Angewandte Chemie International Edition最新文献

Synergistic Conversion of Hydrogen Peroxide and Benzaldehyde in Air by Silver Single‐Atom Modified Thiophene‐Functionalized g‐C3N4

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-04-12 DOI: 10.1002/anie.202505532

Xiaoyu Zhou, Kuanhong Cao, Shouqiang Huang, Haonan Wu, Zhen Cao, Hang Liu, Peng Chen, Dawei Su, Guoxiu Wang, Tianyi Wang, Chengyin Wang, Huan Pang

{"title":"Synergistic Conversion of Hydrogen Peroxide and Benzaldehyde in Air by Silver Single‐Atom Modified Thiophene‐Functionalized g‐C3N4","authors":"Xiaoyu Zhou, Kuanhong Cao, Shouqiang Huang, Haonan Wu, Zhen Cao, Hang Liu, Peng Chen, Dawei Su, Guoxiu Wang, Tianyi Wang, Chengyin Wang, Huan Pang","doi":"10.1002/anie.202505532","DOIUrl":"https://doi.org/10.1002/anie.202505532","url":null,"abstract":"This study reports the synthesis of silver single‐atom‐loaded thiophene‐conjugated carbon nitride ( Ag@T‐C3N4), a material with high carrier concentration and efficient carrier separation. Under visible light, Ag@T‐C3N4 catalyzes hydrogen peroxide (H2O2) production and benzyl alcohol oxidation to benzaldehyde, achieving production rates of 4729.82 µmol·g‐1·h‐1 for H2O2 and 19.71 mmol·g‐1·h‐1 for benzaldehyde. The synergy between thiophene conjugation and silver atoms extends visible light absorption and accelerates the 2‐electron oxygen reduction reaction (ORR), enhancing H2O2 yield. Photogenerated holes oxidize benzyl alcohol to benzaldehyde, while the biphasic benzaldehyde‐water system enables spontaneous product separation. In situ Raman spectroscopy, rotating disk electrode testing, EPR, GC‐MS, and DFT calculations highlight the critical role of thiophene‐silver synergy in optimizing reaction pathways, enhancing catalyst‐intermediate interactions, and reducing Gibbs free energy, improving H2O2 and benzaldehyde synthesis. This study provides new insights for designing carbon nitride‐based photocatalysts and offers a strategy for co‐producing value‐added chemicals.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"37 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-04-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143823005","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

Isolated and Paired Metal Sites in Zeolites using Solid-State Ion Exchange

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-04-12 DOI: 10.1002/anie.202505186

Rio Moore, James Crawford

引用次数: 0

Integrating Ambient Ionization Mass Spectrometry Imaging and Spatial Transcriptomics on the Same Cancer Tissues to Identify Gene‐Metabolite Correlations

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-04-12 DOI: 10.1002/anie.202502028

Trevor M. Godfrey, Yasmin Shanneik, Wanqiu Zhang, Thao Tran, Nico Verbeeck, Nathan H. Patterson, Faith E. Jackobs, Chandandeep Nagi, Maheshwari Ramineni, Livia Schiavinato Eberlin

{"title":"Integrating Ambient Ionization Mass Spectrometry Imaging and Spatial Transcriptomics on the Same Cancer Tissues to Identify Gene‐Metabolite Correlations","authors":"Trevor M. Godfrey, Yasmin Shanneik, Wanqiu Zhang, Thao Tran, Nico Verbeeck, Nathan H. Patterson, Faith E. Jackobs, Chandandeep Nagi, Maheshwari Ramineni, Livia Schiavinato Eberlin","doi":"10.1002/anie.202502028","DOIUrl":"https://doi.org/10.1002/anie.202502028","url":null,"abstract":"Innovations in spatial omics technologies applied to human tissues have led to breakthrough discoveries in various diseases, including cancer. Two of these approaches ‐ spatial transcriptomics and spatial metabolomics ‐ have blossomed independently, fueled by technologies such as spatial transcriptomics (ST) and mass spectrometry imaging (MSI). While powerful, these technologies only offer insights into the spatial distributions of restricted classes of molecules and have not yet been integrated to provide more holistic insights into biological questions. These techniques can be performed on adjacent serial sections from the same sample, but section‐to‐section variability can convolute data integration. We present a novel method combining desorption electrospray ionization mass spectrometry imaging (DESI‐MSI) spatial metabolomics and Visium spatial transcriptomics on the same tissue sections. We show that RNA quality is maintained after performing DESI‐MSI on a tissue and that ST data is unperturbed following DESI‐MSI. We demonstrate this workflow on human breast and lung cancer tissues and identify novel correlations between metabolites and RNA transcripts in cancer specific regions.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"61 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-04-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143823006","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

