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Crack patterns of black ink film: sumi-wari. 黑墨薄膜的裂纹图案:sumi-wari。
IF 2.8 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2026-03-17 DOI: 10.1039/d5sm01281c
Michiko Shimokawa, Lucas Goehring, Akie Kinoshita, Ludovic Pauchard, Hidetsugu Sakaguchi

Local variations in surface tension can induce complex fracture dynamics in thin interfacial films. Here, we investigate the fracture patterns that emerge when a localized surface-tension perturbation is applied to a sumi film supported on a water-glycerol subphase. Sumi is a traditional Japanese carbon black ink, and this process, referred to as sumi-wari, produces aesthetically pleasing, star-shaped crack patterns with multiple spikes radiating from the perturbation site. The number of crack spikes increases with the viscosity of the subphase, controlled here by the addition of glycerol. Atomic force microscopy measurements reveal that the effective stiffness of the sumi film decreases as glycerol concentration increases. This suggests a strong coupling between the subphase properties and the mechanics of the sumi film. To capture the dynamics of sumi-wari, a phenomenological model is outlined, based on an overdamped equation of motion for particles connected by breakable springs. Numerical simulations reproduce both the morphology and the experimental trends of sumi-wari: the number of cracks and their temporal evolution depend on the spring stiffness, mirroring the behavior observed for subphases with different viscosities. These findings demonstrate how the interplay between surface-tension gradients, subphase properties, and film mechanics governs local fracture and pattern formation in fluid-supported thin films.

表面张力的局部变化可引起薄界面膜中复杂的断裂动力学。在这里,我们研究了当局部表面张力扰动应用于水-甘油亚相支撑的sumi膜时出现的断裂模式。Sumi是一种传统的日本炭黑墨水,这一过程被称为Sumi -wari,它会产生美观的星形裂纹图案,从扰动处辐射出多个尖峰。裂纹尖峰的数量随着亚相粘度的增加而增加,这里通过添加甘油来控制。原子力显微镜测量显示,随着甘油浓度的增加,sumi膜的有效刚度降低。这表明在sumi薄膜的亚相性质和力学之间有很强的耦合。为了捕捉sumi-wari的动力学,基于由可断裂弹簧连接的粒子的过阻尼运动方程,概述了一个现象学模型。数值模拟再现了sumi-wari的形态和实验趋势:裂纹的数量及其时间演变取决于弹簧刚度,反映了不同粘度的子相的行为。这些发现证明了表面张力梯度、亚相性质和薄膜力学之间的相互作用如何控制流体支撑薄膜的局部断裂和图案形成。
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引用次数: 0
Mechanisms of electrolyte (coagulant) dipping for thin nitrile gloves. 薄丁腈手套电解液(混凝剂)浸渍机理。
IF 2.8 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2026-03-17 DOI: 10.1039/d5sm01262g
Robert Groves, Kota Hatakeyama, Alexander F Routh

Two mechanisms for film deposition during the electrolyte dipping process are examined. The conventional, widely accepted, mechanism proposes that electrolyte on a former, immersed in latex compound for a controlled dwell time, diffuses into the compound and a wet gel coagulates on the former where the electrolyte concentration is above the critical coagulation value. An alternative mechanism proposes that deposition occurs via particle movement towards the former, driven by diffusiophoresis. The two mechanisms are examined using dipping nitrile latex compound and various mono and divalent cation electrolytes. The similarity of the total solids content (TSC) of the deposit on the former to that of the compound, the coagulated nature of the deposit and the success, at short dwell times, of a diffusion-coagulation model show that diffusion and coagulation operates exclusively for the divalent cations. For the monovalent cation electrolytes, this mechanism is also dominant, but the TSC of the deposits suggests that diffusiophoresis also plays a small part in the deposition process. A model for the two mechanisms acting together was devised and applied to deposition given by three monovalent electrolytes. This gave deposit TSCs that agreed with the diffusiophoretic prediction and was independent of dwell time. Quantitatively, the calculated amounts of deposit agreed reasonably well with experiment. The model therefore provides some support for diffusiophoresis affecting deposition for monovalent electrolytes. The reason(s) for the different diffusiophoresis behaviour of the monovalent and divalent electrolytes is suggested to be due to the much lower critical coagulation concentration for the divalent cations.

