High-entropy alloys (HEAs) are novel materials composed of multiple elements with nearly equal concentrations and they exhibit exceptional properties such as high strength, ductility, thermal stability, and corrosion resistance. However, the intricate and diverse structures of HEAs pose significant challenges to understanding and predicting their behavior at different length scales. This review summarizes recent advances in computational simulations and experiments of structure-property relationships in HEAs at the nano/micro scales. Various methods such as first-principles calculations, molecular dynamics simulations, phase diagram calculations, and finite element simulations are discussed for revealing atomic/chemical and crystal structures, defect formation and migration, diffusion and phase transition, phase formation and stability, stress-strain distribution, deformation behavior, and thermodynamic properties of HEAs. Emphasis is placed on the synergistic effects of computational simulations and experiments in terms of validation and complementarity to provide insights into the underlying mechanisms and evolutionary rules of HEAs. Additionally, current challenges and future directions for computational and experimental studies of HEAs are identified, including accuracy, efficiency, and scalability of methods, integration of multiscale and multiphysics models, and exploration of practical applications of HEAs.
高熵合金（HEAs）是一种新型材料，由浓度几乎相等的多种元素组成，具有高强度、延展性、热稳定性和耐腐蚀性等优异性能。然而，HEAs 复杂多样的结构给理解和预测其在不同长度尺度上的行为带来了巨大挑战。本综述总结了在纳米/微米尺度上对 HEAs 结构-性能关系进行计算模拟和实验的最新进展。文章讨论了第一原理计算、分子动力学模拟、相图计算和有限元模拟等各种方法，以揭示 HEAs 的原子/化学和晶体结构、缺陷形成和迁移、扩散和相变、相形成和稳定性、应力应变分布、变形行为和热力学性质。重点是计算模拟和实验在验证和互补方面的协同作用，以便深入了解 HEAs 的内在机制和演化规律。此外，还确定了 HEA 计算和实验研究的当前挑战和未来方向，包括方法的准确性、效率和可扩展性，多尺度和多物理模型的集成，以及 HEA 的实际应用探索。
{"title":"Accelerating the Exploration of High-Entropy Alloys: Synergistic Effects of Integrating Computational Simulation and Experiments","authors":"Deyu Jiang, Yuhua Li, Liqiang Wang, Lai-Chang Zhang","doi":"10.1002/sstr.202400110","DOIUrl":"https://doi.org/10.1002/sstr.202400110","url":null,"abstract":"High-entropy alloys (HEAs) are novel materials composed of multiple elements with nearly equal concentrations and they exhibit exceptional properties such as high strength, ductility, thermal stability, and corrosion resistance. However, the intricate and diverse structures of HEAs pose significant challenges to understanding and predicting their behavior at different length scales. This review summarizes recent advances in computational simulations and experiments of structure-property relationships in HEAs at the nano/micro scales. Various methods such as first-principles calculations, molecular dynamics simulations, phase diagram calculations, and finite element simulations are discussed for revealing atomic/chemical and crystal structures, defect formation and migration, diffusion and phase transition, phase formation and stability, stress-strain distribution, deformation behavior, and thermodynamic properties of HEAs. Emphasis is placed on the synergistic effects of computational simulations and experiments in terms of validation and complementarity to provide insights into the underlying mechanisms and evolutionary rules of HEAs. Additionally, current challenges and future directions for computational and experimental studies of HEAs are identified, including accuracy, efficiency, and scalability of methods, integration of multiscale and multiphysics models, and exploration of practical applications of HEAs.","PeriodicalId":21841,"journal":{"name":"Small Structures","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141530588","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}
Francois-Marie Allioux, Sahar Nazari, Mohammad B. Ghasemian, Ali Zavabeti, Zengxia Pei, Josh Leverett, Somayeh Rafiezadeh, Amar K. Salih, Curtis P. Irvine, Mahroo Baharfar, Laetitia Bardet, Moonika S. Widjajana, Yuan Chi, Dorna Esrafilzadeh, Ali R. Jalili, Nima Haghdadi, Jianbo Tang, Kevin J. Laws, Cuong Ton-That, Torben Daeneke, Rahman Daiyan, Md Arifur Rahim, Kourosh Kalantar-Zadeh
Gallium-based liquid metal alloys exhibit unconventional and intriguing properties as metallic solvents, demonstrating an exceptional potential to dissolve and reconfigure a vast array of elements within the liquid metal matrix. Leveraging on these distinctive characteristics of gallium-based alloys, the synthesis of high-entropy liquid metal alloys (HELMAs) in low dimensions is reported. The nanoscale HELMAs offer advantages including the solvation of multiple metallic elements at room temperature, while promoting their atomic dispersion at elevated concentrations. Entropy estimations for HELMAs surpass those of high-temperature molten metals, leading to the realization of high-entropy liquid metal systems at room temperature. Through a proof-of-concept hydrogen evolution reaction comparison, the potential of these HELMAs in enhancing the activities of nanocatalysts is demonstrated. In this case, atomic dispersion of Pt is shown in senary GaIn-AuCuPtPd HELMA, contrasting with lower entropy systems in which Pt forms discernible clusters. These presented features can lead to catalytic systems with enhanced and tailored activities.
