Multilayer Lead‐Free Ceramic Capacitors with Ultrahigh Energy Density and Efficiency

The utilization of antiferroelectric (AFE) materials is thought to be an effective approach to enhance the energy density of dielectric capacitors. However, the high energy dissipation and inferior reliability that are associated with the antiferroelectric–ferroelectric phase transition are the main issues that restrict the applications of antiferroelectric ceramics. Here, simultaneously achieving high energy density and efficiency in a dielectric ceramic is proposed by combining antiferroelectric and relaxor features. Based on this concept, a lead‐free dielectric (Na_0.5Bi_0.5)TiO₃‐x(Sr_0.7Bi_0.2)TiO₃ (NBT‐xSBT) system is investigated and the corresponding multilayer ceramic capacitors (MLCCs) are fabricated. A record‐high energy density of 9.5 J cm^?3, together with a high energy efficiency of 92%, is achieved in NBT‐0.45SBT multilayer ceramic capacitors, which consist of ten dielectric layers with the single‐layer thickness of 20 µm and the internal electrode area of 6.25 mm². Furthermore, the newly developed capacitor exhibits a wide temperature usage range of ‐60 to 120 °C, with an energy‐density variation of less than 10%, and satisfactory cycling reliability, with degradation of less than 8% over 10⁶ cycles. These characteristics demonstrate that the NBT‐0.45SBT multilayer ceramic is a promising candidate for high‐power energy storage applications.     

Controllable Synthesis of Atomically Thin Type‐II Weyl Semimetal WTe2 Nanosheets: An Advanced Electrode Material for All‐Solid‐State Flexible Supercapacitors

Compared with 2D S‐based and Se‐based transition metal dichalcogenides (TMDs), Te‐based TMDs display much better electrical conductivities, which will be beneficial to enhance the capacitances in supercapacitors. However, to date, the reports about the applications of Te‐based TMDs in supercapacitors are quite rare. Herein, the first supercapacitor example of the Te‐based TMD is reported: the type‐II Weyl semimetal 1Td WTe₂. It is demonstrated that single crystals of 1Td WTe₂ can be exfoliated into the nanosheets with 2–7 layers by liquid‐phase exfoliation, which are assembled into air‐stable films and further all‐solid‐state flexible supercapacitors. The resulting supercapacitors deliver a mass capacitance of 221 F g^?1 and a stack capacitance of 74 F cm^?3. Furthermore, they also show excellent volumetric energy and power densities of 0.01 Wh cm^?3 and 83.6 W cm^?3, respectively, superior to the commercial 4V/500 µAh Li thin‐film battery and the commercial 3V/300 µAh Al electrolytic capacitor, in association with outstanding mechanical flexibility and superior cycling stability (capacitance retention of ≈91% after 5500 cycles). These results indicate that the 1Td WTe₂ nanosheet is a promising flexible electrode material for high‐performance energy storage devices.     

Fabry–Pérot Oscillation and Room Temperature Lasing in Perovskite Cube‐Corner Pyramid Cavities

Recently, organometal halide perovskite‐based optoelectronics, particularly lasers, have attracted intensive attentions because of its outstanding spectral coherence, low threshold, and wideband tunability. In this work, high‐quality CH₃NH₃PbBr₃ single crystals with a unique shape of cube‐corner pyramids are synthesized on mica substrates using chemical vapor deposition method. These micropyramids naturally form cube‐corner cavities, which are eminent candidates for small‐sized resonators and retroreflectors. The as‐grown perovskites show strong emission ≈530 nm in the vertical direction at room temperature. A special Fabry–Pérot (F–P) mode is employed to interpret the light confinement in the cavity. Lasing from the perovskite pyramids is observed from 80 to 200 K, with threshold ranging from ≈92 µJ cm^?2 to 2.2 mJ cm^?2, yielding a characteristic temperature of T₀ = 35 K. By coating a thin layer of Ag film, the threshold is reduced from ≈92 to 26 µJ cm^?2, which is accompanied by room temperature lasing with a threshold of ≈75 µJ cm^?2. This work advocates the prospect of shape‐engineered perovskite crystals toward developing micro‐sized optoelectronic devices and potentially investigating light–matter coupling in quantum optics.     

