Microfluidics: Fluid physics at the nanoliter scale

Microfabricated integrated circuits revolutionized computation by vastly reducing the space, labor, and time required for calculations. Microfluidic systems hold similar promise for the large-scale automation of chemistry and biology, suggesting the possibility of numerous experiments performed rapidly and in parallel, while consuming little reagent. While it is too early to tell whether such a vision will be realized, significant progress has been achieved, and various applications of significant scientific and practical interest have been developed. Here a review of the physics of small volumes (nanoliters) of fluids is presented, as parametrized by a series of dimensionless numbers expressing the relative importance of various physical phenomena. Specifically, this review explores the Reynolds number Re, addressing inertial effects; the Péclet number Pe, which concerns convective and diffusive transport; the capillary number Ca expressing the importance of interfacial tension; the Deborah, Weissenberg, and elasticity numbers De, Wi, and El, describing elastic effects due to deformable microstructural elements like polymers; the Grashof and Rayleigh numbers Gr and Ra, describing density-driven flows; and the Knudsen number, describing the importance of noncontinuum molecular effects. Furthermore, the long-range nature of viscous flows and the small device dimensions inherent in microfluidics mean that the influence of boundaries is typically significant. A variety of strategies have been developed to manipulate fluids by exploiting boundary effects; among these are electrokinetic effects, acoustic streaming, and fluid-structure interactions. The goal is to describe the physics behind the rich variety of fluid phenomena occurring on the nanoliter scale using simple scaling arguments, with the hopes of developing an intuitive sense for this occasionally counterintuitive world

Experimental and Computational Investigations of Heat Transfer Systems in Fluoride Salt-cooled High-temperature Reactors

Fluoride salt-cooled high-temperature reactors (FHRs) face a number of challenges similar to those faced by other Generation IV advanced reactor concepts. Predicting heat transfer in these systems accurately and reliably is one major challenge. Another is ensuring the safety of these systems during challenging operating conditions across the design basis envelope. Finally, achieving good economics to compete in a modern power generation portfolio is necessary for moving any nuclear power plant concept past the pre-conceptual stage. This dissertation attempts to support, from a thermal-hydraulics research standpoint, the case that the FHR can attain these goals. The dissertation focuses on several aspects of the design. The common thread through the different studies is ultimately rooted in improving plant safety and economics. This dissertation has four major contributions in support of the FHR: experimental investigation of a directional direct reactor auxiliary cooling system (DRACS) heat exchanger (DHX), experimental investigation of twisted versus plain tube heat transfer for molten salt heat exchangers, and two computational studies, one on DRACS reliability and one on heat exchanger optimization. The results for the four studies are presented and discussed. The directional DHX study was performed using a hydrodynamic experimental setup with water as a working fluid and heat transfer performance inferred. The experimental heat transfer work was performed using a simulant fluid, Dowtherm A, to match the important non-dimensional heat transfer parameters. The computational DRACS reliability study was performed using MATLAB and RELAP5-3D, and the computational heat exchanger optimization study was performed using Python and available metaheuristic algorithms. The implications of the various studies are tied together in the conclusions section, with suggestions for future work

USE OF MICROSCALE HYDROPHOBIC SURFACE FEATURES FOR INTEGRATION OF 3D CELL CULTURE INTO MULTI-FUNCTIONAL MICROFLUIDIC DEVICES

3D cell culture and microfluidics both represent powerful tools for replicating critical components of the cell microenvironment; however, challenges involved in integration of the two and compatibility with standard tissue culture protocols still represent a steep barrier to widespread adoption. Here we demonstrate the use of engineered surface roughness in the form of microfluidic channels to integrate 3D cell-laden hydrogels and microfluidic fluid delivery. When a liquid hydrogel precursor solution is pipetted onto a surface containing open microfluidic channels, the solid/liquid/air interface becomes pinned at sharp edges such that the hydrogel forms the “fourth wall” of the channels upon solidification. We designed Cassie-Baxter microfluidic surfaces that leverage this phenomenon, making it possible to have barrier-free diffusion between the channels and hydrogel; in addition, sealing is robust enough to prevent leakage between the two components during fluid flow, but the sealing can also be reversed to facilitate recovery of the cell/hydrogel material after culture. This method was used to culture MDA-MB-231 cells in collagen, which remained viable and proliferated while receiving media exclusively through the microfluidic channels over the course of several days. Further modifications were made to create a multi-functional 3D cell culture platform. Gas impermeable polymer structure and deoxygenated flow were used to lower the oxygen content in the device, and the oxygen content was monitored in real-time using embedded oxygen sensors. This is particularly useful in replication of the tumor microenvironment where hypoxic conditions affect the cellular behavior and morphology. Also, by incorporating two inlets in the microfluidic device, binary concentrations of solutes were introduced into the system which created a lateral concentration gradient across the fluidic path. This allows studying of cell migration and response to various chemoattractant and drug doses. And finally, two high throughput designs to create 4-well and eight-well microfluidic devices were proposed and tested. This enables conducting more replicates of an experiment and even comparative studies on a single chip

