Angewandte Chemie International Edition最新文献_第10页

A Dynamic Self-healing Protective Layer Enabling Stable Zinc Ion Batteries Through Strong Zn-S Affinity and Intramolecular Hydrogen Bonding 一种动态自愈保护层，通过强锌- s亲和力和分子内氢键使锌离子电池稳定

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-13 DOI: 10.1002/anie.202503345

Bao Li, Bo Zhang, Xiang Bai, Jiahui Zhang, Xinyue Chang, Lifeng Hou, Hao Huang, Tiantian Lu, Shi Wang, Zhong Jin, Qian Wang

{"title":"A Dynamic Self-healing Protective Layer Enabling Stable Zinc Ion Batteries Through Strong Zn-S Affinity and Intramolecular Hydrogen Bonding","authors":"Bao Li, Bo Zhang, Xiang Bai, Jiahui Zhang, Xinyue Chang, Lifeng Hou, Hao Huang, Tiantian Lu, Shi Wang, Zhong Jin, Qian Wang","doi":"10.1002/anie.202503345","DOIUrl":"https://doi.org/10.1002/anie.202503345","url":null,"abstract":"Aqueous Zn-ion batteries (AZIBs) are widely regarded as the ideal candidate for large-scale energy storage systems. However, Zn metal anode has long faced challenges, such as: hydrogen evolution reaction, dendrite growth, surface corrosion. Herein, we report the development of a self-healable and strongly adhesive polymer protective layer for AZIBs, which is achieved by polymerizing a natural small molecule, thioctic acid (TA) on Zn surface. Thanks to the strong and spontaneous affinity between Zn metal surface and S atoms on polymer chains, this polymer protective layer can firmly and dynamically adhere to the Zn surface. Thus, even at a thickness of only <1 μm, the protective layer can exhibit a strong adhesion force of up to 10.5 N with Zn surface, while the abundant carboxyl groups in protective layer can form intramolecular hydrogen bonds, endowing its high self-healing property and enhancing its strength. Such a protective layer effectively inhibits the dendrite growth physically, regulates the Zn2+ migration and deposition behavior chemically. Therefore, the symmetric cells can be cycled for ~1000 h at the current density of 1.0 mA cm-2 and 5.0 mA cm-2, respectively. The full cells with NH4V4O10 can also run stably for 1000 cycles with a high capacity retention.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"22 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-05-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143940499","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

Supramolecular Polyanions as Effective Interphase Layers for Anode-Free Lithium Metal Batteries 超分子聚阴离子作为无阳极锂金属电池有效的界面层

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-13 DOI: 10.1002/anie.202505794

Yongfeng Zhou, Jinghan Li, Yupo Xu, Wei You, Chengkai Hong, Shui Yu, Zhaofeng Ouyang, Zhaoming Zhang, Wei Yu, Hao Sun, Chunyang Yu, Wenfeng Jiang

{"title":"Supramolecular Polyanions as Effective Interphase Layers for Anode-Free Lithium Metal Batteries","authors":"Yongfeng Zhou, Jinghan Li, Yupo Xu, Wei You, Chengkai Hong, Shui Yu, Zhaofeng Ouyang, Zhaoming Zhang, Wei Yu, Hao Sun, Chunyang Yu, Wenfeng Jiang","doi":"10.1002/anie.202505794","DOIUrl":"https://doi.org/10.1002/anie.202505794","url":null,"abstract":"Supramolecular polymers (SPs) driven by host-guest interactions have seen considerable advancements over the past decade, but the guest species involved are predominantly neutral molecules or cations. Strong and dependable macrocycle-anion interactions for supramolecular polymerization are highly sought after, yet the functionalities of this class of SPs featuring negatively charged backbones remain largely unexplored. Here we report a novel host-guest interaction between one tetraurea macrocycle and two organophosphate anions with high affinity (association constant Ka = 1.06 × 109 M−2). It can serve as noncovalent joints to efficiently link low-molecular-mass polyethylene oxide (PEO) diorganophosphates into long linear SPs. Being used as an interphase layer in anode-free lithium (Li) metal batteries, the polymer material promotes Li+ absorption and desolvation through electrostatic attractions, and enables fast Li+ transport by the alternatingly arranged anionic linkages and PEO units in the polymer main chain. As a result, the SP layer homogenizes Li+ flux to achieve uniform Li deposition, and significantly improves the electrochemical performance of LiFePO4 full batteries by a factor of 285% with cycling stability over 200 cycles. These findings pave the way for a new family of anion-based SPs with tunable architectures and compositions, and suggest their promising applications in future batteries.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"113 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-05-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143940599","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: Enzyme-Activated Orthogonal Proteolysis Chimeras for Tumor Microenvironment-Responsive Immunomodulation 内封面：用于肿瘤微环境反应性免疫调节的酶激活正交蛋白水解嵌合体