Vertical 1T‐TaS2 Synthesis on Nanoporous Gold for High‐Performance Electrocatalytic Applications

2D metallic TaS₂ is acting as an ideal platform for exploring fundamental physical issues (superconductivity, charge‐density wave, etc.) and for engineering novel applications in energy‐related fields. The batch synthesis of high‐quality TaS₂ nanosheets with a specific phase is crucial for such issues. Herein, the successful synthesis of novel vertically oriented 1T‐TaS₂ nanosheets on nanoporous gold substrates is reported, via a facile chemical vapor deposition route. By virtue of the abundant edge sites and excellent electrical transport property, such vertical 1T‐TaS₂ is employed as high‐efficiency electrocatalysts in the hydrogen evolution reaction, featured with rather low Tafel slopes ≈67–82 mV dec^?1 and an ultrahigh exchange current density ≈67.61 µA cm^?2. The influence of phase states of 1T‐ and 2H‐TaS₂ on the catalytic activity is also discussed with the combination of density functional theory calculations. This work hereby provides fundamental insights into the controllable syntheses and electrocatalytic applications of vertical 1T‐TaS₂ nanosheets achieved through the substrate engineering.     

MXene‐Derived Ferroelectric Crystals

This study demonstrates the first synthesis of MXene‐derived ferroelectric crystals. Specifically, high‐aspect‐ratio potassium niobate (KNbO₃) ferroelectric crystals is successfully synthesized using 2D Nb₂C, MXene, and potassium hydroxide (KOH) as the niobium and potassium source, respectively. Material analysis confirms that a KNbO₃ orthorhombic phase with Amm2 symmetry is obtained. Additionally, ferroelectricity in KNbO₃ is confirmed using standard ferroelectric, dielectric, and piezoresponse force microscopy measurements. The KNbO₃ crystals exhibit a saturated polarization of ≈21 µC cm^?2, a remnant polarization of ≈17 µC cm^?2, and a coercive field of ≈50 kV cm^?1. This discovery illustrates that the 2D nature of MXenes can be exploited to grow ferroelectric crystals.     

Highly Conductive Ti3C2Tx MXene Hybrid Fibers for Flexible and Elastic Fiber‐Shaped Supercapacitors

Fiber‐shaped supercapacitors (FSCs) are promising energy storage solutions for powering miniaturized or wearable electronics. However, the scalable fabrication of fiber electrodes with high electrical conductivity and excellent energy storage performance for use in FSCs remains a challenge. Here, an easily scalable one‐step wet‐spinning approach is reported to fabricate highly conductive fibers using hybrid formulations of Ti₃C₂T_x MXene nanosheets and poly(3,4‐ethylenedioxythiophene):polystyrene sulfonate. This approach produces fibers with a record conductivity of ≈1489 S cm^?1, which is about five times higher than other reported Ti₃C₂T_x MXene‐based fibers (up to ≈290 S cm^?1). The hybrid fiber at ≈70 wt% MXene shows a high volumetric capacitance (≈614.5 F cm^?3 at 5 mV s^?1) and an excellent rate performance (≈375.2 F cm^?3 at 1000 mV s^?1). When assembled into a free‐standing FSC, the energy and power densities of the device reach ≈7.13 Wh cm^?3 and ≈8249 mW cm^?3, respectively. The excellent strength and flexibility of the hybrid fibers allow them to be wrapped on a silicone elastomer fiber to achieve an elastic FSC with 96% capacitance retention when cyclically stretched to 100% strain. This work demonstrates the potential of MXene‐based fiber electrodes and their scalable production for fiber‐based energy storage applications.     

