Chemical Society Reviews最新文献

{"title":"Defect engineered Ti-MOFs and their applications","authors":"Guo-Ying Han, Mingshuo Sun, Ruixin Zhao, Qazi Mohammad Junaid, Guozhen Hou, Numan Zada Khan Mohmand, Chunmei Jia, Yiwei Liu, Pascal Van Der Voort, Lei Shi, Xiao Feng","doi":"10.1039/d4cs01007h","DOIUrl":"https://doi.org/10.1039/d4cs01007h","url":null,"abstract":"Titanium-based metal–organic frameworks (Ti-MOFs) hold great potential for applications in photocatalysis and other fields, owing to Ti's abundant reserves, low toxicity, and excellent photocatalytic and redox activity. However, Ti's strong affinity for oxygen often leads to Ti-MOFs being fully coordinated with ligands, which limits their catalytic and separation performance. Defect engineering provides an effective strategy to enhance the functionality of MOFs by introducing structural imperfections. Despite this, the synthesis of new Ti-MOFs and the incorporation of defects remain challenging due to the complex hydrolysis and reaction processes of Ti precursors and the uncertainty of Ti cluster formation. This review categorizes Ti-MOFs according to their diverse cluster structures, which play a key role in the development of new frameworks and defect engineering. It also examines various defect construction methods and their applications. Finally, insights from defect-engineered Zr-MOFs are discussed to inspire future advancements in the synthesis and application of defective Ti-MOFs.","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":"17 1","pages":""},"PeriodicalIF":46.2,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143858212","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":"Selective two-electron and four-electron oxygen reduction reactions using Co-based electrocatalysts","authors":"Zuozhong Liang, Haitao Lei, Haoquan Zheng, Hong-Yan Wang, Wei Zhang, Rui Cao","doi":"10.1039/d4cs01199f","DOIUrl":"https://doi.org/10.1039/d4cs01199f","url":null,"abstract":"The oxygen reduction reaction (ORR) can take place <em>via</em> both four-electron (4e<small>⁻</small>) and two-electron (2e<small>⁻</small>) pathways. The 4e<small>⁻</small> ORR, which produces water (H<small>₂</small>O) as the only product, is the key reaction at the cathode of fuel cells and metal–air batteries. On the other hand, the 2e<small>⁻</small> ORR can be used to electrocatalytically synthesize hydrogen peroxide (H<small>₂</small>O<small>₂</small>). For the practical applications of the ORR, it is very important to precisely control the selectivity. Understanding structural effects on the ORR provides the basis to control the selectivity. Co-based electrocatalysts have been extensively studied for the ORR due to their high activity, low cost, and relative ease of synthesis. More importantly, by appropriately designing their structures, Co-based electrocatalysts can become highly selective for either the 2e<small>⁻</small> or the 4e<small>⁻</small> ORR. Therefore, Co-based electrocatalysts are ideal models for studying fundamental structure–selectivity relationships of the ORR. This review starts by introducing the reaction mechanism and selectivity evaluation of the ORR. Next, Co-based electrocatalysts, especially Co porphyrins, used for the ORR with both 2e<small>⁻</small> and 4e<small>⁻</small> selectivity are summarized and discussed, which leads to the conclusion of several key structural factors for ORR selectivity regulation. On the basis of this understanding, future works on the use of Co-based electrocatalysts for the ORR are suggested. This review is valuable for the rational design of molecular catalysts and material catalysts with high selectivity for 4e<small>⁻</small> and 2e<small>⁻</small> ORRs. The structural regulation of Co-based electrocatalysts also provides insights into the design and development of ORR electrocatalysts based on other metal elements.","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":"33 1","pages":""},"PeriodicalIF":46.2,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143858214","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":"Hierarchical design of silkworm silk for functional composites.","authors":"Kang Yang, Jingwu Zhang, Chen Zhang, Juan Guan, Shengjie Ling, Zhengzhong Shao","doi":"10.1039/d4cs00776j","DOIUrl":"https://doi.org/10.1039/d4cs00776j","url":null,"abstract":"<p><p>Silk-reinforced composites (SRCs) manifest the unique properties of silkworm silk fibers, offering enhanced mechanical strength, biocompatibility, and biodegradability. These composites present an eco-friendly alternative to conventional synthetic materials, with applications expanding beyond biomedical engineering, flexible electronics, and environmental filtration. This review explores the diverse forms of silkworm silk fibers including fabrics, long fibers, and nanofibrils, for functional composites. It highlights advancements in composite design and processing techniques that allow precise engineering of mechanical and functional performance. Despite substantial progress, challenges remain in making optimally functionalized SRCs with multi-faceted performance and understanding the mechanics for reverse-design of SRCs. Future research should focus on the unique sustainable, biodegradable and biocompatible advantages and embrace advanced processing technology, as well as artificial intelligence-assisted material design to exploit the full potential of SRCs. This review on SRCs will offer a foundation for future advancements in multifunctional and high-performance silk-based composites.