In confinement, liquid flows are governed by a complex interplay of molecular, viscous and elastic forces. When a fluid is confined between two approaching surfaces, a transition is generally observed from a long range dynamical response dominated by viscous forces in the fluid to a short range elasto-hydrodynamic response due to the elastic deformation of the solid materials. This study investigates the behavior of fluids driven between oscillating solid surfaces using a dynamic Surface Force Apparatus.
View Article and Find Full Text PDFProc Natl Acad Sci U S A
October 2024
Hydraulic energy is a key component of the global energy mix, yet there exists no practical way of harvesting it at small scales, from flows with low Reynolds number. This has triggered a search for alternative hydroelectric conversion methodologies, leading to unconventional proposals based on droplet triboelectricity, water evaporation, osmotic energy, or flow-induced ionic Coulomb drag. Yet, these approaches systematically rely on ions as intermediate charge carriers, limiting the achievable power density.
View Article and Find Full Text PDFAlthough friction of liquids on solid surfaces is traditionally linked to wettability, recent works have unveiled the role of the solid's internal excitations on interfacial dissipation. In order to directly evidence such couplings, we take advantage of the considerable variation of the molecular timescales of supercooled glycerol under mild change of temperature to explore how friction depends on the liquid's molecular dynamics. Using a dedicated tuning-fork AFM, we measure the slippage of glycerol on mica.
View Article and Find Full Text PDFNanoscale fluid transport is typically pictured in terms of atomic-scale dynamics, as is natural in the real-space framework of molecular simulations. An alternative Fourier-space picture, that involves the collective charge fluctuation modes of both the liquid and the confining wall, has recently been successful at predicting new nanofluidic phenomena such as quantum friction and near-field heat transfer, that rely on the coupling of those fluctuations. Here, we study the charge fluctuation modes of a two-dimensional (planar) nanofluidic channel.
View Article and Find Full Text PDFFaraday Discuss
October 2023
Is this the dawn of iontronics? Iontronics underpins the notion of devices and ionic machines, whereby ion and water also act as information carriers. Thinking about iontronics gives a vision and a road map, with applications in the water-energy nexus.
View Article and Find Full Text PDFIon transport through biological and solid-state nanochannels is known to be a highly noisy process. The power spectrum of current fluctuations is empirically known to scale like the inverse of frequency, following the long-standing yet poorly understood Hooge's law. Here, we report measurements of current fluctuations across nanometer-scale two-dimensional channels with different surface properties.
View Article and Find Full Text PDFThe emergence of new nanoporous materials, based, e.g., on 2D materials, offers new avenues for water filtration and energy.
View Article and Find Full Text PDFNanofluidics, the field interested in flows at the smallest scales, has grown at a fast pace, reaching an ever finer control of fluidic and ionic transport at the molecular level. Until now, artificial pores are far from reaching the wealth of functionalities of biological channels that regulate sensory detection, biological transport, and neurostransmission-all while operating at energies comparable to thermal noise. Here, we argue that artificial ionic machines can be designed by harnessing the entire wealth of phenomena available at the nanoscales and exploiting techniques developed in various fields of physics.
View Article and Find Full Text PDFIon transport measurements are widely used as an indirect probe for various properties of confined electrolytes. It is generally assumed that the ion concentration in a nanoscale channel is equal to the ion concentration in the macroscopic reservoirs it connects to, with deviations arising only in the presence of surface charges on the channel walls. Here, we show that this assumption may break down even in a neutral channel due to electrostatic correlations between the ions arising in the regime of interaction confinement, where Coulomb interactions are reinforced due to the presence of the channel walls.
View Article and Find Full Text PDFThe transport of fluids at the nanoscale is fundamental to manifold biological and industrial processes, ranging from neurotransmission to ultrafiltration. Yet, it is only recently that well-controlled channels with cross sections as small as a few molecular diameters became an experimental reality. When aqueous electrolytes are confined within such channels, the Coulomb interactions between the dissolved ions are reinforced due to dielectric contrast at the channel walls: We dub this effect "interaction confinement.
