Magnetic-assisted alignment of nanofibers in a polymer nanocomposite for high-temperature capacitive energy storage applications.

Flexible polymer-based dielectrics with high energy storage characteristics over a wide temperature range are crucial for advanced electrical and electronic systems. However, the intrinsic low dielectric constant and drastically degraded breakdown strength hinder the development of polymer-based dielectrics at elevated temperatures. Here, we propose a magnetic-assisted approach for fabricating a polyethyleneimine (PEI)-based nanocomposite with precisely aligned nanofibers within the polymer matrix, and with Al2O3 deposition layers applied on the surface. The resulting polymer nanocomposite exhibits simultaneously increased dielectric constant and enhanced breakdown strength at high temperatures compared to pristine PEI. The enhanced dielectric constant is contributed by the depolarization effect of out-of-plane orientated nanofibers in composite films, while the surficial Al2O3 layers, with a wide bandgap, effectively prevent charge injection and transport at the electrode/dielectric interface. The optimally aligned composite films exhibit a significantly enhanced discharged energy density of 6.5 J cm-3 at 150 °C, with approximately 41% and 132% enhancement compared to random films and pristine PEI films, respectively. Additionally, a metalized multilayer polymer-based capacitor utilizing this composite film produces a high capacitance of 88 nF, while demonstrating excellent cyclability and flexibility at 150 °C. This work offers an effective strategy for developing polymer-based composite dielectrics with superior capacitive performance at elevated temperatures and demonstrates the potential of fabricating high-quality flexible capacitors.

Fully Printed Multilayer Ceramic Capacitors Based on High-k Perovskite Nanosheets.

Printing technology enables the integration of chemically exfoliated perovskite nanosheets into high-performance microcapacitors. Theoretically, the capacitance value can be further enhanced by designing and constructing multilayer structures without increasing the device size. Yet, issues such as interlayer penetration in multilayer heterojunctions constructed using inkjet printing technology further limit the realization of this potential. Herein, a series of multilayer configurations, including Ag/(Ca2NaNb4O13/Ag)n and graphene/(Ca2NaNb4O13/graphene)n (n = 1-3), are successfully inkjet-printed onto diverse rigid and flexible substrates through optimized ink formulations, inkjet printing parameters, thermal treatment conditions, and rational multilayer structural design using high-k perovskite nanosheets, graphene nanosheets and silver. The dielectric performance is optimized by fine-tuning the number of dielectric layers and modifying the electrode/dielectric interface. As a result, the graphene/(Ca2NaNb4O13/graphene)3 multilayer ceramic capacitors exhibit a remarkable capacitance density of 346 ± 12 nF cm-2 and a high dielectric constant of 193 ± 18. Additionally, these devices demonstrate moderate insulation properties, flexibility, thermal stability, and chemical sensitivity. This work shed light on the potential of multilayer structural design in additive manufacturing of high-performance 2D material-based ceramic capacitors.

High-Temperature Superlubricity in MoS2/Graphene van der Waals Heterostructures.

Achieving high-temperature superlubricity is essential for modern extreme tribosystems. Solid lubrication is the sole viable alternative due to the degradation of liquid ones but currently suffers from notable wear, instability, and high friction coefficient. Here, we report robust superlubricity in MoS2/graphene van der Waals heterostructures at high temperatures up to ∼850 K, achieved through localized heating to enable reliable friction testing. The ultralow friction of the MoS2/graphene heterostructure is found to be notably further reduced at elevated temperature and dominantly contributed by the MoS2 edge. The observation can be well described by a multi-contact model, wherein the thermally activated rupture of edge-contacts facilitates the sliding. Our results should be applicable to other van der Waals heterostructures and shed light on their applications for superlubricity at elevated temperature.

Direct Ink Writing of Low-Concentration MXene/Aramid Nanofiber Inks for Tunable Electromagnetic Shielding and Infrared Anticounterfeiting Applications.

