Chemical Reviews最新文献

{"title":"MOF-Based Electrocatalysts: An Overview from the Perspective of Structural Design","authors":"Nana Sun, Syed Shoaib Ahmad Shah, Zhongyuan Lin, Yan-Zhen Zheng, Long Jiao, Hai-Long Jiang","doi":"10.1021/acs.chemrev.4c00664","DOIUrl":"https://doi.org/10.1021/acs.chemrev.4c00664","url":null,"abstract":"The electrocatalytic technique, as an efficient energy storage and conversion technology, has attracted significant attention to address energy exhaustion and environmental pollution. Usually, the activity and selectivity of electrocatalytic reactions are largely dominated by the dynamic process occurring on electrocatalysts. Therefore, high-performance electrocatalysts, which can dominate the pathway and energy barrier of reactions, are of great significance for the advancement of the electrocatalytic technique. Metal–organic frameworks (MOFs), as emerging crystalline porous materials, present structural and component advantages including well-defined structure, high surface area, large porosity, diverse components, and easy tailorability, demonstrating fantastic potential for the precise fabrication of electrocatalysts. In this Review, the emerging strategies in the precise fabrication of electrocatalysts based on MOF-related materials are specifically introduced from the aspects of catalytic site design and microenvironment modulation around catalytic sites. Furthermore, representative progress achieved in various electrocatalytic applications employing MOF-based electrocatalysts is systematically summarized, with special emphasis on the structural design of MOFs for catalytic performance optimization. Finally, the remaining challenges and future perspectives of MOF-based electrocatalysts are further highlighted.","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":"29 1","pages":""},"PeriodicalIF":62.1,"publicationDate":"2025-02-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143435640","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":"Theory and Modeling of Transport for Simple Fluids in Nanoporous Materials: From Microscopic to Coarse-Grained Descriptions","authors":"Alexander Schlaich, Jean-Louis Barrat, Benoit Coasne","doi":"10.1021/acs.chemrev.4c00406","DOIUrl":"https://doi.org/10.1021/acs.chemrev.4c00406","url":null,"abstract":"We present the state-of-the-art of theoretical modeling, molecular simulation, and coarse-graining strategies for the transport of gases and liquids in nanoporous materials (pore size 1–100 nm). Special emphasis is placed on the transport of small molecules in zeolites, active carbons, metal–organic frameworks, but also in nanoporous materials with larger pores such as ordered and disordered mesoporous oxides. We present different atomistic and mesoscopic methods as well as available theoretical formalisms to describe such a complex problem. Attention is given to the investigation of different molecular transport coefficients─including the self, collective and transport diffusivities─but also to the determination of free energy barriers and their role in overall adsorption/separation process rates. We further introduce other available approaches such as hierarchical simulations and upscaling strategies. This review focuses on simple fluids in prototypical nanoporous materials. While the phenomena covered here capture the main physical mechanisms in such systems, complex molecules will exhibit additional specific features. For the sake of clarity and brevity, we also omit multicomponent systems (e.g., fluid mixtures, electrolytes, etc.) and electrokinetic effects arising when charged systems are considered (ionic species, charged surfaces, etc.), both of which add to the complexity.","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":"15 1","pages":""},"PeriodicalIF":62.1,"publicationDate":"2025-02-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143443952","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":"Luminescent Lanthanides in Biorelated Applications: From Molecules to Nanoparticles and Diagnostic Probes to Therapeutics","authors":"Carlson Alexander, Zhilin Guo, Peter B. Glover, Stephen Faulkner, Zoe Pikramenou","doi":"10.1021/acs.chemrev.4c00615","DOIUrl":"https://doi.org/10.1021/acs.chemrev.4c00615","url":null,"abstract":"Lanthanides are particularly effective in their clinical applications in magnetic resonance imaging and diagnostic assays. They have open-shell 4<i>f</i> electrons that give rise to characteristic narrow, line-like emission which is unique from other fluorescent probes in biological systems. Lanthanide luminescence signal offers selection of detection pathways based on the choice of the ion from the visible to the near-infrared with long luminescence lifetimes that lend themselves to