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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2025 · IF 5.4

Dynamic rheology of boundary ultra-lubricated hydrogels in frictional oscillation study

Lu Chen,Mingle Xu,Yue Zhao,Haojia Guo,Guorong Shan,Yihu Song,Qiang Zheng,Miao Du

The sliding behavior of hydrogels, crucial for biomaterial development, is traditionally studied under steady shear. However, biological motions are typically dynamic and oscillatory. This work characterizes the lubrication performance of boundary ultra-lubricated polyvinyl alcohol (PVA) hydrogels based on their nonlinear viscoelastic response under oscillatory shear testing. Physically crosslinked PVA hydrogels, both fixed and slidable (interface-lubricated), were prepared. Their rheological behavior was investigated through large-amplitude oscillatory shear (LAOS) tests, with a focus on the effect of the surfactant Tween 80 (T80). Compared to fixed hydrogels, slidable hydrogels exhibited pronounced strain softening. The addition of T80 to the hydrogel bulk further enhanced this effect, including strong strain softening even at small strains and reducing the transition oscillation amplitude. Analysis of Lissajous-Bowditch plots using the parameters strain-hardening ratio ( S ) and shear-thickening ratio ( T ) revealed an intracycle strain stiffening and shear-thinning tendency in slidably lubricated hydrogels with increasing amplitude. It is proposed that T80 weakens the gel’s physical network via hydrogen bonding with surfactant micelles and prevents direct PVA-chain contact with the opposing surface. Furthermore, a proportional relationship between the steady coefficient of friction (CoF) and the energy dissipation ratio ( κ ), CoF ∝ 10 −2 . 0 κ , was established. This study demonstrates that the nonlinear viscoelastic parameter κ serves as an effective metric for evaluating hydrogel lubrication performance in dynamic rheological studies, providing deeper insight into frictional energy dissipation mechanisms.

CAS / MDL: 9002-89-5
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LANGMUIR · 2021 · IF 3.882

Nonequilibrium Structure Diagram of Pendular Suspensions under Large-Amplitude Oscillatory Shear

Bonan Hao,Benke Li,Wei Yu

For pendular suspensions with particles in contact with immiscible secondary liquid bridges, the shear field significantly influences particle aggregates and networks. In this work, we study the structure of the pendular network and how the structure changes under large-amplitude-oscillatory shear. Using rheology and optical microscopy, we found unique network destruction followed by reconstruction with increasing strain. Two processes show different shear-field dependencies, strain-rate dependency for destruction and strain dependency for reconstruction. A nonequilibrium state diagram is constructed to show the phase behavior, where the critical particle concentration of sol–gel transition is dependent on the shear history and may depend on shear strain nonmonotonically. Two different mechanisms, shear-induced network breakdown at low strain and shear-induced agglomeration at high strain, are suggested to describe the nonmonotonic critical concentration under the upward strain sweep quantitatively.

CAS / MDL: 919-30-2
研究领域: 材料科学 · 流变学
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2025 · IF 8.5

Elucidating the effect of chitosan microgel characteristics on the large amplitude oscillatory shear (LAOS) behavior of their stabilized high internal phase emulsions using the sequence of physical processes (SPP) approach and comparison with mayonnaise

Songmei Kong,Xuxi Ma,Shiyu Zhen,Yantao Liu,Fusheng Sun,Nan Yang

Chitosan microgels ( h -CSMs) were prepared by cross-linking hydrophobically modified chitosan with sodium phytate (SP). Emulsions stabilized by h -CSMs with different inter-phase fraction, microgel concentration and cross-linking density were studied of their microstructural and rheological properties. In particular, the large amplitude oscillatory shear (LAOS) of the high internal phase emulsions (HIPEs) stabilized by h -CSMs were systematically analyzed using the Fourier transform with Chebyshev polynomials (FTC) and sequence of physical processes (SPP) methods to explore their nonlinear rheological properties. It was found that the HIPEs showed Type III LOAS response with weak strain overshoot depending on the emulsion parameters and microgel characteristics. The FTC method enabled the extraction of nonlinearity measures at limiting conditions ( γ  → 0, γ  →  γ max ) showing intracycle strain-hardening and intracycle shear thinning of the HIPEs under LOAS. By providing a detailed process of the emulsion microstructure transformation in each oscillation cycle, the SPP analysis showed that the HIPEs underwent a 3-step gradual sequence of physical processes, and magnified the influence of microgel characteristics on the rheology of the HIPEs. Comparing with commercially available traditional and low-fat mayonnaise samples, the h- CSM stabilized HIPEs exhibited higher flow compliance but stronger thixotropic recovery ability.