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-13 DOI: 10.1002/anie.202510013

Caixia Sun, Songhan Liu, Jun Wei Lau, Hanyu Yang, Yun Chen, Bengang Xing

引用次数: 0

One‐dimensional Covalent Organic Frameworks: From Design, Synthesis to Applications 一维共价有机框架：从设计、合成到应用

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-13 DOI: 10.1002/anie.202507002

Pei Huang, Lu-Hua Hou, Ming-Yi Yang, Cheng Xiao, Yan-Li Wu, Si-Jing Cai, Wen-Jie Guo, Mi Zhang, Meng Lu, Ya-Qian Lan

{"title":"One‐dimensional Covalent Organic Frameworks: From Design, Synthesis to Applications","authors":"Pei Huang, Lu-Hua Hou, Ming-Yi Yang, Cheng Xiao, Yan-Li Wu, Si-Jing Cai, Wen-Jie Guo, Mi Zhang, Meng Lu, Ya-Qian Lan","doi":"10.1002/anie.202507002","DOIUrl":"https://doi.org/10.1002/anie.202507002","url":null,"abstract":"As an important branch of the covalent organic frameworks (COFs) family, one‐dimensional COFs (1D COFs) which formed by the ordered arrangement of confined covalent bonds in one dimension and non‐covalent interactions (van der Waals force, π‐π interactions and hydrogen bonds, etc.) in the vertical two and three dimensions has aroused much attention. Compared with 2D/3D COFs, 1D COFs behaved more easily dispersing and had more opportunities for active sites exposure due to their weaker interchain/interlayer interaction, modified nonlinear edge, and pore structures. These features make them have great application potential in many fields including catalysis, energy storage, adsorption, sensing, and others. In this minireview, we highlight the state‐of‐the‐art advances of 1D COFs in the structure design principles of building blocks, synthesis strategies, and their related applications. Furthermore, we present an in‐depth outlook on the challenges and opportunities faced by 1D COFs, aiming to offer insights for future studies in this intriguing and significant research field.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"124 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-05-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143933415","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

Metal‐Free Electrochemistry‐Driven Decarboxylative Primary Alkyl‐alkoxylation of Olefins 无金属电化学驱动的烯烃伯烷基-烷氧基脱羧反应

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-13 DOI: 10.1002/anie.202506639

Hu Cai, Meiqun Lu, Kailun Chen, Tao Wu

引用次数: 0

Outside Back Cover: Data–Knowledge-Dual-Driven Electrolyte Design for Fast-Charging Lithium Ion Batteries 外后盖：数据-知识-双驱动电解液设计的快速充电锂离子电池

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-13 DOI: 10.1002/anie.202510008

i Yang, Nan Yao, Yu-Chen Gao, Xiang Chen, Yu-Xin Huang, Shuo Zhang, Han-Bing Zhu, Lei Xu, Yu-Xing Yao, Shi-Jie Yang, Zheng Liao, Zeheng Li, Xue-Fei Wen, Peng Wu, Ting-Lu Song, Jin-Hao Yao, Jiang-Kui Hu, Chong Yan, Jia-Qi Huang, Qiang Zhang

引用次数: 0

Bridging Nano to Micron: Architectural Engineering of Supramolecular Bottlebrushes for Extensively Tunable Structures and Photonics 桥接纳米到微米：广泛可调结构和光子学的超分子瓶刷的建筑工程

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-13 DOI: 10.1002/anie.202503633

