interfaces

接口
  • 文章类型: Journal Article
    通过X射线曝光可以实现稀土元素在电解质水溶液及其自由表面之间的可逆循环。这种暴露改变了与螯合配体结合的镧系元素离子之间的竞争平衡,二亚乙基三胺五乙酸(DTPA),在本体溶液中,并在其表面上达到萃取剂二十六烷基磷酸(DHDP)的不溶性单层。通过全反射附近的X射线荧光测量提供了暴露引起的镧系元素表面密度随时间变化的证据。将X射线限制在水性表面区域时的结果与X射线透射到本体溶液中时的结果的比较表明,水性辐射分解在吸附循环中的重要性。DTPA中的胺结合位点被鉴定为放射分解产物的可能靶标。分子DTPA和DHDP类似于用于从矿石中分离镧系元素和核燃料后处理的分子。这些结果表明,可以使用外部X射线源来驱动稀土元素分离。更一般地说,使用X射线控制剂量与镧系元素的液体界面可以触发一系列界面过程,包括增强的金属离子提取,催化作用,和材料合成。
    Reversible cycling of rare-earth elements between an aqueous electrolyte solution and its free surface is achieved by X-ray exposure. This exposure alters the competitive equilibrium between lanthanide ions bound to a chelating ligand, diethylenetriamine pentaacetic acid (DTPA), in the bulk solution and to insoluble monolayers of extractant di-hexadecyl phosphoric acid (DHDP) at its surface. Evidence for the exposure-induced temporal variations in the lanthanide surface density is provided by X-ray fluorescence near total reflection measurements. Comparison of results when X-rays are confined to the aqueous surface region to results when X-rays transmit into the bulk solution suggests the importance of aqueous radiolysis in the adsorption cycle. Amine binding sites in DTPA are identified as a likely target of radiolysis products. The molecules DTPA and DHDP are like those used in the separation of lanthanides from ores and in the reprocessing of nuclear fuel. These results suggest that an external source of X-rays can be used to drive rare-earth element separations. More generally, use of X-rays to controllably dose a liquid interface with lanthanides could trigger a range of interfacial processes, including enhanced metal ion extraction, catalysis, and materials synthesis.
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  • 文章类型: Journal Article
    全固态钾金属电池因其丰富而受到越来越多的关注,成本效益,和高能量/功率密度。然而,它们的发展通常受到缺乏合适的固态电解质的限制。在这里,我们报告了一种新的配合物KCB9H10·2C3H4N2,该配合物通过在温和条件下研磨和加热十氢钾-一碳-氯-脱硼酸钾(KCB9H10)和咪唑(C3H4N2)的混合物而合成,实现了K离子超离子固态电解质。通过FOX软件显示晶体结构为正交晶格,空间群为Pna21。使用爬升图像微动弹性带(CI-NEB)方法计算了晶体结构中K的扩散特性。KCB9H10·2C3H4N2在30°C时表现出1.3×10-4Scm-1的高离子电导率,比KCB9H10高四个数量级。该离子电导率也是所报道的氢化硼酸盐基K导体的最高值。此外,KCB9H10·2C3H4N2的K+转移数为0.96,电化学稳定性窗口为1.2至3.2VK/K+,和良好的稳定性对K金属涂层的咪唑化钾(KIm)。这些出色的性能使KCB9H10·2C3H4N2成为有前途的K离子固态电解质。
    All-solid-state potassium metal batteries have caught increasing interest owing to their abundance, cost-effectiveness, and high energy/power density. However, their development is generally constrained by the lack of suitable solid-state electrolytes. Herein, we report a new complex KCB9H10·2C3H4N2, synthesized by grinding and heating the mixture of potassium decahydrido-monocarba-closo-decaborate (KCB9H10) and imidazole (C3H4N2) under mild conditions, to achieve the K-ion superionic solid-state electrolyte. The crystal structure was revealed as an orthorhombic lattice with the space group of Pna21 by FOX software. The diffusion properties for K+ in the crystal structure were calculated using the climbing image nudged elastic band (CI-NEB) method. KCB9H10·2C3H4N2 exhibited a high ionic conductivity of 1.3 × 10-4 S cm-1 at 30 °C, four orders of magnitude higher than that of KCB9H10. This ionic conductivity is also the highest value of hydridoborate-based K+ conductors reported. Moreover, KCB9H10·2C3H4N2 demonstrated a K+ transference number of 0.96, an electrochemical stability window of 1.2 to 3.2 V vs. K/K+, and good stability against the K metal coated by a layer of potassium imidazolate (KIm). These great performances make KCB9H10·2C3H4N2 a promising K-ion solid-state electrolyte.
