Volkert van Steijn

All-aqueous core-shell droplets produced in a microfluidic device

We present a microfluidic method to compartmentalize aqueous polymer solutions within water-in-water microdroplets, which are continuously generated without using organic solvents or surfactants. Phase separation inside the drops yields all-aqueous core-shell structures (water-in-water-in-water), as we demonstrate using the aqueous two phase system of polyethylene glycol and dextran.

Slow growth of the Rayleigh-Plateau instability in aqueous two phase systems

This paper studies the Rayleigh-Plateau instability for co-flowing immiscible aqueous polymer solutions in a microfluidic channel. Careful vibration-free experiments with controlled actuation of the flow allowed direct measurement of the growth rate of this instability. Experiments for the well-known aqueous two phase system (ATPS, or aqueous biphasic systems) of dextran and polyethylene glycol solutions exhibited a growth rate of 1 s(-1), which was more than an order of magnitude slower than an analogous experiment with two immiscible Newtonian fluids with viscosities and interfacial tension that closely matched the ATPS experiment. Viscoelastic effects and adhesion to the walls were ruled out as explanations for the observed behavior. The results are remarkable because all current theory suggests that such dilute polymer solutions should break up faster, not slower, than the analogous Newtonian case. Microfluidic uses of aqueous two phase systems include separation of labile biomolecules but have hitherto be limited because of the difficulty in making droplets. The results of this work teach how to design devices for biological microfluidic ATPS platforms.

Block-and-break generation of microdroplets with fixed volume.

We introduce a novel type of droplet generator that produces droplets of a volume set by the geometry of the droplet generator and not by the flow rates of the liquids. The generator consists of a classic T-junction with a bypass channel. This bypass directs the continuous fluid around the forming droplets, so that they can fill the space between the inlet of the dispersed phase and the exit of the bypass without breaking. Once filled, the dispersed phase blocks the exit of the bypass and is squeezed by the continuous fluid and broken off from the junction. We demonstrate the fixed-volume droplet generator for (i) the formation of monodisperse droplets from a source of varying flow rates, (ii) the formation of monodisperse droplets containing a gradation of solute concentration, and (iii) the parallel production of monodisperse droplets.

Droplets on inclined plates: local and global hysteresis of pinned capillary surfaces.

Local contact line pinning prevents droplets from rearranging to minimal global energy, and models for droplets without pinning cannot predict their shape. We show that experiments are much better described by a theory, developed herein, that does account for the constrained contact line motion, using as an example droplets on tilted plates. We map out their shapes in suitable phase spaces. For 2D droplets, the critical point of maximum tilt depends on the hysteresis range and Bond number. In 3D, it also depends on the initial width, highlighting the importance of the deposition history.

Calculating the volume of elongated bubbles and droplets in microchannels from a top view image

We present a theoretical model to calculate the volume of non-wetting bubbles and droplets in segmented microflows from given dimensions of the microchannel and measured lengths of bubbles and droplets. Despite the importance of these volumes in interpreting experiments on reaction kinetics and transport phenomena, an accurate model like the one we present here did not yet exist. The model has its theoretical basis in the principle of interfacial energy minimization and is set up such that volume calculations are possible for a wide variety of channel geometries. We successfully validated our model with the 3D numerical energy minimization code SURFACE EVOLVER for the three most commonly used channel geometries in the field of microfluidics and provide accurate user-friendly equations for these geometries.

Microcapsules with a permeable hydrogel shell and an aqueous core continuously produced in a 3D microdevice by all-aqueous microfluidics

We report the continuous production of microcapsules composed of an aqueous core and permeable hydrogel shell, made stable by the controlled photo-cross-linking of the shell of an all-aqueous double emulsion. While most previous work on water-based emulsions focused on active droplet formation, here double emulsion droplets were spontaneously generated at a three-dimensional flow-focusing junction through the break-up of a double jet formed by immiscible aqueous solutions of polyethylene glycol and cross-linkable dextrans. The capsules obtained with this lipid-free, organic-solvent-free, and surfactant-free approach displayed excellent stability under a variety of harsh conditions (3 < pH < 13, high salinity). Drying and rehydration experiments demonstrate the permeability of the shell, which may enable molecular-weight-dependent release and uptake of polar solutes.

Free-standing supramolecular hydrogel objects by reaction-diffusion

Self-assembly provides access to a variety of molecular materials, yet spatial control over structure formation remains difficult to achieve. Here we show how reaction–diffusion (RD) can be coupled to a molecular self-assembly process to generate macroscopic free-standing objects with control over shape, size, and functionality. In RD, two or more reactants diffuse from different positions to give rise to spatially defined structures on reaction. We demonstrate that RD can be used to locally control formation and self-assembly of hydrazone molecular gelators from their non-assembling precursors, leading to soft, free-standing hydrogel objects with sizes ranging from several hundred micrometres up to centimeters. Different chemical functionalities and gradients can easily be integrated in the hydrogel objects by using different reactants. Our methodology, together with the vast range of organic reactions and self-assembling building blocks, provides a general approach towards the programmed fabrication of soft microscale objects with controlled functionality and shape.

Erratum: Free-standing supramolecular hydrogel objects by reaction-diffusion

This corrects the article DOI: 10.1038/ncomms15317.

Modeling and simulation of diffusion-convection-reaction in heterogeneous nanochannels using OpenFOAM

We present a finite volume implementation of a phase field method in OpenFOAM as a tool to simulate reactive multiphase flows on heterogeneous surfaces. Using this tool, we simulate the formation and growth of a droplet due to a chemical reaction on a hydrophilic catalytic patch surrounded by a hydrophobic wall. We compare the growth dynamics with a quasi-static growth model from literature and show that they qualitatively agree.

Reaction-diffusion analysis for one-step plasma etching and bonding of microfluidic devices

A self-similar reaction front develops in reactive ion etching when the ions penetrate channels of shallow height h. This relates to the patterning of microchannels using a single-step etching and bonding, as described by Rhee et al. [Lab Chip 5, 102 (2005)] . Experimentally, we report that the front location scales as xf ? ht1/2 and the width is time-invariant and scales as ? ? h. Mean-field reaction-diffusion theory and Knudsen diffusion give a semiquantitative understanding of these observations and allow optimization of etching times in relation to bonding requirements.