Microfluidic Technologies for Structural Biology

In the post-genomic era, X-ray crystallography has emerged as the workhorse of large-scale structural biology initiatives that seek to understand protein function and interaction at the atomic scale. Despite impressive technological advances in X-ray sources, phasing techniques, and computing power, the determination of protein structure has been severely hampered by the difficulties in obtaining high-quality protein crystals. Emergent technologies utilizing microfluidics now have the potential to solve these problems on several levels, both by allowing researchers to conduct efficient assays in nanoliter reaction volumes, and by exploiting the properties of mass-transport at the micron scale to improve the crystallization process. The technique of Multilayer Soft Lithography (MSL) has been used to developed a set of microfluidic tools suitable for all stages of protein crystallogenesis, including protein solubility phase-space mapping, crystallization screening, harvesting, and in silicone diffraction studies. These tools represent the state of the art in on-chip fluid handling functionality and have been demonstrated to dramatically improve protein crystallization

Flow control for road vehicle drag reduction

This thesis covers topics that span bluff-body aerodynamics, hybrid RANS-LES CFD methods, flow control and model-order reduction. These topics arise from investigating the flow past three geometries: the bullet shaped D-body, the canonical squareback Ahmed body and the commerical Nissan NDP. The study on the D-body was aimed at transitioning the research group from the restrictive block-structured formulated StreamLES solver to the more flexible OpenFOAM code that can use unstructured meshes. Linear feedback control for base pressure increase was applied as was done in the work by Dalla Longa et al. (2017). Identification of the plant, G(s), that represents the wake's response to forcing was completed and correlated well with the results from Dalla Longa et al. (2017). The same can also be said of the sensitivity based designed feedback control law, K(s). When applied in simulation, an attenuation of the base pressure fluctuations was, as desired, achieved, although the base pressure increased by 24.5% as opposed to the 38% achieved by Dalla Longa et al. (2017). In the study on the squareback Ahmed body, wall-resolving (WRLES) and wall-modelled (WMLES) large eddy simulation were successfully applied. First, a simulation setup that is both able to resolve wake bimodality, while remaining reasonable in computational resource use, was created. Subsequently, variants of this setup were used to identify a flow feature that plays a critical role in forcing wake bimodality events. More specifically, a heavily under-resolved WMLES simulation in which both the near-wall and part of the outer-region of the turbulent boundary layer are Reynolds-averaged did not capture the front recirculation bubble near the Ahmed body nose; neither did it resolve a bimodal wake switching event. Meanwhile, the simulations with a more refined near-wall mesh did capture the front separation bubble as well as bimodal switching events of the wake. This front separation bubble sends out powerful hairpin vortices that interact with the rear wake. Specifically, these vortices go on to produce significant amounts of TKE, which, upon convection to the rear of the Ahmed body, ultimately help trigger a bimodal event. The Ahmed body study also involved the application of linear feedback control for drag reduction as was done in the D-body study. In the short term, mean blowing did lead to a base pressure increase, but as the zero-net-mass-flux (ZNMF) jet settled, it oscillated around zero making its effects indiscernible. The final geometry analyzed was the Nissan NDP. This was done by performing benchmark wall-resolving LES (WRLES). First, the benefit of appending a rear cavity to an otherwise "squareback" geometry was assessed. It was concluded that the cavity allows the wake to move more freely about the rear base. Specifically, the wake is freed from its more restricted motion that is present with the "squareback" Nissan NDP. In doing so, the drag reduction achieved with the cavity appendage is about 13.6%. Work on the Nissan NDP also involved an assessment of a moving ground in the simulation. It was concluded that, in the stationary ground simulation, flow detachment at the ground where the flow exits from the underbody has an adverse drag effect. In other words, although moving ground simulations better replicate the real-world conditions, the stationary ground variant is in this case more conservative, as it returns slightly higher drag values.Open Acces

