Angewandte Chemie最新文献_第3页

Dual-Stimulus Programmed Multiphase Separation and Organization in Coacervate Droplets 凝聚液滴的双刺激程序化多相分离与组织

Angewandte Chemie Pub Date : 2025-09-07 DOI: 10.1002/ange.202512266

Yang Zhou, Prof. Dr. Brigitte Voit, Dr. Dietmar Appelhans

{"title":"Dual-Stimulus Programmed Multiphase Separation and Organization in Coacervate Droplets","authors":"Yang Zhou, Prof. Dr. Brigitte Voit, Dr. Dietmar Appelhans","doi":"10.1002/ange.202512266","DOIUrl":"https://doi.org/10.1002/ange.202512266","url":null,"abstract":"Stimuli-responsive (multiphase) coacervates deserve significant attention as cell-like entities that can adapt to their environment and undergo morphological reconfiguration. In this study, a tandem-triggered transition system is presented that enables the transformation of single-phase coacervates into multiphase structures through the sequential application of two external stimuli: pH and salt concentration. A polyanion containing acid-labile amide bond is incorporated into the membrane-less coacervates. Upon exposure to an acidic pH, hydrolysis of the amide bond induces charge reversal from polyanion to polycation, triggering the first transition from single-phase to nested multiphase coacervates. This transformation alters the spatial redistribution and viscosity of coacervate components and influences sequestration behavior toward various (macro) molecules. Subsequently, the introduction of hypertonic environment as secondary stimulus induces selective dissociation and structural reconfiguration of nested multiphase coacervates into vesicular-like multiphase coacervates, further altering the coacervate components' fluidity and partitioning properties. Notably, the diverse inherent properties of coacervates among this tandem-triggered transition enables the variation of spatial organization for enzymatic reactions. Overall, the findings demonstrate a strategy for the sequential control of coacervate structural reconfiguration through dual stimuli, providing a versatile platform for the development of programable and adaptive coacervate-based protocells.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 40","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202512266","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145171925","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

Translational Supramolecular Thioorthoester Chemistry 翻译超分子硫正酯化学

Angewandte Chemie Pub Date : 2025-09-06 DOI: 10.1002/ange.202517072

Dr. Giacomo Renno, Prof. Stefan Matile

引用次数: 0

A Versatile DNAzyme-Amplified Protease-Sensing Platform for Accurate Diagnosis of SARS-CoV-2 and Reliable Classification of Colorectal Cancer 用于SARS-CoV-2准确诊断和结直肠癌可靠分类的多功能dnazyme扩增蛋白酶传感平台

Angewandte Chemie Pub Date : 2025-09-06 DOI: 10.1002/ange.202507241

Benrui Weng, Yifei Wang, Qingqing Zhang, Yuqian Jiang, Jinhua Shang, Prof. Xiaoqing Liu, Prof. Fuan Wang

{"title":"A Versatile DNAzyme-Amplified Protease-Sensing Platform for Accurate Diagnosis of SARS-CoV-2 and Reliable Classification of Colorectal Cancer","authors":"Benrui Weng, Yifei Wang, Qingqing Zhang, Yuqian Jiang, Jinhua Shang, Prof. Xiaoqing Liu, Prof. Fuan Wang","doi":"10.1002/ange.202507241","DOIUrl":"https://doi.org/10.1002/ange.202507241","url":null,"abstract":"Peptide-based biosensors are widely used for in vitro detection of protease activity but often suffer from the limited sensitivity, poor accuracy, and incompatibility with point-of-care testing (POCT) devices. Herein, we developed a versatile deoxyribozyme (DNAzyme)-amplified protease-sensing (DP) platform that integrates the positively charged oligopeptides with a negatively charged DNAzyme biocatalyst for highly-sensitive protease detection. The system leverages the electrostatic peptide–DNAzyme interactions to inhibit DNAzyme catalytic activity, which is reactivated upon the protease-triggered peptide hydrolysis, thus enabling an efficient signal amplification via the successive cleavage of DNAzyme substrate. Compared to conventional peptide-based sensing platform, our DP system offers an enhanced sensitivity and signal-to-noise ratio and is highly modular for detecting various clinically relevant proteases through a simple replacement of the peptide blocker. By introducing a dual-enzyme recognition mechanism, we developed a dual-protease-triggered DP platform for enabling the accurate detection of SARS-CoV-2 proteases in saliva. We also applied the DP platform to differentiate between normal and cancerous colon cells and tissues by detecting colorectal cancer (CRC)-associated proteases. Overall, this work introduces a universal and scalable biosensing strategy for activity-based protease detection with potential applications in both infectious disease diagnostics and cancer classification, advancing the field of DNAzyme-based POCT technologies.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 40","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145171924","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