Dezhi Liu, Zhenli Zhang, Yu-Xia Zhang, Yue-Sheng Li, Dong-Po Song

{"title":"Bridging Nano to Micron: Architectural Engineering of Supramolecular Bottlebrushes for Extensively Tunable Structures and Photonics","authors":"Dezhi Liu, Zhenli Zhang, Yu-Xia Zhang, Yue-Sheng Li, Dong-Po Song","doi":"10.1002/anie.202503633","DOIUrl":"https://doi.org/10.1002/anie.202503633","url":null,"abstract":"Supramolecular bottlebrush block copolymers (BBCPs) offer greater architectural adaptability than covalent BBCPs. However, the dynamic nature of non-covalent interactions hinders precise control over their chain architecture, resulting in poorly controlled self-assembly, unpredictable morphologies, and limited utility. Herein, we introduce a novel molecular design for amphiphilic supramolecular BBCPs that overcomes key challenges in the field. The resulting materials exhibit superior thermodynamic stability in weakly polar solvents. This enables the first demonstration of well-controlled self-assembly of supramolecular surfactants within a complex emulsion system, leading to the formation of photonic supraballs with homogenous porous structures. Critically, precise chain architectural engineering enables pore diameter tuning over an unprecedented nanometer-to-micrometer range (67 nm-1.92 µm), significantly surpassing the maximum domain sizes achievable with self-assembled covalent BBCPs. This extends the photonic bandgap into the mid-wave infrared range, paving the way for next-generation materials with potential applications in thermal management.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"28 1","pages":"e202503633"},"PeriodicalIF":16.6,"publicationDate":"2025-05-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143945843","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

A Heterodimeric Cluster‐based Pair Catalyst for Electrochemical Synthesis of Cyclohexanone Oxime 电化学合成环己酮肟的异二聚簇对催化剂

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-13 DOI: 10.1002/anie.202507569

Tongxin Song, Chenyang Shen, Yiqi Tian, Qingxi Zhai, Shisi Tang, Yan Zhu

{"title":"A Heterodimeric Cluster‐based Pair Catalyst for Electrochemical Synthesis of Cyclohexanone Oxime","authors":"Tongxin Song, Chenyang Shen, Yiqi Tian, Qingxi Zhai, Shisi Tang, Yan Zhu","doi":"10.1002/anie.202507569","DOIUrl":"https://doi.org/10.1002/anie.202507569","url":null,"abstract":"Heterogeneous catalysts are complex chemical ecosystems, where various functional units execute their individual responsibilities to together complete a catalysis ensemble. Here we report a dinuclear catalyst originated from two molecular‐purity monomers including an atomically precise Ag4Pd2(SR)8 cluster and a polyoxotitanium Ti4O2(TBC[4])2(iPrO)4 cluster that are eventually paired off by the bridging sulfur. The heterodimeric catalyst with a unique interface consisted of the Ti‐S‐metal (metal = Pd and Ag) motifs exhibits selective recognition for nitrogen sources, thereby achieving high performances for the electrochemical synthesis of cyclohexanone oxime. The nitrate is favourably deoxygenated on the metal sites to generate nitrite, followed by the flipping of nitrite at the Ti‐S‐metal interface and the stepwise reduction of nitrite on the Ti site to produce hydroxylamine. Sequentially a spontaneous coupling from hydroxylamine and cyclohexanone proceeds to construct the C=N bond for cyclohexanone oxime. Using this combination of distinct functional modules into one catalyst, we develop a strategy for heterogeneous catalysts being designed to increase the substrate conversion while simultaneously increasing the target product selectivity.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"8 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-05-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143933418","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

Bright and Fast-response Hybrid X-ray Scintillators by Molecular and Dielectric Confinement 分子和介电约束下的明亮和快速响应混合x射线闪烁体

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-13 DOI: 10.1002/anie.202504576

Long Gu, Yitong Jiao, Ruizi Li, Haoyang Wang, Weiguo Zhu, Yuan Gao, Feng Xu, Bo Wu, Xiong Huang, Wei Huang