time-resolved measurements for optical multiplexing detection schemes and novel bioimaging applications. The delivery of lanthanide agents in cells allows localized bioresponsive activity for novel therapies. Detection in the near-infrared region of the spectrum coupled with technological advances in microscopies opens new avenues for deep-tissue imaging and surgical interventions. This review focuses on the different ways in which lanthanide luminescence can be exploited in nucleic acid and enzyme detection, anion recognition, cellular imaging, tissue imaging, and photoinduced therapeutic applications. We have focused on the hierarchy of designs that include luminescent lanthanides as probes in biology considering coordination complexes, multimetallic lanthanide systems to metal–organic frameworks and nanoparticles highlighting the different strategies in downshifting, and upconversion revealing some of the opportunities and challenges that offer potential for further development in the field.","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":"49 1","pages":""},"PeriodicalIF":62.1,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143426966","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":"Luminescent Lanthanides in Biorelated Applications: From Molecules to Nanoparticles and Diagnostic Probes to Therapeutics","authors":"Carlson Alexander,&nbsp;Zhilin Guo,&nbsp;Peter B. Glover,&nbsp;Stephen Faulkner and Zoe Pikramenou*,&nbsp;","doi":"10.1021/acs.chemrev.4c0061510.1021/acs.chemrev.4c00615","DOIUrl":"https://doi.org/10.1021/acs.chemrev.4c00615https://doi.org/10.1021/acs.chemrev.4c00615","url":null,"abstract":"<p >Lanthanides are particularly effective in their clinical applications in magnetic resonance imaging and diagnostic assays. They have open-shell 4<i>f</i> electrons that give rise to characteristic narrow, line-like emission which is unique from other fluorescent probes in biological systems. Lanthanide luminescence signal offers selection of detection pathways based on the choice of the ion from the visible to the near-infrared with long luminescence lifetimes that lend themselves to time-resolved measurements for optical multiplexing detection schemes and novel bioimaging applications. The delivery of lanthanide agents in cells allows localized bioresponsive activity for novel therapies. Detection in the near-infrared region of the spectrum coupled with technological advances in microscopies opens new avenues for deep-tissue imaging and surgical interventions. This review focuses on the different ways in which lanthanide luminescence can be exploited in nucleic acid and enzyme detection, anion recognition, cellular imaging, tissue imaging, and photoinduced therapeutic applications. We have focused on the hierarchy of designs that include luminescent lanthanides as probes in biology considering coordination complexes, multimetallic lanthanide systems to metal–organic frameworks and nanoparticles highlighting the different strategies in downshifting, and upconversion revealing some of the opportunities and challenges that offer potential for further development in the field.</p>","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":"125 4","pages":"2269–2370 2269–2370"},"PeriodicalIF":51.4,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.chemrev.4c00615","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143486925","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":"Electrochemical Random-Access Memory: Progress, Perspectives, and Opportunities","authors":"A. Alec Talin*,&nbsp;Jordan Meyer,&nbsp;Jingxian Li,&nbsp;Mantao Huang,&nbsp;Miranda Schwacke,&nbsp;Heejung W. Chung,&nbsp;Longlong Xu,&nbsp;Elliot J. Fuller,&nbsp;Yiyang Li* and Bilge Yildiz*,&nbsp;","doi":"10.1021/acs.chemrev.4c0051210.1021/acs.chemrev.4c00512","DOIUrl":"https://doi.org/10.1021/acs.chemrev.4c00512https://doi.org/10.1021/acs.chemrev.4c00512","url":null,"abstract":"<p >Non-von Neumann computing using neuromorphic systems based on analogue synaptic and neuronal elements has emerged as a potential solution to tackle the growing need for more efficient data processing, but progress toward practical systems has been stymied due to a lack of materials and devices with the appropriate attributes. Recently, solid state electrochemical ion-insertion, also known as electrochemical random access memory (ECRAM) has emerged as a promising approach to realize the needed device characteristics. ECRAM is a three terminal device that operates by tuning electronic conductance in functional materials through solid-state electrochemical redox reactions. This mechanism can be considered as a gate-controlled bulk modulation of dopants and/or phases in the channel. Early work demonstrating that ECRAM can achieve nearly ideal