Extreme Water Uptake of Hygroscopic Hydrogels through Maximized Swelling-Induced Salt Loading.

Hygroscopic hydrogels are emerging as scalable and low-cost sorbents for atmospheric water harvesting, dehumidification, passive cooling, and thermal energy storage. However, devices using these materials still exhibit insufficient performance, partly due to the limited water vapor uptake of the hydrogels. Here, the swelling dynamics of hydrogels in aqueous lithiumchloride solutions, the implications on hydrogel salt loading, and the resulting vapor uptake of the synthesized hydrogel-salt composites are characterized. By tuning the salt concentration of the swelling solutions and the cross-linking properties of the gels, hygroscopic hydrogels with extremely high salt loadings are synthesized, which enable unprecedented water uptakes of 1.79 and 3.86 gg-1 at relative humidity (RH) of 30% and 70%, respectively. At 30% RH, this exceeds previously reported water uptakes of metal-organic frameworks by over 100% and of hydrogels by 15%, bringing the uptake within 93% of the fundamental limit of hygroscopic salts while avoiding leakage problems common in salt solutions. By modeling the salt-vapor equilibria, the maximum leakage-free RH is elucidated as a function of hydrogel uptake and swelling ratio. These insights guide the design of hydrogels with exceptional hygroscopicity that enable sorption-based devices to tackle water scarcity and the global energy crisis.

Unusual Temperature Dependence of Water Sorption in Semicrystalline Hydrogels.

Water vapor sorption is a ubiquitous phenomenon in nature and plays an important role in various applications, including humidity regulation, energy storage, thermal management, and water harvesting. In particular, capturing moisture at elevated temperatures is highly desirable to prevent dehydration and to enlarge the tunability of water uptake. However, owing to the thermodynamic limit of conventional materials, sorbents inevitably tend to capture less water vapor at higher temperatures, impeding their broad applications. Here, an inverse temperature dependence of water sorption in poly(ethylene glycol) (PEG) hydrogels, where their water uptake can be doubled with increasing temperature from 25 to 50 °C, is reported. With mechanistic modeling of water-polymer interactions, this unusual water sorption is attributed to the first-order phase transformation of PEG structures, and the key parameters for a more generalized strategy in materials development are identified. This work elucidates a new regime of water sorption with an unusual temperature dependence, enabling a promising engineering space for harnessing moisture and heat.

Capillary Transfer of Self-Assembled Colloidal Crystals.

Colloidal self-assembly has attracted significant interest in numerous applications including optics, electrochemistry, thermofluidics, and biomolecule templating. To meet the requirements of these applications, numerous fabrication methods have been developed. However, these are limited to narrow ranges of feature sizes, are incompatible with many substrates, and/or have low scalability, significantly limiting the use of colloidal self-assembly. In this work, we study the capillary transfer of colloidal crystals and demonstrate that this approach overcomes these limitations. Enabled by capillary transfer, we fabricate 2D colloidal crystals with nano-to-micro feature sizes spanning 2 orders of magnitude and on typically challenging substrates including those that are hydrophobic, rough, curved, or structured with microchannels. We developed and systemically validated a capillary peeling model, elucidating the underlying transfer physics. Due to its high versatility, good quality, and simplicity, this approach can expand the possibilities of colloidal self-assembly and enhance the performance of applications using colloidal crystals.

A unified approach and descriptor for the thermal expansion of two-dimensional transition metal dichalcogenide monolayers.

Two-dimensional (2D) materials have enabled promising applications in modern miniaturized devices. However, device operation may lead to substantial temperature rise and thermal stress, resulting in device failure. To address such thermal challenges, the thermal expansion coefficient (TEC) needs to be well understood. Here, we characterize the in-plane TECs of transition metal dichalcogenide (TMD) monolayers and demonstrate superior accuracy using a three-substrate approach. Our measurements confirm the physical range of 2D monolayer TECs and, hence, address the more than two orders of magnitude discrepancy in literature. Moreover, we identify the thermochemical electronegativity difference of compositional elements as a descriptor, enabling the fast estimation of TECs for various TMD monolayers. Our work presents a unified approach and descriptor for the thermal expansion of TMD monolayers, which can serve as a guideline toward the rational design of reliable 2D devices.

