Implementation of Low‐Power Electronic Devices Using Solution‐Processed Tantalum Pentoxide Dielectric

The development of solution‐processed field effect transistors (FETs) based on organic and hybrid materials over the past two decades has demonstrated the incredible potential in these technologies. However, solution processed FETs generally require impracticably high voltages to switch on and off, which precludes their application in low‐power devices and prevent their integration with standard logic circuitry. Here, a universal and environmentally benign solution‐processing method for the preparation of Ta₂O₅, HfO₂ and ZrO₂ amorphous dielectric thin films is demonstrated. High mobility CdS FETs are fabricated on such high‐κ dielectric substrates entirely via solution‐processing. The highest mobility, 2.97 cm² V^?1 s^?1 is achieved in the device with Ta₂O₅ dielectric with a low threshold voltage of 1.00 V, which is higher than the mobility of the reference CdS FET with SiO₂ dielectric with an order of magnitude decrease in threshold voltage as well. Because these FETs can be operated at less than 5 V, they may potentially be integrated with existing logic and display circuitry without significant signal amplification. This report demonstrates high‐mobility FETs using solution‐processed Ta₂O₅ dielectrics with drastically reduced power consumption; ≈95% reduction compared to that of the device with a conventional SiO₂ gate dielectric.     

In‐Plane Assembled Orthorhombic Nb2O5 Nanorod Films with High‐Rate Li+ Intercalation for High‐Performance Flexible Li‐Ion Capacitors

Organic hybrid supercapacitors that consist of a battery electrode and a capacitive electrode show greatly improved energy density, but their power density is generally limited by the poor rate capability of battery‐type electrodes. In addition, flexible organic hybrid supercapacitors are rarely reported. To address the above issues, herein an in‐plane assembled orthorhombic Nb₂O₅ nanorod film anode with high‐rate Li⁺ intercalation to develop a flexible Li‐ion hybrid capacitor (LIC) is reported. The binder‐/additive‐free film exhibits excellent rate capability (≈73% capacity retention with the rate increased from 0.5 to 20 C) and good cycling stability (>2500 times). Kinetic analyses reveal that the high rate performance is mainly attributed to the excellent in‐plane assembly of interconnected single‐crystalline Nb₂O₅ nanorods on the current collector, ensuring fast electron transport, facile Li‐ion migration in the porous film, and greatly reduced ion‐diffusion length. Using such a Nb₂O₅ film as anode and commercial activated carbon as cathode, a flexible LIC is designed. It delivers both high gravimetric and high volumetric energy/power densities (≈95.55 Wh kg^?1/5350.9 W kg^?1; 6.7 mW h cm^?3/374.63 mW cm^?3), surpassing previous typical Li‐intercalation electrode‐based LICs. Furthermore, this LIC device still keeps good electrochemical attributes even under serious bending states (30°–180°).     

High‐Yield Synthesis of Multifunctional Tellurium Nanorods to Achieve Simultaneous Chemo‐Photothermal Combination Cancer Therapy

Tellurium (Te) is an important semiconductor material with low band‐gap energy, which has attracted considerable attention in recent years, due to its special chemical and physical properties and wide potential in electrochemistry, optoelectronics, and biological fields. This study demonstrates a facile and high‐yield synthesis strategy of Te nanorods (PTW‐TeNRs) decorated by polysaccharide–protein complex, which can achieve simultaneous chemo‐photothermal combination therapy against cancers. PTW‐TeNRs alone possess high stability under physiological conditions, potent anticancer activities through induction of reactive oxygen species overproduction, and high selectivity among tumor and normal cells. More importantly, they exhibit strong near‐infrared (NIR) absorbance and good photothermal conversion ability from NIR light to heat energy. Furthermore, in combination with NIR laser irradiation, PTW‐TeNRs exhibit excellent chemo‐photothermal efficiency and low toxicity as evidenced by highly efficient tumor ablation ability, but show no obvious histological damage to the major organs. Taken together, this study provides a valid tactic for facile synthesis of multifunctional tellurium nanorods for efficient and combinational cancer therapy.     

