Angewandte Chemie最新文献_第8页

Single-Step Synthesis of a Heterometallic [Cu2PdL4]2+ Hybrid Metal–Organic Coordination Cage 异金属[Cu2PdL4]2+杂化金属-有机配位笼的一步合成

Angewandte Chemie Pub Date : 2025-04-01 DOI: 10.1002/ange.202506064

Shannon Thoonen, Samuel E. Walker, David L. Marshall, Therese M. Fulloon, Samuel Brandon, Alasdair I. McKay, Martin J. Paterson, Kathleen M. Mullen, James D. Crowley, Kellie L. Tuck, David R. Turner

{"title":"Single-Step Synthesis of a Heterometallic [Cu2PdL4]2+ Hybrid Metal–Organic Coordination Cage","authors":"Shannon Thoonen, Samuel E. Walker, David L. Marshall, Therese M. Fulloon, Samuel Brandon, Alasdair I. McKay, Martin J. Paterson, Kathleen M. Mullen, James D. Crowley, Kellie L. Tuck, David R. Turner","doi":"10.1002/ange.202506064","DOIUrl":"https://doi.org/10.1002/ange.202506064","url":null,"abstract":"Traditional methods of assembling low-symmetry heterometallic cage architectures are limited to stepwise construction and combinations of inert and labile metal ions, affording complex, anisotropic cage structures by sacrificing synthetic ease. Herein, a heterometallic [Cu2PdL4]2+ lantern-type cage has been assembled in a single self-assembly step through the use of a heteroditopic ligand with two different metal-binding groups. The resultant cage complex is a fusion of two common lantern-type cage motifs—carboxylate-based metal-organic Cu4L4 cages and pyridyl-based Pd2L4 coordination cages. Evidence for heterometallic cage formation in solution was provided by 1H and diffusion-ordered NMR spectroscopy and electrospray ionization mass spectrometry (ESIMS) data, whereas circular dichroism (CD) spectra confirmed the helical nature of the assembly. The heterometallic cage was then exploited in binding heterotopic guests. It is envisioned that the simple design strategy presented herein will ease the assembly of other structurally complex, low-symmetry cage architectures.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 23","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202506064","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144179020","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Fast and Autonomous Mannosylated Nanomotors for Dynamic Cancer Cell Targeting 用于癌细胞动态靶向的快速自主甘露糖基化纳米马达

Angewandte Chemie Pub Date : 2025-04-01 DOI: 10.1002/ange.202505717

Yuechi Liu, Roberto Terracciano, Jari Scheerstra, Gokhan Yilmaz, Hanglong Wu, Pascal Welzen, Shoupeng Cao, Tania Patino Padial, Loai Abdelmohsen, Jingxin Shao, Bingbing Sun, C. Remzi Becer, Jan C. M. van Hest

{"title":"Fast and Autonomous Mannosylated Nanomotors for Dynamic Cancer Cell Targeting","authors":"Yuechi Liu, Roberto Terracciano, Jari Scheerstra, Gokhan Yilmaz, Hanglong Wu, Pascal Welzen, Shoupeng Cao, Tania Patino Padial, Loai Abdelmohsen, Jingxin Shao, Bingbing Sun, C. Remzi Becer, Jan C. M. van Hest","doi":"10.1002/ange.202505717","DOIUrl":"https://doi.org/10.1002/ange.202505717","url":null,"abstract":"An attractive strategy in cancer cell therapy is to employ motile nanoparticles that can actively search for their target. Herein, we introduce mannosylated compartmentalized cross-linked enzyme-driven nanomotors (c-CLEnM), which exhibit specific and efficient targeting of Hep G2 cells through elevated autonomous motion. In this design, we constructed biodegradable bowl-shaped stomatocytes encapsulating the enzymes glucose oxidase (GOx) and catalase (CAT) within their nanocavity. A subsequent enzyme crosslinking reaction was performed to guarantee their stability. Furthermore, the c-CLEnM were surface modified with a mannose-functional glycopolymer, enabling binding with receptors expressed on Hep G2 cells. Interestingly, the targeting ligands on the nanomotors not only improved their specificity toward cancer cells but also enhanced motility. Compared to the non-mannosylated nanomotors, mannosylated c-CLEnM exhibited enhanced motion and higher targeting efficiency to cells in glucose-containing ionic environments. The unexpected acceleration in speed resulted from the surface modification of these nanomotors with a glycopolymer layer, which increased the zeta potential and created a shielding effect that mitigated the influence of the surrounding ions. This nanomotor design highlights the synergistic effect of functional glycopolymer modification on cellular uptake, adding an additional level of control to nanomotors for application in cancer therapy.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 23","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202505717","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144179228","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","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 离散混合碘(I)体系到一维聚合物的固态光转化

