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Understanding extracellular polymeric substances (EPS)-based hydrogel formation and properties at the nanoscale through MP-SPR and QCM-D techniques 通过MP-SPR和QCM-D技术了解细胞外聚合物(EPS)基水凝胶的形成和纳米级性质。
IF 2.8 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2026-01-09 DOI: 10.1039/D5SM00894H
Lisa Lopes da Costa, Abdo Bou-Sarkis, Corinne Rondeau-Mouro, Yolaine Bessiere, Céline Moreau and Ana Villares

This work investigates the calcium-induced formation and properties at the nanoscale of hydrogels of structural extracellular polymeric substances (EPS) extracted from aerobic granular sludge (AGS) during wastewater treatment. By comparing EPS with model polymers representing the key biochemical families present in EPS—alginate for polysaccharides and bovine serum albumin (BSA) for proteins—we aim to elucidate their respective contributions to the overall hydrogel formation with calcium cations. Nanoscale characterization techniques (MP-SPR, QCM-D, and AFM) were employed to assess how divalent cations influence hydrogel formation and properties. Our findings revealed that polysaccharides played a dominant role in hydrogel formation through ionic crosslinking, as well as in hydrogel softness and water retention, while proteins contributed to the modulation of structure and viscoelasticity. The nanoscale structural analysis conducted in this study lays a valuable foundation for further understanding the macroscopic properties of EPS hydrogels, enhancing their potential applications in bio-based materials science.

本研究研究了在废水处理过程中从好氧颗粒污泥(AGS)中提取的结构细胞外聚合物(EPS)水凝胶在纳米尺度上的钙诱导形成和性质。通过比较EPS与代表EPS中关键生化家族的模型聚合物——海藻酸盐(多糖)和牛血清白蛋白(蛋白)——我们旨在阐明它们各自对钙离子形成整体水凝胶的贡献。纳米级表征技术(MP-SPR, QCM-D和AFM)被用来评估二价阳离子如何影响水凝胶的形成和性质。我们的研究结果表明,多糖在通过离子交联形成水凝胶,以及水凝胶的柔软性和保水性中起主导作用,而蛋白质则对结构和粘弹性的调节起作用。本研究进行的纳米结构分析为进一步了解EPS水凝胶的宏观性质,增强其在生物基材料科学中的潜在应用奠定了有价值的基础。
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引用次数: 0
Correction: Errors matter when measuring Poisson's ratio of nearly incompressible elastomers 更正:测量几乎不可压缩弹性体的泊松比时,误差很重要。
IF 2.8 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2026-01-09 DOI: 10.1039/D5SM90215K
Robert D. Nedoluha, Majed N. Saadawi and Christopher W. Barney

Correction for ‘Errors matter when measuring Poisson's ratio of nearly incompressible elastomers’ by Robert D. Nedoluha et al., Soft Matter, 2025, 21, 6689–6696, https://doi.org/10.1039/D5SM00535C.

Robert D. Nedoluha等人对“测量几乎不可压缩弹性体泊松比时的误差问题”的修正,《软物质》,2025,21,6689-6696,https://doi.org/10.1039/D5SM00535C。
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引用次数: 0
Domain growth and aging in a phase separating binary fluid confined inside a nanopore 纳米孔内相分离二元流体的畴生长和时效。
IF 2.8 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2026-01-06 DOI: 10.1039/D5SM01031D
Saikat Basu, Suman Majumder, Raja Paul and Subir K. Das

Hydrodynamics is known to have strong effects on the kinetics of phase separation. There exist open questions on how such effects manifest in systems under confinement. Here, we have undertaken extensive studies of the kinetics of phase separation in a two-component fluid that is confined inside pores of cylindrical shape. Using a hydrodynamics-preserving thermostat, we carry out molecular dynamics simulations to obtain results for domain growth and aging for varying temperature and pore width. We find that all systems freeze into a morphology where stripes of regions rich in one or the other component of the mixture coexist. Our analysis suggests that, irrespective of the temperature the growth of the average domain size, (t), prior to the freezing into stripped patterns, follows the power law (t) ∼ t2/3, suggesting an inertial hydrodynamic growth, which typically is applicable for bulk fluids only in the asymptotic limit. Similarly, the aging dynamics, probed by the two-time order-parameter autocorrelation function, also exhibits a temperature-independent power-law scaling with an exponent λ ≃ 2.55, much smaller than what is observed for a bulk fluid.