Tetragonal Kondo Insulator EuCd2Sb2 Discovered via High Pressure High Temperature Synthesis

Magnetic and electronic properties of quantum materials heavily rely on the crystal structure even in the same chemical compositions. In this study, it is demonstrated that a layered tetragonal EuCd₂Sb₂ structure can be obtained by treating bulk trigonal EuCd₂Sb₂ under high pressure (6 GPa) and high temperature (600 °C). Magnetization measurements of the newly formed layered tetragonal EuCd₂Sb₂ confirm an antiferromagnetic ordering with Neel temperature (T_N) around 16 K, which is significantly higher than that (T_N ≈ 7 K) of trigonal EuCd₂Sb₂, consistent with heat capacity measurements. Moreover, bad metal behavior is observed in the temperature dependence of the electrical resistivity and the resistivity shows a dramatic increase around the Neel temperature. Electronic structure calculations with local density approximation dynamic mean–field theory (LDA+DMFT) show that this material is strongly correlated with well-formed large magnetic moments, due to Hund's coupling, which is known to dramatically suppress the Kondo scale.     

General Solvothermal Synthesis Method for Complete Solubility Range Bimetallic and High‐Entropy Alloy Nanocatalysts

Nanoalloys (NAs) have extraordinary catalytic properties, but metals are often immiscible giving compositional limits on catalytic design. It is generally believed that solution‐based chemical synthesis is inadequate for obtaining NAs, and often exotic shock synthesis or severe decomposition or reduction reactions are required. However, such methods only work on the laboratory scale making real‐world applications difficult. Here, a general solvothermal method is reported to obtain phase‐pure bimetallic and high‐entropy nano‐alloys across the entire composition range. Tuning of solvent chemistry and precursors leads to six different bimetallic NAs: Pd_xRu_1‐x, Pt_xRu_1‐x, Ir_xRu_1‐x, Rh_xRu_1‐x, Ir_1‐xPt_x, and Rh_1‐xPt_x, without immiscibility regions. All samples have face‐centered‐cubic crystal structures, which have not previously been observed for the ruthenium‐based systems. Additionally, quaternary and quinary systems are produced, demonstrating the ability to obtain medium‐ and high‐entropy NAs. The method described herein provides a simple, general production method of previously unknown solid solutions throughout their entire composition range potentially allowing for detailed tuning of nanocatalyst properties.     

Layer‐Controlled and Wafer‐Scale Synthesis of Uniform and High‐Quality Graphene Films on a Polycrystalline Nickel Catalyst

Chemical vapor deposition (CVD) provides a synthesis route for large‐area and high‐quality graphene films. However, layer‐controlled synthesis remains a great challenge on polycrystalline metallic films. Here, a facile and viable synthesis of layer‐controlled and high‐quality graphene films on wafer‐scale Ni surface by the sequentially separated steps of gas carburization, hydrogen exposure, and segregation is developed. The layer numbers of graphene films with large domain sizes are controlled precisely at ambient pressure by modulating the simplified CVD process conditions and hydrogen exposure. The hydrogen exposure assisted with a Ni catalyst plays a critical role in promoting the preferential segregation through removing the carbon layers on the Ni surface and reducing carbon content in the Ni. Excellent electrical and transparent conductive performance, with a room‐temperature mobility of ≈3000 cm² V^?1 s^?1 and a sheet resistance as low as ≈100 Ω per square at ≈90% transmittance, of the twisted few‐layer grapheme films grown on the Ni catalyst is demonstrated.     

