Sustainable Thermal Regulation of Electronics via Mitigated Supercooling of Porous Gallium-Based Phase Change Materials.

Gallium liquid metal is one of the promising phase change materials for passive thermal management of electronics due to their high thermal conductivity and latent heat per volume. However, it suffers from severe supercooling, in which molten gallium does not return to solid due to the lack of nucleation. It may require 28.2 °C lower temperature than the original freezing point to address supercooling, leading to unstable thermal regulation performance along fluctuations of cooling condition. Here, gallium is infused into porous copper in an oxide-free environment, forming intermetallic compound impurities at the interfaces to reduce the activation energy for heterogeneous nucleation. The porous-shaped gallium provides ≈63% smaller supercooling than that of the bulk type due to large specific surface area (≈9,070 cm2 per cm3) and high wetting characteristics (≈16° of contact angle) on CuGa2 intermetallic layer. During repetitive heating-cooling cycles, porous-shaped gallium consistently shows propagation of crystallization at even near room temperature (≈25 °C) while maintaining stable performance as thermal buffer, whereas droplet-shaped gallium is gradually degraded due to partial-supercooled state. The findings will improve the responsive thermal regulation performance to relieve a rapid increase in temperature of semiconductors/batteries, and also have a potential for energy storage applications.

Investigating the Vapor-Phase Adsorption of Aroma Molecules on the Water-Vapor Interface using Molecular Dynamics Simulations.

Surfactants are amphiphilic additives primarily used to reduce the surface tension of water and manipulate its wettability on various surfaces. Recent reports suggest that volatile surfactants, such as aroma molecules, diffuse more quickly to the interface from the vapor-phase than conventional surfactants typically used in the aqueous phase. The ability to adsorb from the vapor phase, in addition to their use as cosurfactants, expands the potential applications of volatile surfactants, particularly in situations where adding surfactants from the liquid phase is difficult. Here, we present a molecular level understanding of the adsorption kinetics of linalool, a common aroma molecule, on the water interface using molecular dynamics simulations. We note that the value of surface tension while adsorption from vapor and liquid phases is dependent only on the surface coverage. A minimum surface tension of 32 ± 1.8 mN/m is obtained in both cases at a maximum surface coverage of 4.88 µmol/m2 at 300 K. We observe the extent of decrease of the H-bonds between linalool-water and linalool-linalool molecules at various surface coverages to explain the mechanism of surface tension reduction. We solve Gibb's adsorption equation to establish a correlation between the surface coverage of linalool and the corresponding bulk concentration in experiments. We investigate the free energy profile of linalool's adsorption behavior at different surface coverages and temperatures. Our report suggests that linalool adsorption onto the water interface is an enthalpy-driven process primarily dependent on the strength of the interaction between the hydroxyl group of linalool and water molecules. These insights are crucial for selecting a suitable aroma molecule for various applications that target the vapor-phase adsorption mechanism.

Nanomechanical Sensing Using Heater-Integrated Fluidic Resonators.

Micro/nanochannel resonators have been used to measure cells, suspended nanoparticles, or liquids, primarily at or near room temperature while their high temperature operation can offer promising applications such as calorimetric measurements and thermogravimetric analysis. To date, global electrothermal or local photothermal heating mechanisms have been attempted for channel resonators, but both approaches are intrinsically limited by a narrow temperature modulation range, slow heating/cooling, less quantitative heating, or time-consuming optical alignment. Here, we introduce heater-integrated fluidic resonators (HFRs) that enable fast, quantitative, alignment-free, and wide-range temperature modulation and simultaneously offer resistive thermometry and resonant densitometry. HFRs with or without a dispensing nozzle are fabricated, thoroughly characterized, and used for high throughput thermophysical properties measurements, microchannel boiling studies, and atomized spray dispensing. The HFR, without a doubt, opens a new avenue for nanoscale thermal analysis and processing and further encourages the integration of additional functions into channel resonators.

A Scalable Haze-Free Antireflective Hierarchical Surface with Self-Cleaning Capability.