Interlayer Hydrogen‐Bonded Metal Porphyrin Frameworks/MXene Hybrid Film with High Capacitance for Flexible All‐Solid‐State Supercapacitors

2D metal‐porphyrin frameworks (MPFs) are attractive for advanced energy storage devices. However, the inferior conductivity and low structural stability of MPFs seriously limit their application as flexible free‐standing electrodes with high performance. Here, for the first time, an interlayer hydrogen‐bonded MXene/MPFs film is proposed to overcome these disadvantages by intercalation of highly conductive MXene nanosheets into MPFs nanosheets via a vacuum‐assisted filtration technology. The alternant insertion of MXene and MPFs affords 3D interconnected “MPFs‐to‐MXene‐to‐MPFs” conductive networks to accelerate the ionic/electronic transport rates. Meanwhile, the interlayer hydrogen bonds (F···H? O and O···H? O) contribute a high chemical stability due to a favorable tolerance to volume change caused by phase separation and structural collapse during the charge/discharge process. The synergistic effect makes MXene/MPFs film deliver a capacitance of 326.1 F g^?1 at 0.1 A g^?1, 1.64 F cm^?2 at 1 mA cm^?2, 694.2 F cm^?3 at 1 mA cm^?3 and a durability of about 30 000 cycles. The flexible symmetric supercapacitor shows an areal capacitance of 408 mF cm^?2, areal energy density of 20.4 µW h cm^?2, and capacitance retention of 95.9% after 7000 cycles. This work paves an avenue for the further exploration of 2D MOFs in flexible energy storage devices.     

A 1300 mm2 Ultrahigh‐Performance Digital Imaging Assembly using High‐Quality Perovskite Single Crystals

By fine‐tuning the crystal nucleation and growth process, a low‐temperature‐gradient crystallization method is developed to fabricate high‐quality perovskite CH₃NH₃PbBr₃ single crystals with high carrier mobility of 81 ± 5 cm² V^?1 s^?1 (>3 times larger than their thin film counterpart), long carrier lifetime of 899 ± 127 ns (>5 times larger than their thin film counterpart), and ultralow trap state density of 6.2 ± 2.7 × 10⁹ cm^?3 (even four orders of magnitude lower than that of single‐crystalline silicon wafers). In fact, they are better than perovskite single crystals reported in prior work: their application in photosensors gives superior detectivity as high as 6 × 10¹³ Jones, ≈10–100 times better than commercial sensors made of silicon and InGaAs. Meanwhile, the response speed is as fast as 40 µs, ≈3 orders of magnitude faster than their thin film devices. A large‐area (≈1300 mm²) imaging assembly composed of a 729‐pixel sensor array is further designed and constructed, showing excellent imaging capability thanks to its superior quality and uniformity. This opens a new possibility to use the high‐quality perovskite single‐crystal‐based devices for more advanced imaging sensors.     

Vertically Aligned Niobium Nanowire Arrays for Fast‐Charging Micro‐Supercapacitors

Planar micro‐supercapacitors are attractive for system on chip technologies and surface mount devices due to their large areal capacitance and energy/power density compared to the traditional oxide‐based capacitors. In the present work, a novel material, niobium nanowires, in form of vertically aligned electrodes for application in high performance planar micro‐supercapacitors is introduced. Specific capacitance of up to 1 kF m^?2 (100 mF cm^?2) with peak energy and power density of 2 kJ m^?2 (6.2 MJ m^?3 or 1.7 mWh cm^?3) and 150 kW m^?2 (480 MW m^?3 or 480 W cm^?3), respectively, is achieved. This remarkable power density, originating from the extremely low equivalent series resistance value of 0.27 Ω (2.49 µΩ m² or 24.9 mΩ cm²) and large specific capacitance, is among the highest for planar micro‐supercapacitors electrodes made of nanomaterials.     

Co@Co3O4 Core–Shell Three‐Dimensional Nano‐Network for High‐Performance Electrochemical Energy Storage

An alternative routine is presented by constructing a novel architecture, conductive metal/transition oxide (Co@Co₃O₄) core–shell three‐dimensional nano‐network (3DN) by surface oxidating Co 3DN in situ, for high‐performance electrochemical capacitors. It is found that the Co@Co₃O₄ core–shell 3DN consists of petal‐like nanosheets with thickness of <10 nm interconnected forming a 3D porous nanostructure, which preserves the original morphology of Co 3DN well. X‐ray photoelectron spectroscopy by polishing the specimen layer by layer reveals that the Co@Co₃O₄ nano‐network is core–shell‐like structure. In the application of electrochemical capacitors, the electrodes exhibit a high specific capacitance of 1049 F g^?1 at scan rate of 2 mV/s with capacitance retention of ～52.05% (546 F g^?1 at scan rate of 100 mV) and relative high areal mass density of 850 F g^?1 at areal mass of 3.52 mg/cm². It is believed that the good electrochemical behaviors mainly originate from its extremely high specific surface area and underneath core‐Co “conductive network”. The high specific surface area enables more electroactive sites for efficient Faradaic redox reactions and thus enhances ion and electron diffusion. The underneath core‐Co “conductive network” enables an ultrafast electron transport.     

