Iridescent Daytime Radiative Cooling with No Absorption Peaks in the Visible Range.

Coatings for passive radiative cooling applications must be highly reflected in the solar spectrum, and thus can hardly support any coloration without losing their functionality. In this work, a colorful daytime radiative cooling surface based on structural coloration is reported. A designed radiative cooler with a bioinspired array of truncated SiO2 microcones is manufactured via a self-assembly method and reactive ion etching. Complemented with a silver reflector, the radiative cooler exhibits broadband iridescent coloration due to the scattering induced by the truncated microcone array while maintaining an average reflectance of 95% in the solar spectrum and a high thermal emissivity (ε) of 0.95, owing to the reduced impedance mismatch provided by the patterned surface at infrared wavelengths, reaching an estimated cooling power of ≈143 W m-2 at an ambient temperature of 25 °C and a measured average temperature drop of 7.1 °C under direct sunlight. This strong cooling performance is attributed to its bioinspired surface pattern, which promotes both the aesthetics and cooling capacity of the daytime radiative cooler.

Smart Materials for Dynamic Thermal Radiation Regulation.

Thermal radiation in the mid-infrared region profoundly affects human lives in various fields, including thermal management, imaging, sensing, camouflage, and thermography. Due to their fixed emissivities, radiance features of conventional materials are usually proportional to the quadruplicate of surface temperature, which set the limit, that one type of material can only present a single thermal function. Therefore, it is necessary and urgent to design materials for dynamic thermal radiation regulations to fulfill the demands of the age of intelligent machines. Recently, the ability of some smart materials to dynamically regulate thermal radiation has been evaluated. These materials are found to be competent enough for various commands, thereby, providing better alternatives and tremendously promoting the commercial potentials. In this review, the dynamic regulatory mechanisms and recent progress in the evaluation of these smart materials are summarized, including thermochromic materials, electrochromic materials, mechanically and humidity responsive materials, with the potential applications, insufficient problems, and possible strategies highlighted.

Dynamically Switchable Multicolor Electrochromic Films.

The dynamic optical switch of plasmonic nanostructures is highly desirable due to its promising applications in many smart optical devices. To address the challenges in the reversibility and transmittance contrast of the plasmonic electrochromic devices, here, a strategy is reported to fabricate color switchable electrochromic films through electro-responsive dissolution and deposition of Ag on predefined hollow shells of Au/Ag alloy. Using the hollow Au/Ag alloy nanostructures as stable seeds for site-specific deposition of Ag, elimination of the random self-nucleation events is enabled and optimal reversibility in color switching is allowed. The hollow structure further enables excellent transmittance contrast between the bleached and colored states. With its additional advantages such as the convenience for preparation, high sensitivity, and field-tunable optical property, it is believed that this new electrochromic film represents a unique platform for designing novel smart optical devices.

Entropy-Induced Self-Assembly of Colloidal Crystals with High Reflectivity and Narrow Reflection Bandwidth.

Cracks and defects, which could result in lower reflectivity and larger full width at half maximum (FWHM), are the major obstacles for obtaining highly ordered structures of colloidal crystals (CCs). The high-quality CCs with high reflectivity (more than 90%) and 9.2 nm narrow FWHM have been successfully fabricated using a fixed proportion of a soft matter system composed of silica particles (SPs), polyethylene glycol diacrylate (PEGDA), and ethanol. The influences of refractivity difference, volume fractions, and particle dimension on FWHM were illuminated. Firstly, we clarified the influences of the planar interface and the bending interface on the self-assembly. The CCs had been successfully fabricated on the planar interface and presented unfavorable results on the bending interface. Secondly, a hard sphere system consisting of SPs, PEGDA, and ethanol was established, and the entropy-driven phase transition mechanism of a polydisperse system was expounded. The FWHM and reflectivity of CCs showed an increasing trend with increasing temperature. Consequently, high-quality CCs were obtained by adjusting temperatures (ordered structure formed at 90 °C and solidified at 0 °C) based on the surface phase rule of the system. We acquired a profound understanding of the principle and process of self-assembly, which is significant for preparation and application of CCs such as optical filters.

Patterned polyaniline encapsulated in titania nanotubes for electrochromism.