MXene inks offer a promising avenue for the scalable production and customization of printing electronics. However, simultaneously achieving a low solid content and printability of MXene inks, as well as mechanical flexibility and environmental stability of printed objects, remains a challenge. In this study, we overcame these challenges by employing high-viscosity aramid nanofibers (ANFs) to optimize the rheology of low-concentration MXene inks. The abundant entangled networks and hydrogen bonds formed between MXene and ANF significantly increase the viscosity and yield stress up to 103 Pa·s and 200 Pa, respectively. This optimization allows the use of MXene/ANF (MA) inks at low concentrations in direct ink writing and other high-viscosity processing techniques. The printable MXene/ANF inks with a high conductivity of 883.5 S/cm were used to print shields with customized structures, achieving a tunable electromagnetic interference shielding effectiveness (EMI SE) in the 0.2-48.2 dB range. Furthermore, the MA inks exhibited adjustable infrared (IR) emissivity by changing the ANF ratio combined with printing design, demonstrating the application for infrared anticounterfeiting. Notably, the printed MXene/ANF objects possess outstanding mechanical flexibility and environmental stability, which are attributed to the reinforcement and protection of ANF. Therefore, these findings have significant practical implications as versatile MXene/ANF inks can be used for customizable, scalable, and cost-effective production of flexible printed electronics.

Bioinspired Dielectric Nanocomposites with High Charge-Discharge Efficiency Enabled by Superspreading-Induced Alignment of Nanosheets.

High-performance dielectric nanocomposites are promising candidates for thin-film dielectric capacitors for high-power pulse devices. However, the existing nanocomposites suffer from low charge-discharge efficiency (η), which results in severe generation and accumulation of Joule heat and subsequently the failure of the devices. In this work, we report nacre-inspired dielectric nanocomposites with outstanding η, which are enabled by superspreading shear flow-induced highly aligned two-dimensional (2D) nanofillers. Taking boron nitride nanosheets (BNNS) as an example, the highly aligned BNNS in the poly(vinylidene fluoride) (PVDF)-based nanocomposites contributes to a highly efficient Coulomb blockade effect for the injected charge carriers. Therefore, the bioinspired nanocomposites with highly aligned BNNS show significantly reduced dielectric loss (tan δ) (63.3%) and improved η (144.8%), compared to the ones with partially aligned nanosheets fabricated by solution casting. Furthermore, the optimized loading content of BNNS is as low as 3.6 wt %. The resulting nanocomposites exhibit reduced tan δ (0.018) and enhanced Eb (687 kV/mm), η (71%), and Ue (16.74 J/cm3). Our work demonstrates that the realization of high alignment of 2D nanofillers enabled by the superspreading shear flow is a promising way for the development of high-performance dielectric nanocomposites.

Machine Learning Aided Design and Optimization of Thermal Metamaterials.

Artificial Intelligence (AI) has advanced material research that were previously intractable, for example, the machine learning (ML) has been able to predict some unprecedented thermal properties. In this review, we first elucidate the methodologies underpinning discriminative and generative models, as well as the paradigm of optimization approaches. Then, we present a series of case studies showcasing the application of machine learning in thermal metamaterial design. Finally, we give a brief discussion on the challenges and opportunities in this fast developing field. In particular, this review provides: (1) Optimization of thermal metamaterials using optimization algorithms to achieve specific target properties. (2) Integration of discriminative models with optimization algorithms to enhance computational efficiency. (3) Generative models for the structural design and optimization of thermal metamaterials.

High Thermoelectric Performance Related to PVDF Ferroelectric Domains in P-Type Flexible PVDF-Bi0.5 Sb1.5 Te3 Composite Film.

There is increasing demand to power Internet of Things devices using ambient energy sources. Flexible, low-temperature, organic/inorganic thermoelectric devices are a breakthrough next-generation approach to meet this challenge. However, these systems suffer from poor performance and expensive processing preventing wide application of the technology. In this study, by combining a ferroelectric polymer (Polyvinylidene fluoride (PVDF, ß phase)) with p-type Bi0.5 Sb1.5 Te3 (BST) a thermoelectric composite film with maximum is produced power factor. Energy filter from ferroelectric-thermoelectric junction also leads to high Seebeck voltage ≈242 µV K-1 . For the first time, compelling evidence is provided that the dipole of a ferroelectric material is helping decouple electron transport related to carrier mobility and the Seebeck coefficient, to provide 5× or more improvement in thermoelectric power factor. The best composition, PVDF/BST film with BST 95 wt.% has a power factor of 712 µW•m-1  K-2 . A thermoelectric generator fabricated from a PVDF/BST film demonstrated Pmax T 12.02 µW and Pdensity 40.8 W m-2 under 50 K temperature difference. This development also provides a new insight into a physical technique, applicable to both flexible and non-flexible thermoelectrics, to obtain comprehensive thermoelectric performance.

Unraveling bilayer interfacial features and their effects in polar polymer nanocomposites.

