Chemical Society Reviews最新文献

{"title":"Supramolecular gels: a versatile crystallization toolbox","authors":"Rafael Contreras-Montoya, Luis Álvarez de Cienfuegos, José A. Gavira and Jonathan W. Steed","doi":"10.1039/D4CS00271G","DOIUrl":"10.1039/D4CS00271G","url":null,"abstract":"<p >Supramolecular gels are unique materials formed through the self-assembly of molecular building blocks, typically low molecular weight gelators (LMWGs), driven by non-covalent interactions. The process of crystallization within supramolecular gels has broadened the scope of the traditional gel-phase crystallization technique offering the possibility of obtaining crystals of higher quality and size. The broad structural diversity of LMWGs allows crystallization in multiple organic and aqueous solvents, favouring screening and optimization processes and the possibility to search for novel polymorphic forms. These supramolecular gels have been used for the crystallization of inorganic, small organic compounds of pharmaceutical interest, and proteins. Results have shown that these gels are not only able to produce crystals of high quality but also to influence polymorphism and physicochemical properties of the crystals, giving rise to crystals with potential new bio- and technological applications. Thus, understanding the principles of crystallization in supramolecular gels is essential for tailoring their properties and applications, ranging from drug delivery systems to composite crystals with tunable stability properties. In this review, we summarize the use of LMWG-based supramolecular gels as media to grow single crystals of a broad range of compounds.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" 21","pages":" 10604-10619"},"PeriodicalIF":40.4,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/cs/d4cs00271g?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142170927","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"PEDOT-based stretchable optoelectronic materials and devices for bioelectronic interfaces","authors":"Weizhen Li, Yiming Li, Ziyu Song, Yi-Xuan Wang and Wenping Hu","doi":"10.1039/D4CS00541D","DOIUrl":"10.1039/D4CS00541D","url":null,"abstract":"<p >The rapid development of wearable and implantable electronics has enabled the real-time transmission of electrophysiological signals <em>in situ</em>, thus allowing the precise monitoring and regulation of biological functions. Devices based on organic materials tend to have low moduli and intrinsic stretchability, making them ideal choices for the construction of seamless bioelectronic interfaces. In this case, as an organic ionic–electronic conductor, poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) has low impedance to offer a high signal-to-noise ratio for monitoring bioelectrical signals, which has become one of the most promising conductive polymers. However, the initial conductivity and stretchability of pristine PEDOT:PSS are insufficient to meet the application requirements, and there is a trade-off between their improvement. In addition, PEDOT:PSS has poor stability in aqueous environments due to the hygroscopicity of the PSS chains, which severely limits its long-term applications in water-rich bioelectronic interfaces. Considering the growing demands of multi-function integration, the high-resolution fabrication of electronic devices is urgent. It is a great challenge to maintain both electrical and mechanical performance after miniaturization, particularly at feature sizes below 100 μm. In this review, we focus on the combined improvement in the conductivity and stretchability of PEDOT:PSS, as well as the corresponding mechanisms in detail. Also, we summarize the effective strategies to improve the stability of PEDOT:PSS in aqueous environments, which plays a vital role in long-term applications. Finally, we introduce the reliable micropatterning technologies and PEDOT:PSS-based stretchable optoelectronic devices applied at bio-interfaces.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" 21","pages":" 10575-10603"},"PeriodicalIF":40.4,"publicationDate":"2024-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142170928","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":"Advanced electrolytes for high-performance aqueous zinc-ion batteries","authors":"Jie Wei, Pengbo Zhang, Jingjie Sun, Yuzhu Liu, Fajun Li, Haifeng Xu, Ruquan Ye, Zuoxiu Tie, Lin Sun and Zhong Jin","doi":"10.1039/D4CS00584H","DOIUrl":"10.1039/D4CS00584H","url":null,"abstract":"<p >Aqueous zinc-ion batteries (AZIBs) have garnered significant attention in the realm of large-scale and sustainable energy storage, primarily owing to their high safety, low cost, and eco-friendliness. Aqueous electrolytes, serving as an indispensable constituent, exert a direct influence on the electrochemical performance and longevity of AZIBs. Nonetheless, conventional aqueous electrolytes often encounter formidable challenges