Spontaneous imbibition enables the elegant propelling of nano-flows because of the dominance of capillarity at small length scales. The imbibition kinetics are, however, solely determined by the static host geometry, the capillarity, and the fluidity of the imbibed liquid. This makes active control particularly challenging. Here we show for aqueous electrolyte imbibition in nanoporous gold that the fluid flow can be reversibly switched on and off through electric potential control of the solid–liquid interfacial tension, that is, we can accelerate the imbibition front, stop it, and have it proceed at will. Simultaneous measurements of the mass flux and the electrical current allow us to document simple scaling laws for the imbibition kinetics, and to explore the charge transport in the metallic nanopores. Our findings demonstrate that the high electric conductivity along with the pathways for fluid/ionic transport render nanoporous gold a versatile, accurately controllable electrocapillary pump and flow sensor for minute amounts of liquids with exceptionally low operating voltages.
Nanoporous gold made by dealloying exemplifies how the exciting mechanical properties of nanoscale objects can be exploited in designing materials from which macroscopic things can be formed. The homogeneous microstructure and the possibility of adjusting the ligament size, L, between few and few hundred nm, along with the high deformability and reproducible mechanical behavior predestine the material for model studies of small-scale plasticity using reliable macroscopic testing schemes on mm-or cm-size samples. Such experiments tend to agree with the Gibson-Ashby scaling relation for strength versus solid fraction, while suggesting an essentially L −1 scaling of the local strength of the ligaments. By contrast, the elastic compliance is dramatically enhanced compared to the Gibson-Ashby relation for the stiffness. Contrary to intuition, the anomalously compliant behavior of the nanomaterial goes along with a trend for more stiffness at smaller L. This article discusses surface excess elasticity, nonlinear elastic behavior and specifically shear instability of the bulk, network connectivity, and the surface chemistry as relevant issues which deserve further study.
We present a study of the elastic and plastic behavior of nanoporous gold in compression, focusing on molecular dynamics simulation and inspecting experimental data for verification. Both approaches agree on an anomalously high elastic compliance in the early stages of deformation, along with a quasi immediate onset of plastic yielding even at the smallest load. Already before the first loading, the material undergoes spontaneous plastic deformation under the action of the capillary forces, requiring no external load. Plastic deformation under compressive load is accompanied by dislocation storage and dislocation interaction, along with strong strain hardening. Dislocation-starvation scenarios are not supported by our results. The stiffness increases during deformation, but never approaches the prediction by the relevant Gibson-Ashby scaling law. Microstructural disorder affects the plastic deformation behavior and surface excess elasticity might modify elastic response, yet we relate the anomalous compliance and the immediate yield onset to an atomistic origin: the large surface-induced prestress induces elastic shear that brings some regions in the material close to the shear instability of the generalized stacking fault energy curve. These regions are elastically highly compliant and plastically weak.
Structural hierarchy can enhance the mechanical behavior of materials and systems. This is exemplified by the fracture toughness of nacre or enamel in nature and by human-made architected microscale network structures. Nanoscale structuring promises further strengthening, yet macroscopic bodies built this way contain an immense number of struts, calling for scalable preparation schemes. In this work, we demonstrated macroscopic hierarchical network nanomaterials made by the self-organization processes of dealloying. Their hierarchical architecture affords enhanced strength and stiffness at a given solid fraction, and it enables reduced solid fractions by dealloying. Scaling laws for the mechanics and atomistic simulation support the observations. Because they expose the systematic benefits of hierarchical structuring in nanoscale network structures, our materials may serve as prototypes for future lightweight structural materials.
Many experiments exploit curvature-driven, surface-diffusion-mediated coarsening for tuning the characteristic structure size of metal network structures made by dealloying, such as nanoporous gold. Here we study this process by kinetic Monte Carlo simulation. The initial microstructures are leveled Gaussian random fields, approximating spinodally decomposed mixtures, of different solid fraction ϕ. Earlier work establishes these structures as valid representations of the nanoporous gold microstructure. We find that the coarsening law for the characteristic spacing between the ligaments of the network is universal, whereas the time evolution of the characteristic ligament diameter is not. The expected time exponent 1/4 is confirmed by our simulation. Contrary to what may be expected based on continuum models, the degree of surface faceting or roughness has no apparent effect on the coarsening kinetics. In the time interval of our study, the network connectivity-as measured by a scaled density of topological genus-remains sensibly invariant for networks with ϕ 0.3, consistent with previous reports of a self-similar evolution of the microstructure during coarsening. Yet, networks with lesser ϕ lose their connectivity on coarsening and can even undergo a percolation-to-cluster transition. This process is slow for ϕ only little below 0.3 and it accelerates in networks with lesser ϕ. The dependency of the connectivity evolution on ϕ may explain controversial findings on the microstructure evolution of nanoporous gold in experimental studies.
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