Accounts of materials research最新文献

{"title":"From Anisotropic Molecules and Particles to Small-Scale Actuators and Robots: An Account of Polymerized Liquid Crystals","authors":"Negar Rajabi, Matthew Gene Scarfo, Cole Martin Fredericks, Ramón Santiago Herrera Restrepo, Azin Adibi, Hamed Shahsavan","doi":"10.1021/accountsmr.4c00187","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00187","url":null,"abstract":"Untethered small-scale (milli-, micro-, and nano-) soft robots promise minimally invasive and targeted medical procedures in tiny, flooded, and confined environments like inside the human body. Despite such potentials, small-scale robots have not yet found their way to real-world applications. This can be mainly attributed to the fundamental and technical challenges in the fabrication, powering, navigation, imaging, and closed-loop control of robots at submillimiter scales. Pertinent to this Account, the selection of building block materials of small-scale robots also poses a challenge that is directly related to their fabrication and function.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"25 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142488784","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":"Boosting Oxidative Stress with Hydroxyethyl Starch Smart Nanomedicines to Eliminate Cancer Stem Cells","authors":"Zitao Fan, Xing Wang, Xiangliang Yang, Zifu Li","doi":"10.1021/accountsmr.4c00240","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00240","url":null,"abstract":"The significance of cancer stem cells (CSCs), a rare population of cells in tumor tissues, in biology and the treatment of solid malignancies has been widely appreciated for more than two decades. Due to a peculiar self-renewal capability, even one single cancer stem cell can grow into a bulk tumor mass. For this reason, CSCs have long been blamed as the major culprit of tumor initiation, tumor progression, treatment resistance, metastasis, and recurrence. Therefore, it has been postulated that targeting CSCs could provide tremendous clinical benefits for patients with solid tumors. Accumulating studies corroborated that CSCs maintained a tight regulation of redox homeostasis and that the fate of CSCs was extremely sensitive to elevated oxidative stress. Accordingly, a plethora of therapeutic drugs that can generate reactive oxygen species (ROS) have been leveraged to target CSCs. Nonetheless, few drugs or formulations that are capable of elevating oxidative stress have achieved clinical success for eliminating CSCs thus far.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"211 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142488783","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":"Living Biomaterials: Fabrication Strategies and Biomedical Applications","authors":"Qi-Wen Chen, Xian-Zheng Zhang","doi":"10.1021/accountsmr.4c00258","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00258","url":null,"abstract":"Natural or bioengineered living organisms (including mammalian cells, bacteria, microalgaes, yeast, viruses, plant cells, and the multiple organism community) possess many intrinsic or artificial superiorities than the synthesized and inert biomaterials for application in many fields, especially biomedical applications. By leveraging the inherent or artificial therapeutic competences (e.g., disease chemotaxis, drugs production, intelligent delivery, immune activation and metabolic regulation), these living organisms have been developed as critical therapeutic formulations for biomedical applications to solve unmet medical needs. These living organisms are more intelligent, more easily available, more highly active, and more strongly curative than conventional inert formulations, such as inorganic nanocarriers, metal–organic chelating networks, polymeric nanovesicles and biomembrane biohybrids, etc. Nevertheless, nonspecific <i>in vivo</i> circulation, the diseased microenvironment-triggered inactivation, uncontrolled proliferation or colonization, unexpected side effects, and unsatisfactory therapeutic effect severely restricted their further research development and clinical approval. Living biomaterials, fabricated by integrating tailored functional materials with natural or bioengineered living organisms by chemical conjugation, physical assembly, and biological engineering strategies as well as advanced construction techniques, are rapidly developed to preserve or augment bioactivity and therapeutic properties of living organisms and even control their behaviors, decrease their biotoxicity, and impart them with new biofunctionalities, like stress resistance, bioactivity maintenance, safe trafficking, controllable proliferation and colonization, and evolved metabolism properties. These acquired capacities are especially beneficial to improve therapeutic potency and compliance, solve significant therapeutic restrictions, avoid biosafety questions, enhance therapeutic performances, and extend the boundaries of the fabricated living biomaterials on science research and practical biomedical applications. Additionally, the introduction of biocompatible and instructive functional materials, such as inorganic materials, synthetic polymers and polypeptides, functional proteins and enzymes, as well as biological component materials, can also promote the interaction of living biomaterials with the living body and provide feedback to further adapt the biofunctions of living organisms.