Interfacial Modulation through Mixed‐Dimensional Heterostructures for Efficient and Hole Conductor‐Free Perovskite Solar Cells

Advanced Materials

High‐performance perovskite solar cells (PSCs) typically require interfacial passivation, yet this is challenging for the buried interface, owing to the dissolution of passivation agents during the deposition of perovskites. Here, this limitation is overcome with in situ buried‐interface passivation—achieved via directly adding a cyanoacrylic‐acid‐based molecular additive, namely BT‐T, into the perovskite precursor solution. Classical and ab initio molecular dynamics simulations reveal that BT‐T spontaneously may self‐assemble at the buried interface during the formation of the perovskite layer on a nickel oxide hole‐transporting layer. The preferential buried‐interface passivation results in facilitated hole transfer and suppressed charge recombination. In addition, residual BT‐T molecules in the perovskite layer enhance its stability and homogeneity. A power‐conversion efficiency (PCE) of 23.48% for 1.0 cm2 inverted …

Nature

Solar fuels offer a promising approach to provide sustainable fuels by harnessing sunlight,. Following a decade of advancement, Cu2O photocathodes are capable of delivering a performance comparable to that of photoelectrodes with established photovoltaic materials, –. However, considerable bulk charge carrier recombination that is poorly understood still limits further advances in performance. Here we demonstrate performance of Cu2O photocathodes beyond the state-of-the-art by exploiting a new conceptual understanding of carrier recombination and transport in single-crystal Cu2O thin films. Using ambient liquid-phase epitaxy, we present a new method to grow single-crystal Cu2O samples with three crystal orientations. Broadband femtosecond transient reflection spectroscopy measurements were used to quantify anisotropic optoelectronic properties, through which the carrier mobility along the [111 …

Materials Advances

Artificial synapses based on resistive switching have emerged as a promising avenue for brain-inspired computing. Hybrid metal halide perovskites have provided the opportunity to simplify resistive switching device architectures due to their mixed electronic–ionic conduction, yet the instabilities under operating conditions compromise their reliability. We demonstrate reliable resistive switching and synaptic behaviour in layered benzylammonium (BzA) based halide perovskites of (BzA)2PbX4 composition (X = Br, I), showing a transformation of the resistive switching from digital to analog with the change of the halide anion. While (BzA)2PbI4 devices demonstrate gradual set and reset processes with reduced power consumption, the (BzA)2PbBr4 system features a more abrupt switching behaviour. Moreover, the iodide-based system displays excellent retention and endurance, whereas bromide-based devices …

Advanced Materials

Efficient and robust n‐i‐p perovskite solar cells necessitate superior organic hole‐transport materials with both mechanical and electronic prowess. Deciphering the structure−property relationship of these materials is crucial for practical perovskite solar cell applications. Through direct arylation, we synthesized two high glass transition temperature molecular semiconductors, DBC‐ETPA (202 °C) and TPE‐ETPA (180 °C), using dibenzo[g,p]chrysene (DBC) and 1,1,2,2‐tetraphenylethene (TPE) tetrabromides with triphenylene–ethylenedioxythiophene‐dimethoxytriphenylamine (ETPA). In comparison to spiro‐OMeTAD, both semiconductors exhibit shallower HOMO energy levels, resulting in increased hole densities (generated by air oxidation doping) and accelerated hole extraction from photoexcited perovskite. Experimental and theoretical studies highlight the more rigid DBC core, enhancing hole mobility due to …

Advanced Materials

Self‐powered skin optoelectronics fabricated on ultrathin polymer films is emerging as one of the most promising components for the next‐generation Internet of Things (IoT) technology. However, a longstanding challenge is the device underperformance owing to the low process temperature of polymer substrates. In addition, broadband electroluminescence (EL) based on organic or polymer semiconductors inevitably suffers from periodic spectral distortion due to Fabry–Pérot (FP) interference upon substrate bending, preventing advanced applications. Here, ultraflexible skin optoelectronics integrating high‐performance solar cells and monochromatic light‐emitting diodes using solution‐processed perovskite semiconductors is presented. n–i–p perovskite solar cells and perovskite nanocrystal light‐emitting diodes (PNC‐LEDs), with power‐conversion and current efficiencies of 18.2% and 15.2 cd A−1 …

