Angewandte Chemie International Edition最新文献_第4页

Programmable Self-assembly from Two-dimensional Nanosheets to Spiral, Twisted and Branched Nanostructures

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2024-12-17 DOI: 10.1002/anie.202416624

Haohui Hu, Wei Jiang, Xiao Han, Geng Wu, Haoran Wang, Yi Shi, Dayin He, Xianhui Ma, Xun Hong

{"title":"Programmable Self-assembly from Two-dimensional Nanosheets to Spiral, Twisted and Branched Nanostructures","authors":"Haohui Hu, Wei Jiang, Xiao Han, Geng Wu, Haoran Wang, Yi Shi, Dayin He, Xianhui Ma, Xun Hong","doi":"10.1002/anie.202416624","DOIUrl":"https://doi.org/10.1002/anie.202416624","url":null,"abstract":"Self-assembly of nanomaterials into hierarchical structure is of great interest to fabricate functional materials. However, programmable design of the assembled structures remains a great challenge. Herein, we reported a programmable self-assembly strategy to customize the assembled structure. The self-assembly strategy is designed to orderly transform the two-dimensional (2D) Ca ions assembled F127 nanosheets (Ca-F127 NSs) into spiral nanosheet structures (S-Ca-F127 NSs), branched nanosheet structures (B-Ca-F127 NSs), branched-spiral nanosheet structures (B-S-Ca-F127 NSs), and twisted-branched structures (T-Ca-F127 NBs). Wide-angle X-ray scattering (WAXS) and X-ray absorption spectroscopy (XAS) indicate that these different structures maintain the same orthorhombic phase and Ca-O octahedral coordination structure. Selected area electron diffraction (SAED) in the double-tilt liquid nitrogen cooling holder identifies the Eshelby twist in the twisted structures, demonstrating the spiral structure are formed by screw dislocation growth. Cryo-electron microscopy (cryo-EM) proves the oriented epitaxial growth in the B-Ca-F127 NSs. Furthermore, the formation mechanisms of spiral structure and branched structure can be recombined to form complex hierarchical structures. The epitaxial growth along screw dislocation can lead to the formation of B-S-Ca-F127 NSs, while the twisted epitaxial growth in the screw dislocation can lead to the formation of T-Ca F127 NBs.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"122 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142832723","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 Trithia-Bridged N-Heterotriangulene: The Hitherto Missing Electron Donor

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2024-12-16 DOI: 10.1002/anie.202423802

Jan Borstelmann, Viktoria Gensch, Dominik Fehn, Matthias E. Miehlich, Frank Hampel, Frank Rominger, Karsten Meyer, Milan Kivala

引用次数: 0

A Highly Biocompatible Polyoxotungstate with Fenton‐like Reaction Activity for Potent Chemodynamic Therapy of Tumors

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2024-12-16 DOI: 10.1002/anie.202422949

Hui-Ping Xiao, Man-Yi Du, Xian-Bin Sun, Ruo-Fei Xu, Dong-Miao Li, Sheng-Nan Yue, Ping-Wei Cai, Rong-Zhi Sun, Zi-Zhong Zhang, Xing Huang, Xin-Xiong Li, Yu Gao, Shou-Tian Zheng

{"title":"A Highly Biocompatible Polyoxotungstate with Fenton‐like Reaction Activity for Potent Chemodynamic Therapy of Tumors","authors":"Hui-Ping Xiao, Man-Yi Du, Xian-Bin Sun, Ruo-Fei Xu, Dong-Miao Li, Sheng-Nan Yue, Ping-Wei Cai, Rong-Zhi Sun, Zi-Zhong Zhang, Xing Huang, Xin-Xiong Li, Yu Gao, Shou-Tian Zheng","doi":"10.1002/anie.202422949","DOIUrl":"https://doi.org/10.1002/anie.202422949","url":null,"abstract":"Integrating Fenton chemistry and nanomedicine into cancer therapy has significantly promoted the development of chemodynamic therapy (CDT). Nanoscale polyoxometalates (POMs), with their reversible redox properties, exhibit promising potential in developing outstanding CDT drugs by exploring their Fenton‐like catalytic reactivity in tumor environments. However, such research is still in its infancy. In this work, we report the synthesis of a new crystalline antimonotungstate {Dy2Sb2W7O23(OH)(DMF)2(SbW9O33)2} (1, DMF = N, N‐dimethylformamide) with gram‐scale high yield via a facile \"one‐pot\" solvothermal reaction. 1 exhibits not only a soluble and water‐stable POM nanocluster, but also excellent catalytic activity for hydroxyl radical‐generating Fenton‐like reactions. Further biomedical studies reveal that 1 can trigger cell apoptosis and promote lipid peroxidation, exhibiting high cytotoxicity and selectivity towards B16‐F10 mouse melanoma cancer cells with an IC50 value of 4.75 μM. Especially, 1 can inhibit melanoma growth in vivo with favorable biosafety, achieving a 5.2‐fold reduction in tumor volume and a weight loss of 76.0% at the dose of 70 μg/kg. This research not only demonstrates the immense potential of antimonotungstates in CDT drug development for the first time but also provides new insights and directions for the development of novel anticancer drugs.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"26 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142825041","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