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"13 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142488032","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":"Chemical Bonding Engineering: Insights into Physicochemical Performance Optimization for Energy-Storage/Conversion","authors":"Zhifang Zhou, Rui Wei, Xuefan Zhou, Yuan Liu, Dou Zhang, Yuan-Hua Lin","doi":"10.1021/accountsmr.4c00243","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00243","url":null,"abstract":"Chemical bonding is fundamental in determining the physicochemical properties of the materials. Establishing correlations between chemical bonding and these properties may help identify potential materials with unique advantages or guide the composition design for improving the performance of functional materials. However, there is a lack of literature addressing this issue. This Account examines how chemical bonding engineering affects the performance optimization of four widely used or investigated functional materials that are applied in energy-storage/conversion fields, including thermoelectrics, piezoelectrics, lithium-ion batteries (LIBs), and catalysts. The key issues of these materials and correlations between chemical bonding and properties are briefly summarized.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"24 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142440666","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":"Supramolecular Aggregates and Hitchhikers","authors":"Ludan Yue, Guocan Yu, Lang Rao, Ruibing Wang, Xiaoyuan Chen","doi":"10.1021/accountsmr.4c00172","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00172","url":null,"abstract":"Supramolecular chemistry is based on intermolecular bonds, where substances dynamically bind together through noncovalent interactions. These dynamic forces allow the macrocyclic molecules and guest molecules to form stable assemblies, with high stability under physiological conditions, making them suitable for <i>in vivo</i> drug delivery. These dynamic noncovalent bonds are easily influenced by external stimuli such as light, heat, pH, and oxidation; thus, the assemblies induced by supramolecular interactions exhibit high diversity and flexibility in response to external stimuli, providing an effective method for simulating natural and physiological processes. The host–guest interactions induced self-assemblies have been applied across multiple dimensions, ranging from the molecular level to the cellular level, for detoxification, targeted drug delivery, and therapeutic studies. At the molecular level, macrocyclic molecules can encapsulate toxic substances from the bloodstream, serving as a solution for emergency detoxification. At the nanoscale level, host–guest interactions can induce the formation of multiple nanostructures including nanomicelles, nanocapsules, nanovesicles, and nanoparticles. The host–guest interactions can enhance the stability of nanostructures and impart them with stimuli sensitivity, which is highly significant in specific microenvironments like tumors. Nanostructures induced by the host–guest interactions possess optimized drug release profiles and pharmacokinetic features, thereby enhancing the therapeutic efficacy while mitigating side effects. At the microscale level, the host–guest interactions can induce the formation of various microassemblies including hydrogels, microfibers, and microtube aggregates. Moreover, microassemblies show superior potential in morphology transformation for controlling cell activity and diseases. Additionally, at the level of biological components, host–guest interactions can induce the assembly of peptides and organelles within cells and having the cell–cell or cell–particle assemblies as hitchhikers at the cellular level. Therefore, this Account aims to summarize the applications of host–guest interactions induced self-assemblies at various levels and the latest research in supramolecular self-assembly, with a particular focus on the progress in our research group. We hope that this account not only reveals the applications of therapeutic supramolecular self-assemblies but also provides new insights into the design of smart drug delivery systems.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"40 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142431479","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":"Understanding the Intrinsic Reactivity of Black Phosphorus","authors":"Haijiang Tian, Haoyu Wang, Jiahong Wang, Guangbo Qu, Xue-Feng Yu, Guibin Jiang","doi":"10.1021/accountsmr.4c00144","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00144","url":null,"abstract":"Black phosphorus (BP), a rediscovered two-dimensional (2D) material, has garnered significant interest due to its unique structure and physicochemical characteristics, including adjustable direct bandgaps, high carrier mobility, large specific surface area, and pronounced chemical reactivity. Distinct from the flat atomic structure of graphene, BP features a puckered honeycomb-like structure derived from sp³ hybridization. In addition to the three-coordination, each phosphorus atom possesses a lone pair of electrons, leading to an electron-rich nature. A variety of nanostructures such as nanosheets, nanoribbons, and quantum dots are developed from the bulk crystal of BP. The large surface area of nano BP provides numerous reactive sites that augment intralayer chemical interactions. Therefore, nano BP serves as a versatile scaffold for materials engineering, with potential applications across chemistry, catalysis, energy, and biomedicine. It is crucial to have a deep and systematic understanding of the hybridization interactions between BP and diverse molecules or materials, which is essential for functional design of BP-based materials for target applications.