Angewandte Chemie International Edition最新文献_第9页

Multifunctional Interface Layer Constructed by Trace Zwitterions for Highly Reversible Zinc Anodes. 由微量齐聚物构建的多功能界面层用于高可逆锌阳极

IF 16.1 1区化学

Angewandte Chemie International Edition Pub Date : 2024-12-16 Epub Date: 2024-10-24 DOI: 10.1002/anie.202411884

Xixi Zhang, Chenggang Wang, Jinzhao Huang, Chuanlin Li, Guangmeng Qu, Na Li, Shunshun Zhao, Titi Li, Dingzheng Li, Hongjie Qin, Xijin Xu

{"title":"Multifunctional Interface Layer Constructed by Trace Zwitterions for Highly Reversible Zinc Anodes.","authors":"Xixi Zhang, Chenggang Wang, Jinzhao Huang, Chuanlin Li, Guangmeng Qu, Na Li, Shunshun Zhao, Titi Li, Dingzheng Li, Hongjie Qin, Xijin Xu","doi":"10.1002/anie.202411884","DOIUrl":"10.1002/anie.202411884","url":null,"abstract":"The inhomogeneous plating/stripping of Zn anode, attributed to dendrite growth and parasitic reactions at the electrode/electrolyte interface, severely restricts its cycling life-span. Here, trace zwitterions (trifluoroacetate pyridine, TFAPD) are introduced into the aqueous electrolyte to construct a multifunctional interface that enhances the reversibility of Zn anode. The TFA- anions with strong specific adsorption adhere onto the Zn surface to reconstruct the inner Helmholtz plane (IHP), preventing the hydrogen evolution and corrosion side reactions caused by free H2O. The Py+ cations accumulate on the outer Helmholtz plane (OHP) of Zn anode with the force of electric field during Zn2+ plating, forming a shielding layer to uniformize the deposition of Zn2+. Besides, the adsorbed TFA- and Py+ promote the desolvation process of Zn2+ resulting in fast reaction kinetics. Thus, the Zn||Zn cells present an outstanding cycling performance of more than 10000 hours. And even at 85 % utilization rate of Zn, it can stably cycle for over 200 hours at 10 mA cm-2 and 10 mAh cm-2. The Zn||I2 full cell exhibits a capacity retention of over 95 % even after 30000 cycles. Remarkably, the Zn||I2 pouch cells (95 mAh) deliver a high-capacity retention of 99 % after 750 cycles.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":" ","pages":"e202411884"},"PeriodicalIF":16.1,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142102500","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}

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Carbon- and Nitrogen-Based Complexes as Photocatalysts for Prebiotic and Oxygen Chemistry during Earth Evolution. 地球演化过程中作为前生物和氧化学光催化剂的碳基和氮基复合物。

IF 16.1 1区化学

Angewandte Chemie International Edition Pub Date : 2024-12-16 Epub Date: 2024-10-29 DOI: 10.1002/anie.202413768

Yan Wang, Huan Wang, Sibo Wang, Yuanxing Fang

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Mechanochemical Synthesis of Boroxine-linked Covalent Organic Frameworks. 硼氧键共价有机框架的机械化学合成。

IF 16.1 1区化学

Angewandte Chemie International Edition Pub Date : 2024-12-16 Epub Date: 2024-09-20 DOI: 10.1002/anie.202404539

Ehsan Hamzehpoor, Farshid Effaty, Tristan H Borchers, Robin S Stein, Alexander Wahrhaftig-Lewis, Xavier Ottenwaelder, Tomislav Friščić, Dmytro F Perepichka

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CORRIGENDUM: Correction to "Discovery of Hexagonal Structured Pd-B Nanocrystals". 更正：六角结构 Pd-B 纳米晶体的发现。

IF 16.1 1区化学

Angewandte Chemie International Edition Pub Date : 2024-12-16 Epub Date: 2024-11-07 DOI: 10.1002/anie.202419250

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}

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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

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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

NIR-II AIEgens for Infectious Diseases Phototheranostics. 用于传染病光otheranostics 的 NIR-II AIEgens。

IF 16.1 1区化学

Angewandte Chemie International Edition Pub Date : 2024-12-16 Epub Date: 2024-10-25 DOI: 10.1002/anie.202414259

