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The electrochemical nitrate reduction for green ammonia production is attracting increasing attention, where the catalysts are widely investigated by controlling the compositions or structures to achieve high performance. However, their reconstructions under reduction potentials are inevitable and uncontrollable, leading to uncertain performance, and a confused understanding of the mechanism. In this work, a strategy is proposed by controlling the pre‐catalyst's reconstruction chemistry toward electrochemical nitrate reduction reaction (e‐NO3RR) with superior activity and stability. To demonstrate the idea, a pre‐catalyst is fabricated with α‐Co(OH)2 and Cu(OH)2 (α‐Co(OH)2/Cu(OH)2), which is in situ reconstructed to a tandem catalyst with Cu and β‐Co(OH)2 (Cu/β‐Co(OH)2) under working potential. Cu/β‐Co(OH)2 achieves an optimal Faraday efficiency for ammonia of 97.7% with a yield rate of 3.9 mmol h−1 cm−2 at −0.5 V, outperforming other reported metal‐hydroxide catalysts. The experimental and theoretical results demonstrate that a tandem catalytic mechanism is responsible for the exceptional performance: 1) Cu functions as the donor of nitrite; and 2) β‐Co(OH)2 serves as active sites for generating active hydrogen and reducing nitrogen‐containing groups. This work highlights that the controllable reconstruction toward improved performance can be realized, and provides an insightful understanding of the mechanism, which is helpful for developing active and stable catalysts for various catalytic applications. [ABSTRACT FROM AUTHOR]

Active materials play a crucial role in the performance of phototransistors. However, the discovery of a novel and versatile active material is a big challenge. For the first time, phototransistors with ultrathin niobium‐doped indium oxide (InNbO) active layer are fabricated. The InNbO phototransistors without additional light‐absorbing layers exhibit the performance with a high average mobility of 22.86 cm2 V−1s−1, a turn‐on voltage of −0.75 V, a low sub threshold swing of 0.18 V/decade, and a high on/off current ratio of 5.74 × 108. Detailed studies show that Nb is the key to suppress the free carrier generation due to the strong bonding strength of Nb─O. In addition, the InNbO phototransistors exhibit a very broad spectral responsivity with a photocurrent of 4.72 × 10−4 A, a photosensitivity of 1.69 × 108, and a high detectivity of 3.33 × 1013 Jones under violet (405 nm) light illumination, which is significantly higher than that of the IGZO phototransistors. Furthermore, an active‐matrix quantum‐dot light‐emitting diode pixel circuit based on InNbO phototransistors is demonstrated. The findings not only indicate that InNbO is a new active material for phototransistors, but also suggest that InNbO‐based phototransistors have a great potential for the next‐generation interactive display technology. [ABSTRACT FROM AUTHOR]

Inserting an insulating layer between the charge transport layer (CTL) and quantum dot emitting layer (QDL) is widely used in improving the performance of quantum dot light-emitting diodes (QLEDs). However, the additional layer inevitably leads to energy loss and joule heat. Herein, a monolayer silane coupling agent is used to modify the said interfaces via the self-limiting adsorption effect. Because the ultrathin layers induce negligible series resistance to the device, they can partially passivate the interfacial defects on the electron transport side and help confine the electrons within the QDL on the hole transport side. These interfacial modifications can not only suppress the nonradiative recombination but also slow down the aging of the hole transport layer. The findings here underline a low-temperature adsorption-based strategy for effective interfacial modification which can be used in any layer-by-layer device structures.

High-quality conjugated microporous polymer (CMP) films with orientation and controlled structure are extremely desired for applications. Here, we report the effective construction of CMP 3D composite films (pZn/PTPCz) with a controlled porosity structure and preferred orientation using the template-assisted electropolymerization (EP) approach for the first time. The structure of pZn/PTPCz composite thin films and nitrophenol sensing performance were thoroughly studied. When compared to the control CMP film made on flat indium tin oxide (ITO) substrates, the as-prepared pZn/PTPCz composite films showed significantly enhanced fluorescent intensity and much better sensing performance for the model explosive. This was attributed to the metal-enhanced fluorescence (MEF) of porous nanostructured zinc (pZn) and the additional macroporosity of the pZn/PTPCz composite films. This work provides a feasible approach for creating oriented 3D CMP-based thin films for advanced applications., (© 2024 Wiley‐VCH GmbH.)