众所周知,流体力学对相分离动力学有很强的影响。关于这种效应如何在约束下的系统中表现出来,还存在一些悬而未决的问题。在这里,我们已经进行了广泛的动力学研究相分离的双组分流体,被限制在圆柱形孔隙内。利用保持流体动力学的恒温器,我们进行了分子动力学模拟,以获得不同温度和孔径下结构域生长和老化的结果。我们发现所有系统都冻结成一种形态,在这种形态中,条纹区域中富含混合物的一种或另一种成分共存。我们的分析表明,无论温度如何,在冻结成条带模式之前,平均域尺寸(r (t))的增长遵循幂律r (t) ~ t2/3,表明惯性流体动力增长,这通常只适用于渐近极限下的散装流体。同样地,用二阶阶参数自相关函数探测的老化动力学也表现出与温度无关的幂律尺度,其指数λ≃2.55,远小于体积流体的幂律尺度。
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引用次数: 0
A thermodynamic strategy of hydrogels with pearl-necklace-like chains towards excellent hyperelasticity 具有珍珠项链状链的水凝胶获得优异超弹性的热力学策略。
IF 2.8 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2026-01-06 DOI: 10.1039/D5SM01066G
Ziyu Xing, Yifan Liu, Xiaodong Wang, Xiaoling Hu and Rongguo Zhao

Polyelectrolyte hydrogels, characterized by their charged networks, exhibit exceptional deformability and biocompatibility, making them ideal platforms for realizing multifunctional and intelligent material systems, yet the molecular origin of their pearl-necklace-like chains remains controversial. Here we develop a thermodynamic unbinding framework that treats the necklace as an assembly of compact polymeric blobs connected by worm-like spacers. The total free-energy density is decomposed into three additive contributions: (i) conformational entropy of the worm-like chains, (ii) electrostatic interaction, and (iii) interfacial unbinding of the blobs, the latter being modeled through a constrained-junction model that captures non-affine micro-deformation. Conceptualizing the pearl necklace as an assembly of distinct polymer blobs and connecting chains, this approach facilitates a detailed examination of its microstructure and complex mechanical response. Closed-form stress–elongation ratio relations are derived for arbitrary three-dimensional loading. The proposed blob-unbinding strategy offers a universal platform for rationalizing the mechanochemistry of polyelectrolyte networks. The uniaxial tensile data of 50 times deformed hyperelastic hydrogels, regular PAM hydrogels, and ring cross-linked hydrogels, and the planar extension data of PTHF hydrogels were analyzed to illustrate the effectiveness of the proposed model.

聚电解质水凝胶以其带电网络为特征,表现出优异的可变形性和生物相容性,使其成为实现多功能和智能材料系统的理想平台,但其珍珠项链状链的分子起源仍然存在争议。在这里,我们开发了一个热力学解绑定框架,将项链视为由蠕虫状间隔连接的紧凑聚合物团的组装。总自由能密度被分解为三个附加贡献:(i)蠕虫状链的构象熵,(ii)静电相互作用,(iii)斑点的界面解绑定,后者通过捕获非仿射微变形的约束结模型建模。将珍珠项链概念化为不同聚合物斑点和连接链的组合,这种方法有助于详细检查其微观结构和复杂的机械响应。导出了任意三维载荷下的闭式应力-伸长比关系。提出的斑点解结合策略为聚电解质网络的机械化学合理化提供了一个通用平台。通过对50倍变形超弹性水凝胶、规则PAM水凝胶和环状交联水凝胶的单轴拉伸数据和PTHF水凝胶的平面拉伸数据进行分析,验证了该模型的有效性。
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引用次数: 0
Influence of block microstructure on the interaction of styrene-maleic acid copolymer aggregates and lipid nanodiscs 嵌段微观结构对苯乙烯-马来酸共聚物聚集体与脂质纳米圆盘相互作用的影响。
IF 2.8 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2026-01-06 DOI: 10.1039/D5SM01014D
George M. Neville, Aya A. Nasser, James Doutch, Stephen King, Pedro Estrela, Paul Whitley, Gareth J. Price and Karen J. Edler

