Electric Field-Enhanced Ion Rejection Rate in Freeze Desalination.

Freeze desalination is an appealing method for seawater desalination through freezing seawater. The percentage of ions in the liquid phase, which is termed ion rejection rate, is a critical factor affecting the performance of freeze desalination. Improving the ion rejection rate is an important topic for freeze desalination. In this work, we investigate the effects of electric fields on the ion rejection rate during the freezing of seawater through molecular dynamics simulations.  It is found that the ion rejection rate increases with increasing electric field strength.  The enhanced ion rejection rate is due to the reduction of the energy barrier at the ice-water interface caused by the electric field, which affects the orientation of water molecules and ion-water interactions. However, the electric field hinders the ice growth rate, which affects the productivity of freeze desalination. Nevertheless, the finding in this work offers a new idea to improve the ion rejection rate. Practically, a trade-off needs to be found to optimize the overall performance of freeze desalination.

Mask-inspired moisture-transmitting and durable thermochromic perovskite smart windows.

Thermochromic perovskite smart windows (TPWs) are a cutting-edge energy-efficient window technology. However, like most perovskite-based devices, humidity-related degradation limits their widespread application. Herein, inspired by the structure of medical masks, a unique triple-layer thermochromic perovskite window (MTPW) that enable sufficient water vapor transmission to trigger the thermochromism but effectively repel detrimental water and moisture to extend its lifespan is developed. The MTPW demonstrates superhydrophobicity and maintains a solar modulation ability above 20% during a 45-day aging test, with a decay rate 37 times lower than that of a pristine TPW. It can also immobilize lead ions and significantly reduce lead leakage by 66 times. Furthermore, a significant haze reduction from 90% to 30% is achieved, overcoming the blurriness problem of TPWs. Benefiting from the improved optical performance, extended lifespan, suppressed lead leakage, and facile fabrication, the MTPW pushes forward the wide applications of smart windows in green buildings.

Stepless IR Chromism in Ti3 C2 Tx MXene Tuned by Interlayer Water Molecules.

Real-time control over infrared (IR) radiation of objects is highly desired in a variety of areas such as personal thermal regulation and IR camouflage. This requires the dynamic modulation of IR emissivity in a stepless manner over a wide range (>50%), which remains a daunting challenge. Here, an emissivity modulation phenomenon is reported in stacked 2D Ti3 C2 Tx MXene nanosheets, from 12% to 68% as the intercalation/discharging of water molecules within the interlayers. The intercalation of water molecules dynamically changes the electronic properties and the complex permittivity in IR frequencies of Ti3 C2 Tx . This emissivity modulation is a stepless and reversible process without the assistance of any external energy input. Further, intercalating cellulose nanofibers into the Ti3 C2 Tx interlayers makes this dynamic process highly repeatable. Last, a sweat-responsive adaptive textile that can improve thermal comfort of human body under changes in metabolic rates and environmental conditions is demonstrated, showing great potential of this mechanism in passive on-demand radiation modulation.

Shear-Enhanced Ion Rejection during Seawater Freezing.

Ion rejection during seawater freezing is the basis for freeze desalination. A high ion rejection rate is desired for improving the performance of freeze desalination. In this work, we propose a method to enhance the ion rejection rate through external shear, which is demonstrated through molecular dynamics (MD) simulations and experiments. MD simulations show that the ion rejection rate increases with an increasing shear rate. This is attributed to the disruption of the hydration bonds between ions and water molecules in the hydration shell caused by the shear. Consequently, the mobility of ions is increased, and the energy barrier is reduced at the ice-water interface such that ions have a greater chance of diffusing into the aqueous solution, leading to an enhanced ion rejection rate. The MD results in this work are qualitatively confirmed by experiments and provide insights into the enhancement of the ion rejection rate through external parameters.

Hierarchically structured passive radiative cooling ceramic with high solar reflectivity.

Passive radiative cooling using nanophotonic structures is limited by its high cost and poor compatibility with existing end uses, whereas polymeric photonic alternatives lack weather resistance and effective solar reflection. We developed a cellular ceramic that can achieve highly efficient light scattering and a near-perfect solar reflectivity of 99.6%. These qualities, coupled with high thermal emissivity, allow the ceramic to provide continuous subambient cooling in an outdoor setting with a cooling power of >130 watts per square meter at noon, demonstrating energy-saving potential on a worldwide scale. The color, weather resistance, mechanical robustness, and ability to depress the Leidenfrost effect are key features ensuring the durable and versatile nature of the cooling ceramic, thereby facilitating its commercialization in various applications, particularly building construction.

