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Register a new userCreep in reactive colloidal gels: a nanomechanical study of cement hydrates
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From soft polymeric gels to hardened cement paste, amorphous solids under constant load exhibit a pronounced time-dependent deformation called creep. The microscopic mechanism of such a phenomenon is poorly understood and constitutes a significant challenge in densely packed and chemically reactive granular systems. Both features are prominently present in hydrating cement pastes composed of calcium silicate hydrate (C-S-H) nanoparticles, whose packing density increases as a function of time, while cements hydration is taking place. Performing nano-indentation tests and porosity measurements on a large collection of samples at various hydration degrees, we show that the creep response of hydrating cement paste is mainly controlled by the inter-particle distance, and results from slippage between (C-S-H) nanoparticles. Our findings, which pave the way for the design of concrete with improved creep resistance, provide a unique insight into the microscopic mechanism underpinning the creep response in aging granular materials.
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Colloidal gels are formed through the aggregation of attractive particles, whose size ranges from 10~nm to a few micrometers, suspended in a liquid. Such gels are ubiquitous in everyday life applications, from food products to paints or construction materials, in particular thanks to their ability to easily yield, i.e., to turn from a solid to a liquid under the application of a weak external load. Understanding and controlling the mechanical response of colloidal gels is therefore of prime importance. Depending on the details of the system, however, the resulting gel networks present different microstructural organisations that may lead to widely different mechanical responses. This raises important challenges in fully characterizing yielding and in uncovering the mechanisms of nonlinear response in colloidal gels. In this paper, we distinguish between two classes of colloidal gels showing respectively reversible yielding, where the gel network reforms upon load release, and irreversible yielding, where the network is fully destroyed through fractures and phase separation. This broad, empirical distinction is achieved through rheology and local experiments at a mesoscopic scale, intermediate between the network characteristic size and the sample size. We further discuss how the observables derived from creep and fatigue experiments may be modelled to predict yielding and highlight open questions and future research directions in the domain.
Attractive colloidal dispersions, suspensions of fine particles which aggregate and frequently form a space spanning elastic gel are ubiquitous materials in society with a wide range of applications. The colloidal networks in these materials can exist in a mode of free settling when the network weight exceeds its compressive yield stress. An equivalent state occurs when the network is held fixed in place and used as a filter through which the suspending fluid is pumped. In either scenario, hydrodynamic instabilities leading to loss of network integrity occur. Experimental observations have shown that the loss of integrity is associated with the formation of eroded channels, so-called streamers, through which the fluid flows rapidly. However, the dynamics of growth and subsequent mechanism of collapse remain poorly understood. Here, a phenomenological model is presented that describes dynamically the radial growth of a streamer due to erosion of the network by rapid fluid back flow. The model exhibits a finite-time blowup -- the onset of catastrophic failure in the gel -- due to activated breaking of the inter-colloid bonds. Brownian dynamics simulations of hydrodynamically interacting and settling colloids in dilute gels are employed to examine the initiation and propagation of this instability, which is in good agreement with the theory. The model dynamics are also shown to accurately replicate measurements of streamer growth in two different experimental systems. The predictive capabilities and future improvements of the model are discussed and a stability-state diagram is presented providing insight into engineering strategies for avoiding settling instabilities in networks meant to have long shelf lives.
Mechanical creep behaviors of natural gas hydrates (NGHs) are of importance for understanding mechanical instability of gas hydrate-bearing sediments on Earth. Limited by the experimental challenges, intrinsic creep mechanisms of nanocrystalline methane hydrates remain largely unknown yet at molecular scale. Herein, using large-scale molecular dynamics (MD) simulations, mechanical creep behaviors of nanocrystalline methane hydrates are investigated. It is revealed that mechanical creep responses are greatly dictated by internal microstructures of crystalline grain size and external conditions of temperature and static stress. Interestingly, a long steady-state creep is observed in nanocrystalline methane hydrates, which can be described by a modified constitutive Bird-Dorn-Mukherjee model. Microstructural analysis show that deformations of crystalline grains, grain boundary (GB) diffusion and GB sliding collectively govern the mechanical creep behaviors of nanocrystalline methane hydrates. Furthermore, structural transformation also appears important in their mechanical creep mechanisms. This study sheds new insights into understanding the mechanical creep scenarios of gas hydrates.
Shear transformations, as fundamental rearrangement events operating in local regions, hold the key of plastic flow of amorphous solids. Despite their importance, the dynamic features of shear transformations are far from clear. Here, we use a colloidal glass under shear as the prototype to directly observe the shear transformation events in real space. By tracing the colloidal particle rearrangements, we quantitatively determine two basic properties of shear transformations: local shear strain and dilatation (or free volume). It is revealed that the local free volume undergoes a significantly temporary increase prior to shear transformations, eventually leading to a jump of local shear strain. We clearly demonstrate that shear transformations have no memory of the initial free volume of local regions. Instead, their emergence strongly depends on the dilatancy ability of these regions, i.e., the dynamic creation of free volume. More specifically, the particles processing the high dilatancy ability directly participate in subsequent shear transformations. These results experimentally support the Argons statement about the dilatancy nature of shear transformations, and also shed insight into the structural origin of amorphous plasticity.
We sandwich a colloidal gel between two parallel plates and induce a radial flow by lifting the upper plate at a constant velocity. Two distinct scenarios result from such a tensile test: ($i$) stable flows during which the gel undergoes a tensile deformation without yielding, and ($ii$) unstable flows characterized by the radial growth of air fingers into the gel. We show that the unstable regime occurs beyond a critical energy input, independent of the gels macroscopic yield stress. This implies a local fluidization of the gel at the tip of the growing fingers and results in the most unstable wavelength of the patterns exhibiting the characteristic scalings of the classical viscous fingering instability. Our work provides a quantitative criterion for the onset of fingering in colloidal gels based on a local shear-induced yielding, in agreement with the delayed failure framework.
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