in AZIB applications, such as the limited electrochemical stability window and the zinc dendrite growth. In response to these hurdles, a series of advanced aqueous electrolytes have been proposed, such as “water-in-salt” electrolytes, aqueous eutectic electrolytes, molecular crowding electrolytes, and hydrogel electrolytes. This comprehensive review commences by presenting an in-depth overview of the fundamental compositions, principles, and distinctive characteristics of various advanced aqueous electrolytes for AZIBs. Subsequently, we systematically scrutinizes the recent research progress achieved with these advanced aqueous electrolytes. Furthermore, we summarizes the challenges and bottlenecks associated with these advanced aqueous electrolytes, along with offering recommendations. Based on the optimization of advanced aqueous electrolytes, this review outlines future directions and potential strategies for the development of high-performance AZIBs. This review is anticipated to provide valuable insights into the development of advanced electrolyte systems for the next generation of stable and sustainable multi-valent secondary batteries.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" 20","pages":" 10335-10369"},"PeriodicalIF":40.4,"publicationDate":"2024-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142170929","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":"Insights into the pH effect on hydrogen electrocatalysis","authors":"Wen-Gang Cui, Fan Gao, Guoquan Na, Xingqiang Wang, Zhenglong Li, Yaxiong Yang, Zhiqiang Niu, Yongquan Qu, Dingsheng Wang and Hongge Pan","doi":"10.1039/D4CS00370E","DOIUrl":"10.1039/D4CS00370E","url":null,"abstract":"<p >Hydrogen electrocatalytic reactions, including the hydrogen evolution reaction (HER) and the hydrogen oxidation reaction (HOR), play a crucial role in a wide range of energy conversion and storage technologies. However, the HER and HOR display anomalous non-Nernstian pH dependent kinetics, showing two to three orders of magnitude sluggish kinetics in alkaline media compared to that in acidic media. Fundamental understanding of the origins of the intrinsic pH effect has attracted substantial interest from the electrocatalysis community. More critically, a fundamental molecular level understanding of this effect is still debatable, but is essential for developing active, stable, and affordable fuel cells and water electrolysis technologies. Against this backdrop, in this review, we provide a comprehensive overview of the intrinsic pH effect on hydrogen electrocatalysis, covering the experimental observations, underlying principles, and strategies for catalyst design. We discuss the strengths and shortcomings of various activity descriptors, including hydrogen binding energy (HBE) theory, bifunctional theory, potential of zero free charge (pzfc) theory, 2B theory and other theories, across different electrolytes and catalyst surfaces, and outline their interrelations where possible. Additionally, we highlight the design principles and research progress in improving the alkaline HER/HOR kinetics by catalyst design and electrolyte optimization employing the aforementioned theories. Finally, the remaining controversies about the pH effects on HER/HOR kinetics as well as the challenges and possible research directions in this field are also put forward. This review aims to provide researchers with a comprehensive understanding of the intrinsic pH effect and inspire the development of more cost-effective and durable alkaline water electrolyzers (AWEs) and anion exchange membrane fuel cells (AMFCs) for a sustainable energy future.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" 20","pages":" 10253-10311"},"PeriodicalIF":40.4,"publicationDate":"2024-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142138630","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":"Supramolecular-macrocycle-based functional organic cocrystals","authors":"Susu Ren, Guan-Yu Qiao and Jia-Rui Wu","doi":"10.1039/D4CS00654B","DOIUrl":"10.1039/D4CS00654B","url":null,"abstract":"<p >Supramolecular macrocycles, renowned for their remarkable capabilities in molecular recognition and complexation, have emerged as pivotal elements driving advancements across various innovative research fields. Cocrystal materials, an important branch within the realm of crystalline organic materials, have garnered considerable attention owing to their simple preparation methods and diverse potential applications, particularly in optics, electronics, chemical sensing and photothermal conversion. In recent years, macrocyclic entitles have been successfully brought into this field, providing an essential and complementary channel to create novel functional materials, especially those with multiple functionalities and smart stimuli-responsiveness. In this Review, we present an overview of the research efforts on functional cocrystals constructed with macrocycles, covering their design principles, preparation strategies, assembly modes, and diverse functions and applications. Finally, the remaining challenges and perspectives are outlined. We anticipate that this review will serve as a valuable and timely reference for researchers interested in supramolecular crystalline materials and beyond, catalyzing the emergence of more original and innovative studies in related fields.