Ultrasensitive Flexible Thermal Sensor Arrays based on High-Thermopower Ionic Thermoelectric Hydrogel.

Ionic circuits using ions as charge carriers have demonstrated great potential for flexible and bioinspired electronics. The emerging ionic thermoelectric (iTE) materials can generate a potential difference by virtue of selective thermal diffusion of ions, which provide a new route for thermal sensing with the merits of high flexibility, low cost, and high thermopower. Here, ultrasensitive flexible thermal sensor arrays based on an iTE hydrogel consisting of polyquaternium-10 (PQ-10), a cellulose derivative, as the polymer matrix and sodium hydroxide (NaOH) as the ion source are reported. The developed PQ-10/NaOH iTE hydrogel achieves a thermopower of 24.17 mV K-1 , which is among the highest values reported for biopolymer-based iTE materials. The high p-type thermopower can be attributed to thermodiffusion of Na+ ions under a temperature gradient, while the movement of OH- ions is impeded by the strong electrostatic interaction with the positively charged quaternary amine groups of PQ-10. Flexible thermal sensor arrays are developed through patterning the PQ-10/NaOH iTE hydrogel on flexible printed circuit boards, which can perceive spatial thermal signals with high sensitivity. A smart glove integrated with multiple thermal sensor arrays is further demonstrated, which endows a prosthetic hand with thermal sensation for human-machine interaction.

A Highly Transparent Photo-Electro-Thermal Film with Broadband Selectivity for All-Day Anti-/De-Icing.

A photo- and electro-thermal film can convert sunlight and electricity into heat to solve icing problems. Combination of them provides an efficient strategy for all-day anti-/de-icing. However, only opaque surfaces have been reported, due to the mutual exclusiveness between photon absorption and transmission. Herein, a highly transparent and scalable solution-processed photo-electro-thermal film is reported, which exhibits an ultra-broadband selective spectrum to separate the visible light from sunlight and a countertrend suppress of emission in longer wavelength. It absorbs ≈ 85% of invisible sunlight (ultraviolet and near-infrared) for light-heat conversion, meanwhile maintains luminous transmittance > 70%. The reflection of mid-infrared leads to low emissivity (0.41), which further preserves heat on the surface for anti-/de-icing purpose. This ultra-broadband selectivity enables temperature elevation > 40 °C under 1-sun illumination and the mutual support between photo-thermal and electro-thermal effects contributes to > 50% saving of electrical consumption under weak solar exposure (0.4-sun) for maintaining unfrozen surfaces at -35 °C environment. The reverberation from photo-electro-thermal and super-hydrophobic effects illustrates a lubricating removal of grown ice in short time (< 120 s). The self-cleaning ability and the durability under mechanical, electrical, optical, and thermal stresses render the film stable for long-term usage in all-day anti-/de-icing applications.

A UV-Reflective Organic-Inorganic Tandem Structure for Efficient and Durable Daytime Radiative Cooling in Harsh Climates.

Radiative cooling shows great promise in eco-friendly space cooling due to its zero-energy consumption. For subambient cooling in hot humid subtropical/tropical climates, achieving ultrahigh solar reflectance (≥96%), durable ultraviolet (UV) resistance, and surface superhydrophobicity simultaneously is critical, which, however, is challenging for most state-of-the-art scalable polymer-based coolers. Here an organic-inorganic tandem structure is reported to address this challenge, which comprises a bottom high-refractive-index polyethersulfone (PES) cooling layer with bimodal honeycomb pores, an alumina (Al2 O3 ) nanoparticle UV reflecting layer with superhydrophobicity, and a middle UV absorption layer of titanium dioxide (TiO2 ) nanoparticles, thus providing thorough protection from UV and self-cleaning capability together with outstanding cooling performance. The PES-TiO2 -Al2 O3 cooler demonstrates a record-high solar reflectance of over 0.97 and high mid-infrared emissivity of 0.92, which can maintain their optical properties intact even after equivalent 280-day UV exposure despite the UV-sensitivity of PES. This cooler achieves a subambient cooling temperature up to 3 °C at summer noontime and 5 °C at autumn noontime without solar shading or convection cover in a subtropical coastal city, Hong Kong. This tandem structure can be extended to other polymer-based designs, offering a UV-resist but reliable radiative cooling solution in hot humid climates.

