Publications

Aqueous biphasic systems (ABSs), in which two aqueous phases with different compositions coexist as separate liquids, were first reported more than a century ago with polymer solutions. Recent observations of ABS forming from concentrated mixtures of inorganic salts and ionic liquids raise the fundamental question of how “different” the components of such mixtures should be for a liquid–liquid phase separation to occur. Here we show that even two monovalent salts sharing a common cation (lithium) but with different anions, namely, LiCl and lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), may result in the formation of ABSs over a wide range of compositions at room temperature. Using a combination of experimental techniques and molecular simulations, we analyze the coexistence diagram and the mechanism driving the phase separation, arising from the different anion sizes. The understanding and …

Microenergy storage devices are appealing and highly demanded for diverse miniaturized electronic devices, ranging from microelectromechanical system, robotics, to sensing microsystems and wearable electronics. However, making high‐energy microcapacitors with currently available printing technologies remains challenging. Herein, the possibility to use latex polyvinylidene fluoride (PVDF) as aqueous ink for making dielectric capacitors at the microscale is shown. The dielectric properties of printed microcapacitors can be optimized based on a novel approach, i.e., mixing PVDF latex with polyvinyl alcohol (PVA) to realize dielectric organic nanocomposites. The PVA prevents the coalescence of PVDF nanoparticles and serves as a continuous matrix phase with high dielectric breakdown strength. While the well‐dispersed PVDF nanoparticles serve as highly polarizable and isolated domains, providing large

In this work, we propose a new way to measure the viscosity of samples in a microfluidic device. By analysing the shape of droplets after an expansion, we can measure the viscosity of the phase inside the droplet knowing the surface tension between the two liquids, the flow rate, the geometry of the channel and the viscosity of the continuous phase. This work paves the way for future high throughput studies in the framework of digital microfluidics.

Measurements and simulations have found that water moves through carbon nanotubes at exceptionally high rates owing to nearly frictionless interfaces1, 2, 3, 4. These observations have stimulated interest in nanotube-based membranes for applications including desalination, nano-filtration and energy harvesting5, 6, 7, 8, 9, 10, yet the exact mechanisms of water transport inside the nanotubes and at the water–carbon interface continue to be debated11, 12 because existing theories do not provide a satisfactory explanation for the limited number of experimental results available so far13. This lack of experimental results arises because, even though controlled and systematic studies have explored transport through individual nanotubes7, 8, 9, 14, 15, 16, 17, none has met the considerable technical challenge of unambiguously measuring the permeability of a single nanotube11. Here we show that the pressure-driven flow rate through individual nanotubes can be determined with unprecedented sensitivity and without dyes from the hydrodynamics of water jets as they emerge from single nanotubes into a surrounding fluid. Our measurements reveal unexpectedly large and radius-dependent surface slippage in carbon nanotubes, and no slippage in boron nitride nanotubes that are crystallographically similar to carbon nanotubes, but electronically different. This pronounced contrast between the two systems must originate from subtle differences in the atomic-scale details of their solid–liquid interfaces, illustrating that nanofluidics is the frontier at which the continuum picture of fluid mechanics meets the atomic nature of matter.

Salinity gradients have been identified as promising clean, renewable and non-intermittent sources of energy — so-called blue energy. However, the low efficiency of current harvesting technologies is a major limitation for large-scale viability and is mostly due to the low performances of the membrane processes currently in use. Advances in materials fabrication with dedicated chemical properties can resolve this bottleneck and lead to a new class of membranes for blue-energy conversion. In this Perspective, we briefly present current technologies for the conversion of blue energy, describe their performances and note their limitations. We then discuss new avenues for the development of a new class of membranes, combining considerations in nanoscale fluid dynamics and surface chemistry. Finally, we discuss how new functionalities originating from the exotic behaviour of fluids in the nanoscale regime can further boost energy conversion, making osmotic energy a tangible, clean alternative.

The process by which sheared suspensions go through a dramatic change in viscosity is known as discontinuous shear thickening. Although well-characterized on the macroscale, the microscopic mechanisms at play in this transition are still poorly understood. Here, by developing new experimental procedures based on quartz-tuning fork atomic force microscopy, we measure the pairwise frictional profile between approaching pairs of polyvinyl chloride and cornstarch particles in solvent. We report a clear transition from a low-friction regime, where pairs of particles support a finite normal load, while interacting purely hydrodynamically, to a high-friction regime characterized by hard repulsive contact between the particles and sliding friction. Critically, we show that the normal stress needed to enter the frictional regime at nanoscale matches the critical stress at which shear thickening occurs for macroscopic suspensions. Our experiments bridge nano and macroscales and provide long needed demonstration of the role of frictional forces in discontinuous shear thickening.

Friction at the nanoscale differs markedly from that between surfaces of macroscopic extent. Characteristically, the velocity dependence of friction between apparent solid/solid contacts can strongly deviate from the classically assumed velocity independence. Here, we show that a nondestructive friction between solid tips with radius on the scale of hundreds of nanometers and solid hydrophobic self-assembled monolayers has a strong velocity dependence. Specifically, using laterally oscillating quartz tuning forks, we observe a linear scaling in the velocity at the lowest accessed velocities, typically hundreds of micrometers per second, crossing over into a logarithmic velocity dependence. This crossover is consistent with a general multicontact friction model that includes thermally activated breaking of the contacts at subnanometric elongation. We find as well a strong dependence of the friction on the dimensions of the frictional probe.

The slipperiness of ice is an everyday-life phenomenon, which, surprisingly, remains controversial despite a long scientific history. The very small friction measured on ice is classically attributed to the presence of a thin self-lubricating film of meltwater between the slider and the ice. But while the macroscale friction behavior of ice and snow has been widely investigated, very little is known about the interfacial water film and its mechanical properties. In this work, we develop a stroke-probe force measurement technique to uncover the microscopic mechanisms underlying ice lubrication. We simultaneously measure the shear friction of a bead on ice and quantify the in situ mechanical properties of the interfacial film, as well as its thickness, under various regimes of speed and temperature. In contrast with standard views, meltwater is found to exhibit a complex viscoelastic rheology, with a viscosity up to 2 orders of magnitude larger than pristine water. The unconventional rheology of meltwater provides a new, consistent, rationale for ice slipperiness. Hydrophobic coatings are furthermore shown to strongly reduce friction due to a surprising change in the local viscosity, providing an unexpected explanation for waxing effects in winter sports. Beyond ice friction, our results suggest new avenues towards self-healing lubricants to achieve ultralow friction.

Transport of liquid mixtures through porous membranes is central to processes such as desalination, chemical separations and energy harvesting, with ultrathin membranes made from novel 2D nanomaterials showing exceptional promise. Here we derive, for the first time, general equations for the solution and solute fluxes through a circular pore in an ultrathin planar membrane induced by a solute concentration gradient. We show that the equations accurately capture the fluid fluxes measured in finite-element numerical simulations for weak solute-membrane interactions. We also derive scaling laws for these fluxes as a function of the pore size and the strength and range of solute-membrane interactions. These scaling relationships differ markedly from those for concentration-gradient-driven flow through a long cylindrical pore or for flow induced by a pressure gradient or electric field through a pore in an ultrathin membrane. These results have broad implications for transport of liquid mixtures through membranes with a thickness on the order of the characteristic pore size.