Black Phosphorus Revisited: A Missing Metal‐Free Elemental Photocatalyst for Visible Light Hydrogen Evolution

Metal‐free elemental photocatalysts for hydrogen (H₂) evolution are more advantageous than the traditional metal‐based inorganic photocatalysts since the nonmetal elements are generally cheaper, more earth‐abundant, and environmentally friendly. Black phosphorus (BP) has been attracting increasing attention in recent years based on its anisotropic 2D layered structure with tunable bandgap in the range of 0.3–2.0 eV; however, the application of BP for photocatalytic H₂ evolution has been scarcely reported experimentally although being theoretically predicted. Herein, for the first time, the visible light photocatalytic H₂ evolution of BP nanosheets prepared via a facile solid‐state mechanochemical method by ball‐milling bulk BP is reported. Without using any noble metal cocatalyst, the visible light photocatalytic hydrogen evolution rate of BP nanosheets reaches 512 µmol h^?1 g^?1, which is ≈18 times higher than that of the bulk BP, and is comparable or even higher than that of graphitic carbon nitrides (g‐C₃N₄).     

Large‐Scale Growth and Field‐Effect Transistors Electrical Engineering of Atomic‐Layer SnS2

2D layers of metal dichalcogenides are of considerable interest for high‐performance electronic devices for their unique electronic properties and atomically thin geometry. 2D SnS₂ nanosheets with a bandgap of ≈2.6 eV have been attracting intensive attention as one potential candidate for modern electrocatalysis, electronic, and/or optoelectronic fields. However, the controllable growth of large‐size and high‐quality SnS₂ atomic layers still remains a challenge. Herein, a salt‐assisted chemical vapor deposition method is provided to synthesize atomic‐layer SnS₂ with a large crystal size up to 410 µm and good uniformity. Particularly, the as‐fabricated SnS₂ nanosheet‐based field‐effect transistors (FETs) show high mobility (2.58 cm² V^?1 s^?1) and high on/off ratio (≈10⁸), which is superior to other reported SnS₂‐based FETs. Additionally, the effects of temperature on the electrical properties are systematically investigated. It is shown that the scattering mechanism transforms from charged impurities scattering to electron–phonon scattering with the temperature. Moreover, SnS₂ can serve as an ideal material for energy storage and catalyst support. The high performance together with controllable growth of SnS₂ endow it with great potential for future applications in electrocatalysis, electronics, and optoelectronics.     

Direct Laser‐Patterned Micro‐Supercapacitors from Paintable MoS2 Films

Micrometer‐sized electrochemical capacitors have recently attracted attention due to their possible applications in micro‐electronic devices. Here, a new approach to large‐scale fabrication of high‐capacitance, two‐dimensional MoS₂ film‐based micro‐supercapacitors is demonstrated via simple and low‐cost spray painting of MoS₂ nanosheets on Si/SiO₂ chip and subsequent laser patterning. The obtained micro‐supercapacitors are well defined by ten interdigitated electrodes (five electrodes per polarity) with 4.5 mm length, 820 μm wide for each electrode, 200 μm spacing between two electrodes and the thickness of electrode is ～0.45 μm. The optimum MoS₂‐based micro‐supercapacitor exhibits excellent electrochemical performance for energy storage with aqueous electrolytes, with a high area capacitance of 8 mF cm^?2 (volumetric capacitance of 178 F cm^?3) and excellent cyclic performance, superior to reported graphene‐based micro‐supercapacitors. This strategy could provide a good opportunity to develop various micro‐/nanosized energy storage devices to satisfy the requirements of portable, flexible, and transparent micro‐electronic devices.     

