Elucidating the Mechanism of Condensation-Mediated Degradation of Organofunctional Silane Self-Assembled Monolayer Coatings.

Dropwise condensation is favorable for numerous industrial and heat/mass transfer applications due to the enhanced heat transfer performance that results from efficient condensate removal. Organofunctional silane self-assembled monolayer (SAM) coatings are one of the most common ultrathin low surface energy materials used to promote dropwise condensation of water vapors because of their minimal thermal resistance and scalable synthesis process. These SAM coatings typically degrade (i.e., condensation transitions from the efficient dropwise mode to the inefficient filmwise mode) rapidly during water vapor condensation. More importantly, the condensation-mediated coating degradation/failure mechanism(s) remain unknown and/or unproven. In this work, we develop a mechanistic understanding of water vapor condensation-mediated organofunctional silane SAM coating degradation and validate our hypothesis through controlled coating synthesis procedures on silicon/silicon dioxide substrates. We further demonstrate that a pristine organofunctional silane SAM coating resulting from a water/moisture-free coating environment exhibits superior long-term robustness during water vapor condensation. Our molecular/nanoscale surface characterizations, pre- and post-condensation heat transfer testing, indicate that the presence of moisture in the coating environment leads to uncoated regions of the substrate that act as nucleation sites for coating degradation. By elucidating the reasons for formation of these degradation nuclei and demonstrating a method to suppress such defects, this study provides new insight into why low surface energy silane SAM coatings degrade during water vapor condensation. The proposed approach addresses a key bottleneck (i.e., coating failure) preventing the adoption of efficient dropwise condensation methods in industry, and it will facilitate enhanced phase-change heat transfer technologies in industrial applications.

Efficient Heat Shielding of Steel with Multilayer Nanocomposite Thin Film.

In an effort to protect metal substrates from extreme heat, polymer-clay multilayer thin films are studied as expendable thermal barrier coatings. Nanocomposite films with a thickness ranging from 2 to 35 µm were deposited on steel plates and exposed to the flame from a butane torch. The 35 µm coating, composed of 14 deposited bilayers of tris(hydroxymethyl)aminomethane (THAM)-buffered polyethylenimine (PEI) and vermiculite clay (VMT), decreased the maximum temperature observed on the back side of a 0.32 cm thick steel plate by over 100 °C when heated with a butane torch. Upon exposure to high temperature, the polymer and amine salt undergo pyrolysis and intumesce, subsequently forming a char and blowing gas. The char encases the nanoclay platelets, and a ceramic bubble is formed. The macro-scale bubble, in tandem with the nanocomposite coating properties, increases resistance to heat transfer into the underlying metal substrate. This heat shielding behavior occurs through radiative effects and low aggregate through-plane conductivity resulting from multilayer nanodomains and intumesced porosity (i.e., conduction through the gas as the film expands to form a ceramic bubble). These relatively thin and lightweight films could be used to protect important metal parts (in automobiles, aircraft, etc.) from fire-related damage or other types of transient high-temperature situations.

Polymer Infused Porous Surfaces for Robust, Thermally Conductive, Self-Healing Coatings for Dropwise Condensation.

Hydrophobic coatings with low thermal resistance promise a significant enhancement in condensation heat transfer performance by promoting dropwise condensation in applications including power generation, water treatment, and thermal management of high-performance electronics. However, after nearly a century of research, coatings with adequate robustness remain elusive due to the extreme environments within many condensers and strict design requirements needed to achieve enhancement. In this work, we enable long-lasting condensation heat transfer enhancement via dropwise condensation by infusing a hydrophobic polymer, Teflon AF, into a porous nanostructured surface. This polymer infused porous surface (PIPS) uses the large surface area of the nanostructures to enhance polymer adhesion, while the nanostructures form a percolated network of high thermal conductivity material throughout the polymer and drastically reduce the thermal resistance of the composite. We demonstrate over 700% enhancement in the condensation of steam compared to an uncoated surface. This performance enhancement was sustained for more than 200 days without significant degradation. Furthermore, we show that the surfaces are self-repairing upon raising the temperature past the melting point of the polymer, allowing recovery of hydrophobicity and offering a level of durability more appropriate for industrial applications.

High Heat Flux Evaporation of Low Surface Tension Liquids from Nanoporous Membranes.