The rapid evolution of the Internet of Things has engendered increased requirements for low-cost, self-powered UV photodetectors. Herein, high-performance self-driven UV photodetectors are fabricated by designing asymmetric metal-semiconductor-metal structures on the high-quality large-area CsCu 2 I 3 microwire arrays. The asymmetrical depletion region doubles the photocurrent and response speed compared to the symmetric structure device, leading to a high responsivity of 233 mA/W to 355 nm radiation. Notably, at 0 V bias, the asymmetric device produces an open-circuit voltage of 356 mV and drives to a short-circuit current of 372 pA; meanwhile, the switch ratio ( I ph / I dark ) reaches up to 10 3 , indicating its excellent potential for detecting weak light. Furthermore, the device maintains stable responses throughout 10000 UV-light switch cycles, with negligible degradation even after 90-day storage in air. Our work establishes that CsCu 2 I 3 is a good candidate for self-powered UV detection and thoroughly demonstrates its potential as a passive device.

Recently, a new layered material, Mn 3 Si 2 Te 6 , was identified to be a semiconductor with nodal-line topological property and ferrimagnetic ground state. In this work, we propose a series of structures, M 3 Si 2 Te 6 (M = alkaline earth and transition metals), and systematically investigate their mechanical, magnetic and electronic properties, and the strain effect to enrich the family of the layered materials for practical applications. We find 13 stable M 3 Si 2 Te 6 , including 5 semiconductors (M = Ca, Sr, Fe, Ru and Os) and 8 metals (M = Sc, Ti, Nb, Ta, Cr, Mo, W and Tc). Two structures (M = Ti and Cr) are antiferromagnetic (AFM), while other structures are non-magnetic (NM). Similar to Mn 3 Si 2 Te 6 , the AFM structures exhibit magnetic anisotropy energies (MAEs) and semiconductors have anisotropic electron effective masses. We further show that compressions along the z -axis can effectively tune the electronic and magnetic properties, such as the semiconductor-metal and NM-AFM transition in Fe 3 Si 2 Te 6 , the two-fold degeneracy of the valence band maximums in Sr 3 Si 2 Te 6 , as well as the reduced MAE for all magnetic structures. These results demonstrate the diverse properties of the layered M 3 Si 2 Te 6 family and provide promising theoretical predictions for the future design of new layered materials., (© 2023 IOP Publishing Ltd.)

This research explores the influence of renewable fuels, including three kinds of biodiesel along with ethanol on the physical properties and structural characteristics of particulate matter (PM) emitted from a diesel engine in comparison with pure diesel. After adding 10 vol% of grape seed biodiesel, coffee biodiesel and eucalyptus oil into diesel, three biodiesel blended fuels (10% grape seed biodiesel (DGs10), 10% spent coffee ground biodiesel (DC10) and eucalyptus oil biodiesel (DEu10)) were produced and tested in this study. Besides, one ethanol blend containing 9 vol% of ethanol and 1 vol% of biodiesel (blend stabilizer) was also tested to do the comparison. In the present study, scanning transmission electron microscope (STEM) and scanning electron microscope (SEM) were employed for analyzing the microstructure, nanostructure and electron diffraction pattern of PM. Raman spectrometer (RS) was also used for the analysis of structural characterization of PM. In addition, several experimental instruments like microbalance, measuring cup, viscometer, oxygen bomb calorimeter and Gas Chromatography-Mass Spectrometer (GC-MS) were employed to detect the fuel properties, including density, heating value, viscosity, composition and cetane number. A conclusion can be drawn that both biodiesel blends and ethanol blend have a changing effect on the PM properties compared to pure diesel, where biodiesel blends have a slightly weaker influence than ethanol blend. Regarding the biodiesel blends, DGs10 has more impact than DC10 and DEu10 in changes of PM properties, particularly in the reduction of PM mass, making it a good candidate for renewable fuel for diesel engines., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier Ltd. All rights reserved.)