analogue synaptic characteristics has sparked tremendous interest in this approach. More recently, the realization that electrochemical ion insertion can be used to tune the electronic properties of many types of materials including transition metal oxides, layered two-dimensional materials, organic and coordination polymers, and that the changes in conductance can span orders of magnitude has further attracted interest in ECRAM as the basis for analogue synaptic elements for inference accelerators as well as for dynamical devices that can emulate a wide range of neuronal characteristics for implementation in analogue spiking neural networks. At its core, ECRAM shares many fundamental aspects with rechargeable batteries, where ion insertion materials are used extensively for their ability to reversibly store charge and energy. Computing applications, however, present drastically different requirements: systems will require many millions of devices, scaled down to tens of nanometers, all while achieving reliable electronic-state tuning at scaled-up rates and endurances, and with minimal energy dissipation and noise. In this review, we discuss the history, basic concepts, recent progress, as well as the challenges and opportunities for different types of ECRAM, broadly grouped by their primary mobile ionic charge carrier, including Li, protons, and oxygen vacancies.</p>","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":"125 4","pages":"1962–2008 1962–2008"},"PeriodicalIF":51.4,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143486969","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":"Electrochemical Random-Access Memory: Progress, Perspectives, and Opportunities","authors":"A. Alec Talin, Jordan Meyer, Jingxian Li, Mantao Huang, Miranda Schwacke, Heejung W. Chung, Longlong Xu, Elliot J. Fuller, Yiyang Li, Bilge Yildiz","doi":"10.1021/acs.chemrev.4c00512","DOIUrl":"https://doi.org/10.1021/acs.chemrev.4c00512","url":null,"abstract":"Non-von Neumann computing using neuromorphic systems based on analogue synaptic and neuronal elements has emerged as a potential solution to tackle the growing need for more efficient data processing, but progress toward practical systems has been stymied due to a lack of materials and devices with the appropriate attributes. Recently, solid state electrochemical ion-insertion, also known as electrochemical random access memory (ECRAM) has emerged as a promising approach to realize the needed device characteristics. ECRAM is a three terminal device that operates by tuning electronic conductance in functional materials through solid-state electrochemical redox reactions. This mechanism can be considered as a gate-controlled bulk modulation of dopants and/or phases in the channel. Early work demonstrating that ECRAM can achieve nearly ideal analogue synaptic characteristics has sparked tremendous interest in this approach. More recently, the realization that electrochemical ion insertion can be used to tune the electronic properties of many types of materials including transition metal oxides, layered two-dimensional materials, organic and coordination polymers, and that the changes in conductance can span orders of magnitude has further attracted interest in ECRAM as the basis for analogue synaptic elements for inference accelerators as well as for dynamical devices that can emulate a wide range of neuronal characteristics for implementation in analogue spiking neural networks. At its core, ECRAM shares many fundamental aspects with rechargeable batteries, where ion insertion materials are used extensively for their ability to reversibly store charge and energy. Computing applications, however, present drastically different requirements: systems will require many millions of devices, scaled down to tens of nanometers, all while achieving reliable electronic-state tuning at scaled-up rates and endurances, and with minimal energy dissipation and noise. In this review, we discuss the history, basic concepts, recent progress, as well as the challenges and opportunities for different types of ECRAM, broadly grouped by their primary mobile ionic charge carrier, including Li, protons, and oxygen vacancies.","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":"80 4 1","pages":""},"PeriodicalIF":62.1,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143426965","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":"Chemical Design of Magnetic Nanomaterials for Imaging and Ferroptosis-Based Cancer Therapy","authors":"Wei Xu,&nbsp;Guoqiang Guan,&nbsp;Renye Yue,&nbsp;Zhe Dong,&nbsp;Lingling Lei,&nbsp;Heemin Kang* and Guosheng Song*,&nbsp;","doi":"10.1021/acs.chemrev.4c0054610.1021/acs.chemrev.4c00546","DOIUrl":"https://doi.org/10.1021/acs.chemrev.4c00546https://doi.org/10.1021/acs.chemrev.4c00546","url":null,"abstract":"<p >Ferroptosis, an iron-dependent form of regulatory cell death, has garnered significant interest as a therapeutic target in cancer treatment due to its distinct characteristics, including lipid peroxide generation and redox imbalance. However, its clinical application in oncology is currently limited by issues such as suboptimal efficacy and potential off-target effects. The advent of nanotechnology has provided a new way for overcoming these challenges through the development of activatable magnetic nanoparticles (MNPs). These innovative MNPs are designed to improve the specificity and efficacy of ferroptosis induction. This Review delves into the chemical and biological principles guiding the design of MNPs for ferroptosis-based cancer therapies and imaging-guided therapies. It discusses the regulatory mechanisms and biological attributes of ferroptosis, the chemical composition of MNPs, their mechanism of action as ferroptosis inducers, and their integration with advanced imaging techniques for therapeutic monitoring. Additionally, we examine the convergence of ferroptosis with other therapeutic strategies, including chemodynamic therapy, photothermal therapy, photodynamic therapy, sonodynamic therapy, and immunotherapy, within the context of nanomedicine strategies utilizing MNPs. This Review highlights the potential of these multifunctional MNPs to surpass the limitations of conventional treatments, envisioning a future of drug-resistance-free, precision diagnostics and ferroptosis-based therapies for treating recalcitrant cancers.</p>","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":"125 4","pages":"1897–1961 1897–1961"},"PeriodicalIF":51.4,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143486953","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":"Introduction: The Future of Plastics Sustainability.","authors":"Brooks A Abel, Geoffrey W Coates","doi":"10.1021/acs.chemrev.4c00958","DOIUrl":"https://doi.org/10.1021/acs.chemrev.4c00958","url":null,"abstract":"","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":"125 3","pages":"1255-1256"},"PeriodicalIF":51.4,"publicationDate":"2025-02-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143397507","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":"Silver Anniversary of the Renaissance in Metallocorrole Chemistry.","authors":"Atif Mahammed, Harry B Gray, Zeev Gross","doi":"10.1021/acs.chemrev.4c00764","DOIUrl":"https://doi.org/10.1021/acs.chemrev.4c00764","url":null,"abstract":"<p><p>The 1999 discovery of one-pot corrole synthesis opened the floodgates for research on these unique macrocyclic chelating agents. The enormous impact of this discovery has been documented in numerous reviews describing advances in the synthetic chemistry of corroles and selected applications in which corroles are key components. Our silver anniversary review focuses on the structures and reactions of all well characterized corrole-chelated d- and p-block metal complexes, including discussions of their electronic excited-state physics and chemistry. Emphasis is placed on electronic structure of the trinegative N4 coordination core, which stabilizes high-valent metals and activates low-valent ones, and, importantly, profoundly influences ground- and excited-state reactivity. Our story highlights the unique properties of corroles that have made them the molecular components of choice in a plethora of applications. These include their utility for sensing gases and anions, rescue of vital biomolecules from oxidative damage, destruction of cancerous cells, and catalysis of reactions critical for organic synthesis, as well as those involved in clean energy processes such as production of hydrogen and reduction of oxygen. In our view, research on corroles will continue to grow by leaps and bounds, most especially in areas of human health research and renewable energy science and technology.</p>","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":" ","pages":""},"PeriodicalIF":51.4,"publicationDate":"2025-02-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143397514","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":"Introduction: The Future of Plastics Sustainability","authors":"Brooks A. Abel,&nbsp; and ,&nbsp;Geoffrey W. Coates,&nbsp;","doi":"10.1021/acs.chemrev.4c0095810.1021/acs.chemrev.4c00958","DOIUrl":"https://doi.org/10.1021/acs.chemrev.4c00958https://doi.org/10.1021/acs.chemrev.4c00958","url":null,"abstract":"","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":"125 3","pages":"1255–1256 1255–1256"},"PeriodicalIF":51.4,"publicationDate":"2025-02-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143385994","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}