Development of Microwave/Droplet-Microfluidics Integrated Heating and Sensing Platforms for Biomedical and Pharmaceutical Lab-on-a-Chip Applications

Interest in Lab-on-a-chip and droplet-based microfluidics has grown recently because of their promise to facilitate a broad range of scientific research and biological/chemical processes such as cell analysis, DNA hybridization, drug screening and diagnostics. Major advantages of droplet-based microfluidics versus traditional bioassays include its capability to provide highly monodispersed, well-isolated environment for reactions with magnitude higher throughput (i.e. kHz) than traditional high throughput systems, as well as its low reagent consumption and elimination of cross contamination. Major functions required for deploying droplet microfluidics include droplet generation, merging, sorting, splitting, trapping, sensing, heating and storing, among which sensing and heating of individual droplets remain great challenges and demand for new technology. This thesis focuses on developing novel microwave technology that can be integrated with droplet-based microfluidic platforms to address these challenges. This thesis is structured to consider both fundamentals and applications of microwave sensing and heating of individual droplets very broadly. It starts with developing a label-free, sensitive, inexpensive and portable microwave system that can be integrated with microfluidic platforms for detection and content sensing of individual droplets for high-throughput applications. This is, indeed, important since most droplet-based microfluidic studies rely on optical imaging, which usually requires expensive and bulky systems, the use of fluorescent dyes and exhaustive post-imaging analysis. Although electrical detection systems can be made inexpensive, label-free and portable, most of them usually work at low frequencies, which limits their applications to fast moving droplets. The developed microwave circuitry is inexpensive due to the use of off-the-shelf components, and is compact and capable of detecting droplet presence at kHz rates and droplet content sensing of biological materials such as penicillin antibiotic, fetal bovine serum solutions and variations in a drug compound concentration (e.g., for Alzheimer’s Disease). Subsequently, a numerical model is developed based on which parametrical analysis is performed in order to understand better the sensing and heating performance of the integrated platform. Specifically, the microwave resonator structure, which operates at GHz frequency affecting sensing performance significantly, and the dielectric properties of the microfluidic chip components that highly influence the internal electromagnetic field and energy dissipation, are studied systematically for their effects on sensing and heating efficiency. The results provide important findings and understanding on the integrated device operation and optimization strategies. Next, driven by the need for on-demand, rapid mixing inside droplets in many applications such as biochemical assays and material synthesis, a microwave-based microfluidic mixer is developed. Rapid mixing in droplets can be achieved within each half of the droplet, but not the entire droplet. Cross-center mixing is still dominated by diffusion. In this project, the microwave mixer, which works essentially as a resonator, accumulates an intensive, nonuniform electromagnetic field into a spiral capacitive gap (around 200 μm) over which a microchannel is aligned. As droplets pass by the gap region, they receive spatially non-uniform energy and thus have non-uniform temperature distribution, which induces non-uniform Marangoni stresses on the interface and thus three-dimensional (3D) chaotic motion inside the droplet. The 3D chaotic motion inside the droplet enables fast mixing within the entire droplet. The mixing efficiency is evaluated by varying the applied power, droplet length and fluid viscosity. In spite of various existing thermometry methods for microfluidic applications, it remains challenging to measure the temperature of individual fast moving droplets because they do not allow sufficient exposure time demanded by both fluorescence based techniques and resistance temperature detectors. A microwave thermometry method is thus developed here, which relies on correlating fluid temperature with the resonance frequency and the reflection coefficient of the microwave sensor, based on the fact that liquid permittivity is a function of temperature. It is demonstrated that the sensor can detect the temperature of individual droplets with ±1.2 °C accuracy. At the final part of the thesis, I extend my platform technology further to applications such as disease diagnosis and drug delivery. First, I develop a microfluidic chip for controlled synthesis of poly (acrylamide-co-sodium acrylate) copolymer hydrogel microparticles whose structure varies with temperature, chemical composition and pH values. This project investigates the effects of monomer compositions and cross-linker concentrations on the swelling ratio. The results are validated through the Fourier transform infrared spectra (FTIR), SEM and swelling test. Second, a preliminary study on DNA hybridization detection through microwave sensors for disease diagnosis is conducted. Gold sensors and biological protocols of DNA hybridization event are explored. The event of DNA hybridization with the immobilized thiol-modified ss-DNA oligos and complimentary DNA (c-DNA) are monitored. The results are promising, and suggests that microwave integrated Lab-on-a-chip platforms can perform disease diagnosis studies