Stacked 2D perovskites provide more possibilities for next generation photodetector with more new features. Compared with its excellent optoelectronic properties, the good dielectric performance of metal halide perovskite rarely comes into notice. Here, a bifunctional perovskite based photovoltaic detector capable of two wavelength demultiplexing is demonstrated. In the Black Phosphorus/Perovskite/MoS 2 structured photodetector, the comprehensive utilization of the photosensitive and dielectric properties of 2D perovskite allows the device to work in different modes. The device shows normal continuous photoresponse under 405 nm, while it shows a transient spike response to visible light with longer wavelengths. The linear dynamic range, rise/decay time, and self-powered responsivity under 405 nm can reach 100, 38 µs/50 µs, and 17.7 mA W -1 , respectively. It is demonstrated that the transient spike photocurrent with long wavelength exposure is related to the illumination intensity and can coexist with normal photoresponse. Two waveband-dependent signals can be identified and used to reflect more information simultaneously. This work provides a new strategy for multispectral detection and demultiplexing, which can be used to improve data transfer rates and encrypted communications. This work mode can inspire more multispectral photodetectors with different stacked 2D materials, especially to the optoelectronic application of the wide bandgap, high dielectric photosensitive materials., (© 2023 Wiley-VCH GmbH.)

Copper-based halide perovskites have shown great potential in lighting and photodetection due to their excellent photoelectric properties, good stability and lead-free nature. However, as an important piece of copper-based perovskites, the synthesis and application of RbCu 2 I 3 have never been reported. Here, we demonstrate the synthesis of high-quality RbCu 2 I 3 microwires (MWs) by a fast-cooling hot saturated solution method. The prepared MWs exhibit an orthorhombic structure with a smooth surface. Optical measurements show the RbCu 2 I 3 MWs have a sharp ultraviolet absorption edge with 3.63 eV optical band gap and ultra-large stokes shift (300 nm) in photoluminescence. The subsequent photodetector based on a single RbCu 2 I 3 MW shows excellent ultraviolet detection performance. Under the 340 nm illumination, the device shows a specific detectivity of 5.0 × 10 9 Jones and a responsivity of 380 mA·W -1 . The synthesis method and physical properties of RbCu 2 I 3 could be a guide to the future optoelectronic application of the new material., (© 2023 IOP Publishing Ltd.)

Electrides with spatial electrons serving as 'anions' in the cavities or channels exhibit intriguing properties which can be applied in electron injection/emission and high-speed devices. Here, we report a new group of layered electrides, M 2 X (M = Ti, V, and Cr; X = C and N) with electrons distributed in the interlayer spacings. We find that the interstitial electrons tend to be delocalized from the Ti-based structures to the Cr-based ones. We show that the interstitial electrons originate from the d -electrons of transition metal atoms. Our findings prove the existence of tunable interstitial electrons with rich electronic properties in layered MXenes and provide valuable insights into the design and fabrication of new materials with multiple applications., (© 2022 IOP Publishing Ltd.)

Lead-free perovskite has attracted great attention in realizing high-performance optoelectronic devices due to their excellent atmospheric stability and nontoxic characteristics. Although a pronounced ion migration effect has been observed in this new class of materials, its potential in enhancing the overall device performance is yet to be fully explored. In this work, we studied the effect of ion migrations on the carrier transport behavior and found that the recoverable migration process can contribute to enhancing the on/off ratio in a lead-free CsCu 2 I 3 single-crystal microrod-based photodetector. In detail, we synthesized CsCu 2 I 3 single-crystal microrods via an in-plane self-assembly supersaturated crystallization approach. These microrods with well-defined morphologies were then used to construct ultraviolet (UV)-band photodetectors, which outperform most reported lead-free perovskite photodetectors based on individual single crystals. Simultaneously, ion migration can result in asymmetric band bending in the two-terminal device, as confirmed by surface potential profiling with Kelvin probe force microscopy (KPFM). Such an effect can be harnessed to increase the on/off ratio by almost an order of magnitude. Furthermore, the lead-free CsCu 2 I 3 single crystal exhibits excellent thermal and air stabilities. These findings demonstrate that the CsCu 2 I 3 single-crystal microrods can be used in stable and efficient photodetection, and the ion migration effect can potentially be utilized for improving the optoelectronic performance of lead-free devices.

