Accounts of materials research最新文献

{"title":"Data-Driven Combinatorial Design of Highly Energetic Materials","authors":"Linyuan Wen, Yinglei Wang* and Yingzhe Liu*, ","doi":"10.1021/accountsmr.4c0023010.1021/accountsmr.4c00230","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00230https://doi.org/10.1021/accountsmr.4c00230","url":null,"abstract":"<p >In this Account, we present a comprehensive overview of recent advancements in applying data-driven combinatorial design for developing novel high-energy-density materials. Initially, we outline the progress in energetic materials (EMs) development within the framework of the four scientific paradigms, with particular emphasis on the opportunities afforded by the evolution of computer and data science, which has propelled the theoretical design of EMs into a new era of data-driven development. We then discuss the structural features of typical EMs such as TNT, RDX, HMX, and CL-20, namely, a “scaffolds + functional groups” characteristic, underscoring the efficacy of the combinatorial design approach in constructing novel EMs. It has been discerned that those modifications to the scaffolds are the primary driving force behind the enhancement of EMs’ properties.</p><p >Subsequently, we introduce three distinct data-driven design strategies for EMs, each with a different approach to scaffold construction. These strategies are as follows: (1) the known scaffold strategy to identify fused cyclic scaffolds containing oxazole or oxadiazole structures from other fields via database screening and employ a high-throughput combinatorial approach with functional groups to design oxazole (and oxadiazole)-based fused cyclic EMs; (2) the semiknown scaffold strategy to construct semiknown scaffolds by integrating known scaffolds and realize the design of bridged cyclic EMs through a high-throughput combination of functional groups; (3) the unknown scaffold strategy to build caged structural models for quantitative characterization, high-throughput screening caged scaffolds from the database, construct unknown caged scaffolds by substituting atoms or substructures, and combine functional groups to design zero oxygen balance caged EMs. Employing the proposed strategies, the design capacity for EMs reaches an impressive scale of 10<sup>7</sup> molecules, significantly increasing the probability of obtaining high-performance EMs. Furthermore, the incorporation of property assessment models based on machine learning and density functional theory has achieved a balance between computational accuracy and computational speed. Statistical analysis of the virtual screening has revealed the advantages of bicyclic tri- and tetrasubstituted position scaffolds in the construction of high-energy and easily synthesizable fused cyclic EMs. Additionally, the proposed strategies have been successfully applied to design multifunctional modular energetic materials, resulting in the successful synthesis of three target compounds, validating the effectiveness of data-driven combinatorial design approaches.</p><p >Lastly, we discuss the current state of high-throughput combinatorial design and, in light of the multifaceted criteria required for the design of EMs, explore the feasibility of multiobjective optimization methods such as Pareto optimization. Moreover, we envision the ap","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 1","pages":"64–76 64–76"},"PeriodicalIF":14.0,"publicationDate":"2024-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143091872","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":"Data-Driven Combinatorial Design of Highly Energetic Materials","authors":"Linyuan Wen, Yinglei Wang, Yingzhe Liu","doi":"10.1021/accountsmr.4c00230","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00230","url":null,"abstract":"In this Account, we present a comprehensive overview of recent advancements in applying data-driven combinatorial design for developing novel high-energy-density materials. Initially, we outline the progress in energetic materials (EMs) development within the framework of the four scientific paradigms, with particular emphasis on the opportunities afforded by the evolution of computer and data science, which has propelled the theoretical design of EMs into a new era of data-driven development. We then discuss the structural features of typical EMs such as TNT, RDX, HMX, and CL-20, namely, a “scaffolds + functional groups” characteristic, underscoring the efficacy of the combinatorial design approach in constructing novel EMs. It has been discerned that those modifications to the scaffolds are the primary driving force behind the enhancement of EMs’ properties.