In this article, we report the preparation of a TiO2 nanotube array (TNA) film used as a transparent electrochromic material and a TNA/polyaniline patterned hybrid electrochromic film utilized as an information display material. The TNA film was fabricated by an anodizing process, and a surface patterned TNA with extreme wettability contrast (hydrophilic/hydrophobic) on a TNA surface through self-assembly (SAM) and photocatalytic lithography is fabricated. Then the TNA/polyaniline hybrid film was prepared by electrodeposition of aniline in an aqueous solution. Finally, the electrochromic properties of the TNA film and the TNA/polyaniline hybrid film were investigated. Compared with neat TNA film and polyaniline (PANI) films, the hybrid film shows a much higher optical contrast in the near infrared range. The TNA/polyaniline hybrid film shows higher coloration efficiencies of 24.4 cm2 C-1 at a wavelength of 700 nm and 17.1 cm2 C-1 at a wavelength of 1050 nm compared to the TNA coloration efficiency. The color switching time (20.9 s or 22.9 s) of TNA/polyaniline is faster than TNA.

A nanostructured Fc(COCH3)2 film prepared using silica monolayer colloidal crystal templates and its electrochromic properties.

Since oxidation and reduction reactions mainly take place on surfaces, enlarging the specific surface of redox materials is the key to achieving excellent electrochemical performance. In this work, by using silica monolayer colloidal crystal templates (MCCTs), a nanostructured Fc(COCH3)2 film is prepared successfully, and such a nanostructure could exhibit the following unique electrochemical properties: the MCCTs could impede the aggregation tendency of Fc(COCH3)2 and possess high electrochemical activity; Fc(COCH3)2 enlarges the contact area and offers more active sites and faster electronic transmission channels. The structure, optical and electrochemical properties of the nanostructured Fc(COCH3)2 were tested and then compared with those of compact Fc(COCH3)2 films to evaluate the role of the nanoarchitecture. The unique structure design of the Fc(COCH3)2 film enables outstanding performance, showing a large transmittance change (ΔT) of 37% at 550 nm when switched between 0.5 V and -2.5 V, which is approximately ninefold higher than that of the compact Fc(COCH3)2 film (approximately 4%). Response times of coloration and bleaching are found to be only 16.15 s and 5.56 s. Furthermore, the nanostructured Fc(COCH3)2 film shows much better cycling stability than the compact one. The results indicate that the nanostructure could significantly improve the electrochemical performance of the Fc(COCH3)2 film due to the increase in electrochemical active sites and the enhancement of the "D-to-A" redox switch of ferrocene.

Rational selection of amorphous or crystalline V2O5 cathode for sodium-ion batteries.

Vanadium oxide (V2O5), as a potential positive electrode for sodium ion batteries (SIBs), has attracted considerable attention from researchers. Herein, amorphous and crystalline V2O5 cathodes on a graphite paper without a binder and conductive additives have been synthesized via facile anodic electrochemical deposition following different heat treatments. Both the amorphous V2O5 (a-V2O5) cathode and crystalline V2O5 (c-V2O5) cathode show good rate cycling performance and long cycling life. After five rate cycles, the reversible capacities of both the cathodes were almost unchanged at different current densities from 40 to 5120 mA g-1. Long cycling tests with 10 000 cycles were carried out and the two cathodes exhibit excellent cycling stability. The c-V2O5 cathode retains a high specific capacity of 54 mA h g-1 after 10 000 cycles at 2560 mA g-1 and can be charged within 80 s. Interestingly, the a-V2O5 cathode possesses higher reversible capacities than the c-V2O5 cathode at low current densities, whereas it is inversed at high current densities. The c-V2O5 cathode shows faster capacity recovery from 5120 to 40 mA g-1 than the a-V2O5 cathode. When discharged at 80 mA g-1 (long discharge time of 140 min) and charged at 640 mA g-1 (short charge time of 17 min), the a-V2O5 cathode shows a higher discharge capacity than its c-V2O5 counterpart. The different electrochemical performance of a-V2O5 and c-V2O5 cathodes during various electrochemical processes can provide a rational selection of amorphous or crystalline V2O5 cathode materials for SIBs in their practical applications to meet the variable requirements.

Electrodeposition of Three Dimensionally Ordered Macroporous Germanium from Two Different Ionic Liquids.

Three dimensionally ordered macroporous (3DOM) Ge films have been made via ordered polystyrene (PS) templates by electrodeposition from ionic liquids 1-Butyl-3-methylimidazolium bis (trifluoromethylsulfonyl) amide and 1-Ethyl-3-methylimidazolium tris (pentafluoroethyl) trifluorophosphate at room temperature. We discuss the possibility of obtaining high quality 3DOM Ge films from two different ionic liquids by the simple and inexpensive template-assisted electrochemical pathway. Scanning electron microscopy confirms the quality of the samples, and the optical measurements demonstrate that 3DOM Ge made electrochemically shows photonic crystal behavior. Such a material has the potential to make 3DOM Ge feasible for electrical, optical applications and for photonic crystal solar cells.