Aqueous electrochromic battery (ECB) is a multifunctional technology that shows great potential in various applications including energy-saving buildings and wearable batteries with visible energy levels. However, owing to the mismatch between traditional electrochromic materials and the electrolyte, aqueous ECBs generally exhibit poor cycling stability which bottlenecks their practical commercialization. Herein, we present an ultrastable electrochromic system composed of lithium titanate (Li 4 Ti 5 O 12 , LTO) electrode and Al 3+ /Zn 2+ hybrid electrolyte. The fully compatible system exhibits excellent redox reaction reversibility, thus leading to extremely high cycling stabilities in optical contrast (12 500 cycles with unnoticeable degradation) and energy storage (4000 cycles with 82.6% retention of capacity), superior electrochromic performances including high optical contrast (∼74.73%) and fast responses (4.35 s/7.65 s for bleaching/coloring), as well as excellent discharge areal capacity of 151.94 mAh m -2 . The extraordinary cycling stability can be attributed to the robust [TiO 6 ] octahedral frameworks which remain chemically active even upon the gradual substitution of Li + with Al 3+ in LTO over multiple operation cycles. The high-performance electrochromic system demonstrated here not only makes the commercialization of low-cost, high-safety aqueous-based electrochromic devices possible but also provides potential design guidance for LTO-related materials used in aqueous-based energy storage devices.

The lifetime and efficiency of diesel particulate filters (DPFs) strongly depend on the proper and periodic cleaning and servicing. Unfortunately, in some cases, inappropriate methods are applied to clean the DPFs, e.g., using air compressors without proper disposal procedures which can have negative impacts on human health, the environment, and DPF's efficiency. However, there is no information available about the properties of this kind of PM. This research is therefore presented to explore the physicochemical and toxicity properties of aged PM trapped in a DPF (using compressed air for PM sampling) employing STEM, SEM, EDS, Organic Carbon Analyzer, TGA/DSC, and Raman Spectrometer for investigating the physicochemical properties, and assays of cell viability, cellular reactive oxygen species (ROS), interleukin-6, and tumor necrosis factor-alpha (TNF-α) for investigating the toxicity properties. Also, analyses from fresh PM samples from the diesel vehicle at two engine speeds are presented. It is found that at a certain/fixed PM number/mass for all three samples tested, the PM from DPF compared with the fresh PM can have both positive (particularly having the lowest water-soluble total carbon ratio) and negative impacts on human health (particularly having the highest cell death rate of 13.4%, ROS, and TNF-α) and the environment., (Copyright © 2022 Elsevier B.V. All rights reserved.)

Transparent superhydrophobic coatings with mechanical stability, self-cleaning function, and anti-reflective property have drawn much attention due to the great potential in a variety of real-world applications. In this work, we develop an ingenious approach to construct micropatterned transparent superhydrophobic coatings with a multilayer structure (water contact angle ∼153.6°, sliding angle ∼3.2°). A micropatterned ultraviolet-cured resist frame facilitates durability, while the modified silica nanoparticles, which are housed within the micro-cavities and bonded by an epoxy-based adhesive, impart superhydrophobicity. The micropatterned multilayer surface could endure sandpaper abrasion while maintaining satisfactory hydrophobicity. The prepared surfaces also retain the excellent water repellency after water jet impact, acid submerging, and mechanical bending, suggesting that they are sustainable in the case of adverse conditions and can be integrated with objects with non-flat geometries. Further, the superhydrophobic coatings exhibit an anti-reflection property while preserving high transparency. Taken together, we envision that the design strategies here can offer a practicable route to produce transparent superhydrophobic coatings for diverse outdoor applications.

