Chemical Society Reviews最新文献

{"title":"Bis(trimethylsilyl)phosphide chemistry: a half-century of advances across the periodic table","authors":"Jack Baldwin, David P. Mills","doi":"10.1039/d4cs01141d","DOIUrl":"https://doi.org/10.1039/d4cs01141d","url":null,"abstract":"Whilst bis(trimethylsilyl)amide has been used extensively as a ligand across the periodic table, the chemistry of its heavier group 15 congeners is relatively underdeveloped. However, bis(trimethylsilyl)phosphide coordination chemistry has provided unique structural motifs and has also shown potential applications in catalysis, materials science, and bioinorganic chemistry. This review, which marks 55 years since the first report of a bis(trimethylsilyl)phosphide complex, provides a comprehensive overview of the synthesis, characterisation and reactivity of structurally authenticated s-, p-, d- and f-block metal complexes of this ligand, focusing on salient single crystal XRD and NMR spectroscopic data. We discuss the factors influencing the diverse coordination modes and reactivity profiles of bis(trimethylsilyl)phosphide complexes, together with an overview of their potential as precursors for novel solid-state materials, aiming to inspire future research endeavours using this ligand. We also review the small number of bis(triisopropylsilyl)phosphide complexes, in order to provide motivation for the future study of other bis(silyl)phosphide ligands.","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":"17 1","pages":""},"PeriodicalIF":46.2,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143598956","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":"Metal–organic frameworks (MOFs) toward SO2 detection","authors":"Juan L. Obeso, Catalina V. Flores, Ricardo A. Peralta, Margarita Viniegra, N. Martín-Guaregua, Michael T. Huxley, Diego Solis-Ibarra, Ilich A. Ibarra, Christoph Janiak","doi":"10.1039/d4cs00997e","DOIUrl":"https://doi.org/10.1039/d4cs00997e","url":null,"abstract":"Developing technology that can precisely monitor specific air pollutants in diverse settings is essential to control emissions and ensure safe exposure limits are not exceeded. Metal–organic frameworks (MOFs) are crystalline organic–inorganic hybrid materials, which are promising candidates for SO<small>₂</small> detection. Their chemically mutable periodic structure confers outstanding surface area, thermal stability, and a well-defined pore distribution. Moreover, MOFs have exhibited extraordinary performance for SO<small>₂</small> capture. Therefore, research has focused on their possible applications for SO<small>₂</small> sequestration due to the selective and robust chemical and physical interactions of SO<small>₂</small> molecules within MOFs. The variable SO<small>₂</small> affinity presented by MOFs enables the adsorption mechanism and preferential adsorption sites to be resolved. However, for MOF-based SO<small>₂</small> detection, selective SO<small>₂</small> capture at shallow partial pressure (0.01–0.1 bar) is required. Thus, capturing SO<small>₂</small> at low concentration is crucial for SO<small>₂</small> detection, where textural properties of MOFs, mainly the pore-limiting diameter, are essential to achieve selective detection. In this review, we discuss the fundamental aspects of SO<small>₂</small> detection in MOFs, providing a step-by-step methodology for SO<small>₂</small> detection in MOFs. We hope this review can provide valuable background around SO<small>₂</small> detection in MOFs and inspire further research within this new and exciting field.","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":"13 1","pages":""},"PeriodicalIF":46.2,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143582941","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":"Metal pyrazolate frameworks: crystal engineering access to stable functional materials","authors":"Xiang-Jing Kong, Guang-Rui Si, Tao He, Jian-Rong Li","doi":"10.1039/d4cs00989d","DOIUrl":"https://doi.org/10.1039/d4cs00989d","url":null,"abstract":"As the focus evolves from structure discovery/characterization (what it is) to property/performance exploration (what it is for), the pursuit of stable functional metal–organic frameworks (MOFs) has been ongoing in terms of both fundamental research and industrial implementation. Under the guidance of crystal engineering principles, a plethora of research has developed pyrazolate MOFs (metal pyrazaolate frameworks, MPFs) featuring strong coordination M–N bonding. This attribution helps them retain their structures and functions under the alkaline conditions required for practical use. Based on poly-topic pyrazolate ligands, various classic MOFs, such as Co(bdp), Fe<small>₂</small>(BDP)<small>₃</small>, Ni<small>₈</small>L<small>₆</small>, PCN-601, and BUT-55, to name a few, have revealed fascinating architectures, intriguing properties, and record-breaking performances in applications during the past decade. This review will present the full scope of MPFs to date: (1) the superiority and significance of constructing MPFs through the crystal engineering approach, (2) synthetic strategies adopted in building and/or modifying MPFs, (3) structural features and stability of the MPF community, and (4) potential applications in