Tumor Microenvironment-Responsive Polymer Delivery Platforms for Cancer Therapy

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-04-11 DOI: 10.1002/anie.202503776

Wei-Hong Zhu, Yiqi Shi, Qianqian Yu, Lijie Tan, Qi Wang

{"title":"Tumor Microenvironment-Responsive Polymer Delivery Platforms for Cancer Therapy","authors":"Wei-Hong Zhu, Yiqi Shi, Qianqian Yu, Lijie Tan, Qi Wang","doi":"10.1002/anie.202503776","DOIUrl":"https://doi.org/10.1002/anie.202503776","url":null,"abstract":"Most chemotherapeutic and bioimaging agents struggle with inadequate bioavailability, primarily due to their limited biocompatibility and lack of specificity in targeting, leading to low or decreased anticancer efficacy and inaccurate imaging. To surmount these obstacles, the development of stimuli-responsive polymer delivery platforms, predominantly leveraging the tumor microenvironment (TME), has emerged as a promising strategy. Therapeutic and diagnostic agents can be released controllably at the tumor site by virtue of the bond cleavage or hydrophobic to hydrophilic transformation of TME-sensitive linkages in TME-responsive systems, thus augmenting cancer treatment and imaging precision, while simultaneously attenuating the damage to healthy tissues and false imaging signals caused by non-specific drug leakage. In this comprehensive review, we scrutinize recent studies of TME-responsive polymer delivery platforms, encompassing pH-, ROS-, GSH-, enzyme-, and hypoxia-responsive vectors, significantly from the perspective of their molecular design and responsive mechanism, and further summarizing their bio-application in drug delivery and diagnostic imaging. Moreover, this review encapsulates the critical challenges and offers an insightful perspective on the future prospects of TME-responsive polymer delivery platforms in terms of molecular and vector design.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"183 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143819919","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

Catalytic Asymmetric Synthesis of Chiral Caged Hydrocarbons as Arenes Bioisosteres

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-04-11 DOI: 10.1002/anie.202505803

Xue-Chun Yang, Ji-Jie Wang, Yuanjiu Xiao, Jian-Jun Feng

{"title":"Catalytic Asymmetric Synthesis of Chiral Caged Hydrocarbons as Arenes Bioisosteres","authors":"Xue-Chun Yang, Ji-Jie Wang, Yuanjiu Xiao, Jian-Jun Feng","doi":"10.1002/anie.202505803","DOIUrl":"https://doi.org/10.1002/anie.202505803","url":null,"abstract":"The utilization of caged hydrocarbons as bioisosteres for arenes, especially the phenyl ring, in bioactive compounds has resulted in significant enhancements in potency, solubility, and metabolic stability. These improvements highlight the potential of C(sp3)-rich polycyclic scaffolds as a promising motif for the development of drug candidates. However, this strategy has also increased the structural complexity of these molecules, posing synthetic challenges in controlling the chirality of caged and highly decorated bioactive scaffolds. Over the past two years, remarkable progress has been achieved in catalytic asymmetric methodologies for the synthesis of caged hydrocarbons, significantly advancing their utility in chiral drug discovery and development. This Minireview provides a comprehensive summary of recent breakthroughs in the catalytic asymmetric synthesis of chiral caged hydrocarbons, encompassing bicyclo[n.1.1]alkanes, cubanes, and related three-dimensional scaffolds. Additionally, we highlight the intriguing applications of enantiomerically pure caged hydrocarbons in biological studies. It is anticipated that this Minireview will inspire further advancements in the enantioselective synthesis of these pharmaceutically valuable caged hydrocarbons.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"25 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143819914","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

Visible-Light-Driven Photocatalytic Methanol Activation on Hexagonal CdS for Triggering C–H Methylation

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-04-11 DOI: 10.1002/anie.202507093

Gang Chen, Lei Li, Yi Liu, Zhihao Li, Yanyun Hu, Hui Wang, Xiaodong Zhang, Yi Xie