Investigation of the properties of membrane proteins (MPs) is essential to the successful development of medicines and biotechnology. However, their study is often complicated by denaturation caused by the use of detergents during conventional extraction methods. Copolymers of styrene and maleic acid (SMA) have shown promise in extracting MPs directly from cells while reconstituting lipid membranes into nanodiscs. Despite their potential, there remains a dearth of information on the precise interactions that take place between the copolymers and lipid membranes although they are known to be sensitive to small variations in copolymer composition or structure. We have used reversible addition–fragmentation chain transfer (RAFT) polymerisation to synthesise SMA copolymers with equivalent molar mass, but with inverted block sequences and end group termini. Through a range of experiments, including dynamic light scattering and small-angle neutron scattering (SANS) on SMA aggregates and nanodisc formation studies using UV-vis spectroscopy with both model DMPC lipids and E. coli membranes, the impact of both block distribution and end group chemistry on copolymer–membrane interactions was investigated. It was found that mismatched hydrophilic and hydrophobic end groups on the styrene block and alternating block, respectively, impeded membrane disruption and subsequent solubilisation. This highlights not only how the amphiphilic balance of these blocks is important for efficient nanodisc formation, but also how end groups influence these and may be optimised towards extraction of more challenging MPs. The work contributes to a better understanding of SMA behaviour and offers insight into how these nanomaterials may be better designed and tailored for specific applications.

膜蛋白特性的研究对药物和生物技术的成功开发至关重要。然而,他们的研究往往是复杂的,因为在传统的提取方法中使用洗涤剂引起的变性。苯乙烯和马来酸共聚物(SMA)在直接从细胞中提取MPs的同时,将脂质膜重组成纳米圆盘。尽管它们具有潜力,但关于共聚物和脂质膜之间发生的精确相互作用的信息仍然缺乏,尽管已知它们对共聚物组成或结构的微小变化很敏感。我们已经使用可逆加成-破碎链转移(RAFT)聚合来合成具有等效摩尔质量的SMA共聚物,但具有倒置的嵌段序列和端基末端。通过一系列实验,包括动态光散射和小角中子散射(SANS)对SMA聚集体的影响,以及使用UV-vis光谱对模型DMPC脂质和大肠杆菌膜纳米盘形成的研究,研究了嵌段分布和端基化学对共聚物-膜相互作用的影响。研究发现,苯乙烯嵌段和交替嵌段上的亲水和疏水端基不匹配,阻碍了膜的破坏和随后的溶解作用。这不仅强调了这些块的两亲性平衡对高效纳米盘形成的重要性,而且还强调了端基如何影响这些平衡,并可能优化提取更具挑战性的MPs。这项工作有助于更好地理解SMA的行为,并为这些纳米材料如何更好地设计和定制特定应用提供了见解。
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引用次数: 0
A spectrum of p-atic symmetries and defects in confluent epithelia 融合上皮的p-atic对称性和缺陷谱。
IF 2.8 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2026-01-06 DOI: 10.1039/D5SM01010A
Lea Happel, Griseldis Oberschelp, Anneli Richter, Gwenda Roselene Rode, Valeriia Grudtsyna, Amin Doostmohammadi and Axel Voigt