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  • 文章类型: Journal Article
    在柔性基板上转换的钙钛矿太阳能电池(PSC)技术作为物联网(IOT)的替代供电解决方案的需求很高。PSC在刚性基板上的效率为26.1%,在柔性基板上的效率为25.09%。Further,据报道,F-PSC模块的表面积为900cm2,PCE为16.43%。这种性能是F-PSC器件的世界纪录,比100cm2更重要。工艺优化,以及新运输材料的使用,接口,和构图工程,以及钝化,有助于实现F-PSC的这种性能。因此,本文主要综述了F-PSC的研究进展以及钙钛矿薄膜的低温制备方法,形态均匀性,和更好的结晶度。透光率,带隙匹配,载波移动性,和低温加工的容易性是界面层的关键品质因数。电极材料的柔性和透明性质增强了装置的机械稳定性。稳定性,灵活性,和可扩展的F-PSC制造挑战也得到解决。最后,还将详细讨论基于成本的F-PSC应用商业化前景。
    The perovskite solar cells (PSCs) technology translated on flexible substrates is in high demand as an alternative powering solution to the Internet of Things (IOTs). An efficiency of ∼26.1% on rigid and ∼25.09% on flexible substrates has been achieved for the PSCs. Further, it is also reported that F-PSC modules have a surface area of ∼900 cm2, with a PCE of ∼16.43%. This performance is a world record for an F-PSC device more significant than ∼100 cm2. The process optimization, and use of new transport materials, interface, and compositional engineering, as well as passivation, have helped in achieving such kind of performance of F-PSCs. Hence, the review focuses mainly on the progress of F-PSCs and the low-temperature fabrication methods for perovskite films concerning their full coverage, morphological uniformity, and better crystallinity. The transmittance, band gap matching, carrier mobility, and ease of low-temperature processing are the key figures of merit of interface layers. Electrode material\'s flexible and transparent nature has enhanced the device\'s mechanical stability. Stability, flexibility, and scalable F-PSC fabrication challenges are also addressed. Finally, an outlook on F-PSC applications for their commercialization based on cost will also be discussed in detail.