{"title":"Bright and Fast-response Hybrid X-ray Scintillators by Molecular and Dielectric Confinement","authors":"Long Gu, Yitong Jiao, Ruizi Li, Haoyang Wang, Weiguo Zhu, Yuan Gao, Feng Xu, Bo Wu, Xiong Huang, Wei Huang","doi":"10.1002/anie.202504576","DOIUrl":"https://doi.org/10.1002/anie.202504576","url":null,"abstract":"Scintillators featuring bright and fast-response properties are essential for high-speed and dynamic X-ray imaging. Nevertheless, simultaneously possessing high light yields and fast response remains a significant challenge for most scintillators. Herein, we propose a strategy to achieve the bright and fast-response characteristics of scintillators by leveraging the combined effects of dielectric and molecular confinement in organic-inorganic hybrid scintillators (TPA)2MnBr4. Thereinto, large tetrapropylammonium cations (TPA+) surround [MnBr4]2− units, forming a zero-dimensional (0D) molecular confinement structure that promotes electron localization and achieves a notable light yield of 56800 photons MeV−1. Meanwhile, the low dielectric constant of TPA+ can enhance dielectric confinement of [MnBr4]2− units, mitigating exciton capture by deep defects. These synergistic effects in the scintillators lead to a large exciton binding energy of 1028.8 meV and an ultrafast response time of 500 fs. Notably, under the irradiation of X-rays, (TPA)2MnBr4 exhibits an extremely low detection limit of 18.7 nGyair s−1 and an exceptional spatial resolution of 21.0 lp mm−1. Given the bright and fast-response features of scintillators, we demonstrate the potential applications in 3D dynamic and real-time X-ray imaging. These findings lay the groundwork for designing high-performance scintillators and open avenues for innovative applications in high-resolution and dynamic imaging","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"106 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-05-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143940498","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

Ultrasound-Responsive Lipid Nanosonosensitizers with Size Reduction and NO Release: Synergistic Sonodynamic-Chemo-Immunotherapy for Pancreatic Tumors 超声反应性脂质纳米超声增敏剂缩小尺寸和释放NO：协同声动力-化学-免疫治疗胰腺肿瘤

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-13 DOI: 10.1002/anie.202507388

Leyi Fang, Wenhui Zeng, Yili Liu, Yinxing Miao, Chunmei Lu, Zhonghan Xu, Shenshen Zhou, Qi Xue, Yitong Xu, Xiqun Jiang, Jingjuan Xu, Yan Zhang, Deju Ye

{"title":"Ultrasound-Responsive Lipid Nanosonosensitizers with Size Reduction and NO Release: Synergistic Sonodynamic-Chemo-Immunotherapy for Pancreatic Tumors","authors":"Leyi Fang, Wenhui Zeng, Yili Liu, Yinxing Miao, Chunmei Lu, Zhonghan Xu, Shenshen Zhou, Qi Xue, Yitong Xu, Xiqun Jiang, Jingjuan Xu, Yan Zhang, Deju Ye","doi":"10.1002/anie.202507388","DOIUrl":"https://doi.org/10.1002/anie.202507388","url":null,"abstract":"Pancreatic cancer (PC) remains difficult to treat due to its dense extracellular matrix (ECM), immunosuppressive tumor microenvironment (TME), and deep-seated anatomy. To address these challenges, we developed IR&ZnPc@LNP-NO, an ultrasound (US)-responsive lipid nanosonosensitizer that synergizes sonodynamic therapy (SDT), chemotherapy, and immunotherapy for orthotopic PC. IR&ZnPc@LNP-NO undergoes three key US-activated responses: (1) size reduction, (2) controlled release of irinotecan (IR) and nitric oxide (NO), and (3) generation of reactive oxygen species (ROS). Under low-dose US, IR&ZnPc@LNP-NO reduces in size (from ~120 nm to ~40 nm), enhancing tumor penetration, and releases NO to remodel the TME by normalizing vasculature and degrading ECM. This enhances nanosonosensitizers accumulation and cytotoxic T cells (CTLs) infiltration. High-dose US irradiation triggers the generation of cytotoxic ROS, which, in combination with IR-mediated chemotherapy, induces immunogenic cell death (ICD) and enhances antitumor immunity. Additionally, combining IR&ZnPc@LNP-NO with PD-L1 antibody (αPD-L1) immunotherapy significantly prolongs survival in orthotopic PC models. The cascade strategy—size reduction, TME remodeling, and multimodal therapy—effectively overcomes stromal and immunosuppressive barriers, offering a robust platform for treating deep-seated PC.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"51 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-05-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143940592","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