Traction–separation laws and stick–slip shear phenomenon of interfaces between cellulose nanocrystals

Cellulose nanocrystals (CNCs) are one of nature's most abundant structural material building blocks and possess outstanding mechanical properties including a tensile modulus comparable to Kevlar. It remains challenging to upscale these properties in CNC neat films and nanocomposites due to the difficulty of characterizing interfacial bonding between CNCs that governs stress transfer under deformation. Here we present new analyses based on atomistic simulations of shear and tensile failure of the interfaces between Iβ CNCs, providing new insight into factors governing the mechanical behavior of hierarchical nanocellulose materials. We compare the two most relevant crystal interfaces and find that hydrogen bonded surfaces have greater tensile strength compared to the surfaces governed by weaker interactions. On the contrary, shearing simulations reveal that friction between the atomic interfaces depends not only on surface energy but also the energy landscape along the shear direction. While being a weaker interface, the intersheet plane exhibits greater energy barriers to shear. The molecular roughness of this interface, characterized by a greater energy barrier, exhibits stick–slip deformation behavior as opposed to a more continuous sliding and rebonding mechanism observed for the interfaces with hydrogen bonds. Analytical models to describe the energy landscapes are developed using energy scaling relations for van der Waals surfaces in combination with a modification of the Prandtl–Tomlinson model for atomic friction. Our simulations pave the way for tailoring hierarchical CNC materials by taking a similar approach to techniques employed for describing metals, where mechanical properties can be tuned through a deeper understanding of grain boundary physics and nanoscale interfaces.     

Analysis of plastic deformation in nanoscale metallic multilayers with coherent and incoherent interfaces

Nanoscale metallic multilayered (NMM) composites possess ultra high strength (order of GPa) and high ductility, and exhibit high fatigue resistance. Their mechanical behavior is governed mainly by interface properties (coherent and/or incoherent interfaces), dislocation mechanisms in small volume, and dislocation-interface interaction. In this work, we investigate these effects within a dislocation dynamics (DD) framework and analyze the mechanical behavior of two systems: (1) a bi-material system (CuNi) with coherent interface and (2) a newly developed tri-material system (CuNiNb) composed of both coherent and incoherent interfaces. For the bi-material case we analyze the influence of networks of interfacial dislocations whose nature and distribution are commensurate with the level of relaxation and loading of the structure. Misfit and pre-deposited interfacial dislocation arrays, as well as combinations of both, are studied and the dependence of strength on layer thickness is reported, along with observed dislocation mechanisms. It is shown that interfacial defect configurations significantly alter the strength and mechanical behavior of the material. Furthermore, it is shown that the implementation of penetrable interfaces in DD captures the strength dependence at layer thicknesses on the order of 3-7 nm. For the tri-material case we analyze the effects of coherent and incoherent interfaces in large-scale simulations. The results show that these materials have strong strength-size dependence but are limited by the strength of the incoherent (CuNb) interface which is weak in shear. The weak interface acts as a dislocation sink. This in turn induces an internal shear stress field that activates cross-slip in the adjacent CuNi interlace and thus causing softening. Moreover, it is shown that the yield stress of the CuNiNb system is controlled by the volume fraction of the Nb. Because Nb is the most compliant of the three materials, an increase in volume fraction of Nb decreases the overall yield strength of the material.     

改性石墨烯增强聚四氟乙烯摩擦学性能的分子模拟研究

采用分子动力学模拟研究了接枝改性氧化石墨烯对聚四氟乙烯(PTFE)的增强作用与摩擦学性能的影响,首先选用KH550、KH560和KH570三种硅烷偶联剂接枝氧化石墨烯(GO),在填入纯聚四氟乙烯后计算其机械性能与摩擦性能. 对比得出KH560的增强效果最好,杨氏模量和剪切模量分别提高了205%和116%,摩擦系数提高了39.6%. 然后选用聚酰亚胺(PI)接枝氧化石墨烯,对比了接枝改性与物理共混两种方式对增强效果的影响,结果表明接枝改性的增强效果优于物理共混. 最后通过分析界面间相互作用力、结合能、原子相对浓度和原子运动速度等方式揭示了接枝氧化石墨烯对聚四氟乙烯基体的增强机理.      