A Janus Textile Capable of Radiative Subambient Cooling and Warming for Multi-Scenario Personal Thermal Management.

Textiles with radiative cooling/warming capabilities provide a green and effective solution to personal thermal comfort in different climate scenarios. However, developing multiple-mode textiles for wearing in changing climates with large temperature variation remains a challenge. Here a Janus textile is reported, comprising a polyethersulfone (PES)-Al2 O3 cooling layer optically coupled with a Ti3 C2 Tx warming layer, which can realize sub-ambient radiative cooling, solar warming, and active Joule heating. Owing to the intrinsically high refractive index of PES and the rational design of the fiber topology, the nanocomposite PES textile features a record high solar reflectance of 0.97. Accompanied by an infrared (IR) emittance of 0.91 in the atmospheric window, sub-ambient cooling of 0.5-2.5 °C is achieved near noontime in humid summer under ≈1000 W m-2 solar irradiation in Hong Kong. The simulated skin covered with the textile is ≈10 °C cooler than that with white cotton. The Ti3 C2 Tx layer provides a high solar-thermal efficiency of ≈80% and a Joule heating flux of 66 W m-2 at 2 V and 15 °C due to its excellent spectral selectivity and electrical conductivity. The switchable multiple working modes enable effective and adaptive personal thermal management in changing environments.

Reversible bipolar thermopower of ionic thermoelectric polymer composite for cyclic energy generation.

The giant thermopower of ionic thermoelectric materials has attracted great attention for waste-heat recovery technologies. However, generating cyclic power by ionic thermoelectric modules remains challenging, since the ions cannot travel across the electrode interface. Here, we reported a reversible bipolar thermopower (+20.2 mV K-1 to -10.2 mV K-1) of the same composite by manipulating the interactions of ions and electrodes. Meanwhile, a promising ionic thermoelectric generator was proposed to achieve cyclic power generation under a constant heat course only by switching the external electrodes that can effectively realize the alternating dominated thermodiffusion of cations and anions. It eliminates the necessity to change the thermal contact between material and heat, nor does it require re-establish the temperature differences, which can favor improving the efficiency of the ionic thermoelectrics. Furthermore, the developed micro-thermal sensors demonstrated high sensitivity and responsivity in light detecting, presenting innovative impacts on exploring next-generation ionic thermoelectric devices.

Unlocking the High Capacity Ammonium-Ion Storage in Defective Vanadium Dioxide.

Aqueous ammonium-ion storage has been considered a promising energy storage competitor to meet the requirements of safety, affordability, and sustainability. However, ammonium-ion storage is still in its infancy in the absence of reliable electrode materials. Here, defective VO2 (d-VO) is employed as an anode material for ammonium-ion batteries with a moderate transport pathway and high reversible capacity of ≈200 mAh g-1 . Notably, an anisotropic or anisotropic behavior of structural change of d-VO between c-axis and ab planes depends on the state of charge (SOC). Compared with potassium-ion storage, ammonium-ion storage delivers a higher diffusion coefficient and better electrochemical performance. A full cell is further fabricated by d-VO anode and MnO2 cathode, which delivers a high energy density of 96 Wh kg-1 (based on the mass of VO2 ), and a peak energy density of 3254 W kg-1 . In addition, capacity retention of 70% can be obtained after 10 000 cycles at a current density of 1 A g-1 . What's more, the resultant quasi-solid-state MnO2 //d-VO full cell based on hydrogel electrolyte also delivers high safety and decent electrochemical performance. This work will broaden the potential applications of the ammonium-ion battery for sustainable energy storage.

Experimental Evidence of Superdiffusive Thermal Transport in Si0.4Ge0.6 Thin Films.

