Accounts of materials research最新文献

{"title":"Fast Scanning Calorimetry of Semicrystalline Polymers: From Fundamental Research to Industrial Applications","authors":"Rui Zhang, Mengxue Du, Katalee Jariyavidyanont, René Androsch, Evgeny Zhuravlev, Christoph Schick","doi":"10.1021/accountsmr.5c00031","DOIUrl":"https://doi.org/10.1021/accountsmr.5c00031","url":null,"abstract":"The global production of polymer products currently exceeds 400 megatons annually. To ensure effective and environmentally responsible use of this vast resource, optimizing the properties of the products is essential. Achieving this requires precise control over the internal structure of the polymers. Depending on the materials used, polymers can exist in either amorphous or semicrystalline states. Processing is often performed from the melt state, and the cooling rate plays a critical role in determining whether amorphous or semicrystalline products are formed alongside other process parameters such as the pressure and shear rates.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"136 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143876324","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Synthesis of Homogeneous Plasmonic Nanostructures for Generating Uniform and Reproducible Photonic Environments","authors":"Yoonhee Kim, Yuna Kwak, Jihyeon Choi, Jwa-Min Nam","doi":"10.1021/accountsmr.5c00043","DOIUrl":"https://doi.org/10.1021/accountsmr.5c00043","url":null,"abstract":"The preserved bosonic nature of surface plasmon polaritons from incident photons allows plasmonic nanomaterials to serve as effective photonic platforms. The strong light–matter interaction occurring at the surface concentrates light energy within a narrow region, thereby altering the local density of optical states. This modified photonic environment is typically expressed as near-field enhancement and improves the transition probability of nearby molecules or quantum emitters. However, despite the potential of plasmonic nanostructures to act as signal-transducers, issues in generating reproducible and consistent photonic responses with these platforms hinder their wide use for practical applications. As the parameters of plasmonic modulation are highly sensitive to even minor differences in surface morphology, a key origin of fluctuation in optical responses is the physical heterogeneity of the constituent nanostructures themselves. Therefore, although statistical and analytical techniques can obtain optically consistent signals from plasmonic nanostructures, the necessity of synthesizing uniform plasmonic nanostructures to achieve identical optical signals is becoming ever-more evident.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143876242","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Cell–Material Interactions in Vascular Tissue Engineering","authors":"Connor D Amelung, Sharon Gerecht","doi":"10.1021/accountsmr.4c00390","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00390","url":null,"abstract":"The vascular system, encompassing blood and lymphatic vessels, is essential for nutrient transport, waste elimination, and homeostasis regulation. Composed of endothelial cells and mural cells, such as smooth muscle cells and pericytes, the vasculature is critical for various physiological processes, including development, organogenesis, wound healing, and tumor metastasis. The interplay between the biophysical properties of the extracellular matrix and its biochemical composition significantly influences vascular function and integrity. However, studying these complex interactions <i>in vivo</i> presents considerable challenges, underscoring the need for innovative research methodologies. For example, traditional 2D cell culture fails to account for the complex, multifaceted environment that cells are exposed to <i>in vivo</i>. Vascular tissue engineering has emerged as a promising approach, aiming to replicate the architecture and functionality of blood vessels to enhance understanding of vascular development and pathology. A central facet of vascular tissue engineering is biomaterial design, in which natural or synthetic polymers are assembled into water-swollen networks, or hydrogels, for 3D cell cultures that can last days or weeks. By utilizing hydrogel biomaterials, researchers can create tunable model systems that closely mimic the natural vascular environment, such as by modifying polymer backbone functionalization and the local biochemical environment or altering the resultant physical properties of the hydrogel. These customizable microenvironments facilitate critical cell–matrix interactions, enabling investigations into key vascular mechanisms such as adhesion, migration, proliferation, and differentiation. This Account explores key aspects of cell–matrix interactions in vascular tissue engineering and the biomaterials designed to study them. We begin with advancements in material design that replicate the spatial and mechanical properties of vascular