Angewandte Chemie International Edition最新文献_第6页

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

引用次数: 0

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}

引用次数: 0

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

Aptamer as a molecular tethering agent induces PrPC aggregation and degradation to inhibit melanoma proliferation 适配体作为分子系带剂诱导PrPC聚集和降解抑制黑色素瘤增殖

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-04-30 DOI: 10.1002/anie.202425051

Tiantian Xie, Yibin Zhang, Neng Ling, Yijun Yuan, Weibin Liu, Junxiao Guo, Xianhua Wei, Tianhuan Peng, Zhiyan Wang, Jing Dai, Wenjing Chen, Ming Yan, Xiaoqiu Wu, Wencan Wu, Mao Ye, Weihong Tan

{"title":"Aptamer as a molecular tethering agent induces PrPC aggregation and degradation to inhibit melanoma proliferation","authors":"Tiantian Xie, Yibin Zhang, Neng Ling, Yijun Yuan, Weibin Liu, Junxiao Guo, Xianhua Wei, Tianhuan Peng, Zhiyan Wang, Jing Dai, Wenjing Chen, Ming Yan, Xiaoqiu Wu, Wencan Wu, Mao Ye, Weihong Tan","doi":"10.1002/anie.202425051","DOIUrl":"https://doi.org/10.1002/anie.202425051","url":null,"abstract":"Melanoma, a malignant tumor originating from melanocytes, is the most aggressive and deadly form of skin cancer. Previous studies have revealed that the cellular prion protein (PrPC) is frequently overexpressed in melanoma, contributing to tumor progression. This study presents the first proof-of-concept evidence that nucleic acid aptamers can be used to construct a molecular tethering agent that regulates PrPC protein levels by inducing membrane-bound PrPC aggregation for anti-melanoma therapy. Using a screening strategy combining cell-SELEX and cell-internalization SELEX, we obtained an ssDNA aptamer, TT-1e, specifically binding to melanoma cells and tissues. We identified that the binding site of TT-1e is located at the octapeptide repeat region of glycosylated PrPC. Based on the binding characteristics of TT-1e, we engineered an aptamer-based molecular tethering agent TTe-TTe. We found that TTe-TTe induces aggregation of cell surface PrPC, promoting its internalization and facilitating its lysosomal degradation. This process resulted in the inhibition of AKT pathway activation. Importantly, in vivo studies confirmed the ability of TTe-TTe to target melanoma xenografts and suppress tumor growth through this unique mechanism. Our study presents a promising strategy for targeted melanoma therapy and introduces a paradigm-shifting approach for manipulating protein levels using aptamers as molecular tethering agents.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"41 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-04-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143889511","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 Cyclic Olefin Polymers via Group Transfer Radical Cyclopolymerization for High Performance in Anode-Free Batteries 基团转移自由基环聚合法制备高性能无阳极电池用环烯烃聚合物

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-04-30 DOI: 10.1002/anie.202507557

Yasu Chen, Shuo Wang, Tongkun Wang, Xianjin Wang, Hao Sun, Chen Zhu

{"title":"Preparation of Cyclic Olefin Polymers via Group Transfer Radical Cyclopolymerization for High Performance in Anode-Free Batteries","authors":"Yasu Chen, Shuo Wang, Tongkun Wang, Xianjin Wang, Hao Sun, Chen Zhu","doi":"10.1002/anie.202507557","DOIUrl":"https://doi.org/10.1002/anie.202507557","url":null,"abstract":"Cyclic olefin polymers (COPs) are of high importance in optical and medical materials. These materials are typically synthesized via ring-opening metathesis polymerization (ROMP) of norbornene derivatives, using metallocene catalysts, followed by high-pressure hydrogenation catalyzed by noble metals. However, the complex synthetic processes, the continuous use of expensive catalysts, and the need to remove metal residues remain substantial barriers in COP production. In contrast, radical cyclopolymerization of dienes, which eliminates the need for metal catalysis and hydrogenation, offers a promising alternative for COP synthesis. Nevertheless, chain transfer reactions hinder the radical polymerization of non-conjugated dienes. To address these challenges, we present a novel strategy, group transfer radical cyclopolymerization (GTRCP), which effectively suppresses chain transfer and enables radical polymerization of dienes to yield COPs. This approach allows for the production of a broad range of sequenceregulated COPs with high molecular weights and low dispersity. Density functional theory (DFT) calculations support the proposed GTRCP mechanism, highlighting its efficiency and selectivity, driven by substantial thermodynamic forces. The resulting COPs demonstrate great potentials as the interphase layer materials in anode-free lithium metal batteries, significantly enhancing the cycling performance towards practical energy storage applications.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"19 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-04-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143889517","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

Thrombus Boring Microrobot Prepared by an Integrated Phase Separation and Interfacial Self-Assembly Process towards Thrombolysis 基于相分离和界面自组装的溶栓微机器人

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-04-30 DOI: 10.1002/anie.202503221

Han Bao, Sen Zhang, Jing Luo, Jingxin Meng, Shutao Wang

{"title":"Thrombus Boring Microrobot Prepared by an Integrated Phase Separation and Interfacial Self-Assembly Process towards Thrombolysis","authors":"Han Bao, Sen Zhang, Jing Luo, Jingxin Meng, Shutao Wang","doi":"10.1002/anie.202503221","DOIUrl":"https://doi.org/10.1002/anie.202503221","url":null,"abstract":"The pathological formation of thrombi is the primary etiological factor of acute cardiovascular and cerebrovascular diseases, accounting for one-quarter of global fatalities. Traditional thrombolytic drugs are constrained by short half-life, low utilization, and severe complications. Inspired by the tunnel boring machine to excavate strata into small rocks, we reported urokinase plasminogen activator (uPA)-modified thrombus boring microrobots (uTBMs), prepared by a one-step integrated phase separation and interfacial self-assembly process, for effective thrombolysis. The uTBMs are composed of microspheres capped with dual-layered structures of magnetic nanoparticles (MNPs) and cilia nanostructures. In situ observation reveals the integrated phase separation and interfacial self-assembly process of the uTBMs within an emulsion droplet. The capped layer of MNPs allows for controllable motion and rotation behavior under the manipulation of a remote magnetic field. The uPA-modified cilia nanostructures grasp and degrade the fibrin network, synergizing with the uTBMs rotation to mechanically excavate blood cells from thrombus individually, achieving ~8.5-fold higher thrombolytic efficacy than uPA alone. This research demonstrates the feasibility of controllably fabricating and modifying complex-structured microrobots via the simple process towards the potential thrombus therapy.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"102 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-04-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143889519","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