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"67 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142579959","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":"UCl3-Type Solid Electrolytes: Fast Ionic Conduction and Enhanced Electrode Compatibility","authors":"Yi-Chen Yin, Jin-Da Luo and Hong-Bin Yao*, ","doi":"10.1021/accountsmr.4c0007310.1021/accountsmr.4c00073","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00073https://doi.org/10.1021/accountsmr.4c00073","url":null,"abstract":"","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 1","pages":"1–5 1–5"},"PeriodicalIF":14.0,"publicationDate":"2024-10-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143091818","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":"UCl3-Type Solid Electrolytes: Fast Ionic Conduction and Enhanced Electrode Compatibility","authors":"Yi-Chen Yin, Jin-Da Luo, Hong-Bin Yao","doi":"10.1021/accountsmr.4c00073","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00073","url":null,"abstract":"Figure 1. Origin of the superionic conduction of UCl<sub>3</sub>-type SEs with the non-close-packed framework. (a) Li<sup>+</sup> probability density, represented by green isosurfaces from AIMD simulations in the vacancy-contained LaCl<sub>3</sub> lattice. Reproduced with permission from reference (21). Copyright 2023 the author(s), under exclusive license to Springer Nature Limited. (b) Schematic of diffusion channel. Reproduced with permission from reference (24). Copyright 2024 John Wiley and Sons. (c) Diffusion channel size distribution of Li<sub>3</sub>YCl<sub>6</sub>, Li<sub>3</sub>InCl<sub>6</sub>, LiNbOCl<sub>4</sub>, and UCl<sub>3</sub>-type Li<sub>0.388</sub>Ta<sub>0.238</sub>La<sub>0.475</sub>Cl<sub>3</sub> (LTLC). Reproduced with permission from reference (24). Copyright 2024 John Wiley and Sons. (d) Schematic illustration of the effects of inherent distortion on energy landscape. Reproduced with permission from reference (24). Copyright 2024 John Wiley and Sons. Figure 2. Ionic conductivity values at room temperature of crystalline chloride SEs, including conventional close-packed Li<sub><i>x</i></sub>M<sub><i>y</i></sub>Cl<sub><i>n</i></sub> SEs and UCl<sub>3</sub>-type LaCl<sub>3</sub>-based SEs. (1−4,10−14,21) Reproduced with permission from reference (21). Copyright 2023 the author(s), under exclusive license to Springer Nature Limited. Figure 3. UCl<sub>3</sub>-type SEs with a more stable interface toward lithium metal anode. (a) Depth-dependent La 3d<sub>5/2</sub> X-ray photoelectron spectroscopy (XPS) spectra of the interface of Li<sub>0.388</sub>Ta<sub>0.238</sub>La<sub>0.475</sub>Cl<sub>3</sub> SE after 50 h of cycling. Reproduced with permission from reference (21). Copyright 2023 by Springer Nature Limited. (b) Depth-dependent La 3d<sub>5/2</sub> XPS spectra of the interface of Li<sub>0.388</sub>Ta<sub>0.238</sub>La<sub>0.475</sub>Cl<sub>3</sub> SE after 50 h of cycling. Reproduced with permission from reference (21). Copyright 2023 the author(s), under exclusive license to Springer Nature Limited. (c) Voltage profile of a Li/Li<sub>0.388</sub>Ta<sub>0.238</sub>La<sub>0.475</sub>Cl<sub>3</sub>/Li symmetric cell cycled under a current density of 0.2 mA cm<sup>–2</sup> and areal capacity of 1 mAh cm<sup>–2</sup> at 30 °C. Insets: corresponding magnified voltage profiles indicate steady Li plating/stripping voltages. Reproduced with permission from reference (21). Copyright 2023 the author(s), under exclusive license to Springer Nature Limited. (d) La 3d<sub>5/2</sub> (left) and Zr 3d (right) XPS spectra of the Li|Li<sub>0.8</sub>Zr<sub>0.25</sub>La<sub>0.5</sub>Cl<sub>2.7</sub>O<sub>0.3</sub> interface after 500 h cycling, respectively. Reproduced with permission from reference (23). Copyright 2024 Royal Society of Chemistry. (e) Comparison of the critical current density (CCD) of Li metal symmetric cells with different solid electrolytes (Ga-LLZO (Li<sub>6.4</sub>Ga<sub>0.2</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub>); ","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"12 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-10-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142556497","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":"Methodologies to Improve the Stability of High-Efficiency Perovskite Solar Cells","authors":"Sanjay Sandhu, Nam-Gyu Park","doi":"10.1021/accountsmr.4c00237","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00237","url":null,"abstract":"Organic–inorganic lead halide perovskite solar cells (PSCs) have attracted significant interest from the photovoltaic (PV) community due to suitable optoelectronic properties, low manufacturing cost, and tremendous PV performance with a certified power conversion efficiency (PCE) of up to 26.5%. However, long-term operational stability should be guaranteed for future commercialization. Over the past decade, intensive research has focused on improving the PV performance and device stability through the development of novel charge transport materials, additive engineering, compositional engineering, interfacial modifications, and the synthesis of perovskite single crystals. In this Account, we provide a comprehensive overview of recent progress and