Accounts of materials research最新文献

{"title":"Fiber Sorbents – A Versatile Platform for Sorption-Based Gas Separations","authors":"João Marreiros, Yuxiang Wang, MinGyu Song, William J. Koros, Matthew J. Realff, Christopher W. Jones and Ryan P. Lively*, ","doi":"10.1021/accountsmr.4c0020110.1021/accountsmr.4c00201","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00201https://doi.org/10.1021/accountsmr.4c00201","url":null,"abstract":"<p >Increasing demand for high-purity fine chemicals and a drive for process intensification of large-scale separations have driven significant work on the development of highly engineered porous materials with promise for sorption-based separations. While sorptive separations in porous materials offer energy-efficient alternatives to longstanding thermal-based methods, the particulate nature of many of these sorbents has sometimes limited their large-scale deployment in high-throughput applications such as gas separations, for which the necessary high feed flow rates and gas velocities accrue prohibitive operational costs.</p><p >These processability limitations have been historically addressed through powder shaping methods aimed at the fabrication of structured sorbent contactors based on pellets, beads or monoliths, commonly obtained as extrudates. These structures overcome limitations such as elevated pressure drops commonly recorded across powder adsorption beds but often accrue thermal limitations arising from elevated particle density and aggregation, which ultimately cap their maximum separation performance. Furthermore, the harsh mechanical strain to which powder particles are subjected during contactor fabrication, in the form of extrusion/compression forces, can result in partial pore occlusion and framework degradation, further limiting their performance.</p><p >Here, we present the development of porous fiber sorbents as an alternative sorbent contactor design capable of addressing sorbent processability limitations while enabling an array of performance-maximizing heat integration capabilities. This new sorbent form factor leverages pre-existing know-how from hollow fiber spinning to produce fiber-shaped sorbent contactors through the phase inversion of known polymers in a process known as dry-jet/wet quenching. The process of phase inversion allows microporous sorbent particles to be latched onto a macroporous polymer matrix under mild processing conditions, thus making it compatible with soft porous materials prone to amorphization under traditional pelletization conditions.</p><p >Sorbent fibers can be created with different geometries through control of the spinning apparatus and process, offering the possibility to produce monolithic and hollow fibers alike, the latter of which can be integrated with thermalization fluid flows. In this Account, we summarize our progress in the field of fiber sorbents from both design and application standpoints. We further guide the reader through the evolution of this field from the early inceptive work on zeolite hollow fibers to recent developments on MOF fibers. We highlight the versatile nature of fiber sorbents, both from the composition, fabrication and structure points of view, and further demonstrate how fiber sorbents offer alternative paths in tackling new and challenging chemical separation challenges like direct air capture (DAC), with a final perspective on the future of the fiel","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 1","pages":"6–16 6–16"},"PeriodicalIF":14.0,"publicationDate":"2024-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/accountsmr.4c00201","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143084232","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":"Plasmonic Metal Oxide Nanocrystals as Building Blocks for Infrared Metasurfaces","authors":"Woo Je Chang, Allison M. Green, Zarko Sakotic, Daniel Wasserman*, Thomas M. Truskett* and Delia J. Milliron*, ","doi":"10.1021/accountsmr.4c0030210.1021/accountsmr.4c00302","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00302https://doi.org/10.1021/accountsmr.4c00302","url":null,"abstract":"<p >Metamaterials operating at infrared (IR) frequencies have garnered significant attention due to the opportunities for resonant interactions with vibrational modes of molecules and materials and manipulation of thermal emission. These metamaterials usually consist of periodic arrangements of subwavelength scale metallic or dielectric elements, patterned either top-down by nanolithographic methods or bottom-up by nanocrystal (NC) assembly. However, conventional metals are inherently constrained by their fixed electron concentrations, which limits the degrees of freedom in the design of the meta-atom unit cells to achieve the desired optical response. In this context, doped metal oxide NCs, with the prototypical case being tin-doped indium oxide (ITO) NCs, are exceptional candidates for self-assembled IR metamaterials, owing to their relatively low and synthetically tunable electron concentrations that govern the frequencies of their IR plasmon resonances. Focusing on ITO NCs as building blocks, this Account describes recent progress in the synthetic tuning of NC optical properties, NC superlattice monolayer preparation methods for fabricating IR resonant metamaterials, and the emerging understanding of the optical response, facilitated by recently developed simulation methods.