The lotus effect indicates that a superhydrophobic, self-cleaning surface can be obtained by roughening the topography of a hydrophobic surface. However, attaining high transmittance and clarity through a roughened surface remains challenging because of its strong scattering characteristics. Here, a haze-free, antireflective superhydrophobic surface that consists of hierarchically designed nanoparticles is demonstrated. Close-packed, deep-subwavelength-scale colloidal silica nanoparticles and their upper, chain-like fumed silica nanoparticles individually fulfill haze-free broadband antireflection and self-cleaning functions. These double-layered hierarchical surfaces are obtained via a scalable spraying process that permits precise control over the coating morphology to attain the desired optical and wetting properties. They provide a "specular" visible transmittance of >97% when double-side coated and a record-high self-cleaning capability with a near-zero sliding angle. Self-cleaning experiments on photovoltaic devices verify that the developed surfaces can significantly enhance power conversion efficiencies and aid in retaining pristine device performance in a dusty environment.

Spherical Micro/Nano Hierarchical Structures for Energy and Water Harvesting Devices.

Three-dimensional (3D) hierarchical structures have been explored for various applications owing to the synergistic effects of micro- and nanostructures. However, the development of spherical micro/nano hierarchical structures (S-HSs), which can be used as energy/water harvesting systems and sensing devices, remains challenging owing to the trade-off between structural complexity and fabrication difficulty. This paper presents a new strategy for facile, scalable S-HS fabrication using a thermal expansion of microspheres and nanopatterned structures. When a specific temperature is applied to a composite film of microspheres and elastomers with nanopatterned surfaces, microspheres are expanded and 3D spherical microstructures are generated. Various nanopatterns and densities of spherical microstructures can thereby be quantitatively controlled. The fabricated S-HSs have been used in renewable electrical energy harvesting and sustainable water management applications. Compared to a triboelectric nanogenerator (TENG) with bare film, the S-HS-based TENG exhibited 4.48 times higher triboelectric performance with high mechanical durability. Furthermore, an S-HS is used as a water harvesting device to capture water in a fog environment. The water collection rate is dramatically enhanced by the increased surface area and locally concentrated vapor diffusion flux due to the spherical microstructures.

High-Temperature Carbonized Ceria Thermophotovoltaic Emitter beyond Tungsten.

Thermophotovoltaics (TPVs) require emitters with a regulated radiation spectrum tailored to the spectral response of integrated photovoltaic cells. Such spectrally engineered emitters developed thus far are structurally too complicated to be scalable, are thermally unstable, or lack reliability in terms of temperature cycling. Herein, we report wafer-scale, thermal-stress-free, and wavelength-selective emitters that operate for high-temperature TPVs equipped with GaSb photovoltaic cells. One inch crystalline ceria wafers were prepared by sequentially pressing and annealing the pellets of ceria nanoparticles. The direct pyrolysis of citric acid mixed with ceria nanoparticles created agglomerated, pyrolytic carbon and ceria microscale dots, thus forming a carbonized film strongly adhering to a wafer surface. Depending on the thickness of the carbonized film that was readily tuned based on the amount of citric acid used in the reaction, the carbonized ceria emitter behaved as a tungsten-like emitter, a graphite-like emitter, or their hybrid in terms of the absorptivity spectrum. A properly synthesized carbonized ceria emitter produced a power density of 0.63 W/cm2 from the TPV system working at 900 °C, providing 13 and 9% enhancements compared to tungsten and graphite emitters, respectively. Furthermore, only the carbonized ceria emitter preserved its pristine absorptivity spectrum after a 48 h heating test at 1000 °C. The scalable and facile fabrication of thermostable emitters with a structured spectrum will prompt the emergence of thermal emission-harnessed energy devices.

Endowing antifouling properties on metal substrata by creating an artificial barrier layer based on scalable metal oxide nanostructures.