Dense PLZT films grown on nickel substrates by PVP-modified sol–gel method

We have successfully grown ferroelectric Pb_0.92La_0.08Zr_0.52Ti_0.48O₃ (PLZT) films on base metal foils by chemical solution deposition using sol–gel solutions containing polyvinylpyrrolidone. Under zero-bias field, we measured a dielectric constant of ≈820 and dielectric loss of ≈0.06 at room temperature, and a dielectric constant of ≈1250 and dielectric loss of ≈0.03 at 150 °C. In addition, leakage current density of ≈1.5 × 10^?8 A/cm², remanent polarization of ≈11.2 μC/cm², and coercive field of ≈40.6 kV/cm were measured at room temperature on a ≈3-μm-thick PLZT film grown on LaNiO₃-buffered nickel substrate. Finally, energy density ≈25 J/cm³ was measured from the P–E hysteresis loop at an applied field of 2 × 10⁶ V/cm.     

Room‐Temperature Solution‐Synthesized p‐Type Copper(I) Iodide Semiconductors for Transparent Thin‐Film Transistors and Complementary Electronics

Here, room‐temperature solution‐processed inorganic p‐type copper iodide (CuI) thin‐film transistors (TFTs) are reported for the first time. The spin‐coated 5 nm thick CuI film has average hole mobility (µ_FE) of 0.44 cm² V^?1 s^?1 and on/off current ratio of 5 × 10². Furthermore, µ_FE increases to 1.93 cm² V^?1 s^?1 and operating voltage significantly reduces from 60 to 5 V by using a high permittivity ZrO₂ dielectric layer replacing traditional SiO₂. Transparent complementary inverters composed of p‐type CuI and n‐type indium gallium zinc oxide TFTs are demonstrated with clear inverting characteristics and voltage gain over 4. These outcomes provide effective approaches for solution‐processed inorganic p‐type semiconductor inks and related electronics.     

Strong Surface‐Bound Sulfur in Carbon Nanotube Bridged Hierarchical Mo2C‐Based MXene Nanosheets for Lithium–Sulfur Batteries

In this work, hydroxyl‐functionalized Mo₂C‐based MXene nanosheets are synthesized by facilely removing the Sn layer of Mo₂SnC. The hydroxyl‐functionalized surface of Mo₂C suppresses the shuttle effect of lithium polysulfides (LiPSs) through strong interaction between Mo atoms on the MXenes surface and LiPSs. Carbon nanotubes (CNTs) are further introduced into Mo₂C phase to enlarge the specific surface area of the composite, improve its electronic conductivity, and alleviate the volume change during discharging/charging. The strong surface‐bound sulfur in the hierarchical Mo₂C‐CNTs host can lead to a superior electrochemical performance in lithium–sulfur batteries. A large reversible capacity of ≈925 mAh g ^{? 1} is observed after 250 cycles at a current density of 0.1 C (1 C = 1675 mAh g^?1) with good rate capability. Notably, the electrodes with high loading amounts of sulfur can also deliver good electrochemical performances, i.e., initial reversible capacities of ≈1314 mAh g^?1 (2.4 mAh cm^?2), ≈1068 mAh g^?1 (3.7 mAh cm^?2), and ≈959 mAh g^?1 (5.3 mAh cm^?2) at various areal loading amounts of sulfur (1.8, 3.5, and 5.6 mg cm^?2) are also observed, respectively.     

Ultrafast Growth of High‐Quality Monolayer WSe2 on Au

The ultrafast growth of high‐quality uniform monolayer WSe₂ is reported with a growth rate of ≈26 µm s^?1 by chemical vapor deposition on reusable Au substrate, which is ≈2–3 orders of magnitude faster than those of most 2D transition metal dichalcogenides grown on nonmetal substrates. Such ultrafast growth allows for the fabrication of millimeter‐size single‐crystal WSe₂ domains in ≈30 s and large‐area continuous films in ≈60 s. Importantly, the ultrafast grown WSe₂ shows excellent crystal quality and extraordinary electrical performance comparable to those of the mechanically exfoliated samples, with a high mobility up to ≈143 cm² V^?1 s^?1 and ON/OFF ratio up to 9 × 10⁶ at room temperature. Density functional theory calculations reveal that the ultrafast growth of WSe₂ is due to the small energy barriers and exothermic characteristic for the diffusion and attachment of W and Se on the edges of WSe₂ on Au substrate.     