The literature shows that information about the physical, chemical, and cell toxicity properties of particulate matter (PM) from diesel vehicles is not rich as the existence of a remarkable number of studies about the combustion, performance, and emissions of diesel vehicles using renewable liquid fuels, particularly biodiesels and alcohols. Also, the PM analyses from combustion of spent coffee ground biodiesel have not been comprehensively explored. Therefore, this research is presented. Pure diesel, 90% diesel + 10% biodiesel, and 90% diesel + 9% ethanol + 1% biodiesel, volume bases, were tested under a fast idle condition. STEM, SEM, EDS, Organic Carbon Analyzer, TGA/DSC, and Raman Spectrometer were employed for investigating the PM physical and chemical properties, and assays of cell viability, cellular reactive oxygen species, interleukin-6, and tumor necrosis factor-alpha were examined for investigating the PM cell toxicity properties. It is found that the application of both biodiesel and ethanol has the potential to change the PM properties, while the impact of ethanol is more than biodiesel on the changes. Regarding the important aspects, biodiesel can be effective for better human health (due to a decrease in cell death (-60.8%)) as well as good diesel particulate filter efficiency (due to lower activation energy (-7.6%) and frequency factor (-83.2%)). However, despite a higher impact of ethanol on the reductions in activation energy (-24.8%) and frequency factor (-99.0%), this fuel causes an increase in cell death (84.1%). Therefore, biodiesel can be an appropriate fuel to have a positive impact on human health, the environment, and emissions catalysts performance, simultaneously., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022 Elsevier B.V. All rights reserved.)

Interfacial quality of functional layers plays an important role in the carrier transport of sandwich-structured devices. Although the suppression of interface states is crucial to the overall device performance, our understanding on their formation and annihilation mechanism via direct characterization is still quite limited. Here, we present a thorough study on the interface states present in the electron transport layer (ETL) of blue quantum dot (QD) light-emitting diodes (QLEDs). A ZnO/ZnMgO bilayer ETL is adopted to enhance the electron injection into blue QDs. By probing the ETL band structure with photoelectron spectroscopy, we discover that substantial band bending exists at the ZnO/ZnMgO interface, elucidating the presence of a high density of interface states which hinder electron transport. By inserting a ZnO@ZMO interlayer composed of mixed ZnO and ZnMgO nanoparticles, the band bending and thus the interface states are observed to reduce significantly. We attribute this to the hybrid surface properties of ZnO@ZMO, which can annihilate the surface states of both the ZnO and ZnMgO layers. The introduction of a bridging layer has led to ∼40% enhancement in the power efficiency of blue QLEDs and noticeable performance boosts in green and red QLEDs. The findings here demonstrate a direct observation of interface states via detailed band structure studies and outline a potential pathway for eliminating these states for better performances in sandwich-structured devices.

With many advantages including superior color saturation and efficiency, quantum dot light-emitting diodes (QLEDs) are considered a promising candidate for the next-generation displays. Emission uniformity over the entire device area is a critical factor to the overall performance and reliability of QLEDs. In this work, we performed a thorough study on the origin of dark spots commonly observed in operating QLEDs and developed a strategy to eliminate these defects. Using advanced cross section fabrication and imaging techniques, we discovered the occurrence of voids in the organic hole transport layer and directly correlated them to the observed emission nonuniformity. Further investigations revealed that these voids are thermal damages induced during the subsequent thermal deposition of other functional layers and can act as leakage paths in the device. By inserting a thermo-tolerant 1,4,5,8,9,11-hexaazatriphenylene-hexacarbonitrile (HATCN) interlayer with an optimized thickness, the thermally induced dark spots can be completely suppressed, leading to a current efficiency increase by 18%. We further demonstrated that such a thermal passivation strategy can work universally for various types of organic layers with low thermal stability. Our findings here provide important guidance in enhancing the performances and reliability of QLEDs and also other sandwich-structured devices via the passivation of heat-sensitive layers.