{"title":"Atomic Dispersion via High-Entropy Liquid Metal Alloys","authors":"Francois-Marie Allioux, Sahar Nazari, Mohammad B. Ghasemian, Ali Zavabeti, Zengxia Pei, Josh Leverett, Somayeh Rafiezadeh, Amar K. Salih, Curtis P. Irvine, Mahroo Baharfar, Laetitia Bardet, Moonika S. Widjajana, Yuan Chi, Dorna Esrafilzadeh, Ali R. Jalili, Nima Haghdadi, Jianbo Tang, Kevin J. Laws, Cuong Ton-That, Torben Daeneke, Rahman Daiyan, Md Arifur Rahim, Kourosh Kalantar-Zadeh","doi":"10.1002/sstr.202400294","DOIUrl":"https://doi.org/10.1002/sstr.202400294","url":null,"abstract":"Gallium-based liquid metal alloys exhibit unconventional and intriguing properties as metallic solvents, demonstrating an exceptional potential to dissolve and reconfigure a vast array of elements within the liquid metal matrix. Leveraging on these distinctive characteristics of gallium-based alloys, the synthesis of high-entropy liquid metal alloys (HELMAs) in low dimensions is reported. The nanoscale HELMAs offer advantages including the solvation of multiple metallic elements at room temperature, while promoting their atomic dispersion at elevated concentrations. Entropy estimations for HELMAs surpass those of high-temperature molten metals, leading to the realization of high-entropy liquid metal systems at room temperature. Through a proof-of-concept hydrogen evolution reaction comparison, the potential of these HELMAs in enhancing the activities of nanocatalysts is demonstrated. In this case, atomic dispersion of Pt is shown in senary GaIn-AuCuPtPd HELMA, contrasting with lower entropy systems in which Pt forms discernible clusters. These presented features can lead to catalytic systems with enhanced and tailored activities.","PeriodicalId":21841,"journal":{"name":"Small Structures","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141514424","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}
Beatriz Merillas, Carlos A. García-González, Tomás Enrique Gómez Álvarez-Arenas, Miguel Ángel Rodríguez-Pérez
The aerogel performance for industrial uses can be tailored using several chemical and physical strategies. The effects of a controlled densification on polyurethane aerogels are herein studied by analyzing their textural, mechanical, sound, optical, and thermal insulating properties. The produced aerogels are uniaxially compressed to different strains (30%–80%) analyzing the consequent changes in the structures and, therefore, final properties. As expected, their mechanical stiffness can be significantly increased by compression (until 55-fold higher elastic modulus for 80%-strain), while the light transmittance does not noticeably worsen until it is compressed more than 60%. Additionally, the modifications produced in the heat transfer contributions are analyzed, obtaining the optimum balance between density increase and pore size reduction. The minimum thermal conductivity (14.5%-reduction) is obtained by compressing the aerogel to 50%-strain, where the increment in the solid conduction is surpassed by the reduction of the radiative and gas contributions. This strategy avoids tedious chemical modifications in the synthesis procedure to control the final structure of the aerogels, leading to the possibility of carefully adapting their structure and properties through a simple method such as densification. Thus, it allows to obtain aerogels for current and on-demand applications, which is one of the main challenges in the field.
