Angewandte Chemie International Edition最新文献_第2页

Non‐Classical Hydrogen Bond Based Efficient Solid‐State Organic Emitters Enabled by a Synergistic Anion and Mechanical Bond Effect

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-04-02 DOI: 10.1002/anie.202505774

Yi An, Ru Zhou, Ningjin Zhang, Aocheng Chen, Junfei Xing, Shu Zhang, Quan Li

引用次数: 0

Probing Inside the Catalyst Layer on Gas Diffusion Electrodes in Electrochemical Reduction of CO and CO2

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-04-02 DOI: 10.1002/anie.202504715

Qiwen Sun, Jin Wang, Linke Fu, Yao Ye, Xiaoxia Chang, Bingjun Xu

引用次数: 0

Cation‐Anion‐Engineering Modified Oxychloride Zr‐Based Lithium Superionic Conductors for All‐Solid‐State Lithium Batteries

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-04-01 DOI: 10.1002/anie.202501749

Zongnan Li, Yongbiao Mu, Kunxi Lü, Guojian Kang, Ting Yang, Shuping Huang, Mingdeng Wei, Lin Zeng, Yafeng Li

{"title":"Cation‐Anion‐Engineering Modified Oxychloride Zr‐Based Lithium Superionic Conductors for All‐Solid‐State Lithium Batteries","authors":"Zongnan Li, Yongbiao Mu, Kunxi Lü, Guojian Kang, Ting Yang, Shuping Huang, Mingdeng Wei, Lin Zeng, Yafeng Li","doi":"10.1002/anie.202501749","DOIUrl":"https://doi.org/10.1002/anie.202501749","url":null,"abstract":"Within the family of halide solid electrolytes (SEs), Li2ZrCl6 demonstrates high oxidative stability, cost‐effectiveness, and mechanical deformability, positioning it as a promising candidate for SEs. However, the application of Li2ZrCl6 as a SEs was hindered by its low ionic conductivity at room temperature. Current strategies to enhance the ionic conductivity of Li2ZrCl6 primarily are focused on single cation or anion sublattice‐engineering, each with distinct advantages and limitations. Here, we propose a novel cation and anion‐sublattice‐engineering strategy, termed CASE, to increase the amorphous content and thus enhance ionic conductivity. The incorporation of Cu2+ and O2‐ induces distinctive structural modifications within Li2ZrCl6. This structure corroborated through analytic data of X‐ray absorption spectroscopy, the neutron diffraction, and ab initio molecular dynamics. Consequently, the amorphous Li2.1Zr0.95Cu0.05Cl4.4O0.8 achieves an enhanced ionic conductivity of 2.05 mS cm‐1 at 25 °C. Furthermore, all‐solid‐state lithium batteries utilizing the amorphous Li2.1Zr0.95Cu0.05Cl4.4O0.8 as an electrolyte and LiNi0.83Co0.11Mn0.06O2 as a cathode exhibit a superior long‐term cycling stability retaining 90.3% of capacity after 1000 cycles at 2 C under room temperature, which are much higher than those of Zr‐based halide electrolytes in publications. Such a result might stimulate the development of more amorphous structures with high ionic conductivity in the CASE strategy.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"26 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143745095","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

Microporous Hard Carbon Support Provokes Exceptional Performance of Single Atom Electrocatalysts for Advanced Air Cathodes

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-04-01 DOI: 10.1002/anie.202501307

Haijing Liu, Ping Li, Kaicai Fan, Fenghong Lu, Qi Sun, Qi Zhang, Bin Li, Yajie Shu, Lingbo Zong, Lei Wang

