mass transport

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  • 文章类型: Journal Article
    高效的电化学能量转换技术,如燃料电池和水电解槽,需要高电流密度以降低大规模商业化的资本成本,但通常受到质量传输的限制。在这项研究中,我们在质子电解质膜水电解槽(PEMWE)中展示了出色的电化学性能,使用皮秒激光在多孔传输层(MPCPTL)中创建了微图案化的孔通道。这种方法产生了1.82V@2A·cm-2的令人印象深刻的性能,优于商业PTL1.90V@2Acm-2。显著的性能增强归因于微图案化的多孔通道结构,促进氧气气泡的有效排出和反应物水的输入。这项工作为电化学能量转换技术中负责双相传输的PTL的设计提供了有价值的见解。
    Efficient electrochemical energy conversion technologies, such as fuel cells and water electrolyzers, require high current densities to lower the capital cost for large-scale commercialization but are often limited by mass transport. In this study, we demonstrated exceptional electrochemical performances in proton electrolyte membrane water electrolyzers (PEMWEs) creating micropatterned pore channels in the porous transport layer (MPC PTL) using a picosecond laser. This approach yielded an impressive performance of 1.82 V @ 2 A·cm-2, which is better than commercial PTL of 1.90 V @ 2 A cm-2. The significant performance enhancement is attributed to the micropatterned porous channel structure, facilitating the efficient expulsion of oxygen bubbles and input of reactant water. This work provides valuable insights for the design of PTL responsible for biphasic transport in electrochemical energy conversion technologies.
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  • 文章类型: Journal Article
    通过电穿孔的药物递送对于治疗人体内不同类型的患病组织可能是非常有益的。在这项工作中,提出了一个可逆组织电穿孔的数学模型,用于将药物注射到病变细胞中。该模型强调注射药物的组织边界作为点源。此外,详细研究了药物通过细胞外空间在组织边界丢失的影响。施加多个脉冲以将足够量的药物递送到靶细胞中。对物理环境进行建模的微分方程组进行数值求解。该模型获得传质系数(MTC),就控制药物从细胞外空间向细胞内空间转运的孔分数系数和药物渗透性而言。为了施加不同的脉冲,捕获贯穿组织的药物渗透。在这项研究中强调了对药物浓度的边界影响。提倡的模型能够进行均匀的药物转运到细胞中,从而完全治疗受影响的组织。该模型可用于通过避免冗长且昂贵的体内和体外实验来优化临床实验。
    Drug delivery through electroporation could be highly beneficial for the treatment of different types of diseased tissues within the human body. In this work, a mathematical model of reversible tissue electroporation is presented for injecting drug into the diseased cells. The model emphasizes the tissue boundary where the drug is injected as a point source. In addition, the effect of drug loss at tissue boundaries through extracellular space is studied elaborately. Multiple pulses are applied to deliver a sufficient amount of drug into the targeted cells. The set of differential equations that model the physical circumstances are solved numerically. This model obtains a mass transfer coefficient (MTC), in terms of pore fraction coefficient and drug permeability that controls the drug transport from extracellular to intracellular space. The drug penetration throughout the tissue is captured for the application of different pulses. The boundary effects on drug concentration are highlighted in this study. The advocated model is able to perform homogeneous drug transport into the cells so that the affected tissue is treated completely. This model can be applied to optimize clinical experiments by avoiding the lengthy and costly in vivo and in vitro experiments.
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  • 文章类型: Journal Article
    近岸区域原来是塑料碎片浓度较高的区域,出于这个原因,重要的是要了解影响这种垃圾的运输和命运的过程。这项研究的重点是研究主要由波浪引起的几种流体动力学条件下各种塑料类型的动力学。2D测试是在Messina大学的液压实验室进行的,再现了波在平面海滩上传播期间发生的主要现象。测试了200多个不同的条件,改变了波浪特性,水深,塑料碎片特性(密度和形状),和固定底部的粗糙度。总的来说,可以观察到,颗粒位移的减少是由于:i)波陡度降低;ii)深度增加;iii)颗粒尺寸增加;iv)塑性密度增加。然而,实验研究表明,一些塑性特性和床层粗糙度,即使液压平稳,可以改变这些结果。实验数据分析确定了预测波浪作用下塑料碎片短期命运的标准。这个标准来确定平衡条件,基于经验关系,考虑到波浪的特性,床层粗糙度和坡度,还有碎片的重量.