{"title":"Towards the Optimization of Polyurethane Aerogel Properties by Densification: Exploring the Structure–Properties Relationship","authors":"Beatriz Merillas, Carlos A. García-González, Tomás Enrique Gómez Álvarez-Arenas, Miguel Ángel Rodríguez-Pérez","doi":"10.1002/sstr.202400120","DOIUrl":"https://doi.org/10.1002/sstr.202400120","url":null,"abstract":"The aerogel performance for industrial uses can be tailored using several chemical and physical strategies. The effects of a controlled densification on polyurethane aerogels are herein studied by analyzing their textural, mechanical, sound, optical, and thermal insulating properties. The produced aerogels are uniaxially compressed to different strains (30%–80%) analyzing the consequent changes in the structures and, therefore, final properties. As expected, their mechanical stiffness can be significantly increased by compression (until 55-fold higher elastic modulus for 80%-strain), while the light transmittance does not noticeably worsen until it is compressed more than 60%. Additionally, the modifications produced in the heat transfer contributions are analyzed, obtaining the optimum balance between density increase and pore size reduction. The minimum thermal conductivity (14.5%-reduction) is obtained by compressing the aerogel to 50%-strain, where the increment in the solid conduction is surpassed by the reduction of the radiative and gas contributions. This strategy avoids tedious chemical modifications in the synthesis procedure to control the final structure of the aerogels, leading to the possibility of carefully adapting their structure and properties through a simple method such as densification. Thus, it allows to obtain aerogels for current and on-demand applications, which is one of the main challenges in the field.","PeriodicalId":21841,"journal":{"name":"Small Structures","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141514425","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}
Green and highly selective synthesis of ammonia (NH3) via electrochemical reduction reaction of toxic nitrite (NO2−RR) in a neutral electrolyte is a feasible solution for energy and environmental issues. Dual-nature electrocatalysts combining metal and metal-derived materials are crucial for enhancing the selectivity parameter and efficacy of this reaction. Here, Pd-, Pt-, Ru-, and Ir-decorated Co3(PO4)2 (CoPi) composites with a robust metal–support interaction are obtained via the one-pot pulsed laser ablation in liquid method. Among the designed composites, Ir–CoPi affords ≈100% Faradaic efficiency, mass balance, and selectivity toward NH3 product at sufficiently low potentials. Further, it affords the highest NH3 yield rate of 19.13 mg h−1 cm−2 with 78.1% removal of toxic NO2− with a rate constant kapp = 0.31 mm min−1 under −1.6 V versus Ag/AgCl. In situ experiments and theoretical investigations reveal the underlying mechanisms responsible for this outstanding performance of Ir–CoPi, which can be accredited to the generation of specific active sites on the Ir component. Insights derived from the evolving intermediate reactive species provide new opportunities for large-scale NH3 production through electrochemical techniques, density functional theory calculations, and the improvement of the corresponding industrial processes.