tissues: matrix stiffness can be tuned to mimic the stiffness of <i>in vivo</i> tissues, viscoelasticity is introduced to replicate the time-dependent strain associated with biologic fluids and tissues, spatial orientation is designed to mimic the architecture common to naturally occurring extracellular matrix, and degradation is an inherent feature of these materials to facilitate cell-caused microenvironment remodeling. We then examine how the biochemical properties of materials influence vascular function: matrix composition can replicate the factors expected in the vascular extracellular matrix, bioactive cues are presented to match the complex gradients formed by paracrine signaling, and hypoxia can be introduced via material design to understand how angiogenesis occurs at the edges of existing vascular networks. Finally, we identify major challenges in the field, highlighting current obstacles and proposing future strategies to enhance the characterization of vascular tissue const","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"12 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143858271","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Lattice Energy Reservoir in Metal Halide Perovskites","authors":"Xiaoming Wen, Baohua Jia","doi":"10.1021/accountsmr.5c00047","DOIUrl":"https://doi.org/10.1021/accountsmr.5c00047","url":null,"abstract":"Figure 1. Scheme of lattice energy reservoir as dynamic nanodomain in halide perovskites. Blue LER: before energy storage, red LER: energy accumulation by phonon-lattice coupling, higher potential energy is established over the surrounding. (ph-phonon) Figure 2. (a) Scheme for LER suppress hot carrier cooling. The homojunction with strain of different lattice suppress thermal transport to the surrounding lattice and then induces acoustic-optical phonon upconversion. (b) Proposed phonon dynamics in Perovskites. The labeled phonon dynamic processes are (1) Fröhlich interaction of carriers primarily on the lead-halide framework; (2) relaxation of lead-halide LO phonon, organic sublattice can be excited by phonon–phonon scattering; (3) propagation of acoustic phonon is blocked due to anharmonic phonon–phonon scatterings; (4) upconversion of acoustic phonons; and (5) carrier reheating. (3) Reproduced with permission from ref (3). Copyright 2017 The Authors. Figure 3. PL enhancement in halide perovskites with continuous illumination at the time scale of seconds. PL Intensity (a) and PL decay curves (b) in MAPbI<sub>3</sub> nanoplatelet under continuous illumination (405 nm 200 mW/cm<sup>2</sup>). Figure 4. Schematic photobrightening by LER induced subgap carrier upconversion. (a) Without LER effect before illumination and (c) display a short carrier lifetime. (b) Upon illumination hot LERs form (red regions) and the subgap carrier can be upconverted back to the CB, (d) resulting in a significantly prolonged carrier lifetime. (TS: trapping/metastable states, ph: phonon, e: electron.) Figure 5. Schematic subgap electron upconversion driven by hot LERs under illumination. Figure 6. (a) Time-dependent PL spectra in MAPbBr<sub>3</sub> single crystal under 405 nm excitation at a fluence of 350 mW/cm<sup>2</sup>. (b) Fluorescence intermittency in MAPbBr<sub>3</sub> single grain as a function of time under the continuous excitation of 405 nm. Dr Wen Xiaoming was awarded bachelor’s and master’s degrees from Zhejiang University, and a PhD from Swinburne University, Australia in 2007. From 1989 to 2003, he worked at Yunnan University as full professor and deputy head of department. He has performed research at the University of Melbourne, University of New South Wales, Swinburne University of Technology in Australia and Academia Sinica in Taiwan on ultrafast spectroscopy and photophysics of materials. He is currently a senior researcher and theme leader at RMIT University, focusing on the photophysics of perovskites and photovoltaic applications. Prof Baohua Jia was awarded a PhD from Swinburne University. She is a Fellow of Australian Academy of Technological Sciences and Technologies (FTSE), a Future Fellow of Australian Research Council and Founding Director of Centre for Atomaterials and Nanomanufacturing (CAN) at RMIT University, Australia. Professor Jia serves as Editor-in-Chief for NPJ Nanophotonics. Prof Jia is a Fellow of Optica, and a Fellow of the Inst","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"41 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143836896","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"A Perspective on the Rational Design of Spinel Catalysts for Polysulfide Conversion","authors":"Wen Xie, Qian Wu, Zhichuan J. Xu","doi":"10.1021/accountsmr.5c00092","DOIUrl":"https://doi.org/10.1021/accountsmr.5c00092","url":null,"abstract":"Figure 1. Illustration of normal spinel, inverse spinel, and defected inverse spinel structures. Figure 2. Illustration of d-orbitals splitting in (a) octahedral field and (b) tetrahedral field. Figure 3. Schematic