single particle

单粒子
  • 文章类型: Journal Article
    由于AlH3能够提供高的比冲和优异的燃烧性能,因此作为燃料添加剂获得了相当大的关注。然而,很少有研究集中在AlH3的破碎和团聚行为上。这项研究调查了AlH3和AlH3/PVDF颗粒的碎裂对热分解的影响,点火,团聚,和HTPB推进剂的燃烧。热分析表明,AlH3和AlH3/PVDF可以通过丰富的活性位点促进高氯酸铵的分解,以吸附分解中间体。单颗粒燃烧揭示了AlH3颗粒定向喷射熔融Al和AlH3/PVDF颗粒碎裂的机理。多孔Al的熔化由于固液界面张力和氧化物壳的结构恢复而引起颗粒收缩,这因此导致AlH3的氧化物壳中的裂缝的密封。此外,内部拉伸应力的积累导致这些裂纹的重新打开和熔融Al的定向喷射。柔性氧化物壳有助于AlH3/PVDF颗粒的最小归一化直径较小,帮助产生内部拉伸应力,而AlF3的升华诱导了碎裂。基于同步加速器的X射线成像揭示了熔融Al促进的聚集体的形成,由于氢爆炸导致的AlH3聚集体的分裂,由于氢爆炸和AlF3升华的协同作用,AlH3/PVDF的碎裂增强。与原始颗粒相比,SP2推进剂的CCP(冷凝燃烧产物)显示平均尺寸减少了48%(D50=24.5μm),而SP3推进剂的CCP的粒径减少了89%以上(D50=5.14μm)。这项研究有助于了解AlH3和AlH3/PVDF在点火和燃烧时的碎裂,为含AlH3推进剂的开发和优化提供有价值的见解。
    AlH3 has gained considerable attention as a fuel additive due to its ability to offer high specific impulse and superior combustion performance. However, few studies have focused on the fragmentation and agglomeration behavior of AlH3. This study investigated the effects of fragmentation of AlH3 and AlH3/PVDF particles on the thermal decomposition, ignition, agglomeration, and combustion of HTPB propellants. Thermal analysis indicated that AlH3 and AlH3/PVDF can accelerate the decomposition of ammonium perchlorate by abundant active sites for the adsorption of the decomposition intermediates. Single-particle combustion uncovered the mechanism behind the directional spray of molten Al from the AlH3 particle and the fragmentation of the AlH3/PVDF particle. The melting of porous Al induces particle shrinkage due to solid-liquid interfacial tension and the structural restoration of the oxide shell, which consequently results in the sealing of cracks in the oxide shell of AlH3. Additionally, the accumulation of internal tensile stress leads to the reopening of these cracks and the directional ejection of the molten Al. The flexible oxide shell contributes to a smaller minimum normalized diameter of the AlH3/PVDF particle, aiding in the generation of internal tensile stress, while the sublimation of AlF3 induced the fragmentation. Synchrotron-based X-ray imaging revealed the formation of aggregates promoted by molten Al, the splitting of AlH3 aggregates due to hydrogen explosion, and the enhanced fragmentation of AlH3/PVDF due to the synergistic effect of hydrogen explosion and the sublimation of AlF3. Compared to raw particles, the CCPs (condensed combustion products) of SP2 propellant display a 48% reduction in average size (D50 = 24.5 μm), whereas there is an over 89% decrease in particle size for the CCPs of SP3 propellant (D50 = 5.14 μm). This study contributes to understanding the fragmentation of AlH3 and AlH3/PVDF upon ignition and combustion, providing valuable insights for the development and optimization of propellants containing AlH3.