</p><p >Based on experimental and simulation methods we helped develop, we are advancing a mechanistic understanding of how self-assembled NC metamaterials can produce distinctive near- and far-field optical properties not readily achievable in lithographically patterned structures. First, the impacts of the inevitable defects and disorder associated with self-assembly can be rationalized and, in some cases, recognized as advantageous. Second, self-assembly enables intimate nanoscale intermixing of different NC and molecular components. By incorporating probe molecules within the gaps between NCs where the electric field enhancement is the strongest, we show enhanced detection of molecular vibrations that can be optimized by tuning the size and resonance frequency of the NCs. We show how metasurfaces incorporating mixtures of NCs with different doping concentrations can achieve an epsilon-near-zero dielectric response over a broad frequency range. Finally, considering the NC metasurface itself as a building block, we show how photonic structures incorporating these assemblies can harness and amplify their distinctive properties. Through modeling the NC monolayer as a slab with an effective permittivity response, we designed a frequency-tunable IR perfect absorber by layering the NCs on a simple open cavity structure. Since the perfect absorption architecture further enhances the IR electric field localization strength, we expect that this integration strategy can enhance molecular vibration coupling or nonlinear optical response. The versatility of the NC assembly and integration approach suggests opportunities for various metal oxide NC superstructures, including mixing a","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 1","pages":"104–113 104–113"},"PeriodicalIF":14.0,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143084648","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":"Plasmonic Metal Oxide Nanocrystals as Building Blocks for Infrared Metasurfaces","authors":"Woo Je Chang, Allison M. Green, Zarko Sakotic, Daniel Wasserman, Thomas M. Truskett, Delia J. Milliron","doi":"10.1021/accountsmr.4c00302","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00302","url":null,"abstract":"Metamaterials operating at infrared (IR) frequencies have garnered significant attention due to the opportunities for resonant interactions with vibrational modes of molecules and materials and manipulation of thermal emission. These metamaterials usually consist of periodic arrangements of subwavelength scale metallic or dielectric elements, patterned either top-down by nanolithographic methods or bottom-up by nanocrystal (NC) assembly. However, conventional metals are inherently constrained by their fixed electron concentrations, which limits the degrees of freedom in the design of the meta-atom unit cells to achieve the desired optical response. In this context, doped metal oxide NCs, with the prototypical case being tin-doped indium oxide (ITO) NCs, are exceptional candidates for self-assembled IR metamaterials, owing to their relatively low and synthetically tunable electron concentrations that govern the frequencies of their IR plasmon resonances. Focusing on ITO NCs as building blocks, this Account describes recent progress in the synthetic tuning of NC optical properties, NC superlattice monolayer preparation methods for fabricating IR resonant metamaterials, and the emerging understanding of the optical response, facilitated by recently developed simulation methods.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"49 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142805092","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":"Piezoionic Skin Sensors for Wearable Applications","authors":"Chao Lu*, Xiaohong Zhang and Xi Chen, ","doi":"10.1021/accountsmr.4c0031510.1021/accountsmr.4c00315","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00315https://doi.org/10.1021/accountsmr.4c00315","url":null,"abstract":"<p >Piezoionic skin sensors are one kind of artificial electrical skin that can output sensing signals in response to external strain or stress stimulus with merits of flexibility, lightness, scalability, and high sensitivity. They have been emerging as an important platform in artificial intelligence, such as in smart healthcare, bionic robotics, and microelectromechanical systems. Piezoionic sensors are typically composed of an electrolyte laminated with symmetric electrodes and are based on ion migration and redistribution under a gradient strain or stress field. However, existing challenges significantly impede the sensing performance