Scientific Reports

In this work we study in-depth the antireflection and filtering properties of ultrathin-metal-film-based transparent electrodes (MTEs) integrated in thin-film solar cells. Based on numerical optimization of the MTE design and the experimental characterization of thin-film perovskite solar cell (PSC) samples, we show that reflection in the visible spectrum can be strongly suppressed, in contrast to common belief (due to the compact metal layer). The optical loss of the optimized electrode (~ 2.9%), composed of a low-resistivity metal and an insulator, is significantly lower than that of a conventional transparent conductive oxide (TCO ~ 6.3%), thanks to the very high transmission of visible light within the cell (> 91%) and low thickness (< 70 nm), whereas the reflection of infrared light (~ 70%) improves by > 370%. To assess the application potentials, integrated current density > 25 mA/cm2, power conversion …

Joule

A widely used component of high-efficiency perovskite solar cells (PSCs) is the molecular hole-transport material (HTM) spiro-OMeTAD. This organic solid needs to be p-doped to acquire sufficient hole conductivity. However, the conventional doping method using LiTFSI in the air is slow, sensitive to the environment, and may lead to the deterioration of the PSCs by unintended oxidation or dopant migration. It is thus highly desirable to develop fast doping approaches that avoid exposing the PSC to ambient air and easy-to-move dopant ions. We report here that light absorption by spiro-OMeTAD itself triggers redox photochemistry that has so far been ignored. Strikingly, we found that Y(III) or La(III)-tBP complexes catalyze the symmetry-breaking charge separation of photo-excited spiro-OMeTAD, resulting in the efficient p-doping of the HTM. Using this photo-redox process, we realize PSCs with superior stability over …

Advanced Materials

Efficient and robust n‐i‐p perovskite solar cells necessitate superior organic hole‐transport materials with both mechanical and electronic prowess. Deciphering the structure−property relationship of these materials is crucial for practical perovskite solar cell applications. Through direct arylation, we synthesized two high glass transition temperature molecular semiconductors, DBC‐ETPA (202 °C) and TPE‐ETPA (180 °C), using dibenzo[g,p]chrysene (DBC) and 1,1,2,2‐tetraphenylethene (TPE) tetrabromides with triphenylene–ethylenedioxythiophene‐dimethoxytriphenylamine (ETPA). In comparison to spiro‐OMeTAD, both semiconductors exhibit shallower HOMO energy levels, resulting in increased hole densities (generated by air oxidation doping) and accelerated hole extraction from photoexcited perovskite. Experimental and theoretical studies highlight the more rigid DBC core, enhancing hole mobility due to …

Advanced Materials Interfaces

Interfacial space charges significantly influence transport and recombination of charge carriers in optoelectronic devices. Due to the mixed ionic‐electronic conducting properties of halide perovskites, not only electronic effects, but also ionic interactions at their interfaces need to be considered in the analysis of space charges. Understanding of these interactions and their control is currently missing. This study elucidates the ionic effects on space charge formation at the interface between methylammonium lead iodide (MAPI) and alumina, and its modulation through surface modification using organic molecules. Embedding insulating alumina nanoparticles within MAPI films leads to enhancement of the electronic conductivity. This effect is consistent with the formation of an interfacial inversion layer in MAPI and can only be explained on the basis of ionic interactions. Such an effect is attenuated by surface …

Solar fuels offer a promising approach to provide sustainable fuels by harnessing sunlight. Following a decade of advancement, Cu2O photocathodes are capable of delivering a performance comparable to that of photoelectrodes with established photovoltaic materials. However, considerable bulk charge carrier recombination that is poorly understood still limits further advances in performance. Here we demonstrate performance of Cu2O photocathodes beyond the state-of-the-art by exploiting a new conceptual understanding of carrier recombination and transport in single-crystal Cu2O thin films. Using ambient liquid-phase epitaxy, we present a new method to grow single-crystal Cu2O samples with three crystal orientations. Broadband femtosecond transient reflection spectroscopy measurements were used to quantify anisotropic optoelectronic properties, through which the carrier mobility along the [111] orientation was found to be an order of magnitude higher than those along other orientations. Driven by these findings, we developed a polycrystalline Cu2O photocathode with an extraordinarily pure (111) orientation and (111) terminating facets using a simple and low-cost method, which delivers 7 mA cm− 2 current density (more than 70% improvement compared to that of state-of-the-art electrodeposited devices) at 0.5 V versus a reversible hydrogen electrode under air mass 1.5 G illumination, and stable operation over at least 120 h.

