{"title":"Design strategies for tetrazine fluorogenic probes for bioorthogonal imaging.","authors":"Aiwen Yu, Xinyu He, Tianruo Shen, Xinyu Yu, Wuyu Mao, Weijie Chi, Xiaogang Liu, Haoxing Wu","doi":"10.1039/d3cs00520h","DOIUrl":"https://doi.org/10.1039/d3cs00520h","url":null,"abstract":"<p><p>Tetrazine fluorogenic probes play a critical role in bioorthogonal chemistry, selectively activating fluorescence upon reaction to enhance precision in imaging and sensing within complex biological environments. Recent structural innovations-such as varied fluorophore choices, spacer optimization, and direct tetrazine integration within a fluorophore's π-conjugated system-have expanded their spectral range from visible to NIR, enhancing adaptability across various applications. This review examines advancements in the rational design and synthesis of these probes. We examine key fluorogenic mechanisms, such as energy transfer, internal conversion, and electron/charge transfer, that significantly influence fluorescence activation. We also highlight representative applications in live-cell imaging, super-resolution microscopy, and therapeutic monitoring, underscoring the expanding role of tetrazine probes in biomedical research and diagnostics. Collectively, these insights provide a strategic foundation for developing next-generation tetrazine probes with tailored properties to address evolving diagnostic and therapeutic challenges.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" ","pages":""},"PeriodicalIF":40.4,"publicationDate":"2025-02-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143397619","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}
Debashis Dhara, Laurence A Mulard, Marcel Hollenstein
{"title":"Natural, modified and conjugated carbohydrates in nucleic acids.","authors":"Debashis Dhara, Laurence A Mulard, Marcel Hollenstein","doi":"10.1039/d4cs00799a","DOIUrl":"https://doi.org/10.1039/d4cs00799a","url":null,"abstract":"<p><p>Storage of genetic information in DNA occurs through a unique ordering of canonical base pairs. However, this would not be possible in the absence of the sugar-phosphate backbone which is essential for duplex formation. While over a hundred nucleobase modifications have been identified (mainly in RNA), Nature is rather conservative when it comes to alterations at the level of the (deoxy)ribose sugar moiety. This trend is not reflected in synthetic analogues of nucleic acids where modifications of the sugar entity is commonplace to improve the properties of DNA and RNA. In this review article, we describe the main incentives behind sugar modifications in nucleic acids and we highlight recent progress in this field with a particular emphasis on therapeutic applications, the development of xeno-nucleic acids (XNAs), and on interrogating nucleic acid etiology. We also describe recent strategies to conjugate carbohydrates and oligosaccharides to oligonucleotides since this represents a particularly powerful strategy to improve the therapeutic index of oligonucleotide drugs. The advent of glycoRNAs combined with progress in nucleic acid and carbohydrate chemistry, protein engineering, and delivery methods will undoubtedly yield more potent sugar-modified nucleic acids for therapeutic, biotechnological, and synthetic biology applications.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" ","pages":""},"PeriodicalIF":40.4,"publicationDate":"2025-02-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143397620","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}
{"title":"Biocatalytic cascade reactions for management of diseases.","authors":"Ya-Ping Xiao, Jiayingzi Wu, Peng-Hang Chen, Shan Lei, Jing Lin, Xin Zhou, Peng Huang","doi":"10.1039/d3cs00410d","DOIUrl":"https://doi.org/10.1039/d3cs00410d","url":null,"abstract":"<p><p>Biocatalytic cascade reactions, which evolve from the confinement of multiple enzymes within living cells, represent a promising strategy for disease management. Using tailor-made nanoplatforms, reactions induced by multiple enzymes and/or nanozymes can be precisely triggered at pathogenic sites. These promote further cascade reactions that generate therapeutic species prompting effective therapeutic outcomes with minimal side effects. Over the past few years, this approach has seen widespread applications in disease management. This review attempts to critically assess and summarize the recent advances in the use of biocatalytic cascade reactions for the management of diseases. Emphasis is placed on the design of cascade catalytic systems of high efficiency and selectivity and the implementation of specific cascade processes that respond to the endogenous substances produced in the pathological processes. The various types of biocatalytic cascade reactions are outlined according to the timeline of the catalytic steps through a series of reported examples. The challenges and outlook in the field are also discussed to encourage the further development of personalized treatments based on biocatalytic cascade reactions.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" ","pages":""},"PeriodicalIF":40.4,"publicationDate":"2025-02-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143397618","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}