of piezoionic sensors, including the low electromechanical coupling efficiency of the electrode materials, instability of electrolyte materials, and strain-induced interface separation of sensor interfaces. In recent years, our group and collaborators have made attempts addressing the as-mentioned critical challenges in order to achieve flexible piezoionic sensors with satisfying performance for wearable smart applications. First, for the electromechanical coupling efficiency of electrode materials, we have developed various electrode materials with highly efficient ion storage and transfer, such as graphdiyne, quinone composites, and graphitic carbon nitride. These materials present superior electrical and mechanical properties with enhanced electromechanical coupling efficiency. Second, in order to improve the stability of electrolytes, especially in an air environment, we have developed ionogel electrolytes instead of conventional hydrogel electrolytes. Ionogels contain highly stable ionic liquids, which effectively improve the air stability of sensor electrolytes, and the sensing properties of devices are preserved even after several months. Third, with regard to sensor interface separation, we have engineered stable material interfaces for piezoionic sensors with elaborate structures. The as-designed tree-root-inspired interfaces show high mechanical stability under various flexible conditions, and the piezoionic sensors display negligible performance deterioration under thousands of bending cycles in an ambient environment. Finally, we have obtained flexible piezoionic sensors and studied their practical applications, such as wearable electronics, health monitoring, and smart detections. For example, we have realized the accurate detection of blood pressure based on an out-of-plane piezoionic mechanism. This innovative technique completely avoids the cuff issue that commercial sphygmomanometers have. Moreover, we have developed multifinger-touch piezoionic sensor arrays for effective braille recognition, which have the potential to eliminate communication barriers with sight-impaired people. Human voices can be easily differentiated by detecting vocal-cord vibrations based on captured sensing signals with obviously different patterns. This smart technique is promising for extended and applied use in virtua","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 1","pages":"114–123 114–123"},"PeriodicalIF":14.0,"publicationDate":"2024-12-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143086911","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":"Piezoionic Skin Sensors for Wearable Applications","authors":"Chao Lu, Xiaohong Zhang, Xi Chen","doi":"10.1021/accountsmr.4c00315","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00315","url":null,"abstract":"Piezoionic skin sensors are one kind of artificial electrical skin that can output sensing signals in response to external strain or stress stimulus with merits of flexibility, lightness, scalability, and high sensitivity. They have been emerging as an important platform in artificial intelligence, such as in smart healthcare, bionic robotics, and microelectromechanical systems. Piezoionic sensors are typically composed of an electrolyte laminated with symmetric electrodes and are based on ion migration and redistribution under a gradient strain or stress field. However, existing challenges significantly impede the sensing performance of piezoionic sensors, including the low electromechanical coupling efficiency of the electrode materials, instability of electrolyte materials, and strain-induced interface separation of sensor interfaces. In recent years, our group and collaborators have made attempts addressing the as-mentioned critical challenges in order to achieve flexible piezoionic sensors with satisfying performance for wearable smart applications. First, for the electromechanical coupling efficiency of electrode materials, we have developed various electrode materials with highly efficient ion storage and transfer, such as graphdiyne, quinone composites, and graphitic carbon nitride. These materials present superior electrical and mechanical properties with enhanced electromechanical coupling efficiency. Second, in order to improve the stability of electrolytes, especially in an air environment, we have developed ionogel electrolytes instead of conventional hydrogel electrolytes. Ionogels contain highly stable ionic liquids, which effectively improve the air stability of sensor electrolytes, and the sensing properties of devices are preserved even after several months. Third, with regard to sensor interface separation, we have engineered stable material interfaces for piezoionic sensors with elaborate structures. The as-designed tree-root-inspired interfaces show high mechanical stability under various flexible conditions, and the piezoionic sensors display negligible performance deterioration under thousands of bending cycles in an ambient environment. Finally, we have obtained