Three-Tier Hierarchical Structures for Extreme Pool Boiling Heat Transfer Performance.

Boiling is an effective energy-transfer process with substantial utility in energy applications. Boiling performance is described mainly by the heat-transfer coefficient (HTC) and critical heat flux (CHF). Recent efforts for the simultaneous enhancement of HTC and CHF have been limited by an intrinsic trade-off between them-HTC enhancement requires high nucleation-site density, which can increase bubble coalescence resulting in limited CHF enhancement. In this work, this trade-off is overcome by designing three-tier hierarchical structures. The bubble coalescence is minimized to enhance the CHF by defining nucleation sites with microcavities interspersed within hemi-wicking structures. Meanwhile, the reduced nucleation-site density is compensated for by incorporating nanostructures that promote evaporation for HTC enhancement. The hierarchical structures demonstrate the simultaneous enhancement of HTC and CHF up to 389% and 138%, respectively, compared to a smooth surface. This extreme boiling performance can lead to significant energy savings in a variety of boiling applications.

Thermophotovoltaic efficiency of 40.

Thermophotovoltaics (TPVs) convert predominantly infrared wavelength light to electricity via the photovoltaic effect, and can enable approaches to energy storage1,2 and conversion3-9 that use higher temperature heat sources than the turbines that are ubiquitous in electricity production today. Since the first demonstration of 29% efficient TPVs (Fig. 1a) using an integrated back surface reflector and a tungsten emitter at 2,000 °C (ref. 10), TPV fabrication and performance have improved11,12. However, despite predictions that TPV efficiencies can exceed 50% (refs. 11,13,14), the demonstrated efficiencies are still only as high as 32%, albeit at much lower temperatures below 1,300 °C (refs. 13-15). Here we report the fabrication and measurement of TPV cells with efficiencies of more than 40% and experimentally demonstrate the efficiency of high-bandgap tandem TPV cells. The TPV cells are two-junction devices comprising III-V materials with bandgaps between 1.0 and 1.4 eV that are optimized for emitter temperatures of 1,900-2,400 °C. The cells exploit the concept of band-edge spectral filtering to obtain high efficiency, using highly reflective back surface reflectors to reject unusable sub-bandgap radiation back to the emitter. A 1.4/1.2 eV device reached a maximum efficiency of (41.1 ± 1)% operating at a power density of 2.39 W cm-2 and an emitter temperature of 2,400 °C. A 1.2/1.0 eV device reached a maximum efficiency of (39.3 ± 1)% operating at a power density of 1.8 W cm-2 and an emitter temperature of 2,127 °C. These cells can be integrated into a TPV system for thermal energy grid storage to enable dispatchable renewable energy. This creates a pathway for thermal energy grid storage to reach sufficiently high efficiency and sufficiently low cost to enable decarbonization of the electricity grid.

How Coalescing Bubbles Depart from a Wall.

Bubble evolution plays a fundamental role in boiling and gas-evolving electrochemical systems. One key stage is bubble departure, which is traditionally considered to be buoyancy-driven. However, conventional understanding cannot provide the full physical picture, especially for departure events with small bubble sizes commonly observed in water splitting and high heat flux boiling experiments. Here, we report a new regime of bubble departure owing to the coalescence of two bubbles, where the departure diameter can be much smaller than the conventional buoyancy limit. We show the significant reduction of the bubble base area due to the dynamics of the three-phase contact line during coalescence, which promotes bubble departure. More importantly, combining buoyancy-driven and coalescence-induced bubble departure modes, we demonstrate a unified relationship between the departure diameter and nucleation site density. By elucidating how coalescing bubbles depart from a wall, our work provides design guidelines for energy systems which can largely benefit from efficient bubble departure.

Enhancement of Boiling with Scalable Sandblasted Surfaces.