Lattice Modulation on Singlet‐Triplet Splitting of Silver Cluster Boosting Near‐Unity Photoluminescence Quantum Yield

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2024-12-16 DOI: 10.1002/anie.202421656

Wei-Dong Tian, Chengkai Zhang, Sayan Paul, Wei-Dan Si, Zhi Wang, Pan-Pan Sun, Anakuthil Anoop, Chen-Ho Tung, Di Sun

{"title":"Lattice Modulation on Singlet‐Triplet Splitting of Silver Cluster Boosting Near‐Unity Photoluminescence Quantum Yield","authors":"Wei-Dong Tian, Chengkai Zhang, Sayan Paul, Wei-Dan Si, Zhi Wang, Pan-Pan Sun, Anakuthil Anoop, Chen-Ho Tung, Di Sun","doi":"10.1002/anie.202421656","DOIUrl":"https://doi.org/10.1002/anie.202421656","url":null,"abstract":"Developing thermally activated delayed fluorescence (TADF)‐active silver clusters with near‐unity quantum efficiency is of practical importance in cutting‐edge optoelectronic devices, but remains a tremendous challenge due to the difficulty of de novo synthesis and uncertainty of properties. Herein, we demonstrate a lattice modulation on parent TADF‐activate silver cluster, acheving TADF‐driven photoluminescence quantum yield (PLQY) from 12% to near‐unity. Systematic experimental and calculated results reveal that the lattice modulation effectively lower the singlet‐triplet splitting (ΔEST) from 718 to 549 cm‐1, thereby facilitating thermally activated reverse intersystem crossing: T5→S5, leading to extremely efficient TADF by surpassing both phosphorescence and non‐radiative decay, thus boosting the near‐unity PLQY. Such high PLQY are extremely rare in the TADF‐active silver clusters and even in the whole noble‐metal clusters. This research showcases an unparalleled example of lattice modulation to realize near unity PLQY of TADF‐active silver clusters.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"10 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142825242","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

Toward Rhenium‐based Circularly Polarized OLEDs Using Tailored Chiral Re(CO)3 Emitters

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2024-12-16 DOI: 10.1002/anie.202419788

Maria P. Davydova, Ting Xu, Alexander M. Agafontsev, Lingqiang Meng, Mariusz Wolff, Maxim Yu. Petyuk, Irina Yu. Bagryanskaya, Alexey S. Berezin, Alexey V. Tkachev, Hong Meng, Alexander V. Artem'ev

{"title":"Toward Rhenium‐based Circularly Polarized OLEDs Using Tailored Chiral Re(CO)3 Emitters","authors":"Maria P. Davydova, Ting Xu, Alexander M. Agafontsev, Lingqiang Meng, Mariusz Wolff, Maxim Yu. Petyuk, Irina Yu. Bagryanskaya, Alexey S. Berezin, Alexey V. Tkachev, Hong Meng, Alexander V. Artem'ev","doi":"10.1002/anie.202419788","DOIUrl":"https://doi.org/10.1002/anie.202419788","url":null,"abstract":"Chiral rhenium(I) emitters showing circularly polarized phosphorescence (CPP) are an attractive mainstay for CP organic light‐emitting diodes (CP‐OLEDs). However, the efficiency of such emitters is not ideal, and they have never been explored for circularly polarized electroluminescence (CPEL) applications. Here, we have tailored robust chiral Re(I) complexes with improved CPP properties, and firstly demonstrated CPEL from rhenium emitters. The designed chiral Re(I) complexes exhibit a yellow CPP with enhanced |glum| factors (up to 2.5×10–2) and a good quantum efficiency. The pioneering Re(I)‐based CP‐OLEDs (based on the obtained emitters) exhibit yellow CPEL with |gEL| factors of up to 6.2×10–3 and maximal external quantum efficiency of 13.2%. Furthermore, we have demonstrated for the first time a suppressive effect of a magnetic field on the CPP strength of Re(I) emitters. This work highlights the good potential of chiral Re(I) emitters for CPEL applications, and opens up a new shortcut to CPP‐active Re(I) complexes.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"22 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142825231","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