Synthesis of Metal Oxide Nanoparticles by Rapid,High‐Temperature 3D Microwave Heating

Microwave‐assisted fabrication has propelled the recent synthesis and processing approaches of various nanomaterials. However, in most previous studies, the synthesis temperature is limited to below 1100 K, which restricts its application. Here, a rapid, in situ 3D heating method to manufacture well‐dispersed metal oxide nanoparticles on a 3D carbonized wood (denoted as C‐wood) host using microwaves as the driving power is reported. The moderate electronic conductivity of C‐wood contributes to the local Joule heating and the good thermal conductivity guarantees the rapid 3D heating of the overall material. The temperature of the C‐wood increases from room temperature to ≈2200 K in 4 s (≈550 K s^?1), stabilizing to 1400 K, and then cooling back down to room temperature within 2 s. The preloaded precursor salts rapidly decompose and form ultrafine (≈11 nm) metal oxide nanoparticles on the surface of the C‐wood during the rapid quenching. The process takes place in air, which helps prevent the metal oxides from being reduced by the carbon. The 3D heating method offers an effective route to the rapid and scalable synthesis of metal oxide nanoparticles.     

Cobalt‐Doped SnS2 with Dual Active Centers of Synergistic Absorption‐Catalysis Effect for High‐S Loading Li‐S Batteries

The application of Li‐S batteries is hindered by low sulfur utilization and rapid capacity decay originating from slow electrochemical kinetics of polysulfide transformation to Li₂S at the second discharge plateau around 2.1 V and harsh shuttling effects for high‐S‐loading cathodes. Herein, a cobalt‐doped SnS₂ anchored on N‐doped carbon nanotube (NCNT@Co‐SnS₂) substrate is rationally designed as both a polysulfide shield to mitigate the shuttling effects and an electrocatalyst to improve the interconversion kinetics from polysulfides to Li₂S. As a result, high‐S‐loading cathodes are demonstrated to achieve good cycling stability with high sulfur utilization. It is shown that Co‐doping plays an important role in realizing high initial capacity and good capacity retention for Li‐S batteries. The S/NCNT@Co‐SnS₂ cell (3 mg cm^?2 sulfur loading) delivers a high initial specific capacity of 1337.1 mA h g^?1 (excluding the Co‐SnS₂ capacity contribution) and 1004.3 mA h g^?1 after 100 cycles at a current density of 1.3 mA cm^?2, while the counterpart cell (S/NCNT@SnS₂) only shows an initial capacity of 1074.7 and 843 mA h g^?1 at the 100th cycle. The synergy effect of polysulfide confinement and catalyzed polysulfide conversion provides an effective strategy in improving the electrochemical performance for high‐sulfur‐loading Li‐S batteries.     

Fluorinated Polyimide as a Novel High‐Voltage Binder for High‐Capacity Cathode of Lithium‐Ion Batteries

An increase in the energy density of lithium‐ion batteries has long been a competitive advantage for advanced wireless devices and long‐driving electric vehicles. Li‐rich layered oxide, xLi₂MnO₃?(1?x)LiMn_1?y?zNi_yCo_zO₂, is a promising high‐capacity cathode material for high‐energy batteries, whose capacity increases by increasing charge voltage to above 4.6 V versus Li. Li‐rich layered oxide cathode however suffers from a rapid capacity fade during the high‐voltage cycling because of instable cathode–electrolyte interface, and the occurrence of metal dissolution, particle cracking, and structural degradation, particularly, at elevated temperatures. Herein, this study reports the development of fluorinated polyimide as a novel high‐voltage binder, which mitigates the cathode degradation problems through superior binding ability to conventional polyvinylidenefluoride binder and the formation of robust surface structure at the cathode. A full‐cell consisting of fluorinated polyimide binder‐assisted Li‐rich layered oxide cathode and conventional electrolyte without any electrolyte additive exhibits significantly improved capacity retention to 89% at the 100th cycle and discharge capacity to 223–198 mA h g^?1 even under the harsh condition of 55 °C and high charge voltage of 4.7 V, in contrast to a rapid performance fade of the cathode coated with polyvinylidenefluoride binder.     