Hydrogen photochromism in Nb2O5 powders.

In this paper, we report on the hydrogen photochromism in Nb2O5 powders with different structures. Four different powder phases were prepared by calcining Nb2O5·nH2O powders at various temperatures, and their morphology, structure, and electronic band structure were characterized by scanning electron microscopy, structural analyses, thermogravimetric analysis, differential scanning calorimetry, and optical spectroscopy. Nb2O5 powders with different structures and very different properties were formed after different high-temperature treatments of the polymorphous oxide. A pronounced photochromic effect was observed in the M and H phases of Nb2O5, whereas the other phases exhibited poor photochromic responses. Because photochromism arises due to the detachment of hydrogen atoms under the action of light from hydrogen donor molecules previously adsorbed on the oxide surface, the electronic band structure and the morphology have strong influences on the photochromic properties of Nb2O5 powders. For these reasons, a pronounced photochromic effect was achieved in the H phase.

Rejuvenation of Electrochromic Devices.

Electrochromic devices (ECDs) are a hot pot due to their significant energy-saving effect in green buildings. However, the ECDs suffer from degradation induced by ion trapping during cycling, which restricts their further development. Here, it is demonstrated that the electrochromic performance of the degraded ECDs can be rejuvenated by heat treatment method The release mechanism of trapped ions in films is simulated and validated using three types of ECDs. The semi-solid-state ECD evinces a state of near-failure at low temperatures can regain its initial performance by heating. All-solid-state ECDs, including amorphous WO3 (a-WO3 ECD) and crystalline WO3 (c-WO3 ECD) as the electrochromic layer, can also release the trapped ions and regain the performance (97.3% and 95.5% of initial optical modulation) by annealing, regardless of the way of degradation. The research has extended the lifespan of multiple ECDs, providing significant practical value and promoting sustainable, and eco-friendly development.

Unprecedented Spatial Manipulation and Transformation of Dynamic Thermal Radiation Based on Vanadium Dioxide.

Reconfigurable infrared (IR) materials have widespread applications in thermal management and smart IR concealment. Although various reconfigurable IR materials can be customized by positive or negative differential VO2-based resonators, their insightful mechanism remains unknown. Here, we comprehensively investigate the fundamental design rule of reconfigurable thermal radiation between positive and negative differential thermal radiation properties for the first time. Importantly, the skin depth of VO2 film in the metal state is investigated to clarify the transformation from positive to negative differential thermal radiation properties, and the critical thickness is further derived, providing important guidance in designing the reconfigurable thermal radiation regulator. Furthermore, the reconfigurable multistate thermal images had been presented into one plate. The resulting emittance variation (△ε8-14 µm) of the VO2-based resonator can change from 0.61 to -0.53, which consummates the ability for diverse demands such as infrared concealment, thermal illusion, and thermal management. This work constitutes a promising and universal route toward designing whole smart devices and may create new scientific and technological opportunities for platforms that can benefit from reconfigurable electromagnetic manipulation.

Tunable High-Performance Electromagnetic Interference Shielding of VO2 Nanowires-Based Composite.

The unique metal-insulator transition of VO2 is very suitable for dynamic electromagnetic (EM) regulation materials due to its sharp change in electrical conductivity. Here, we have developed an off/on switchable electromagnetic interference (EMI) shielding composite by interconnecting VO2 nanowires (NWs) in poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) to form conductive networks, resulting in outstanding performance at the X and Ku bands with maximum change values of 44.8 and 59.4 dB, respectively. The unique insulator-to-metal transition (IMT) of VO2 NWs has dominated the variation of polarization loss (εp″) and conductivity loss (εσ″) for the composites, which is the mechanism of EMI shielding switching between off and on states. Furthermore, the composite exhibits good cycling stability of the off/on switchable EMI shielding performance and has excellent mechanical properties, especially with 200 times abrasion resistance without obvious weight loss. This study provides a unique approach for dynamic switching of EM response with the potential to construct practical intelligent EM response systems for next-generation smart electromagnetic devices in various scenarios.

Two-dimensional Si(x)Ge(1-x) films with variable composition made via multilayer colloidal template-guided ionic liquid electrodeposition.