3D printed,bio-inspired prototypes and analytical models for structured suture interfaces with geometrically-tuned deformation and failure behavior

Geometrically structured interfaces in nature possess enhanced, and often surprising, mechanical properties, and provide inspiration for materials design. This paper investigates the mechanics of deformation and failure mechanisms of suture interface designs through analytical models and experiments on 3D printed polymer physical prototypes. Suture waveforms with generalized trapezoidal geometries (trapezoidal, rectangular, anti-trapezoidal, and triangular) are studied and characterized by several important geometric parameters: the presence or absence of a bonded tip region, the tip angle, and the geometry. It is shown that a wide range (in some cases as great as an order of magnitude) in stiffness, strength, and toughness is achievable dependent on tip bonding, tip angle, and geometry. Suture interfaces with a bonded tip region exhibit a higher initial stiffness due to the greater load bearing by the skeletal teeth, a double peak in the stress–strain curve corresponding to the failure of the bonded tip and the failure of the slanted interface region or tooth, respectively, and an additional failure and toughening mechanism due to the failure of the bonded tip. Anti-trapezoidal geometries promote the greatest amplification of properties for suture interfaces with a bonded tip due the large tip interface area. The tip angle and geometry govern the stress distributions in the teeth and the ratio of normal to shear stresses in the interfacial layers, which together determine the failure mechanism of the interface and/or the teeth. Rectangular suture interfaces fail by simple shearing of the interfaces. Trapezoidal and triangular suture interfaces fail by a combination of shear and tensile normal stresses in the interface, leading to plastic deformation, cavitation events, and subsequent stretching of interface ligaments with mostly elastic deformation in the teeth. Anti-trapezoidal suture interfaces with small tip angles have high stress concentrations in the teeth and fail catastrophically by tooth failure, whereas larger tip angles exhibit a shear failure of the interfaces. Therefore, larger tip angles and trapezoidal or triangular geometries promote graceful failure, and smaller tip angles and anti-trapezoidal geometries promote more brittle-like failure. This dependence is reminiscent of biological systems, which exhibit a range of failure behaviors with limited materials and varied geometry. Triangular geometries uniquely exhibit uniform stress distributions in its teeth and promote the greatest amplification of mechanical properties. In both the bonded and unbonded cases, the predictions from the presented analytical models and experimental results on 3D printed prototypes show excellent agreement. This validates the analytical models and allows for the models to be used as a tool for the design of new materials and interfaces with tailored mechanical behavior.     

Effective property of piezoelectric composites containing coated nano-elliptical fibers with interfacial debonding

Based on both the spring layer interface model and the Gurtin-Murdoch surface/interface model, the anti-plane shear problem is studied for piezoelectric composites containing coated nano-elliptical fibers with imperfect interfaces. By using the complex function method and the technique of conformal mapping, the exact solutions of the electroelastic fields in fiber, coating, and matrix of piezoelectric nanocomposites are derived under far-field anti-plane mechanical and in-plane electrical loads. Furthermore, the generalized self-consistent method is used to accurately predict the effective electroelastic moduli of the piezoelectric nanocomposites containing coated nano-elliptical fibers with imperfect interfaces. Numerical examples are illustrated to show the effects of the material constants of the imperfect interface layers, the aspect ratio of the fiber section, and the fiber volume fraction on the effective electroelastic moduli of the piezoelectric nanocomposites. The results indicate that the effective electroelastic moduli of the piezoelectric nanocomposites can be significantly reduced by the interfacial debonding, but it can be improved by the surface/interface stresses at the small scale, which provides important theoretical reference for the design and optimization of piezoelectric nanodevices and nanostructures.     

The strength limit in a bio-inspired metallic nanocomposite

Large-scale molecular dynamics simulations are performed to investigate the plastic deformation behavior of a bio-inspired metallic nanocomposite which consists of hard nanosized Ni platelets embedded in a soft Al matrix. The investigation is restricted to an idealized nanocomposite structure with regular platelet distributions in a quasi-two-dimensional geometry under quasi-static loading conditions. This restriction enables us to study size dependent material properties over a wide range of length scales with a fully atomistic resolution of the material and thus without any a priori assumptions of the deformation processes. The simulation results are analyzed with respect to the prevailing deformation mechanisms and their influence on the mechanical properties of the nanocomposite with various geometrical variations. It is found that interfacial sliding contributes significantly to the plastic deformation despite a strong bonding across the interface. Critical for the strength of the nanocomposite is the geometric confinement of dislocation processes in the plastic phase, which strongly depends on the length scale and the morphology of the nanostructure. However, for the smallest structural scales, the softening caused by interfacial sliding prevails, giving rise to a maximum strength.     