Water is often considered as the highest performance working fluid for liquid-vapor phase change due to its high thermal conductivity and large enthalpy of vaporization. However, a wide range of industrial systems require using low surface tension liquids where heat transfer enhancement has proved challenging for boiling and evaporation. Here, we enable a new paradigm of phase change heat transfer, which favors high volatility, low surface tension liquids rather than water. We utilized a nanoporous membrane of ≈600 nm thickness and <140 nm pore diameters supported on efficient liquid supply architectures, decoupling capillary pumping from viscous loss. Proof-of-concept devices were microfabricated and tested in a custom-built environmental chamber. We used R245fa, pentane, methanol, isopropyl alcohol, and water as working fluids with devices of total membrane area varying from 0.017 to 0.424 cm2. We realized a device-level pure evaporation heat flux of 144 ± 6 W/cm2 for water, and the highest evaporation heat flux was obtained with pentane at 550 ± 90 W/cm2. We developed a three-level model to understand vapor dynamics near the interface and thermal conduction within the device, which showed good agreement with experiments. We then compared pore-level heat transfer of different fluids, where R245fa showed approximately 10 times the performance of water under the same working conditions. Finally, we illustrate the usefulness of a figure of merit extracted from the kinetic theory for evaporation. The current work provides fundamental insights into the evaporation of low surface tension liquids, which can impact various applications such as refrigeration and air conditioning, petroleum and solvent distillation, and on-chip electronics cooling.

Unified Modeling Framework for Thin-Film Evaporation from Micropillar Arrays Capturing Local Interfacial Effects.

Thin-film evaporation from micropillar array porous media has gained attention in a number of fields including energy conversion and thermal management of electronics. Performance in these applications is enhanced by leveraging the geometries of the micropillar arrays to both optimize flow through these arrays via capillary pumping and increase the curved liquid-vapor interface (meniscus) area for active phase-change heat transfer. In this work, we present a unified semianalytical modeling framework to predict the dry-out heat flux accurately for thin-film evaporation from micropillar arrays with the precise prediction of (i) the pressure profile along the wick achieved by discretizing the porous media domain and (ii) the local permeability that depends on the local meniscus shape. We validate the permeability model with 3D numerical simulations and verify the accuracy of the thin-film evaporation modeling framework with available experimental data from the literature. We emphasize the importance of predicting an accurate liquid-vapor interface shape for the prediction accuracy of both the permeability and the associated governing equations for liquid propagation and phase-change heat transfer through porous materials. This modeling framework is an accurate non-CFD-based methodology for predicting the dry-out heat flux during thin-film evaporation from micropillar arrays and will serve as a general framework for modeling steady liquid-vapor phase-change processes (evaporation and condensation) in porous media.

Acoustically driven oscillatory flow fields in a cylindrical resonator at resonance.

Generation and development of acoustic waves in an air-filled cylindrical resonator driven by a conical electro-mechanical speaker are studied experimentally and simulated numerically. The driving frequencies of the speaker are chosen such that a standing wave field is produced at each chosen frequency in the resonator. The amplitude of the generated acoustic (pressure) waves is measured along the axis of the resonator by a fast response piezo-resistive pressure transducer, while the radial distribution of the oscillatory axial velocities is measured at the corresponding velocity anti-node locations by a constant temperature hot-film anemometer. For the cases studied, the acoustic Reynolds number ranged between 20.0 and 60.0 and the flow fields were always found to be in the laminar regime. The flow field in the resonator is also simulated by a high-fidelity numerical scheme with low numerical diffusion. Formation of the standing wave and quasi-steady acoustic streaming are numerically simulated by solving the fully compressible form of the Navier-Stokes equations. The effects of the sound field intensity (i.e., input power to the speaker) and driving frequency on the standing wave field and the resultant formation process of the streaming structures are also investigated.

Capillary-Enhanced Filmwise Condensation in Porous Media.