energy and environmental related fields. The future opportunities of MPFs are also discussed for designing the next-generation of smart materials. Overall, this review attempts to provide insights and guidelines for the customization of pyrazolate-based MOFs for specific purposes, which would also promote the development of stable functional porous materials for addressing societal challenges.","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":"76 1","pages":""},"PeriodicalIF":46.2,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143570154","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":"Formulation principles and synergistic effects of high-voltage electrolytes","authors":"Zewei Wei, Du Yuan, Xuedi Yuan, Yalin Zhang, Jianmin Ma, Suojiang Zhang, Haitao Zhang","doi":"10.1039/d4cs00826j","DOIUrl":"https://doi.org/10.1039/d4cs00826j","url":null,"abstract":"The energy density of lithium-ion batteries (LIBs) is primarily determined by the working potential of devices and the specific capacity of cathode compounds. Carbonate-based electrolytes have received considerable attention due to their significance for advancing current cell-assembly process. However, the commercially available liquid LiPF<small>₆</small> based electrolytes cannot withstand the harsh high-voltage environment and the effects of cathode, due to issues such as the undesired oxidative decomposition of ethylene carbonate (EC), the catalytic influence of dissolved transition metal ions (TMs), and the poor performance of interphases with unstable morphologies and components. Furthermore, the complex working mechanisms of high-voltage electrolytes (HVEs) are not fully understood. This review presents a comprehensive summary of the HVEs, including their physical properties, solvation structures, and interface chemistry. Specifically, chemical environment of high-voltage cathode compounds and failure mechanisms of commercial electrolytes are investigated, followed by a discussion of expected functions of HVEs. Then, screening criteria for single-component electrolytes, considering their oxidation resistance and decomposition mechanism, and screening mechanism of interphase species are explored based on their energy level positions. Next, a cross-scale evolution framework is proposed, from the solvation structure to interphase characteristics, aimed at uncovering the formulation principles and synergistic effects of HVEs. Operational mechanisms are systematically scrutinized, starting from the conventional tuning of solvation structure to the incorporation of multiple components and further to the role of entropy-driven effects, all of which will favor the understanding of formulation principles and synergistic effects. Finally, integration of advanced computational methods and mature experimental techniques is expected to foster the development of novel perspectives and promising electrolyte candidates.","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":"53 1","pages":""},"PeriodicalIF":46.2,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143561345","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":"Synthesis innovations for crystallizing covalent organic framework thin films on biological and non-biological substrates","authors":"Ashok Kumar Mahato, Satyadip Paul and Rahul Banerjee","doi":"10.1039/D4CS01222D","DOIUrl":"10.1039/D4CS01222D","url":null,"abstract":"<p >Thin film technology has emerged as a pivotal field with numerous industrial applications. Depending on their properties—such as magnetic characteristics, conductivity, architectural structure, stability, and functional backbones—thin films are widely utilized in optoelectronics, thin-film coatings, solar cells, energy storage devices, semiconductors, and separation applications. However, for all these applications, thin films must be securely attached to specific substrates, and substrate compatibility with both the thin film and the film-growth process is crucial for optimal performance. In this review, we emphasize the significance of growing thin films, particularly covalent organic framework (COF) thin films, on suitable substrates tailored for various applications. For separation technologies, polymer thin films are commonly fabricated on porous polymeric or metal-based membranes. In contrast, thin films of metals and metal oxides are typically deposited on conducting substrates, serving as current collectors for energy storage devices. Semiconductor thin films, on the other hand, are often grown on silicon or glass substrates for transistor applications. Emerging COF thin films, with their tunable properties, well-defined pore channels, and versatile functional backbones, have demonstrated exceptional potential in separation, energy storage, and electronic and optoelectronic applications. However, the interplay between COF thin films and the substrates, as well as the compatibility of growth conditions, remains underexplored. Studies investigating COF thin film growth on substrates such as metals, metal oxides, glass, silicon, polymers, ITO, and FTO have provided insights into substrate properties that promote superior film growth. The quality of the film formed on these substrates significantly influences performance in applications. Additionally, we discuss the stabilization of biological substrates, like peptide-based biomimetic catalysts and enzymes, which often suffer from instability in non-aqueous environments, limiting their industrial use. Growing COF membranes on these biological substrates can enhance their stability under harsh conditions. We also highlight techniques for growing COF membranes on biological substrates, ensuring the preservation of their structural integrity and functional properties.