illustration of the role of spin state and M-O covalency in regulating the polysulfide conversion activity of spinel oxides. (a) The role of spin state in regulating the bonding and antibonding states of molecular orbitals between metal cations and sulfur species. (b) The optimized structures of the (111) plane of spinel oxides. The right box shows that one oxygen atom is connected to one tetrahedral cation and two octahedral cations. (c) Illustration of different M<sub>Oct</sub>–O–M<sub>Td</sub> covalencies and their corresponding active sites in spinel oxides. The top box indicates that the M<sub>Td</sub>- active sites are more likely to be generated when the covalency of M<sub>Td</sub>–O is weaker than that of M<sub>Oct</sub>–O. Otherwise, M<sub>Oct</sub>– active sites are more likely to be generated, as shown in the bottom box. [Reproduced with permission from ref (14). Copyright 2020, Springer Nature.] (d) Illustration of the role of M–O covalency in regulating the electron distribution after bond breakage. A weak M–O covalency leads to an unequal distribution of electrons after bond breakage and the generation of two partially ionic parts. In contrast, a strong M–O covalency makes bond breakage more difficult. Only intermediate M–O covalency contributes to the equal distribution of electrons after bond breakage and the exposure of active sites. [Reproduced with permission from ref (14). Copyright 2020, Springer Nature.] Figure 4. Schematic illustration of the design strategies of spinel catalysts. (a) Illustration of site occupancy switch in spinel structures by adjusting the annealing temperature. X indicates anions (e.g., O, S). [Reproduced with permission from ref (3). Copyright 2025, American Chemical Society, Washington, DC.] (b) The role of doping in regulating the valence electrons of metal and lattice sulfur sites of spinel sulfides. [Reproduced with permission from ref (23). Copyright 2025, Wiley-VCH.] (c) The evolution of Co<sup>3+</sup> spin state and the construction of Co–O–Co spin channel. [Reproduced with permission from ref (24). Copyright 2021, Wiley-VCH.] (d) Illustration of the adsorption–conversion process of polysulfides on the surface of CoFeMnO YSNCs. [Reproduced with permission from ref (18). Copyright 2022, Wiley-VCH.] Figure 5. Outlook and perspectives on the rational design of spinel catalysts for polysulfide conversion. The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/accountsmr.5c00092. Additional discussion on spinel structure, cation coordination environment and spin state, and M–O covalency (PDF) A Perspective\u0000on the Rational Design of Spinel Catalysts\u0000for Polysulfide Conversion <span> 2 </span><span> views </span> <span> 0 </span><span> shares </span> <spa","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"50 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143832484","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Advancing Thermal Management Technology for Power Semiconductors through Materials and Interface Engineering","authors":"Man Li, Suixuan Li, Zhihan Zhang, Chuanjin Su, Bryce Wong, Yongjie Hu","doi":"10.1021/accountsmr.4c00349","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00349","url":null,"abstract":"Power semiconductors and chips are essential in modern electronics, driving applications from personal devices and data centers to energy technologies, vehicles, and Internet infrastructure. However, efficient heat dissipation remains a critical challenge, directly affecting their performance, reliability, and lifespan. High-power electronics based on wide- and ultrawide-bandgap semiconductors can exhibit power densities exceeding 10 kW/cm², hundreds of times higher than digital electronics, posing significant thermal management challenges. Addressing this issue requires advanced materials and interface engineering, alongside a comprehensive understanding of materials physics, chemistry, transport dynamics, and various electronic, thermal, and mechanical properties.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"59 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143798531","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"2D Perovskite Oxides toward High-Performance Ultraviolet Photodetection","authors":"Ming Deng, Xiaosheng Fang","doi":"10.1021/accountsmr.5c00014","DOIUrl":"https://doi.org/10.1021/accountsmr.5c00014","url":null,"abstract":"Ultraviolet (UV) light, spanning wavelengths from 10 to 400 nm, is ubiquitous in military, livelihood, and scientific domains. Accurate UV photodetection is therefore essential for monitoring environmental radiation, safeguarding human health, and advancing technological applications in fields such as aerospace, medical science, and ecology. The fabrication of high-performance UV photodetection devices fundamentally depends on the development of high-sensitivity UV photosensitive materials. The evolution of UV photodetection materials has progressed from early wide-bandgap semiconductors like ZnS