{"title":"Development of hydrophobic catalysts for reducing the CO<sub>2</sub> emission during the conversion of syngas into chemicals and fuels.","authors":"Yanfei Xu, Mingyue Ding","doi":"10.1039/d4cs00731j","DOIUrl":"https://doi.org/10.1039/d4cs00731j","url":null,"abstract":"<p><p>Syngas conversion is a key process for the production of chemicals and fuels from non-petroleum resources, such as biomass, coal, and natural gas. Water produced during syngas conversion can not only boost the production of CO<sub>2</sub> by-products <i>via</i> inducing the water-gas shift side reaction, but also inhibit the conversion of CO by occupying the active sites on the catalyst, leading to high CO<sub>2</sub> emission and low carbon utilization efficiency. Reducing CO<sub>2</sub> emission during syngas conversion is a main development direction of the energy chemical industry toward the goal of carbon neutrality. It has been reported that hydrophobic modification can reduce a surface's affinity to water molecules, and many breakthroughs in the development of hydrophobic catalysts for weakening the negative effect of water on syngas conversion have been made recently. A rapidly growing number of studies have demonstrated the versatility of hydrophobic catalysts. In this review, we systematically summarize and discuss the development of hydrophobic catalysts in syngas chemistry since the 2000s. These hydrophobic catalysts can be divided into three categories, <i>i.e.</i>, catalysts with hydrophobic surfaces, catalysts with hydrophobic supports, and catalysts physically mixed with hydrophobic promoters. Different categories of hydrophobic catalysts play different roles in syngas conversion. The perspectives and challenges for the future design of hydrophobic catalysts are also discussed.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" ","pages":""},"PeriodicalIF":40.4,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143389539","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}
Yitao Wu, Meiqi Tang, Michael L Barsoum, Zhijie Chen, Feihe Huang
{"title":"Functional crystalline porous framework materials based on supramolecular macrocycles.","authors":"Yitao Wu, Meiqi Tang, Michael L Barsoum, Zhijie Chen, Feihe Huang","doi":"10.1039/d3cs00939d","DOIUrl":"https://doi.org/10.1039/d3cs00939d","url":null,"abstract":"<p><p>Crystalline porous framework materials like metal-organic frameworks (MOFs) and covalent-organic frameworks (COFs) possess periodic extended structures, high porosity, tunability and designability, making them good candidates for sensing, catalysis, gas adsorption, separation, <i>etc.</i> Despite their many advantages, there are still problems affecting their applicability. For example, most of them lack specific recognition sites for guest uptake. Supramolecular macrocycles are typical hosts for guest uptake in solution. Macrocycle-based crystalline porous framework materials, in which macrocycles are incorporated into framework materials, are growing into an emerging area as they combine reticular chemistry and supramolecular chemistry. Organic building blocks which incorporate macrocycles endow the framework materials with guest recognition sites in the solid state through supramolecular interactions. Distinct from solution-state molecular recognition, the complexation in the solid state is ordered and structurally achievable. This allows for determination of the mechanism of molecular recognition through noncovalent interactions while that of the traditional recognition in solution is ambiguous. Furthermore, crystalline porous framework materials in the solid state are well-defined and recyclable, and can realize what is impossible in solution. In this review, we summarize the progress of the incorporation of macrocycles into functional crystalline porous frameworks (<i>i.e.</i>, MOFs and COFs) for their solid state applications such as molecular recognition, chiral separation and catalysis. We focus on the design and synthesis of organic building blocks with macrocycles, and then illustrate the applications of framework materials with macrocycles. Finally, we propose the future directions of macrocycle-based framework materials as reliable carriers for specific molecular recognition, as well as guiding the crystalline porous frameworks with their chemistry, applications and commercialization.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" ","pages":""},"PeriodicalIF":40.4,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143389540","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}