Surface engineering has been leveraged by researchers to enhance boiling heat transfer performance, with benefits ranging from improved thermal management to more efficient power generation. While engineered surfaces fabricated using cleanroom processes have shown promising boiling results, scalable methods for surface engineering are still limited despite most real-world industry-scale applications involving large boiling areas. In this work, we investigate the use of sandblasting as a scalable surface engineering technique for the enhancement of pool boiling heat transfer. We vary the size of an abrasive Al2O3 sandblasting medium (25, 50, 100, and 150 µm) and quantify its effects on silicon surface conditions and boiling characteristics. The surface morphology and capillary wicking performance are characterized by optical profilometry and capillary rise tests, respectively. Pool boiling results and surface characterization reveal that surface roughness and volumetric wicking rate increase with the abrasive size, which results in improvements in the critical heat flux and the heat transfer coefficient of up to 192.6 and 434.3% compared to a smooth silicon surface, respectively. The significant enhancement achieved with sandblasted surfaces indicates that sandblasting is a promising option for improving boiling performance in industry-scale applications.

Highly efficient and salt rejecting solar evaporation via a wick-free confined water layer.

Recent advances in thermally localized solar evaporation hold significant promise for vapor generation, seawater desalination, wastewater treatment, and medical sterilization. However, salt accumulation is one of the key bottlenecks for reliable adoption. Here, we demonstrate highly efficient (>80% solar-to-vapor conversion efficiency) and salt rejecting (20 weight % salinity) solar evaporation by engineering the fluidic flow in a wick-free confined water layer. With mechanistic modeling and experimental characterization of salt transport, we show that natural convection can be triggered in the confined water. More notably, there exists a regime enabling simultaneous thermal localization and salt rejection, i.e., natural convection significantly accelerates salt rejection while inducing negligible additional heat loss. Furthermore, we show the broad applicability by integrating this confined water layer with a recently developed contactless solar evaporator and report an improved efficiency. This work elucidates the fundamentals of salt transport and offers a low-cost strategy for high-performance solar evaporation.

Kinetics of Sorption in Hygroscopic Hydrogels.

Hygroscopic hydrogels hold significant promise for high-performance atmospheric water harvesting, passive cooling, and thermal management. However, a mechanistic understanding of the sorption kinetics of hygroscopic hydrogels remains elusive, impeding an optimized design and broad adoption. Here, we develop a generalized two-concentration model (TCM) to describe the sorption kinetics of hygroscopic hydrogels, where vapor transport in hydrogel micropores and liquid transport in polymer nanopores are coupled through the sorption at the interface. We show that the liquid transport due to the chemical potential gradient in the hydrogel plays an important role in the fast kinetics. The high water uptake is attributed to the expansion of hydrogel during liquid transport. Moreover, we identify key design parameters governing the kinetics, including the initial porosity, hydrogel thickness, and shear modulus. This work provides a generic framework of sorption kinetics, which bridges the knowledge gap between the fundamental transport and practical design of hygroscopic hydrogels.

Turning traditionally nonwetting surfaces wetting for even ultra-high surface energy liquids.

We present a surface-engineering approach that turns all liquids highly wetting, including ultra-high surface tension fluids such as mercury. Previously, highly wetting behavior was only possible for intrinsically wetting liquid/material combinations through surface roughening to enable the so-called Wenzel and hemiwicking states, in which liquid fills the surface structures and causes a droplet to exhibit a low contact angle when contacting the surface. Here, we show that roughness made of reentrant structures allows for a metastable hemiwicking state even for nonwetting liquids. Our surface energy model reveals that with liquid filled in the structure, the reentrant feature creates a local energy barrier, which prevents liquid depletion from surface structures regardless of the intrinsic wettability. We experimentally demonstrated this concept with microfabricated reentrant channels. Notably, we show an apparent contact angle as low as 35° for mercury on structured silicon surfaces with fluorinated coatings, on which the intrinsic contact angle of mercury is 143°, turning a highly nonwetting liquid/material combination highly wetting through surface engineering. Our work enables highly wetting behavior for previously inaccessible material/liquid combinations and thus expands the design space for various thermofluidic applications.

Temporal Evolution of Surface Contamination under Ultra-high Vacuum.

Ultra-high vacuum (UHV) is essential to many surface characterization techniques and is often applied with the intention of reducing exposure to airborne contaminants. Surface contamination under UHV is not well-understood, however, and introduces uncertainty in surface elemental characterization or hinders surface-sensitive manufacturing approaches. In this work, we investigated the time-dependent surface composition of gold samples with different initial levels of contamination under UHV over a period of 24 h with both experiments and physical modeling. Our results show that surface hydrocarbon concentration under UHV can be explained by molecular adsorption-desorption competition theory. Gold surfaces that were initially pristine adsorbed hydrocarbons over time under UHV; conversely, surfaces that were initially heavily contaminated desorbed hydrocarbons over time. During both adsorption and desorption, the concentration of contaminants tended toward the same equilibrium value. This study provides a comprehensive evaluation of the temporal evolution of surface contamination under UHV and highlights routes to mitigate surface contamination effects.

