{"title":"Diverse Magnetic Chains in Inorganic Compounds","authors":"Larisa V. Shvanskaya, Alexander N. Vasiliev","doi":"10.1021/accountsmr.4c00083","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00083","url":null,"abstract":"In both inorganic and metal–organic compounds, transition metals surrounded by ligands form regular or distorted polyhedra, which can be either isolated or interconnected. Distortion of the polyhedron can be caused by the degeneracy in the population of atomic or molecular orbitals, which can be removed by the cooperative Jahn–Teller effect. This effect is often accompanied by the formation of low-dimensional magnetic structures, of which we will consider only chain, or quasi-one-dimensional, magnetic compounds variety. Magnetic chains are formed when transition metal polyhedra bond through a vertex, edge, or face. Moreover, the magnetic entities can be coupled through various nonmagnetic units like NO<sub>3</sub>, SiO<sub>4</sub>, <i>Pn</i>O<sub>3</sub> or <i>Pn</i>O<sub>4</sub>, <i>Ch</i>O<sub>3</sub> or <i>Ch</i>O<sub>4</sub>, where <i>Pn</i> is the pnictide and <i>Ch</i> is the chalcogen. In most cases, the local environment of the transition metal is represented by oxygen and/or halogens. The prevailing number of chain systems is based on 3<i>d</i> transition metals, albeit 4<i>d</i> and 5<i>d</i> systems attract more and more attention. Mixed 3<i>d</i>–4<i>f</i> single chain magnets became popular objects in metal–organic chemistry.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"27 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141309298","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":"Computational Design of Sorbent Materials for Per- and Polyfluoroalkyl Substances (PFAS) Remediation","authors":"Boran Ma","doi":"10.1021/accountsmr.4c00142","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00142","url":null,"abstract":"Figure 1. Number of publications from 2019 to 2023 found on Web of Science by searching PFAS-related keywords. Figure 2. Schematic of potential design parameters (e.g., thickness, surface roughness, nanoconfinement, and surface functionalization) for sorbent materials for PFAS adsorption and removal. <b>Boran Ma</b> is an Assistant Professor in the School of Polymer Science and Engineering at the University of Southern Mississippi. Prior to starting her independent career in January 2023, she was a postdoctoral associate at Duke University. She received her PhD in Materials Science and Engineering from Northwestern University in 2019 and her BEng in Materials Science and Engineering from Harbin Institute of Technology in 2014. The Ma Research Lab focuses on computation- and data-driven research of polymeric materials and systems for energy and sustainability applications. The author thanks the Director of the School of Polymer Science and Engineering, the Dean of the College of Arts and Sciences, and the Vice President for Research, all at the University of Southern Mississippi, for their support with generous start-up funds. This article references 15 other publications. This article has not yet been cited by other publications. Figure 1. Number of publications from 2019 to 2023 found on Web of Science by searching PFAS-related keywords. Figure 2. Schematic of potential design parameters (e.g., thickness, surface roughness, nanoconfinement, and surface functionalization) for sorbent materials for PFAS adsorption and removal. This article references 15 other publications.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"94 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-06-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141509908","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":"Computational Design of Sorbent Materials for Per- and Polyfluoroalkyl Substances (PFAS) Remediation","authors":"Boran Ma*, ","doi":"10.1021/accountsmr.4c0014210.1021/accountsmr.4c00142","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00142https://doi.org/10.1021/accountsmr.4c00142","url":null,"abstract":"","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"5 7","pages":"772–774 772–774"},"PeriodicalIF":14.0,"publicationDate":"2024-06-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/accountsmr.4c00142","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141959323","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}
Yingzhen Wei, Jingyi Feng, Buyuan Guan and Jihong Yu*,