Arpita Roy, Ronak Afshari, Saumya Jain, Yuting Zheng, Min-Hsuan Lin, Shea Zenkar, Junyi Yin, Jun Chen, Nicholas A. Peppas, Nasim Annabi
{"title":"Advances in conducting nanocomposite hydrogels for wearable biomonitoring","authors":"Arpita Roy, Ronak Afshari, Saumya Jain, Yuting Zheng, Min-Hsuan Lin, Shea Zenkar, Junyi Yin, Jun Chen, Nicholas A. Peppas, Nasim Annabi","doi":"10.1039/d4cs00220b","DOIUrl":"https://doi.org/10.1039/d4cs00220b","url":null,"abstract":"Recent advancements in wearable biosensors and bioelectronics have led to innovative designs for personalized health management devices, with biocompatible conducting nanocomposite hydrogels emerging as a promising building block for soft electronics engineering. In this review, we provide a comprehensive framework for advancing biosensors using these engineered nanocomposite hydrogels, highlighting their unique properties such as high electrical conductivity, flexibility, self-healing, biocompatibility, biodegradability, and tunable architecture, broadening their biomedical applications. We summarize key properties of nanocomposite hydrogels for thermal, biomechanical, electrophysiological, and biochemical sensing applications on the human body, recent progress in nanocomposite hydrogel design and synthesis, and the latest technologies in developing flexible and wearable devices. This review covers various sensor types, including strain, physiological, and electrochemical sensors, and explores their potential applications in personalized healthcare, from daily activity monitoring to versatile electronic skin applications. Furthermore, we highlight the blueprints of design, working procedures, performance, detection limits, and sensitivity of these soft devices. Finally, we address challenges, prospects, and future outlook for advanced nanocomposite hydrogels in wearable sensors, aiming to provide a comprehensive overview of their current state and future potential in healthcare applications.","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":"1 1","pages":""},"PeriodicalIF":46.2,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375737","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}
Jianlu Sun, Yichen Du, Yijiang Liu, Dongbo Yan, Xiaodong Li, Dong Ha Kim, Zhiqun Lin, Xiaosi Zhou
{"title":"Recent advances in potassium metal batteries: electrodes, interfaces and electrolytes.","authors":"Jianlu Sun, Yichen Du, Yijiang Liu, Dongbo Yan, Xiaodong Li, Dong Ha Kim, Zhiqun Lin, Xiaosi Zhou","doi":"10.1039/d4cs00845f","DOIUrl":"https://doi.org/10.1039/d4cs00845f","url":null,"abstract":"<p><p>The exceptional theoretical capacity of potassium metal anodes (687 mA h g<sup>-1</sup>), along with their low electrochemical potential, makes potassium metal batteries (PMBs) highly attractive for achieving high energy density. This review first provides an overview of potassium metal anodes, including their origin, current development status, and distinctive advantages compared to other metal anodes. Then, it discusses the composition and characteristics of emerging breakthrough PMBs, such as K-S, K-O<sub>2</sub>, K-CO<sub>2</sub> batteries, and anode-free metal batteries. Subsequently, we delve into the pivotal challenges and theoretical research pertaining to PMBs, such as potassium metal nucleation/stripping, dendritic growth in PMBs, and unstable interfaces. Furthermore, we comprehensively examine the latest strategies in electrode design (including alloy, host, and current collector design), interface engineering (such as artificial solid electrolyte interphase layers, barrier layer design, and separator modification), and electrolyte optimization concerning nucleation, cycling stability, coulombic efficiency, and the development of PMBs. Finally, we introduce key characterization techniques, including <i>in situ</i> liquid phase secondary ion mass spectrometry, titration gas chromatography, neutron-based characterization, and computational simulation. This review will propel advancements in electrodes, separators, and electrolytes for innovative PMBs and other similar alkali metal batteries.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" ","pages":""},"PeriodicalIF":40.4,"publicationDate":"2025-02-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143363320","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}