研究了电解液浸镀过程中膜沉积的两种机制。传统的、被广泛接受的机制是,电解质在前者上浸入乳胶化合物中一段受控的停留时间,扩散到化合物中,当电解质浓度高于临界凝固值时,湿凝胶在前者上凝固。另一种机制提出,沉积是由扩散电泳驱动的粒子向前者运动而发生的。用浸渍丁腈乳胶复合物和各种一价和二价阳离子电解质考察了这两种机理。沉积物的总固体含量(TSC)与化合物的总固体含量(TSC)相似,沉积物的凝固性质以及在短停留时间内成功的扩散-混凝模型表明,扩散和混凝只对二价阳离子起作用。对于单价阳离子电解质,这一机制也占主导地位,但沉积物的TSC表明扩散电泳在沉积过程中也起着很小的作用。设计了两种机制共同作用的模型,并将其应用于三种单价电解质的沉积。这使得沉积的tsc与扩散电泳预测一致,并且不受停留时间的影响。定量计算结果与实验结果吻合较好。因此,该模型为影响单价电解质沉积的扩散电泳提供了一些支持。一价电解质和二价电解质的扩散电泳行为不同的原因是由于二价阳离子的临界凝固浓度要低得多。
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引用次数: 0
Tunable thin elasto-drops. 可调的薄弹性滴。
IF 2.8 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2026-03-16 DOI: 10.1039/d5sm01192b
A Eddi, S Perrard, J Zhang

We present an experimental method to fabricate centimetric thin elastic capsules with a highly uniform thickness and negligible bending stiffness using silicone elastomers. In our experiments, the capsule thickness is tunable at fabrication, while internal pressure and hoop (circumferential) stress are adjustable via hydrostatic inflation once the capsules are filled and immersed in water. Capsule mechanics are probed through hydro-elastic waves generated by weak mechanical perturbations at the capsule interface. By analyzing the surface wave dynamics in the Fourier domain, we extract the in-plane stress and demonstrate that the hydro-elastic waves are exclusively governed by hoop stress. This provides a controllable macroscopic analogue of liquid drops characterised by an effective surface tension, allowing the capsules to be modeled as large-scale "elasto-drops" with an inflation and thickness tunable effective surface tension. In this limit, bending stiffness is negligible over the experimentally relevant wavelengths, so that the shell dynamics are governed primarily by in-plane tension. Our work demonstrates that elasto-drops serve as a robust model system for parametric studies of large-scale analogues of liquid drops with experimentally adjustable surface tension.

我们提出了一种实验方法来制造厘米薄弹性胶囊具有高度均匀的厚度和可忽略的弯曲刚度的硅弹性体。在我们的实验中,胶囊的厚度在制造时是可调的,而一旦胶囊被填充并浸入水中,内部压力和环向(周向)应力可以通过流体静力膨胀来调节。胶囊力学是通过在胶囊界面处由弱力学扰动产生的水弹性波来探测的。通过在傅里叶域中分析表面波动力学,我们提取了面内应力,并证明了水弹性波完全受环向应力控制。这为液滴提供了一个可控的宏观模拟,其特征是有效的表面张力,允许胶囊被建模为具有膨胀和厚度可调的有效表面张力的大型“弹性滴”。在这个极限下,弯曲刚度在实验相关波长上可以忽略不计,因此壳层动力学主要由面内张力控制。我们的工作表明,弹性液滴作为一个强大的模型系统,可用于实验可调表面张力的大规模液滴类似物的参数化研究。
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引用次数: 0
4D printing of fully programmable sheets of digital metamaterials. 4D打印完全可编程的数字超材料。
IF 2.8 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2026-03-16 DOI: 10.1039/d5sm00780a
Ido Levin, Ela Sachyani, Rama Lieberman, Noa Trink, Eran Sharon, Shlomo Magdassi

Advances in 3D printing technology now enable the precise positioning of microscopic material voxels to form complex structures. Combined with emerging multi-material capabilities and printable responsive materials, this opens new possibilities for digital composite materials and 3D printing of shape-transforming structures, a process known as 4D printing. Building upon these advancements, we present a novel methodology for designing and fabricating digitized 4D-printed shape-transforming sheets. We 3D print responsive continuous sheets composed of two layers, each consisting of active and passive voxels meticulously positioned to form thin structures that transform on demand. Our approach addresses a long-standing challenge in the field: the independent and simultaneous programming of lateral geometry and intrinsic curvature. This unprecedented control over the resulting shape unlocks new opportunities in synthetic shape-morphing materials. We provide a general algorithmic approach that is material-agnostic and enables systematic design of shape transformations with potential capabilities for programmable mechanical properties and multi-actuation-mode systems and applications in soft robotics and deployable structures.