{"title":"Visible-Light-Driven Photocatalytic Methanol Activation on Hexagonal CdS for Triggering C–H Methylation","authors":"Gang Chen, Lei Li, Yi Liu, Zhihao Li, Yanyun Hu, Hui Wang, Xiaodong Zhang, Yi Xie","doi":"10.1002/anie.202507093","DOIUrl":"https://doi.org/10.1002/anie.202507093","url":null,"abstract":"Light-driven methanol activation paves the way for pursuing C–H methylation of N-heteroarenes, where selectively converting methanol into the corresponding hydroxymethyl radical (•CH2OH) is an essential prerequisite. Inspired by the versatile methanol activation on photoexcited solids, we here report a practicable semiconductor-based photocatalytic system for C–H methylation of N-heteroarenes. To be specific, hexagonal cadmium sulfide (h-CdS) was identified to be an ideal platform for visible-light-driven photocatalytic methanol activation, where selective •CH2OH generation undergoing a hole-transfer process without any additional co-catalysts or co-solvent could trigger C–H hydroxymethylation of N-heteroarenes. The following electron transfer between photoexcited h-CdS and hydroxymethylated intermediates could finally lead to the formation of methylated N-heteroarenes. The transformations facilitate the cascade utilization of photoinduced hole and electron, thereby endowing h-CdS with extraordinary photocatalytic performance. Besides, selective generation of hydroxymethylated/methylated product could be facilely implemented in the presence/absence of electron scavengers.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"14 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143819921","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

Plasmonic-Hydrogel Hybrid Biomaterials via In Situ Seeded Growth

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-04-11 DOI: 10.1002/anie.202501854

Gail Vinnacombe-Willson, Manuel Núñez-Martínez, Ada Herrero-Ruiz, Francisco Bevilacqua, Raquel Pazos, Lara Troncoso-Afonso, Marta Gallego-González, Leonardo Scarabelli, Luis M Liz-Marzán

{"title":"Plasmonic-Hydrogel Hybrid Biomaterials via In Situ Seeded Growth","authors":"Gail Vinnacombe-Willson, Manuel Núñez-Martínez, Ada Herrero-Ruiz, Francisco Bevilacqua, Raquel Pazos, Lara Troncoso-Afonso, Marta Gallego-González, Leonardo Scarabelli, Luis M Liz-Marzán","doi":"10.1002/anie.202501854","DOIUrl":"https://doi.org/10.1002/anie.202501854","url":null,"abstract":"The combination of hydrogels and functional plasmonic metal nanoparticles affords the development of unique hybrid systems, such as actuators, biosensors, and drug delivery systems, among others. Being typically prepared in colloidal suspension, incorporating shape-controlled plasmonic nanoparticles on polymer substrates typically requires lengthy processes involving synthesis, washing, and self-assembly. We report an alternative, robust in situ seed-mediated growth method, whereby either isotropic or anisotropic Au and Ag nanoparticles can be prepared directly on gelatin-based hydrogels, taking advantage of the polymer’s native chemical functionalities. In-depth characterization of gold precursor - polymer interactions enabled the rational growth of branched gold nanoparticles on biocompatible hydrogels with different physicochemical properties. In situ seeded growth circumvents traditional limitations imposed by the need of colloidal stability, thereby enabling gold nanoparticle synthesis under surfactant-free conditions and in high ionic strength solutions, thus enhancing their suitability for applications with live cells. This method can be expanded to create libraries of hybrid plasmonic materials with potential impact in the fabrication of functional 3D cell culture substrates, as well as biological and chemical sensors.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"695 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143819913","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

Deciphering Complex Electrochemical Reaction Dynamics and Interactions of Single Nano-Entities via Evanescent Scattering Microscopy

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-04-11 DOI: 10.1002/anie.202506226

Jiaying Li, Peng Lin, Liwei Wu, Yuxi Yue, Guangzhong Ma

{"title":"Deciphering Complex Electrochemical Reaction Dynamics and Interactions of Single Nano-Entities via Evanescent Scattering Microscopy","authors":"Jiaying Li, Peng Lin, Liwei Wu, Yuxi Yue, Guangzhong Ma","doi":"10.1002/anie.202506226","DOIUrl":"https://doi.org/10.1002/anie.202506226","url":null,"abstract":"Electrochemical reactions at the nanoscale are governed by intricate surface interactions, yet existing imaging techniques often lack the surface sensitivity and throughput needed to resolve these dynamics clearly. Here, we introduce electrochemical evanescent scattering microscopy (EC-ESM), a high-throughput, surface-sensitive imaging technique that enables real-time tracking of single-nanoentity electrochemistry with high resolution. Using EC-ESM, we monitored the motion and dissolution dynamics of silver nanoparticles and identified a clear relationship between nanoparticle velocity and electron transfer rates. The high throughput of EC-ESM not only ensures statistical reliability but also allows the detection of rare electron transfer events in molecularly modified AgNPs. Additionally, EC-ESM’s high resolution enabled direct imaging of both single and interacting silver nanowires, revealing diverse dissolution behaviors that provide insights into structural and surface properties. We envision EC-ESM as a powerful platform for advancing nanoscale electrochemical research and interfacial charge transfer studies.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"29 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143823096","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