High‐κ Solid‐Gate Transistor Configured Graphene Biosensor with Fully Integrated Structure and Enhanced Sensitivity

A fully integrated graphene field‐effect transistor (GFET) nanosensor utilizing a novel high‐κ solid‐gating geometry for a practical biosensor with enhanced sensitivity is presented. Herein, an “in plane” gate supplying electrical field through a 30 nm HfO₂ dielectric layer is employed to eliminate the cumbrous external wire electrode in conventional liquid‐gate GFET nanosensors that undesirably limits the device potential in on‐site sensing applications. In addition to the advantage in the device integration degree, the transconductance level is found to be increased by about 50% over liquid‐gate GFET devices in aqueous‐media, thereby improves the sensitivity performance in sensor applications. As the first demonstration of biosensing applications, a small‐molecule antibiotic, kanamycin A, is detected by means of an aptameric competitive affinity principle. It is experimentally shown that the label‐free and specific quantification of kanamycin A with a concentration resolution at 11.5 × 10^?9 m is achievable through a single direct observation of the 200 s fast bioassay without any further noise canceling. These results demonstrate the utility and practicability of the new devices in label‐free biosensing as a novel analytical tool, and potentially hold great promise in other significant biomedical applications.     

Graphene Oxide Gel‐Derived,Free‐Standing,Hierarchically Porous Carbon for High‐Capacity and High‐Rate Rechargeable Li‐O2 Batteries

Lithium‐oxygen (Li‐O₂) batteries are one of the most promising candidates for high‐energy‐density storage systems. However, the low utilization of porous carbon and the inefficient transport of reactants in the cathode limit terribly the practical capacity and, in particular, the rate capability of state‐of‐the‐art Li‐O₂ batteries. Here, free‐standing, hierarchically porous carbon (FHPC) derived from graphene oxide (GO) gel in nickel foam without any additional binder is synthesized by a facile and effective in situ sol‐gel method, wherein the GO not only acts as a special carbon source, but also provides the framework of a 3D gel; more importantly, the proper acidity via its intrinsic COOH groups guarantees the formation of the whole structure. Interestingly, when employed as a cathode for Li‐O₂ batteries, the capacity reaches 11 060 mA h g^?1 at a current density of 0.2 mA cm^?2 (280 mA g^?1); and, unexpectedly, a high capacity of 2020 mA h g^?1 can be obtained even the current density increases ten times, up to 2 mA cm^?2 (2.8 A g^?1), which is the best rate performance for Li‐O₂ batteries reported to date. This excellent performance is attributed to the synergistic effect of the loose packing of the carbon, the hierarchical porous structure, and the high electronic conductivity of the Ni foam.     

High‐Performance n‐ and p‐Type Field‐Effect Transistors Based on Hybridly Surface‐Passivated Colloidal PbS Nanosheets

Colloidally synthesized nanomaterials are among the promising candidates for future electronic devices due to their simplicity and the inexpensiveness of their production. Specifically, colloidal nanosheets are of great interest since they are conveniently producible through the colloidal approach while having the advantages of two‐dimensionality. In order to employ these materials, according transistor behavior should be adjustable and of high performance. It is shown that the transistor performance of colloidal lead sulfide nanosheets is tunable by altering the surface passivation, the contact metal, or by exposing them to air. It is found that adding halide ions to the synthesis leads to an improvement of the conductivity, the field‐effect mobility, and the on/off ratio of these transistors by passivating their surface defects. Superior n‐type behavior with a field‐effect mobility of 248 cm² V^?1 s^?1 and an on/off ratio of 4 × 10⁶ is achieved. The conductivity of these stripes can be changed from n‐type to p‐type by altering the contact metal and by adding oxygen to the working environment. As a possible solution for the post‐Moore era, realizing new high‐quality semiconductors such as colloidal materials is crucial. In this respect, the results can provide new insights which helps to accelerate their optimization for potential applications.     