CAS / MDL: 25952-53-8 9012-76-4
研究领域: 食品科学 · 材料科学 · 化学工程
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2022 · IF 5.518

The micromorphology and large amplitude oscillatory shear behaviors of hydrocarbon gel fuels filled with fumed silica and aluminium sub-microparticles

Jian Li,Han Ma,Yaning Li,Zeyu Yang,Guibiao He,Boliang Wang

The gel network structure filled with attractive nanoparticles (NPs) significantly affects the viscoelasticity of the nanocomposites , which is poorly understood and troubles industrial processes. In this work, the nanoparticle gel matrices were prepared with hydrophilic fumed silica (FS), and filled with aluminium sub-microparticles (Al SMPs) loading in the range of 10%− 50%. The effects of particle content and composition on the large amplitude oscillatory shear (LAOS) behaviors are investigated by stress decomposition methods. Meanwhile, the higher harmonics and the Chebyshev harmonics coefficients were obtained. We found that the gels exhibit consistent progressive stiffening with particles filling, companying with plastic transformation and weak strain overshoot (WSO). With aluminum increasing, nonlinear viscoelastic responses gradually weaken in LAOS, severely decreasing the linear viscoelastic (LVE) region, and were validated by strain stiffening index S , T and high-order harmonics. In confocal microscopy (CFM) images, the aluminum particles were fluorescently labeled and found to be adhered together with FS clusters. This article could provide a perspective on understanding the flow mechanism of particulate network structure by combining morphological details and LAOS behaviors.

CAS / MDL: 142-82-5 1712-64-7
研究领域: 材料科学 · 流变学
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MOLECULES · 2023 ·Vol. 28 ·期 12 ·4868 · IF 4.6

Understanding Gel-Powers: Exploring Rheological Marvels of Acrylamide/Sodium Alginate Double-Network Hydrogels

Shi-Chang Wang,Shu-Tong Du,Saud Hashmi,Shu-Ming Cui,Ling Li,Stephan Handschuh-Wang,Xuechang Zhou,Florian J. Stadler

This study investigates the rheological properties of dual-network hydrogels based on acrylamide and sodium alginate under large deformations. The concentration of calcium ions affects the nonlinear behavior, and all gel samples exhibit strain hardening, shear thickening, and shear densification. The paper focuses on systematic variation of the alginate concentration—which serves as second network building blocks—and the Ca2+-concentration—which shows how strongly they are connected. The precursor solutions show a typical viscoelastic solution behavior depending on alginate content and pH. The gels are highly elastic solids with only relatively small viscoelastic components, i.e., their creep and creep recovery behavior are indicative of the solid state after only a very short time while the linear viscoelastic phase angles are very small. The onset of the nonlinear regime decreases significantly when closing the second network (alginate) upon adding Ca2+, while at the same time the nonlinearity parameters (Q0, I3/I1, S, T, e3/e1, and v3/v1) increase significantly. Further, the tensile properties are significantly improved by closing the alginate network by Ca2+at intermediate concentrations.Keywords:acrylamide;sodium alginate;double network hydrogel;large amplitude oscillatory shear;Fourier transform rheology

研究领域: 材料科学 · 流变学
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CHINESE JOURNAL OF POLYMER SCIENCE · 2022 ·Vol. 41 ·期 1 ·153-165 · IF 3.815

Strain Softening of Styrene-Isoprene-Styrene Copolymers under Large Amplitude Oscillatory Shear for Clarifying Payne Effect in Rubbers and Their Nanocomposites

Fan Xin-Peng,Song Yi-Hu,Zheng Qiang,Wang Wan-Jie

To illustrate mechanisms of Payne effect in rubbers and their nanocomposites experiencing large amplitude oscillatory shear (LAOS), comparison studies were performed in styrene-isoprene-styrene (SIS) copolymers and their selectively crosslinked materials at temperatures below and above glass transition temperature of the polystyrene (PS) phase. It was found that under periodic dynamic shear, the strain softening is reversible when the polyisoprene (PI) phase, either crosslinked or not, is restricted by hard PS domains but it shows hysteresis once the PS domains disassociate. The strain softening can happen at the time scale of intrinsic Rouse relaxation of elastically active network strands. Critical stress of strain softening scales with number density of elastically active network strands, a simple relation being verified not only in the selectively crosslinked SIS copolymers but also in PI gum vulcanizates and carbon black filled PI compounds. Payne effect is traditionally used to term strain softening of highly filled rubber vulcanizates under LAOS deformation while evidenced herein is that the Payne effect of highly filled rubber vulcanizates shares the mechanism being common to the strain softening of SIS copolymers.