Angewandte Chemie Pub Date : 2025-04-01 DOI: 10.1002/ange.202503763

Jas S. Ward, Aaron Mailman

{"title":"Solid-State Photoconversion of a Discrete Mixed Iodine(I) System to a 1D Polymer","authors":"Jas S. Ward, Aaron Mailman","doi":"10.1002/ange.202503763","DOIUrl":"https://doi.org/10.1002/ange.202503763","url":null,"abstract":"The first example of a mixed halogen(I) complex (2), containing three distinct iodine(I) moieties ([N―I―N]+, O―I―N, and [O―I―O]−) within the same structure, was synthesized with 4-styrylpyridine (4-stypy) and 3,4,5,6-tetrafluorophthalate as the stabilizing Lewis bases. This complex was observed to be in equilibrium with its respective bis(OIN) complex (1a), with isolated samples of 2 also being found to convert to 1a in solution. Upon UV irradiation of 2, a single-crystal-to-single-crystal [2 + 2] cycloaddition reaction was observed, converting the discrete salt 2 to the 1D polymer 5. Complex 5 retained all the iodine(I) moieties from prior to photoconversion and represents the first example of nondestructive photoconversion of a halogen(I) complex. To facilitate comparisons to 2 and 5, several additional closely related iodine(I) complexes were synthesized, with the iodine(I) complexes characterized by NMR (1H, 1H-15N HMBC) and SCXRD, as well as by Raman and IR spectroscopy for 2, 5, and their close structural analogue 1a.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 23","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144178977","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","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 微孔硬碳载体激发了先进空气阴极单原子电催化剂的卓越性能

Angewandte Chemie Pub Date : 2025-04-01 DOI: 10.1002/ange.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/ange.202501307","DOIUrl":"https://doi.org/10.1002/ange.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 promote its protonation and accelerate the 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":7803,"journal":{"name":"Angewandte Chemie","volume":"137 23","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144179074","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

A Nucleus-Targeting Ruthenium(II) Complex Induces DNA Condensation in Cisplatin-Resistant Tumor Cells 一种核靶向钌（II）复合物在顺铂耐药肿瘤细胞中诱导DNA缩聚

Angewandte Chemie Pub Date : 2025-04-01 DOI: 10.1002/ange.202504970

Ying Zhou, Kai Xiong, Tao Feng, Xianbo Wu, Jinzhe Liang, Yu Chen, Hui Chao

{"title":"A Nucleus-Targeting Ruthenium(II) Complex Induces DNA Condensation in Cisplatin-Resistant Tumor Cells","authors":"Ying Zhou, Kai Xiong, Tao Feng, Xianbo Wu, Jinzhe Liang, Yu Chen, Hui Chao","doi":"10.1002/ange.202504970","DOIUrl":"https://doi.org/10.1002/ange.202504970","url":null,"abstract":"One of the conventional ways to eradicate tumor cells is to utilize chemotherapy agents, e.g., cisplatin, to induce DNA damage. However, DNA damage repair mechanisms can significantly limit the therapeutic efficacy of cisplatin. These mechanisms enable tumor cells to repair the DNA damage caused by the drug, leading to resistance. Cisplatin and similar drugs bind to specific DNA sites without significantly altering their conformation. As a result, DNA repair enzymes can still attach to and repair the damaged DNA. To address this issue, we designed four Ru(II) complexes (RuC3, RuC6, RuC9, and RuC12) with high positive charges of +8 valence and regulated their nuclear accumulation levels by adjusting the length of alkyl chains. RuC9 exhibits the highest nucleus accumulation level. DNA conformation was significantly altered by inducing DNA condensation through indiscriminately neutralizing the negative charge of the DNA backbone. This significant change prevents DNA-related enzymes from binding to DNA, ultimately leading to the efficient eradication of various tumor cell lines. To the best of our knowledge, it is the first work that kills tumor cells and overcomes cisplatin resistance through inducing DNA condensation.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 23","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144178976","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Introducing the Aziridination of Fluorinated Olefins by Metal-Catalyzed Nitrene Transfer 介绍了金属催化硝基烯转移的氟化烯烃叠氮化反应