research directions in the fabrication of highly efficient and stable PSCs, including key outcomes from our group. We begin by highlighting the critical challenges and their causes that are detrimental to the development of stable PSCs. We then discuss the fundamentals of halide perovskites including their optical and structural properties. This is followed by a description of the fabrication methods for perovskite crystals, films, and various device architectures. Next, we introduced target-oriented key strategies such as developing high-quality single crystals for redissolution as a perovskite precursor to fabricate phase-stable and reproducible PSCs, along with reduced material costs, employing multifunctional additives to get uniform, robust, and stable perovskite films, and interfacial engineering techniques for effective surface and buried interface defect passivation to improve charge transport and long-term stability. Finally, we conclude with a critical assessment and perspective on the future development of PSCs. This Account will provide valuable insights into the current state-of-the-art PSCs and promising strategies tailored to specific roles that can be combined to manipulate the perovskite structure for novel outcomes and further advancements.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"5 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142542226","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":"Extremely Downsized Materials: Ball-Milling-Enabled Universal Production and Size-Reduction-Induced Performance Enhancement","authors":"Ce Zhao, Liuyang Xiao, Zhexue Chen and Yong Zhang*, ","doi":"10.1021/accountsmr.4c0030610.1021/accountsmr.4c00306","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00306https://doi.org/10.1021/accountsmr.4c00306","url":null,"abstract":"<p >Extremely downsized (including quantum-sized and subnanometer-sized) materials with sizes between atoms and nanoparticles have attracted tremendous attention thanks to their unique structures and exotic physical and chemical properties. Such unusual materials will induce a range of enhanced performances compared with their nanoscale and bulk counterparts, which can be beneficial to driving advancements of materials science as well as nanoscience and nanotechnology. However, it is quite challenging to prepare extremely downsized materials due to their ultrasmall sizes and ultralarge surfaces. Up to now, a variety of strategies have been explored for the preparation of extremely downsized materials, among which the basic categories are top-down and bottom-up methods. The former generally tailors bulk materials into downsized nanomaterials by physical routes, while the latter usually involves chemical (solution) processes to synthesize nanomaterials. During past decades, most efforts have been devoted to bottom-up methods for the synthesis of extremely downsized materials (e.g., colloidal quantum dots, sub-nanometer-sized materials, clusters, and supermolecules). Meanwhile, the production of extremely downsized materials through top-down methods is far from satisfactory, limited by their low manufacturing capacities and relatively expensive facilities. Note that nanomaterials produced by top-down physical methods exhibit entirely exposed surface/edge lattices, while the surface/edge lattices synthesized by bottom-up chemical methods are protected by ligands, making the surface/edge effects greatly obscured. Undoubtedly, exploiting a robust strategy to produce extremely downsized materials with maximized exposed lattices by all-physical top-down methods is required and desired. Our group has been focusing on all-physical production and extreme performances of extremely downsized materials since 2015. We have developed a universal and scalable strategy (i.e., the combination of silica-assisted ball-milling and sonication-assisted solvent exfoliation and treatment) for the all-physical production of quantum-sized materials. A series of quantum-sized materials with intrinsic characteristics have been produced, pushing forward the establishment of a complete database/library. Recently, two-stage silica-assisted ball-milling has been employed to realize the universal production of sub-nanometer-sized materials with entirely exposed and broken intrinsic lattices, suggesting that the top-down fabrication limit has reached the subnanometer (single-lattice) scale. Enhanced performances are demonstrated in both quantum-sized and sub-nanometer-sized materials because of their numerous broken lattices on surfaces/edges.