Energy & Environmental Materials

The systematic advances in the power conversion efficiency (PCE) and stability of perovskite solar cells (PSCs) have been driven by the developments of perovskite materials, electron transport layer (ETL) materials, and interfacial passivation between the relevant layers. While zinc oxide (ZnO) is a promising ETL in thin film photovoltaics, it is still highly desirable to develop novel synthetic methods that allow both fine‐tuning the versatility of ZnO nanomaterials and improving the ZnO/perovskite interface. Among various inorganic and organic additives, zwitterions have been effectively utilized to passivate the perovskite films. In this vein, we develop novel, well‐characterized betaine‐coated ZnO QDs and use them as an ETL in the planar n‐i‐p PSC architecture, combining the ZnO QDs‐based ETL with the ZnO/perovskite interface passivation by a series of ammonium halides (NH4X, where X = F, Cl, Br). The …

Energy & Environmental Science

Light-induced degradation in metal halide perovskites is a major concern that can potentially hamper the commercialization of perovskite optoelectronic devices. The phenomena viz. ion migration, phase segregation, and defect intolerance are believed to be the factors behind the degradation. However, a detailed mechanistic understanding of how and why light reduces the long-term stability of perovskites is still lacking. Here, by combining multiscale characterization techniques and computational studies, we uncover the role of white light in the surface degradation of state-of-the-art FAPbI3-rich perovskite absorbers (reaching up to 22% PCE in solar cells). We unravel the degradation kinetics and found that white light triggers the chemical degradation of perovskite into secondary phases with higher work function and metallic I–V characteristics. Furthermore, we demonstrate that perovskite degradation is triggered …

Energy & Environmental Materials

The systematic advances in the power conversion efficiency (PCE) and stability of perovskite solar cells (PSCs) have been driven by the developments of perovskite materials, electron transport layer (ETL) materials, and interfacial passivation between the relevant layers. While zinc oxide (ZnO) is a promising ETL in thin film photovoltaics, it is still highly desirable to develop novel synthetic methods that allow both fine‐tuning the versatility of ZnO nanomaterials and improving the ZnO/perovskite interface. Among various inorganic and organic additives, zwitterions have been effectively utilized to passivate the perovskite films. In this vein, we develop novel, well‐characterized betaine‐coated ZnO QDs and use them as an ETL in the planar n‐i‐p PSC architecture, combining the ZnO QDs‐based ETL with the ZnO/perovskite interface passivation by a series of ammonium halides (NH4X, where X = F, Cl, Br). The …

Advanced Materials

High‐performance perovskite solar cells (PSCs) typically require interfacial passivation, yet this is challenging for the buried interface, owing to the dissolution of passivation agents during the deposition of perovskites. Here, this limitation is overcome with in situ buried‐interface passivation—achieved via directly adding a cyanoacrylic‐acid‐based molecular additive, namely BT‐T, into the perovskite precursor solution. Classical and ab initio molecular dynamics simulations reveal that BT‐T spontaneously may self‐assemble at the buried interface during the formation of the perovskite layer on a nickel oxide hole‐transporting layer. The preferential buried‐interface passivation results in facilitated hole transfer and suppressed charge recombination. In addition, residual BT‐T molecules in the perovskite layer enhance its stability and homogeneity. A power‐conversion efficiency (PCE) of 23.48% for 1.0 cm2 inverted …

Solar Rrl

The carrier transport layer plays a critical role in high efficiency and stable perovskite solar cells (PSCs). Herein, CsPbBr3 quantum dots‐sensitized mesoporous TiO2 (CPB–TiO2) electron transport layer for fabricating high‐quality perovskite films with enhanced phase stability is developed. The CPB–TiO2 layer enhances the perovskite crystallinity, phase stability, and reduces the nonradiative carrier recombination in PSCs. As a result, the CPB–TiO2 significantly improves the power conversion efficiency of FAPbI3 PSCs from 23.11% to 24.46% and reduces the device hysteresis. The CPB–TiO2–FAPbI3 device shows enhanced stability, retaining 90% of its initial efficiency after 500 h operation at maximum power point tracking under 1 sun illumination, whereas the control device degrades to 80% of initial performance in the first 200 h. In addition, this strategy is applicable to CsPbI3 perovskite, which provides a …