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" 20","pages":" 10312-10334"},"PeriodicalIF":40.4,"publicationDate":"2024-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142138631","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":"Active template synthesis","authors":"Romain Jamagne, Martin J. Power, Zhi-Hui Zhang, Germán Zango, Benjamin Gibber and David A. Leigh","doi":"10.1039/D4CS00430B","DOIUrl":"10.1039/D4CS00430B","url":null,"abstract":"<p >The active template synthesis of mechanically interlocked molecular architectures exploits the dual ability of various structural elements (metals or, in the case of metal-free active template synthesis, particular arrangements of functional groups) to serve as both a template for the organisation of building blocks and as a catalyst to facilitate the formation of covalent bonds between them. This enables the entwined or threaded intermediate structure to be covalently captured under kinetic control. Unlike classical passive template synthesis, the intercomponent interactions transiently used to promote the assembly typically do not ‘live on’ in the interlocked product, meaning that active template synthesis can be traceless and used for constructing mechanically interlocked molecules that do not feature strong binding interactions between the components. Since its introduction in 2006, active template synthesis has been used to prepare a variety of rotaxanes, catenanes and knots. Amongst the metal–ion-mediated versions of the strategy, the copper(<small>I</small>)-catalysed alkyne–azide cycloaddition (CuAAC) remains the most extensively used transformation, although a broad range of other catalytic reactions and transition metals also provide effective manifolds. In metal-free active template synthesis, the recent discovery of the acceleration of the reaction of primary amines with electrophiles through the cavity of crown ethers has proved effective for forming an array of rotaxanes without recognition elements, including compact rotaxane superbases, dissipatively assembled rotaxanes and molecular pumps. This Review details the active template concept, outlines its advantages and limitations for the synthesis of interlocked molecules, and charts the diverse set of reactions that have been used with this strategy to date. The application of active template synthesis in various domains is discussed, including molecular machinery, mechanical chirality, catalysis, molecular recognition and various aspects of materials science.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" 20","pages":" 10216-10252"},"PeriodicalIF":40.4,"publicationDate":"2024-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11376342/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142131234","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Aggregation-induced emission-active supramolecular polymers: from controlled preparation to applications","authors":"Beibei Wang, Yuhao Liu, Xueqian Chen, Xiao-Ting Liu, Zhongyi Liu and Chao Lu","doi":"10.1039/D3CS00017F","DOIUrl":"10.1039/D3CS00017F","url":null,"abstract":"<p >Supramolecular polymers are typical self-assemblies, in which repeating monomer units are bonded together with dynamic and reversible noncovalent interactions. Supramolecular polymers can combine the advantages of polymer science and supramolecular chemistry. Aggregation-induced emission (AIE) means that a molecule remains faintly emissive in the dispersed state but intensively luminescent in a highly aggregated state. AIE has brought new opportunities and further development potential to the field of polymeric chemistry. The integration of AIE luminogens with supramolecular interactions can provide new vitality for supramolecular polymers. Therefore, it is essential for scientists to understand the preparation and applications of AIE-active supramolecular polymers. This review focuses on the recent advanced progress in the preparation of AIE-active supramolecular polymers. In addition, we summarize the newly developed supramolecular polymers with an AIE nature and their applications in chemical sensing, and <em>in vitro</em> and <em>in vivo</em> imaging, as well as the visualization of their structure and properties. Finally, the development trends and challenges of AIE-active supramolecular polymers are prospected.