Angewandte Chemie Pub Date : 2025-04-01 DOI: 10.1002/ange.202419188

Jorge Pérez-Ruíz, Antonio Rosales Martínez, M. Mar Díaz-Requejo, Pedro J. Pérez

引用次数: 0

Chiral Zinc Sulfide Nanoparticles Scavenging Reactive Oxygen Species for Remodeling Intestinal Homeostasis 手性硫化锌纳米颗粒清除活性氧重塑肠道内稳态

Angewandte Chemie Pub Date : 2025-04-01 DOI: 10.1002/ange.202503654

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

{"title":"Chiral Zinc Sulfide Nanoparticles Scavenging Reactive Oxygen Species for Remodeling Intestinal Homeostasis","authors":"Jun Luo, Baimei Shi, Changlong Hao, Maozhong Sun, Liguang Xu, Hua Kuang, Aihua Qu","doi":"10.1002/ange.202503654","DOIUrl":"https://doi.org/10.1002/ange.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. Chirality gives NPs unique bioactivity. 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":7803,"journal":{"name":"Angewandte Chemie","volume":"137 23","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144179195","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Nonclassical Hydrogen Bond-Based Efficient Solid-State Organic Emitters Enabled by a Synergistic Anion and Mechanical Bond Effect 基于非经典氢键的高效固体有机发射体，由协同阴离子和机械键效应实现

Angewandte Chemie Pub Date : 2025-04-01 DOI: 10.1002/ange.202505774

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

引用次数: 0

Halogen-Atom Transfer Enabled Z-Selective Styrene Synthesis via Dual Cobalt and Photocatalysis Through Coupling of Unactivated Alkyl Iodides With Terminal Arylalkynes 卤素原子转移使双钴和未活化的烷基碘化物与端芳炔偶联光催化合成z选择性苯乙烯

Angewandte Chemie Pub Date : 2025-04-01 DOI: 10.1002/ange.202501630

Anxiang Huang, Zhao Liu, Ruobin Wang, Xinran Chang, Mingxing Feng, Yuxin Xiang, Xiaotian Qi, Jun Zhu

{"title":"Halogen-Atom Transfer Enabled Z-Selective Styrene Synthesis via Dual Cobalt and Photocatalysis Through Coupling of Unactivated Alkyl Iodides With Terminal Arylalkynes","authors":"Anxiang Huang, Zhao Liu, Ruobin Wang, Xinran Chang, Mingxing Feng, Yuxin Xiang, Xiaotian Qi, Jun Zhu","doi":"10.1002/ange.202501630","DOIUrl":"https://doi.org/10.1002/ange.202501630","url":null,"abstract":"An efficient Z-selective cobalt-catalyzed reductive hydroalkylation of terminal aryl alkynes with unactivated alkyl iodides has been achieved, providing a straightforward and modular route to access 1,2-disubstituted Z-styrenes. This reaction operates under mild conditions without requiring over-stoichiometric amounts of metal terminal reductants. Excellent Z/E ratios and good to excellent yields can be achieved for diverse and complex scaffolds with remarkable functional-group compatibility. One potential utility of this reaction is demonstrated by the efficient synthesis of several syn homoallylic alcohols in a one-pot two-step sequence. Control experiments strongly support that the halogen-atom transfer (XAT) process is the key to generating carbon radicals. DFT studies suggest that the catalytic system involves the Co(II)/Co(III) cycle and the steric repulsion between the Co(II) catalyst, and the alkenyl radical in radical capture by Co(II) is the dominant factor controlling the Z/E selectivity. This approach represents the first example of merging photo-XAT with cobalt-catalyzed reductive coupling of terminal aryl alkynes with unactivated alkyl iodides.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 23","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144179226","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Probing Inside the Catalyst Layer on Gas Diffusion Electrodes in Electrochemical Reduction of CO and CO2 CO和CO2电化学还原中气体扩散电极催化剂层内部的探测

Angewandte Chemie Pub Date : 2025-04-01 DOI: 10.1002/ange.202504715

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

引用次数: 0