Experimental and theoretical works covering a wide range of photosynthetic and biohydrogen topics, from the primary processes of electron transfer and energy bioconversion to the physiological aspects of photosynthesis and applied aspects of hydrogen production are discussed at the conference. Considerable attention is paid to discussion of structural organization of photosynthetic reaction centers, structure and function of photosystems, artificial photosynthesis, mechanisms of hydrogen production etc. The book will be of interest to researchers and students involved in the study of photosynthesis and bio-hydrogen production

Solar RRL

Wide‐bandgap hybrid halide perovskites are increasingly relevant in the fabrication of tandem solar cells. However, their efficiency and stability during operation are still limited by several factors, among which ion migration at the interface with charge‐selective extraction layers is one of the most detrimental ones. Herein, a host–guest complexation strategy is employed to control interfacial ion migration by using dibenzo‐21‐crown‐7 in wide‐bandgap hybrid halide perovskites based on methylammonium lead bromide. The capacity of the crown ether is demonstrated that affect the performances and stabilities of MAPbBr3 solar cells. As a result, power conversion efficiencies of up to 5.9% are achieved with an open circuit voltage as high as 1.5 V, which is accompanied by stability over 300 h at 85 °C under nitrogen atmosphere, as well as more than 300 h at ambient temperature, maintaining ∼80% of initial …

Advanced Functional Materials

Cholesteric liquid crystal elastomers (CLCEs) are unique anisotropic rubbers that can change their structural color in response to various stimuli such as heat, chemicals, electric fields, and mechanical stress. Methods such as anisotropic deswelling and surface alignment have been adopted to prepare CLCEs; however, they have limitations in creating spatially controlled CLCE geometries. In this work, a direct ink writing (DIW)‐based 3D‐printable CLCE that can be prepared by extruding viscous CLC ink is developed through a 3D printer nozzle, followed by photopolymerization. Interestingly, the helical axis is inclined to the printing direction by ≈32° due to a combination of the shear‐induced alignment causes during extrusion and the elongational force generated during deposition onto the substrate. This unusual helical axis distortion leads to both blue and red shifts of the reflection color depending on the …

Advanced Functional Materials

Shape memory polymers (SMPs) capable of generating various deformations from anisotropic temporary shapes to permanent shapes have been emerging as soft robots. However, traditional SMPs cannot imitate the antagonistic movement of human skeletal muscles due to their modulus limitations in shape programming and recovery process. Herein, hydration programmable shape memory polymer (HP‐SMP)‐based fibers that can undergo reversible actuation by assembling antagonistic pairs are reported, where the shape programming of the antagonist muscle relies on the contraction of agonist muscle. HP‐SMP fibers are composed of tunicate cellulose nanocrystals (TCNCs) reinforced semi‐interpenetrating polymer networks. Leveraging their distinctive structure and hydration programmability, the HP‐SMP fibers exhibit large actuation strain (−60%) and high work capacity (751 J kg−1), allowing for …

Advanced Functional Materials

In article number 2309589, Zong-Liang Tseng, Shun-Wei Liu, and co-workers demonstrate an effective strategy for improving the leakage resistance and turn-on voltage of solution-processed upconversion devices. Emissive perovskite quantum dots and a synergistic hole-transporting layer ensure the quality of quantum-dot films and provide a new way for designing high-performance solutionprocessed upconversion devices.

Advanced Functional Materials

The oxygen reduction reaction (ORR) plays a fundamental role in sustainable energy technologies. However, the creation of non‐precious metal electrocatalysts with high ORR activity and durability under all pH conditions is of great significance but remains challenging. Herein, the aim is to overcome this challenge by creating a Fe single atom catalyst on a 2D defect‐containing nitrogen‐doped carbon support (Fe1/DNC) via a microenvironment engineering strategy. Microkinetic modeling reveals that FeN4(OH) moieties are the real active sites under reaction conditions. Due to the synergistic promotion effect of denser accessible FeN4(OH) moieties and defect‐induced electronic properties, Fe1/DNC catalyst achieves extraordinary ORR activity under alkaline, acidic, and neutral conditions, with half‐wave potentials of 0.95, 0.82, and 0.70 V, respectively. Moreover, a negligible performance decay is observed with …