{"title":"Reaction development: a student's checklist.","authors":"Jasper L Tyler, Dirk Trauner, Frank Glorius","doi":"10.1039/d4cs01046a","DOIUrl":"https://doi.org/10.1039/d4cs01046a","url":null,"abstract":"<p><p>So you've discovered a reaction. But how do you turn this new discovery into a fully-fledged program that maximises the potential of your novel transformation? Herein, we provide a student's checklist to serve as a helpful guide for synthesis development, allowing you to thoroughly investigate the chemistry in question while ensuring that no key aspect of the project is overlooked. A wide variety of the most illuminating synthetic and spectroscopic techniques will be summarised, in conjunction with literature examples and our own insights, to provide sound justifications for their implementation towards the goal of developing new reactions.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" ","pages":""},"PeriodicalIF":40.4,"publicationDate":"2025-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143254391","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}
Hui Zhu S, Yu Wu, Jianyou Mao, Jingkai Xu, Patrick J Walsh, Hang Shi
{"title":"C-H functionalization through benzylic deprotonation with π-coordination or cation-π-interactions.","authors":"Hui Zhu S, Yu Wu, Jianyou Mao, Jingkai Xu, Patrick J Walsh, Hang Shi","doi":"10.1039/d4cs00466c","DOIUrl":"https://doi.org/10.1039/d4cs00466c","url":null,"abstract":"<p><p>Benzylic C-H functionalization is a valuable tool to make complex aromatic molecules from simple, readily available alkylbenzenes. While methods that involve benzylic radicals or cations generated by hydrogen atom transfer or oxidation have been well demonstrated, they often require oxidative conditions. In contrast, deprotonation methods offer a complementary approach to transform benzylic C-H bonds through a benzylic carbanion generated by deprotonation. Electrophilic transition metal complexes acidify benzylic protons upon π-coordination to the phenyl ring of substrates, facilitating deprotonation by stabilizing the corresponding benzylic carbanion. Cation-complexes with group(I) metals also acidify benzylic C-H bonds. These approaches enable a significant expansion of the scope and diversity of alkylarenes with various electrophilic reagents. In this review, we discuss the development of benzylic functionalization through deprotonation of η<sup>6</sup>-arene complexes of transition-metals and cation-π interactions with group(I) metals, as well as progress made in catalysis through reversible arene-metal interactions.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" ","pages":""},"PeriodicalIF":40.4,"publicationDate":"2025-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143254390","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}
{"title":"Recent developments in polymer semiconductors with excellent electron transport performances.","authors":"Yunchao Zhang, Weifeng Zhang, Zhihui Chen, Liping Wang, Gui Yu","doi":"10.1039/d4cs00504j","DOIUrl":"https://doi.org/10.1039/d4cs00504j","url":null,"abstract":"<p><p>Benefiting from molecular design and device innovation, electronic devices based on polymer semiconductors have achieved significant developments and gradual commercialization over the past few decades. Most of high-performance polymer semiconductors that have been prepared exhibit p-type performances, and records of their carrier mobilities are constantly being broken through. Although ambipolar and n-type polymers are necessary for constructing p-n heterojunctions and logic circuits, only a few materials show outstanding device performances, which leads to their developments lagging far behind that of p-type analogues. As a consequence, it is extremely significant to summarize polymer semiconductors with excellent electron transport performances. This review focuses on the design considerations and bonding modes between monomers of polymer semiconductors with high electron mobilities. To enhance electron transport performances of polymer semiconductors, the structural modification strategies are described in detail. Subsequently, the electron transport, thermoelectric, mixed ionic-electronic conduction, intrinsically stretchable, photodetection, and spin transport performances of high-electron mobility polymers are discussed from the perspective of molecular engineering. In the end, the challenges and prospects in this research field are presented, which provide valuable guidance for the design of polymer semiconductors with excellent electron transport performances and the exploration of more advanced applications in the future.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" ","pages":""},"PeriodicalIF":40.4,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143187867","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}