Superdiffusive thermal transport represents a unique phenomenon in heat conduction, which is characterized by a size (L) dependence of thermal conductivity (κ) in the form of κ ∝ Lß with a constant ß between 0 and 1. Although superdiffusive thermal transport has been theoretically predicted for SiGe alloys, direct experimental evidence is still lacking. Here, we report on a systematic experimental study of the thickness-dependent thermal conductivity of Si0.4Ge0.6 thin films grown by molecular beam epitaxy. The cross-plane thermal conductivity of Si0.4Ge0.6 thin films spanning a thickness range from 20 to 1120 nm was measured in the temperature range 120-320 K via a differential three-omega method. Results show that the thermal conductivity follows a consistent κ ∝ t0.26 power law with the film thickness (t) at different temperatures, providing direct experimental evidence that alloy-scattering dominated thermal transport in SiGe is superdiffusive.

Uncooled self-powered hemispherical biomimetic pit organ for mid- to long-infrared imaging.

Infrared vision is highly desirable for applications in multifarious fields. Of the few species with this visual capability, snakes have exceptional infrared perception with the assistance of pit organs. Inspired by the pit organ design we present here a hemispherical biomimetic infrared imaging device. The devices use high-density ionic thermoelectric polymer nanowire arrays that serve as the sensing nerve cells. The individual nanowires exhibit notable voltage response to temperature variation in test objects. An infrared sensor array with 625 pixels on the hemispherical substrate is successfully demonstrated with an ultrawide field of view up to 135°. The device can image body temperature objects without a cooling system and external power supply. This work opens up opportunities for the design and fabrication of bioinspired infrared imaging devices based on emerging ionic thermoelectric materials.

Self-Protecting Aqueous Lithium-Ion Batteries.

Capacity degradation and destructive hazards are two major challenges for the operation of lithium-ion batteries at high temperatures. Although adding flame retardants or fire extinguishing agents can provide one-off self-protection in case of emergency overheating, it is desirable to directly regulate battery operation according to the temperature. Herein, smart self-protecting aqueous lithium-ion batteries are developed using thermos-responsive separators prepared through in situ polymerization on the hydrophilic separator. The thermos-responsive separator blocks the lithium ion transport channels at high temperature and reopens when the battery cools down; more importantly, this transition is reversible. The influence of lithium salts on the thermos-responsive behaviors of the hydrogels is investigated. Then suitable lithium salt (LiNO3 ) and concentration (1 m) are selected in the electrolyte to achieve self-protection without sacrificing battery performance. The shut-off temperature can be tuned from 30 to 80 °C by adjusting the hydrophilic and hydrophobic moiety ratio in the hydrogel for targeted applications. This self-protecting LiMn2 O4 /carbon coated LiTi2 (PO4 )3 (LMO/C-LTP) battery shows promise for smart energy storage devices with high safety and extended lifespan in case of high operating temperatures.

Selective Solar Harvesting Windows for Full-Spectrum Utilization.

Smart windows can selectively regulate excess solar radiation to reduce heating and cooling energy consumption in the built environment. However, the inevitable dissipation of ultraviolet and near-infrared into waste heat results in inefficient solar utilization. Herein, a dual-band selective solar harvesting (SSH) window is developed to realize full-spectrum utilization. A transparent photovoltaic, converting ultraviolet into electricity, and a transparent solar absorber, converting near-infrared into thermal energy, are integrated and coupled with a ventilation system to extract heat for indoor use. Compared with common transparent photovoltaics, the SSH window increases solar harvesting efficiency up to threefold while maintaining a considerable visible transmittance. Simulations suggest that the SSH window, besides generating electricity, delivers energy savings by over 30% higher than common smart windows. This is the first integration of transparent photovoltaic and transparent solar absorber into a window, which may open up a new avenue for the development of energy-efficient buildings.

Nanoparticle-on-Mirror Metamaterials for Full-Spectrum Selective Solar Energy Harvesting.

Most broadband metamaterial absorbers are realized by patterning periodic arrays of plasmonic nanoparticles (>100 nm) on dielectric/metallic substrates to enable both electric and magnetic resonances. These metamaterials, however, require costly nanolithographic top-down techniques for fabrication. Here, we demonstrate new-concept nanoparticle-on-mirror (NoM) metamaterial absorbers by densely packing plasmonic nanoparticles of much smaller size (∼30 nm) on metal films directly. Such a simple but rational design enables the use of all-solution-based bottom-up processes. Because of the decoupling of electric and magnetic polarizations in these ultrasmall nanoparticles, excellent impedance match and near-perfect light absorption can be achieved in a broad band over the solar spectrum with weak thermal emission. Proof-of-concept large-area NoM metamaterial absorbers that offer a solar absorptance of 94% but a low IR emittance of 2% are experimentally demonstrated. The outstanding performance, bottom-up process, and great compatibility render the design promising for efficient and large-scale solar energy harvesting.