{"title":"Pulsed Laser-Initiated Dual-Catalytic Interfaces for Directed Electroreduction of Nitrite to Ammonia","authors":"Talshyn Begildayeva, Jayaraman Theerthagiri, Vy Thuy Nguyen, Ahreum Min, Hyeyoung Shin, Myong Yong Choi","doi":"10.1002/sstr.202400187","DOIUrl":"https://doi.org/10.1002/sstr.202400187","url":null,"abstract":"Green and highly selective synthesis of ammonia (NH<sub>3</sub>) via electrochemical reduction reaction of toxic nitrite (NO<sub>2</sub><sup>−</sup>RR) in a neutral electrolyte is a feasible solution for energy and environmental issues. Dual-nature electrocatalysts combining metal and metal-derived materials are crucial for enhancing the selectivity parameter and efficacy of this reaction. Here, Pd-, Pt-, Ru-, and Ir-decorated Co<sub>3</sub>(PO<sub>4</sub>)<sub>2</sub> (CoPi) composites with a robust metal–support interaction are obtained via the one-pot pulsed laser ablation in liquid method. Among the designed composites, Ir–CoPi affords ≈100% Faradaic efficiency, mass balance, and selectivity toward NH<sub>3</sub> product at sufficiently low potentials. Further, it affords the highest NH<sub>3</sub> yield rate of 19.13 mg h<sup>−1</sup> cm<sup>−2</sup> with 78.1% removal of toxic NO<sub>2</sub><sup>−</sup> with a rate constant <i>k</i><sub>app</sub> = 0.31 m<span>m</span> min<sup>−1</sup> under −1.6 V versus Ag/AgCl. In situ experiments and theoretical investigations reveal the underlying mechanisms responsible for this outstanding performance of Ir–CoPi, which can be accredited to the generation of specific active sites on the Ir component. Insights derived from the evolving intermediate reactive species provide new opportunities for large-scale NH<sub>3</sub> production through electrochemical techniques, density functional theory calculations, and the improvement of the corresponding industrial processes.","PeriodicalId":21841,"journal":{"name":"Small Structures","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141514525","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}
Heebae Kim, Eunbin Jang, Jinil Cho, Seonmi Pyo, Heejun Yun, Jeewon Lee, Byeongyun Min, Juyeon Han, Jeeyoung Yoo, Youn Sang Kim
All-solid-state Li-metal battery (ASSLB) represents advantageous energy storage system for automotive applications. For ASSLB, inorganic solid electrolyte is essential in determining safety and cycling performance. However, significant challenges persist in practical construction of ASSLB with optimized electrolyte. Specifically, electrolyte's structural instability influencing its electrochemical performance remains critical issue within typical operating temperatures for ASSLB in electric vehicles. Herein, this challenge is fundamentally addressed by substituting trace amount of lithium with cadmium, which lacks crystal field stabilization energy. This strategy of atomic interaction modification has induced electrolyte's structural distortion and electronic alteration by deliberately introducing disorder at local lithium sites. Li symmetric cell with cadmium-substituted antiperovskite solid electrolyte exhibits outstanding critical current density of 11.5 mA cm−2 (5.75 mAh cm−2) and excellent stability for 3000 h at 10.0 mA cm−2 (5.0 mAh cm−2). This study highlights explicit research direction for breakthrough of ASSLB, focusing on understanding how local distortion affects complex inorganic materials.
全固态锂金属电池（ASSLB）是汽车应用中的优势储能系统。对于全固态锂金属电池而言，无机固体电解质对其安全性和循环性能至关重要。然而，在实际建造具有优化电解质的 ASSLB 时，仍然面临着巨大的挑战。具体来说，电解质的结构不稳定性会影响其电化学性能，这在电动汽车 ASSLB 的典型工作温度下仍是一个关键问题。在这里，通过用缺乏晶体场稳定能量的镉替代微量锂，从根本上解决了这一难题。这种原子相互作用修饰策略通过故意在局部锂位点引入无序状态，诱发电解质结构畸变和电子变化。使用镉取代的反包晶石固体电解质的锂对称电池表现出卓越的临界电流密度，达到 11.5 mA cm-2（5.75 mAh cm-2），并在 10.0 mA cm-2（5.0 mAh cm-2）的条件下保持了 3000 小时的卓越稳定性。这项研究强调了突破 ASSLB 的明确研究方向，重点是了解局部变形如何影响复杂的无机材料。