Topological defects provide a unifying language to describe how orientational order breaks down in active and living matter. Considering cells as elongated particles confluent, epithelial tissues can be interpreted as nematic fields and their defects have been linked to extrusion, migration, and morphogenetic transformations. Yet, epithelial cells are not restricted to nematic order: their irregular shapes can express higher rotational symmetries, giving rise to p-atic order with p > 2. Here we introduce a framework to extract p-atic fields and their defects directly from experimental images. Applying this method to MDCK cells, we find that all symmetries from p = 2 to p = 6 generate defects. Surprisingly, the statistics reveal an even–odd asymmetry, with odd p producing more defects than even p, consistent with geometric frustration arguments based on tilings. In contrast, no strong positional or orientational correlations are found between nematic and hexatic defects, suggesting that different symmetries coexist largely independently. These results demonstrate that epithelial tissues should not be described by nematic order alone, but instead host a spectrum of p-atic symmetries. Our work provides experimental evidence for this multivalency of order and offers a route to test and refine emerging p-atic liquid crystal theories of living matter.

拓扑缺陷提供了一种统一的语言来描述在活性物质和生物物质中取向秩序是如何分解的。考虑到细胞是细长的颗粒融合,上皮组织可以解释为向列场,它们的缺陷与挤压、迁移和形态发生转化有关。然而,上皮细胞并不局限于向列序:它们的不规则形状可以表达更高的旋转对称性,从而产生p向序和p >2。本文介绍了一种从实验图像中直接提取p-atic场及其缺陷的框架。将此方法应用于MDCK细胞,我们发现从p = 2到p = 6的所有对称性都会产生缺陷。令人惊讶的是,统计数据揭示了奇偶不对称,奇数p比偶数p产生更多的缺陷,这与基于平铺的几何挫折论点一致。相反,在向列和六向缺陷之间没有发现强的位置或取向相关性,这表明不同的对称性在很大程度上是独立共存的。这些结果表明,上皮组织不应仅用向列顺序来描述,而是具有p-atic对称的谱。我们的工作为这种多价秩序提供了实验证据,并为测试和完善生物物质的新兴p-atic液晶理论提供了一条途径。
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引用次数: 0
Memory and recovery effects in the strain hardening regime of glassy polymers: theory and simulations 玻璃状聚合物应变硬化过程中的记忆和恢复效应:理论与模拟。
IF 2.8 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2026-01-06 DOI: 10.1039/D5SM01077B
Thomas C. Merlette, Jérôme Hem, Caroline Crauste-Thibierge, Sergio Ciliberto, Jérôme Bikard and Didier R. Long

Complex memory effects under applied strain are a defining feature of glassy polymers in the strain hardening regime. We proposed recently a theory for plastic flow and strain hardening as controlled by two contributions to the free energy barriers in glassy polymers submitted to an applied deformation. Free energy barriers decrease under the effect of the stress, which leads to yielding and the onset of plastic flow. Conversely, monomer orientation increases the barriers. These two contributions have very different kinetics. The contribution related to the stress relaxes quickly as a function of the applied stress whereas the orientation contribution relaxes by rotational diffusion, which is very slow at depth in the glassy state. This description could account for the main feature of the Bauschinger effect when considering a stop of the deformation followed by a resuming of the deformation after some waiting time, or for describing deformation cycles, e.g. a tensile test followed by a compression, or the reverse. We show here that the same model allows for interpreting and explaining memory effects in complex deformation histories as regard the distribution of relaxation times, the evolution of tangent delta measured by dielectric spectroscopy and the kinetics of recovery of the reference curve as a function of the waiting time and allows for the interpretation of recent experimental results obtained by small probes reorientation dynamics and dielectric spectroscopy.