现在,3D打印技术的进步使微观材料体素的精确定位能够形成复杂的结构。结合新兴的多材料能力和可打印的响应材料,这为数字复合材料和形状转换结构的3D打印开辟了新的可能性,这一过程被称为4D打印。在这些进步的基础上,我们提出了一种设计和制造数字化4d打印变形片的新方法。我们3D打印由两层组成的响应连续片,每层由主动和被动体素组成,精心定位形成按需转换的薄结构。我们的方法解决了该领域长期存在的挑战:横向几何和固有曲率的独立和同步编程。这种对最终形状的前所未有的控制为合成形状变形材料带来了新的机会。我们提供了一种与材料无关的通用算法方法,能够系统地设计形状转换,具有可编程机械性能和多驱动模式系统的潜在能力,并应用于软机器人和可展开结构。
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引用次数: 0
Ultra-giant lipid vesicles functioning as a centimeter-sized smart chemical reactor. 超大的脂质囊泡就像一个厘米大小的智能化学反应器。
IF 2.8 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2026-03-16 DOI: 10.1039/d5sm01226k
Nobuyuki Magome, Kaichi Nomura, Masato Hayashi, Yutaka Sumino, Kenichi Yoshikawa

We report a simple and robust method for generating centimeter-sized lipid vesicles (ultra-giant lipid vesicles, UGLVs) by dripping an aqueous solution onto a thin lipid layer floating on the surface of an aqueous phase. A mixture of oleic acid and phospholipids was used to form an interfacial lipid layer. During dripping, the aqueous droplet initially remained above the lipid layer but gradually sank owing to gravity as its volume increased. Once the droplet volume reached several cubic centimeters, it detached from the air-liquid interface and spontaneously formed a stable vesicle with a diameter of several centimeters. Notably, the UGLV remained stable even under mechanical perturbation using a spatula. Furthermore, UGLVs encapsulating the Belousov-Zhabotinsky oscillatory reaction medium were successfully prepared. Neighboring UGLVs exhibit spontaneous synchronization of chemical waves upon contact, demonstrating that UGLVs can function as a unique type of smart chemical reactor.

我们报告了一种简单而可靠的方法,通过将水溶液滴到漂浮在水相表面的薄脂层上,产生厘米大小的脂质囊泡(超大型脂质囊泡,ugvs)。油酸和磷脂的混合物被用来形成界面脂层。在滴注过程中,液滴最初停留在脂质层上方,但随着体积的增大,由于重力作用,液滴逐渐下沉。一旦液滴体积达到几立方厘米,它就会脱离气液界面,自发地形成一个直径几厘米的稳定囊泡。值得注意的是,即使在使用刮刀的机械扰动下,ugv也保持稳定。成功制备了封装Belousov-Zhabotinsky振荡反应介质的uglv。相邻的ugv在接触时表现出自发的化学波同步,表明ugv可以作为一种独特的智能化学反应器。
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引用次数: 0
Rheological properties and shear-induced structures of ferroelectric nematic liquid crystals. 铁电向列液晶的流变特性和剪切诱导结构。
IF 2.8 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2026-03-16 DOI: 10.1039/d5sm01207d
Ashish Chandra Das, Sathyanarayana Paladugu, Oleg D Lavrentovich

Recently discovered ferroelectric nematic (NF) liquid crystals are fluids with a polar orientational order. The electric polarization vector can be aligned by an electric field and by surface anchoring. Here, we explore how the polarization field and effective viscosity of the NF materials are affected by shear flows. We explore three NF materials, abbreviated RM734, DIO, and a room-temperature FNLC919, all of which exhibit a paraelectric nematic (N) and an NF phase. All materials show an increase in the effective viscosity upon cooling, with Arrhenius behavior in broad temperature ranges except near the phase transitions. In DIO and FNLC919, the antiferroelectric SmZA phase separating the N and NF phases shows a strong dependence of the effective viscosity on the shear rate: this viscosity is lower than the viscosity of the N and NF phases at high shear rates ( = 500 s-1) but is much higher when the shear rate is low, = 2.5 s-1. The behavior is associated with the layered structure of the SmZA phase. All mesophases in all three materials exhibit shear-thinning behavior at low shear rates (<100 s-1) and a nearly Newtonian behavior at higher shear rates. In terms of alignment, we observe three regimes in the N and NF phases: flow-alignment at low shear rates, < 102 s-1, a log-rolling regime with the director and polarization along the vorticity axis at > 103 s-1, and polydomain structures at intermediate rates. In the flow-aligning regime, the NF polarization does not tilt away from the shear direction, which is in sharp contrast to the flow-induced tilt of the N director. The effect is attributed to the avoidance of splay deformations and associated space charge in the flowing NF. The temperature and shear rate dependencies of the viscosity and the uncovered shear-induced structural effects of NF advance our understanding of these materials and potentially facilitate their applications.