{"title":"Structural Engineering of Hierarchical Zeolite-Based Catalysts","authors":"Yingzhen Wei, Jingyi Feng, Buyuan Guan and Jihong Yu*, ","doi":"10.1021/accountsmr.4c0007610.1021/accountsmr.4c00076","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00076https://doi.org/10.1021/accountsmr.4c00076","url":null,"abstract":"<p >Zeolites are important inorganic crystalline materials with unique microporous structures, intrinsic acidic sites, and high hydrothermal stabilities, which have been widely used in the catalytic field such as methanol conversion, catalytic cracking, and NO<sub><i>x</i></sub> removal. Although the regular channel structures afford zeolite catalysts excellent shape selectivity, the diffusion hindrance caused by the narrow pores (typically less than 2 nm) significantly limits their catalytic activities and lifetimes. Introducing secondary mesopores (2–50 nm) and/or macropores (>50 nm) into the micropore system of zeolites can significantly reduce diffusion limitations and enhance the exposure of more active sites. On the other hand, the delicate integration of microporous zeolites with other functional porous materials into hierarchical heterostructures could offer enhanced or even new catalytic properties that cannot be achieved with single hierarchical zeolite catalysts. For example, tailored meso-/macroporous materials can be combined with zeolites to create composite heterostructures with controllable hierarchical architectures and spatial distributions of functional components from the nano-/microscale to the macroscale in purposeful ways, thus extending their applicability to more intricate and broad heterogeneous catalytic systems. Therefore, the rational design and synthesis of hierarchical zeolite-based materials, spanning from multilevel nanostructures to monoliths, with fascinating catalytic properties hold great significance in the development of efficient energy and environmental catalytic processes.</p><p >In this Account, we summarize our efforts devoted to the structural engineering of zeolite-based catalysts with hierarchical architectures. At first, we present a brief summary of synthesis strategies of hierarchical zeolite-based materials in the nano-/microscale with particular emphasis on innovative approaches we have recently developed, including kinetic-modulated crystallization, anisotropic-kinetics transformation, and regioselective surface assembly strategies. Notably, we also explore the application of three-dimensional (3D) printing technology as a customizable and scalable manufacturing method to fabricate monolithic catalysts with industrialization potential at the macroscale by superassembly of nano-/microsized zeolite and other functional porous materials as structural subunits. Subsequently, we discuss several representative hierarchical zeolite-based catalysts including hierarchical zeolites, along with zeolite@layered double hydroxide (LDH), zeolite@mesoporous carbon, and zeolite@porous SiO<sub>2</sub> hierarchically porous heterostructures. These hierarchical zeolite-based catalysts with multilevel pore structures and chemical composition distributions exhibit enhanced catalytic performances in various catalytic reactions. Finally, we point out the remaining challenges and future perspectives for the fabricat","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"5 7","pages":"857–871 857–871"},"PeriodicalIF":14.0,"publicationDate":"2024-06-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141955630","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":"Structural Engineering of Hierarchical Zeolite-Based Catalysts","authors":"Yingzhen Wei, Jingyi Feng, Buyuan Guan, Jihong Yu","doi":"10.1021/accountsmr.4c00076","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00076","url":null,"abstract":"Zeolites are important inorganic crystalline materials with unique microporous structures, intrinsic acidic sites, and high hydrothermal stabilities, which have been widely used in the catalytic field such as methanol conversion, catalytic cracking, and NO<sub><i>x</i></sub> removal. Although the regular channel structures afford zeolite catalysts excellent shape selectivity, the diffusion hindrance caused by the narrow pores (typically less than 2 nm) significantly limits their catalytic activities and lifetimes. Introducing secondary mesopores (2–50 nm) and/or macropores (>50 nm) into the micropore system of zeolites can significantly reduce diffusion limitations and enhance the exposure of more active sites. On the other hand, the delicate integration of microporous zeolites with other functional porous materials into hierarchical heterostructures could offer enhanced or even new catalytic properties that cannot be achieved with single hierarchical zeolite catalysts. For example, tailored meso-/macroporous materials can be combined with zeolites to create composite heterostructures with controllable hierarchical architectures and spatial distributions of functional components from the nano-/microscale to the macroscale in purposeful ways, thus extending their applicability to more intricate and broad heterogeneous catalytic systems. Therefore, the rational design and synthesis of hierarchical zeolite-based materials, spanning from multilevel nanostructures to monoliths, with fascinating catalytic properties hold great significance in the development of efficient energy and environmental catalytic processes.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"2013 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-06-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141246409","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}
Qianqian Xu, Qing Li, Haipeng Yu, Jian Li and Wenshuai Chen*,