The binary alloy system Si(x)Ge(1-x) provides a continuous series of materials with gradually varying properties. In this paper, we report on a fundamental basis a method to make large-area macroporous Si(x)Ge(1-x) films with variable Ge content by electrodeposition in an ionic liquid, with SiCl(4) and GeCl(4) as precursors. The chemical composition of the products can be modified by changing the molar ratio of the precursors. Periodical macroporous Si(x)Ge(1-x) was made by a multilayer polystyrene (PS) template assembled as face-centered cubic lattice. Two-dimensional (2-D) Si(x)Ge(1-x) bowl-like and fishing-net structures can be obtained by applying different deposition temperatures. The results highlight the potential applications, including photonic bandgap and battery materials, as well as ultra-thin gratings, due to the effect of modification of light and improved tunability of composition, although Si(x)Ge(1-x) made by our method is sensitive to oxidation by air.

Electrostatic Interfacial Cross-Linking and Structurally Oriented Fiber Constructed by Surface-Modified 2D MXene for High-Performance Flexible Pseudocapacitive Storage.

Fiber supercapacitors are promising power supplies suitable for wearable electronics, but the internally insufficient cross-linking and random structure of fiber electrodes restrict their performance. This study describes how interfacial cross-linking and oriented structure can fabricate an MXene fiber with high flexibility and electrochemical performance. The continuous and highly oriented macroscopic fibers were constructed by 2D MXene sheets via a liquid-crystalline wet-spinning assembly. The oxyanion-enriched terminations of surface-modified MXene in situ could reinforce the interfacial cross-linking by electrostatic interactions while mediating the sheet-to-sheet lamellar structure within the fiber. The resultant MXene fiber exhibits high electrical conductivity (3545 S cm-1) and mechanical strength (205.5 MPa) and high pseudocapacitance charge storage capability up to 1570.5 F cm-3. Notably, the assembled fiber supercapacitor delivers an energy density of 77.6 mWh cm-3 at 401.9 mW cm-3, exceptional flexibility and stability exhibiting ∼99.5% capacitance retention under mechanical deformation, and can be integrated into commercial textiles to power microelectronic devices. This work provides insight into the fabrication of an advanced MXene fiber and the development of high-performance flexible fiber supercapacitors.

Polyaniline-Based Infrared Dynamic Patterned Encoder with Multiple Thermal Radiation Characteristics.

A high-level infrared dynamic patterned encoder (IR-DPE) possesses prospective applications for energy-harvesting and information, but a simple and reliable method for fabrication remains challenging. Herein, we first report an IR-DPE with multiple thermal radiation characteristics based on polyaniline (PANI). Specifically, the electron-beam evaporation technique is introduced to obtain the divanadium pentoxide (V2O5) coating, and then the V2O5 film acts as an oxidant to drive in situ polymerization of the PANI film. During the process, we experimentally explore the relationship between the thickness of V2O5 and the emissivity of PANI to obtain up to six emissivity levels and achieve the IR pattern integrated into multiple thermal radiation characteristics. The device shows multiple thermal radiation characteristics at the oxidized state, realizing a pattern visible with the IR camera and the same thermal radiation properties at the reduced state, leading to the pattern concealed in the IR regime. In addition, the highest emissivity tunability of the device is to be tuned from 0.40 to 0.82 (Δε = 0.42) at 2.5-25 µm. Meanwhile, the device exhibits a maximum temperature control of up to 5.9 °C. The results show the enormous potential of IR-DPEs for IR information transfer and thermal management.

Core-Shell-Structured Electrorheological Fluid with a Polarizability-Tunable Nanocarbon Shell for Enhanced Stimuli-Responsive Activity.

The incorporation of nanocarbon-based materials into electrorheological fluids has been shown to be an effective means of improving the electrorheological (ER) response. However, the mechanism of the sp2/sp3-hybridized carbon structure and high ER response is still under investigation. Herein, barium titanate@nanocarbon shell (BTO@NCs) composites are proposed and prepared by introducing carbonized polydopamine (C-PDA) into a shell. When the polymerization time of dopamine is tuned, the shell thickness, surface polar functional groups, and sp2/sp3-hybridized carbon can be effectively controlled. The maximum yield stress of the BTO@NCs-24 h ER fluid reaches 2.5 kPa under an electric field of 4 kV mm-1, which is attributed to the increased content of sp3 C-OH and oxygenous functional groups within the shell, resulting in a rapidly achievable polarization. Furthermore, the SiO2@NCs and TiO2@NCs ER fluids are also prepared with enhanced ER behavior in these phenomena, confirming an approach to high-performance ER fluids based on nanocarbon composites.