flexible piezoionic sensors and studied their practical applications, such as wearable electronics, health monitoring, and smart detections. For example, we have realized the accurate detection of blood pressure based on an out-of-plane piezoionic mechanism. This innovative technique completely avoids the cuff issue that commercial sphygmomanometers have. Moreover, we have developed multifinger-touch piezoionic sensor arrays for effective braille recognition, which have the potential to eliminate communication barriers with sight-impaired people. Human voices can be easily differentiated by detecting vocal-cord vibrations based on captured sensing signals with obviously different patterns. This smart technique is promising for extended and applied use in virtual re","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"69 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-12-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142793621","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":"Multifunctional Fluorescent Probes Unveiling Complex Pathways in Alzheimer’s Disease Pathogenesis","authors":"Priyam Ghosh, Parameswar Krishnan Iyer","doi":"10.1021/accountsmr.4c00303","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00303","url":null,"abstract":"Alzheimer’s disease (AD) is a complex neurological disorder with a progressive nature, posing challenges in diagnosis and treatment. It is characterized by the formation of Aβ plaques and neurofibrillary tangles (NFTs), which have been the focus of clinical diagnosis and treatment. Despite decades of research, the elusive nature of AD has made it difficult to develop widely recognized diagnostic and treatment methods. However, recent advances have led to new diagnostic and therapeutic techniques targeting Aβ and tau. These technologies aim to address gaps in our understanding by targeting biomarkers using multifunctional fluorescent organic-molecule-based theranostics. There is a leading hypothesis that Aβ and its oligomers are crucial pathogenic features in AD-afflicted brains. Metals found in Aβ plaques have been linked to AD, contributing to oxidative stress and stabilizing toxic Aβ oligomers. Drug research is addressing AD’s diverse toxicity, including protein aggregation, metal toxicity, oxidative stress, mitochondrial damage, and neuroinflammation. Drug development is adopting multifaceted approaches, focusing on the intricate interaction of AD contributors. Diverse diagnostic techniques and innovative drug development tactics are crucial for AD diagnosis and therapy advances.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"214 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-12-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142763572","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":"Multifunctional Fluorescent Probes Unveiling Complex Pathways in Alzheimer’s Disease Pathogenesis","authors":"Priyam Ghosh,&nbsp; and ,&nbsp;Parameswar Krishnan Iyer*,&nbsp;","doi":"10.1021/accountsmr.4c0030310.1021/accountsmr.4c00303","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00303https://doi.org/10.1021/accountsmr.4c00303","url":null,"abstract":"<p >Alzheimer’s disease (AD) is a complex neurological disorder with a progressive nature, posing challenges in diagnosis and treatment. It is characterized by the formation of Aβ plaques and neurofibrillary tangles (NFTs), which have been the focus of clinical diagnosis and treatment. Despite decades of research, the elusive nature of AD has made it difficult to develop widely recognized diagnostic and treatment methods. However, recent advances have led to new diagnostic and therapeutic techniques targeting Aβ and tau. These technologies aim to address gaps in our understanding by targeting biomarkers using multifunctional fluorescent organic-molecule-based theranostics. There is a leading hypothesis that Aβ and its oligomers are crucial pathogenic features in AD-afflicted brains. Metals found in Aβ plaques have been linked to AD, contributing to oxidative stress and stabilizing toxic Aβ oligomers. Drug research is addressing AD’s diverse toxicity, including protein aggregation, metal toxicity, oxidative stress, mitochondrial damage, and neuroinflammation. Drug development is adopting multifaceted approaches, focusing on the intricate interaction of AD contributors. Diverse diagnostic techniques and innovative drug development tactics are crucial for AD diagnosis and therapy advances.