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"11 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-10-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142374486","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":"Ammonia Storage in Metal–Organic Framework Materials: Recent Developments in Design and Characterization","authors":"Wanpeng Lu, Dukula De Alwis Jayasinghe, Martin Schröder, Sihai Yang","doi":"10.1021/accountsmr.4c00183","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00183","url":null,"abstract":"Since the advent of the Haber–Bosch process in 1910, the global demand for ammonia (NH&lt;sub&gt;3&lt;/sub&gt;) has surged, driven by its applications in agriculture, pharmaceuticals, and energy. Current methods of NH&lt;sub&gt;3&lt;/sub&gt; storage, including high-pressure storage and transportation, present significant challenges due to their corrosive and toxic nature. Consequently, research has turned towards metal–organic framework (MOF) materials as potential candidates for NH&lt;sub&gt;3&lt;/sub&gt; storage due to their potential high adsorption capacities and structural tunability. MOFs are coordination networks composed of metal nodes and organic linkers, offering unprecedented porosity and surface area, and allowing incorporation of various functional groups and metal sites that can enhance NH&lt;sub&gt;3&lt;/sub&gt; adsorption. However, the stability of MOFs in the presence of NH&lt;sub&gt;3&lt;/sub&gt; is a significant concern since many degrade upon exposure to NH&lt;sub&gt;3&lt;/sub&gt;, primarily due to ligand displacement and framework collapse. To address this, recent studies have focused on the synthesis and postsynthetic modification of MOFs to enhance both NH&lt;sub&gt;3&lt;/sub&gt; uptake and stability. In this Account, we summarize recent developments in the design and characterization of MOFs for NH&lt;sub&gt;3&lt;/sub&gt; storage. The choice of metal centers in MOFs is crucial for stability and performance. High-valence metals such as Al&lt;sup&gt;III&lt;/sup&gt; and Ti&lt;sup&gt;IV&lt;/sup&gt; form strong metal–linker bonds, enhancing the stability of the framework to NH&lt;sub&gt;3&lt;/sub&gt;. The MFM-300 series of materials composed of high-valence 3+ and 4+ metal ions and carboxylic linkers demonstrates high stability and high NH&lt;sub&gt;3&lt;/sub&gt; uptake capacities. Ligand functionalization is another effective strategy for improving the NH&lt;sub&gt;3&lt;/sub&gt; adsorption. Polar functional groups such as –NH&lt;sub&gt;2&lt;/sub&gt;, –OH, and –COOH enhance the interaction between the framework and NH&lt;sub&gt;3&lt;/sub&gt;, particularly at low partial pressures, while postsynthetic modification allows fine-tuning of these functionalities to optimize the framework for higher adsorption capacities and stability. For example, MFM-303(Al), incorporating free carboxylic acid groups, exhibits a high NH&lt;sub&gt;3&lt;/sub&gt; packing density comparable to that of solid NH&lt;sub&gt;3&lt;/sub&gt;. Creating defect sites by removing linkers or adding metal ions increases the number of active sites available for NH&lt;sub&gt;3&lt;/sub&gt; adsorption and shows promise for enhancing uptake. UiO-66, a stable MOF framework, can be modified to include defect sites, significantly enhancing the level of NH&lt;sub&gt;3&lt;/sub&gt; uptake. The full characterization of MOFs and especially their interactions with NH&lt;sub&gt;3&lt;/sub&gt; are vital for understanding and improving their performance. Techniques such as neutron powder diffraction (NPD), inelastic neutron scattering (INS), diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), electron paramagnetic resonance (EPR) spectroscopy, and solid-state nuclear magnetic resonance (ssNMR) spectros","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"21 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142374493","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":"Rational Fabrication of Functionally-Graded Surfaces for Biological and Biomedical Applications","authors":"Tong Wu, Xiaoran Li, Jiajia Xue, Younan Xia","doi":"10.1021/accountsmr.4c00186","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00186","url":null,"abstract":"As a ubiquitous feature of the biological world, gradation, in either composition or structure, is essential to many functions and processes. Taking protein gradation as an example, it plays a pivotal role in the development and evolution of human bodies, including stimulation and direction of the outgrowth of peripheral nerves in a developing fetus. It is also critically involved in wound healing by attracting and guiding immune cells to the site of injury or infection. Another good example can be found in the tendon-to-bone enthesis that relies on gradations in composition, structure, and cell phenotype to create a gradual change in mechanical stiffness. It is these unique gradations that eliminate the high level of stress at the interface, enabling the effective transfer of mechanical load from tendon to bone. How to fabricate and utilize graded surfaces and materials has been a constant theme of research in the context of materials science, chemistry, cell biology, and biomedical engineering. In cell biology, for example, graded surfaces are employed to investigate the fundamental mechanisms related to embryo development and to elucidate cell behaviors under chemo-, hapto-, or mechano-taxis. Scaffolds based upon graded materials have also been widely explored to enhance tissue repair or regeneration by accelerating cell migration and/or controlling stem cell differentiation.