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  • 文章类型: Journal Article
    近年来,自组装已经成为制造功能材料的强大工具。由于自组装从根本上是由系统中的粒子相互作用决定的,如果我们能完全控制这些相互作用,它将为通过设计创造功能材料打开大门。在本文中,我们利用液体界面处胶体颗粒之间的毛细管相互作用来创建二维(2D)材料,其中颗粒相互作用和自组装可以单独使用颗粒形状完全编程。具体来说,我们认为胶体颗粒是多边形板,具有均匀的表面化学和起伏的边缘,因为这种颗粒的几何形状为我们提供了对短程硬核排斥和远程毛细管相互作用的精确和独立的控制。为了说明我们的系统为编程自组装提供的巨大潜力,我们使用最小能量计算和蒙特卡罗模拟来显示具有不同平面内形状的多边形板(六边形,截断三角形,三角形,正方形)和不同多极阶的边缘起伏(六极,八极,十二极)可用于创建丰富多样的2D结构,包括密排六角形,蜂窝,Kagome,和准晶体晶格。由于所需的颗粒形状可以很容易地通过实验制造,我们可以使用我们的胶体系统来控制材料设计的整个过程链,从建筑砌块的初始设计和制造开始,最终组装出的2D材料。
    In recent years, self-assembly has emerged as a powerful tool for fabricating functional materials. Since self-assembly is fundamentally determined by the particle interactions in the system, if we can gain full control over these interactions, it would open the door for creating functional materials by design. In this paper, we exploit capillary interactions between colloidal particles at liquid interfaces to create two-dimensional (2D) materials where particle interactions and self-assembly can be fully programmed using particle shape alone. Specifically, we consider colloidal particles which are polygonal plates with homogeneous surface chemistry and undulating edges as this particle geometry gives us precise and independent control over both short-range hard-core repulsions and longer-range capillary interactions. To illustrate the immense potential provided by our system for programming self-assembly, we use minimum energy calculations and Monte Carlo simulations to show that polygonal plates with different in-plane shapes (hexagons, truncated triangles, triangles, squares) and edge undulations of different multipolar order (hexapolar, octopolar, dodecapolar) can be used to create a rich variety of 2D structures, including hexagonal close-packed, honeycomb, Kagome, and quasicrystal lattices. Since the required particle shapes can be readily fabricated experimentally, we can use our colloidal system to control the entire process chain for materials design, from initial design and fabrication of the building blocks, to final assembly of the emergent 2D material.
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  • 文章类型: Journal Article
    分层薄膜提供高性能和多功能,然而,实现完全分层的电影仍然是一个挑战。逐层方法,涉及每一层的顺序沉积,已普遍用于分层薄膜制造。然而,这种方法很耗时,劳动密集型,并且容易在薄膜内留下缺陷。或者,利用干燥二元胶体混合物的自分层过程最近得到了广泛的发展,但是它依赖于严格的操作条件,通常产生异质夹层。在这项研究中,介绍了一种用于创建完全分层的纳米颗粒(NP)膜的主动界面分层过程。该技术利用在空气-水界面处具有变化的界面活性的NP。在消耗压力的帮助下,NP混合物在界面处的横向压缩会导致界面活性较低的NP单独解吸到子相中,而更多的界面活性NP保留在界面处。这种简单的压缩导致具有可控性的近乎完美的分层NP膜,普遍性,和可扩展性。结合溶剂退火工艺,主动分层方法使得能够制造在NP层顶上包含聚合物层的分层膜。这项工作为设计药物封装和控释提供了深刻的启示,以及制造透明和柔性电极。
    Stratified films offer high performance and multifunctionality, yet achieving fully stratified films remains a challenge. The layer-by-layer method, involving the sequential deposition of each layer, has been commonly utilized for stratified film fabrication. However, this approach is time-consuming, labor-intensive, and prone to leaving defects within the film. Alternatively, the self-stratification process exploiting a drying binary colloidal mixture is intensively developed recently, but it relies on strict operating conditions, typically yielding a heterogeneous interlayer. In this study, an active interfacial stratification process for creating completely stratified nanoparticle (NP) films is introduced. The technique leverages NPs with varying interfacial activity at the air-water interface. With the help of depletion pressure, the lateral compression of NP mixtures at the interface induces individual desorption of less interfacial active NPs into the subphase, while more interfacial active NPs remain at the interface. This simple compression leads to nearly perfect stratified NP films with controllability, universality, and scalability. Combined with a solvent annealing process, the active stratification process enables the fabrication of stratified films comprising a polymeric layer atop a NP layer. This work provides insightful implications for designing drug encapsulation and controlled release, as well as manufacturing transparent and flexible electrodes.