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  • 文章类型: Journal Article
    巨自噬/自噬是细胞成分降解的一个高度保守的过程,在维持细胞稳态中起着至关重要的作用。在自噬过程中,形成称为自噬体的专门的双膜囊泡,并隔离细胞质货物,并将它们输送到溶酶体或液泡中进行分解。这个过程的核心是自噬相关(ATG)蛋白,ATG9是该核心机制中唯一的完整膜蛋白,在介导自噬体形成中起着核心作用。近年来,低温电子显微镜(cryo-EM)和单粒子分析已成为蛋白质复合物高分辨率结构测定的强大工具。这些进步大大加深了我们对自噬体生物发生的复杂分子机制的理解。在这项研究中,我们提出了一个协议,详细介绍了从拟南芥获得ATG9的三维结构。通过单粒子低温电子显微镜(cryo-EM)确定的结构分辨率达到7.8µ。
    Macroautophagy/autophagy is a highly conserved process for the degradation of cellular components and plays an essential role in cellular homeostasis maintenance. During autophagy, specialized double-membrane vesicles known as autophagosomes are formed and sequester cytoplasmic cargoes and deliver them to lysosomes or vacuoles for breakdown. Central to this process are autophagy-related (ATG) proteins, with the ATG9-the only integral membrane protein in this core machinery-playing a central role in mediating autophagosome formation. Recent years have witnessed the maturation of cryo-electron microscopy (cryo-EM) and single-particle analysis into powerful tools for high-resolution structural determination of protein complexes. These advancements have significantly deepened our understanding of the intricate molecular mechanisms underlying autophagosome biogenesis. In this study, we present a protocol detailing the acquisition of the three-dimensional structure of ATG9 from Arabidopsis thaliana. The structural resolution achieved 7.8 Å determined by single-particle cryo-electron microscopy (cryo-EM).
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  • 文章类型: Journal Article
    在单粒子水平上对纳米粒子进行准确的定量元素和同位素分析对于更好地了解其起源至关重要,属性和行为。单粒子电感耦合等离子体质谱(spICP-MS)已成为一种有前途的纳米粒子分析技术。然而,通过常规四极杆(QMS)或飞行时间质量分析仪(TOF-MS)获得小尺寸纳米粒子的准确和一致的元素分布和比率仍然存在挑战,因为它们的低水平和瞬态性质。在本文中,我们提出了一种新的分析方法,使用多收集器ICP-MS(MC-ICP-MS)结合现代高速数字示波器进行单纳米颗粒分析。使用“事件触发信号捕获”(ETSC)技术获取单粒子事件,这使得能够以纳秒时间分辨率同时捕获和可视化瞬时单个粒子分布的多个同位素。这极大地促进了纳米颗粒的精确和有效的分析。对于AgNPs,计算出的最小可检测粒径小至8nm(~1ag109Ag)。基于从2000个颗粒获得的109/107Ag比率,在20nm上测量109/107Ag比率的精度,40nm,60nm,80nm和100nm约为0.086(SD),0.063(SD),0.051(SD),0.040(SD),和0.029(SD),这受到同位素信号统计量的限制。此外,即使测量20nmAgNPs(N=17,000),也可以将109/107Ag的标准误差降低到亚permil水平(0.7‰)。这些结果表明,ETSC为单个粒子的同位素分析提供了一种独特的方法,具有增强我们对纳米粒子的理解的巨大潜力。
    Accurate quantitative elemental and isotope analysis of nanoparticles at the single-particle level is crucial for better understanding their origin, properties and behaviors. Single particle inductively coupled plasma-mass spectrometry (spICP-MS) has emerged as a promising technique for nanoparticle analysis. However, challenges persist in obtaining accurate and consistent element profiles and ratios for small-sized nanoparticles by conventional quadrupole (QMS) or time-of-flight mass analyzers (TOF-MS) due to their low level and transient nature. In this paper, we present a novel analytical method for single nanoparticle analysis using multiple collector ICP-MS (MC-ICP-MS) combined with a modern high-speed digital oscilloscope. The single particle events are acquired using an \"event-triggered signal capture\" (ETSC) technique, which enables the simultaneously capture and visualization of multiple isotopes of transient individual particle profiles with nanosecond time resolution. This greatly facilitates precise and efficient analysis of nanoparticles. The minimum detectable particle size is calculated to be as small as 8 nm (∼1 ag 109Ag) for AgNPs. Based on the 109/107Ag ratios obtained from 2000 particles, the precisions of 109/107Ag ratio measurements on 20 nm, 40 nm, 60 nm, 80 nm and 100 nm were approximately 0.086 (SD), 0.063 (SD), 0.051 (SD), 0.040 (SD), and 0.029 (SD), which is limited by counting statistics of the isotopic signals. Furthermore, the achieved standard error of 109/107Ag can be reduced to sub-permil level (0.7 ‰) even for the measurement of 20 nm AgNPs (N = 17,000). These results demonstrate that the ETSC provides a unique method for isotope analysis of single particles, holding great potential for enhancing our understanding of nanoparticles.