{"title":"Microporous Hard Carbon Support Provokes Exceptional Performance of Single Atom Electrocatalysts for Advanced Air Cathodes","authors":"Haijing Liu, Ping Li, Kaicai Fan, Fenghong Lu, Qi Sun, Qi Zhang, Bin Li, Yajie Shu, Lingbo Zong, Lei Wang","doi":"10.1002/anie.202501307","DOIUrl":"https://doi.org/10.1002/anie.202501307","url":null,"abstract":"Single atom catalysts embracing metal‐nitrogen (MNx) moieties show promising performance for oxygen reduction reaction (ORR). The modification on spatially confined microenvironments, which won copious attention with respect to achieving efficient catalysts, are auspicious but yet to be inspected for MNx moieties from modulating the energetics and kinetics of ORR. Here, Fe single atoms (SAs) are immobilized in microporous hard carbon (Fe‐SAs/MPC), in which the microporous structure with crumpled graphene sheets serves confined microenvironment for catalysis. Fe‐SAs/MPC holds a remarkable half‐wave potential of 0.927 V and excellent stability for ORR. Theoretical studies unveil that hydrogen bonding between the intermediate of O* and micropore interior surfaces substantially promotes its protonation and accelerates overall ORR kinetics. Both the aqueous and quasi‐solid‐state zinc‐air batteries driven by Fe‐SAs/MPC air cathode show excellent stability with small charging/discharging voltage gaps. Importantly, when used as the air cathode for industrial chlor‐alkali process, the applied voltage of Fe‐SAs/MPC‐based flow cell to reach 300 mA cm−2 is 1.57 V, which is 210 mV smaller than Pt/C‐based one. These findings provide in‐depth insights into the confined microenvironment of MNx moieties for boosted electrochemical performance, and pave the pathways for future catalyst development satisfying the requirement of industrial applications.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"183 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143745098","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 Versatile Azetidinecarboxamide‐Based Fluorophore‐Ligand Conjugates for High‐Resolution Cell Imaging

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-04-01 DOI: 10.1002/anie.202505579

Ning Xu, Qinglong Qiao, Chao Wang, Wei Zhou, Pengjun Bao, Jin Li, Shaowei Wu, Xiaogang Liu, Zhaochao Xu

{"title":"Bright and Versatile Azetidinecarboxamide‐Based Fluorophore‐Ligand Conjugates for High‐Resolution Cell Imaging","authors":"Ning Xu, Qinglong Qiao, Chao Wang, Wei Zhou, Pengjun Bao, Jin Li, Shaowei Wu, Xiaogang Liu, Zhaochao Xu","doi":"10.1002/anie.202505579","DOIUrl":"https://doi.org/10.1002/anie.202505579","url":null,"abstract":"Fluorophore‐ligand conjugates play a pivotal role in cellular imaging, providing high target specificity. However, simultaneously achieving conjugates with high brightness and ligand‐targeting diversity presents significant challenges. Traditional strategies often require complex, multi‐step modifications for fluorophore enhancement and ligand conjugation. Here, we present an azetidinecarboxamide strategy that addresses these challenges by integrating brightness enhancement and ligand conjugation capabilities within a single molecular framework. The azetidinecarboxamide core suppresses twisted intramolecular charge transfer (TICT), thereby enhancing fluorescence quantum yield. Its carbonyl group provides a versatile site for conjugating a wide range of targeting ligands, enabling the rapid development of diverse and tunable fluorophore‐ligand conjugates. This streamlined approach reduces synthetic complexity, accelerates probe development, and is compatible with a wide variety of fluorophores, such as coumarin, naphthalimide, NBD, rhodol, rhodamine, and silicon‐rhodamine, facilitating the creation of high‐performance, multifunctional probes for advanced cellular imaging.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"88 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143745116","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

Hydrophobicity‐Controlled Self‐Assembly of Supramolecular Peptide Nanotubes in Water

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-04-01 DOI: 10.1002/anie.202423828