CAS / MDL: 540-84-1
研究领域: 材料科学 · 高分子物理
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FOOD CHEMISTRY · 2023 · IF 8.8

Towards the development of novel bicomponent phytosterol-based oleogels with natural phenolics

Jia Jia,Jing Zhang,Xiao-Wei Chen,Shang-De Sun,Yong-Hui Wang,An-Chi Wei

Structuring liquid oils into edible oleogels from natural and abundant plant ingredients has great significance in fields ranging from foods to pharmaceuticals but has proven challenging. Herein, novel bicomponent phytosterol-based oleogels were developed with natural phenolics. Investigating diverse natural phenolics, cinnamic acid (CA) and ethyl ferulate (EF) successfully formed oleogels in combination with phytosterols (PS), where a synergistic effect on the oleogelation and crystallization was observed compared to the corresponding single component formulations. FTIR and UV–vis spectra showed that the gel network was primarily driven by hydrogen bonding and π - π stacking. Furthermore, oscillatory shear demonstrated oleogels featured higher elastic and network structure deformation at molar ratio of 5:5 and 3:7. Moreover, the bicomponent phytosterol-based oleogels displayed partially reversible shear deformation and a reversible solid–liquid transition. Such information was useful for engineering the functional properties of oleogel-based lipidic materials, providing significance for the application in foods, cosmetics and pharmaceuticals industries.

研究领域: 食品科学 · 药学 · 材料科学 · 化学
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CHEMICAL ENGINEERING RESEARCH & DESIGN · 2025 · IF 3.9

The morphology on the large amplitude oscillatory shear rheological behaviors of hydrocarbon-based gel fuels: A case of study for spherical and flake aluminum particles

Guibiao He,Jian Li,Yaning Li,Saichao Song,Mingshuai Xue,Boliang Wang

Aluminum (Al) particles have been extensively filled into conventional liquid and solid fuels to improve energy density. However, introducing these particles will modify the rheological properties of hydrocarbon-based gel fuels (GFs). A comprehensive understanding the nonlinear rheological behaviors of GFs is essential, because the utilization of GFs often involves large deformation. In this study, the effects of flake and spherical aluminum (FAl and SAl) particles on the nonlinear responses of hydrocarbon-based GFs were investigated by large amplitude oscillatory shear (LAOS) at different frequencies. The solid-liquid transition behavior was characterized by Lissajous-Bowditch (L-B) curves and Fourier Transform-rheology. Stress sweep results revealed that GFs containing FAl particles exhibited significant viscoelastic characteristics than GFs containing SAl particles. The L-B curves demonstrsted that increasing the SAl particles content slowed transition from linear to nonlinear response, whereas higher FAl particles concentration accelerated this transition. Based on the stress softening ratio (R) and shear thinning ratio (Q), GFs containing FAl particles showed more significant stress stiffening and shear thickening than GFs with SAl particles as aluminum particles content increased. The higher harmonics ratio indicated that nonlinear responses were intensified with increasing FAl particles concentration. while this trend was reversed in GFs containing SAl particles.

研究领域: 流变学 · 能源材料 · 胶体与界面科学 · 推进剂化学 · 功能复合材料
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POLYMER · 2024 · IF 4.1

Influences of non-rubber components on the molecular network and viscoelasticity of natural rubber gum

Tingting Lao,Xinpeng Fan,Xiao Li,Yi Wang,Yanchan Wei,Shuangquan Liao

The molecular network of natural rubber (NR) gum is determined by the interparticle diffusion when NR latex coagulates. However, the roles played by the non-rubber components (NRC) species on the heterogeneous network structure and on the viscoelasticity of NR gum have not been throughly investigated. Here, the molecular relaxation was studied by linear rheology. In addition, the inter- and intra-cycle nonlinearities under large amplitude oscillatory shear (LAOS) were studied for gums with extracted and added NRC. It was found that the high molecular weight free protein restricts the interdiffusion and improves the entanglement density, while the added lipid induces homogeneous distribution of NRC. The physical associations coming from free proteins increase the segment friction and retard the terminal relaxation. Onset of the strain softening was found to be induced by entangled network density. Both the elastic and viscous LAOS nonlinearities can be regulated by adjusting the NRC species. This work sheds light on the contributions of major NRC species on the network structure and nonlinear viscoelasticity of NR gum.