</p><p >In this Account, we emphasize the preparation strategies and enhanced performances for extremely downsized materials, particularly highlighting the contributions of our research group in the past few years. The representative key adv","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"5 12","pages":"1583–1597 1583–1597"},"PeriodicalIF":14.0,"publicationDate":"2024-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143127564","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":"The Microenvironment Frontier for Electrochemical CO2 Conversion","authors":"Andrew B. Wong*, ","doi":"10.1021/accountsmr.4c0029410.1021/accountsmr.4c00294","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00294https://doi.org/10.1021/accountsmr.4c00294","url":null,"abstract":"","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"5 12","pages":"1453–1456 1453–1456"},"PeriodicalIF":14.0,"publicationDate":"2024-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/accountsmr.4c00294","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143127706","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"The Microenvironment Frontier for Electrochemical CO2 Conversion","authors":"Andrew B. Wong","doi":"10.1021/accountsmr.4c00294","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00294","url":null,"abstract":"low CO<sub>2</sub> solubility in aqueous conditions the delicate balance between the delivery of essential proton donors for CO<sub>2</sub>RR versus the strong tendency to convert donated protons to H<sub>2</sub> via the competing hydrogen evolution reaction (HER) the delicate balance between reaction pathways toward multiple CO<sub>2</sub>RR products dynamic changes in local pH, ion concentrations, hydrophobicity, and active sites in response to phenomena such as carbonate formation and restructuring of electrocatalysts Figure 1. Schematic overview of CO<sub>2</sub>RR microenvironment effects. (a) Microenvironment impact on CO<sub>2</sub>RR performance. (b) Microenvironment considerations: experimental conditions, electrocatalyst characteristics, and electrolyte characteristics. (c) Description of the activity and activity coefficient for CO<sub>2</sub>, CO, and H<sub>2</sub>O (or other proton donors). Activity is the lens through which to understand numerous phenomena within the CO<sub>2</sub>RR microenvironment Figure 2. Schematic overview for macroscale, microscale, and nanoscale effects on planar (a–c) and porous (d–f) electrodes. First, the activity coefficient and concentration terms offer a helpful parameter space to compare the effects of various interventions and adjustments to the microenvironment that had previously been difficult to compare based on objective measures (Figure 1b). Second, this approach highlights the importance of improving our understanding of the relative contributions of three-phase (gas–liquid–solid) and larger area two-phase (liquid–solid) interfaces on CO<sub>2</sub>RR, which has attracted recent attention. (12,13) Third, this understanding highlights the importance of developing new <i>in situ</i> and <i>in operando</i> analytical techniques to probe the local distributions of CO<sub>2</sub>, CO, and H<sub>2</sub>O under reaction conditions. Attenuated total reflectance surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) has already shown promise for quantifying bound versus free water during CO<sub>2</sub>RR. (13) What are strategies to extend recent fundamental developments on controlling water activity to improve CO<sub>2</sub>RR performance at high current densities? How can we use the microenvironment to explore electrochemical strategies to simultaneously accomplish CO<sub>2</sub> capture and conversion? Based on the historical development of CO<sub>2</sub>RR approaches, can we or should we adopt new materials for CO<sub>2</sub>RR GDLs and ionomers (typically materials developed for other chemical transformations with different requirements) to specialize in CO<sub>2</sub>RR’s requirements? In CO<sub>2</sub>RR, what is the structure of the three-phase gas–liquid–solid and other interfaces under reaction conditions? Leveraging the microenvironment, how can CO<sub>2</sub> be used to make higher-value products or products that can integrate into the economy to achieve net negative CO<sub>2</sub> ","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"16 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142542229","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":"Methodologies to Improve the Stability of High-Efficiency Perovskite Solar Cells","authors":"Sanjay Sandhu,&nbsp; and ,&nbsp;Nam-Gyu Park*,&nbsp;","doi":"10.1021/accountsmr.4c0023710.1021/accountsmr.4c00237","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00237https://doi.org/10.1021/accountsmr.4c00237","url":null,"abstract":"<p >Organic–inorganic lead halide perovskite solar cells (PSCs) have attracted significant interest from the photovoltaic (PV) community due to suitable optoelectronic properties, low manufacturing cost, and tremendous PV performance with a certified power conversion efficiency (PCE) of up to 26.5%. However, long-term operational stability should be guaranteed for future commercialization. Over the past decade, intensive research has focused on improving the PV performance and device stability through the development of novel charge transport