Recently, owing to their special spatial structures, peptide-based macrocycles have shown tremendous promise and aroused great interest in multidisciplinary research ranging from potent antibiotics against resistant strains to functional biomaterials with novel properties. Besides traditional monocyclic peptides, many fascinating polycyclic and remarkable higher-order cyclic, spherical and cylindric peptidic systems have come into the limelight owing to breakthroughs in various chemical (e.g., native chemical ligation and transition metal catalysis), biological (e.g., post-translational enzymatic modification and genetic code reprogramming), and supramolecular (e.g., mechanically interlocked, metal-directed folding and self-assembly via noncovalent interactions) macrocyclization strategies developed in recent decades. In this tutorial review, diverse state-of-the-art macrocyclization methodologies and techniques for peptides and peptidomimetics are surveyed and discussed, with insights into their practical advantages and intrinsic limitations. Finally, the synthetic-technical aspects, current unresolved challenges, and outlook of this field are discussed.
{"title":"Recent advances in peptide macrocyclization strategies.","authors":"Pengyuan Fang, Wing-Ka Pang, Shouhu Xuan, Wai-Lun Chan, Ken Cham-Fai Leung","doi":"10.1039/d3cs01066j","DOIUrl":"https://doi.org/10.1039/d3cs01066j","url":null,"abstract":"<p><p>Recently, owing to their special spatial structures, peptide-based macrocycles have shown tremendous promise and aroused great interest in multidisciplinary research ranging from potent antibiotics against resistant strains to functional biomaterials with novel properties. Besides traditional monocyclic peptides, many fascinating polycyclic and remarkable higher-order cyclic, spherical and cylindric peptidic systems have come into the limelight owing to breakthroughs in various chemical (<i>e.g.</i>, native chemical ligation and transition metal catalysis), biological (<i>e.g.</i>, post-translational enzymatic modification and genetic code reprogramming), and supramolecular (<i>e.g.</i>, mechanically interlocked, metal-directed folding and self-assembly <i>via</i> noncovalent interactions) macrocyclization strategies developed in recent decades. In this tutorial review, diverse state-of-the-art macrocyclization methodologies and techniques for peptides and peptidomimetics are surveyed and discussed, with insights into their practical advantages and intrinsic limitations. Finally, the synthetic-technical aspects, current unresolved challenges, and outlook of this field are discussed.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" ","pages":""},"PeriodicalIF":40.4,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142666649","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}
Youxin Fu, Xing Zhang, Luling Wu, Miaomiao Wu, Tony D James, Run Zhang
Over the past two decades, bioorthogonal chemistry has undergone a remarkable development, challenging traditional assumptions in biology and medicine. Recent advancements in the design of probes tailored for bioorthogonal applications have met the increasing demand for precise imaging, facilitating the exploration of complex biological systems. These state-of-the-art probes enable highly sensitive, low background, in situ imaging of biological species and events within live organisms, achieving resolutions comparable to the size of the biomolecule under investigation. This review provides a comprehensive examination of various categories of bioorthogonally activated in situ fluorescent labels. It highlights the intricate design and benefits of bioorthogonal chemistry for precise in situ imaging, while also discussing future prospects in this rapidly evolving field.
{"title":"Bioorthogonally activated probes for precise fluorescence imaging.","authors":"Youxin Fu, Xing Zhang, Luling Wu, Miaomiao Wu, Tony D James, Run Zhang","doi":"10.1039/d3cs00883e","DOIUrl":"10.1039/d3cs00883e","url":null,"abstract":"<p><p>Over the past two decades, bioorthogonal chemistry has undergone a remarkable development, challenging traditional assumptions in biology and medicine. Recent advancements in the design of probes tailored for bioorthogonal applications have met the increasing demand for precise imaging, facilitating the exploration of complex biological systems. These state-of-the-art probes enable highly sensitive, low background, <i>in situ</i> imaging of biological species and events within live organisms, achieving resolutions comparable to the size of the biomolecule under investigation. This review provides a comprehensive examination of various categories of bioorthogonally activated <i>in situ</i> fluorescent labels. It highlights the intricate design and benefits of bioorthogonal chemistry for precise <i>in situ</i> imaging, while also discussing future prospects in this rapidly evolving field.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" ","pages":""},"PeriodicalIF":40.4,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646096","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}
Sara Catherine Sand, Jennifer L M Rupp, Bilge Yildiz
In the transition to safer, more energy-dense solid state batteries, polymer-ceramic composite electrolytes may offer a potential route to achieve simultaneously high Li-ion conductivity and enhanced mechanical stability. Despite numerous studies on the polymer-ceramic composite electrolytes, disagreements persist on whether the polymer or the ceramic is positively impacted in their constituent ionic conductivity for such composite electrolytes, and even whether the interface is a blocking layer or a highly conductive lithium ion path. This lack of understanding limits the design of effective composite solid electrolytes. By thorough and critical analysis of the data collected in the field over the last three decades, we present arguments for lithium conduction through the bulk of the polymer, ceramic, or their interface. From this analysis, we can conclude that the unexpectedly high conductivity reported for some ceramic-polymer composites cannot be accounted for by the ceramic phase alone. There is evidence to support the theory that the Li-ion conductivity in the polymer phase increases along this interface in contact with the ceramic. The potential mechanisms for this include increased free volume, decreased crystallinity, and modulated Lewis acid-base effects in the polymer, with the former two to be the more likely mechanisms. Future work in this field requires understanding these factors more quantitatively, and tuning of the ceramic surface chemistry and morphology in order to obtain targeted structural modifications in the polymer phase.
{"title":"A critical review on Li-ion transport, chemistry and structure of ceramic-polymer composite electrolytes for solid state batteries.","authors":"Sara Catherine Sand, Jennifer L M Rupp, Bilge Yildiz","doi":"10.1039/d4cs00214h","DOIUrl":"https://doi.org/10.1039/d4cs00214h","url":null,"abstract":"<p><p>In the transition to safer, more energy-dense solid state batteries, polymer-ceramic composite electrolytes may offer a potential route to achieve simultaneously high Li-ion conductivity and enhanced mechanical stability. Despite numerous studies on the polymer-ceramic composite electrolytes, disagreements persist on whether the polymer or the ceramic is positively impacted in their constituent ionic conductivity for such composite electrolytes, and even whether the interface is a blocking layer or a highly conductive lithium ion path. This lack of understanding limits the design of effective composite solid electrolytes. By thorough and critical analysis of the data collected in the field over the last three decades, we present arguments for lithium conduction through the bulk of the polymer, ceramic, or their interface. From this analysis, we can conclude that the unexpectedly high conductivity reported for some ceramic-polymer composites cannot be accounted for by the ceramic phase alone. There is evidence to support the theory that the Li-ion conductivity in the polymer phase increases along this interface in contact with the ceramic. The potential mechanisms for this include increased free volume, decreased crystallinity, and modulated Lewis acid-base effects in the polymer, with the former two to be the more likely mechanisms. Future work in this field requires understanding these factors more quantitatively, and tuning of the ceramic surface chemistry and morphology in order to obtain targeted structural modifications in the polymer phase.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" ","pages":""},"PeriodicalIF":40.4,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646083","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}