David B. Konrad 大卫·b·康拉德

Angewandte Chemie Pub Date : 2025-09-04 DOI: 10.1002/ange.202516578

David B. Konrad

引用次数: 0

Topology-Engineered Guide RNAs for Programmable Control of CRISPR/Cas Activity 用于CRISPR/Cas活性可编程控制的拓扑工程向导rna

Angewandte Chemie Pub Date : 2025-09-04 DOI: 10.1002/ange.202511756

Liang Cheng

{"title":"Topology-Engineered Guide RNAs for Programmable Control of CRISPR/Cas Activity","authors":"Liang Cheng","doi":"10.1002/ange.202511756","DOIUrl":"https://doi.org/10.1002/ange.202511756","url":null,"abstract":"CRISPR/Cas systems have transformed genome editing, yet achieving precise temporal and conditional control remains challenging. Traditional strategies involving linear guide RNAs (gRNAs) modified with multiple chemical groups throughout their strands often face limitations such as heterogeneous reaction outcomes, irreversibility, and variable editing efficiencies. To overcome these issues, topology-engineered guide RNAs (TE-gRNAs) have emerged, featuring defined structural architectures including polymeric, circular, and dendrimer-like topologies that enable precise spatial control, reversibility, and programmable activation of CRISPR activity. By selectively incorporating physical or chemically responsive linkers and stimuli-sensitive groups at specific sites, TE-gRNAs facilitate dynamic and conditional genome editing that can be activated or deactivated with external triggers such as light or chemical signals. These engineered RNA structures significantly improve synthesis feasibility, stability, reduce off-target effects, and provide unprecedented control over gene editing processes. Recent advancements in TE-gRNAs demonstrate their broad applicability in synthetic biology, functional genomics, and therapeutic interventions, highlighting their potential to achieve precise spatiotemporal modulation of CRISPR systems. This review summarizes the current strategies, benefits, and challenges associated with TE-gRNAs, and discusses future directions for enhancing their performance and utility in complex genome editing applications.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 41","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145230581","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

Tibor Szilvási

Angewandte Chemie Pub Date : 2025-09-04 DOI: 10.1002/ange.202518924

Tibor Szilvási

引用次数: 0

Unlocking the Full Potential of SERS: Merging Direct and Indirect Approaches for Enhanced Analysis of Multiplex Plasticizer Analogs in Matrices 释放SERS的全部潜力：将直接和间接方法合并用于矩阵中多重增塑剂类似物的增强分析

Angewandte Chemie Pub Date : 2025-09-04 DOI: 10.1002/ange.202507156

Shan Huei Lim, Lam Bang Thanh Nguyen, Emily Xi Tan, Prof. In Yee Phang, Dr. Untzizu Elejalde, Prof. Xing Yi Ling