and ZnSe to third-generation semiconductors such as GaN and Ga₂O₃, and most recently to two-dimensional (2D) wide-bandgap materials that combine exceptional optoelectronic properties with compelling physicochemical properties. Among these, 2D perovskite oxides stand out due to their prominent advantages for UV detection. First, this large family of materials generally features wide bandgaps, strong UV absorption, and high spectral selectivity. Second, the tunable bandgaps of 2D perovskite oxides enable precise detection at specific wavelengths. Third, their excellent processability and flexibility facilitate feasible integration into devices, making them promising candidates for flexible photodetectors. Furthermore, 2D perovskite oxides boast other properties such as high stability, dielectricity, ferroelectricity, and biocompatibility. These characteristics have promoted the blossoming of 2D perovskite oxides for high-performance UV photodetection and are poised to expand their applications in novel functional optoelectronics.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"103 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143745720","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Design and Development of Fire-Safety Materials in Artificial Intelligence Era","authors":"Teng Fu, Yu-Zhong Wang","doi":"10.1021/accountsmr.5c00065","DOIUrl":"https://doi.org/10.1021/accountsmr.5c00065","url":null,"abstract":"Figure 1. (a) Previous methods for deducing mechanism and (b) our proposed novel approach for revealing the real burning behavior and flame-retardant mechanism. Figure 2. (a) Illustration of the previous structure–activity relationship theory and (b) our proposed theoretical flame retardancy model based on the flame-retardant roles. Figure 3. AI-assistant self-iterative, high-throughput, and generalizable flame-retardant material design framework. Traditional flame retardants and flame-retardant polymeric materials struggle to meet the stringent requirements of emerging areas. For instance, fire incidents involving new energy vehicles, extreme wildfires, and hydrogen fuel cells, etc. present extreme conditions with higher temperatures and greater heat flux, demanding enhanced thermal stability and heat shock resistance in flame-retardant polymeric materials. Additionally, materials used in ultrahigh-voltage electrical systems must withstand extreme voltages and large currents, necessitating improved electrical insulation and thermal stability to ensure operational safety and reliability. Some halogen-based and certain phosphorus-based flame retardants are still associated with persistent, bioaccumulative, and toxic (PBT) hazards. (25−27) Future research should prioritize the development of low-toxicity, low-pollution flame-retardant solutions that minimize environmental accumulation risks while preventing the release of hazardous gases or persistent pollutants during combustion. Traditional flame retardants are primarily derived from nonrenewable fossil resources, which conflicts with carbon neutrality and sustainability goals. Future research should explore the use of renewable biomass resources, such as polysaccharides, lignin, and proteins, to develop efficient and low-carbon flame retardants. Flame retardants are typically incorporated into polymeric materials through physical or chemical means, where incorporating flame-retardant elements often complicates waste management by limiting material reuse and increasing environmental impact. (28) Therefore, considering the recyclability of flame-retardant polymeric materials in the initial material design or the physical/chemical/biological recovery of the discarded flame-retardant polymeric materials is necessary to reduce the impact on the environment and improve resource utilization. Figure 4. AI-assistant material design framework applying to flame retardant or flame-retardant materials research. T.F. and Y.-Z.W. discussed the topic and proposed the outline, wrote the draft, and revised the manuscript. Teng Fu received his Ph.D. in polymer chemistry and physics in 2019 from Sichuan University. He joined Professor Yu-Zhong Wang’s group in 2019, and now he is a researcher at Sichuan University. His current research interests are focused on fire-safety materials, devices and apparatus. Yu-Zhong Wang received his Ph.D. from Sichuan University in 1994 and became a Full Professor of Sichuan Universi","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"75 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143745719","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Nanospace Engineering of Metal–Organic Frameworks for Adsorptive Gas Separation","authors":"Lingshan Gong, Shyam Chand Pal, Yingxiang Ye, Shengqian Ma","doi":"10.1021/accountsmr.5c00006","DOIUrl":"https://doi.org/10.1021/accountsmr.5c00006","url":null,"abstract":"Gas separation is a critical process in the industrial production of chemicals, polymers, plastics, and fuels, which traditionally rely on