Colloidal all-inorganic perovskites nanocrystals (NCs) have emerged as a promising material for display and lighting due to their excellent optical properties. However, blue emissive NCs usually suffer from low photoluminescence quantum yields (PLQYs) and poor stability, rendering them the bottleneck for full-color all-perovskite optoelectronic applications. Herein, a facile approach is reported to enhance the emission efficiency and stability of blue emissive perovskite nano-structures via surface passivation with potassium bromide. By adding potassium oleate and excess PbBr 2 to the perovskite precursor solutions, potassium bromide-passivated (KBr-passivated) blue-emitting (≈450 nm) CsPbBr 3 nanoplatelets (NPLs) is successfully synthesized with a respectably high PLQY of 87%. In sharp contrast to most reported perovskite NPLs, no shifting in emission wavelength is observed in these passivated NPLs even after prolonged exposures to intense irradiations and elevated temperature, clearly revealing their excellent photo- and thermal-stabilities. The enhancements are attributed to the formation of K-Br bonding on the surface which suppresses ion migration and formation of Br-vacancies, thus improving both the PL emission and stability of CsPbBr 3 NPLs. Furthermore, all-perovskite white light-emitting diodes (WLEDs) are successfully constructed, suggesting that the proposed KBr-passivated strategy can promote the development of the perovskite family for a wider range of optoelectronic applications., (© 2021 Wiley-VCH GmbH.)

2D materials have been interesting for applications into nanodevices due to their intriguing physical properties. In this work, four types of unique structures are designed that are composed of MXenes and C/N-Si layers (CNSi), where MXene is sandwiched by the CNSi layers with different thicknesses, for their practical applications into integrated devices. The systematic calculations on their elastic constants, phonon dispersions, and thermodynamic properties show that these structures are stable, depending on the composition of MXene. It is found: 1) different from MXene or N-functionalized MXene (M 2 CN 2 ), SiN 2 /M 2 X/SiN 2 possess new electronic properties with free carriers only in the middle, leading to 2D free electron gas; 2) CNSi/MXene/CNSi shows an intrinsic Ohmic semiconductor-metal-semiconductor (S-M-S) contact, which is potential for applications into nanodevices; and 3) O/M 2 C/SiN 2 and N/M 2 C/OSiN are also stable and show different electronic properties, which can be semiconductor or metal as a whole depending on the interface. A method is further proposed to fabricate the 2D structures based on the industrial availability. The findings may provide a novel strategy to design and fabricate the 2D structures for their application into nanodevices and integrated circuits., (© 2021 Wiley-VCH GmbH.)

Hybrid organic-inorganic lead halide perovskite microwires are potential building blocks for realizing on-chip integrated optoelectronic devices. However, the length-controllable synthesis of one-dimensional hybrid perovskite microwires has been rarely reported, especially the ones with lengths in the millimeter scale. Herein, methylammonium lead bromide (MAPbBr 3 ) and formamidinium lead bromide (FAPbBr 3 ) micro and milliwires are demonstrated using single-crystal PbBr 2 microwires synthesized via template-free solution-phase growth as the lattice framework. Following the PbBr 2 template, the as-converted perovskite microwires possess controllable lengths ranging from tens to thousands of micrometers. In addition, Fabry-Perot (FP) lasing was realized in both MAPbBr 3 and FAPbBr 3 microwires, attesting to their excellent crystal quality and the efficient optical confinement of the natural cavity. These unique properties result in the first demonstration of FP perovskite microwire lasers with submillimeter lengths. More interestingly, the microwire lasers show excellent photostability under repetitive pulsed laser excitation for over 8 × 10 6 cycles. Such findings demonstrate that the solution-converted hybrid lead bromide microwires have excellent optoelectronic performances promising for practical applications, and the size controllability indicates that this novel fabrication process may be feasible for large-scale industrial production.

Aggregation-induced luminescence quenching of carbon nanodots (CDs) is the main obstacle for their applications in solid-state light emitting devices. Herein, we developed a one-step synthesis of solid-state emissive CDs with surface aluminum-based polymerization by adding AlCl 3 in citric acid and urea via a microwave-heating dehydration process. Due to the strong coordination ability of Al ions with N and O atoms, considerable steric hindrance of Al-based cross-linked polymerization was introduced on the surface of the CDs, which not only avoided aggregation of the green emissive carbon cores but also facilitated efficient energy transfer from the blue emissive polymerized surface to the green emissive carbon cores in aggregates, leading to enhanced green emissions with a photoluminescence quantum yield (PLQY) of 72.7% in the solid state.