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    文章类型: Journal Article
    组成是系统生物学的强大原理,专注于接口,互连,和分布式进程的编排。尽管大多数系统生物学模型都专注于受控条件下特定子系统的结构或动力学,组合系统生物学旨在将此类模型连接到综合多尺度模拟中。这强调了模型之间的空间——组合观点问应该通过子模型的接口暴露哪些变量?耦合模型如何跨尺度连接和转换?我们如何连接跨生物和物理研究领域的特定领域模型以推动新知识的合成?将不同数据集和子模型集成到统一多尺度模拟中的软件需要什么?如何访问由此产生的集成模型,灵活地重组成新形式,并由研究人员社区迭代地完善?这篇文章提供了组成系统生物学的关键组成部分的高级概述,包括:1)概念框架和相应的图形框架来表示接口,构图模式,和编排模式;2)标准化的组合模式,为可组合的数据类型和模型提供一致的格式,为可以灵活组装的模拟模块注册表培养强大的基础设施;3)一组基础的生物模板-细胞和分子界面的模式,可以填充详细的子模型和数据集,并旨在整合揭示细胞分子出现的知识;4)通过用户友好的界面促进科学合作,将研究人员与数据集和模型联系起来,并允许研究人员社区有效地建立细胞系统的综合多尺度模型。
    Composition is a powerful principle for systems biology, focused on the interfaces, interconnections, and orchestration of distributed processes. Whereas most systems biology models focus on the structure or dynamics of specific subsystems in controlled conditions, compositional systems biology aims to connect such models into integrative multiscale simulations. This emphasizes the space between models-a compositional perspective asks what variables should be exposed through a submodel\'s interface? How do coupled models connect and translate across scales? How can we connect domain-specific models across biological and physical research areas to drive the synthesis of new knowledge? What is required of software that integrates diverse datasets and submodels into unified multiscale simulations? How can the resulting integrative models be accessed, flexibly recombined into new forms, and iteratively refined by a community of researchers? This essay offers a high-level overview of the key components for compositional systems biology, including: 1) a conceptual framework and corresponding graphical framework to represent interfaces, composition patterns, and orchestration patterns; 2) standardized composition schemas that offer consistent formats for composable data types and models, fostering robust infrastructure for a registry of simulation modules that can be flexibly assembled; 3) a foundational set of biological templates-schemas for cellular and molecular interfaces, which can be filled with detailed submodels and datasets, and are designed to integrate knowledge that sheds light on the molecular emergence of cells; and 4) scientific collaboration facilitated by user-friendly interfaces for connecting researchers with datasets and models, and which allows a community of researchers to effectively build integrative multiscale models of cellular systems.
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  • 文章类型: Journal Article
    目的:薄液膜在各种系统和应用中起着至关重要的作用。了解调节其形态的机制是一项科学挑战,对应用优化具有明显的意义。捕获在气泡和气液界面之间的薄液膜可以显示出受其变形历史和系统特性影响的各种构型。
    方法:此处使用干涉测量技术研究了在表面活性分子存在下形成的薄液膜的形态。研究了三种具有不同界面性能的不同系统,以了解它们对薄膜形态的影响。将特定的变形历史应用于膜以产生复杂的膜结构。
    结果:我们通过对空气-液体界面实施受控的气泡运动来实现相当稳定的wimple的创建。我们提供了基于润滑理论的螺纹形成准则。还研究了wimple的长期稳定性,和更复杂的多wimple结构是在实现wimple稳定性的基础上通过实验生产的。
    OBJECTIVE: Thin liquid films play a crucial role in various systems and applications. Understanding the mechanisms that regulate their morphology is a scientific challenge with obvious implications for application optimization. Thin liquid films trapped between bubbles and air-liquid interface can show various configurations influenced by their deformation history and system characteristics.
    METHODS: The morphology of thin liquid films formed in the presence of surface-active molecules is here studied with interferometric techniques. Three different systems with varying interfacial properties are investigated to understand their influence on film morphology. Specific deformation histories are applied to the films to generate complex film structures.
    RESULTS: We achieve the creation of a rather stable wimple by implementing controlled bubble motions against the air-liquid interface. We provide a criterion for wimple formation based on lubrication theory. The long-term stability of the wimple is also investigated, and more complex multi-wimple structures are experimentally produced building upon the achieved wimple stability.