Mass Transfer‐Enhanced Photothermal Membranes with Synergistic Light Utilization for High‐Turbidity Wastewater Purification

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2024-12-16 DOI: 10.1002/anie.202421800

Jiangchen Fu, Shaoze Xiao, Jiazhen Cao, Zhiyan Liang, Jiabin Chen, Yue Jiang, Mingyang Xing

{"title":"Mass Transfer‐Enhanced Photothermal Membranes with Synergistic Light Utilization for High‐Turbidity Wastewater Purification","authors":"Jiangchen Fu, Shaoze Xiao, Jiazhen Cao, Zhiyan Liang, Jiabin Chen, Yue Jiang, Mingyang Xing","doi":"10.1002/anie.202421800","DOIUrl":"https://doi.org/10.1002/anie.202421800","url":null,"abstract":"The photo‐Fenton process faces significant limitations in treating high‐turbidity, colored wastewater due to light attenuation and impurity interference (blocked mass transfer). To address these issues, we developed a suspended photothermal Fenton membrane by loading a photothermal catalyst on a hydrophobically modified cotton filter paper, enabling precise suspension 1 mm below the water surface. This design achieved 89.49 % light utilization and high chemical oxygen demand (COD) removal, even in wastewater with extreme chromaticity (10 multiples) and turbidity (703 NTU). The enhanced photothermal conversion accelerated molybdenum co‐catalyzed Fenton reactions and improved peroxymonosulfate (PMS) activation, maintaining over 90 % phenol removal for 15 days. Mechanistic simulations revealed improved mass transfer of reactive oxygen species (ROS) and pollutants at the solid‐liquid interface, with PMS diffusion identified as the rate‐limiting step. The membrane resisted fouling from suspended solids and maintained stable operation in soil‐containing solutions for 10 days. This innovative approach offers an efficient solution for degrading pollutants in dark‐colored, high‐turbidity wastewater, overcoming traditional process limitations.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"37 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142825039","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

Atomically Dispersed Fe2 and Ni Sites for Efficient and Durable Oxygen Electrocatalysis 原子分散的 Fe2 和 Ni 基底实现高效持久的氧电催化

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2024-12-16 DOI: 10.1002/anie.202421168

Tewodros (Teddy) Asefa, Guiyuan Yang, Meihong Fan, Qing Liang, Xingquan He, Wei Zhang

{"title":"Atomically Dispersed Fe2 and Ni Sites for Efficient and Durable Oxygen Electrocatalysis","authors":"Tewodros (Teddy) Asefa, Guiyuan Yang, Meihong Fan, Qing Liang, Xingquan He, Wei Zhang","doi":"10.1002/anie.202421168","DOIUrl":"https://doi.org/10.1002/anie.202421168","url":null,"abstract":"Developing highly efficient, cost‐effective, and robust electrocatalysts for the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER) is paramount for the large‐scale commercialization of renewable fuel cells and rechargeable metal‐air batteries. Herein, a new ternary‐atom catalyst that is composed of paired Fe sites and single Ni sites (as Fe2‐N6 and Ni‐N4) coordinated onto hollow nitrogen‐doped carbon microspheres is developed. The as‐synthesized catalyst exhibits remarkable activities toward both the ORR and OER in an alkaline media, with superior performances to those of the control materials that contain only Fe2‐N6 or Ni‐N4 sites. Density functional theory calculations and in situ infrared (IR) spectroscopic studies clearly reveal that the Fe2‐N6 centers are the active sites for both ORR and OER, and their electrocatalytic activities are synergistically enhanced through optimization of their d‐band centers by the Ni‐N4 sites. This ternary‐atom catalyst may be a promising, alternative, sustainable catalyst to commercially used Pt‐ and Ru‐based catalysts to drive both ORR and OER in rechargeable zinc‐air batteries and other related applications.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"250 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142825239","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

Ligand-Protected Golden Fullerene Au42 with Unprecedented Metal Coordination Number of 15 配体保护的金色富勒烯 Au42 具有前所未有的 15 个金属配位数

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2024-12-16 DOI: 10.1002/anie.202417904

Heng-Wang Luyang, Cong-Qiao Xu, Shang-Fu Yuan, Jun Li, Quan-Ming Wang

引用次数: 0

A Catch-Release Strategy for the Genomics-Driven Discovery of Antiproliferative Furan-Functionalized Peptides 基因组学驱动的抗增殖呋喃功能化多肽发现的捕获-释放策略