Advanced Functional Materials

Superconducting niobium (Nb) thin films have recently attracted significant attention due to their utility for quantum information technologies. In the processing of Nb thin films, fluoride‐based chemical etchants are commonly used to remove surface oxides that are known to affect superconducting quantum devices adversely. However, these same etchants can also introduce hydrogen to form Nb hydrides, potentially negatively impacting microwave loss performance. Here, comprehensive materials characterization of Nb hydrides formed in Nb thin films as a function of fluoride chemical treatments is presented. In particular, secondary‐ion mass spectrometry, X‐ray scattering, and transmission electron microscopy reveal the spatial distribution and phase transformation of Nb hydrides. The rate of hydride formation is determined by the fluoride solution acidity and the etch rate of Nb2O5, which acts as a diffusion barrier …

Advanced Functional Materials

As an important method of image processing, image differentiation enables edge detection of targets to achieve recognition of object features and information compression and the computation speed can be boosted by optical information techniques. Traditional optical image differentiation methods mainly rely on spatial spectrum filtering by using classical 4f system, while some work focus on 1D or single‐direction differentiation. It is only in recent years that the rapid development of metasurfaces has facilitated image differentiation methods. In this work, a Laplace operation device is demonstrated based on a silicon hollow brick dielectric resonant metasurface for incident light field. The optical transfer function (OTF) required by the optical Laplace operation can be obtained by exciting an angularly selective toroidal dipole (TD) resonance supported by the metasurface. This hollow silicon brick differentiator not only …

Advanced Functional Materials

The large‐pore interconnected channels in cryogels, allow convectional flow and rapid mass‐transport of solute constituents between the solution and cryogel polymer framework, as compared to slower, diffusionally‐controlled mass‐transport in small‐pore hydrogels. These features are applied to develop enzyme‐loaded polyacrylamide (pAAm) cryogels, and glucose oxidase (GOx)‐loaded pH‐responsive DNA‐based pAAm cryogels, revealing enhanced biocatalytic transformations, enhanced temporal stiffness changes, and mechanical bending functions, as compared to analog hydrogels. DNA‐based pAAm cryogel/hydrogel matrices, revealing pH‐switchable stiffness properties through reversible reconfiguration of DNA‐bridging units into i‐motif structures, are introduced. Enhanced switchable stiffness changes of DNA‐based pAAm cryogels, as compared to analog hydrogels, are demonstrated upon …

Advanced Functional Materials

It is envisioned that the efficient and stable blue OLED phosphors can be synthesized using Ir(III) complexes with electron‐deficient carbene cyclometalates. Therefore, three facially coordinated Ir(III) phosphors f‐ct7a‐ c bearing isomeric purinylidene chelates are obtained. They possess three, two, and one 4‐t‐butylphenyl cyclometalate together with the same number of N‐phenyl appendage on carbene fragments, and exhibit photoluminescence centered (λmax) at 452‒461 nm, fast radiative rate constants (kr) of 7.5–11.3 × 105 s‒1, and high quantum yield (PLQY) up to 80% in degassed toluene at RT. Representative OLED based on f‐ct7c gives maximum external quantum efficiency (EQEmax) of 26.6%, CIE(x,y) of 0.16, 0.15, and low roll‐off with EQE of 22.3% at 1000 cd m‒2. Furthermore, they can be utilized to sensitize a deep blue multiple resonance thermally activated delay fluorescence emitter (MR‐TADF …

Advanced Functional Materials

BiVO4 is one of the most promising candidates for photoelectrochemical water oxidation. However, the poor crystallinity and short hole diffusion length limit its charge separation. One bottleneck stems from the contradiction between high crystallinity and small particles via conventional furnace heating processes. This paper describes the design and fabrication of BiVO4 photoanodes via rapid thermal process (RTP), rather than furnace heating, to decouple the constraints between nucleation, crystallization, and growth processes of BiVO4. The higher heating ramp rate of RTP compared with furnace heating promotes the fast diffusion of reactant molecules, which elevates the nucleation rate above the particle growth rate of BiVO4, leading to small particles with high crystallinity. Moreover, the ultra‐high heating temperature makes it possible to crystallize the small BiVO4 particle within a short time. Thus, a high …

Advanced Functional Materials

The fabrication and integration of high‐quality structures of Yttrium Iron Garnet (YIG) is critical for magnonics. Films with excellent properties are obtained only on single crystal Gadolinium Gallium Garnet (GGG) substrates using high‐temperature processes. The subsequent realization of magnonic structures via lithography and etching is not straightforward as it requires a tight control of the edge roughness, to avoid magnon scattering, and planarization in case of multilayer devices. In this work a different approach is described based on local laser annealing of amorphous YIG films, avoiding the need for subjecting the entire sample to high thermal budgets and for physical etching. Starting from amorphous and paramagnetic YIG films grown by pulsed laser deposition at room temperature on GGG, a 405 nm laser is used for patterning arbitrary shaped ferrimagnetic structures by local crystallization. In thick films …