Polymer nanocomposites with nanoparticles dispersed in polymer matrices have attracted extensive attention due to their significantly improved overall performance, in which the nanoparticle-polymer interface plays a key role. Understanding the structures and properties of the interfacial region, however, remains a major challenge for polymer nanocomposites. Here, we directly observe the presence of two interfacial polymer layers around a nanoparticle in polar polymers, i.e., an inner bound polar layer (~10 nm thick) with aligned dipoles and an outer polar layer (over 100 nm thick) with randomly orientated dipoles. Our results reveal that the impacts of the local nanoparticle surface potential and interparticle distance on molecular dipoles induce interfacial polymer layers with different polar molecular conformations from the bulk polymer. The bilayer interfacial features lead to an exceptional enhancement in polarity-related properties of polymer nanocomposites at ultralow nanoparticle loadings. By maximizing the contribution of inner bound polar layer via a nanolamination design, we achieve an ultrahigh dielectric energy storage density of 86 J/cm3, far superior to state-of-the-art polymers and nanocomposites.

Periodic fracture behaviour of nanomembranes.

Fracture control in membranes is highly desirable in nano-technology, but is a great challenge because of the 'multi-scale' complexity of fracture initiation and propagation. Here, we devise a method that can controllably direct fractures in stiff nanomembranes, realized by 90° peeling of the nanomembrane overlaid on a soft film, i.e., a stiff/soft bilayer, from a substrate underneath. The peeling allows the stiff membrane to be creased into a soft film periodically in the bending region and fractured along the unique bottom line of the crease, i.e, the fracture route is strictly straight and periodic. The facture period is tunable, because the surface perimeter of the creases is determined by the thickness and modulus of the stiff membranes. This is a new kind of fracture behavior of stiff membranes, which is unique to stiff/soft bilayers but universally exists in such systems, promising a new generation of technology for cutting nanomembranes.

Laser CVD Growth of Uniquely <010>-oriented ß-Ga2 O3 Films on Quartz Substrate with Ultrafast Photoelectric Response.

The oriented growth of ß-Ga2 O3 films has triggered extensive interest due to the remarkable and complex anisotropy found in the ß-Ga2 O3 bulks. Remarkable properties, including stronger solar-blind ultraviolet (SBUV) absorption, better mobility, and higher thermal conductivity, are usually observed along <010> direction as compared to other low-index axes. So far, <010>-oriented ß-Ga2 O3 film growth has been hindered by the lack of suitable substrates and higher surface energy of the (010) crystal plane. Herein, the first growth of uniquely <010>-oriented ß-Ga2 O3 films on quartz substrates by laser chemical vapor deposition (LCVD) are reported. By investigating the effects of deposition temperature (Tdep ) and O2 flow rate (RO2 ) on the growth of ß-Ga2 O3 films, it is found that the formation of <010> orientation is closely related to the higher stability of oxygen close-packed planes under O-rich condition. As a result, a grain size of up to ≈2 µm and a deposition rate of up to ≈ 40 µm h-1 are obtained. Metal-semiconductor-metal (MSM) type detector based on <010>-oriented ß-Ga2 O3 film exhibits ultra-fast response speed, 1-2 orders of magnitude higher than those of most detectors based on ß-Ga2 O3 films with other orientations.

Universal Behavior of Highly Confined Heat Flow in Semiconductor Nanosystems: From Nanomeshes to Metalattices.

Nanostructuring on length scales corresponding to phonon mean free paths provides control over heat flow in semiconductors and makes it possible to engineer their thermal properties. However, the influence of boundaries limits the validity of bulk models, while first-principles calculations are too computationally expensive to model real devices. Here we use extreme ultraviolet beams to study phonon transport dynamics in a 3D nanostructured silicon metalattice with deep nanoscale feature size and observe dramatically reduced thermal conductivity relative to bulk. To explain this behavior, we develop a predictive theory wherein thermal conduction separates into a geometric permeability component and an intrinsic viscous contribution, arising from a new and universal effect of nanoscale confinement on phonon flow. Using experiments and atomistic simulations, we show that our theory applies to a general set of highly confined silicon nanosystems, from metalattices, nanomeshes, porous nanowires, to nanowire networks, of great interest for next-generation energy-efficient devices.

Optimizing Electromagnetic Interference Shielding of Ultrathin Nanoheterostructure Textiles through Interfacial Engineering.