Multi-Scale Experiments and Interfacial Mechanical Modeling of Carbon Nanotube Fiber

The multi-scale deformation and interfacial mechanical behavior of carbon nanotube fibers with multi-level structures are investigated by experimental and theoretical methods. Multi-scale experiments including uniaxial tensile testing, in situ Raman spectroscopy, and scanning electron microscopy are conducted to measure the mechanical response of multi-level structures within the fiber under tension. A two-level interfacial mechanical model is then presented to analyze the interfacial bonding strength of mesoscopic bundles and microscopic nanotubes. The evolution characteristics of multi-scale deformation of the fiber are described based on experimental characterization and interfacial strength analysis. The strengthening mechanism of the fiber is further studied. Comprehensive analysis shows that the property of multi-level interfaces is a critical factor for the fiber strength and toughness. Finally, the method of improving the mechanical properties of fiber-based materials is discussed. The result can be used to guide multi-level interface engineering of carbon nanotube fibers and fiber-based composites to produce high performance materials.     

氢键对氧化石墨烯复合结构层间剪切行为影响研究

针对氧化石墨烯层状复合结构性能优化设计要求及其对环境湿度的高敏感性,开展了氧化石墨烯在湿润环境下的层间剪切行为研究.首先,采用连续力学理论,获取不同氧化浓度时氧化石墨烯层状结构层间粘结能、层间氢键相互作用能及剪切应力表达式;所获得的层间能量理论值与分子动力学模拟结果基本一致.其次,通过在氧化石墨烯层间加入不同含量水分子...     

石墨烯与柔性基底界面载荷传递的拉曼光谱实验

本文研究了CVD制备的大尺寸石墨烯与柔性PET基底在拉伸变形过程中切向界面载荷传递的问题,采用原位拉曼光谱实验给出了加载过程中石墨烯的正应变、正应力以及界面切应力的分布曲线。分析表明,石墨烯与PET基底间的载荷传递存在四个阶段,分别是初始阶段、粘附阶段、滑移阶段和界面脱粘破坏阶段。在此基础上,本文对50μm、140μm、270μm和600μm四种尺寸石墨烯试件的界面力学性能进行测量,得到了不同尺寸石墨烯试件的界面力学性能参数,并初步给出了基底变形引起的石墨烯切向界面粘接能的变化,同时分析了试件尺寸对石墨烯界面力学性能的影响。实验结果表明,石墨烯材料和柔性基底最大切应力与临界脱粘切向界面粘接能等界面强度指标受到尺寸的显著影响,尺寸越小切向界面强度越高,反之,尺寸越大则越低。     

层状粘接复合结构界面力学参数声导波定征方法

在推导层状粘接复合结构良好粘接及存在弱界面、滑移界面和脱层等几种不同界面条件下声导波的广义频散方程的基础上,分析了界面径向与轴向力学参数对声导波传播特性的影响,进一步提出以频散特性为基础的超声导波定征方法和在最小二乘意义下的反向算法对粘接复合结构层间界面力学参数进行了估计,分析了影响估计准确性的各种因素,研究了超声导波定征方法对粘接复合结构层间力学参数的灵敏度及其在误差传递中的意义。     

Surface rheology of sorbitan tristearate and β-lactoglobulin: Shear and dilatational behavior

Proteins and surfactants behave very differently under shear and dilatational deformation. In this work, we compare specifically their surface properties by evaluating their rheological response. Oil-soluble surfactant, sorbitan tristearate (Span 65), and globular protein, β-lactoglobulin, were spread and adsorbed onto the surface, respectively. A 2D searle-type measuring geometry with a biconical bob was used for measuring the surface shear rheology, and a pendant drop film balance was used for measuring the dilatational rheology. Both equipments provided the viscoelastic properties (surface shear and dilatational complex moduli) of interfacial layers. Also, the linear and non-linear rheology of these systems was studied by increasing the amplitude of the oscillation. Linear rheology showed that dilatational deformation is mostly affected by the nature of the molecular structure at the interface, whereas shear deformation is affected by the strength of the surface film due to the intermolecular interactions. Furthermore, large-amplitude oscillatory shear rheology indicated that the non-linearity increases with the surface concentration, and is higher for insoluble Span 65 spread films than for soluble protein adsorbed layers. Dilatational and shear deformation provide complementary information about interfacial layers that can be optimized so as to fully characterize the surface depending of the type of film (spread or adsorbed) and the technique used (shear or dilatational rheology under linear or non-linear regimes). This information is useful to correlate the structure and the mechanical properties of interfacial systems.     