</p><p >This Account is focused on analyzing the interaction between fluorescent molecular probes in the context of AD theranostics. It explores their design methods, imaging techniques, and therapeutic applications to develop innovative approaches for diagnosing and treating AD, thereby contributing to the advancement of precision medicine in neurodegenerative disorders. The first section explains the pathological factors associated with AD, while the second part discusses recently identified multifunctional fluorescent compounds as therapeutic and diagnostic targets. We also delve into the multifunctional probes developed in our laboratory over the past decade for the purpose of AD theranostics. The subsequent section covers small molecule and conjugated polymer (CP) chemistry, design, and functions. Our research aims to shed light on AD development by studying the link between Aβ, metal ions, and particularly metal-Aβ interactions. We utilize multifunctional fluorescent molecular probes to target metal-Aβ species, modulate interaction, and guide aggregation into nontoxic, off-pathway aggregates. These multipotent ligands reduce oxidative stress by preventing the production of reactive intermediate species (RIS) from redox-active metal-Aβ. Ongoing research aims to enhance fluorescent compounds for early and accurate detection of AD and to prevent its associated causes. We also explore current challenges and potential methods for developing multifunctional probes for AD theranostics. This Account aims to aid readers in understanding the multifaceted nature of AD and the development of novel multifunctional molecules that target its multifaceted toxicity.</p>","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 1","pages":"89–103 89–103"},"PeriodicalIF":14.0,"publicationDate":"2024-12-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143087430","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":"Symmetry Manipulation of Two-Dimensional Semiconductors by Janus Structure","authors":"Xueqiu Zheng, Yi Zhou, Yunfan Guo","doi":"10.1021/accountsmr.4c00236","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00236","url":null,"abstract":"Figure 1. Schematic diagram of structure, synthesis, properties and performance of Janus TMDCs. Reproduced with permission from refs (2−5). Copyright 2021 The Authors, 2021 American Chemical Society, 2023 The Authors, 2017 American Chemical Society. Figure 2. Structures of Janus TMDCs and their heterostructures. (a) Lattice structures of monolayer 1T’ MoSSe and 2H MoSSe. (b) Schematic illustration of the topological band inversion of 1T’ MoSSe (left) and 2H MoSSe (right). Reproduced with permission from ref (4). Copyright 2023 The Authors. (c) Schematic illustration of a monolayer lateral multi-heterostructure composed with MoS&lt;sub&gt;2&lt;/sub&gt;-Janus MoSSe-Janus MoSeS-MoSe&lt;sub&gt;2&lt;/sub&gt;. (d) Kelvin probe force microscope image of monolayer lateral multi-heterostructure composed of MoS&lt;sub&gt;2&lt;/sub&gt;–MoSSe-MoSeS-MoSe&lt;sub&gt;2&lt;/sub&gt;. Reproduced with permission from ref (2). Copyright 2021 The Authors. (e) Schematic illustration of MoSSe/MoS&lt;sub&gt;2&lt;/sub&gt; vertical heterostructure. (f) Optical microscopy (OM) images of Janus heterostructures with AA, AB, AAA, AAB, and ABA stacking modes. Scale bars: 4 μm. Scale bars: 1.2 μm. Reproduced with permission from ref (6). Copyright 2020 American Chemical Society. Figure 3. Synthesis of Janus TMDCs and their lateral heterostructures. (a) Contrast of activation energy barriers between RT-ALS strategy (red) and conventional substitution in high temperature (blue). (b) Raman spectra of pristine monolayer MoS&lt;sub&gt;2&lt;/sub&gt;, Janus MoSSe, and converted MoSe&lt;sub&gt;2&lt;/sub&gt;. (c) Spatially resolved Raman mapping for A&lt;sub&gt;1g&lt;/sub&gt; mode intensity of a monolayer multi-heterostructure made with MoS&lt;sub&gt;2&lt;/sub&gt;–MoSSe-MoSeS-MoSe&lt;sub&gt;2&lt;/sub&gt;. Reproduced with permission from ref (2). Copyright 2021 The Authors. Figure 4. Properties and potential applications of Janus TMDCs. (a) HHG image of 1T’ MoSSe observed by CCD camera. (b) Left: schematic illustration of angle-resolved SHG setup measuring out-of-plane dipole of Janus MoSSe. Right: angle-dependent SHG intensity ratio between &lt;i&gt;p&lt;/i&gt; and &lt;i&gt;s&lt;/i&gt; polarization (I&lt;sub&gt;p&lt;/sub&gt; and I&lt;sub&gt;s&lt;/sub&gt;) in 1T’ MoSSe, 2H MoSSe, and 2H MoS&lt;sub&gt;2&lt;/sub&gt;. Reproduced with permission from ref (4). Copyright 2023 The Authors. (c) Calculated volcano curve of hydrogen evolution reaction (HER) of various catalysts, including Janus WSSe. Reproduced with permission from ref (13). Copyright 2018 American Chemical Society. (d) DFT calculation of shift current susceptibility tensor element σ&lt;sub&gt;&lt;i&gt;xzx&lt;/i&gt;&lt;/sub&gt;&lt;sup&gt;(2)&lt;/sup&gt; and σ&lt;sub&gt;&lt;i&gt;zxx&lt;/i&gt;&lt;/sub&gt;&lt;sup&gt;(2)&lt;/sup&gt;. The dark (red) blue curve indicates shift current for Janus MoSeS (MoSSe) monolayer. Reproduced with permission from ref (15). Copyright 2022 American Chemical Society. &lt;b&gt;Xueqiu Zheng&lt;/b&gt; received her B.S. Degree in Department of Chemistry in Zhejiang University in 2023. She is a Master degree candidate in Department of Chemistry in Zhejiang University currently. Her research focuses on the controllable synthesis of Janus TMDCs and their heterostructur","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"8 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-11-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142718912","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":"van