Development of sustainable processes for hydrocarbons synthesis is a fundamental challenge in chemistry since these are of unquestionable importance for the production of many essential synthetic chemicals, materials and carbon-based fuels. Current industrial processes rely on non-abundant metal catalysts, temperatures of hundreds of Celsius and pressures of tens of bars. We propose an alternative gas phase process under mild reaction conditions using only atomic carbon, molecular hydrogen and an inert carrier gas.
View Article and Find Full Text PDFDissolution and dissociation of CO2 in an aqueous phase induce diffusiophoretic motion of suspended particles with a nonzero surface charge. We report CO2-driven diffusiophoresis of colloidal particles and bacterial cells in a circular Hele-Shaw geometry. Combining experiments and model calculations, we identify the characteristic length and time scales of CO2-driven diffusiophoresis in relation to system dimensions and CO2 diffusivity.
View Article and Find Full Text PDFA submerged finite cylinder moving under its own weight along a soft incline lifts off and slides at a steady velocity while also spinning. Here, we experimentally quantify the steady spinning of the cylinder and show theoretically that it is due to a combination of an elastohydrodynamic torque generated by flow in the variable gap, and the viscous friction on the edges of the finite-length cylinder. The relative influence of the latter depends on the aspect ratio of the cylinder, the angle of the incline, and the deformability of the substrate, which we express in terms of a single scaled compliance parameter.
View Article and Find Full Text PDFWe present a microfluidic crossflow separation of colloids enabled by the dissolution of CO gas in aqueous suspensions. The dissolved CO dissociates into H and HCO ions, which are efficient candidates for electrolytic diffusiophoresis, because of the fast diffusion of protons. By exposing CO gas to one side of a microfluidic flow channel, a crossflow gradient can be created, enabling the crossflow diffusiophoresis of suspended particles.
View Article and Find Full Text PDFThe transport of particulate matter to and from dead-end pores is difficult to achieve due to confinement effects. Diffusiophoresis is a phenomenon that results in the controlled motion of colloids along solute concentration gradients. Thus, by establishing an electrolyte concentration gradient within dead-end pores, it is possible to induce the flow of particles into and out of the pores via diffusiophoresis, as has been demonstrated recently.
View Article and Find Full Text PDFThe accurate measurement of wall zeta potentials and solute-surface interaction length scales for electrolyte and non-electrolyte solutes, respectively, is critical to the design of many biomedical and microfluidic applications. We present a novel microfluidic approach using diffusioosmosis for measuring either the zeta potentials or the characteristic interaction length scales for surfaces exposed to, respectively, electrolyte or non-electrolyte solutes. When flows containing different solute concentrations merge in a junction, local solute concentration gradients can drive diffusioosmotic flow due to electrokinetic, steric, and other interactions between the solute molecules and solid surfaces.
View Article and Find Full Text PDFWe combine numerical simulations and an analytic approach to show that the capture of finite, inertial particles during flow in branching junctions is due to invisible, anchor-shaped three-dimensional flow structures. These Reynolds-number-dependent anchors define trapping regions that confine particles to the junction. For a wide range of Stokes numbers, these structures occupy a large part of the flow domain.
View Article and Find Full Text PDFThe diffusiophoretic motion of suspended colloidal particles under one-dimensional solute gradients is solved using numerical and analytical techniques. Similarity solutions are developed for the injection and withdrawal dynamics of particles into semi-infinite pores. Furthermore, a method of characteristics formulation of the diffusion-free particle transport model is presented and integrated to realize particle trajectories.
View Article and Find Full Text PDFThe zeta potential is an electric potential in the Debye screening layer of an electrolyte, which represents a key physicochemical surface property in various fields ranging from electrochemistry to pharmaceuticals. Thus, characterizing the zeta potential is essential for many applications, but available measurement techniques are limited. Electrophoretic light scattering is typically used to measure the zeta potential of particles in suspension, whereas zeta potential measurements of a solid wall in solution rely on either streaming potential or electroosmotic mobility measurement techniques, both of which are expensive and sophisticated.
View Article and Find Full Text PDFWe show experimentally that a flow-induced, Reynolds number-dependent particle-capture mechanism in branching junctions can be enhanced or eliminated by varying the junction angle. In addition, numerical simulations are used to show that the features responsible for this capture have the signatures of classical vortex breakdown, including an approach flow aligned with the vortex axis and a pocket of subcriticality. We show how these recirculation regions originate and evolve and suggest a physical mechanism for their formation.
View Article and Find Full Text PDFProc Natl Acad Sci U S A
January 2016
Transport of colloids in dead-end channels is involved in widespread applications including drug delivery and underground oil and gas recovery. In such geometries, Brownian motion may be considered as the sole mechanism that enables transport of colloidal particles into or out of the channels, but it is, unfortunately, an extremely inefficient transport mechanism for microscale particles. Here, we explore the possibility of diffusiophoresis as a means to control the colloid transport in dead-end channels by introducing a solute gradient.
View Article and Find Full Text PDFFusion between suspended lipid vesicles is difficult to achieve without membrane proteins or ions because the vesicles have extremely low equilibrium membrane tension and high poration energy. Nonetheless, vesicle fusion in the absence of mediators can also be achieved by mechanical forcing that is strong enough to induce membrane poration. Here, we employ a strong fluid shear stress to achieve vesicle fusion.
View Article and Find Full Text PDFSpherical catalytic micromotors fabricated as described in Wheat et al. [Langmuir 26, 13052 (2010)] show fuel concentration dependent translational and rotational velocity. The motors possess short-time and long-time diffusivities that scale with the translational and rotational velocity with respect to fuel concentration.
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