Oxygen vacancy modulated amorphous tungsten oxide films for fast-switching and ultra-stable dual-band electrochromic energy storage smart windows.

Dual-band electrochromic energy storage (DEES) windows, which are capable of selectively controlling visible (VIS) and near-infrared (NIR) light transmittance, have attracted research attention as energy-saving devices that integrate electrochromic (EC) and energy storage functions. However, there are few EC materials with spectrally selective modulation. Herein, oxygen vacancy modulated amorphous tungsten oxide (a-WO3-x-OV) is firstly shown to be a potential material for DEES windows. Furthermore, experimental results and density functional theory (DFT) calculations demonstrate that an oxygen vacancy not only enables the a-WO3-x-OV films to modulate NIR light transmittance selectively, but also enhances ion adsorption and diffusion in the a-WO3-x host to obtain excellent EC performance and a large energy storage capacity. Consequently, the a-WO3-x-OV film can selectively control VIS and NIR light transmittance with a state-of-the-art EC performance, including high optical modulation (91.8% and 80.3% at 633 and 1100 nm, respectively), an unprecedentedly fast switching speed (tb/tc = 4.1/5.3 s), high coloration efficiency (167.96 cm2 C-1), high specific capacitance (314 F g-1 at 0.5 A g-1), and ultra-robust cycling stability (83.3% optical modulation retention after 8000 cycles). The fast-switching and ultra-stable dual-band EC properties with efficient energy recycling are also successfully demonstrated in a DEES prototype. The results demonstrate that the a-WO3-x-OV films show great potential for application in high-performance DEES smart windows.

Enhanced photoluminescence of ordered macroporous germanium electrochemically prepared from ionic liquids.

Recently we reported our results on the successful synthesis of 3-D highly ordered macroporous (3DOM) structure of germanium via the template-assisted electrochemical deposition from air- and water stable ionic liquids. Herein we report our new results on the photoluminescence (PL) properties of the obtained ordered macroporous Ge and the Ge/polystyrene composite opal structure. The latter showed a strong green emission compared to a Ge film and a Ge inverse opal. The enhancement of PL intensity was ascribed to the disorder multiple scattering in polystyrene colloidal crystal structure which increased both the excitation light absorption efficiency and the light extraction efficiency. The X-ray photoelectron spectroscopy (XPS) results suggested that the ordered macroporous Ge was capped with an oxide layer including a considerable amount of GeO(2). The observed green emission (539 nm) was related to GeO(2), likely resulting from the Ge-O bond related intrinsic defects.

Enhanced photon absorption of single nanowire α-Si solar cells modulated by silver core.

Single nanowire solar cells are a promising candidate as nanoelectronic power sources. Metallic cores were integrated in single nanowire solar cells, and the influence of the silver core on the absorption efficiency and the short circuit current was studied in this work. A Full-wave Vectorial Finite Element Method approach was used to rigorously solve Maxwell's equations in two dimensions. The photon absorption in solar cells was modulated delicately to achieve higher absorption efficiencies and short circuit currents, by tuning the core size and radius of nanowire solar cells. The light trapping stemmed mainly from the localized surface plasmons and also from Mie scattering and leaky mode resonances. The results showed that an enhancement of 16.6% in the photocurrent could be achieved by α-Si nanowire solar cells with the proper core size and filling-ratio compared to that without silver core.

Three-dimensionally ordered macroporous silicon films made by electrodeposition from an ionic liquid.

Three dimensionally ordered macroporous (3DOM) silicon films have been made via ordered polystyrene (PS) templates by electrodeposition from an ionic liquid (IL). For this purpose, the ionic liquid 1-butyl-1-methylpyrrolidinium bis(trifluoromethylsulfonyl)amide ([Py(1,4)]Tf(2)N) with SiCl(4) dissolved in it was used as an electrolyte and the electrodeposition of macroporous silicon could be achieved at room temperature (~20 °C). Self-assembled PS colloidal crystals with different diameters were used as templates. Scanning electron microscopy and X-ray photoelectron spectroscopy confirm the quality of the samples, and the optical transmission measurement demonstrates that the 3DOM silicon film has a bandgap in the near infrared regime. Such a material has the potential to make 3DOM silicon feasible for electrical and optical applications.