materials, additive engineering, compositional engineering, interfacial modifications, and the synthesis of perovskite single crystals. In this Account, we provide a comprehensive overview of recent progress and research directions in the fabrication of highly efficient and stable PSCs, including key outcomes from our group. We begin by highlighting the critical challenges and their causes that are detrimental to the development of stable PSCs. We then discuss the fundamentals of halide perovskites including their optical and structural properties. This is followed by a description of the fabrication methods for perovskite crystals, films, and various device architectures. Next, we introduced target-oriented key strategies such as developing high-quality single crystals for redissolution as a perovskite precursor to fabricate phase-stable and reproducible PSCs, along with reduced material costs, employing multifunctional additives to get uniform, robust, and stable perovskite films, and interfacial engineering techniques for effective surface and buried interface defect passivation to improve charge transport and long-term stability. Finally, we conclude with a critical assessment and perspective on the future development of PSCs. This Account will provide valuable insights into the current state-of-the-art PSCs and promising strategies tailored to specific roles that can be combined to manipulate the perovskite structure for novel outcomes and further advancements.</p>","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"5 12","pages":"1544–1557 1544–1557"},"PeriodicalIF":14.0,"publicationDate":"2024-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143127707","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":"Extremely Downsized Materials: Ball-Milling-Enabled Universal Production and Size-Reduction-Induced Performance Enhancement","authors":"Ce Zhao, Liuyang Xiao, Zhexue Chen, Yong Zhang","doi":"10.1021/accountsmr.4c00306","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00306","url":null,"abstract":"Extremely downsized (including quantum-sized and subnanometer-sized) materials with sizes between atoms and nanoparticles have attracted tremendous attention thanks to their unique structures and exotic physical and chemical properties. Such unusual materials will induce a range of enhanced performances compared with their nanoscale and bulk counterparts, which can be beneficial to driving advancements of materials science as well as nanoscience and nanotechnology. However, it is quite challenging to prepare extremely downsized materials due to their ultrasmall sizes and ultralarge surfaces. Up to now, a variety of strategies have been explored for the preparation of extremely downsized materials, among which the basic categories are top-down and bottom-up methods. The former generally tailors bulk materials into downsized nanomaterials by physical routes, while the latter usually involves chemical (solution) processes to synthesize nanomaterials. During past decades, most efforts have been devoted to bottom-up methods for the synthesis of extremely downsized materials (e.g., colloidal quantum dots, sub-nanometer-sized materials, clusters, and supermolecules). Meanwhile, the production of extremely downsized materials through top-down methods is far from satisfactory, limited by their low manufacturing capacities and relatively expensive facilities. Note that nanomaterials produced by top-down physical methods exhibit entirely exposed surface/edge lattices, while the surface/edge lattices synthesized by bottom-up chemical methods are protected by ligands, making the surface/edge effects greatly obscured. Undoubtedly, exploiting a robust strategy to produce extremely downsized materials with maximized exposed lattices by all-physical top-down methods is required and desired. Our group has been focusing on all-physical production and extreme performances of extremely downsized materials since 2015. We have developed a universal and scalable strategy (i.e., the combination of silica-assisted ball-milling and sonication-assisted solvent exfoliation and treatment) for the all-physical production of quantum-sized materials. A series of quantum-sized materials with intrinsic characteristics have been produced, pushing forward the establishment of a complete database/library. Recently, two-stage silica-assisted ball-milling has been employed to realize the universal production of sub-nanometer-sized materials with entirely exposed and broken intrinsic lattices, suggesting that the top-down fabrication limit has reached the subnanometer (single-lattice) scale. Enhanced performances are demonstrated in both quantum-sized and sub-nanometer-sized materials because of their numerous broken lattices on surfaces/edges.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"135 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142542228","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}