最近发现的铁电向列液晶是具有极性取向顺序的流体。电极化矢量可以通过电场和表面锚定来对准。本文研究了剪切流对NF材料极化场和有效粘度的影响。我们研究了三种NF材料,简称RM734, DIO和室温FNLC919,它们都表现出一个拟电向列(N)和一个NF相。所有材料在冷却后都表现出有效粘度的增加,除了相变附近,在很宽的温度范围内都表现出阿伦尼乌斯行为。在DIO和FNLC919中,分离N相和NF相的反铁电SmZA相的有效粘度对剪切速率有很强的依赖性:在高剪切速率下(= 500 s-1),该粘度低于N相和NF相的有效粘度,而在剪切速率较低时(= 2.5 s-1),该粘度要高得多。这种行为与SmZA相的分层结构有关。在低剪切速率(-1)下,三种材料的所有中间相都表现出剪切减薄行为,在高剪切速率下表现出接近牛顿的行为。在排列方面,我们观察到N和NF相的三种状态:低剪切速率下的流动排列,< 102 s-1,沿涡量轴方向和极化的原木滚动状态,> 103 s-1,以及中等速率下的多畴结构。在流调质区,NF极化不会偏离剪切方向,这与流致N方向的倾斜形成鲜明对比。这种效果是由于在流动的NF中避免了弯曲变形和相关的空间电荷。粘度对温度和剪切速率的依赖关系以及NF未发现的剪切诱导结构效应促进了我们对这些材料的理解,并有可能促进它们的应用。
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引用次数: 0
Ice-rubber friction mechanisms across scales. 冰-橡胶跨尺度摩擦机制。
IF 2.8 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2026-03-16 DOI: 10.1039/d5sm01200g
Anderson Dalavale Kaiser Pinto, Denis Mazuyer, Juliette Cayer-Barrioz

Rubber-ice friction is governed by the coupled contributions of viscoelastic adhesion and interfacial heating. This work provides unique in situ/in operando insight into the friction mechanisms from the macroscopic to the molecular scale using combined experimental measurements and analytical modelling approaches. Simultaneous force and real contact area imaging were used to quantify the real shear stress of SBR-silica elastomers spanning a small-strain, low-frequency shear-modulus range of 1-8 MPa (a low glass transition temperature of ∼-60 °C) during pure sliding over 50 µm s-1-1 m s-1 and at environmental temperatures down to -30 °C. The normalized real contact area exhibited a non-monotonic velocity dependence; together with a bell-shaped shear stress-velocity curve, this revealed three friction regimes: at low velocity, adhesion and viscoelastic dissipation dominated thermal effects; near the peak, frictional heat generation increased; and at high velocity, thermally driven mechanisms, including advection-dominated heat removal, became more significant, with the possible occurrence of localized interfacial melting. No bulk melting was observed. The novelty of this work relies on bridging the scales in ice-rubber friction mechanisms. At the macroscopic scale, a simple thermal analysis of the rubber-ice sliding interface yielded a dimensionless average contact temperature that collapsed across all compounds and test conditions considered. At the molecular scale, Chernyak-Leonov kinetics was used to describe elastomer chain attachment-detachment on ice and its temperature dependence. Successfully confronting our experimental results with this multiscale model led to a predictive interfacial shear stress model that, when supplied with the measured real contact area, reproduced both the magnitude and shape of the friction response.