CAS / MDL: 151-21-3
研究领域: 聚合物科学 · 材料科学 · 流变学
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JOURNAL OF APPLIED POLYMER SCIENCE · 2022 ·Vol. 140 ·期 4 ·e53372 · IF 3.057

Synthesis and performance evaluation of crosslinker for seawater-based fracturing fluid

Guohao Miao,Hai Zhang,Yu Yang,Jin Qu,Xinru Ma,Junping Zheng,Xiaofei Liu

Zirconium is one of the most commonly used crosslinkers for guar gum-based fracturing fluid. Nevertheless, it is difficult for zirconium crosslinkers applied in fracturing to possess both high temperature resistance and adjustable crosslinking time. Meanwhile, few people did systematical research on the crosslinking process of fracturing fluid. In this study, an organic zirconium crosslinker with high temperature resistance and controllable crosslinking time was synthesized. The seawater-based fracturing fluid gel prepared with the crosslinker could perform well under 170°C. Oscillatory shear experiments were conducted to analyze the rheology of the gelation process. Moreover, steady-state shear and micro-rheological tests were conducted to analyze the dynamic and static crosslinking process of the fracturing fluid, respectively. Meanwhile, rheo-kinetic equation was used to fit the data and the effects that various factors had on the gelation process were illustrated thoroughly. This study not only prepared an organic zirconium crosslinker with good performances, but also explored the crosslinking process of fracturing fluid gel, which could improve its further application in oilfields.

CAS / MDL: 1310-73-2
研究领域: 石油工程 · 化学工程 · 材料科学
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POLYMER · 2022 · IF 4.432

Payne effect and Mullins effect of silica filled butadiene rubber nanocomposites vulcanizates and their unextractable gels

Xinke Zhong,Yihu Song,Qiang Zheng

Rubber nanocomposites exhibit strain softening under large-amplitude oscillation shear and large-strain cyclic tension while the mechanisms remain unresolved. Herein we systematically investigate the Payne effect and Mullins effect of unfilled and silica filled butadiene rubber (BR) vulcanizates to clarify the impacts of crosslinking density, sol fractions, and filler content. During large-amplitude oscillation shear, the critical strain amplitude for the onset of Payne effect is closely related to storage modulus in the linear viscoelastic region. During cyclic tension deformations, the recovery hysteresis energy and accumulating softening energy are involved in the local deformation of the rubber matrix, which is promoted by the filler phase. These findings are illuminative for optimizing performance of rubber nanocomposite products by controlling the nonideal network structure of viscoelastic rubber matrix.

CAS / MDL: 3290-92-4
研究领域: 材料科学 · 高分子科学 · 机械工程
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2020 · IF 3.99

Thermo-associating polymers based on cross-linked 2-acrylamido-methylpropane sulfonic acid, part A: Synthesis and solution behavior

Alain Pierre Tchameni,Binqiang Xie,Hui Zhang,Lin Zhao,Mingwang Luo,Jiantai Wen

A novel thermo-thickening hydrophilic copolymer (CGBA) was prepared by free-radical copolymerization of sodium 2-acrylamido-2-methylpropane sulfonic acid (NaAMPS) with a newly-synthesized thermo-sensitive macromonomer (BA) and cross-linking N,N’-methylenebisacrylamide (MBA) in aqueous solution under optimal conditions. Its aqueous solution viscosity behavior with respect to temperature was preliminarily evaluated in comparison with its cross-linked sulfonated copolymer (CPAMPS) counterpart (without BA side-chains). Particular attention is dedicated to the thermo-thickening of the aqueous copolymer solutions as studied by the viscosity measurements . In pure water, and above 0.5 wt.%, CGBA manifested an abrupt macroscopic property above the critical association temperature ( T cass ), while CPAMPS exhibited shear-thinning behavior following an Arrhenius law under the same conditions. The composition and length of BA side-chains were identified as the key parameters to envision the self-assembling behavior of CGBA. The results obtained from complementary experiments, performed by proton nuclear magnetic resonance ( 1 H-NMR), Differential scanning calorimetry (DSC), and pyrene fluorescence showed the phase transition of BA side-chains above the T cass . In addition, well above the T cass (70 and 80 °C), the oscillatory shear experiments proved that the storage and loss modulus could be fitted with the single relation time Maxwell model at low frequencies. Furthermore, the magnitude of the thickening effect and the T cass could be modulated using external factors such as shear rates, salinity, and pH. This, in combination with the cost-effectiveness, and the need to further broaden the established theory of thermo-sensitive comonomer, make this copolymer especially interesting for application not only in polymer flooding, but also in drilling fluid.

CAS / MDL: 103-67-3
研究领域: 高分子化学 · 材料科学 · 胶体与界面科学 · 石油工程
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