{"title":"Nanocellulose Building Block for the Construction of Hygroscopic Aerogels","authors":"Qianqian Xu, Qing Li, Haipeng Yu, Jian Li and Wenshuai Chen*, ","doi":"10.1021/accountsmr.4c0008510.1021/accountsmr.4c00085","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00085https://doi.org/10.1021/accountsmr.4c00085","url":null,"abstract":"<p >Moisture, a ubiquitous component in the atmosphere, offers a wealth of opportunities and presents various challenges in our daily lives and the surrounding environment. On the one hand, people can obtain clean drinking water from air and use the moisture to create new energy sources. On the other hand, many people across the world still face long-term drought or damp hazards caused by extremely low or high humidity. Therefore, the sustainable management of atmospheric moisture is crucial for creating a comfortable lifestyle for humanity. Cooling condensation and desiccant drying are established methods for adjusting atmospheric humidity, yet they still face a range of challenges including energy usage, efficiency levels, operational simplicity, and broad applicability. Recently, hygroscopic materials, which can regulate environmental humidity, material performance, and collect water by adsorbing moisture from air and managing the adsorbed moisture, are attracting increasing attention. For the efficient and scalable production of hygroscopic materials, it is fundamental to carefully select and ingeniously assemble the building blocks that dictate their performance.</p><p >Nanocellulose, an emerging biopolymer nanofiber, is predominantly biosynthesized by higher plants, positioning it as an ideal building block for constructing hygroscopic materials. Its appeal lies in the sustainable and plentiful nature of its raw materials, coupled with its distinctive one-dimensional nanostructure, abundant surface hydroxyl groups, and outstanding mechanical strength. Furthermore, its capacity to readily assemble into diverse structures through straightforward processes makes it a compelling choice for advancing the development of next-generation biopolymer-based hygroscopic materials. Lightweight and self-standing hygroscopic aerogels can be fabricated after integration nanocellulose with various hygroscopic salts through a series of methods. As well as adsorbing atmospheric moisture, they can transform gaseous water into liquid water, and transport it to their interiors for storage. Water evaporation and release are realized by simply exposing the moisture-adsorbed aerogels to sunlight. These properties qualify plant material-derived hygroscopic aerogels as sustainable moisture management platform that are useful in many fields.</p><p >In the present Account, we describe recent progress in the use of nanocellulose as a building block for constructing hygroscopic aerogels. We will begin with the introduction of some fundamental knowledge about nanocellulose, with a specific focus on the extraction of nanofibrillated cellulose, a kind of nanocellulose mainly individualized from wood powders by chemical pretreatment combined with mechanical nanofibrillation, as well as its nanostructure characteristics. We will then describe the methods for manufacturing various types of nanocellulose hygroscopic aerogels and their hierarchical structures. Subsequently, we w","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"5 7","pages":"846–856 846–856"},"PeriodicalIF":14.0,"publicationDate":"2024-05-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141956676","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":"Nanocellulose Building Block for the Construction of Hygroscopic Aerogels","authors":"Qianqian Xu, Qing Li, Haipeng Yu, Jian Li, Wenshuai Chen","doi":"10.1021/accountsmr.4c00085","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00085","url":null,"abstract":"Moisture, a ubiquitous component in the atmosphere, offers a wealth of opportunities and presents various challenges in our daily lives and the surrounding environment. On the one hand, people can obtain clean drinking water from air and use the moisture to create new energy sources. On the other hand, many people across the world still face long-term drought or damp hazards caused by extremely low or high humidity. Therefore, the sustainable management of atmospheric moisture is crucial for creating a comfortable lifestyle for humanity. Cooling condensation and desiccant drying are established methods for adjusting atmospheric humidity, yet they still face a range of challenges including energy usage, efficiency levels, operational simplicity, and broad applicability. Recently, hygroscopic materials, which can regulate environmental humidity, material performance, and collect water by adsorbing moisture from air and managing the adsorbed moisture, are attracting increasing attention. For the efficient and scalable production of hygroscopic materials, it is fundamental to carefully select and ingeniously assemble the building blocks that dictate their performance.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"48 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-05-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140954451","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}
Zhong-Qiu Li, Li-Qiu Huang, Kang Wang and Xing-Hua Xia*,