{"title":"Unlocking the Full Potential of SERS: Merging Direct and Indirect Approaches for Enhanced Analysis of Multiplex Plasticizer Analogs in Matrices","authors":"Shan Huei Lim, Lam Bang Thanh Nguyen, Emily Xi Tan, Prof. In Yee Phang, Dr. Untzizu Elejalde, Prof. Xing Yi Ling","doi":"10.1002/ange.202507156","DOIUrl":"https://doi.org/10.1002/ange.202507156","url":null,"abstract":"Rapid and accurate identification of harmful plasticizer analogs in their native matrix is crucial for contaminant monitoring across industries. Surface-enhanced Raman scattering (SERS) shows promise for detecting structurally similar analogs but faces challenges like subtle receptor signal changes and distortion with weakly adsorbing plasticizer analytes. We address these limitations by integrating direct and indirect SERS to capture intrinsic Raman signals and receptor-analyte interactions, achieving 100% classification accuracy eight plasticizer analogs and multiplex quantification of three major plasticizers extracted from canola oil with < 5% predictive errors at a limit of detection (LOD) of 0.01 mg L−1, despite interference from other lipophilic contaminants such as adipates. Experimental SERS data and interaction energy calculations affirm that direct SERS detects alkyl chains, while indirect SERS identifies aromatic rings and carboxyl groups in eight plasticizer analogs with varying alkyl structures. A hybrid direct-indirect superspectrum was constructed, enabling the differentiation of eight analogs via Partial-Least-Squares Discriminant Analysis (PLS-DA) and further analysis using SHapley Additive exPlanations (SHAP) reveals equal contribution from all platforms, which highlights their complementary roles. These findings pave the way for broader applications in rapid, on-site detection of complex contaminants across industries.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 40","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145171917","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

Nickelaelektro-katalysierte C–H Aktivierung zur Darstellung β-arylierter Pyrrole via mehrfacher Dehydrierung 镍电催化C - H活化，通过多次脱水制备β-芳基化吡咯

Angewandte Chemie Pub Date : 2025-09-04 DOI: 10.1002/ange.202510233

Dr. Kazuhiro Okamoto, Simon L. Homölle, Dr. Tristan von Münchow, Sven E. Peters, Sven Trienes, Dr. João C. A. Oliveira, Prof. Dr. Lutz Ackermann

引用次数: 0

Advancing Organic Chemistry Using High-Throughput Experimentation 利用高通量实验推进有机化学

Angewandte Chemie Pub Date : 2025-09-03 DOI: 10.1002/ange.202506588

Reem Nsouli, Gaurav Galiyan, Prof. Laura K. G. Ackerman-Biegasiewicz

{"title":"Advancing Organic Chemistry Using High-Throughput Experimentation","authors":"Reem Nsouli, Gaurav Galiyan, Prof. Laura K. G. Ackerman-Biegasiewicz","doi":"10.1002/ange.202506588","DOIUrl":"https://doi.org/10.1002/ange.202506588","url":null,"abstract":"High-throughput experimentation (HTE), the miniaturization and parallelization of reactions, is a valuable tool for accelerating diverse compound library generation, optimizing reaction conditions, and enabling data collection for machine learning (ML) applications. When applied to organic synthesis and methodology, HTE still poses various challenges due to the diverse workflows and reagents required, motivating advancements in reaction design, execution, analysis, and data management. To address these limitations, cutting-edge technologies, automation, and artificial intelligence (AI) have been implemented to standardize protocols, enhance reproducibility, and improve efficiency. Additionally, strategies to reduce bias and promote serendipitous discoveries have further strengthened HTE's impact. This review highlights recent advances at every stage of the HTE workflow, including the development of customized workflows, diverse analysis, and improved data management practices for greater accessibility and shareability. Furthermore, we examine the current state of the field, outstanding challenges, and future directions toward transforming HTE into a fully integrated, flexible, and democratized platform that drives innovation in organic synthesis.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 40","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202506588","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145171915","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

Frontispiece: Chiral Self-Sorting of Flexible Covalent Organic Pillars for Adaptive Molecular Recognition 前言：用于适应性分子识别的柔性共价有机支柱的手性自分类

Angewandte Chemie Pub Date : 2025-09-02 DOI: 10.1002/ange.202583601

引用次数: 0