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2024-12-16 DOI: 10.1002/anie.202421760

Friedrich J. Ehinger, Kirstin Scherlach, Felix Trottmann, Jonas Fiedler, Christian Hertweck

{"title":"A Catch-Release Strategy for the Genomics-Driven Discovery of Antiproliferative Furan-Functionalized Peptides","authors":"Friedrich J. Ehinger, Kirstin Scherlach, Felix Trottmann, Jonas Fiedler, Christian Hertweck","doi":"10.1002/anie.202421760","DOIUrl":"https://doi.org/10.1002/anie.202421760","url":null,"abstract":"Abstract: Furan-functionalized peptides are of significant pharmacological interest due to their pronounced bioactivities and unique potential for orthogonal bioconjugation and derivatization. However, naturally occurring peptides with furyl side chains are exceedingly rare. This study presents a streamlined method to predict and assess the microbial production of peptides incorporating 3-furylalanine (Fua) moieties. The approach integrates genome mining and the reversible, chemoselective tagging of furyl residues, utilizing their unique Diels-Alder reactivity, for mass spectrometry-guided identification of candidate compounds. By employing the rhizonin Fua synthase as a bioinformatic handle and through heterologous reconstitution of Fua biosynthesis, we identified previously unknown Fua biosynthetic pathways in diverse bacterial phyla, including actinomycetes, cyanobacteria, actinobacteria, and g-proteobacteria, suggesting that Fua-containing peptides are remarkably widely distributed. Metabolic profiling by reversible tagging facilitated the detection of native Fua-containing metabolites. The successful adaptation of this method for solid support enabled the direct enrichment of furyl-substituted peptides from complex mixtures. This multi-pronged approach enabled the discovery and characterization of two novel families of Fua cyclopeptides (rubriamides and typhamides) with potent antiproliferative effects against human tumor cells and nematodes. The innovative catch-and-release strategy, in conjunction with genome mining, represents a valuable tool for the discovery of new furan-substituted natural products.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"253 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142825655","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

Enhanced Antitumor Immunity of a Globo H‐Based Vaccine Enabled by the Combination Adjuvants of 3D‐MPL and QS‐21

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2024-12-16 DOI: 10.1002/anie.202418948

Wenjing Ma, Zhuojia Xu, Changcai Teng, Chang Cao, Ruixue Wu, Xiao Meng, Qiang Sui, Qi Gao, Chengli Zong, Tiehai Li

{"title":"Enhanced Antitumor Immunity of a Globo H‐Based Vaccine Enabled by the Combination Adjuvants of 3D‐MPL and QS‐21","authors":"Wenjing Ma, Zhuojia Xu, Changcai Teng, Chang Cao, Ruixue Wu, Xiao Meng, Qiang Sui, Qi Gao, Chengli Zong, Tiehai Li","doi":"10.1002/anie.202418948","DOIUrl":"https://doi.org/10.1002/anie.202418948","url":null,"abstract":"Globo H, a specific carbohydrate antigen overexpressed on various human malignancies, has attracted considerable interest as an antigenic target for anticancer vaccine development. Despite several Globo H‐based carbohydrate vaccines that have been designed, efficient access to Globo H hexasaccharide antigen and development of powerful adjuvants for enhancing antitumor immunity remain challenging. Herein, we reported a streamlined chemoenzymatic approach to prepare this hexasaccharide antigen, relying on chemical synthesis of Gb5 pentasaccharide by a stereoconvergent [2+3] strategy and subsequent enzymatic α‐fucosylation to easily install α1,2‐fucose residue. Separately, a modular assembly approach to efficiently synthesize 3‐O‐deacyl‐monophosphoryl lipid A (3D‐MPL) was developed by the integration of stereocontrolled glycosylation, regioselective acylation, site‐specific phosphorylation, and facile global deprotection. After efficient construction of Globo H‐CRM197 conjugate, we conducted systematic immunological evaluations of Globo H‐CRM197 formulated with various adjuvants and adjuvant combinations, comprising saponin QS‐21, synthetic 3D‐MPL and α‐galactosylceramide derivative S34. The results revealed that Globo H‐CRM197 conjugate adjuvanted with QS‐21 and 3D‐MPL elicited robust IgG2a and IgG3 antibody responses and Th1 cellular immunity in mice. Moreover, antibodies induced by this formulation effectively bound to Globo H‐positive MCF‐7 cancer cells and exhibited superior complement‐dependent cytotoxicity and antibody‐dependent cellular phagocytosis, holding promise for further development of effective anticancer vaccines.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"8 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142825236","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