Advanced Functional Materials

Despite the critical role of hydrogels in material science and biotechnology, current methods for analyzing their formation lack real‐time monitoring and require complex sample preparation and instrumentation. In this work, an innovative methodology is introduced for the real‐time analysis of enzymatically catalyzed hydrogelation. Electrochemical impedance spectroscopy (EIS) coupled with interdigitated electrodes (IDEs) to sense and transduce the gelation reaction of model precursor carboxymethyl cellulose‐tyramine (CMC‐TA) conjugates that undergoes enzymatic cross‐linking by horseradish peroxidase (HRP) and hydrogen peroxide (H2O2). Real‐time monitoring involves single‐frequency analyses at 3 × 105 Hz, where the measured impedance consists solely of a resistive component, and the admittance equates to solution conductance. The gelation trajectories for all tested enzymatically cross‐linked …

Advanced Functional Materials

The groundbreaking discovery of unconventional ferroelectricity in HfO2 opens exciting prospects for next‐generation memory devices. However, the practical implementation, particularly its epitaxial stabilization and a clearer understanding of its intrinsic ferroelectricity has been a significant challenge. The study arouses the potential importance of atomic layer deposition (ALD) for mass production in modern industries, demonstrating its proficiency in achieving epitaxial growth of ferroelectric Hf0.5Zr0.5O2 (HZO) thin films on Yttria‐stabilized zirconia (YSZ) substrates. Moreover, with distinct ferroelectric switching currents, the work reveals the ferroelectric characteristics of epitaxial HZO thin films deposited through ALD on YSZ‐buffered Si substrates, which aligns well with CMOS technology. Overall, the results pave the way for a scalable synthesis system for ferroelectric HfO2‐based materials, hinting at a bright …

Advanced Functional Materials

The exploration of waste graphite from used lithium ion batteries (LIBs) and its derivatives for versatile applications is an efficient route to promote the environmental and eco‐friendly recycling of used LIBs. Sodium ion batteries (SIBs) are alternative candidates to LIBs mainly due to similar electrochemical mechanism of SIBs to LIBs and rich natural resource of Na. Herein, a holey waste graphite (hGw) with well‐defined porous structure is produced by the annealing of lithiated waste graphite (Li/Gw) from used LIBs under a flow gas of H2O and subsequent lithium leaching in DI water. Benefiting from the holey structure of hGw, holey graphene nanoplatelets (hGnw) with ultrahigh‐level edge‐grafted oxygen groups (≈37.8 at%) are synthesized by mechanical balling of hGw. As anode for SIBs, the hGnw present outstanding sodium ion storage properties with high initial Coulombic efficiency of 82.4%, high reversible …

Advanced Functional Materials

The development of flexible and stretchable devices is crucial for realizing future electronics. In particular, for dielectric layer, conventional inorganic materials are limited by their brittle nature, while organic materials suffer from a low dielectric constant. Here, a novel intrinsically photopatternable high‐k Parylene‐based thin film (Parylene‐OH) is fabricated via a chemical vapor deposition process based on the Gorham method, which provides pin‐hole free, conformal polymeric film on any type of surface. Parylene‐OH can be photo‐patterned by UV crosslinking without further lithography processes and dielectric constant of Parylene‐OH increases from 6.05 to 7.53 after crosslinking, without degrading other parameters, making it comparable to conventional high‐k dielectric, Al2O3. Flexible In─Ga─Zn─O (IGZO) thin‐film transistors (TFTs) with patterned dielectric layers can withstand higher strain owing to the …

Advanced Functional Materials

Electrochromic devices can facilitate the realization of a wide set of future applications, ranging from energy‐saving windows to smart wearables and stealth. Historically, tungsten oxides have been the most studied materials for electrochromism, albeit with bottlenecks like limited conductivity, high charge transport barrier, and low ion diffusivity. Here, inspired by the recent MXene materials, the study has engineered an electrochromic composite of MXene nanosheets (Ti3C2Tx) and W18O49 nanowires (NWs). A transparent conductive electrode is fabricated by co‐assembly of Ag and W18O49NWs, followed by depositing W18O49 NW/Ti3C2Tx layers for the fabrication of the electrochromic device. The incorporation of Ti3C2Tx nanosheets enhances the transport of electrons and ions within the electrochromic layer, leading to a significant improvement in the electrochromic performance. Noteworthily, the film …