    The nearshore zone turns out to be the area with the higher concentration of plastic debris and, for this reason, it is important to know the processes that affect the transport and the fate of this type of litter. This study focuses on investigating the dynamics of various plastic types under several hydrodynamic conditions primarily induced by waves. 2D tests were carried out at the Hydraulic Laboratory of the University of Messina reproducing the main phenomena that occurred during the wave propagation on a planar beach. More than 200 different conditions were tested changing the wave characteristics, the water depth, the plastic debris characteristics (density and shape), and the roughness of the fixed bottom. In general, it can be observed that the reduction in particle displacement occurs due to: i) a decrease in wave steepness; ii) an increase in depth; iii) an increase in particle size; iv) an increase in plastic density. However, the experimental investigation shows that some plastic characteristics and bed roughness, even when hydraulically smooth, can alter these results. The experimental data analysis identified a criterion for predicting the short-term fate of plastic debris under wave action. This criterion to determine equilibrium conditions, based on an empirical relationship, takes into account the wave characteristics, the bed roughness and slope, and the weight of the debris.
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  • 文章类型: Journal Article
    该研究的假设是(1)3D打印药物递送系统(DDS)可以在药物释放过程中使用NMR/MRI技术在传质现象描述(界面现象)方面进行原位表征,特别是对于处理两个流动相的系统(例如,水和低分子量液体聚合物);(2)因此,可以推断这些界面传质现象如何影响3D打印DDS的功能特性。基质给药系统,使用掩模立体光刻(MSLA)制备,作为示例制剂,研究了含有聚(乙二醇)二丙烯酸酯(PEGDA)和低分子量聚乙二醇(PEG)以及盐酸罗匹尼罗(RH)的制剂。PEGDA与PEG(流动相)浓度比影响药物释放。反映在使用磁共振成像(MRI)获得的参数T2弛豫时间(T2)和振幅(A)图像的时空变化中,以及使用低场时域核磁共振(LFTDNMR)弛豫法获得的T1-T2弛豫时间相关性在水中孵育期间。对于大多数测试的配方,通过MRI弛豫测定法(参数T2/A图像)评估水合基质中与PEG和水相关的两个信号分量。PEG组分由于PEG向外扩散而淡出,并逐渐被水组分取代。这两个组件在空间和时间上都改变了它们的参数,反映不断发展的水-聚合物相互作用。研究表明,与双向传质相关的动态现象可以使用NMR和MRI技术原位量化,以深入了解3D打印DDS系统的药物释放机制。
    The hypothesis of the study was that (1) 3D printed drug delivery systems (DDS) could be characterized in situ during drug release using NMR/MRI techniques in terms of mass transport phenomena description (interfacial phenomena), particularly for systems dealing with two mobile phases (e.g., water and low molecular weight liquid polymer); (2) consequently, it could be possible to deduce how these interfacial mass transport phenomena influence functional properties of 3D printed DDS. Matrix drug delivery systems, prepared using masked stereolithography (MSLA), containing poly(ethylene glycol) diacrylate (PEGDA) and low molecular weight polyethylene glycol (PEG) with ropinirole hydrochloride (RH) were studied as example formulations. The PEGDA to PEG (mobile phase) concentration ratio influenced drug release. It was reflected in spatiotemporal changes in parametric T2 relaxation time (T2) and amplitude (A) images obtained using magnetic resonance imaging (MRI) and T1-T2 relaxation time correlations obtained using low-field time-domain nuclear magnetic resonance (LF TD NMR) relaxometry during incubation in water. For most of the tested formulations, two signal components related to PEG and water were assessed in the hydrated matrices by MRI relaxometry (parametric T2/A images). The PEG component faded out due to outward PEG diffusion and was gradually replaced by the water component. Both components spatially and temporally changed their parameters, reflecting evolving water-polymer interactions. The study shows that dynamic phenomena related to bidirectional mass transport can be quantified in situ using NMR and MRI techniques to gain insight into drug release mechanisms from 3D printed DDS systems.
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  • 文章类型: Journal Article
    生物系统中毛细管力的力学在细胞内和细胞间结构的形成中起着关键作用,可以调解组织,形态发生,和生物分子缩合物的稳态。目前的技术可能不允许在细胞内和细胞间尺度下直接和精确测量毛细管力。通过在液-液界面保留液滴,我们发现并研究了理想模型,即,界面液体和大理石,为了理解存在于液体中的液体系统中的一般毛细管力学,例如,生物分子缩合物。界面液体的出乎意料的长聚结时间表明,当液桥的半径接近零时,斯托克斯方程不成立。证明存在第三种惯性有限的粘性体系。此外,可以通过用疏水或两亲性颗粒涂覆液滴表面来阻止从液滴到液体储存器的液体输送,形成界面液体大理石。独特的特点,包括高稳定性,透明度,气体渗透率,和自组装,观察到界面液体大理石。由纳米结构材料的形成引起的相变和分离可以在界面液体大理石内直接观察到,而不需要表面活性剂和搅拌,使它们成为研究界面力学的有用工具。
    The mechanics of capillary force in biological systems have critical roles in the formation of the intra- and inter-cellular structures, which may mediate the organization, morphogenesis, and homeostasis of biomolecular condensates. Current techniques may not allow direct and precise measurements of the capillary forces at the intra- and inter-cellular scales. By preserving liquid droplets at the liquid-liquid interface, we have discovered and studied ideal models, i.e., interfacial liquids and marbles, for understanding general capillary mechanics that existed in liquid-in-liquid systems, e.g., biomolecular condensates. The unexpectedly long coalescence time of the interfacial liquids revealed that the Stokes equation does not hold as the radius of the liquid bridge approaches zero, evidencing the existence of a third inertially limited viscous regime. Moreover, liquid transport from a liquid droplet to a liquid reservoir can be prohibited by coating the droplet surface with hydrophobic or amphiphilic particles, forming interfacial liquid marbles. Unique characteristics, including high stability, transparency, gas permeability, and self-assembly, are observed for the interfacial liquid marbles. Phase transition and separation induced by the formation of nanostructured materials can be directly observed within the interfacial liquid marbles without the need for surfactants and agitation, making them useful tools to research the interfacial mechanics.