Microtubular Fuel Cell with Ultrahigh Power Output per Footprint

A novel realization of microtubular direct methanol fuel cells (µ DMFC) with ultrahigh power output is reported by using “rolled‐up” nanotechnology. The microtube (Pt‐RuO₂‐RUMT) is prepared by rolling up Ru₂O layers coated with magnetron‐sputtered Pt nanoparticles (cat‐NPs). The µ DMFC is fabricated by embedding the tube in a fluidic cell. The footprint of per tube is as small as 1.5 × 10^?4 cm². A power density of ≈257 mW cm^?2 is obtained, which is three orders of magnitude higher than the present microsized DFMCs. Atomic layer deposition technique is applied to alleviate the methanol crossover as well as improve stability of the tube, sustaining electrolyte flow for days. A laminar flow driven mechanism is proposed, and the kinetics of the fuel oxidation depends on a linear‐diffusion‐controlled process. The electrocatalytic performance on anode and cathode is studied by scanning both sides of the tube wall as an ex situ working electrode, respectively. This prototype µ DFMC is extremely interesting for integration with micro‐ and nanoelectronics systems.     

A tunable B-site doping SBT-BNT-SMN ceramic composite with high recoverable energy density and temperature stability

We synthesize a group of three-phase ferroelectric ceramics 0.35(Sr_0.7Bi_0.2) TiO₃–0.65(Bi_0.5Na_0.5)TiO₃–xSr(Mg_1/3Nb_2/3)O₃ (BST–BNT–xSMN) using conventional solid-phase sintering method. When tunning the volume of SMN to 0.01, the ceramic sheet shows homogeneous microcrystal grains and highly dense crystal morphology, which favors a reductive dielectric permittivity (ε_r) of 2250 and loss of 0.05. Under a high electric field of 100 kV cm^?1, the BST–BNT-_0.01SMN sample achieves a slender polarization versus electrical field (P–E) loop with saturation and residual polarization of 37.1 µC cm^?2 and 3.0 µC cm^?2, respectively, corresponding to a high energy density of 1.32 J cm^?3 and a large η of 81%. Strikingly, the BST–BNT–xSMN ceramics show the excellent temperature stability below 100 °C, which facilitates energy storage in relaxed ferroelectric ceramics and provides an efficient method for obtaining pulsed power capacitors with excellent energy-recoverable characteristics and high efficiency in BNT-based ceramics.

Graphical abstract

The three-phase ferroelectric ceramics 0.35(Sr_0.7Bi_0.2)TiO_3- 0.65(Bi_0.5Na_0.5)TiO_3-xSr(Mg_1/3Nb_2/3)O₃ (BST- BNT- xSMN) possesses a slender polarization versus electrical field loop with saturation and residual polarization of 37.1 µC cm^-2 and 3.0 µC cm^-2 respectively at 100 kV cm^-1, which corresponds to a high energy density of 1.32 J cm^-3 and a large η of 81%.

     

Carbon‐MEMS‐Based Alternating Stacked MoS2@rGO‐CNT Micro‐Supercapacitor with High Capacitance and Energy Density

A novel process to fabricate a carbon‐microelectromechanical‐system‐based alternating stacked MoS₂@rGO–carbon‐nanotube (CNT) micro‐supercapacitor (MSC) is reported. The MSC is fabricated by successively repeated spin‐coating of MoS₂@rGO/photoresist and CNT/photoresist composites twice, followed by photoetching, developing, and pyrolysis. MoS₂@rGO and CNTs are embedded in the carbon microelectrodes, which cooperatively enhance the performance of the MSC. The fabricated MSC exhibits a high areal capacitance of 13.7 mF cm^?2 and an energy density of 1.9 µWh cm^?2 (5.6 mWh cm^?3), which exceed many reported carbon‐ and MoS₂‐based MSCs. The MSC also retains 68% of capacitance at a current density of 2 mA cm^?2 (5.9 A cm^?3) and an outstanding cycling performance (96.6% after 10 000 cycles, at a scan rate of 1 V s^?1). Compared with other MSCs, the MSC in this study is fabricated by a low‐cost and facile process, and it achieves an excellent and stable electrochemical performance. This approach could be highly promising for applications in integration of micro/nanostructures into microdevices/systems.