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  • 文章类型: Journal Article
    金属基纳米粒子(MNPs)越来越多地释放到海洋环境中,潜在的环境风险。然而,控制海湾MNPs环境发生和分布的因素仍然缺乏全面的了解。在这里,我们从两个相邻的海湾(大亚湾和红海湾,具有相似的水质),并确定了多元素MNPs的颗粒浓度和大小(Ti-,Cu-,Zn-,Ag-,Mn-,基于Pb和Cr的NP)通过单颗粒电感耦合等离子体质谱法(spICP-MS)。大亚湾的内部循环导致海水和沉积物中MNPs的颗粒浓度和大小均匀分布,而红海湾的陆地排放导致MNPs浓度从近岸到近海呈梯度下降趋势。此外,红海湾MNPs相对较高的丰度,造成了比大亚湾高2.35倍的环境风险。总的来说,这项研究为塑造MNPs发生和分布的关键但被忽视的因素提供了确凿的证据,为风险管理和排放监管提供新的见解。
    Metal-based nanoparticles (MNPs) are increasingly being released into the marine environment, posing potential environmental risks. However, factors governing the environmental occurrence and distribution of MNPs in bays still lack a comprehensive understanding. Herein, we collected seawater and sediment samples from two adjacent bays (Daya Bay and Honghai Bay, which have similar water qualities), and determined the particle concentrations and sizes of multi-element MNPs (Ti-, Cu-, Zn-, Ag-, Mn-, Pb- and Cr-based NPs) via single particle inductively coupled plasma-mass spectrometry (spICP-MS). The internal circulation in Daya Bay has resulted in an even distribution of MNPs\' particle concentrations and sizes in both seawater and sediments, while the terrestrial discharge in Honghai Bay has led to a gradient-decreasing trend in MNPs\' concentrations from nearshore to offshore. Moreover, the relatively high abundance of MNPs in Honghai Bay has contributed to 2.35-fold higher environmental risks than Daya Bay. Overall, this study has provided solid evidence on the critical but overlooked factors that have shaped the occurrence and distribution of MNPs, providing new insights for risk management and emission regulation.
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  • 文章类型: Journal Article
    合理快速设计高性能材料的关键是实时监测和理解单个颗粒内的动态过程,特别是深入了解纳米粒子的各向异性。在现实的工作条件下,纳米粒子的固有特性通常从一个晶面到下一个晶面变化。这里,我们引入操作碰撞电化学来解决光电化学中的单银纳米棱柱(AgNP)各向异性。我们直接确定了各向异性对单一NP/电解质界面处等离子体辅助电化学的影响。统计碰撞频率表明,晶体晶面之间的异质扩散系数有助于AgNP向金超微电极进行方向依赖的传质。随后,瞬态事件的电流幅度表明,各向异性使得在光热过程中动态界面电子转移行为发生变化。这里提出的结果表明,碰撞电化学的测量精度可以扩展到亚纳米粒子水平,通过纳米级的全面动力学信息,突出了高通量材料筛选的潜力。
    The key to rationally and rapidly designing high-performance materials is the monitoring and comprehension of dynamic processes within individual particles in real-time, particularly to gain insight into the anisotropy of nanoparticles. The intrinsic property of nanoparticles typically varies from one crystal facet to the next under realistic working conditions. Here, we introduce the operando collision electrochemistry to resolve the single silver nanoprisms (Ag NPs) anisotropy in photoelectrochemistry. We directly identify the effect of anisotropy on the plasmonic-assisted electrochemistry at the single NP/electrolyte interface. The statistical collision frequency shows that heterogeneous diffusion coefficients among crystal facets facilitate Ag NPs to undergo direction-dependent mass transfer toward the gold ultramicroelectrode. Subsequently, the current amplitudes of transient events indicate that the anisotropy enables variations in dynamic interfacial electron transfer behaviors during photothermal processes. The results presented here demonstrate that the measurement precision of collision electrochemistry can be extended to the sub-nanoparticle level, highlighting the potential for high-throughput material screening with comprehensive kinetics information at the nanoscale.