Membraneless Electrolyzers for Solar Fuels Production

Solar energy has the potential to meet all of society’s energy demands, but challenges remain in storing it for times when the sun is not shining. Electrolysis is a promising means of energy storage which applies solar-derived electricity to drive the production of chemical fuels. These so-called solar fuels, such as hydrogen gas produced from water electrolysis, can be fed back to the grid for electricity generation or used directly as a fuel in the transportation sector. Solar fuels can be generated by coupling a photovoltaic (PV) cell to an electrolyzer, or by directly converting light to chemical energy using a photoelectrochemical cell (PEC). Presently, both PV-electrolyzers and PECs have prohibitively high capital costs which prevent them from generating hydrogen at competitive prices. This dissertation explores the design of membraneless electrolyzers and PECs in order to simplify their design and decrease their overall capital costs. A membraneless water electrolyzer can operate with as few as three components: A cathode for the hydrogen evolution reaction, an anode for the oxygen evolution reaction, and a chassis for managing the flows of a liquid electrolyte and the product gas streams. Absent from this device is an ionically conducting membrane, a key component in a conventional polymer electrolyte membrane (PEM) electrolyzer that typically serves as a physical barrier for separating product gases generated at the anode and cathode. These membranes can allow for compact and efficient electrolyzer designs, but are prone to degradation and failure if exposed to impurities in the electrolyte. A membraneless electrolyzer has the opportunity to reduce capital costs and operate in non-pristine environments, but little is known about the performance limitations and design rules that govern operation of membraneless electrolyzers. These design rules require a thorough understanding of the thermodynamics, kinetics, and transport processes in electrochemical systems. In Chapter 2, these concepts are reviewed and a framework is provided to guide the continuum scale modeling of the performance of membraneless electrochemical cells. Afterwards, three different studies are presented which combine experiment and theory to demonstrate the mechanisms of product transport and efficiency loss. Chapter 3 investigates the dynamics of hydrogen bubbles during operation of a membraneless electrolyzer, which can strongly affect the product purity of the collected hydrogen. High-speed video imaging was implemented to quantify the size and position of hydrogen gas bubbles as they detach from porous mesh electrodes. The total hydrogen detected was compared to the theoretical value predicted by Faraday’s law. This analysis confirmed that not all electrochemically generated hydrogen enters the gas phase at the cathode surface. In fact, significant quantities of hydrogen remain dissolved in solution, and can result in lower product collection efficiencies. Differences in bubble volume fraction evolved along the length of the cathode reflect differences in the local current densities, and were found to be in agreement with the primary current distribution. Overall, this study demonstrates the ability to use in-situ HSV to quantitatively evaluate key performance metrics of membraneless electrolyzers in a non-invasive manner. This technique can be of great value for future experiments, where statistical analysis of bubble sizes and positions can provide information on how to collect hydrogen at maximum purity. Chapter 4 presents an electrode design where selective placement of the electrocatalyst is shown to enhance the purity of hydrogen collected. These “asymmetric electrodes” were prepared by coating only one planar face of a porous titanium mesh electrode with platinum electrocatalyst. For an opposing pair of electrodes, the platinum coated surface faces outwards such that the electrochemically generated bubbles nucleate and grow on the outside while ions conduct through the void spacing in the mesh and across the inter-electrode gap. A key metric used in evaluating the performance of membraneless electrolyzers is the hydrogen cross-over percentage, which is defined as the fraction of electrochemically generated hydrogen that is collected in the headspace over the oxygen-evolving anode. When compared to the performance of symmetric electrodes – electrodes coated on both faces with platinum – the asymmetric electrodes demonstrated significantly lower rates of cross-over. With optimization, asymmetric electrodes were able to achieve hydrogen cross-over values as low as 1%. These electrodes were then incorporated into a floating photovoltaic electrolysis device for a direct demonstration of solar driven electrolysis. The assembled “solar fuels rig” was allowed to float in a reservoir of 0.5 M sulfuric acid under a light source calibrated to simulate sunlight, and a solar to hydrogen efficiency of 5.3% was observed. In Chapter 5, the design principles for membraneless electrolyzers were applied to a photoelectrochemical (PEC) cell. Whereas an electrolyzer is externally powered by electricity, a PEC cell can directly harvest light to drive an electrochemical reaction. The PEC reactor was based on a parallel plate design, where the current was demonstrated to be limited by the intensity of light and the concentration of the electrolyte. By increasing the average flow rate of the electrolyte, mass transport limitations could be alleviated. The limiting current density was compared to theoretical values based off of the solution to a convection-diffusion problem. This modeled solution was used to predict the limitations to PEC performance in scaled up designs, where solar concentration mirrors could increase the total current density. The mass transport limitations of a PEC flow cell are also highly relevant to the study of CO2 reduction, where the solubility limit of CO2 in aqueous electrolyte can also limit performance