{"title":"Strategic Atomic Interaction Modification for Highly Durable Inorganic Solid Electrolytes in Advanced All-Solid-State Li-Metal Batteries","authors":"Heebae Kim, Eunbin Jang, Jinil Cho, Seonmi Pyo, Heejun Yun, Jeewon Lee, Byeongyun Min, Juyeon Han, Jeeyoung Yoo, Youn Sang Kim","doi":"10.1002/sstr.202400091","DOIUrl":"https://doi.org/10.1002/sstr.202400091","url":null,"abstract":"All-solid-state Li-metal battery (ASSLB) represents advantageous energy storage system for automotive applications. For ASSLB, inorganic solid electrolyte is essential in determining safety and cycling performance. However, significant challenges persist in practical construction of ASSLB with optimized electrolyte. Specifically, electrolyte's structural instability influencing its electrochemical performance remains critical issue within typical operating temperatures for ASSLB in electric vehicles. Herein, this challenge is fundamentally addressed by substituting trace amount of lithium with cadmium, which lacks crystal field stabilization energy. This strategy of atomic interaction modification has induced electrolyte's structural distortion and electronic alteration by deliberately introducing disorder at local lithium sites. Li symmetric cell with cadmium-substituted antiperovskite solid electrolyte exhibits outstanding critical current density of 11.5 mA cm<sup>−2</sup> (5.75 mAh cm<sup>−2</sup>) and excellent stability for 3000 h at 10.0 mA cm<sup>−2</sup> (5.0 mAh cm<sup>−2</sup>). This study highlights explicit research direction for breakthrough of ASSLB, focusing on understanding how local distortion affects complex inorganic materials.","PeriodicalId":21841,"journal":{"name":"Small Structures","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141552072","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}
Piers Coia, Bhagya Dharmasiri, David J. Hayne, Ameya Borkar, Carol Hua, Elmer Austria, Behnam Akhavan, Mia Angela Nuñeza Judicpa, Ken Aldren Sumaya Usman, Joselito Razal, Luke C. Henderson
The multifunctionality of carbon fiber (CF) is being extensively explored. Herein, polyimide covalent organic frameworks (PI-COFs) are grafted bound to CF to enhance their mechanical and electrochemical properties. Here, a range of COF scaffolds are grafted to the surface of CFs via a two-step functionalization. First, melamine is tethered to the fiber surface to provide an anchoring point for the COFs followed by a “graft from” approach to grow three different sized PI-COFs utilizing three differently sized dianhydride, PMDA to form MA-PMDA, NTCDA to form MA-NTCDA, and PTCDA to form MA-PTCDA COFs. These COFs increase the capacitance of CF by a maximum of 2.9 F g−1 (480% increase) for the MA-PTCDA, this coincides with an increase in interfacial shear strength by 67.5% and 52% for MA-NTCDA and MA-PTCDA, respectively. This data represents that the first-time CF has been modified with PI-COFs and allows access to COF properties including their porosity and CO2 capture ability while being attached to a substrate. This may lead to additional high-value recyclability and second-life applications for CFs.
{"title":"Hierarchical Polyimide-Covalent Organic Frameworks Carbon Fiber Structures Enhancing Physical and Electrochemical Properties","authors":"Piers Coia, Bhagya Dharmasiri, David J. Hayne, Ameya Borkar, Carol Hua, Elmer Austria, Behnam Akhavan, Mia Angela Nuñeza Judicpa, Ken Aldren Sumaya Usman, Joselito Razal, Luke C. Henderson","doi":"10.1002/sstr.202400166","DOIUrl":"https://doi.org/10.1002/sstr.202400166","url":null,"abstract":"The multifunctionality of carbon fiber (CF) is being extensively explored. Herein, polyimide covalent organic frameworks (PI-COFs) are grafted bound to CF to enhance their mechanical and electrochemical properties. Here, a range of COF scaffolds are grafted to the surface of CFs via a two-step functionalization. First, melamine is tethered to the fiber surface to provide an anchoring point for the COFs followed by a “graft from” approach to grow three different sized PI-COFs utilizing three differently sized dianhydride, PMDA to form <b>MA-PMDA</b>, NTCDA to form <b>MA-NTCDA,</b> and PTCDA to form <b>MA-PTCDA</b> COFs. These COFs increase the capacitance of CF by a maximum of 2.9 F g<sup>−1</sup> (480% increase) for the <b>MA-PTCDA</b>, this coincides with an increase in interfacial shear strength by 67.5% and 52% for <b>MA-NTCDA</b> and <b>MA-PTCDA,</b> respectively. This data represents that the first-time CF has been modified with PI-COFs and allows access to COF properties including their porosity and CO<sub>2</sub> capture ability while being attached to a substrate. This may lead to additional high-value recyclability and second-life applications for CFs.","PeriodicalId":21841,"journal":{"name":"Small Structures","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141514427","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}