Catch, Cut, or Block? – Versatile 4‐N‐Derivatized Sialyl Glycosides for Influenza Virus Neuraminidase Detection and Purification

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-04-11 DOI: 10.1002/anie.202505903

Yue Yuan, Hai Yu, Anand Kumar Agrahari, Jin Gao, Hyeog Kang, Robert Daniels, Xi Chen

{"title":"Catch, Cut, or Block? – Versatile 4‐N‐Derivatized Sialyl Glycosides for Influenza Virus Neuraminidase Detection and Purification","authors":"Yue Yuan, Hai Yu, Anand Kumar Agrahari, Jin Gao, Hyeog Kang, Robert Daniels, Xi Chen","doi":"10.1002/anie.202505903","DOIUrl":"https://doi.org/10.1002/anie.202505903","url":null,"abstract":"Seasonal influenza continues to threaten human lives and pose a significant burden to healthcare systems and the economy, emphasizing the need for developing better influenza vaccines, diagnostics, and anti‐viral therapeutics. To address these challenges, we generated a library of structurally diverse sialyl glycosides containing 4‐N‐derivatized sialic acids by a highly efficient one‐pot two‐enzyme chemoenzymatic sialylation strategy. Sialosides containing 4‐azido‐substituted sialic acid were selectively cleaved by sialidases from influenza viruses, whereas sialosides containing 4‐acetamido‐modified sialic acid were resistant to sialidase cleavage. Interestingly, sialosides containing 4‐amino‐ or 4‐guanidino‐substituted sialic acid were effective inhibitors moderately or highly resistant to cleavage by influenza sialidases (also called neuraminidases). The sialosides containing the 4‐guanidino‐substituted sialic acid represent a new class of sialidase substrate analog‐based inhibitors. We took advantage of this unique property to create a ligand‐based approach for efficiently isolating influenza virions from egg allantoic fluid with high purity. Together, these compounds are versatile probes and ligands for developing new approaches to detect, profile, isolate, and characterize influenza viruses via neuraminidases on their surface.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"24 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143819233","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

Low-Redox-Barrier Two-Electron p-Type Phenoselenazine Cathode for Superior Zinc-Organic Batteries

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-04-11 DOI: 10.1002/anie.202501278

Ting Shi, Ziyang Song, Chengmin Hu, Qi Huang, Yaokang Lv, Ling Miao, Lihua Gan, Dazhang Zhu, Mingxian Liu

{"title":"Low-Redox-Barrier Two-Electron p-Type Phenoselenazine Cathode for Superior Zinc-Organic Batteries","authors":"Ting Shi, Ziyang Song, Chengmin Hu, Qi Huang, Yaokang Lv, Ling Miao, Lihua Gan, Dazhang Zhu, Mingxian Liu","doi":"10.1002/anie.202501278","DOIUrl":"https://doi.org/10.1002/anie.202501278","url":null,"abstract":"Organic p-type cathode materials with high redox potentials and fast kinetics have captured widespread attention in propelling Zn-organic batteries (ZOBs). However, their anion-accessible capacity is insufficient due to single electron reaction and/or high energy barrier of each redox-active unit. Here we design two-electron-donating p-type organic chalcogen small molecules (phenoxazine (PO), phenothiazine (PS) and phenoselenazine (PSe)) with tuned charge distributions and electron transfer behaviors as cathode materials for ZOBs. With the decrease of chalcogenide electronegativity (O>S>Se), PSe liberates the strongest coordination activity, efficient electron delocalization, and charge storage kinetics with an ultralow redox activation energy (0.23 vs. 0.34 eV of PS and 0.41 eV of PO), which contributes to high dual-electron utilization of phenazine motifs of 99.2% (vs. 68.8% of PS and 52.7% of PO). Consequently, Zn||PSe battery delivers the highest capacity storage (227 mAh g−1) and energy density (273 Wh kg−1) among the reported p-type cells, along with long life (10,000 cycles). A two-electron redox mechanism is unlocked at amine/selenium sites of PSe, accompanied by reversible uptake of two CF3SO3− anions. This study highlights the considerable potential of low-energy-barrier multielectron design for high-performance organic cathodes towards advanced ZOBs.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"4 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143819917","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