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  • 文章类型: Journal Article
    作为电动汽车,便携式电子设备和工具对电池能量密度和功率密度的要求越来越高,不断提高电池性能成为研究热点。准确测量活性材料的构效关系是推进高性能电池研究的关键。然而,活性材料的常规性能测试是基于含有活性材料的多孔复合电极的电化学测量,聚合物粘合剂,和导电碳添加剂,这不能与微区的物理表征建立准确的结构-活性关系。在这次审查中,为了促进对材料结构-活性关系的准确测量和理解,综述了单粒子尺度下储能材料的电化学测量和物理表征。提出了单粒子电化学测量和物理表征的潜在问题和可能的改进方案。展望了它们在单粒子电化学模拟和机器学习中的潜在应用。本文旨在促进单粒子电化学测量和物理表征在储能材料中的进一步应用。希望实现三维统一的物理表征评价,电化学测量,单粒子尺度下的理论模拟,为高性能电池的发展提供新的启示。本文受版权保护。保留所有权利。
    As electric vehicles, portable electronic devices, and tools have increasingly high requirements for battery energy density and power density, constantly improving battery performance is a research focus. Accurate measurement of the structure-activity relationship of active materials is key to advancing the research of high-performance batteries. However, conventional performance tests of active materials are based on the electrochemical measurement of porous composite electrodes containing active materials, polymer binders, and conductive carbon additives, which cannot establish an accurate structure-activity relationship with the physical characterization of microregions. In this review, in order to promote the accurate measurement and understanding of the structure-activity relationship of materials, the electrochemical measurement and physical characterization of energy storage materials at single-particle scale are reviewed. The potential problems and possible improvement schemes of the single particle electrochemical measurement and physical characterization are proposed. Their potential applications in single particle electrochemical simulation and machine learning are prospected. This review aims to promote the further application of single particle electrochemical measurement and physical characterization in energy storage materials, hoping to achieve 3D unified evaluation of physical characterization, electrochemical measurement, and theoretical simulation at the single particle scale to provide new inspiration for the development of high-performance batteries.
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  • 文章类型: Journal Article
    氧化有机分子(OOMs)的形成和老化过程对于了解该领域二次有机气溶胶(SOA)的形成机理非常重要。在这项研究中,我们调查了OOM颗粒的混合状态,通过确定几个含氧物种以及次级有机碳(SOC)在清洁和臭氧(O3)污染期间的分布2022年7月和9月在广州,中国。7月和9月,含OOM的颗粒分别占检测到的单个颗粒总数的57%和49%,分别。大多数OOM颗粒内部与硫酸盐和硝酸盐混合,而元素碳和碳氢化合物物种不存在。尽管9月份的SOC/OC比率(81%)高于7月份的SOC/OC比率(72%),质谱的比较研究,昼夜模式,OOM颗粒的分布表明,在两个O3污染时期,OOM的组成和老化状态相同。随着O3浓度从清洁期增加到污染期,SOC与OC的比值随着总OOM颗粒中次级OOM颗粒的相对丰度而增加。相比之下,OC型OOM粒子的相对丰度逐渐降低,表明随着SOC/OC比率的增加,烃类物质转化为OOM。通过过滤器测量对SOC的整体分析和OOM颗粒的混合状态都表明,在O3污染时期,OOM的产生和氧化程度高于清洁时期。这些结果阐明了O3污染对OOM形成过程的影响,并为基于过滤器采样和单颗粒测量的SOA生产联合研究提供了新的视角。