Condensation is prevalent in various industrial and heat/mass transfer applications, and improving condensation heat transfer has a direct effect on process efficiency. Enhancing condensation performance has historically been achieved via the use of low surface energy coatings to promote the efficient dropwise mode over the typical filmwise mode of condensation. However, low surface tension fluids condense on these coatings in the filmwise mode, and low surface energy coatings are generally not robust at thicknesses required to enhance condensation heat transfer. We present a robust and scalable condensation enhancement method where a high heat transfer coefficient is achieved by leveraging capillary forces within a high thermal conductivity porous wick to promote condensate removal. The capillary pressure is supported by a pump to sustain steady condensate removal, and the high thermal conductivity of the wick decreases the overall thermal resistance. This technique has the potential to enhance condensation for a variety of fluids including low surface tension fluids and is capable of operating in both a gravity and a micro- (or zero-) gravity environment. We highlight key characteristics and enhancements achieved through this capillary-enhanced filmwise condensation technique using a porous media flow model. The model results indicate that increased wick thickness and permeability increase the operational envelope and delay the failure that occurs when the condensate floods the wick. However, increasing the permeability is more favorable as both the heat transfer coefficient and the flooding threshold are increased. The working fluid thermophysical properties determine both the degree of enhancement possible and the relative contributions from gravitational and capillary pressure forces when condensation occurs in the presence of gravity. This study provides fundamental insight into an enhanced filmwise condensation technique and an improved framework for modeling porous media flows with mass addition via condensation.

Heat Transfer Enhancement During Water and Hydrocarbon Condensation on Lubricant Infused Surfaces.

Vapor condensation is routinely used as an effective means of transferring heat or separating fluids. Dropwise condensation, where discrete droplets form on the condenser surface, offers a potential improvement in heat transfer of up to an order of magnitude compared to filmwise condensation, where a liquid film covers the surface. Low surface tension fluid condensates such as hydrocarbons pose a unique challenge since typical hydrophobic condenser coatings used to promote dropwise condensation of water often do not repel fluids with lower surface tensions. Recent work has shown that lubricant infused surfaces (LIS) can promote droplet formation of hydrocarbons. In this work, we confirm the effectiveness of LIS in promoting dropwise condensation by providing experimental measurements of heat transfer performance during hydrocarbon condensation on a LIS, which enhances heat transfer by ≈450% compared to an uncoated surface. We also explored improvement through removal of noncondensable gases and highlighted a failure mechanism whereby shedding droplets depleted the lubricant over time. Enhanced condensation heat transfer for low surface tension fluids on LIS presents the opportunity for significant energy savings in natural gas processing as well as improvements in thermal management, heating and cooling, and power generation.

Nanoporous membrane device for ultra high heat flux thermal management.

High power density electronics are severely limited by current thermal management solutions which are unable to dissipate the necessary heat flux while maintaining safe junction temperatures for reliable operation. We designed, fabricated, and experimentally characterized a microfluidic device for ultra-high heat flux dissipation using evaporation from a nanoporous silicon membrane. With ~100 nm diameter pores, the membrane can generate high capillary pressure even with low surface tension fluids such as pentane and R245fa. The suspended ultra-thin membrane structure facilitates efficient liquid transport with minimal viscous pressure losses. We fabricated the membrane in silicon using interference lithography and reactive ion etching and then bonded it to a high permeability silicon microchannel array to create a biporous wick which achieves high capillary pressure with enhanced permeability. The back side consisted of a thin film platinum heater and resistive temperature sensors to emulate the heat dissipation in transistors and measure the temperature, respectively. We experimentally characterized the devices in pure vapor-ambient conditions in an environmental chamber. Accordingly, we demonstrated heat fluxes of 665 ± 74 W/cm2 using pentane over an area of 0.172 mm × 10 mm with a temperature rise of 28.5 ± 1.8 K from the heated substrate to ambient vapor. This heat flux, which is normalized by the evaporation area, is the highest reported to date in the pure evaporation regime, that is, without nucleate boiling. The experimental results are in good agreement with a high fidelity model which captures heat conduction in the suspended membrane structure as well as non-equilibrium and sub-continuum effects at the liquid-vapor interface. This work suggests that evaporative membrane-based approaches can be promising towards realizing an efficient, high flux thermal management strategy over large areas for high-performance electronics.

Design of Lubricant Infused Surfaces.