Dingyuan Yan, Zheng Li, Michelle M S Lee, Ben Zhong Tang, Dong Wang

{"title":"NIR-II AIEgens for Infectious Diseases Phototheranostics.","authors":"Dingyuan Yan, Zheng Li, Michelle M S Lee, Ben Zhong Tang, Dong Wang","doi":"10.1002/anie.202414259","DOIUrl":"10.1002/anie.202414259","url":null,"abstract":"Pathogenic infectious diseases have persistently posed significant threats to public health. Phototheranostics, which combines the functions of diagnostic imaging and therapy, presents an extremely promising solution to block the spread of pathogens as well as the outbreak of epidemics owing to its merits of a wide-spectrum of activity, high controllability, non-invasiveness, and difficult to acquire resistance. Among multifarious phototheranostic agents, second near-infrared (NIR-II, 1000-1700 nm) aggregation-induced emission luminogens (AIEgens) are notable by virtue of their deep penetration depth, excellent biocompatibility, balanced radiative and nonradiative decay and aggregation-enhanced theranostic performance, making them an ideal option for combating pathogens. This minireview provides a systematical summary of the latest advancements in NIR-II AIEgens with emphasis on the molecular design and nanoplatform formulation to fulfill high-efficiency in treating bacterial and viral pathogens, classified by disease models. Then, the current challenges, potential opportunities, and future research directions are presented to facilitate the further progress of this emerging field.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":" ","pages":"e202414259"},"PeriodicalIF":16.1,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142054280","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

Optimizing s‐p Orbital Overlap between Sodium Polysulfides and Single‐Atom Indium Catalyst for Efficient Sulfur Redox Reaction 优化多硫化钠与单原子铟催化剂之间的 s-p 轨道重叠，实现高效的硫氧化还原反应

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2024-12-16 DOI: 10.1002/anie.202422208

Guangxuan Wu, Tongfeng Liu, Zhoujie Lao, Yihao Cheng, Tianshuai Wang, Jing Mao, Haichang Zhang, Enzuo Liu, Chunsheng Shi, Guangmin Zhou, Chunnian He, Wenbin Hu, Naiqin Zhao, Ningning Wu, Biao Chen

{"title":"Optimizing s‐p Orbital Overlap between Sodium Polysulfides and Single‐Atom Indium Catalyst for Efficient Sulfur Redox Reaction","authors":"Guangxuan Wu, Tongfeng Liu, Zhoujie Lao, Yihao Cheng, Tianshuai Wang, Jing Mao, Haichang Zhang, Enzuo Liu, Chunsheng Shi, Guangmin Zhou, Chunnian He, Wenbin Hu, Naiqin Zhao, Ningning Wu, Biao Chen","doi":"10.1002/anie.202422208","DOIUrl":"https://doi.org/10.1002/anie.202422208","url":null,"abstract":"P‐block metal carbon‐supported single‐atom catalysts (C‐SACs) have emerged as a promising candidate for high‐performance room‐temperature sodium‐sulfur (RT Na‐S) batteries, due to their high atom utilization and unique electronic structure. However, the ambiguous electronic‐level understanding of Na‐dominant s‐p hybridization between sodium polysulfides (NaPSs) and p‐block C‐SACs limits the precise control of coordination environment tuning and electro‐catalytic activity manipulation. Here, s‐p orbital overlap degree (OOD) between the s orbitals of Na in NaPSs and the p orbitals of p‐block C‐SACs is proposed as a descriptor for sulfur reduction reaction (SRR) and sulfur oxidation reaction (SOR). Compared to NG and NG‐supported InN4 (NG‐InN4) SACs, the nitrogen‐doped graphene‐supported InN5 (NG‐InN5) SACs show the largest s‐p OOD, demonstrating the weakest shuttle effect and the lowest reaction energy barriers in both SRR and SOR. Accordingly, the designed catalysts allow the Na‐S pouch batteries to retain a high capacity of 490.7 mAh g‐1 at 2 A g‐1 with a Coulombic efficiency of 96% at a low electrolyte/sulfur (E/S) ratio of 4.5 μl. This work offers an s‐p orbital overlap descriptor describing the interaction between NaPSs and p‐orbital‐dominated catalysts for high‐performance RT Na‐S batteries.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"23 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142825235","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