    The formation and aging processes of oxygenated organic molecules (OOMs) are important for understanding the formation mechanisms of secondary organic aerosols (SOAs) in the field. In this study, we investigated the mixing states of OOM particles by identifying several oxygenated species along with the distributions of secondary organic carbon (SOC) during both clean and ozone (O3)-polluted periods in July and September of 2022 in Guangzhou, China. OOM-containing particles accounted for 57 % and 49 % of the total detected single particles in July and September, respectively. Most of the OOM particles were internally mixed with sulfate and nitrate, while elemental carbon and hydrocarbon species were absent. Despite the higher SOC/OC ratio in September (81 %) than it in July (72 %), comparative investigations of the mass spectra, diurnal patterns, and distributions of OOM particles revealed the same composition and aging states of OOMs in two O3 pollution periods. As the O3 concentration increased from the clean to the polluted periods, the ratio of SOC to OC increased along with the relative abundance of secondary OOM particles among total OOM particles. In contrast, the relative abundance of OC-type OOM particles gradually decreased, indicating the conversion of hydrocarbon species into OOMs as the SOC/OC ratio increased. Both the bulk analysis of SOC from filter measurement and the mixing states of OOM particles suggested that OOM production and degree of oxidation were higher in the O3-polluted periods than in the clean periods. These results elucidate the effects of O3 pollution on the OOM formation process and offer new perspectives for the joint investigation of SOA production based on filter sampling and single-particle measurements.
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  • 文章类型: Journal Article
    在本研究中,我们提出了一种通过吸附在单个二氧化硅颗粒上的辣根过氧化物酶(HRP)和荧光显微光谱法检测H2O2的方案。当二氧化硅颗粒浸入HRP溶液中时,由于HRP吸附在二氧化硅表面,因此与本体水溶液相比,二氧化硅颗粒中的HRP浓度增加了690倍。当将含有HRP的单个颗粒添加到H2O2和AmplexRed的混合溶液中时,来自间苯二酚的荧光,它是由HRP反应产生的,H2O2和Amplex红,被观察到。在溶液中加入单个颗粒后,来自颗粒中的间苯二酚的荧光增加,并观察到间苯二酚的释放。随着H2O2(CH2O2)浓度的降低,荧光强度达到最大值所需的时间较短。在本系统中H2O2的检测极限为980nM。使用球形扩散模型评估了单个二氧化硅颗粒的反应行为,这解释了二氧化硅颗粒中间苯二酚的近似浓度变化。该方法具有样品制备和检测简单的优点,低样品消耗,和一个短的检测时间。
    In the present study, we propose a scheme for detecting H2O2 by using horseradish peroxidase (HRP) adsorbed onto single silica particles and fluorescence microspectroscopy. When the silica particles were immersed in an HRP solution, the HRP concentration in the silica particles increased by a factor of 690 compared to that in the bulk aqueous solution because HRP was adsorbed on the silica surface. When a single particle containing HRP was added to a mixed solution of H2O2 and Amplex Red, fluorescence from resorufin, which was produced by the reaction of HRP, H2O2, and Amplex Red, was observed. The fluorescence from the resorufin in the particles increased after a single particle was added to the solution, and the release of resorufin was observed. As the concentration of H2O2 (CH2O2) decreased, the time it takes for fluorescence intensity to reach its maximum was shorter. The detection limit for H2O2 in the present system was 980 nM. The reaction behavior of a single silica particle was evaluated using a spherical diffusion model, which explains the approximate concentration change of resorufin in the silica particle. The proposed method has the advantages of simple sample preparation and detection, low sample consumption, and a short detection time.