橡胶与冰的摩擦受粘弹性粘附和界面加热的共同作用。这项工作通过结合实验测量和分析建模方法,为从宏观到分子尺度的摩擦机制提供了独特的原位/ operando见解。同时力和实际接触面积成像用于量化sbr -硅弹性体在50 μ m s-1-1 m s-1纯滑动过程中,在环境温度低至-30°C时,在1-8 MPa的小应变、低频剪切模量范围内(低玻璃化转变温度为~ -60°C)的真实剪切应力。归一化实际接触面积表现出非单调的速度依赖性;结合钟形剪切应力-速度曲线,揭示了三种摩擦状态:低速时,粘着和粘弹性耗散主导了热效应;在峰值附近,摩擦产热增大;在高速下,热驱动机制,包括以平流为主的热量去除,变得更加重要,可能发生局部界面熔化。未观察到大面积熔化。这项工作的新颖之处在于在冰橡胶摩擦机制中架起桥梁。在宏观尺度上,对橡胶-冰滑动界面的简单热分析得出了一个无量纲的平均接触温度,该温度在所有化合物和测试条件下都崩溃了。在分子尺度上,用Chernyak-Leonov动力学描述了弹性体链在冰上的附着-分离及其温度依赖性。成功地将我们的实验结果与这个多尺度模型进行对比,得到了一个预测的界面剪切应力模型,当提供测量的实际接触面积时,该模型可以再现摩擦响应的大小和形状。
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引用次数: 0
Droplet breakup against an isolated obstacle. 液滴在孤立的障碍物上破裂。
IF 2.8 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2026-03-16 DOI: 10.1039/d5sm01266j
David J Meer, Shivnag Sista, Mark D Shattuck, Corey S O'Hern, Eric R Weeks

We describe combined experiments and simulations of single droplet breakup during flow-driven interactions with a circular obstacle in a quasi-two-dimensional microfluidic chamber. Due to a lack of in-plane confinement, the droplets can also slip past the obstacle without breaking. Droplets are more likely to break when they have a higher flow velocity, larger size (relative to the obstacle radius R), smaller surface tension, and for head-on collisions with the obstacle. We also observe that droplet-obstacle collisions are more likely to result in breakup when the height of the sample chamber is increased. We define a nondimensional breakup number Bk ∼ Ca that accounts for changes in the likelihood of droplet break up with variations in these parameters, where Ca is the Capillary number. As Bk increases, we find in both experiments and discrete element method (DEM) simulations of the deformable particle model that the behavior changes from droplets never breaking (Bk ≪ 1) to always breaking for Bk ≫ 1, with a rapid change in the probability of droplet breakup near Bk = 1. We also find that Bk ∼ S4/3, where S characterizes the symmetry of the collision, which implies that the minimum symmetry required for breakup is controlled by a characteristic distance hR.

我们描述了在准二维微流控室中,单液滴在流动驱动与圆形障碍物相互作用过程中破碎的联合实验和模拟。由于缺乏平面内约束,液滴也可以滑过障碍物而不破裂。当液滴具有较高的流速、较大的尺寸(相对于障碍物半径R)、较小的表面张力以及与障碍物正面碰撞时,液滴更容易破裂。我们还观察到,当样品室的高度增加时,液滴与障碍物的碰撞更容易导致破裂。我们定义了一个无量纲破裂数Bk ~ Ca,它解释了液滴破裂的可能性随这些参数的变化而变化,其中Ca是毛细数。随着Bk的增大,我们在实验和可变形颗粒模型的离散元法(DEM)模拟中发现,液滴的行为从从不破裂(Bk≪1)转变为在Bk≠1时总是破裂,在Bk = 1附近液滴破裂的概率发生快速变化。我们还发现了Bk ~ S4/3,其中S表征了碰撞的对称性,这意味着分裂所需的最小对称性由特征距离h ~ R控制。
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引用次数: 0
Water droplet attraction and coalescence on liquid-crystal-infused textured and porous surfaces. 水滴在液晶注入的纹理和多孔表面上的吸引和聚并。
IF 2.8 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2026-03-13 DOI: 10.1039/d5sm01184a
Filip Ferš, Xiaoguang Wang, Uroš Tkalec

Coalescence of droplets on liquid-infused surfaces has been extensively investigated for isotropic lubricants, where interfacial and hydrodynamic responses are well described by geometry-based and mass-spring models. However, the corresponding dynamics on anisotropic lubricating films, such as liquid crystals (LCs), remain largely unexplored. In this work, we report the use of high-speed imaging to study the attraction and coalescence of millimetre-sized water droplets on two classes of substrates, covered with a thin LC overlayer: LC-infused textured surfaces (LCITS) and LC-infused porous surfaces (LCIPS). On both substrates, the droplets coalesce in three stages over approximately one minute: long-range capillary-mediated attraction, drainage of the lubricant within the wetting ridge, and final merging accompanied by in-plane oscillations of the formed droplet. On LCITS, the initial approach velocities and post-merging dynamics are broadly consistent with the geometry-based mass-spring model developed for oil-impregnated surfaces of a similar type. However, on LCIPS, where a thicker lubricating film produces a larger wetting ridge, we observe substantially reduced attraction and merging velocities, no oscillations were resolved within our temporal resolution at the first velocity peak, and drainage times strongly influenced by evaporation. In the final stage, the peak velocity mainly depends on the LC mesophase and is nearly independent of droplet size, while the oscillation period scales approximately with the square root of the droplet radius. These results clarify how the porous LC scaffold and enlarged wetting ridge alter droplet-droplet interactions and coalescence dynamics relative to textured silicone substrates.