Here, by creating different types of artificial barrier layer against bacterial attachment, anti-biofouling properties were endowed on three metallic surfaces - aluminum, stainless steel and titanium. To each metallic surface, a tailored chemical oxidation process was applied to grow scalable oxide structures with an additional appropriate coating, resulting in three different types of anti-biofouling barrier, a thin water film, an air layer and an oil layer. Fluorescence images of the attached bacteria showed that the water layer improved the anti-biofouling performance up to 8-12 h and the air layer up to 12-24 h, comparable with the lifetime of the air layer. In comparison, the oil layer exhibited the best anti-biofouling performance by suppressing the fouled area by < 10% up to 72 h regardless of the substratum type. The present work provides simple, low-cost, scalable strategies to enhance the anti-biofouling performance of industrially important metallic surfaces. [Formula: see text].

Water penetration dynamics through a Janus mesh during drop impact.

Here, we study the water penetration dynamics through a Janus membrane with opposite wettability, i.e., (super-) hydrophobic on one side and (super-) hydrophilic on the other side, during drop impact. It is demonstrated that the penetration dynamics through the membrane consists of two temporally distinct events: dynamic pressure driven penetration dynamics on a shorter timescale and capillary pressure driven penetration dynamics on a longer timescale. For penetration under dynamic pressure, the threshold velocity for the penetration is dependent on the wettability of the impact side, such that a smaller impact velocity is required for water penetration when a water drop is impinged onto the superhydrophobic side over the superhydrophilic side. We demonstrate that this difference in the penetration dynamics upon drop impact can still be accounted for by the balance between the dynamic pressure and the capillarity pressure after adjusting the relative magnitude of the two contrasting pressures required for the penetration. Meanwhile, it is demonstrated that the penetration dynamics under capillary pressure is governed by the balance between the capillary pressure and the viscous pressure while the penetration mainly proceeds through the penetration area, which is formed during short-time penetration, showing the dynamic coupling between the two penetration dynamics. By elucidating the penetration dynamics on a Janus membrane, we believe that our results can help in designing Janus membranes for various fluidic applications such as oil-water separation, aeration, and water harvesting.

Contact time on curved superhydrophobic surfaces.

When a water drop impinges on a flat superhydrophobic surface, it bounces off the surface after a certain dwelling time, which is determined by the Rayleigh inertial-capillary timescale. Recent works have demonstrated that this dwelling time (i.e., contact time) is modified on curved superhydrophobic surfaces, as the drop asymmetrically spreads over the surface. However, the contact time on the curved surfaces still remains poorly understood, while no successful physical model for the contact time has been proposed. Here, we propose that the asymmetric spreading on the curved surface is driven by either the Coanda effect or inertia depending on the ratio of the drop diameter to the curvature diameter. Then, based on scaling analysis, we develop the contact time model that successfully predicts the contact time measured under a wide range of experiment conditions such as different impact velocities and curvature diameters. We believe that our results illuminate the underlying mechanism for the asymmetric spreading over the curved surface, while the proposed contact time model can be utilized for the design of superhydrophobic surfaces for various thermal applications, where the thermal exchange between the surface and the water drop occurs via a direct physical contact.

Brushed lubricant-impregnated surfaces (BLIS) for long-lasting high condensation heat transfer.

Recently, lubricant-impregnated surfaces (LIS) have emerged as a promising condenser surface by facilitating the removal of condensates from the surface. However, LIS has the critical limitation in that lubricant oil is depleted along with the removal of condensates. Such oil depletion is significantly aggravated under high condensation heat transfer. Here we propose a brushed LIS (BLIS) that can allow the application of LIS under high condensation heat transfer indefinitely by overcoming the previous oil depletion limit. In BLIS, a brush replenishes the depleted oil via physical contact with the rotational tube, while oil is continuously supplied to the brush by capillarity. In addition, BLIS helps enhance heat transfer performance with additional route to droplet removal by brush sweeping. By applying BLIS, we maintain the stable dropwise condensation mode for > 48 hours under high supersaturation levels along with up to 61% heat transfer enhancement compared to hydrophobic surfaces.

Passive Anti-Flooding Superhydrophobic Surfaces.

