interphase studies and advancing this technology.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"16 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143713799","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

An Enantioselective Spirocyclization of Pd-Enolates and Isocyanates

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-03-27 DOI: 10.1002/anie.202502583

Brian Stoltz, Jay P. Barbor, Kaylin N. Flesch, Melinda Chan, Hannah R. Ang

引用次数: 0

Unveiling the Influence of Dehydrofluorination of Poly(vinylidene fluoride) Binder on the Failure of Graphite Anode in Potassium‐ion Batteries

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-03-27 DOI: 10.1002/anie.202502872

Yangtian Yan, Junyang Hu, Yueteng Gao, Tingzhen Hou, Biao Zhang, Baohua Li, Jin Liang, Feiyu Kang, Dengyun Zhai

{"title":"Unveiling the Influence of Dehydrofluorination of Poly(vinylidene fluoride) Binder on the Failure of Graphite Anode in Potassium‐ion Batteries","authors":"Yangtian Yan, Junyang Hu, Yueteng Gao, Tingzhen Hou, Biao Zhang, Baohua Li, Jin Liang, Feiyu Kang, Dengyun Zhai","doi":"10.1002/anie.202502872","DOIUrl":"https://doi.org/10.1002/anie.202502872","url":null,"abstract":"The poly(vinylidene fluoride) (PVDF) binder has been successfully employed in lithium‐ion batteries (LIBs), but it unexpectedly exhibits detrimental effects on the anode performance in potassium‐ion batteries (PIBs). The PVDF‐based graphite electrode shows a low Coulombic efficiency and even fails to maintain the electrode integrity after several cycles in the 0.8 M KPF6 ethylene carbonate/diethyl carbonate electrolyte. In this study, we unveil that the dehydrofluorination reaction of PVDF initiated by potassium ethoxide may be the key factor causing the above issues. The dehydrofluorination not only disables the binder but also releases detrimental ethanol into the electrolyte. The released ethanol can dissolve the organic components of solid electrolyte interphase (SEI) and deplete the potassium resource, thereby resulting in a reduction of Coulombic efficiency and a more severe accumulation of SEI. The crowding of more accumulated SEI coupled with the large volume expansion of intercalated graphite results in the failure of PVDF‐based graphite electrodes. This fundamental finding may provide a deeper insight into the failure mechanism of PVDF as a binder in PIBs, and meanwhile, give valuable guidance for the use of PVDF in battery communities containing sodium‐ion batteries and LIBs.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"20 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143712861","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