{"title":"Developing Solid-State Single-, Arrayed-, and Composite-Nanopore Sensors for Biochemical Sensing Applications","authors":"Zhong-Qiu Li, Li-Qiu Huang, Kang Wang and Xing-Hua Xia*, ","doi":"10.1021/accountsmr.4c00090","DOIUrl":"10.1021/accountsmr.4c00090","url":null,"abstract":"<p >Ions, small molecules, and biomacromolecules are important components of the human body. They usually play important roles in various physiological and pathological events, showing a close relationship with human health. However, due to the ultralow concentrations of these substances and the presence of interfering chemicals, accurate and reliable measurement of these ions and molecules remains a huge challenge. Nanopore sensors, which combine nanofluidic and electrochemical technologies, have received a great deal of attention in recent years. Nanopore sensing is generally realized by measuring the electrochemical behaviors of ions in nanopores, which endows this technique with the advantages of high sensitivity, fast response, high sampling frequency, and experimental simplicity. In addition, owing to the confinement effect, the interaction between analytes and the nanopore is greatly enhanced, which can further improve the sensing sensitivity, even achieving single-entity analysis. With the development of materials science, micro/nanoprocessing technologies, and mass transport theories at the nanoscale, nanopore sensors have established themselves as a promising tool for the analysis of ions, biomolecules, and nanoparticles. Nanopore materials, as the core of nanopore sensors, can be classified into three categories based on the pore structure: single nanopores, arrayed nanopores, and composite nanopores. Single nanopores include two-dimensional (2D) material based single nanopores and glass/quartz nanopipettes. The single-pore structure can offer high sensitivity and spatial resolution, making single nanopores suitable for single-entity analysis. Arrayed nanopores consist of a large number of orderly arranged pores, generally including polymer nanopores and metal oxide nanopores. Arrayed-nanopore sensors possess advantages, including easy preparation, low cost, and high throughput, making them widely applicable in biochemical and environmental analysis. Composite nanopores, on the other hand, combine nanopores with other materials, such as conductive polymers and plasmonic metals, which can further enhance the sensitivity and accuracy of nanopore sensing. Through introducing recognition elements into these nanopores, the interaction between the analyte and the recognition elements can produce predictable changes in the nanopore properties, such as diameter, pore shape, surface charge, and wettability, resulting in readable changes in ion-current signals.</p><p >In this Account, we summarize the recent advancements in nanopore materials, nanopore-sensing mechanisms, and practical nanopore sensing applications, which are mainly based on work published by our group. We first briefly introduce single-, arrayed-, and composite-nanopore materials and their corresponding fabrication methods and then summarize the functionalization techniques employed to incorporate recognition sites within the nanopores. Then, we provide a glimpse of the fundam","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"5 6","pages":"761–771"},"PeriodicalIF":14.0,"publicationDate":"2024-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140949834","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}
Wei Shen, Pengfei Da, Linchuan Guo, Pinxian Xi* and Chun-Hua Yan*,
{"title":"Rare Earth Interface Structure Materials: Synthesis, Applications, and Mechanisms","authors":"Wei Shen, Pengfei Da, Linchuan Guo, Pinxian Xi* and Chun-Hua Yan*, ","doi":"10.1021/accountsmr.4c00061","DOIUrl":"10.1021/accountsmr.4c00061","url":null,"abstract":"<p >Rare earth interface structure materials (RE-ISM) play a crucial role in the field of inorganic synthesis and provide an effective means of achieving the refined utilization of rare earth elements. By capitalizing on the unique properties of rare earth, these materials are designed for functional applications at interfaces. Given the escalating energy and environmental concerns, there is an urgent need to expedite the development of efficient pathways for clean energy storage and conversion. Electrocatalytic conversion of an energetic small molecule is an efficient way of energy storage and conversion with clean energy as the carrier. However, the development of catalysts is often constrained by limitations in the catalyst system and a lack of clarity regarding synthesis and reaction processes. It provides new opportunities for the design of energetic small molecule catalytic materials by developing RE-ISM and analyzing the dynamic evolution process across time and space dimensions.