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" 20","pages":" 10189-10215"},"PeriodicalIF":40.4,"publicationDate":"2024-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142124241","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":"Heavier tetrylene- and tetrylyne-transition metal chemistry: it's no carbon copy","authors":"Terrance J. Hadlington","doi":"10.1039/D3CS00226H","DOIUrl":"10.1039/D3CS00226H","url":null,"abstract":"<p >Since the late 19th century, heavier tetrylene- and tetrylyne-transition metal chemistry has formed an important cornerstone in both main-group and organometallic chemistry alike. Driven by the success of carbene systems, significant efforts have gone towards the thorough understanding of the heavier group 14 derivatives, with examples now known from across the d-block. This now leads towards applications in cooperative bond activation, and moves ultimately towards well-defined catalytic systems. This review aims to summarise this vast field, from initial discoveries of tetrylene and tetrylyne complexes, to the most recent developments in reactivity and catalysis, as a platform to the future of this exciting, blossoming field.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" 19","pages":" 9738-9831"},"PeriodicalIF":40.4,"publicationDate":"2024-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11373607/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142124244","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Enzyme-responsive, multi-lock optical probes for molecular imaging and disease theranostics","authors":"Penghui Cheng and Kanyi Pu","doi":"10.1039/D4CS00335G","DOIUrl":"10.1039/D4CS00335G","url":null,"abstract":"<p >Optical imaging is an indispensable tool for non-invasive visualization of biomolecules in living organisms, thereby offering a sensitive approach for disease diagnosis and image-guided disease treatment. Single-lock activatable optical probes (SOPs) that specifically switch on optical signals in the presence of biomarkers-of-interest have shown both higher detection sensitivity and imaging quality as compared to conventional “always-on” optical probes. However, such SOPs can still show “false-positive” results in disease diagnosis due to non-specific biomarker expression in healthy tissues. By contrast, multi-lock activatable optical probes (MOPs) that simultaneously detect multiple biomarkers-of-interest could improve detection specificity towards certain biomolecular events or pathological conditions. In this Review, we discuss the recent advancements of enzyme-responsive MOPs, with a focus on their biomedical applications. The higher detection specificity of MOPs could in turn enhance disease diagnosis accuracy and improve treatment efficacy in image-guided disease therapy with minimal toxicity in the surrounding healthy tissues. Finally, we discuss the current challenges and suggest future applications of MOPs.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" 20","pages":" 10171-10188"},"PeriodicalIF":40.4,"publicationDate":"2024-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142124243","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":"Nanoscale chemical characterization of materials and interfaces by tip-enhanced Raman spectroscopy","authors":"Yi-Fan Bao, Meng-Yuan Zhu, Xiao-Jiao Zhao, Hong-Xuan Chen, Xiang Wang and Bin Ren","doi":"10.1039/D4CS00588K","DOIUrl":"10.1039/D4CS00588K","url":null,"abstract":"<p >Materials and their interfaces are the core for the development of a large variety of fields, including catalysis, energy storage and conversion. In this case, tip-enhanced Raman spectroscopy (TERS), which combines scanning probe microscopy with plasmon-enhanced Raman spectroscopy, is a powerful technique that can simultaneously obtain the morphological information and chemical fingerprint of target samples at nanometer spatial resolution. It is an ideal tool for the nanoscale chemical characterization of materials and interfaces, correlating their structures with chemical performances. In this review, we begin with a brief introduction to the nanoscale characterization of materials and interfaces, followed by a detailed discussion on the recent theoretical understanding and technical improvements of TERS, including the origin of enhancement, TERS instruments, TERS tips and the application of algorithms in TERS. Subsequently, we list the key experimental issues that need to be addressed to conduct successful TERS measurements. Next, we focus on the recent progress of TERS in the study of various materials, especially the novel low-dimensional materials, and the progresses of TERS in studying different interfaces, including both solid–gas and solid–liquid interfaces. Finally, we provide an outlook on the future developments of TERS in the study of materials and interfaces.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" 20","pages":" 10044-10079"},"PeriodicalIF":40.4,"publicationDate":"2024-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142124245","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}