Superhydrophobic (SHPo) surfaces can provide high condensation heat transfer due to facilitated droplet removal. However, such high performance has been limited to low supersaturation conditions due to surface flooding. Here, we quantify flooding resistance defined as the rate of increase in the fraction of water-filled cavities with respect to the supersaturation level. Based on the quantitative understanding of surface flooding, we suggest effective anti-flooding strategies through tailoring the nanoscale coating heterogeneity and structure length scale. Experimental verification is conducted using CuO nanostructures having different length scales combined with hydrophobic coatings with different nanoscale heterogeneities. The proposed anti-flooding SHPo can provide a ∼130% enhanced average heat transfer coefficient with ∼14% larger supersaturation range for droplet jumping compared to a previous CuO SHPo. The proposed anti-flooding parameter and the scalable SHPo will help develop high-performance condensers for real-world applications operating in a wide range of supersaturation levels.

Optical Tunneling Mediated Sub-Skin-Depth High Emissivity Tungsten Radiators.

Tailoring the spectrum of thermal radiation at high temperatures is a central issue in the study of thermal radiation harnessed energy resources. Although bulk metals with periodic cavities incorporated into their surfaces provide high emissivity, they require a complicated micron metal etch, thereby precluding reliable, continuous operation. Here, we report thermally stable, highly emissive, ultrathin (<20 nm) tungsten (W) radiators that were prepared in a scalable and cost-effective route. Alumina/W/alumina multiwalled, submicron cavity arrays were fabricated sequentially using nanoimprinting lithography, thin film deposition, and calcination processes. To highlight the practical importance of high-temperature radiators, we developed a thermophotovoltaic (TPV) system equipped with fabricated W radiators and low-bandgap GaSb photovoltaic cells. The TPV system produced electric power reliably during repeated temperature cycling between 500 and 1200 K; the power density at 1200 K was fixed to be approximately 1.0 W/cm2. The temperature-dependent electric power was quantitatively reproduced using a one-dimensional energy conversion model. The symmetric configuration of alumina/W/alumina multiwall together with the presence of a void inside each cavity alleviated thermal stress, which was responsible for the stable TPV performance. The short-current-density (JSC) of developed TPV system was augmented significantly by decreasing the W thickness below its skin depth. A 17 nm thick W radiator yielded a 32% enhancement in JSC compared to a 123 nm thick W radiator. Electromagnetic analysis indicated that subskin-depth W cavity arrays led to suppressed surface reflection due to the mitigated screening effect of free electrons, thereby enhancing the absorption of light within each W wall. Such optical tunneling-mediated absorption or radiation was valid for any metal material and morphology (e.g., planar or patterned).

Continuous scavenging of broadband vibrations via omnipotent tandem triboelectric nanogenerators with cascade impact structure.

Ambient vibration energy is highly irregular in force and frequency. Triboelectric nanogenerators (TENG) can convert ambient mechanical energy into useable electricity. In order to effectively convert irregular ambient vibrations into electricity, the TENG should be capable of reliably continuous operation despite variability in input forces and frequencies. In this study, we propose a tandem triboelectric nanogenerator with cascade impact structure (CIT-TENG) for continuously scavenging input vibrations with broadband frequencies. Based on resonance theory, four TENGs were explicitly designed to operate in tandem and cover a targeted frequency range of 0-40 Hz. However, due to the cascade impact structure of CIT-TENG, each TENG could produce output even under non-resonant conditions. We systematically studied the cascade impact dynamics of the CIT-TENG using finite element simulations and experiments to show how it enables continuous scavenging from 0-40 Hz even under low input accelerations of 0.2 G-0.5 G m/s2. Finally, we demonstrated that the CIT-TENG could not only scavenge broadband vibrations from a single source such as a car dashboard, but it could also scavenge very low frequency vibrations from water waves and very high frequency vibrations from air compressor machines. Thus, we showed that the CIT-TENG can be used in multiple applications without any need for redesign validating its use as an omnipotent vibration energy scavenger.