</p><p >In this Account, we mainly focus on the research progress in the synthesis, application, and mechanism of RE-ISM in order to effectively design high-performance materials. RE-ISM are classified into three categories based on the rare earth interface structure and the size of the substrate, following the guidance provided by the phase diagram. It mainly includes atomic interfaces, cluster interfaces, and heterstructures. By strategically designing diverse rare earth interface structures, it is feasible to effectively synthesize catalytic material systems that are tailored toward a multitude of functional applications. The synthesized RE-ISM is employed for electrocatalytic energy conversion of small molecules, offering novel prospects for catalytic electrode materials. The redox reaction process in both negative and positive grades involves the conversion of functional structural molecules through electron transfer. RE-ISM are effective catalysts for facilitating such conversion reactions. Achieving efficient construction of RE-ISM necessitates an in-depth analysis of catalytic reaction mechanisms by employing in situ spectroscopy technology. The transformation process of morphology, structure, and mechanism of RE-ISM in the catalytic process was analyzed from the perspective of time resolution, spatial resolution, and spectral resolution. We elucidate the correlation between the rare earth interface interaction mechanism and the intrinsic structure based on a cognitive foundation of in situ process analysis. This provides theoretical support for the design of high-performance RE-ISM. In summary, we expect that the development of RE-ISM will provide new design ideas and insights for inorganic energy small molecule conversion materials and further promote the rapid development of high performance electrocatalytic materials.</p>","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"5 6","pages":"712–725"},"PeriodicalIF":14.0,"publicationDate":"2024-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140949947","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":"Highly Organized Monolayer Arrangement of 2D Materials and Its Applications","authors":"Nobuyuki Sakai*, and , Takayoshi Sasaki*, ","doi":"10.1021/accountsmr.4c00072","DOIUrl":"10.1021/accountsmr.4c00072","url":null,"abstract":"<p >2D materials, also termed 2D nanosheets, have attracted significant interest due to their unique molecularly thin 2D structure to exhibit various attractive properties. They include a diverse range of materials, such as graphene, chalcogenide, oxide, hydroxide, and carbide. Such 2D materials can be produced via the delamination of their precursor layered compounds. Different from graphite and van der Waals layered compounds, there are a wide range of layered materials accommodating interlayer counterions, serving as a trigger for delamination upon exchange with suitable species. Since interlayer galleries swell evenly and infinitely, single-layer nanosheets can be obtained in high yield in the form of a colloidal suspension.</p><p >The arrangement of unilamellar 2D nanosheets on a substrate surface, avoiding large gaps and overlaps, is crucial for fully harnessing their performance. A resulting monolayer film of neatly tiled 2D nanosheets can provide a molecularly thin interface and a well-defined crystalline surface, leading to the development of unique properties and reactivities. Consequently, considerable efforts have been focused on developing solution-based assembly techniques, including electrostatic self-assembly, the Langmuir–Blodgett (LB) method, and spin coating, to produce highly organized monolayer films.</p><p >In the electrostatic self-assembly process, a substrate with an oppositely charged surface is immersed in the nanosheet suspension, and nanosheets are adsorbed on the substrate through electrostatic attraction, forming a monolayer film of nanosheets in a self-assembly fashion. In the case of LB and spin coating methods, nanosheets trapped at the air–liquid interface are densely packed in a lateral direction to achieve neat monolayer tiling on a solvent surface, which is then transferred onto a substrate surface. Compared to the electrostatic self-assembled film, the LB method yields a higher-quality monolayer film of nanosheets without large gaps or overlaps thanks to the surface compression. Similar neat tiling has been achieved by using the spin coating method with optimized deposition parameters. The advantage of this method is its ability to fabricate the film in a shorter period (∼a few minutes), making it most suitable for practical use.</p><p >Neatly tiled monolayer films of nanosheets have been applied to modify the surface and interface properties of materials, as exemplified by the performance enhancement of batteries and epitaxial growth of crystalline thin films. Furthermore, the precise monolayer tiling serves as the fundamental step for constructing multilayer films of each nanosheet or even artificial lattice-like films, where nanosheets are stacked in a designed sequence, allowing for the evolution of sophisticated functionalities via synergetic coupling between constituent nanosheets. It has been demonstrated that heterostructured films, composed of various types of nanosheets, can enhance the individual","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"5 6","pages":"752–760"},"PeriodicalIF":14.0,"publicationDate":"2024-05-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140907442","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}