Facile Preparation of High‐Content N‐Doped CNT Microspheres for High‐Performance Lithium Storage

Herein, high‐content N‐doped carbon nanotube (CNT) microspheres (HNCMs) are successfully synthesized through simple spray drying and one‐step pyrolysis. HNCM possesses a hierarchically porous architecture and high‐content N‐doping. In particular, HNCM800 (HNCM pyrolyzed at 800 °C) shows high nitrogen content of 12.43 at%. The porous structure derived from well‐interconnected CNTs not only offers a highly conductive network and blocks diffusion of soluble lithium polysulfides (LiPSs) in physical adsorption, but also allows sufficient sulfur infiltration. The incorporation of N‐rich CNTs provides strong chemical immobilization for LiPSs. As a sulfur host for lithium–sulfur batteries, good rate capability and high cycling stability is achieved for HNCM/S cathodes. Particularly, the HNCM800/S cathode delivers a high capacity of 804 mA h g^?1 at 0.5 C after 1000 cycles corresponding to low fading rate (FR) of only 0.011% per cycle. Remarkably, the cathode with high sulfur loading of 6 mg cm^?2 still maintains high cyclic stability (capacity of 555 mA h g^?1 after 1000 cycles, FR 0.038%). Additionally, CNT/Co₃O₄ microspheres are obtained by the oxidation of CNTs/Co in the air. The as‐prepared CNT/Co₃O₄ microspheres are employed as an anode for lithium‐ion batteries and present excellent cycling performance.     

Ti3+ Self‐Doped Dark Rutile TiO2 Ultrafine Nanorods with Durable High‐Rate Capability for Lithium‐Ion Batteries

Dark‐colored rutile TiO₂ nanorods doped by electroconducting Ti³⁺ have been obtained uniformly with an average diameter of ≈7 nm, and have been first utilized as anodes in lithium‐ion batteries. They deliver a high reversible specific capacity of 185.7 mAh g^?1 at 0.2 C (33.6 mA g^?1) and maintain 92.1 mAh g^?1 after 1000 cycles at an extremely high rate 50 C with an outstanding retention of 98.4%. Notably, the coulombic efficiency of Ti³⁺–TiO₂ has been improved by approximately 10% compared with that of pristine rutile TiO₂, which can be mainly attributed to its prompt electron transfer because of the introduction of Ti³⁺. Again the synergetic merits are noticed when the promoted electronic conductivity is combined with a shortened Li⁺ diffusion length resulting from the ultrafine nanorod structure, giving rise to the remarkable rate capabilities and extraordinary cycling stabilities for applications in fast and durable charge/discharge batteries. It is of great significance to incorporate Ti³⁺ into rutile TiO₂ to exhibit particular electrochemical characteristics triggering an effective way to improve the energy storage properties.     

Orthorhombic Ti2O3: A Polymorph‐Dependent Narrow‐Bandgap Ferromagnetic Oxide

Magnetic semiconductors are highly sought in spintronics, which allow not only the control of charge carriers like in traditional electronics, but also the control of spin states. However, almost all known magnetic semiconductors are featured with bandgaps larger than 1 eV, which limits their applications in long‐wavelength regimes. In this work, the discovery of orthorhombic‐structured Ti₂O₃ films is reported as a unique narrow‐bandgap (≈0.1 eV) ferromagnetic oxide semiconductor. In contrast, the well‐known corundum‐structured Ti₂O₃ polymorph has an antiferromagnetic ground state. This comprehensive study on epitaxial Ti₂O₃ thin films reveals strong correlations between structure, electrical, and magnetic properties. The new orthorhombic Ti₂O₃ polymorph is found to be n‐type with a very high electron concentration, while the bulk‐type trigonal‐structured Ti₂O₃ is p‐type. More interestingly, in contrast to the antiferromagnetic ground state of trigonal bulk Ti₂O₃, unexpected ferromagnetism with a transition temperature well above room temperature is observed in the orthorhombic Ti₂O₃, which is confirmed by X‐ray magnetic circular dichroism measurements. Using first‐principles calculations, the ferromagnetism is attributed to a particular type of oxygen vacancies in the orthorhombic Ti₂O₃. The room‐temperature ferromagnetism observed in orthorhombic‐structured Ti₂O₃, demonstrates a new route toward controlling magnetism in epitaxial oxide films through selective stabilization of polymorph phases.     