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  • 文章类型: Journal Article
    对控制金属纳米结构上热载流子反应性的机制的解释至关重要,然而难以捉摸,推进等离子体光催化。在这项工作中,我们探索了分子扩散对固液界面处的热载流子提取速率的影响,这是提高光电器件效率的根本利益。通过空间定义的扫描光电化学显微镜研究,我们确定了一种扩散控制的机制,阻碍了等离子体驱动的金属纳米结构的光化学活性。使用低功率单色照明(<2Wcm-2),我们揭示了质量传输对等离子体光催化剂量子效率的潜在影响。分子在固液界面的可用性直接限制了热孔的提取,根据他们的性质和能量,在超薄TiO2衬底上Au纳米岛的反应点上。出现了一个有趣的问题:由热效应引起的质量传输增强是否解锁了稳态下非热载体的反应性?
    The interpretation of mechanisms governing hot carrier reactivity on metallic nanostructures is critical, yet elusive, for advancing plasmonic photocatalysis. In this work, we explored the influence of the diffusion of molecules on the hot carrier extraction rate at the solid-liquid interface, which is of fundamental interest for increasing the efficiency of photodevices. Through a spatially defined scanning photoelectrochemical microscopy investigation, we identified a diffusion-controlled regime hindering the plasmon-driven photochemical activity of metallic nanostructures. Using low-power monochromatic illumination (<2 W cm-2), we unveiled the hidden influence of mass transport on the quantum efficiency of plasmonic photocatalysts. The availability of molecules at the solid-liquid interface directly limits the extraction of hot holes, according to their nature and energy, at the reactive spots in Au nanoislands on an ultrathin TiO2 substrate. An intriguing question arises: does the mass transport enhancement caused by thermal effects unlock the reactivity of nonthermal carriers under steady state?
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  • 文章类型: Journal Article
    将金属有机骨架(MOF)集成到复合体系中作为提高这些材料的可加工性的有效策略。值得注意的是,MOF/纤维复合材料作为捕获和修复化学战剂的防护设备显示出很大的希望。然而,这些复合材料的实际应用需要了解它们的质量传输特性,因为表面处的传质阻力和材料内的扩散都会影响这些材料的功效。在这项工作中,我们合成了MOF-808和胺肟官能化的固有微孔聚合物(PIM-1-AX)的复合纤维,并测量了正己烷和2-氯乙基乙基硫醚(CEES)的吸附和传质行为,硫磺芥末模拟物。我们开发了一种新的圆柱形Fickian扩散模型,以适应从商业容积吸附装置获得的动态吸附数据,并发现复合纤维中的传质行为与纯PIM纤维中的传质行为非常相似。无论MOF加载。此外,我们发现正己烷吸附反映了CEES,表明它可以用作未来的硫芥子气模拟物吸附研究的结构模拟物。这些初步的见解和这项工作中引入的新模型为设计用于实际应用的下一代复合材料奠定了基础。
    The integration of metal-organic frameworks (MOFs) into composite systems serves as an effective strategy to increase the processability of these materials. Notably, MOF/fiber composites have shown much promise as protective equipment for the capture and remediation of chemical warfare agents. However, the practical application of these composites requires an understanding of their mass transport properties, as both mass transfer resistance at the surface and diffusion within the materials can impact the efficacy of these materials. In this work, we synthesized composite fibers of MOF-808 and amidoxime-functionalized polymers of intrinsic microporosity (PIM-1-AX) and measured the adsorption and mass transport behavior of n-hexane and 2-chloroethyl ethyl sulfide (CEES), a sulfur mustard simulant. We developed a new Fickian diffusion model for cylindrical shapes to fit the dynamic adsorption data obtained from a commercial volumetric adsorption apparatus and found that mass transport behavior in composite fibers closely resembled that in the pure PIM fibers, regardless of MOF loading. Moreover, we found that n-hexane adsorption mirrors that of CEES, indicating that it could be used as a structural mimic for future adsorption studies of the sulfur mustard simulant. These preliminary insights and the new model introduced in this work lay the groundwork for the design of next-generation composite materials for practical applications.