The edge reconstruction of two-dimensional (2D) materials is significant for the stability, properties, and applications. Significant progress has been made in understanding the edge reconstruction of 2D materials. Herein, an overview of the latest theoretical and experimental advances on edge reconstruction of α-phase phosphorene nanoribbon and IV–VI group binary compounds MX (M = Ge, Sn; X = S, Se), focusing on the mechanism, stability, physical, and chemical properties of the edge reconstructions is provided. The status, challenges, and contradictions in experiments and theory are addressed and the progress in edge reconstruction of α-phase puckered 2D materials as well as the effects of edge reconstruction on physicochemical properties are systematically introduced. A novel tube-like edge reconstruction is suggested to be universal for α-phase puckered monolayers. While ZZ(U) edge can be another important reconstruction in bilayer. Beyond the review, the edge structures of phosphorene have odd–even layered oscillations are also proposed. The edge terminations can affect the exfoliation mechanism and electronic, transport properties. Interesting, unique U-edge, which has been verified by experiment, exhibits nearly edgeless electronic and thermal transport, which is beneficial for ultrafast microelectronics.
{"title":"The Unique Edge Reconstructions and Related Edgeless Properties of Mono- and Few-Layered α-Phase Puckered 2D Materials","authors":"Mingyue Xia, Yuan Chang, Zhigen Yu, Hongsheng Liu, Si Zhou, Jijun Zhao, Junfeng Gao","doi":"10.1002/sstr.202400191","DOIUrl":"https://doi.org/10.1002/sstr.202400191","url":null,"abstract":"The edge reconstruction of two-dimensional (2D) materials is significant for the stability, properties, and applications. Significant progress has been made in understanding the edge reconstruction of 2D materials. Herein, an overview of the latest theoretical and experimental advances on edge reconstruction of <i>α</i>-phase phosphorene nanoribbon and IV–VI group binary compounds MX (M = Ge, Sn; X = S, Se), focusing on the mechanism, stability, physical, and chemical properties of the edge reconstructions is provided. The status, challenges, and contradictions in experiments and theory are addressed and the progress in edge reconstruction of <i>α</i>-phase puckered 2D materials as well as the effects of edge reconstruction on physicochemical properties are systematically introduced. A novel tube-like edge reconstruction is suggested to be universal for <i>α</i>-phase puckered monolayers. While ZZ(U) edge can be another important reconstruction in bilayer. Beyond the review, the edge structures of phosphorene have odd–even layered oscillations are also proposed. The edge terminations can affect the exfoliation mechanism and electronic, transport properties. Interesting, unique U-edge, which has been verified by experiment, exhibits nearly edgeless electronic and thermal transport, which is beneficial for ultrafast microelectronics.","PeriodicalId":21841,"journal":{"name":"Small Structures","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141552068","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}
Caiying Li, Gengjia Chen, Tan Li, Peiyi Xie, Decai Ma, Long Yang, Zecong Xiao, Xintao Shuai, Xiaochun Meng
Immunotherapy has made great progress in various solid tumors. However, the “cold” tumor immune microenvironment of microsatellite stable subtype colorectal cancer (MSS-CRC) hinders the effectiveness of immunotherapy. Therefore, reshaping the immunosuppressive microenvironment and initiating efficient antitumor immune responses are critical for immunotherapy of MSS-CRC. According to the analysis of clinical samples, it is found that the levels of fat mass and obesity-associated protein (FTO) and M2-like tumor-associated macrophages (TAMs) infiltration are significantly elevated in CRC tissue, which has driven one to construct a targeted cationic liposome to simultaneously enhance the RNA methylation and inhibit the CD47 immune checkpoint expression of tumor cells in the hope of promoting the M1-like TAMs polarization and phagocytosis. By upregulating the m6A modification of tumor cells, the lactate secretion is decreased to promote the TAMs repolarized into M1-like. Meanwhile, CD47 siRNA codelivered by the cationic liposomes downregulates the expression of immune checkpoint CD47 on the cancer cell surface, which enhances the phagocytic ability of the M1-like TAMs. The combination treatment scheme is expected to provide a new option for treating MSS-CRC, which may also be extended for treating other immunologically “cold” tumors.