Mechanics of interface failure in the trilayer elastic composite

An exact analysis of the mechanics of interface failure is presented for a trilayer composite system consisting of geometrically and materially distinct linear elastic layers separated by straight nonlinear, uniform and nonuniform decohesive interfaces. The technical significance of this system stems from its utility in representing two slabs joined together by a third adhesive layer whose thickness cannot be neglected. The formulation, based on exact infinitesimal strain elasticity solutions for rectangular domains, employs a methodology recently developed by the authors to investigate both solitary defect as well as multiple defect interaction problems in layered systems under arbitrary loading. Interfacial integral equations, governing the normal and tangential displacement jump components at the interfaces, are solved for the uniformly loaded trilayer system. Interfacial defects, taken in the form of interface perturbations and nonbonded portions of interface, are modeled by coordinate dependent interface strengths. They are examined in a variety of configurations chosen so as to shed light on the various interfacial failure mechanisms active in layered systems.     

Optimization design of strong and tough nacreous nanocomposites through tuning characteristic lengths

How nacreous nanocomposites with optimal combinations of stiffness, strength and toughness depend on constituent property and microstructure parameters is studied using a nonlinear shear-lag model. We show that the interfacial elasto-plasticity and the overlapping length between bricks dependent on the brick size and brick staggering mode significantly affect the nonuniformity of the shear stress, the stress-transfer efficiency and thus the failure path. There are two characteristic lengths at which the strength and toughness are optimized respectively. Simultaneous optimization of the strength and toughness is achieved by matching these lengths as close as possible in the nacreous nanocomposite with regularly staggered brick-and-mortar (BM) structure where simultaneous uniform failures of the brick and interface occur. In the randomly staggered BM structure, as the overlapping length is distributed, the nacreous nanocomposite turns the simultaneous uniform failure into progressive interface or brick failure with moderate decrease of the strength and toughness. Specifically there is a parametric range at which the strength and toughness are insensitive to the brick staggering randomness. The obtained results propose a parametric selection guideline based on the length matching for rational design of nacreous nanocomposites. Such guideline explains why nacre is strong and tough while most artificial nacreous nanocomposites aere not.     

Roles of interfacial dynamics in the interaction behaviours between deformable oil droplets

Drainage and deformation of the intervening film can arguably represent the dynamic nature of colliding soft matters. The development of an interaction force analysis between soft interfaces helps to probe the drop deformation and the interfacial properties. Based on the SRYL model, the fluid flow inside the droplet and the convection-diffusion of the surfactant at the oil-water interface is coupled to model the distribution of a non-ionic surfactant (Span80) during drop deformation using AFM. This study quantifies the in situ interfacial concentration with a trace amount of surfactant at the interface and indicates its effect on the interaction forces between two immersed oil droplets in an aqueous solution.     

Interfacial gradient plasticity governs scale-dependent yield strength and strain hardening rates in micro/nano structured metals

The effect of the material microstructural interfaces increases as the surface-to-volume ratio increases. It is shown in this work that interfacial effects have a profound impact on the scale-dependent yield strength and strain hardening of micro/nano-systems even under uniform stressing. This is achieved by adopting a higher-order gradient-dependent plasticity theory [Abu Al-Rub, R.K., Voyiadjis, G.Z., Bammann, D.J., 2007. A thermodynamic based higher-order gradient theory for size dependent plasticity. Int. J. Solids Struct. 44, 2888–2923] that enforces microscopic boundary conditions at interfaces and free surfaces. Those nonstandard boundary conditions relate a microtraction stress to the interfacial energy at the interface. In addition to the nonlocal yield condition for the material’s bulk, a microscopic yield condition for the interface is presented, which determines the stress at which the interface begins to deform plastically and harden. Hence, two material length scales are incorporated: one for the bulk and the other for the interface. Different expressions for the interfacial energy are investigated. The effect of the interfacial yield strength and interfacial hardening are studied by analytically solving a one-dimensional Hall–Petch-type size effect problem. It is found that when assuming compliant interfaces the interface properties control both the material’s global yield strength and rates of strain hardening such that the interfacial strength controls the global yield strength whereas the interfacial hardening controls both the global yield strength and strain hardening rates. On the other hand, when assuming a stiff interface, the bulk length scale controls both the global yield strength and strain hardening rates. Moreover, it is found that in order to correctly predict the increase in the yield strength with decreasing size, the interfacial length scale should scale the magnitude of both the interfacial yield strength and interfacial hardening.     