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  • 文章类型: Journal Article
    液-液相分离产生的生物分子冷凝物有助于不同的细胞过程,如基因表达。将客户分子分成缩合物对调节缩合物的组成和功能是关键的。以前的研究表明,客户端大小限制了分区,从缩合物中排除>5nm的葡聚糖。这里,我们问是否更大的颗粒,如大分子复合物,可以根据颗粒-冷凝物相互作用分成冷凝物。我们试图发现生物物理原理,这些原理使用具有定制表面化学的聚合物纳米颗粒作为大分子复合物的模型来控制凝结物中的颗粒包含或排除。用聚乙二醇(PEG)涂覆的颗粒不分配到缩合物中。接下来,我们利用PEG化的颗粒作为惰性平台,我们将特定的粘合剂部分缀合到该惰性平台。用生物素官能化的颗粒分配到含有链霉亲和素的缩合物中,由高亲和力生物素-链霉亲和素结合驱动。寡核苷酸修饰的颗粒表现出不同程度的分配成缩合物,取决于冷凝物的组成。通过改变盐浓度来调整寡核苷酸包被的颗粒的分配,寡核苷酸长度,和寡核苷酸表面密度。值得注意的是,具有不同表面化学性质的珠子正交分配为不混溶的冷凝物。根据我们的实验,我们得出的结论是,任意大的颗粒可以可控地分配到生物分子缩合物,给予足够强的缩合物-颗粒相互作用,我们的粗粒度分子动力学模拟和理论也支持了这一结论。这些发现可以提供对各种细胞过程是如何实现的基础上,大客户分配到生物分子缩合物的见解,以及为开发选择性靶向疾病相关生物分子缩合物的药物递送系统提供设计原则。
    生物分子缩合物是选择性募集或排除客户分子的亚细胞区室,即使冷凝物缺乏封闭的膜。许多生化重建实验已经研究了无膜细胞器控制分配的机制,模拟细胞如何时空招募成分进入凝聚体以调节细胞功能。一个悬而未决的问题是分区是否受到客户端大小的严格限制。在这项工作中,我们设计了具有各种尺寸和表面功能的纳米颗粒,并测量了这些变量如何决定分配。我们观察到大颗粒的受控和正交分配为几种冷凝类型,由强烈的粒子-冷凝物相互作用驱动。分子模拟概括了关键结果。我们的工作推进了对凝析油成分如何调节的理解,我们的纳米粒子工具箱也可能激发药物输送的平台。
    Biomolecular condensates arising from liquid-liquid phase separation contribute to diverse cellular processes, such as gene expression. Partitioning of client molecules into condensates is critical to regulating the composition and function of condensates. Previous studies suggest that client size limits partitioning, with dextrans >5 nm excluded from condensates. Here, we asked whether larger particles, such as macromolecular complexes, can partition into condensates based on particle-condensate interactions. We sought to discover the biophysical principles that govern particle inclusion in or exclusion from condensates using polymer nanoparticles with tailored surface chemistries as models of macromolecular complexes. Particles coated with polyethylene glycol (PEG) did not partition into condensates. We next leveraged the PEGylated particles as an inert platform to which we conjugated specific adhesive moieties. Particles functionalized with biotin partitioned into condensates containing streptavidin, driven by high-affinity biotin-streptavidin binding. Oligonucleotide-decorated particles exhibited varying degrees of partitioning into condensates, depending on condensate composition. Partitioning of oligonucleotide-coated particles was tuned by altering salt concentration, oligonucleotide length, and oligonucleotide surface density. Remarkably, beads with distinct surface chemistries partitioned orthogonally into immiscible condensates. Based on our experiments, we conclude that arbitrarily large particles can controllably partition into biomolecular condensates given sufficiently strong condensate-particle interactions, a conclusion also supported by our coarse-grained molecular dynamics simulations and theory. These findings may provide insights into how various cellular processes are achieved based on partitioning of large clients into biomolecular condensates, as well as offer design principles for the development of drug delivery systems that selectively target disease-related biomolecular condensates.
