Angewandte Chemie International Edition最新文献_第4页

Access to N‐Monofluoromethylated (Thio)Carbamates, Formamides, Alkynamides and Related Derivatives N‐单氟甲基化（硫代）氨基甲酸酯、甲酰胺、烷基酰胺及相关衍生物的获取

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-01 DOI: 10.1002/anie.202505478

Filip G. Zivkovic, Fritz Bahns, Che-Ming Hsu, Franziska Schoenebeck

引用次数: 0

Hydrogen-Bonded Organic Framework with Desolventization and Lithium-Rich Sites for High-Performance Lithium Metal Anodes 高性能金属锂阳极用脱氧富锂氢键有机骨架

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-01 DOI: 10.1002/anie.202506892

Songling Wu, Xiaomeng Lu, Yiwen Sun, Haichao Wang, Muhammad Ahsan Waseem, Junaid Aslam, Yi Xu, Li-Ping Lv, Yong Wang

{"title":"Hydrogen-Bonded Organic Framework with Desolventization and Lithium-Rich Sites for High-Performance Lithium Metal Anodes","authors":"Songling Wu, Xiaomeng Lu, Yiwen Sun, Haichao Wang, Muhammad Ahsan Waseem, Junaid Aslam, Yi Xu, Li-Ping Lv, Yong Wang","doi":"10.1002/anie.202506892","DOIUrl":"https://doi.org/10.1002/anie.202506892","url":null,"abstract":"Effectively managing Li+ migration behaviors and addressing the issues of side reactions at the electrolyte–electrode interface is crucial for advancing high-performance lithium metal batteries (LMBs). Herein, this work introduces a two-dimensional hydrogen-bonded organic framework (HOF) enriched with multi-site H-bonding and lithiophilic sites for the first time to tailor the electronic structure and solvation chemistry in lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) based electrolyte and stabilize the lithium metal anodes (LMAs) interface. Initially, the abundant lithiophilic sites (C=O, C=N) in the HOF coordinate with Li+, acting as key electron donors to optimize the electronic structure while also reducing the desolvation energy barrier when Li+ dissociates from the solvent sheath. Moreover, the multifunctional hydrogen bonding not only acts as the “appended manipulator” to anchor -NH2 to LiTFSI and reduces the adverse reactions at the LMAs interface but also mitigates the mechanical stress during lithium deposition. As evidenced by various in/ex situ characterizations, the HOF-modified lithium-metal symmetric batteries exhibit ultra-long cycling performance (11000 h) and low voltage fluctuations at 3 mA cm-2. This unique strategy of hydrogen-bonded synergistic lithiophilic sites provides a new perspective on the design of artificial interfacial layers for stabilizing lithium metal batteries.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"35 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143897740","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

Simultaneous improvement of mechanical strength, toughness, and self‐healability of elastomers enabled by F–H‐bond‐based nanoconfinement 同时提高弹性体的机械强度、韧性和自愈性，使基于F-H键的纳米约束成为可能

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-01 DOI: 10.1002/anie.202505848

Yujie Jia, Chengzhen Chu, Zekai Wu, Yufeng Ni, Shichun Cao, Tao Liao, Ce Shi, Yongfeng Men, Junfen Sun, Zhengwei You

{"title":"Simultaneous improvement of mechanical strength, toughness, and self‐healability of elastomers enabled by F–H‐bond‐based nanoconfinement","authors":"Yujie Jia, Chengzhen Chu, Zekai Wu, Yufeng Ni, Shichun Cao, Tao Liao, Ce Shi, Yongfeng Men, Junfen Sun, Zhengwei You","doi":"10.1002/anie.202505848","DOIUrl":"https://doi.org/10.1002/anie.202505848","url":null,"abstract":"There are often trade‐offs among high mechanical strength, high toughness, and efficient self‐healing. Herein, we present a biomimetic strategy utilizing F–H bonds for nanoconfinement to achieve the simultaneous enhancement of these conflicting properties. The mechanical strength, toughness, and self‐healing efficiency of a fluorinated crosslinked poly(urethane‐urea) (CPUU‐FA) elastomer are improved 1.3‐, 1.5‐, and 1.2‐fold, respectively, compared with those of its non‐fluorinated counterpart. Notably, the CPUU‐FA has the highest recorded puncture energy (887 mJ) among polymeric elastomers and the highest fracture energy (117 kJ m–2) among reported thermoset elastomers. Moreover, it exhibits excellent self‐healing efficiency (99%), remarkable reprocessability, and a low surface energy (56 MJ m–2). The application of self‐healing elastomers in the fabrication of soft electronics is further demonstrated. The molecular design strategy is anticipated to inspire new developments in high‐performance materials for cutting‐edge applications.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"56 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143893745","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

Understanding the Position Effects of Monoatom Doping in Silver Nanoclusters on Oxygen Reduction by Single Entity Electrochemistry 单实体电化学研究银纳米团簇中单原子掺杂对氧还原的位置影响