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" 7","pages":" 3578-3598"},"PeriodicalIF":40.4,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/cs/d4cs01222d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143555376","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":"Opto-digital molecular analytics","authors":"Chelsea Violita Stanley, Yi Xiao, Tong Ling, Dong-Sheng Li and Peng Chen","doi":"10.1039/D5CS00023H","DOIUrl":"10.1039/D5CS00023H","url":null,"abstract":"<p >In contrast to conventional ensemble-average-based methods, opto-digital molecular analytic approaches digitize detection by physically partitioning individual detection events into discrete compartments or directly locating and analyzing the signals from single molecules. The sensitivity can be enhanced by signal amplification reactions, signal enhancement interactions, labelling by strong signal emitters, advanced optics, image processing, and machine learning, while specificity can be improved by designing target-selective probes and profiling molecular dynamics. With the capabilities to attain a limit of detection several orders lower than the conventional methods, reveal intrinsic molecular information, and achieve multiplexed analysis using a small-volume sample, the emerging opto-digital molecular analytics may be revolutionarily instrumental to clinical diagnosis, molecular chemistry and science, drug discovery, and environment monitoring. In this article, we provide a comprehensive review of the recent advances, offer insights into the underlying mechanisms, give comparative discussions on different strategies, and discuss the current challenges and future possibilities.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" 7","pages":" 3557-3577"},"PeriodicalIF":40.4,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/cs/d5cs00023h?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143538584","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":"Implantable hydrogels as pioneering materials for next-generation brain–computer interfaces","authors":"Wasid Ullah Khan, Zhenzhen Shen, Samuel M. Mugo, Hongda Wang and Qiang Zhang","doi":"10.1039/D4CS01074D","DOIUrl":"10.1039/D4CS01074D","url":null,"abstract":"<p >Use of brain–computer interfaces (BCIs) is rapidly becoming a transformative approach for diagnosing and treating various brain disorders. By facilitating direct communication between the brain and external devices, BCIs have the potential to revolutionize neural activity monitoring, targeted neuromodulation strategies, and the restoration of brain functions. However, BCI technology faces significant challenges in achieving long-term, stable, high-quality recordings and accurately modulating neural activity. Traditional implantable electrodes, primarily made from rigid materials like metal, silicon, and carbon, provide excellent conductivity but encounter serious issues such as foreign body rejection, neural signal attenuation, and micromotion with brain tissue. To address these limitations, hydrogels are emerging as promising candidates for BCIs, given their mechanical and chemical similarities to brain tissues. These hydrogels are particularly suitable for implantable neural electrodes due to their three-dimensional water-rich structures, soft elastomeric properties, biocompatibility, and enhanced electrochemical characteristics. These exceptional features make them ideal for signal recording, neural modulation, and effective therapies for neurological conditions. This review highlights the current advancements in implantable hydrogel electrodes, focusing on their unique properties for neural signal recording and neuromodulation technologies, with the ultimate aim of treating brain disorders. A comprehensive overview is provided to encourage future progress in this field. Implantable hydrogel electrodes for BCIs have enormous potential to influence the broader scientific landscape and drive groundbreaking innovations across various sectors.