Min Zeng, William Parsons, Yixuan Chen, David K. Chalmers, Sebastien Perrier

{"title":"Hydrophobicity‐Controlled Self‐Assembly of Supramolecular Peptide Nanotubes in Water","authors":"Min Zeng, William Parsons, Yixuan Chen, David K. Chalmers, Sebastien Perrier","doi":"10.1002/anie.202423828","DOIUrl":"https://doi.org/10.1002/anie.202423828","url":null,"abstract":"Polymer‐conjugated peptides are attractive building blocks for the construction of new nanomaterials. However, the ability to control the self‐assembly of these materials remains a major limitation to their wider utilization. Herein, we report a facile strategy to fine‐tune the assembly of water‐soluble hydrophilic polymer‐conjugated cyclic peptides by incorporating a defined, short hydrocarbon linker between the polymer and peptide. This addition creates a well‐defined hydrophobic ‘inner shell’ that suppresses water from disrupting the organized peptide hydrogen bond network. Our approach is demonstrated using a series of cyclic peptide‐linker‐PDMA conjugates which were evaluated by asymmetric flow field flow fractionation, small angle neutron scattering and transmission electron microscopy. Molecular dynamics simulations were also used to show how the polymer and the peptide stacks interact and illustrate the impact of this hydrophobic inner shell approach. This strategy provides a modular approach to fine control the nanotube self‐assembling behavior. We expect that this technique will improve the versatility of peptide nanotubes for the engineering of advanced nanomaterials.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"47 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143745115","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

Symmetry-Breaking Strategy Yields Dopant-Free Small Molecule Hole Transport Materials for Inorganic Perovskite Solar Cells with 20.58% Efficiency and Outstanding Stability 打破对称性策略为无机包晶太阳能电池提供无掺杂剂的小分子空穴传输材料，效率达 20.58% 并具有出色的稳定性

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-04-01 DOI: 10.1002/anie.202502478

Huimin Cai, Qiliang Zhu, Tianchen Pan, Lunbi Wu, Xin Gu, Chenghao Duan, Liangbin Xiong, Jiaying Wu, Sha Liu, Liyang Yu, Ruipeng Li, Keyou Yan, Ruijie Ma, Shengjian Liu, Tao Jia, Gang Li

{"title":"Symmetry-Breaking Strategy Yields Dopant-Free Small Molecule Hole Transport Materials for Inorganic Perovskite Solar Cells with 20.58% Efficiency and Outstanding Stability","authors":"Huimin Cai, Qiliang Zhu, Tianchen Pan, Lunbi Wu, Xin Gu, Chenghao Duan, Liangbin Xiong, Jiaying Wu, Sha Liu, Liyang Yu, Ruipeng Li, Keyou Yan, Ruijie Ma, Shengjian Liu, Tao Jia, Gang Li","doi":"10.1002/anie.202502478","DOIUrl":"https://doi.org/10.1002/anie.202502478","url":null,"abstract":"Inorganic perovskites are known for their excellent photothermal stability; however, the photothermal stability of all-inorganic n-i-p perovskite solar cells (PSCs) is compromised due to ion diffusion and free radical-induced degradation caused by the use of doped Spiro-OMeTAD hole transport materials (HTMs). In this study, two isomeric D-A-D type small molecules, namely HBT and HiBT, were developed and used as dopant-free HTMs, using 2,1,3-benzothiadiazole or benzo[d][1,2,3]thiadiazole as acceptor moieties. The HiBT molecule, with its symmetry-breaking features, exhibits a large dipole moment, enhanced coordination-active sites, and a well-aligned energy level structure, all of which contribute to passivating perovskite surface defects and improving free charge separation. As a result, inorganic CsPbI3 PSCs with HiBT HTM achieved an impressive power conversion efficiency (PCE) of 20.58%, the highest reported for dopant-free HTM-based inorganic PSCs. Moreover, the enhanced hydrophobic properties of HiBT molecules, coupled with their ability to passivate perovskite surface defects, contribute to significantly improved device stability.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"16 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143745567","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

Influence of Ligand Design and Non-Covalent Interactions on the Isoselective Ring-Opening Polymerization of rac-ß-Butyrolactone using Salan and Salalen Rare-Earth Metal Catalysts

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-04-01 DOI: 10.1002/anie.202504513