Advanced Functional Materials

The fabrication of pressure sensitive adhesives (PSAs) using liquid crystal elastomers (LCEs), which are known for their excellent dissipation properties, is explored in this work. The adhesive properties of the PSAs are evaluated using the 180° peeling test at various conditions. The performance of the LCE adhesives is found to show significant rate and temperature dependence. When the adhesion energy is plotted against the rate, LCE shows an anomalously large power law exponent (n ≈ 1.17) compared to existing PSAs (n ≈ 0.1–0.6). The unusual rate sensitivity is hypothesized to originate from the synergy of soft elasticity and non‐linear viscoelasticity. The adhesive properties at various rates and temperatures are correlated to the results from dynamic mechanical analysis. Moreover, the large strain stiffening behavior of LCE under uniaxial tension reveals the distinctive advantages offered by LCE as …

Advanced Functional Materials

Most flexible ionic tactile sensors can hardly be used in deep sea due to their poor antiswelling and anticompression properties under high hydrostatic pressure. To achieve pressure and position sensing under high hydrostatic pressure, a self‐powered underwater tactile sensor made of a porous thermoplastic polyurethane (TPU) film is presented in this paper. The sensor works by generating an electric current due to the different moving velocities of ions in the porous film under pressing. Experimental results show that the magnitude of the generated current signal increases with the applied pressure, the contacting area, and ion concentration of the solution. The direction and magnitude of the current signal depend on the pressing position of the film. The signal magnitude decreased with the closer to the center of the film. The maximum pressure sensitivity and positioning resolution are 0.62 kPa−1 and 1.31 mm …

Advanced Functional Materials

Transition‐metal nanoparticles hold great promise as electrocatalysts for alkaline hydrogen evolution reaction (HER), however, addressing the simultaneous challenges of ensuring sufficient active sites, promoting favorable water dissociation, and optimizing binding energy toward hydrogen intermediates remains a formidable task. To overcome these hurdles, a novel gaseous hydrogen engineering strategy is proposed by in situ embedding cobalt nanoparticles within a samarium hydride matrix (Co/SmH2) via hydrogen‐induced disproportionation of SmCo5 particles for efficient alkaline HER. The as‐designed Co/SmH2 delivered an overpotential as low as 252 mV at 100 mA cm−2, surpassing the performance of pristine Co by 100 mV. Notably, this catalyst lasts remarkably long maintaining a durability at ≈500 mA cm−2 for 120 h. A combination of in situ Raman spectroscopy, in situ X‐ray absorption …

Advanced Functional Materials

Developing energy harvesting devices is crucial to mitigate the dependence on conventional and rigid batteries in wearable electronics, ensuring their autonomous operation. Nanogenerators offer a cost‐effective solution for enabling continuous operation of wearable electronics. Herein, this study proposes a novel strategy that combines freeze‐casting, freeze‐drying, and printing technologies to fabricate a fully printed triboelectric nanogenerator (TENG) based on polyvinylidene fluorid‐etrifluoroethylene P(VDF‐TrFE) porous aerogel. First, the effects of porosity and poling on the stretchability and energy harvesting capabilities of P(VDF‐TrFE) are investigated, conducting a comprehensive analysis of this porous structure's impact on the mechanical, ferroelectric, and triboelectric properties compared to solid P(VDF‐TrFE) films. The results demonstrate that structural modification of P(VDF‐TrFE) significantly …

Advanced Functional Materials

Direct‐current triboelectric nanogenerators (DC‐TENGs), which are used in smart electronics and energy storage, have attracted tremendous scientific interest owing to their rectification‐free and high energy utilization efficiency. In this study, the authors propose a new type of DC‐TENG that operates in the contact–separation mode with a unique adhesive–conductive interface for the first time. The results demonstrate that the TENG output increases with increasing interfacial adhesion strength; both the adhesive polymer and conductive tribomaterial are essential factors for the DC output. The proposed mechanism is based on mechanoion generation via covalent bond cleavage during material transfer and the charge leakage effect. Specifically, the DC‐TENG exhibits unique frequency‐decreasing and force‐enhancing output characteristics. It can directly drive LEDs or charge commercial capacitors. By integrating …