der Waals Gap Engineering of Emergent Two-Dimensional Materials","authors":"Zejun Li*,&nbsp;Zhi Zhang and Jiong Lu*,&nbsp;","doi":"10.1021/accountsmr.4c0027010.1021/accountsmr.4c00270","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00270https://doi.org/10.1021/accountsmr.4c00270","url":null,"abstract":"<p >Layered materials bound by weak van der Waals (vdW) interactions offer a rich platform for exploring intriguing fundamental science in the two-dimensional (2D) limit and advancing technological innovations. Transition from bulk to 2D geometry results in profound alterations in electronic structures and crystallographic symmetries, giving rise to a plethora of novel physical effects and functionalities. Due to their atomic-scale thinness, 2D materials with a high specific surface area enable post-processing chemical modification of their basal planes to further regulate their intrinsic physical properties. Moreover, the interfacial effects induced by surface modifications can modulate properties without altering the original lattice, facilitating the emergence of novel electronic phases and exotic quantum phenomena. Consequently, extensive research is delving into surface modifications of 2D materials, paving the way to further expand the research fields of 2D materials.</p><p >Notably, layered materials also feature a subnanometer-sized vdW gap between adjacent layers, enabling the incorporation of guest species and evoking a new type of surface modification called vdW gap engineering, without the need for pre-exfoliation into 2D structures. Unlike postprocessing surface modifications, direct vdW gap engineering protects guest species within the layers from environmental degradation, fostering stable guest–host structures with enhanced environmental stability. Additionally, the confined vdW gap engineering prompts electronic interactions between guest species and host materials, resulting in new physics and functionalities that cannot be achieved through traditional surface modifications. Furthermore, vdW gap engineering also enables the creation of a new class of hybrid vdW superlattices with highly adaptable structural motifs, harnessing the synergistic effects of guest species and host materials.</p><p >This Account highlights recent advancements in vdW gap engineering of 2D materials from our group and other researchers. We focus on three key aspects of vdW gap engineering including the design and synthesis of low-dimensional materials, modulation of phase transitions, and fabrication of hybrid superlattices. Specifically, we provide a comprehensive overview of current vdW gap engineering methodologies such as intercalation, interlayer growth, and direct chemical growth. Various forms of host–guest interactions and their underlying mechanisms are introduced along with the exciting physical properties and functional applications. Finally, we outline the present challenges and future prospects for vdW gap engineering of 2D materials. We emphasize the crucial role of in situ characterization techniques and machine learning in advancing vdW gap engineering studies as well as potential new research directions that could open new frontiers in creating artificial vdW materials for technological innovations.</p>","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 1","pages":"52–63 52–63"},"PeriodicalIF":14.0,"publicationDate":"2024-11-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143091826","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":"van der Waals Gap Engineering of Emergent Two-Dimensional Materials","authors":"Zejun Li, Zhi Zhang, Jiong Lu","doi":"10.1021/accountsmr.4c00270","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00270","url":null,"abstract":"Layered materials bound by weak van der Waals (vdW) interactions offer a rich platform for exploring intriguing fundamental science in the two-dimensional (2D) limit and advancing technological innovations. Transition from bulk to 2D geometry results in profound alterations in electronic structures and crystallographic symmetries, giving rise to a plethora of novel physical effects and functionalities. Due to their atomic-scale thinness, 2D materials with a high specific surface area enable post-processing chemical modification of their basal planes to further regulate their intrinsic physical properties. Moreover, the interfacial effects induced by surface modifications can modulate properties without altering the original lattice, facilitating the emergence of novel electronic phases and exotic quantum phenomena. Consequently, extensive research is delving into surface modifications of 2D materials, paving the way to further expand the research fields of 2D materials.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"53 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-11-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142712759","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}