Strong electromagnetic wave reflection loss concomitant with second emission pollution limits the wide applications of electromagnetic interference (EMI) shielding textiles. Decoration of textiles by using various dielectric materials has been found efficient for the development of highly efficient EMI shielding textiles, but it is still a challenge to obtain EMI shielding composites with thin thickness. A route of interfacial engineering may offer a twist to overcome these obstacles. Here, we fabricated a Ni nanoparticle/SiC nanowhisker/carbon cloth nanoheterostructure, where SiC nanowhiskers were deposited by a simple manufacturing method, namely, laser chemical vapor deposition (LCVD), directly grown on carbon cloth. Through directly constructing a Ni/SiC interface, we find that the formation of Schottky contact can influence the interfacial polarization associated with the generation of dipole electric fields, leading to an enhancement of dielectric loss. A striking feature of this interfacial engineering strategy is able to enhance the absorption of the incident electromagnetic wave while suppressing the reflection. As a result, our Ni/SiC/carbon cloth exhibits an excellent EMI shielding effectiveness of 68.6 dB with a thickness of only 0.39 mm, as well as high flexibility and long-term duration stability benefited from the outstanding mechanical properties of SiC nanowiskers, showing potential for EMI shielding applications.

Dual-compressed photoacoustic single-pixel imaging.

Photoacoustic imaging, an acoustic imaging modality with potentially optical resolution in an optical turbid medium, has attracted great attention. However, the convergence of wavefront optimization and raster scanning in computational photoacoustic imaging leads to the challenge of fast mapping, especially for a spatial resolution approaching the acoustic deep-subwavelength regime. As a sparse sampling paradigm, compressive sensing has been applied in numerous fields to accelerate data acquisition without significant quality losses. In this work, we propose a dual-compressed approach for photoacoustic surface tomography that enables high-efficiency imaging with 3D spatial resolution unlimited by the acoustics in a turbid environment. The dual-compressed photoacoustic imaging with single-pixel detection, enabled by spatially optical modulation with synchronized temporally photoacoustic coding, allows decoding of the fine optical information from the modulated acoustic signal even when the variance of original photoacoustic signals is weak. We perform a proof-of-principle numerical demonstration of dual-compressed photoacoustic imaging, that resolves acoustic sub-acoustic-wavelength details with a significantly reduced number of measurements, revealing the potential for dynamic imaging. The dual-compressed concept, which transforms unobtrusive spatial difference into spatio-temporal detectable information, can be generalized to other imaging modalities to realize efficient, high-spatial-resolution imaging.

Enhanced Electromagnetic Shielding and Thermal Management Properties in MXene/Aramid Nanofiber Films Fabricated by Intermittent Filtration.

High-efficiency electromagnetic interference (EMI) shielding and heat dissipation synergy materials with flexible, robust, and environmental stability are urgently demanded in next-generation integration electronic devices. In this work, we report the lamellar MXene/Aramid nanofiber (ANF) composite films, which establish a nacre-like structure for EMI shielding and heat dissipation by using the intermittent filtration strategy. The MXene/ANF composite film filled with 50 wt % MXene demonstrates enhanced mechanical properties with a strength of 230.5 MPa, an elongation at break of 6.2%, and a toughness of 11.8 MJ·m3 (50 wt % MXene). These remarkable properties are attributed to the hydrogen bonding and highly oriented structure. Furthermore, due to the formation of the MXene conductive network, the MXene/ANF composite film shows an outstanding conductivity of 624.6 S/cm, an EMI shielding effectiveness (EMI SE) of 44.0 dB, and a superior specific SE value (SSE/t) of 18847.6 dB·cm2/g, which is better than the vacuum filtration film. Moreover, the MXene/ANF composite film also shows a great thermal conductivity of 0.43 W/m·K. The multifunctional MXene/ANF composite films with high-performance EMI shielding, heat dissipation, and joule heating show great potential in the field of aerospace, military, microelectronics, microcircuit, and smart wearable electronics.

3D MXene-Based Flexible Network for High-Performance Pressure Sensor with a Wide Temperature Range.

With the increasing popularity of smart wearable devices, flexible pressure sensors are highly desired in various complex application scenarios. A great challenge for existing flexible pressure sensors is to maintain high sensitivity over a wide temperature range, which is critical for their applications in harsh environments. Herein, a flexible piezoresistive sensor made of polyetherimide (PEI) fibrous network evenly covered with MXene nanosheets is reported to construct conductive pathways, showing ultrahigh sensitivity over a wide temperature range from -5 °C (sensitivity of 80 kPa-1 ) to 150 °C (20 kPa-1 ), low detection limit of 9 Pa, fast response time of 163 ms, outstanding durability over 10 000 cycles at room temperature, 2000 cycles at 100 °C and 500 cycles at -5 °C. The pressure sensor can monitor various human activities in real-time, apply to human-machine interaction, and measure pressure distribution. It also can sensitively respond to external mechanical stimuli at 150 °C and extremely low temperature (in liquid nitrogen). Moreover, the fibrous network exhibits an excellent Joule heating performance, which can reach 78 °C at an applied voltage of 12 V. Thus, the piezoresistive sensor has considerable potential for wearable garments and personal heating applications in harsh temperature conditions.