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  • 文章类型: Journal Article
    当前通过单粒子电感耦合等离子体质谱法分析土壤中纳米材料(NMs)的样品制备策略在准确性方面存在重大限制。样品通量和适用性(即,NMs和土壤的类型)。在这项工作中,系统研究了微波辅助萃取(MAE)对土壤NMs表征的优缺点。为此,测试了不同的萃取剂(超纯水;NaOH,NH4OH,柠檬酸钠和焦磷酸四钠)和MAE操作条件通过实验设计进行了优化。接下来,所开发的方法适用于不同类型的金属(oid)纳米粒子(Se-,Ag-,PT-和AuNP)和土壤(碱性,酸,sandy,clayey,SL36,壤土ERMCC141;污泥修正ERM483)。结果表明,通过使用20mL的0.1MNaOH溶液,可以在800W烘箱中在6分钟(12个循环,每个循环30s)内保存并从土壤中定量提取Pt和AuNPs。该方法适用于除富含粘土的样品外,具有广泛理化性质的土壤。如果黏土分数显著(>15%),NMs被有效地保留在土壤中,从而导致不良的回收率(<10%)。通过这种方法分析不稳定的NM例如Se-和AgNPs是不可行的,因为提取条件有利于溶解。最后,与目前的提取方法相比(例如,超声,浊点提取,等。),由于处理速度和同时处理多个样品的可能性,MAE提供更好或相当的准确度和精密度以及更高的样品处理量。
    Current sample preparation strategies for nanomaterials (NMs) analysis in soils by means single particle inductively coupled plasma mass spectrometry have significant constrains in terms of accuracy, sample throughput and applicability (i.e., type of NMs and soils). In this work, strengths and weakness of microwave assisted extraction (MAE) for NMs characterization in soils were systematically investigated. To this end, different extractants were tested (ultrapure water; NaOH, NH4OH, sodium citrate and tetrasodium pyrophosphate) and MAE operating conditions were optimized by means of design of experiments. Next, the developed method was applied to different type of metallic(oid) nanoparticles (Se-, Ag-, Pt- and AuNPs) and soils (alkaline, acid, sandy, clayey, SL36, loam ERMCC141; sludge amended ERM483). Results show that Pt- and AuNPs are preserved and quantitatively extracted from soils in 6 min (12 cycles of 30 s each) inside an 800 W oven by using 20 mL of 0.1 M NaOH solution. This methodology is applicable to soils showing a wide range of physicochemical properties except for clay rich samples. If clay soil fraction is significant (>15%), NMs are efficiently retained in the soil thus giving rise to poor recoveries (<10%). The analysis of labile NMs such as Se- and AgNPs is not feasible by means this approach since extraction conditions favors dissolution. Finally, when compared to current extraction methodologies (e.g., ultrasound, cloud point extraction, etc.), MAE affords better or equivalent accuracies and precision as well as higher sample throughput due to treatment speed and the possibility to work with several samples simultaneously.
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  • 文章类型: Journal Article
    纳米材料通过控制药物的药代动力学,彻底改变了医学,生物分布,和生物相容性。然而,大多数纳米治疗批次是高度异质的,意味着它们包含大小不同的纳米粒子,形状,charge,composition,和配体官能化。同样,单个纳米治疗剂通常具有异质分布的成分,配体,和收费。这篇综述讨论了纳米治疗异质性的来源和对实验读数和治疗效果的影响。在其他主题中,它表明异质性存在于几乎所有的纳米治疗类型,检查纳米治疗异质性是如何产生的,并讨论了异质性如何影响纳米材料的体外和体内行为。还显示了纳米治疗异质性如何扭曲实验读数并使其优化和临床翻译复杂化。最后,综述了限制纳米治疗异质性的策略,并提供了开发更可重复和有效的纳米治疗的建议.
    Nanomaterials have revolutionized medicine by enabling control over drugs\' pharmacokinetics, biodistribution, and biocompatibility. However, most nanotherapeutic batches are highly heterogeneous, meaning they comprise nanoparticles that vary in size, shape, charge, composition, and ligand functionalization. Similarly, individual nanotherapeutics often have heterogeneously distributed components, ligands, and charges. This review discusses nanotherapeutic heterogeneity\'s sources and effects on experimental readouts and therapeutic efficacy. Among other topics, it demonstrates that heterogeneity exists in nearly all nanotherapeutic types, examines how nanotherapeutic heterogeneity arises, and discusses how heterogeneity impacts nanomaterials\' in vitro and in vivo behavior. How nanotherapeutic heterogeneity skews experimental readouts and complicates their optimization and clinical translation is also shown. Lastly, strategies for limiting nanotherapeutic heterogeneity are reviewed and recommendations for developing more reproducible and effective nanotherapeutics provided.
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