View Article and Find Full Text PDFCarbon has emerged as a unique material in nanofluidics, with reports of fast water transport, molecular ion separation and efficient osmotic energy conversion. Many of these phenomena still await proper rationalization due to the lack of fundamental understanding of nanoscale ionic transport, which can only be achieved in controlled environments. Here we develop the fabrication of 'activated' two-dimensional carbon nanochannels.
View Article and Find Full Text PDFThe flow of water in carbon nanochannels has defied understanding thus far, with accumulating experimental evidence for ultra-low friction, exceptionally high water flow rates and curvature-dependent hydrodynamic slippage. In particular, the mechanism of water-carbon friction remains unknown, with neither current theories nor classical or ab initio molecular dynamics simulations providing satisfactory rationalization for its singular behaviour. Here we develop a quantum theory of the solid-liquid interface, which reveals a new contribution to friction, due to the coupling of charge fluctuations in the liquid to electronic excitations in the solid.
View Article and Find Full Text PDFThe possibility of controlling electrokinetic transport through carbon and hexagonal boron nitride (hBN) nanotubes has recently opened new avenues for nanofluidic approaches to face outstanding challenges such as energy production and conversion or water desalination. The pH-dependence of experimental transport coefficients points to the sorption of hydroxide ions as the microscopic origin of the surface charge and recent ab initio calculations suggest that these ions behave differently on carbon and hBN, with only physisorption on the former and both physisorption and chemisorption on the latter. Using classical non-equilibrium molecular dynamics simulations of interfaces between an aqueous electrolyte and three models of hBN and graphite surfaces, we demonstrate the major influence of the sorption mode of hydroxide ions on the interfacial transport properties.
View Article and Find Full Text PDFOf relevance to energy storage, electrochemistry and catalysis, ionic and dipolar liquids display unexpected behaviours-especially in confinement. Beyond adsorption, over-screening and crowding effects, experiments have highlighted novel phenomena, such as unconventional screening and the impact of the electronic nature-metallic versus insulating-of the confining surface. Such behaviours, which challenge existing frameworks, highlight the need for tools to fully embrace the properties of confined liquids.
View Article and Find Full Text PDFRecent advances in nanofluidics have enabled the confinement of water down to a single molecular layer. Such monolayer electrolytes show promise in achieving bioinspired functionalities through molecular control of ion transport. However, the understanding of ion dynamics in these systems is still scarce.
View Article and Find Full Text PDFFluid and ionic transport at the nanoscale has recently demonstrated a wealth of exotic behaviours. However, artificial nanofluidic devices are still far from demonstrating the advanced functionalities existing in biological systems, such as electrically and mechanically activated transport. Here, we focus on ionic transport through 2-nm-radius individual multiwalled carbon nanotubes under the combination of mechanical and electrical forcings.
View Article and Find Full Text PDFTo overcome the traditional paradigm of filtration, where separation is essentially performed upon steric sieving principles, we explore the concept of dynamic osmosis through active membranes. A partially permeable membrane presents a time-tuneable feature that changes the effective pore interaction with the solute and thus actively changes permeability with time. In general, we find that slow flickering frequencies effectively decrease the osmotic pressure and large flickering frequencies do not change it.
View Article and Find Full Text PDFSince the historical experiments of Crookes, the direct manipulation of matter by light has been both a challenge and a source of scientific debate. Here we show that laser illumination allows to displace a vial of nanoparticle solution over centimetre-scale distances. Cantilever-based force measurements show that the movement is due to millisecond-long force spikes, which are synchronised with a sound emission.
View Article and Find Full Text PDFIonic current measurements through solid-state nanopores consistently show a power spectral density that scales as 1/ at low frequency , with an exponent α ∼ 0.5-1.5, but strikingly, the physical origin of this behavior remains elusive.
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