Droplet microfluidics is a powerful technology that finds many applications in chemistry and biomedicine. Among different configurations, droplets confined in a capillary (or plugs) present a number of advantages: they allow positional identification and simplify the integration of complex multi-steps protocols. However, these protocols rely on the control of droplet speed, which is affected by a complex and still debated interplay of various physico-chemical parameters like droplet length, viscosity ratio between droplets and carrier fluid, flow rate and interfacial tension. We present here a systematic investigation of the droplet speed as a function of their length and interfacial tension, and propose a novel, simple and robust methodology to control the relative distance between consecutive droplets flowing in microfluidic channels through the addition of surfactants either into the dispersed and/or into the continuous phases. As a proof of concept application, we present the possibility to accurately trigger in space and time the merging of two confined droplets flowing in a uniform cross-section circular capillary. This approach is further validated by monitoring a conventional enzymatic reaction used to quantify the concentration of H2O2 in a biological sample, showing its potentialities in both continuous and stopped assay methods.
We have studied the motion of drops on inclined liquid-impregnated surfaces (LISs) subject to vertical vibrations. The liquid drops comprise distilled water and different aqueous solutions of glycerol of increasing viscosity. The use of weak pinning LISs strongly affects the dynamical phase diagram. First of all, there is no trace of the dominant static region at low oscillating amplitudes reported for oscillating solid surfaces characterized by contact angle hysteresis. On the contrary, at sufficiently low oscillating amplitudes, the drops always move downwards with a velocity that depends only on the drop viscosity. Further increasing the oscillating amplitude may drive the drop upwards against gravity, as reported for dry surfaces. The use of more viscous drops widens this climbing region. Arguably, the main novelty of this work concerns the observation of two distinct descending regimes where the downhill speed differs by a factor of five or more. Fast-rate videos show that the evolution of the drop profile is diverse in the two regimes, likely because the vertical oscillations reduce the effect of the oil meniscus surrounding the drop at high accelerations.
The flow of emulsions in confined microfluidic channels is affected by surface roughness. Directional roughness effects have recently been reported in channels with asymmetric boundary conditions featuring a flat wall, and a wall textured with a directional roughness, the latter promoting a change in the velocity profiles when the flow direction of emulsions is inverted [D. Filippi et al., Adv. Mater. Technol.8, 2201748 (2023)]. An operative protocol is needed to reconstruct the stress profile inside the channel from velocity data to shed light on the trigger of the directional response. To this aim, we performed lattice Boltzmann numerical simulations of the flow of model emulsions with a minimalist model of directional roughness in two dimensions: a confined microfluidic channel with one flat wall and the other patterned by right-angle triangular-shaped posts. Simulations are essential to develop the protocol based on mechanical arguments to reconstruct stress profiles. Hence, one can analyze data to relate directional effects in velocity profiles to different rheological responses close to the rough walls associated with opposite flow directions. We finally show the universality of this protocol by applying it to other realizations of directional roughness by considering experimental data on emulsions in a microfluidic channel featured with a flat wall and a wall textured by herringbone-shaped roughness.
Fluidization of soft glassy materials (SGMs) in microfluidic channels is affected by the wall roughness in the form of microtexturing. When SGMs flow across microgrooves, their constituents are likely trapped within the grooves' gap, and the way they are released locally modifies the fluidization close to the walls. By leveraging a suitable combination of experiments and numerical simulations on concentrated emulsions (a model SGM), we quantitatively report the existence of two physically different scenarios. When the gap is large compared to the droplets in the emulsion, the droplets hit the solid obstacles and easily escape scrambling with their neighbors. Conversely, as the gap spacing is reduced, droplets get trapped inside, creating a “soft roughness” layer, i.e. a complementary series of deformable posts from which overlying droplets are in turn released. In both cases, the induced fluidization scales with the grooves' density, although with a reduced prefactor for narrow gaps, accounting for the softness of the roughness. Both scenarios are also well distinguished via the statistics of the droplets displacement field close to the walls, with large deviations induced by the surface roughness, depending on its stiffness.
8 November 2024 in Environmental Science & Technology
High-resolution mass spectrometry (HRMS) has become an indispensable tool in the characterization of organic aerosols (OA) providing information on air quality, health assessment, climate trends, reactions, and source apportionment. Spectra-derived lists of formulas and their relative abundances are used to compare ambient OA from different sources or to monitor secondary OA formation under controlled laboratory conditions in smog chamber experiments. Various techniques are implemented to visualize common and unique features, series of precursors, and products. The disadvantage of this conventional approach is in associating elemental compositions to specific compounds, while due to several analytical limitations, the structural information remains hidden. We argue that some of the conclusions derived from this data analysis can be misleading. In this study, we applied in-ESI source H/D exchange (HDX), which facilitated enumeration of labile protons in molecules behind elemental compositions of OA. We applied this technique to compare OA from three different locations representing urban, forest, and marine environments and to examine tentative chemical information derived from Kendrick mass defect (KMD) series analysis. Significant discrepancies were found between numbers of labile protons in protogenic functional groups and the stoichiometry of chemical reactions, which are associated with KMD series. Only a portion of chemical pairs matched target stoichiometries, which highlights the existing limitations in environmental applications of conventional formula-based HRMS data interpretation strategies.
9 January 2024 in ACS Applied Materials & Interfaces
Controlled splitting of liquid droplets is a key function in many microfluidic applications. In recent years, various methodologies have been used to accomplish this task. Here, we present an optofluidic technique based on an engineered surface formed by coating a z-cut iron-doped lithium niobate crystal with a lubricant-infused layer, which provides a very slippery surface. Illuminating the crystal with a light spot induces surface charges of opposite signs on the two crystal faces because of the photovoltaic effect. If the light spot is sufficiently intense, millimetric water droplets placed near the illuminated spot split into two charged fragments, one fragment being trapped by the bright spot and the other moving away from it. The latter fragment does not move randomly but rather follows one of three well-defined trajectories separated by 120°, which reflect the anisotropic crystalline structure of Fe:LiNbO3. Numerical simulations explain the behavior of water droplets in the framework of the forces induced by the interplay of pyroelectric, piezoelectric, and photovoltaic effects, which originate simultaneously inside the illuminated crystal. Such a synergetic effect can provide a valuable feature in applications that require splitting and coalescence of droplets, such as chemical microreactors and biological encapsulation and screening.