{"title":"Multifunctional Nanodrug-Mediated Immunotherapy in Microsatellite Stable Colorectal Cancer via Promoting m6A Modification and M1-Like Tumor-Associated Macrophages Polarization","authors":"Caiying Li, Gengjia Chen, Tan Li, Peiyi Xie, Decai Ma, Long Yang, Zecong Xiao, Xintao Shuai, Xiaochun Meng","doi":"10.1002/sstr.202400100","DOIUrl":"https://doi.org/10.1002/sstr.202400100","url":null,"abstract":"Immunotherapy has made great progress in various solid tumors. However, the “cold” tumor immune microenvironment of microsatellite stable subtype colorectal cancer (MSS-CRC) hinders the effectiveness of immunotherapy. Therefore, reshaping the immunosuppressive microenvironment and initiating efficient antitumor immune responses are critical for immunotherapy of MSS-CRC. According to the analysis of clinical samples, it is found that the levels of fat mass and obesity-associated protein (FTO) and M2-like tumor-associated macrophages (TAMs) infiltration are significantly elevated in CRC tissue, which has driven one to construct a targeted cationic liposome to simultaneously enhance the RNA methylation and inhibit the CD47 immune checkpoint expression of tumor cells in the hope of promoting the M1-like TAMs polarization and phagocytosis. By upregulating the m6A modification of tumor cells, the lactate secretion is decreased to promote the TAMs repolarized into M1-like. Meanwhile, CD47 siRNA codelivered by the cationic liposomes downregulates the expression of immune checkpoint CD47 on the cancer cell surface, which enhances the phagocytic ability of the M1-like TAMs. The combination treatment scheme is expected to provide a new option for treating MSS-CRC, which may also be extended for treating other immunologically “cold” tumors.","PeriodicalId":21841,"journal":{"name":"Small Structures","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141552069","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}
Hematopoietic stem cell (HSC) transplantation is used to treat blood and immunodeficient diseases. HSC expansion techniques must be developed to prevent complications and ensure reliable therapeutic efficacy. Hence, several studies have attempted in vitro expansion of HSCs using scaffolds but failed to mimic the diverse and complex nature of HSC environments. Herein, an artificial HSC microenvironment, bone marrow (BM) niches is created, through in vivo engineering using carbonate apatite honeycomb scaffolds and the potential of these scaffolds in restoring lost hematopoietic function and immunity is investigated. BM niches are generated in every honeycomb channel, wherein HSCs are gradually aggregated. Compared to the actual BM, the scaffolds exhibit a 9.9- and 78-fold increase in the number of stored CD45− CD34+ side scatterlow cells that are mainly considered HSCs at 8 and 12 weeks, respectively. The transplantation of the honeycomb scaffold containing HSCs and BM niches into immunocompromised mice increases peripheral blood chimerism and restores hematopoietic function and the number of immunocytes (monocytes and lymphocytes) to normal levels. This study contributes to the development of efficient HSC transplantation techniques. Additionally, in vivo-engineered integrated tissues using honeycomb scaffolds can be used to elucidate the interplay between the BM niches and resident cells.