Performance Analysis of Gravity-Driven Oil-Water Separation Using Membranes with Special Wettability.

A membrane with selective wettability to either oil or water has been utilized for highly efficient, environmentally friendly membrane-based oil-water separation. However, a predictive model, which can be used to evaluate the overall separation performance of the membrane, still needs further development. Herein, we investigate three separation performance parameters, that is, separation efficiency, liquid intrusion pressure, and mass flux in particular, as a function of pore geometry and liquid properties using metallic meshes whose surface wettability is modified by scalable spray coating. We show that the prepared membrane exhibits a separation efficiency over 98% below the intrusion pressure, while the intrusion pressure increases with the decrease of pore size of the membrane. Particularly, we develop a semi-empirical model for the mass flux through the membrane. As application examples of our performance analysis, we successfully predict the separation time for one-way and two-way gravity-driven separation of the oil-water mixture, the decrease of the mass flux due to membrane fouling, and the maximum allowable separation capacity of the given membrane. This work can help to design optimal membrane-based oil-water separation systems for actual industrial applications by providing a selection guideline for separation membranes.

Mesoporous Highly-Deformable Composite Polymer for a Gapless Triboelectric Nanogenerator via a One-Step Metal Oxidation Process.

The oxidation of metal microparticles (MPs) in a polymer film yields a mesoporous highly-deformable composite polymer for enhancing performance and creating a gapless structure of triboelectric nanogenerators (TENGs). This is a one-step scalable synthesis for developing large-scale, cost-effective, and light-weight mesoporous polymer composites. We demonstrate mesoporous aluminum oxide (Al2O3) polydimethylsiloxane (PDMS) composites with a nano-flake structure on the surface of Al2O3 MPs in pores. The porosity of mesoporous Al2O3-PDMS films reaches 71.35% as the concentration of Al MPs increases to 15%. As a result, the film capacitance is enhanced 1.8 times, and TENG output performance is 6.67-times greater at 33.3 kPa and 4 Hz. The pressure sensitivity of 6.71 V/kPa and 0.18 µA/kPa is determined under the pressure range of 5.5⁻33.3 kPa. Based on these structures, we apply mesoporous Al2O3-PDMS film to a gapless TENG structure and obtain a linear pressure sensitivity of 1.00 V/kPa and 0.02 µA/kPa, respectively. Finally, we demonstrate self-powered safety cushion sensors for monitoring human sitting position by using gapless TENGs, which are developed with a large-scale and highly-deformable mesoporous Al2O3-PDMS film with dimensions of 6 × 5 pixels (33 × 27 cm²).

Condensation Heat-Transfer Performance of Thermally Stable Superhydrophobic Cerium-Oxide Surfaces.

We introduce a thin (<200 nm) superhydrophobic cerium-oxide surface formed by a one-step wet chemical process to enhance the condensation heat-transfer performance with improved thermal stability compared to silane-treated surfaces. The developed cerium-oxide surface showed a superhydrophobic characteristic with a low (<5°) contact angle hysteresis because of the unique surface morphology and hydrophobicity of cerium oxide. The surface was successfully incorporated to popular engineering materials including copper, aluminum, and steel. Thermal stability of the surfaces was investigated by exposing them to hot (∼100 °C) steam conditions for 12 h. The introduced ceria surfaces could maintain active dropwise condensation after the thermal stability test, whereas silane-treated surfaces completely lost their hydrophobicity. The heat-transfer coefficient was calculated using the thermal network model incorporating the droplet size distribution and morphology obtained from the microscopic measurement. The analysis shows that the suggested cerium-oxide surfaces can provide approximately 2 times and 5 times higher heat-transfer coefficient before and after the thermal stability test, respectively, mainly because of the decrease in the thermal conduction resistance across droplets. The results indicate that the introduced nanostructured cerium-oxide surface is a promising condenser coating to enhance the droplet mobility and the resulting condensation heat-transfer performance for various thermal and environmental applications, especially those being exposed to hot steam conditions.

Anisotropic drop spreading on superhydrophobic grates during drop impact.