Using geometric complexity to enhance the interfacial strength of heterogeneous structures fabricated in a multi-stage,multi-piece molding process

Interfaces in heterogeneous structures are typically engineered for optimal strength through the control of surface roughness and the choice of adhesives. Advances in manufacturing technologies are now making it possible to also tailor the geometries of interfaces from the nanoscale to the macroscale to create geometrically complex interfaces that exhibit enhanced performance characteristics. However, the impact of geometric complexity on the mechanical behavior of interfaces has not yet been ascertained. In this investigation, the first step is taken towards understanding the effects of geometric complexity on interfacial strength. A new multi-stage, multi-piece molding process is used to create heterogeneous polymer structures with geometrically complex interfaces consisting of rectangular and circular interlocking features. The structural integrity of these heterogeneous structures is characterized through interfacial tension testing. The full-field deformation measurement technique known as digital image correlation is also used during the testing to visualize the deformation fields around the geometrically complex features. Through this characterization, it is determined that the complex geometries increase the interfacial strength by approximately 20–25%, while reducing the statistical variation by 50%. These effects are attributed to a transition in the failure mechanism from interfacial fracture to homogeneous ligament failure. Results also indicate that geometrically complexity can be used on completely debonded interfaces to increase the strength to at least 25–35% of the bonded interface. Based on these results, some simple design rules have been proposed that enable geometrically complex interfaces to be engineered with enhanced strengths approaching the weaker of the two base materials. These design rules can also be used in the engineering of interfaces to facilitate the development of heterogeneous structures using new design paradigms, such as design for recyclability and the design of products based on bio-inspired concepts.     

Hysteretic linear and nonlinear acoustic responses from pressed interfaces

An analysis of the linear and nonlinear acoustic responses from an interface between rough surfaces in elastoplastic contact is presented as a model of the ultrasonic wave interactions with imperfect interfaces and closed cracks. A micromechanical elastoplastic contact model predicts the linear and second order interfacial stiffness from the topographic and mechanical properties of the contacting surfaces during a loading–unloading cycle. The effects of those surface properties on the linear and nonlinear reflection/transmission of elastic longitudinal waves are shown. The second order harmonic amplitudes of reflected/transmitted waves decrease by more than an order of magnitude during the transition from the elastic contact mode to the elastoplastic contact mode. It is observed that under specific loading histories the interface between smooth surfaces generates higher elastoplastic hysteresis in the interfacial stiffness and the acoustic nonlinearity than interfaces between rough surfaces. The results show that when plastic flow in the contacting asperities is significant, the acoustic nonlinearity is insensitive to the asperity peak distribution. A comparison with existing experimental data for the acoustic nonlinearity in the transmitted waves is also given with a discussion on its contact mechanical implication.     

Interfacial localization of nanoclay particles in oil-in-water emulsions and its reflection in interfacial moduli

The localization of nanoclay particles dispersed in the oil phase of a model oil-in-water emulsion depends on the wetting property of layered nanoparticles. Investigation at a single droplet interface shows that nanoclay is located at different interfacial regions depending on the hydrophilic property of the nanoclay surface. Hydrophobic nanoclays do not present Pickering phenomena at the interface and hardly form an interfacial layer. Hydrophilic nanoclay particles quickly move to the interface and form a Pickering interface with a high interfacial shear modulus. With surfactant, poor hydrophilic nanoclays can be located at the interface due to improvement of the wetting behavior caused by the surfactants dissolved in the aqueous continuous phase. With ionic molecules changing the wetting behavior of particles, the interfacial localization of nanoclays can be controlled and improve the mechanical property of emulsion.     

微粒填充流变材料界面开裂的局部临界应力及尺寸效应的理论分析

研究了以等轴粒子填充流变材料的边界开裂机理，采用能量准则导出了以界面能表示的界面开裂局部临界应力的简洁表达式。由于临界应力正比于１√α，从而可以非常方便地研究粒子开裂的尺寸效应，以碳酸钙微粒填充的聚丙烯复合材料为例进行了理论分析，通过比较界面开裂的能量准则和张应力准则得出结论：即使按照保守的方法估算，即在界面强度等于基体强度的条件下，只要粒径不超过０．２微米，若能量准则得到满足，则张应力准则也会得