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" 6","pages":" 2832-2880"},"PeriodicalIF":40.4,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143538712","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":"C3-symmetric aromatic triimides as useful building blocks for supramolecular chemistry and advanced materials","authors":"De-Hui Tuo, Xu-Dong Wang and De-Xian Wang","doi":"10.1039/D4CS00892H","DOIUrl":"10.1039/D4CS00892H","url":null,"abstract":"<p > <em>C</em> <small>₃</small>-symmetric aromatic triimides (ATIs) represent an interesting class of electron-deficient molecular backbones, characterized by π-conjugated aromatic cores symmetrically substituted with three imide groups. Their unique structural and electronic features, combined with exceptional stability and straightforward <em>N</em>-functionalization at three imide sites, make ATIs promising as versatile building blocks for applications in supramolecular chemistry and materials science. Despite their promising attributes, research on ATIs remains underexplored compared to the extensively studied aromatic imides and diimides, largely due to the synthetic challenges involved in constructing three imide groups on the aromatic frameworks. In recent years, advances in synthetic protocols have significantly propelled ATI-related chemistry, expanding their applications in the realm of functional materials. This review compiles advancements in the synthesis, structural and physicochemical properties, and applications of ATIs in supramolecular chemistry and advanced materials. We anticipate that this review will not only draw greater attention to ATIs but also serve as a valuable guide for future research into these molecular building blocks.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" 7","pages":" 3535-3556"},"PeriodicalIF":40.4,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143538711","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":"Stability of photoelectrochemical cells based on colloidal quantum dots","authors":"Kanghong Wang, Yi Tao, Zikun Tang, Haiguang Zhao, Xuhui Sun, Federico Rosei, Dong Liu and Yujie Xiong","doi":"10.1039/D4CS00587B","DOIUrl":"10.1039/D4CS00587B","url":null,"abstract":"<p >Solar-driven photoelectrochemical (PEC) cells, sensitized by colloidal quantum dots (QDs), are emerging as a promising approach for solar-to-fuel conversion, including hydrogen evolution and peroxide production. The high absorption coefficient and customizable size/composition/shape of QDs can effectively enhance and broaden the light absorption capabilities of the system. Additionally, QD-based heterostructures can facilitate carrier transfer, thereby enhancing the overall performance. To date, the photocurrent density of QD based photoelectrodes for water splitting has significantly surpassed that of conventional metal oxides and sulfides. However, despite recent advances in enhancing the photocurrent density of QD-based photoelectrodes, long-term operational stability remains a key challenge for their practical applications. Few studies so far have investigated in depth the stability mechanism of QD-based PEC cells alongside potential fabrication improvements. In this Review, we first discuss the dominant factors and mechanisms responsible for the deterioration of both QDs and QD-based PEC devices. Subsequently, we outline the prevalent processing techniques and effective strategies for the fabrication of durable PEC cells. Finally, future perspectives and research directions in this field are proposed.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" 7","pages":" 3513-3534"},"PeriodicalIF":40.4,"publicationDate":"2025-03-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143532650","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":"Functional gel materials for next-generation electrochromic devices and applications","authors":"Yuyang Wang, Xiaoyan Sun, Quanbing Liu and Guihua Yu","doi":"10.1039/D4CS01256A","DOIUrl":"10.1039/D4CS01256A","url":null,"abstract":"<p >Flexible, wearable, bistable displays, visualized energy storage devices and large-area smart windows based on electrochromic (EC) technology are regarded as promising next-generation sustainable display technologies, with the potential to improve people's lives by enabling low-energy consumption, vision-friendly, smart display, and energy-efficient building solutions. Recently, gel-based EC devices have gained considerable research interest and have emerged as an effective platform for EC applications due to their unique and enhanced properties. Compared to solid-state and liquid-state EC devices, gel-based EC systems offer superior processability and scalability, improved mechanical properties such as flexibility and stretchability, and high ionic conductivity without leakage or volatility issues. This review summarizes and analyzes the gelation chemistry in EC systems, focusing on their relationship with key EC properties of the device. Ionic conductivity, temperature adaptability, and mechanical characteristics of the gels such as stretchability, self-healing ability, flexibility, and viscosity are foundational for enabling diverse functional EC applications. We introduce the preparation methods of related gels for EC devices and then discuss the factors influencing the properties and the strategies for tuning them, including the control of morphology, network architecture, polymer skeletons, functional groups, and additives within ion gels. Representative and latest applications of gel-based electrolytes in EC devices for various promising displays were then presented. Finally, we critically analyze the remaining challenges that need to be addressed to enable the practical deployment of gel-based EC devices and offer more insights into future directions for advancing EC technologies.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" 7","pages":" 3475-3512"},"PeriodicalIF":40.4,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143522077","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}