Electrostatic control and enhancement of film boiling heat transfer

Boiling heat transfer is severely degraded at high surface temperatures due to the formation of a vapor layer at the surface, commonly known as the Leidenfrost effect. Heat transfer is limited to a critical heat flux (CHF); higher heat fluxes lead to surface dryout and temperature excursions. An externally applied electric field in the vapor layer can significantly enhance boiling heat transfer for electrically conducting or polar liquids. In such liquids, the electric field is concentrated in the vapor layer, and promotes liquid-surface contact, which can significantly enhance boiling heat transfer. This dissertation is a fundamental study of the influence of concentrated interfacial electric fields on film boiling heat transfer for liquids with finite electrical conductivity (like water and organic solvents). This dissertation describes experimental, analytical and numerical studies on various aspects of the physics underlying electrostatic suppression of film boiling. This dissertation also quantifies the heat transfer benefits associated with electrostatic suppression of film boiling. This dissertation is divided into five main studies, which analyze different aspects of electrostatic suppression of the Leidenfrost state. The first part of this dissertation (Chapter 2) describes droplet-based experimental investigations on electrostatic suppression of the Leidenfrost state. It is demonstrated that the Leidenfrost state can be suppressed and surface dryout can be prevented using externally applied electric fields (AC or DC). Elimination of the Leidenfrost state increases heat dissipation capacity by more than one order of magnitude. In preliminary experiments, heat removal capacities exceeding 500 W/cm² are measured for water, which is five times the CHF of water on common engineering surfaces. A multiphysics analytical model is developed to predict the vapor layer thickness in the Leidenfrost state. The second part of this dissertation (Chapter 3) analyzes the fundamental mechanisms underlying electrostatic suppression of Leidenfrost state. It is shown that the interplay of destabilizing and stabilizing forces determines the minimum (threshold) voltage required to suppress the Leidenfrost state. Detailed linear instability analysis is conducted to investigate the growth of electrostatically-induced perturbations on the liquid-vapor interface in the Leidenfrost state, and predict the threshold voltage required for suppression. The third part of this dissertation (Chapter 4) focuses on suppression of the Leidenfrost state on soft, deformable surfaces, like liquids. It is seen that the nature of electrostatic suppression on a deformable liquid substrate is drastically different from that on a solid substrate. This is due to the existence of an electric field inside the substrate and the deformability of the substrate. A multiphysics analytical model is developed to predict the vapor layer thickness on deformable liquids. The fourth part of this dissertation (Chapter 5) includes experimental studies on suppression of film boiling during high temperature quenching of metals. It is shown that an electric field can fundamentally change the boiling patterns, wherein the stable vapor layer (film boiling) is replaced by intermittent wetting of the surface. This fundamental switch in the heat transfer mode significantly accelerates cooling during quenching. An order of magnitude increase in the cooling rate is observed, with the heat transfer seen approaching saturation at higher voltages. An analytical model is developed to extract voltage dependent heat transfer rates from the measured cooling curve. The fifth part of this dissertation (Chapter 6) develops the concept of using acoustic signature tracking to study electrostatic suppression of film boiling. It is shown that acoustic signature tracking can be the basis for objective measurements of the threshold voltage and frequency required for suppression. Acoustic signature tracking can also detect various boiling patterns associated with electrostatically-assisted quenching. With appropriate calibration, this technique can be used to estimate surface temperatures, heat flux and onset of dryout associated with electrically enhanced boiling. In summary, this dissertation has led to seminal contributions in the field of boiling heat transfer, and essentially opened up a new area of study in the field. This work has shown that electric fields can make the CHF limit irrelevant, and reshape the boiling curve. The present work lays the foundations for electrically tunable boiling heat transfer with conducting liquids. The impact of the proposed work is evident in the area of quenching, where electrically tunable cooling offers a new tool to control the microstructure and mechanical properties of metals.Mechanical Engineerin