energy-intensive cryogenic distillation techniques. In contrast, adsorptive separation using porous materials has emerged as a promising alternative, presenting substantial potential for energy savings and improved operational efficiency. Among these materials, metal–organic frameworks (MOFs) have garnered considerable attention due to their unique structural and functional characteristics. MOFs are a class of crystalline porous materials constructed from inorganic metal ions or clusters connected by organic linkers through strong coordination bonds. Their precisely engineered architectures create well-defined nanoscale spaces capable of selectively trapping guest molecules. In contrast to traditional porous materials such as zeolites and activated carbons, emerging MOFs not only demonstrate exceptional capabilities for pore regulation and interior modification through nanospace engineering but also hold great promise as a superior platform for the development of high-performance functional materials. By virtue of the isoreticular principle and building unit assembly strategies in MOF chemistry, precise adjustments to pore structures─including pore size, shape, and surface chemistry─can be readily achieved, making them well-suited for addressing the separation of intractable industrial gas mixtures, particularly those with similar sizes and physicochemical properties.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"9 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723696","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Design Strategies, Properties, and Applications toward Cycloarenes and Heterocycloarenes","authors":"Jiangyu Zhu, Rong Zhang, Dongyue An, Yuanhe Gu, Xuefeng Lu, Yunqi Liu","doi":"10.1021/accountsmr.5c00041","DOIUrl":"https://doi.org/10.1021/accountsmr.5c00041","url":null,"abstract":"Cycloarenes, fully benzene-annelated macrocyclic systems with inward-facing carbon–hydrogen bonds, serve as ideal models for defects in graphene, offering great application potential in organic electronics, supramolecular chemistry, and optics. They offer an attractive combination of synthesis challenge, aesthetic appeal, fundamental problems, and potential applications. Initially, the most typical cycloarene, kekulene, was expected to provide a crucial experimental test to determine whether π-electrons are delocalized over the entire molecule or delocalized at the benzenoid rings. This question has captivated synthetic chemists for decades. After numerous failed attempts, Staab and Diederich achieved the first conclusive synthesis of kekulene in 1978. The deshielded inner protons in the <sup>1</sup>H NMR spectrum conclusively demonstrated that the π-electrons in cycloarenes are delocalized at individual benzenoid rings. However, owing to limited synthetic methods, complex reaction routes, and poor solubility of the final products, progress in cycloarene research has been slow. Over the next four decades, only a few contracted or expanded kekulene homologues were reported. Nevertheless, the changes in their chemical structure bring some exciting physicochemical properties. The enlargement of the central ring of kekulene induces a transition from a planar to a saddle-shaped structure, further influencing its electronic and optical properties and unlocking unexpected applications in supramolecular chemistry. Therefore, developing new rational synthetic methods to controllably synthesize structurally diverse cycloarenes is crucial. With the continuous development of synthetic science, in recent years, some functional cycloarenes and heteroatom-embedded heterocycloarenes have been reported. Owing to their unique topological structures, well-defined cavities, and large cyclic conjugated systems, these (hetero)cycloarenes have been applied in fields such as supramolecular chemistry, organic field-effect transistors, and solar cells. However, the limited understanding of the structure–property relationship in (hetero)cycloarenes poses a formidable challenge to their custom synthesis for specific functions. Herein, we review our efforts in the design, synthesis, and applications of cycloarenes and heterocycloarenes. First, we summarize four representative synthetic methods for cycloarenes. Subsequently, we present a comprehensive overview of three molecular design strategies: π-extension, heteroatom embedding, and acceptor moiety insertion, to achieve the molecular structure diversity of cycloarenes. Then, we highlight their synthetic methods, geometries, fundamental optoelectronic properties, and unique applications in ultranarrowband emission, organic transistor devices, and supramolecular chemistry. We also delve into the intrinsic correlations among structures, properties, and applications of these cycloarenes and heterocycloarenes. Finally, we envis","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"183 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143713782","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}