Stefanie Hörl, Ion Chiorescu, Jonas Bruckmoser, Jonas Futter, Bernhard Rieger

{"title":"Influence of Ligand Design and Non-Covalent Interactions on the Isoselective Ring-Opening Polymerization of rac-ß-Butyrolactone using Salan and Salalen Rare-Earth Metal Catalysts","authors":"Stefanie Hörl, Ion Chiorescu, Jonas Bruckmoser, Jonas Futter, Bernhard Rieger","doi":"10.1002/anie.202504513","DOIUrl":"https://doi.org/10.1002/anie.202504513","url":null,"abstract":"We herein report the influence of the ligand framework on the isoselective ring-opening polymerization (ROP) of rac-β-butyrolactone using highly active in situ generated salan [ONNO]H2 and salalen [ONNO]H rare-earth metal complexes. The stereochemistry was found to be highly dependent on the ortho-substituents, enabling the synthesis of either isotactic poly(3-hydroxybutyrate) (PHB) (up to Pm = 0.92) or syndiotactic PHB (up to Pr = 0.91). To obtain further information on the mechanism of the isoselective ROP, which exhibits an enantiomorphic site control, the new hybrid Y[ONNO]H(N(SiHMe2)2)(THF) complex was isolated and characterized via NMR, DFT and mass-spectrometry experiments. The impact of non-covalent interactions (NCIs) was demonstrated by the addition of NCI inhibitors. Kinetic studies revealed a secondary kinetic isotope effect (KIE) of 1.14, indicating that the pre-coordination of the monomer plays a significant role in the mechanism. These findings provide a foundation for the future design of catalysts for isoselective ROP.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"32 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143745337","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

Solid‐State Photoconversion of a Discrete Mixed Iodine(I) System to a 1D Polymer

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-04-01 DOI: 10.1002/anie.202503763

Jas S. Ward, Aaron Mailman

引用次数: 0

Chiral Zinc Sulfide Nanoparticles Scavenging Reactive Oxygen Species for Remodeling Intestinal Homeostasis

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-04-01 DOI: 10.1002/anie.202503654

Aihua Qu, Jun Luo, Baimei Shi, Changlong Hao, Maozhong Sun, Liguang Xu, Hua Kuang

{"title":"Chiral Zinc Sulfide Nanoparticles Scavenging Reactive Oxygen Species for Remodeling Intestinal Homeostasis","authors":"Aihua Qu, Jun Luo, Baimei Shi, Changlong Hao, Maozhong Sun, Liguang Xu, Hua Kuang","doi":"10.1002/anie.202503654","DOIUrl":"https://doi.org/10.1002/anie.202503654","url":null,"abstract":"Elevated levels of reactive oxygen species (ROS) and gut microbiota dysbiosis are crucial factors that exacerbate inflammatory bowel disease (IBD). To address this, we successfully synthesized zinc sulfide nanoparticles (ZnS NPs) with a particle size of approximately 500 nm and a maximum g-factor of 0.07, utilizing l-/d-cysteine as chiral ligands. In vitro experiments revealed that these chiral ZnS NPs could enter macrophages through the CD44 and clathrin pathways, which enhanced the ability to scavenge ROS, in turn significantly inhibited the NF-κB and NLRP3 signaling pathways, thereby reducing the secretion of TNF-α, IL-6, and IL-1β, while upregulating IL-10. In vivo experimental data showed that l-ZnS NPs outperformed 5-aminosalicylic acid, significantly improving body weight, reducing the IBD activity index, and attenuating tissue damage, concurrently, l-ZnS NPs exhibited a marked prophylactic effect. The benchmark studies verified that l-ZnS NPs increased the abundance of the beneficial Lachnospiraceae NK4A136 by 10.55-fold and decreased harmful Enterobacter by 2914.00-fold, thereby reshaping the intestinal microecological balance. Pharmacokinetic and biosafety assessments confirmed the safety of l-ZnS NPs. Our findings indicate that chiral ZnS NPs hold great potential as nanodrugs for the treatment and prevention of IBD, providing an important foundation for the development of IBD therapeutic strategies.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"66 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758559","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