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-01 DOI: 10.1002/anie.202506627

Wei Ma, Zehui Sun, Cheng Chen, Mengdan Wei, Haifeng Wang, Jianfu Chen

{"title":"Understanding the Position Effects of Monoatom Doping in Silver Nanoclusters on Oxygen Reduction by Single Entity Electrochemistry","authors":"Wei Ma, Zehui Sun, Cheng Chen, Mengdan Wei, Haifeng Wang, Jianfu Chen","doi":"10.1002/anie.202506627","DOIUrl":"https://doi.org/10.1002/anie.202506627","url":null,"abstract":"Alloying nanoclusters (NCs) with monoatom doping represent an effective strategy to enhance catalytic performances due to the synergistic interactions between the dopant and host atoms. However, in‐depth understanding the position effects of monoatom doping within alloying NCs, particularly at the atomic level, remains elusive. Here, we employed single entity collision electrochemistry method to investigate the electrocatalytic behaviors of individual monoatom‐doped bimetallic M1Ag24 (M= Ag, Au, Pt, Cu) NCs toward oxygen reduction reaction (ORR). By relying on high‐resolution and high‐throughput electrochemical measurements, we successfully discriminated the effects of monoatom variation in M1Ag24 NCs on ORR activity at the single atom resolution and identified different M1Ag24 NCs across characteristic populations. Our experimental findings and theoretical calculations reveal the electrocatalytic reaction dynamics associated with intracluster migration of Au monoatom during the dynamic alloying process of Au1Ag24 NCs. This work demonstrates a novel approach for in situ indentifying the position effects of foreign doping atoms on the electrocatalytic activity of alloy NCs at the single atom level.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"72 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143893744","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

Induced Chirality and Vibrational Optical Activity in an Ionic-Liquid Anion 离子-液体阴离子的诱导手性和振动光学活性

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-01 DOI: 10.1002/anie.202502885

Tom Frömbgen, Katrin Drysch, Thierry Tassaing, Thierry Buffeteau, Oldamur Holloczki, Barbara Kirchner

{"title":"Induced Chirality and Vibrational Optical Activity in an Ionic-Liquid Anion","authors":"Tom Frömbgen, Katrin Drysch, Thierry Tassaing, Thierry Buffeteau, Oldamur Holloczki, Barbara Kirchner","doi":"10.1002/anie.202502885","DOIUrl":"https://doi.org/10.1002/anie.202502885","url":null,"abstract":"Here, we show that the four conformers of the regularly used ionic liquid anion bis(trifluoromethylsulfonyl)imide [NTf2]- are true enantiomeric pairs by analyzing their calculated vibrational circular dichroism spectra.\u0000The significant modes involve those atoms of the anion that form specific hydrogen bond patterns with the chiral probe molecule propylene oxide.\u0000Adding this probe molecule to the ionic liquid 1-ethyl-3-methylimidazolium bis(trifluoromethyl-sulfonyl)imide, the experimental and simulated spectra indicate intermolecular interaction between the chiral molecule and the liquid and thus the induction of chirality in the anion.\u0000This emergence of chirality in the ionic liquid takes place via the hydrogen bonding between the anion of the ionic liquid and the solute, which results in a redistribution of the symmetric occurrence of conformers to an asymmetric one.\u0000Altogether this study reveals the mechanism of chiral induction from the propylene oxide molecule to the ionic liquid anion, while pointing out the importance of rational over a random choice of the ionic liquid building units.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"134 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143897739","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

Highly Enantioselective Organocatalysis with Bidentate Halogen Bond Donors 双齿卤素键供体的高对映选择性有机催化

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-01 DOI: 10.1002/anie.202506476

Julian Wolf, Meghana Poliyodath Mohanan, Raphaël Robidas, Revannath L. Sutar, Elric Engelage, Claude Y. Legault, Stefan Matthias Huber

引用次数: 0

Tailoring Zn-ion Solvation Structures for Enhanced Durability and Efficiency in Zinc-Bromine Flow Batteries 定制锌离子溶剂化结构，提高锌-溴液流电池的耐用性和效率

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-01 DOI: 10.1002/anie.202502739

Norah S. Alghamdi, Dmitrii Rakov, Xiyue Peng, Jaeho Lee, Yongxin Huang, Xingchen Yang, Shuangbin Zhang, Ian R. Gentle, Lianzhou Wang, Bin Luo