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" ","pages":""},"PeriodicalIF":40.4,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143953422","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":"Exploring guest species in zeolites using transmission electron microscopy: a review and outlook.","authors":"Zhiling Yu, Huang Lin, Hui Zhang, Yu Han","doi":"10.1039/d5cs00159e","DOIUrl":"https://doi.org/10.1039/d5cs00159e","url":null,"abstract":"<p><p>Zeolites, with their well-defined microporous frameworks, accommodate diverse guest species, including metal ions, atoms, clusters, complexes, and organic molecules. Direct imaging of these species and their interactions with the framework is crucial for understanding their structural and functional roles. Transmission electron microscopy (TEM), particularly aberration-corrected scanning TEM (STEM), has become an indispensable tool, offering atomic-resolution real-space insights. This review summarizes key (S)TEM techniques for probing guest species in zeolites, with a focus on low-dose strategies to minimize beam damage. We discuss the principles, applications, and limitations of various imaging modalities and highlight recent advances in visualizing metallic and organic species. Finally, we explore future directions for (S)TEM in zeolite research, emphasizing the opportunities and challenges of <i>in situ</i>, three-dimensional, and cryogenic imaging for resolving host-guest interactions with greater precision.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" ","pages":""},"PeriodicalIF":40.4,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143951871","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":"State-of-the-art and perspectives of hydrogen generation from waste plastics","authors":"Feng Niu, Zeqi Wu, Da Chen, Yuexiang Huang, Vitaly V. Ordomsky, Andrei Y. Khodakov, Kevin M. Van Geem","doi":"10.1039/d4cs00604f","DOIUrl":"https://doi.org/10.1039/d4cs00604f","url":null,"abstract":"Waste plastic utilization and hydrogen production present significant economic and social challenges but also offer opportunities for research and innovation. This review provides a comprehensive analysis of the latest advancements and innovations in hydrogen generation coupled with waste plastic recycling. It explores various strategies, including pyrolysis, gasification, aqueous phase reforming, photoreforming, and electrocatalysis. Pyrolysis and gasification in combination with catalytic reforming or water gas-shift are currently the most feasible and scalable technologies for hydrogen generation from waste plastics, with pyrolysis operating in an oxygen-free environment and gasification in the presence of steam, though both require high energy inputs. Aqueous phase reforming operates at moderate temperatures and pressures, making it suitable for oxygenated plastics, but it faces challenges related to feedstock limitations, catalyst costs and deactivation. Photoreforming and electrocatalytic reforming are emerging, sustainable methods that use sunlight and electricity, respectively, to convert plastics into hydrogen. Still, they suffer from low efficiency, scalability issues, and limitations to specific plastic types like oxygenated polymers. The challenges and solutions to commercializing plastic-to-hydrogen technologies, drawing on global industrial case studies have been outlined. Maximizing hydrogen productivity and selectivity, minimizing energy consumption, and ensuring stable operation and scaleup of plastic recycling are crucial parameters for achieving commercial viability.","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":"38 1","pages":""},"PeriodicalIF":46.2,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143832309","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":"The evolution of machine learning potentials for molecules, reactions and materials","authors":"Junfan Xia, Yaolong Zhang, Bin Jiang","doi":"10.1039/d5cs00104h","DOIUrl":"https://doi.org/10.1039/d5cs00104h","url":null,"abstract":"Recent years have witnessed the fast development of machine learning potentials (MLPs) and their widespread applications in chemistry, physics, and material science. By fitting discrete <em>ab initio</em> data faithfully to continuous and symmetry-preserving mathematical forms, MLPs have enabled accurate and efficient atomistic simulations in a large scale from first principles. In this review, we provide an overview of the evolution of MLPs in the past two decades and focus on the state-of-the-art MLPs proposed in the last a few years for molecules, reactions, and materials. We discuss some representative applications of MLPs and the trend of developing universal potentials across a variety of systems. Finally, we outline a list of open challenges and opportunities in the development and applications of MLPs.","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":"13 1","pages":""},"PeriodicalIF":46.2,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143827245","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":"Chiral nanographenes exhibiting circularly polarized luminescence","authors":"Viksit Kumar, José L. Páez, Sandra Míguez-Lago, Juan M. Cuerva, Carlos M. Cruz, Araceli G. Campaña","doi":"10.1039/d4cs00745j","DOIUrl":"https://doi.org/10.1039/d4cs00745j","url":null,"abstract":"Chiral nanographenes constitute an unconventional material class that deviates from planar graphene cutouts. They have gained considerable attention for their ability to exhibit circularly polarized luminescence (CPL), which offers new opportunities in chiral optoelectronics. Their unique π-conjugated architectures, coupled with the ability to introduce chirality at the molecular level, have made them powerful contenders in developing next-generation optoelectronic devices. This review thoroughly explores recent advances in the synthesis, structural design, and CPL performance of chiral nanographenes. We delve into diverse strategies for inducing chirality, including covalent functionalization, helically twisted frameworks, and heteroatom doping, each of which unlocks distinct CPL behaviors. In addition, we discuss the mechanistic principles governing CPL and future directions in chiral nanographenes to achieve high dissymmetry factors (<em>g</em><small>_lum</small>) and tunable emission properties. We also discuss the key challenges in this evolving