Lubricant infused surfaces (LIS) are a recently developed and promising approach to fluid repellency for applications in biology, microfluidics, thermal management, lab-on-a-chip, and beyond. The design of LIS has been explored in past work in terms of surface energies, which need to be determined empirically for each interface in a given system. Here, we developed an approach that predicts a priori whether an arbitrary combination of solid and lubricant will repel a given impinging fluid. This model was validated with experiments performed in our work as well as in literature and was subsequently used to develop a new framework for LIS with distinct design guidelines. Furthermore, insights gained from the model led to the experimental demonstration of LIS using uncoated high-surface-energy solids, thereby eliminating the need for unreliable low-surface-energy coatings and resulting in LIS repelling the lowest surface tension impinging fluid (butane, γ ≈ 13 mN/m) reported to date.

Coexistence of Pinning and Moving on a Contact Line.

Textured surfaces are instrumental in water repellency or fluid wicking applications, where the pinning and depinning of the liquid-gas interface plays an important role. Previous work showed that a contact line can exhibit nonuniform behavior due to heterogeneities in surface chemistry or roughness. We demonstrate that such nonuniformities can be achieved even without varying the local energy barrier. Around a cylindrical pillar, an interface can reside in an intermediate state where segments of the contact line are pinned to the pillar top while the rest of the contact line moves along the sidewall. This partially pinned mode is due to the global nonaxisymmetric pattern of the surface features and exists for all textured surfaces, especially when superhydrophobic surfaces are about to be flooded or when capillary wicks are close to dryout.

Prediction and Characterization of Dry-out Heat Flux in Micropillar Wick Structures.

Thin-film evaporation in wick structures for cooling high-performance electronic devices is attractive because it harnesses the latent heat of vaporization and does not require external pumping. However, optimizing the wick structures to increase the dry-out heat flux is challenging due to the complexities in modeling the liquid-vapor interface and the flow through the wick structures. In this work, we developed a model for thin-film evaporation from micropillar array wick structures and validated the model with experiments. The model numerically simulates liquid velocity, pressure, and meniscus curvature along the wicking direction by conservation of mass, momentum, and energy based on a finite volume approach. Specifically, the three-dimensional meniscus shape, which varies along the wicking direction with the local liquid pressure, is accurately captured by a force balance using the Young-Laplace equation. The dry-out condition is determined when the minimum contact angle on the pillar surface reaches the receding contact angle as the applied heat flux increases. With this model, we predict the dry-out heat flux on various micropillar structure geometries (diameter, pitch, and height) in the length scale range of 1-100 µm and discuss the optimal geometries to maximize the dry-out heat flux. We also performed detailed experiments to validate the model predictions, which show good agreement. This work provides insights into the role of surface structures in thin-film evaporation and offers important design guidelines for enhanced thermal management of high-performance electronic devices.

Dynamic Evolution of the Evaporating Liquid-Vapor Interface in Micropillar Arrays.

Capillary assisted passively pumped thermal management devices have gained importance due to their simple design and reduction in energy consumption. The performance of these devices is strongly dependent on the shape of the curved interface between the liquid and vapor phases. We developed a transient laser interferometry technique to investigate the evolution of the shape of the liquid-vapor interface in micropillar arrays during evaporation heat transfer. Controlled cylindrical micropillar arrays were fabricated on the front side of a silicon wafer, while thin-film heaters were deposited on the reverse side to emulate a heat source. The shape of the meniscus was determined using the fringe patterns resulting from interference of a monochromatic beam incident on the thin liquid layer. We studied the evolution of the shape of the meniscus on these surfaces under various operating conditions including varying the micropillar geometry and the applied heating power. By monitoring the transient behavior of the evaporating liquid-vapor interface, we accurately measured the absolute location and shape of the meniscus and calculated the contact angle and the maximum capillary pressure. We demonstrated that the receding contact angle which determines the capillary pumping limit is independent of the microstructure geometry and the rate of evaporation (i.e., the applied heating power). The results of this study provide fundamental insights into the dynamic behavior of the liquid-vapor interface in wick structures during phase-change heat transfer.

Real-time manipulation with magnetically tunable structures.

Magnetically tunable micropillar arrays with uniform, continuous and extreme tilt angles for real-time manipulation are reported. We experimentally show uniform tilt angles ranging from 0° to 57°, and develop a model to accurately capture the behavior. Furthermore, we demonstrate that the flexible uniform responsive microstructures (µFUR) can dynamically manipulate liquid spreading directionality, control fluid drag, and tune optical transmittance over a large range.