{"title":"Tailoring Zn-ion Solvation Structures for Enhanced Durability and Efficiency in Zinc-Bromine Flow Batteries","authors":"Norah S. Alghamdi, Dmitrii Rakov, Xiyue Peng, Jaeho Lee, Yongxin Huang, Xingchen Yang, Shuangbin Zhang, Ian R. Gentle, Lianzhou Wang, Bin Luo","doi":"10.1002/anie.202502739","DOIUrl":"https://doi.org/10.1002/anie.202502739","url":null,"abstract":"Aqueous zinc-bromine flow batteries (ZBFBs) are among the most appealing technologies for large-scale stationary energy storage due to their scalability, cost-effectiveness, safety and sustainability. However, their long-term durability is challenged by issues like the hydrogen evolution reaction (HER) and dendritic zinc electroplating. Herein, we address these challenges by reshaping the Zn2+ ion solvation structures in zinc bromide (ZnBr2) aqueous electrolytes using a robust hydrogen bond acceptor as a co-solvent additive. Our findings highlight the critical role of interactions within the first and second Zn2+ solvation shells in determining electrochemical performance. By selectively incorporating a low volume percentage of organic additive into the second coordination shell, we achieve effective proton capture, electrolyte pH stabilisation during the Zn0 electroplating, and mitigation of ion transport resistance. This approach prevents the formation of a passivation interphase layer on the electrode surface, which typically occurs with higher additive concentrations, leading to increased interphase resistance, viscosity and cell polarization. This work opens a new avenue in modulating Zn2+ reactivity and stability through precise solvation structure design, enabling efficient and reversible Zn0/2+ cycling in aqueous electrolytes without H2 evolution. These findings pave the way for the development of commercially viable, high-performance ZBFBs for energy storage applications.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"72 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143893556","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

On‐Surface Synthesis of Nanographenes Through Domino Cyclization Reactions 通过多米诺环化反应在表面合成纳米石墨烯

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-01 DOI: 10.1002/anie.202425167

Shijie Sun, Qingyan Li, Takatsugu Onishi, Goudappagouda -, Hangjing Zhou, Lei Gao, Yoshinori Okada, Jianchen Lu, Akimitsu Narita, Jinming Cai

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Lysine-targeting, Covalent Inhibitors of Bromodomain BD1 of BET Proteins in Live Cells and Animals 活细胞和动物中以赖氨酸为靶点的溴域BD1共价抑制剂

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-01 DOI: 10.1002/anie.202424832

Tao Li, Wenjie Zhang, Yiqing Wang, Guangyu Xu, Fengfei Miao, Peng Chen, Guanghui Tang, Xiaotong Ze, Jing Xiang, Jiaqian Yan, Miaomiao Wang, Min Liu, Xiaojie Wang, Wei Tang, Fan Yi, Zhi-Min Zhang, Rui Wang, Shao Q Yao, Yusheng XIE

{"title":"Lysine-targeting, Covalent Inhibitors of Bromodomain BD1 of BET Proteins in Live Cells and Animals","authors":"Tao Li, Wenjie Zhang, Yiqing Wang, Guangyu Xu, Fengfei Miao, Peng Chen, Guanghui Tang, Xiaotong Ze, Jing Xiang, Jiaqian Yan, Miaomiao Wang, Min Liu, Xiaojie Wang, Wei Tang, Fan Yi, Zhi-Min Zhang, Rui Wang, Shao Q Yao, Yusheng XIE","doi":"10.1002/anie.202424832","DOIUrl":"https://doi.org/10.1002/anie.202424832","url":null,"abstract":"The bromodomain extra-terminal (BET) family of proteins are valuable therapeutic targets for cancer and other diseases. The adverse events of current pan-BET inhibitors (BETi) make the development of BET BD1- or BD2-selective inhibitors as a fresh avenue to overcome safety challenges. On the basis of various lysine-reactive covalent warheads, herein we report a set of activity-based probes (ABPs; P3-P7) capable of global profiling of ligandable lysines within bromodomains (BRDs) in live cells and animals. Chemoproteomic experiments with P7 which utilizes 2-ethynylbenzaldehyde (EBA) identified 16 endogenous BRDs, thus giving a global landscape of ligandable lysines in BRDs. By further introducing EBA and salicylaldehyde into PLX51107 (a noncovalent BETi), we generated lysine-reactive, irreversible (BDS1-4) and reversible (BDS5-6) BD1 covalent inhibitors. Mass spectrometry and X-ray crystallography confirmed the successful covalent engagement between EBA and K91 near the acetylated lysine (Kac)-binding site of BD1 in BRD4. BDS4 showed 104-fold selectivity for BD1 over BD2 with prolonged anticancer effects. Importantly, BDS4 retained robust activity against fibrosis in cells and animals when compared to RVX-208 (a reported BD2-selective noncovalent inhibitor) which showed only marginal effects. Our work serves as a useful tool to delineate distinct functions of BD1 and BD2 in future studies.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"51 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143897741","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}

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Photodriven Aquatic Locomotion in Liquid Crystalline Elastomer Composites with Tunable Wettability 具有可调润湿性的液晶弹性体复合材料的光驱动水上运动

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-04-30 DOI: 10.1002/anie.202505300

Avijit Das, Joselle McCracken, Mohsin Saeed, Dhriti Nepal, Timothy J White

引用次数: 0