We study the influence of geometric anisotropy of micro-grate structures on the spreading dynamics of water drops after impact. It is found that the maximal spreading diameter along the parallel direction to grates becomes larger than that along the transverse direction beyond a certain Weber number, while the extent of such an asymmetric spreading increases with the structural pitch of grates and Weber number. By employing grates covered with nanostructures, we exclude the possible influences coming from the Cassie-to-Wenzel transition and the circumferential contact angle variation on the spreading diameter. Then, based on a simplified energy balance model incorporating slip length, we propose that slip length selectively enhances the spreading diameter along the parallel direction, being responsible for the asymmetric drop spreading. We believe that our work will help better understand the role of microstructures in controlling the drop dynamics during impact, which has relevance to various engineering applications.

Effect of geometrical parameters on rebound of impacting droplets on leaky superhydrophobic meshes.

When a droplet impacts a superhydrophobic sieve, a part of the droplet penetrates through it when the dynamic pressure (ρU2) of the impinging droplet exceeds the breakthrough pressure (γΓ/A). At higher impact velocities, the ejected-jet breaks and separates from the main droplet. The remaining part of the droplet bounces off the surface showing different modes (normal bouncing as a vertically elongated drop or pancake bouncing). In this work, we have studied the effect of different geometrical parameters of superhydrophobic copper meshes on different modes of droplet rebound. We observe three different effects in our study. Firstly, we observe pancake like bouncing, which is attributed to the capillary energy of the rebounding interface formed after the breaking of the ejected-jet. Secondly, we observe leakage of the droplet volume and kinetic energy due to the breaking of the ejected-jet, which leads to reduction in the contact times. Finally, we observe that for flexible meshes, the transition to pancake type bouncing is induced at lower Weber numbers. Flexibility also leads to a reduction in the volume loss from the ejected-jet. This study will be helpful in the design of superhydrophobic meshes for use under impact scenarios.

Water Penetration through a Superhydrophobic Mesh During a Drop Impact.

When a water drop impacts a mesh having submillimeter pores, a part of the drop penetrates through the mesh if the impact velocity is sufficiently large. Here we show that different surface wettability, i.e., hydrophobicity and superhydrophobicity, leads to different water penetration dynamics on a mesh during drop impact. We show, despite the water repellence of a superhydrophobic surface, that water can penetrate a superhydrophobic mesh more easily (i.e., at a lower impact velocity) over a hydrophobic mesh via a penetration mechanism unique to a superhydrophobic mesh. On a superhydrophobic mesh, the water penetration can occur during the drop recoil stage, which appears at a lower impact velocity than the critical impact velocity for water penetration right upon impact. We propose that this unique water penetration on a superhydrophobic mesh can be attributed to the combination of the hydrodynamic focusing and the momentum transfer from the water drop when it is about to bounce off the surface, at which point the water drop retrieves most of its kinetic energy due to the negligible friction on superhydrophobic surfaces.

The effects of surface wettability on the fog and dew moisture harvesting performance on tubular surfaces.

The efficient water harvesting from air-laden moisture has been a subject of great interest to address world-wide water shortage issues. Recently, it has been shown that tailoring surface wettability can enhance the moisture harvesting performance. However, depending on the harvesting condition, a different conclusion has often been reported and it remains unclear what type of surface wettability would be desirable for the efficient water harvesting under the given condition. Here we compare the water harvesting performance of the surfaces with various wettability under two different harvesting conditions-dewing and fogging, and show that the different harvesting efficiency of each surface under these two conditions can be understood by considering the relative importance of the water capturing and removal efficiency of the surface. At fogging, the moisture harvesting performance is determined by the water removal efficiency of the surface with the oil-infused surfaces exhibiting the best performance. Meanwhile, at dewing, both the water capturing and removal efficiency are crucial to the harvesting performance. And well-wetting surfaces with a lower barrier to nucleation of condensates exhibit a better harvesting performance due to the increasing importance of the water capture efficiency over the water removal efficiency at dewing.