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.

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.

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.

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.

Spectrally Selective Absorbers/Emitters for Solar Steam Generation and Radiative Cooling-Enabled Atmospheric Water Harvesting.

Renewable energy harvesting from the sun and outer space have aroused significant interest over the past decades due to their great potential in addressing the energy crisis. Furthermore, the harvested renewable energy has benefited another global challenge, water scarcity. Both solar steam generation and passive radiative cooling-enabled atmospheric water harvesting are promising technologies that produce freshwater in green and sustainable ways. Spectral control is extremely important to achieve high efficiency in the two complementary systems based on absorbing/emitting light in a specific wavelength range. For this reason, a broad variety of solar absorbers and IR emitters with great spectral selectivity have been developed. Although operating in different spectral regions, solar selective absorbers and IR selective emitters share similar design strategies. At this stage, it is urgent and necessary to review their progress and figure out their common optical characteristics. Herein, the fundamental mechanisms and recent progress in solar selective absorbers and IR selective emitters are summarized, and their applications in water production are reported. This review aims to identify the importance of selective absorbers/emitters and inspire more research works on selective absorbers/emitters through the summary of advances and the establishment of the connection between solar absorbers and IR emitters.

Solution-Processed All-Ceramic Plasmonic Metamaterials for Efficient Solar-Thermal Conversion over 100-727 °C.

Low-cost and large-area solar-thermal absorbers with superior spectral selectivity and excellent thermal stability are vital for efficient and large-scale solar-thermal conversion applications, such as space heating, desalination, ice mitigation, photothermal catalysis, and concentrating solar power. Few state-of-the-art selective absorbers are qualified for both low- (<200 °C) and high-temperature (>600 °C) applications due to insufficient spectral selectivity or thermal stability over a wide temperature range. Here, a high-performance plasmonic metamaterial selective absorber is developed by facile solution-based processes via assembling an ultrathin (≈120 nm) titanium nitride (TiN) nanoparticle film on a TiN mirror. Enabled by the synergetic in-plane plasmon and out-of-plane Fabry-Pérot resonances, the all-ceramic plasmonic metamaterial simultaneously achieves high, full-spectrum solar absorption (95%), low mid-IR emission (3% at 100 °C), and excellent stability over a temperature range of 100-727 °C, even outperforming most vacuum-deposited absorbers at their specific operating temperatures. The competitive performance of the solution-processed absorber is accompanied by a significant cost reduction compared with vacuum-deposited absorbers. All these merits render it a cost-effective, universal solution to offering high efficiency (89-93%) for both low- and high-temperature solar-thermal applications.