在应变作用下的复杂记忆效应是玻璃状聚合物在应变硬化过程中的一个显著特征。我们最近提出了一个理论,塑性流动和应变硬化是由两个贡献控制的自由能垒在玻璃聚合物提交的应用变形。自由能垒在应力作用下降低,导致屈服和塑性流动的发生。相反,单体取向增加了势垒。这两种贡献有非常不同的动力学。与应力有关的贡献作为外加应力的函数迅速松弛,而取向贡献通过旋转扩散松弛,在玻璃态下,旋转扩散在深度上非常缓慢。当考虑到变形停止后,经过一段等待时间后,变形又恢复,或者描述变形周期,例如,拉伸试验之后是压缩试验,或者相反,这种描述可以解释鲍辛格效应的主要特征。我们在这里表明,相同的模型允许解释和解释关于松弛时间分布的复杂变形历史中的记忆效应,由介电光谱测量的正切delta的演变和参考曲线的恢复动力学作为等待时间的函数,并允许解释最近由小探针重新定向动力学和介电光谱获得的实验结果。
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引用次数: 0
Swimming velocity modulates enhanced diffusion in bacterial suspensions 游泳速度调节细菌悬浮液中增强的扩散。
IF 2.8 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2026-01-05 DOI: 10.1039/D5SM00824G
Shirui Ruan, Rui He, Rongjing Zhang and Junhua Yuan

The activity of swimming bacteria fundamentally alters the transport properties of passive particles through active agitation. While particle diffusion enhancement is known to scale linearly with the active bacterial flux (the product of swimmer density and velocity), the factors controlling the proportionality coefficient β, which represents the efficiency of energy transfer per swimmer, remain unclear. Here, we systematically investigate how bacterial swimming behavior modulates diffusion enhancement using Escherichia coli and Pseudomonas aeruginosa suspensions. We compare wild-type and smooth-swimming E. coli strains to isolate the effect of tumbling, and we tune swimming velocities in both E. coli and P. aeruginosa to test generality across species with different motility phenotypes. Our results show that bacterial reorientation dynamics have little effect on β, as both wild-type and smooth-swimming E. coli exhibit similar enhancement. In contrast, swimming velocity has a pronounced effect on β in both species. Direct measurements reveal that bacteria-tracer interactions are confined to a radius of approximately 5 µm, with microsphere velocity decaying as r−1.3 with distance from the nearest bacterium. These findings establish swimming velocity as a key determinant of diffusion enhancement in active suspensions, with implications for understanding nutrient transport and mixing in microbial environments.

游动细菌的活性通过主动搅拌从根本上改变了被动颗粒的运输特性。虽然已知颗粒扩散增强与活性细菌通量(游泳者密度和速度的乘积)成线性关系,但控制比例系数β的因素仍不清楚,该系数表示每个游泳者的能量传递效率。在这里,我们系统地研究了细菌游泳行为如何调节大肠杆菌和铜绿假单胞菌悬浮液的扩散增强。我们比较了野生型和平稳游泳的大肠杆菌菌株,以分离翻滚的影响,我们调整了大肠杆菌和铜绿假单胞菌的游泳速度,以测试具有不同运动表型的物种的普遍性。我们的研究结果表明,细菌重定向动力学对β的影响很小,因为野生型和平稳游动的大肠杆菌都表现出类似的增强作用。相比之下,游泳速度对两个物种的β有明显的影响。直接测量表明,细菌-示踪剂相互作用的半径约为5 μ m,微球速度随距离最近的细菌的距离而衰减为r-1.3。这些发现表明,游泳速度是活性悬浮液中扩散增强的关键决定因素,这对理解微生物环境中的营养物质运输和混合具有重要意义。
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引用次数: 0
Microbubble-based measurement of shear and loss moduli in polyacrylamide hydrogels at MHz frequencies 基于微泡的测量剪切和损失模量在聚丙烯酰胺水凝胶在兆赫频率。
IF 2.8 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2026-01-05 DOI: 10.1039/D5SM00552C
Ali Rezaei, Kay Dijs, David Fernandez Rivas, Jacco H. Snoeijer, Michel Versluis and Guillaume Lajoinie