3D Printed High‐Loading Lithium‐Sulfur Battery Toward Wearable Energy Storage

Wearable electronic devices are the new darling of consumer electronics, and energy storage devices are an important part of them. Here, a wearable lithium‐sulfur (Li‐S) bracelet battery using three‐dimensional (3D) printing technology (additive manufacturing) is designed and manufactured for the first time. The bracelet battery can be easily worn to power the wearable device. The “additive” manufacturing characteristic of 3D printing provides excellent controllability of the electrode thickness with much simplified process in a cost‐effective manner. Due to the conductive 3D skeleton providing interpenetrating transmission paths and channels for electrons and ions, the 3D Li‐S battery can provide 505.4 mAh g^?1 specific capacity after 500 cycles with an active material loading as high as 10.2 mg cm^?1. The practicality is illustrated by wearing the bracelet battery on the wrist and illuminating the red light‐emitting diode. Therefore, the bracelet battery manufactured by 3D printing technology can address the needs of the wearable power supply.     

Solution‐Processable,High‐Performance Flexible Electroluminescent Devices Based on High‐k Nanodielectrics

Flexible alternating‐current electroluminescent (ACEL) devices have attracted considerable attention for their ability to produce uniform light emission under bent conditions and have enormous potential for applications in back lighting panels, decorative lighting in automobiles, and panel displays. Nevertheless, flexible ACEL devices generally require a high operating bias, which precludes their implementation in low power devices. Herein, solution‐processed La‐doped barium titanate (BTO:La) nanocuboids (≈150 nm) are presented as high dielectric constant (high‐k) nanodielectrics, which can enhance the dielectric constant of an ACEL device from 2.6 to 21 (at 1 kHz), enabling the fabrication of high‐performance flexible ACEL devices with a lower operating voltage as well as higher brightness (≈57.54 cd m^?2 at 240 V, 1 kHz) than devices using undoped BTO nanodielectrics (≈14.3 cd m^?2 at 240 V, 1 kHz). Furthermore, a uniform brightness across the whole panel surface of the flexible ACEL devices and excellent device reliability are achieved via the use of uniform networks of crossaligned silver nanowires as highly conductive and flexible electrodes. The results offer experimental validation of high‐brightness flexible ACELs using solution‐processed BTO:La nanodielectrics, which constitutes an important milestone toward the implementation of high‐k nanodielectrics in flexible displays.     

Scalable Synthesis of Ultrathin Mn3N2 Exhibiting Room‐Temperature Antiferromagnetism

Ultrathin and 2D magnetic materials have attracted a great deal of attention recently due to their potential applications in spintronics. Only a handful of stable ultrathin magnetic materials have been reported, but their high‐yield synthesis remains a challenge. Transition metal (e.g., manganese) nitrides are attractive candidates for spintronics due to their predicted high magnetic transition temperatures. Here, a lattice matching synthesis of ultrathin Mn₃N₂ is employed. Taking advantage of the lattice match between a KCl salt template and Mn₃N₂, this method yields the first ultrathin magnetic metal nitride via a solution‐based route. Mn₃N₂ flakes show intrinsic magnetic behavior even at 300 K, enabling potential room‐temperature applications. This synthesis procedure offers an approach to the discovery of other ultrathin or 2D metal nitrides.     

Advanced Materials for High‐Temperature Thermal Transport

High temperature processes are widely used in a variety of existing and emerging industrial and aerospace applications. The thermal properties of high‐temperature materials thus play an important role in controlling the thermal energy, as highlighted by successful applications of thermal barrier coating and aerogels. While thermal transport processes at room and low temperature have witnessed tremendous progress in the past two decades, particularly on the fronts of understanding basic heat transfer properties at the micro‐ and nanoscale, the understanding at high temperature is still at the nascent stage, owing to several unique features at high temperature, such as the dominant Umklapp scattering effect that can render a crystalline material amorphous‐like thermal properties, and the important radiation contribution at high temperature. This lack of systematic understanding, coupled with the challenges in maintaining high‐temperature stability in a large number of materials, has limited the development of materials to meet the thermal transport properties pertaining to several current and emerging high‐temperature applications. This Review is aimed at providing an overview of the basic mechanisms governing thermal transport processes at high temperature, to identify their unique features and challenges, and to explore opportunities in material research for high‐temperature thermal materials.