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  • 文章类型: Journal Article
    在纳米多孔材料中通常观察到表面屏障。尽管研究人员已经探索了修复缺陷或制造完美无瑕的晶体以减轻表面屏障的方法,这些方法在靶向金属-有机骨架(MOF)中可能不总是实用的或容易实现的。在我们的研究中,我们提出了一种替代方法,重点是将多种配体引入到MOF-808节点上,以精细调节其吸附和传质特性。重要的是,我们的发现表明,虽然吸附曲线可以根据MOF的化学组成和探测分子推断,表面渗透性根据所使用的特定探针和掺入的配体表现出变化。我们的调查,考虑仅在被吸附物之间的范德华力(例如,正己烷,丙烷,和苯)和吸附剂,表明,增加这些相互作用确实可以在一定程度上改善表面渗透。相反,氢键相互作用产生的强吸附,特别是改性MOFs中的水,导致MOF晶体内渗透受损。这些结果为多孔材料社区提供了有价值的见解,并为开发对气体和蒸气具有增强的亲和力和优越的传质性能的吸附剂提供了指导。
    Surface barriers are commonly observed in nanoporous materials. Although researchers have explored methods to repair defects or create flawless crystals to mitigate surface barriers, these approaches may not always be practical or readily achievable in targeted metal-organic frameworks (MOFs). In our study, we propose an alternative approach focusing on the introduction of diverse ligands onto a MOF-808 node to finely adjust its adsorption and mass transport characteristics. Significantly, our findings indicate that while adsorption curves can be inferred based on the MOF\'s chemical composition and the probing molecule, surface permeabilities exhibit variations dependent on the specific probe utilized and the incorporated ligand. Our investigation, considering van der Waals forces exclusively between the adsorbate (e.g., n-hexane, propane, and benzene) and the adsorbent, revealed that augmenting these interactions can indeed improve surface permeation to a certain extent. Conversely, strong adsorption resulting from hydrogen bonding interactions, particularly with water in modified MOFs, led to compromised permeation within the MOF crystals. These outcomes provide valuable insights for the porous materials community and offer guidance in the development of adsorbents with enhanced affinity and superior mass transport properties for gases and vapors.
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  • 文章类型: Journal Article
    在这一章中,我们介绍了装置的设计和制造以及方案的实施,以实现微量滴定板内免疫测定效率的提高。该装置,WellProbe,是一种3D结构的探头,可用于在标准孔板底部提供精确的流量,以使用流体动力限制的流量建立剪切应力强度的同心区域。协议涉及操作和数据分析。
    In this chapter, we present the design and fabrication of a device and implementation of a protocol to realize increased efficiency of immunoassays within microtiter plates. The device, WellProbe, is a 3D-structured probe that can be used to deliver precise flows at the bottom of standard well plates to establish concentric areas of shear stress intensities using hydrodynamically confined flows. The protocols involve both operation and data analysis.
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  • 文章类型: Journal Article
    在零间隙气相光电电解槽中使用基于UiO-66-NH2的改性金属有机框架光电阴极进行CO2还原。采用四种具有不同润湿性的多孔碳纤维层来定制阴极表面反应的局部环境。优化对甲酸盐的活性和选择性,甲醇,和乙醇。结果可以通过光电阴极中碳纤维支撑层的不同类型和排列以及UiO-66-NH2催化剂上产生的局部环境的质量传输来解释。使用最疏水性的碳纤维(H23C2)可实现对碳氢化合物的1.06%的最高能量到燃料转化效率。结果是进一步理解光电化学电解槽中电极的设计和组成如何影响CO2还原效率和选择性的步骤。
    A modified Metal-Organic Framework UiO-66-NH2-based photocathode in a zero-gap gas phase photoelectrolyzer was applied for CO2 reduction. Four types of porous carbon fiber layers with different wettability were employed to tailor the local environment of the cathodic surface reactions, optimizing activity and selectivity towards formate, methanol, and ethanol. Results are explained by mass transport through the different type and arrangement of carbon fiber support layers in the photocathodes and the resulting local environment at the UiO-66-NH2 catalyst. The highest energy-to-fuel conversion efficiency of 1.06 % towards hydrocarbons was achieved with the most hydrophobic carbon fiber (H23C2). The results are a step further in understanding how the design and composition of the photoelectrodes in photoelectrochemical electrolyzers can impact the CO2 reduction efficiency and selectivity.
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