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  • 文章类型: Journal Article
    我们研究了复杂形成时内在无序区域(IDR)的转变,利用X射线解析的蛋白质-DNA和蛋白质-RNA复合物的结构数据集,以及它们可用的未结合蛋白质形式。识别出的IDR分为三类:无序有序(DO),无序到部分有序(D-PO)和无序到无序(DD)在未绑定和复杂形式中进行比较后。在DO类中,IDR形成类似线圈的次级结构,螺旋,和与核酸结合后的链。尽管这些IDR中的大多数存在于复合物的表面,在界面处还观察到大量的IDR,并参与极性相互作用。由界面IDR(B_IDR)与磷酸盐和核酸碱基形成的氢键相对比糖形成的氢键更多。B_IDR与蛋白质-RNA中的核糖形成的H键比与蛋白质-DNA中的脱氧核糖形成的H键更多。在B_IDR中,Arg和Lys更喜欢与DNA和RNA的主沟和小沟相互作用,分别。Ser,然而,更喜欢两个核酸中的小凹槽。有趣的是,我们报告了31个蛋白质-DNA和22个蛋白质-RNA复合物中的61个和48个IDR,分别,表明核酸与蛋白质的结合也可能导致有序到无序的转换。
    We study transitions in intrinsically disordered regions (IDRs) upon complex formation, utilizing X-ray-solved structural dataset of protein-DNA and protein-RNA complexes, along with their available unbound protein forms. The identified IDRs are categorized into three classes: Disordered-to-Ordered (D-O), Disordered-to-Partial Ordered (D-PO) and Disordered-to-Disordered (D-D) after comparing them in unbound and complex forms. In the D-O class, IDRs form secondary structures like coils, helices, and strands upon binding to nucleic acids. Though a majority of these IDRs are present at the surface of the complexes, a significant number of IDRs are also observed at the interfaces and are involved in polar interactions. The hydrogen bonds made by the interface IDRs (B_IDRs) with phosphates and bases of nucleic acids are comparatively more than those formed with sugars. B_IDRs form more H-bonds with the ribose in protein-RNA than with the deoxyribose in protein-DNA. Among the B_IDRs, Arg and Lys prefer to interact with the major and minor grooves of DNA and RNA, respectively. Ser, however, prefers the minor groove in both the nucleic acids. Interestingly, we report 61 and 48 IDRs in 31 protein-DNA and 22 protein-RNA complexes, respectively, suggesting nucleic acid binding to proteins may also result in ordered-to-disordered transitions.
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  • 文章类型: Journal Article
    考虑了用于接枝反应的两个模型衬底:未脱光的硅,其表面被薄氧化物层覆盖,其表面上具有反应性硅烷醇基团;和脱釉的硅,其中通过用氢氟酸处理去除氧化物层。反应性聚合物是分子量为3.9至13.9kg·mol·1的羟基封端的聚苯乙烯。接枝反应在两种不同的基材上在不同的温度和不同的时间段内进行。评价所得刷子的厚度和热稳定性。此外,通过共混两种不同分子量的聚合物来模拟高度分散体系的接枝。尽管在去釉的硅上发现刷子厚度增长更快,短链的优先接枝在两种底物上都具有相同的链选择倾向。
    Two model substrates for the grafting to reaction are considered: not-deglazed silicon, whose surface is coated by a thin oxide layer with reactive silanol groups on its surface; and deglazed silicon, where the oxide layer is removed by treatment with hydrofluoric acid. The reactive polymers are hydroxy-terminated polystyrenes with molecular weights ranging from 3.9 to 13.9 kg mol⁻1. The grafting to reaction is carried out at different temperatures and for different periods of time on the two different substrates. The thickness and the thermal stability of the resulting brushes are evaluated. Furthermore, the grafting of a highly dispersed system is simulated by blending two polymers with different molecular weights. Although the brush thickness growth is found to be faster on deglazed silicon, the preferential grafting of short chains occurs with equal chain selection propensity on both substrates.
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