field, including designing robust chiral frameworks, optimizing CPL efficiency, and scaling up real-world applications. Through this review, we aim to shed light on recent developments in the bottom-up synthesis of structurally precise chiral nanographenes and evaluate their impact on the growing domain of circularly polarized luminescent materials.","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":"19 1","pages":""},"PeriodicalIF":46.2,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143819194","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":"Boron cluster leveraged polymeric building blocks","authors":"Jianwei Li, Jong Seung Kim, Jiangli Fan, Xiaojun Peng and Pavel Matějíček","doi":"10.1039/D4CS01288G","DOIUrl":"10.1039/D4CS01288G","url":null,"abstract":"<p >Boron cluster compounds (BCCs) are inorganic molecules characterized by their unique physical and chemical properties. Polymeric materials incorporating BCCs exhibit significant chemical and thermal stability, making them valuable for applications in biomedical fields, energy storage, ultrahigh stability materials, and π-conjugated luminochromic polymers. This review article aims to explore the primary methods for integrating these distinctive clusters into traditional carbon-based polymers. Both boron and carbon atoms possess catenation abilities, enabling the formation of extensive macromolecular structures. While carbon forms long linear chains, boron typically leads to three-dimensional polyhedral clusters. We first examine hybrid nanostructures, focusing on weak non-covalent interactions such as dihydrogen bonding, hydrophobic, and chaotropic effects between boron clusters and polymer chains. We then discuss classical chemical bonding approaches. Despite their inorganic nature, boron clusters can undergo exoskeletal substitution akin to organic counterparts, allowing their attachment as side groups to polymer repeating units. Additionally, polyhedral boron clusters can be incorporated into polymer backbones primarily through polycondensation reactions, resulting in hybrid macromolecules with exceptional physical and chemical attributes. Finally, we summarize the applications of BCC-containing polymeric materials, including their use in boron neutron capture therapy (BNCT), solid polymer electrolytes (SPEs) for metal ion batteries, and as electron acceptor groups in stimuli-responsive luminescent materials. In summary, BCC-containing polymeric materials are increasingly considered viable alternatives to traditional hydrocarbon-based polymers for biomedical applications, ion-conducting materials, luminescent materials, and temperature-resistant materials.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" 9","pages":" 4104-4134"},"PeriodicalIF":40.4,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143806225","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":"Opportunities for the renewable energy transition via reactive carbon capture","authors":"Eleanor Kearns, Rachel E. Siegel, Deanna M. D’Alessandro, Ji-Woong Lee and Louise A. Berben","doi":"10.1039/D4CS00741G","DOIUrl":"10.1039/D4CS00741G","url":null,"abstract":"<p >In this viewpoint article, we give a brief overview definition of reactive carbon capture (RCC) and its relationship to traditional carbon capture (CC) technologies. We also discuss possible short- and long-term roles for RCC in the transition to a renewable energy economy, along with opportunities for support and recent scientific progress in selected areas of the world.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" 9","pages":" 4096-4103"},"PeriodicalIF":40.4,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143797673","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":"The structuring of porous reticular materials for energy applications at industrial scales","authors":"Mehrdad Asgari, Pablo Albacete, Dhruv Menon, Yuexi Lyu, Xu Chen, David Fairen-Jimenez","doi":"10.1039/d5cs00166h","DOIUrl":"https://doi.org/10.1039/d5cs00166h","url":null,"abstract":"Reticular synthesis constructs crystalline architectures by linking molecular building blocks with robust bonds. This process gave rise to reticular chemistry and permanently porous solids. Such precise control over pore shape, size and surface chemistry makes reticular materials versatile for gas storage, separation, catalysis, sensing, and healthcare applications. Despite their potential, the transition from laboratory to industrial applications remains largely limited. Among various factors contributing to this translational gap, the challenges associated with their formulation through structuring and densification for industrial compatibility are significant yet underexplored areas. Here, we focus on the shaping strategies for porous reticular materials, particularly metal–organic frameworks (MOFs) and covalent organic frameworks (COFs), to facilitate their industrial application. We explore techniques that preserve functionality and ensure durability under rigorous industrial conditions. The discussion highlights various configurations – granules, monoliths, pellets, thin films, gels, foams, and glasses – structured to maintain the materials’ intrinsic microscopic properties at a macroscopic level. We examine the foundational theory and principles behind these shapes and structures, employing both <em>in situ</em> and post-synthetic methods. Through case studies, we demonstrate the performance of these materials in real-world settings, offering a structuring blueprint to inform the selection of techniques and shapes for diverse applications. Ultimately, we argue that advancing structuring strategies for porous reticular materials is key to closing the gap between laboratory research and industrial utilization.","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":"11 1","pages":""},"PeriodicalIF":46.2,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143797672","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}