在各向同性润滑剂中,液滴在注入液体表面上的聚结现象已经得到了广泛的研究,其中界面和流体动力学响应可以通过基于几何和质量弹簧的模型很好地描述。然而,各向异性润滑膜,如液晶(lc)的相应动力学仍未得到充分研究。在这项工作中,我们报告了使用高速成像来研究两类基板上毫米大小的水滴的吸引和聚并,覆盖有薄LC覆盖层:LC注入的纹理表面(LCITS)和LC注入的多孔表面(LCIPS)。在这两种基质上,液滴在大约一分钟的时间内分三个阶段聚结:远程毛细管介导的吸引,湿润脊内润滑剂的排水,以及伴随着形成的液滴的面内振荡的最终合并。在LCITS上,初始接近速度和合并后动力学与基于几何的质量-弹簧模型的相似类型的油浸渍表面大体一致。然而,在LCIPS上,更厚的润滑膜产生更大的润湿脊,我们观察到吸引力和合并速度大大降低,在第一个速度峰值的时间分辨率内没有解决振荡,并且排水时间受到蒸发的强烈影响。在最后阶段,峰值速度主要取决于LC中间相,几乎与液滴大小无关,而振荡周期近似与液滴半径的平方根成正比。这些结果阐明了多孔LC支架和扩大的润湿脊如何改变液滴之间的相互作用和聚结动力学。
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引用次数: 0
Liquid-liquid phase separation and self-assembly of hexanoic acid and ethyl hexanoate in ethanol-water systems: a model for aged colloidal Baijiu. 乙醇-水体系中己酸和己酸乙酯的液-液相分离和自组装:陈化胶体白酒的模型。
IF 2.8 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2026-03-13 DOI: 10.1039/d6sm00143b
Chaoyu Zhao, Xinyue Jiang, Yuqun Xie

Liquid-liquid phase separation (LLPS) in the pre-Ouzo region governs the early-stage aggregation of amphiphiles, dictating the non-equilibrium evolution of soft materials. However, classical turbidimetry, which defines phase boundaries by macroscopic cloudiness, is blind to this metastable regime. Here, we introduce an integrated fluorescence-microscopy ternary phase mapping approach that directly probes the pre-Ouzo region in a canonical ethanol-water-amphiphile system. This method reveals critical aggregation concentrations that are 2-3 orders of magnitude below the binodal-a regime inaccessible to turbidimetry. Applying this diagram to naturally aged Baijiu (1-20 years), a dynamically evolving colloidal system, uncovers a pronounced aging-enhanced solubilization: the dissolution ratios of key amphiphiles (hexanoic acid and ethyl hexanoate) exceed 96%, with dissolved concentrations far surpassing static equilibrium predictions. Mechanistic investigations show that this phenomenon arises from the synergistic restructuring of ethanol-water hydrogen-bond networks and the expansion of hydrophobic microdomains. Our work not only provides a high-resolution tool for mapping non-equilibrium phase behavior but also establishes a direct link between slow microstructural evolution and the emergence of kinetically stabilized, supersaturated states in complex fluids.

前ouzo区域的液-液相分离(LLPS)控制着两亲体的早期聚集,决定了软材料的非平衡演化。然而,经典浊度法通过宏观云量来定义相界,对这种亚稳态状态是盲目的。在这里,我们介绍了一种集成的荧光显微镜三元相映射方法,直接探测典型乙醇-水两亲体系中的前ouzo区域。该方法揭示的临界聚集浓度比双浓度低2-3个数量级,这是浊度法无法达到的。将这张图应用于自然陈酿的白酒(1-20年),这是一个动态发展的胶体系统,发现了明显的陈酿增强增溶作用:关键的两亲物质(己酸和己酸乙酯)的溶解率超过96%,溶解浓度远远超过静态平衡预测。机理研究表明,这种现象是由乙醇-水氢键网络的协同重组和疏水微域的扩展引起的。我们的工作不仅为绘制非平衡相行为提供了高分辨率工具,而且还在复杂流体中缓慢的微观结构演化与动力学稳定、过饱和状态的出现之间建立了直接联系。
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Soft Matter
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