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"50 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142329288","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":"Thermally Drawn Semiconductor Fibers: Fabrication Strategies and Applications","authors":"Zhixun Wang, Lei Wei","doi":"10.1021/accountsmr.4c00132","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00132","url":null,"abstract":"Wearable electronics enable seamless incorporation of electronics into our daily lives. Consumer-grade wearables, such as smart rings, bands, and watches, have gained popularity in recent years due to their capacity to offer consistent and dependable data collection and assistance for daily activities. Moreover, wearable electronics are emerging in professional medical services, such as continuous glucose monitoring and minimally invasive thrombectomy, to aid healthcare professionals in diagnosing and treating. In addition, the proliferation of the Internet of Things (IoT) has further fueled the demand for wearable electronics, as they are the critical components for an IoT system to support the sharing and analysis of data across multiple devices and platforms. The market for wearable electronics predictably continues to expand in the future. Semiconductors are crucial components of wearable electronics, and especially in fiber form factor, they enable monolithic fiber electronics and smart textiles. Several techniques are developed for fabricating inorganic semiconductor fibers, such as the Czochralski growth method, micropulling-down process, and thermal drawing technique. Thermal drawing of semiconductor fibers is a technique in which semiconductor materials are supported by glassy cladding materials and heated into fluid melts, with the combination drawn to fiber dimensions. Among the various fabrication methods, the thermal drawing technique has the advantages of a high yield rate, feasible integration of multiple materials, the capability of achieving designable sophisticated structures, and an extended single-strand fiber length. The as-drawn semiconductor fibers may serve as the building blocks of wearable electronics directly or subject to postprocessing procedures for on-demand alteration of dimension, geometry, or phase structure before employment. Research efforts within the fundamental understanding of fluid dynamics, rheology, and molecular structure evolution seek to improve the performance and quality of thermally drawn semiconductor fibers such as conductivity, bandgap, electron mobility, thermal stability, and mechanical strength. In this Account, we systematically recapitulate our efforts in developing semiconductor fibers and their application in wearable electronics, including diodes, sensors, energy harvesters, and more. We begin by introducing the three primary thermal drawing methods, highlighting the unique features of each. Next, postprocessing methods to further alter the materials, structures, and geometries of semiconductor fibers are discussed. We then discuss the various devices and applications and conclude with an examination of current challenges and our perspectives on future research directions. This Account aims to inspire further research efforts to expand the scope of fiber materials, the design of in-fiber structures, and configurations of device assembly to achieve widespread adoption of semiconductor fib","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"22 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142329153","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":"Stabilization of Superionic Copper Selenide Based Thermoelectric Materials","authors":"Jincheng Yu, Haihua Hu, Hua-Lu Zhuang, Hezhang Li, Jing-Feng Li","doi":"10.1021/accountsmr.4c00229","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00229","url":null,"abstract":"Thermoelectric (TE) technology enables the direct conversion between heat and electricity, thereby contributing to the alleviation of the prevailing energy crisis and the mitigation of environmental concerns. Bismuth telluride-based TE materials have been commercially utilized, while they are mainly applied to solid-state cooling rather than energy harvesting. Superionic conductors including copper chalcogenides and silver chalcogenides are rendered as promising TE candidates for power generation due to their superior thermoelectric figure of merit (<i>ZT</i>) at middle or high temperatures; the liquid-like behavior of ions aligns these systems with the concept of phonon-liquid electron-crystal (PLEC). Although the mobile ions are beneficial to enhancing the electrical transport and phonon scattering, their directional migration driven by an electric field or temperature gradient can result in the unintended deposition of metals, which can impair both the TE properties and the service stability of the materials. Therefore, it is imperative to identify stabilized liquid-like TE materials that can withstand current strike and high temperature.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142317723","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}