Rational Fabrication of Nano-to-Microsphere Polycrystalline Opals Using Slope Self-Assembly.

Self-assembly of artificial opals has garnered significant interest as a facile nanofabrication technique capable of producing highly ordered structures for optical, electrochemical, biomolecular, and thermal applications. In these applications, the optimum opal particle diameter can vary by several orders of magnitude because the properties of the resultant structures depend strongly on the feature size. However, current opal fabrication techniques only produce high-quality structures over a limited range of sphere sizes or require complex processes and equipment. In this work, the rational and simple fabrication of polycrystalline opals with diameters between 500 nm and 10 µm was demonstrated using slope self-assembly of colloids suspended in ethanol-water. The role of the various process parameters was elucidated through a scaling-based model that accurately captures the variations of opal substrate coverage for spheres of size 2 µm or smaller. For spheres of 10 µm and larger, capillary forces were shown to play a key role in the process dynamics. Based on these insights, millimeter-scale monolayered opals were successfully fabricated, while centimeter-scale opals were possible with sparse sphere stacking or small uncovered areas. These insights provide a guide for the simple and fast fabrication of opals that can be used as optical coatings, templates for high power density electrodes, molecule templates, and high-performance thermo-fluidic devices.

Toward Optimal Heat Transfer of 2D-3D Heterostructures via van der Waals Binding Effects.

Two-dimensional (2D) materials and their heterogeneous integration have enabled promising electronic and photonic applications. However, significant thermal challenges arise due to numerous van der Waals (vdW) interfaces limiting the dissipation of heat generated in the device. In this work, we investigate the vdW binding effect on heat transport through a MoS2-amorphous silica heterostructure. We show using atomistic simulations that the cross-plane thermal conductance starts to saturate with the increase of vdW binding energy, which is attributed to substrate-induced localized phonons. With these atomistic insights, we perform device-level heat transfer optimizations. Accordingly, we identify a regime, characterized by the coupling of in-plane and cross-plane heat transport mediated by vdW binding energy, where maximal heat dissipation in the device is achieved. These results elucidate fundamental heat transport through the vdW heterostructure and provide a pathway toward optimizing thermal management in 2D nanoscale devices.

Bottom-Up Synthesized All-Thermal-Catalyst Aerogels for Heat-Regenerative Air Filtration.

Airborne particular matter (PM) pollution is an increasing global issue and alternative sources of filter fibers are now an area of significant focus. Compared with relatively mature hazardous gas treatments, state of the art high-efficiency PM filters still lack thermal decomposition ability for organic PM pollutants, such as soot from coal-fired power plants and waste-combustion incinerators, resulting in frequent replacement, high cost, and second-hand pollution. In this manuscript, we propose a bottom-up synthesis method to make the first all-thermal-catalyst air filter (ATCAF). Self-assembled from ∼50 nm diameter TiO2 fibers, ATCAF could not only capture the combustion-generated PM pollutants with >99.999% efficiency but also catalyze the complete decomposition of the as-captured hydrocarbon pollutants at high temperature. It has the potential of in situ eliminating the PM pollutants from burning of hydrocarbon materials leveraging the burning heat.

Solar-Driven Soft Robots.

Stimuli-responsive materials have been lately employed in soft robotics enabling new classes of robots that can emulate biological systems. The untethered operation of soft materials with high power light, magnetic field, and electric field has been previously demonstrated. While electric and magnetic fields can be stimulants for untethered actuation, their rapid decay as a function of distance limits their efficacy for long-range operations. In contrast, light-in the form of sunlight or collimated from an artificial source (e.g., laser, Xenon lamps)-does not decay rapidly, making it suitable for long-range excitation of untethered soft robots. In this work, an approach to harnessing sunlight for the untethered operation of soft robots is presented. By employing a selective solar absorber film and a low-boiling point (34 °C) fluid, light-operated soft robotic grippers are demonstrated, grasping and lifting objects almost 25 times the mass of the fluid in a controllable fashion. The method addresses one of the salient challenges in the field of untethered soft robotics. It precludes the use of bulky peripheral components (e.g., compressors, valves, or pressurized gas tank) and enables the untethered long-range operation of soft robots.