Scalable Assembly of High-Quality Graphene Films via Electrostatic-Repulsion Aligning.

Assembling pristine graphene into freestanding films featuring high electrical conductivity, superior flexibility, and robust mechanical strength aims at meeting the all-around high criteria of new-generation electronics. However, voids and defects produced in the macroscopic assembly process of graphene nanosheets severely degrade the performance of graphene films, and mechanical brittleness often limits their applications in wide scenarios. To address such challenges, an electrostatic-repulsion aligning strategy is demonstrated to produce highly conductive, ultraflexible, and multifunctional graphene films. Typically, the high electronegativity of titania nanosheets (TiNS) induces the aligning of negatively charged graphene nanosheets via electrostatic repulsion in the film assembly. The resultant graphene films show fine microstructure, enhanced mechanical properties, and improved electrical conductivity up to 1.285 × 105 S m-1 . Moreover, the graphene films can withstand 5000 repeated folding without structural damage and electrical resistance fluctuation. These comprehensive improved properties, combined with the facile synthesis method and scalable production, make these graphene films a promising platform for electromagnetic interference (EMI) shielding and thermal-management applications in smart and wearable electronics.

Bridging sheet size controls densification of MXene films for robust electromagnetic interference shielding.

Numerous voids among the incompact layer-structure of MXene films result in their low ambient stability and poor innate conductivity for electromagnetic interference (EMI) shielding. Herein, we report a bridging-sheet-size-controlled densification process of MXene films by applying graphene oxide (GO) as a bridging agent. Specifically, the sheet size of GO is tailored to quantify a negative correlation of sheet size with densification for directing the preparation of most compact MXene-GO films. Benefiting from the shortest electron-transport-distance in the most compact structure, the conductivity of the MXene-GO film achieves 1.7 times (∼1.6 × 105 S/m) that of MXene film. The EMI shielding performance (5.2 × 106 dB/m) reaches the record-value among reported MXene films at 10 µm-scale thickness. Moreover, the compact structure boosts the ambient stability of MXene-GO films where the conductivity and EMI shielding performance remain 88.7% and 90.0% after 15 days, respectively. The findings rationale the structure-activity relationship of compact MXene films for flexible electronics.

AWI-Assembled TPU-BNNS Composite Films with High In-Plane Thermal Conductivity for Thermal Management of Flexible Electronics.

Thermal management of flexible/stretchable electronics has been a crucial issue. Mass supernumerary thermal heat is created in the repetitive course of deformation because of the large nanocontact resistance between electric conductive fillers, as well as the interfacial resistance between fillers and the polymer matrix. Here, we report a stretchable thermoplastic polyurethane (TPU)-boron nitride nanosheet (BNNS) composite film with a high in-plane thermal conductivity based on an air/water interfacial (AWI) assembly method. In addition to rigid devices, it was capable for thermal management of flexible electronics. During more than 2000 cycles of the bending-releasing process, the average saturated surface temperature of the flexible conductor covered with composite film with 30 wt % BNNSs was approximately 40.8 ± 1 °C (10.5 °C lower than that with pure TPU). Moreover, the thermal dissipating property of the composite under stretching was measured. All the results prove that this TPU-BNNS composite film is a candidate for thermal management of next-generation flexible/stretchable electronics with high power density.

Concurrent Enhancement of Breakdown Strength and Dielectric Constant in Poly(vinylidene Fluoride) Film with High Energy Storage Density by Ultraviolet Irradiation.

Polyvinylidene fluoride (PVDF) film with high energy storage density has exhibited great potential for applications in modern electronics, particle accelerators, and pulsed lasers. Typically, dielectric/ferroelectric properties of PVDF film have been tailored for energy storage through stretching, annealing, and defect modification. Here, PVDF films were prepared by the solution casting method followed by an ultraviolet (UV) irradiation process, with special emphasis on how such treatment influences their dielectric and energy storage properties. Upon UV irradiation, the dielectric constant and breakdown strength of the PVDF film were enhanced simultaneously. A high energy density of 18.6 J/cm3, along with a charge-discharge efficiency of 81% at 600 MV/m, was achieved in PVDF after exposure to UV for 15 min. This work may provide a simple and yet effective route to enhance energy storage density of PVDF-based polymers.