The rheology of soft materials is routinely measured at low strain rates to extract constitutive laws necessary for understanding and modeling their behavior. High-frequency rheology, however, remains difficult to access. Consequently, the mechanical properties of soft materials at MHz strain rates are largely unknown. Ultrasound-driven microbubbles, widely used in biomedical imaging, drug delivery, and therapy, act as efficient mechanical actuators at MHz frequencies. Their dynamics depend on nonlinear resonance behavior, the viscoelasticity of their stabilizing shells, and the viscoelastic properties of the surrounding medium. Here, we make use of (nonlinear) bubble dynamics to characterize the rheology of polyacrylamide (PAM) hydrogels at strain rates exceeding 106 s−1. Narrow resonance curves of single coated microbubbles embedded in PAM, obtained through high-speed imaging, were compared to a Rayleigh–Plesset-type model. The results show that the shear modulus is similar in both the Hz and MHz regimes, while the loss modulus behaves very differently, exhibiting an effective shear viscosity at MHz frequencies comparable to that of water. These findings demonstrate a new approach for probing the high-frequency rheology of viscoelastic media.

软材料的流变学通常在低应变率下测量,以提取理解和建模其行为所必需的本构定律。然而,高频流变学仍然难以获得。因此,软材料在MHz应变速率下的力学性能在很大程度上是未知的。超声驱动的微泡,广泛应用于生物医学成像,药物输送和治疗,作为有效的机械驱动器在兆赫频率。它们的动力学取决于非线性共振行为、稳定壳的粘弹性以及周围介质的粘弹性。在这里,我们利用(非线性)气泡动力学来表征聚丙烯酰胺(PAM)水凝胶在应变速率超过106 s-1时的流变性。通过高速成像获得的单包覆微泡嵌入PAM的窄共振曲线,与rayleigh_€plesset型模型进行了比较。结果表明,剪切模量在Hz和MHz频率下相似,而损失模量表现出非常不同的特性,在MHz频率下表现出与水相当的有效剪切粘度。这些发现为探索粘弹性介质的高频流变性提供了一种新的方法。
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引用次数: 0
Differential crosslinking and contractile motors drive nuclear chromatin compaction. 差动交联和收缩马达驱动核染色质压实。
IF 2.8 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2026-01-05 DOI: 10.1039/d5sm00812c
Ligesh Theeyancheri, Edward J Banigan, J M Schwarz

During interphase, the cell nucleus exhibits spatial compartmentalization between transcriptionally active euchromatin and transcriptionally repressed heterochromatin. In conventional nuclear organization, euchromatin is enriched in the nuclear interior, while heterochromatin - approximately 50% denser - resides near the periphery. The nuclear lamina, a deformable structural shell, further modulates peripheral chromatin organization. Here, we investigate a chromatin model in which an active, crosslinked polymer is tethered to a deformable lamina shell. We show that contractile motor activity, shell deformability, and the spatial distribution of crosslinks jointly determine compartmentalization. Specifically, a radial crosslink density gradient, even with a small increase toward the periphery, coupled with motor activity, drives genomic segregation consistent with experimental observations. This effect arises as motors preferentially draw crosslinks toward the periphery, forming dense domains that promote heterochromatin formation. Our model also predicts increased stiffness of nuclear wrinkles due to heterochromatin compaction beneath the lamina, consistent with instantaneous stiffening observed under nanoindentation. We conclude by outlining potential experimental approaches to validate our model predictions.

在间期,细胞核在转录活跃的常染色质和转录抑制的异染色质之间表现出空间区隔。在传统的核组织中,常染色质富集于核内部,而异染色质(密度约为50%)分布在核外围。核层,一个可变形的结构壳,进一步调节外周染色质组织。在这里,我们研究了一种染色质模型,其中一种活性的交联聚合物被拴在可变形的层状壳上。我们发现,收缩运动活动、壳的可变形性和交联的空间分布共同决定了区隔化。具体来说,径向交联密度梯度,即使是向外围的少量增加,加上运动活动,驱动基因组分离与实验观察一致。这种效应的产生是由于马达优先将交联指向外围,形成促进异染色质形成的致密结构域。我们的模型还预测,由于层下的异染色质压实,核皱纹的刚度增加,与纳米压痕下观察到的瞬时硬化一致。最后,我们概述了验证模型预测的潜在实验方法。
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引用次数: 0
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Soft Matter
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