{"title":"Hematopoietic Function Restoration by Transplanting Bone Marrow Niches In Vivo Engineered Using Carbonate Apatite Honeycomb Bioreactors","authors":"Koichiro Hayashi, Ryo Kishida, Akira Tsuchiya, Kunio Ishikawa","doi":"10.1002/sstr.202400065","DOIUrl":"https://doi.org/10.1002/sstr.202400065","url":null,"abstract":"Hematopoietic stem cell (HSC) transplantation is used to treat blood and immunodeficient diseases. HSC expansion techniques must be developed to prevent complications and ensure reliable therapeutic efficacy. Hence, several studies have attempted in vitro expansion of HSCs using scaffolds but failed to mimic the diverse and complex nature of HSC environments. Herein, an artificial HSC microenvironment, bone marrow (BM) niches is created, through in vivo engineering using carbonate apatite honeycomb scaffolds and the potential of these scaffolds in restoring lost hematopoietic function and immunity is investigated. BM niches are generated in every honeycomb channel, wherein HSCs are gradually aggregated. Compared to the actual BM, the scaffolds exhibit a 9.9- and 78-fold increase in the number of stored CD45<sup>−</sup> CD34<sup>+</sup> side scatter<sup>low</sup> cells that are mainly considered HSCs at 8 and 12 weeks, respectively. The transplantation of the honeycomb scaffold containing HSCs and BM niches into immunocompromised mice increases peripheral blood chimerism and restores hematopoietic function and the number of immunocytes (monocytes and lymphocytes) to normal levels. This study contributes to the development of efficient HSC transplantation techniques. Additionally, in vivo-engineered integrated tissues using honeycomb scaffolds can be used to elucidate the interplay between the BM niches and resident cells.","PeriodicalId":21841,"journal":{"name":"Small Structures","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141552070","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}
Halloysite nanotubes (HNTs) have a layered structure of clay silicate minerals and a tubular shape, which is suitable for the uniform loading of small substrates and drug molecules. The inner diameter of HNTs with an acidic solvent is selectively etched to increase the loading capacity of magnetic iron–platinum (FePt) nanoparticles. The FePt nanoparticles and etched HNTs (eHNT) are then composited by vacuum decompression. The resulting product is named FePt@eHNT and is used as a contrast agent for T2-weighted magnetic resonance imaging. According to a comprehensive analysis of the material and its magnetic properties, by adding different proportions of HNTs before and after modification, the saturation magnetization can reach 23.769 emu g−1, which is higher than that of the composite materials studied in previous studies. This is because the tubular structure promotes the orderly displacement of the FePt nanoparticles under three-dimensional space constraints and the uniform effect of the magnetic field. In addition, the magnetothermal effect of the composite material is observed and its potential as an imaging agent is investigated. In this study, the enhancement of its ferromagnetism and its potential to become a multifunctional composite material for applications in drug delivery, magnetic hyperthermia, and bioimaging is demonstrated.
{"title":"Magnetically Guided Theranostics: Novel Nanotubular Magnetic Resonance Imaging Contrast System Using Halloysite Nanotubes Embedded with Iron–Platinum Nanoparticles for Hepatocellular Carcinoma Treatment","authors":"Ming-Hsien Chan, Chi-Yu Lee, Chien-Hsiu Li, Yu-Chan Chang, Da-Hua Wei, Michael Hsiao","doi":"10.1002/sstr.202300526","DOIUrl":"https://doi.org/10.1002/sstr.202300526","url":null,"abstract":"Halloysite nanotubes (HNTs) have a layered structure of clay silicate minerals and a tubular shape, which is suitable for the uniform loading of small substrates and drug molecules. The inner diameter of HNTs with an acidic solvent is selectively etched to increase the loading capacity of magnetic iron–platinum (FePt) nanoparticles. The FePt nanoparticles and etched HNTs (eHNT) are then composited by vacuum decompression. The resulting product is named FePt@eHNT and is used as a contrast agent for T2-weighted magnetic resonance imaging. According to a comprehensive analysis of the material and its magnetic properties, by adding different proportions of HNTs before and after modification, the saturation magnetization can reach 23.769 emu g<sup>−1</sup>, which is higher than that of the composite materials studied in previous studies. This is because the tubular structure promotes the orderly displacement of the FePt nanoparticles under three-dimensional space constraints and the uniform effect of the magnetic field. In addition, the magnetothermal effect of the composite material is observed and its potential as an imaging agent is investigated. In this study, the enhancement of its ferromagnetism and its potential to become a multifunctional composite material for applications in drug delivery, magnetic hyperthermia, and bioimaging is demonstrated.","PeriodicalId":21841,"journal":{"name":"Small Structures","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141530590","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}
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