Microtube Surfaces for the Simultaneous Enhancement of Efficiency and Critical Heat Flux during Pool Boiling.

Boiling is an essential process in numerous applications including power plants, thermal management, water purification, and steam generation. Previous studies have shown that surfaces with microcavities or biphilic wettability can enhance the efficiency of boiling heat transfer, that is, the heat transfer coefficient (HTC). Surfaces with permeable structures such as micropillar arrays, in contrast, have shown significant enhancement of the critical heat flux (CHF). In this work, we investigated microtube structures, where a cavity is defined at the center of a pillar, as structural building blocks to enhance HTC and CHF simultaneously in a controllable manner. We demonstrated simultaneous CHF and HTC enhancements of up to 62 and 244%, respectively, compared to those of a smooth surface. The experimental data along with high-speed images elucidate the mechanism for simultaneous enhancement where bubble nucleation occurs in the microtube cavities for increased HTC and microlayer evaporation occurs around microtube sidewalls for increased CHF. Furthermore, we combined micropillars and microtubes to create surfaces that further increased CHF by achieving a path to separate nucleating bubbles and rewetting liquids. This work provides guidelines for the systematic surface design for boiling heat transfer enhancement and has important implications for understanding boiling heat transfer mechanisms.

Transport-Based Modeling of Bubble Nucleation on Gas Evolving Electrodes.

Bubble nucleation is ubiquitous in gas evolving reactions that are instrumental for a variety of electrochemical systems. Fundamental understanding of the nucleation process, which is critical to system optimization, remains limited as prior works generally focused on the thermodynamics and have not considered the coupling between surface geometries and different forms of transport in the electrolytes. Here, we establish a comprehensive transport-based model framework to identify the underlying mechanism for bubble nucleation on gas evolving electrodes. We account for the complex effects on the electrical field, ion migration, ion diffusion, and gas diffusion arising from surface heterogeneities and gas pockets initiated from surface crevices. As a result, we show that neglecting these effects leads to significant underprediction of the energy needed for nucleation. Our model provides a non-monotonic relationship between the surface cavity size and the overpotential required for nucleation, which is physically more consistent than the monotonic relationship suggested by a traditional thermodynamics-based model. We also identify the significance of the gas diffuse layer thickness, a parameter controlled by external flow fields and overall electrode geometries, which has been largely overlooked in previous models. Our model framework offers guidelines for practical electrochemical systems whereby, without changing the surface chemistry, nucleation on electrodes can be tuned by engineering the cavity size and the gas diffuse layer thickness.

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.

Quasi-Newtonian Environmental Scanning Electron Microscopy (QN-ESEM) for Monitoring Material Dynamics in High-Pressure Gaseous Environments.

Environmental scanning electron microscopy (ESEM) is a powerful technique that enables imaging of diverse specimens (e.g., biomaterials, chemical materials, nanomaterials) in a hydrated or native state while simultaneously maintaining micro-to-nanoscale resolution. However, it is difficult to achieve high signal-to-noise and artifact-free secondary electron images in a high-pressure gaseous environment due to the intensive electron-gas collisions. In addition, nanotextured substrates can mask the signal from a weakly scattering sample. These drawbacks limit the study of material dynamics under extreme conditions and correspondingly our understanding in many fields. In this work, an imaging framework called Quasi-Newtonian ESEM is proposed, which introduces the concepts of quasi-force and quasi-work by referencing the scattering force in light-matter interactions, to break these barriers without any hardware changes. It is shown that quasi-force is a more fundamental quantity that has a more significant connection with the sample morphology than intensity in the strongly scattering regime. Experimental and theoretical studies on the dynamics of droplet condensation in a high-pressure environment (up to 2500 Pa) successfully demonstrate the effectiveness and robustness of the framework and that the overwhelmed signal of interest in ESEM images can be reconstructed through information stored in the time domain, i.e., frames captured at different moments.