Near-Infrared-Activated Thermochromic Perovskite Smart Windows.

Perovskite-based thermochromic smart windows that can change color have attracted much interest. However, the high transition temperature (>45 °C in air) hinders their practical application. Herein, a near-infrared (NIR) activated thermochromic perovskite window that enables reversible transition cycles at room temperature is proposed. Under natural sunlight (>700 W m-2 ), it efficiently harvests 78% NIR light to trigger the thermochromism of perovskites, blocking the heat gain from both the visible and NIR light. Meanwhile, it also exhibits a low mid-infrared emissivity of <0.3, suppressing thermal radiation to the indoor environment. A field test demonstrates that this smart window can reduce the indoor temperature by 8 °C compared to a normal glass window at noon. The near-room-temperature color change, multispectral thermal management, outstanding energy-saving ability, and climate adaptability, and solution-based process of this window make it unique and promising for real applications.

All-weather thermochromic windows for synchronous solar and thermal radiation regulation.

Adaptive control of solar and thermal radiation through windows is of pivotal importance for building energy saving. However, such synchronous passive regulations are challenging to be integrated into one thermochromic window. Here, we develop a solar and thermal regulatory (STR) window by integrating poly(N-isopropylacrylamide) (pNIPAm) and silver nanowires (AgNWs) into pNIPAm/AgNW composites. A hitherto unexplored mechanism, originating from the temperature-triggered water capture and release due to pNIPAm phase transition, is exploited to achieve simultaneous regulations of solar transmission and thermal emission. The STR window shows excellent solar modulation (58.4%) and thermal modulation (57.1%) and demonstrates effective regulation of indoor temperatures during both daytime and nighttime. Compared to other thermochromic technologies, the STR window reduces heat loss in cold environment while promotes heat dissipation in hot conditions, achieving efficient energy saving in all weathers. This dual solar and thermal regulation mechanism may provide unidentified insights into the advancement of smart window technology.

Selectively tuning ionic thermopower in all-solid-state flexible polymer composites for thermal sensing.

There has been increasing interest in the emerging ionic thermoelectric materials with huge ionic thermopower. However, it's challenging to selectively tune the thermopower of all-solid-state polymer materials because the transportation of ions in all-solid-state polymers is much more complex than those of liquid-dominated gels. Herein, this work provides all-solid-state polymer materials with a wide tunable thermopower range (+20~-6 mV K-1), which is different from previously reported gels. Moreover, the mechanism of p-n conversion in all-solid-state ionic thermoelectric polymer material at the atomic scale was presented based on the analysis of Eastman entropy changes by molecular dynamics simulation, which provides a general strategy for tuning ionic thermopower and is beneficial to understand the fundamental mechanism of the p-n conversion. Furthermore, a self-powered ionic thermoelectric thermal sensor fabricated by the developed p- and n-type polymers demonstrated high sensitivity and durability, extending the application of ionic thermoelectric materials.

A Solution-Processed Inorganic Emitter with High Spectral Selectivity for Efficient Subambient Radiative Cooling in Hot Humid Climates.

Daytime radiative cooling provides an eco-friendly solution to space cooling with zero energy consumption. Despite significant advances, most state-of-the-art radiative coolers show broadband infrared emission with low spectral selectivity, which limits their cooling temperatures, especially in hot humid regions. Here, an all-inorganic narrowband emitter comprising a solution-derived SiOx Ny layer sandwiched between a reflective substrate and a self-assembly monolayer of SiO2 microspheres is reported. It shows a high and diffusive solar reflectance (96.4%) and strong infrared-selective emittance (94.6%) with superior spectral selectivity (1.46). Remarkable subambient cooling of up to 5 °C in autumn and 2.5 °C in summer are achieved under high humidity without any solar shading or convection cover at noontime in a subtropical coastal city, Hong Kong. Owing to the all-inorganic hydrophobic structure, the emitter shows outstanding resistance to ultraviolet and water in long-term durability tests. The scalable-solution-based fabrication renders this stable high-performance emitter promising for large-scale deployment in various climates.