Two-dimensional (2D) materials have attracted increasing interest in the past decades due to their unique physical and chemical properties for diverse applications. In this work, we present a first-principles design on a novel 2D family, MSi 2 C x N 4-x (M = Cr, Mo, and W; x = 1 and 2), based on density-functional theory (DFT). We find that all MSi 2 C x N 4-x monolayers are stable by investigating their mechanic, dynamic, and thermodynamic properties. Interestingly, we see that the alignment of magnetic moments can be tuned to achieve non-magnetism (NM), ferromagnetism (FM), anti-ferromagnetism (AFM) or paramagnetism (PM) by arranging the positions of carbon atoms in the 2D systems. Accordingly, their electronic properties can be controlled to obtain semiconductor, half-metal, or metal. The FM states in half-metallic 2D systems are contributed to the hole-mediated double exchange, while the AFM states are induced by super-exchange. Our findings show that the physical properties of 2D systems can be tuned by compositional and structural engineering, especially the layer of C atoms, which may provide guidance on the design and fabrication of novel 2D materials with projected properties for multi-functional applications.

Hydrogen evolution reaction (HER) is a key step for electrochemical energy conversion and storage. Developing well defined nanostructures as noble-metal-free electrocatalysts for HER is promising for the application of hydrogen technology. Herein, it is reported that 3D porous hierarchical CoNiP/Co x P multi-phase heterostructure on Ni foam via an electrodeposition method followed by phosphorization exhibits ultra-highly catalytic activity for HER. The optimized CoNiP/Co x P multi-phase heterostructure achieves an excellent HER performance with an ultralow overpotential of 36 mV at 10 mA cm -2 , superior to commercial Pt/C. Importantly, the multi-phase heterostructure shows exceptional stability as confirmed by the long-term potential cycles (30,000 cycles) and extended electrocatalysis (up to 500 h) in alkaline solution and natural seawater. Experimental characterizations and DFT calculations demonstrate that the strong electronic interaction at the heterointerface of CoNiP/CoP is achieved via the electron transfer from CoNiP to the heterointerface, which directly promotes the dissociation of water at heterointerface and desorption of hydrogen on CoNiP. These findings may provide deep understanding on the HER mechanism of heterostructure electrocatalysts and guidance on the design of earth-abundant, cost-effective electrocatalysts with superior HER activity for practical applications., (© 2021 Wiley-VCH GmbH.)

Searching for two-dimensional (2D) materials with a high phase-transition temperature and magnetic anisotropy is critical to the development of spintronics. Herein, we investigate the electronic and magnetic properties of 2D TiX 3 (X = F, Cl, Br and I) monolayers based on density-functional theory (DFT). We show that the 2D TiX 3 monolayers are stable dynamically and thermodynamically as evidenced by phonon and molecular dynamics calculations, respectively, and show their semiconducting nature. We find that the TiBr 3 and TiI 3 monolayers are ferromagnetic with magnetic anisotropy out of plane, which are intrinsic without the need for external intervention. The magnetic anisotropy energies of the TiBr 3 and TiI 3 monolayers are 0.8 and 2.5 meV per s.f., respectively. The Curie temperatures of TiBr 3 and TiI 3 are 75 K and 90 K, respectively. We further show that the interlayer magnetic coupling and magnetic anisotropy energies (MAE) of the bilayer TiI 3 can be tuned by the interlayer distance. Additionally, a two-step transition in the magnetic state is observed in the bilayer TiI 3 with AB' stacking under applied strain in a vertical direction. It is expected that our design may enrich two-dimensional functional materials, which may find versatile applications.

Here, we report the extraordinary electrochemical energy storage capability of NiMoO 4 @NiMoO 4 homogeneous hierarchical nanosheet-on-nanowire arrays (SOWAs), synthesized on nickel substrate by a two-stage hydrothermal process. Comparatively speaking, the SOWAs electrode displays superior electrochemical performances over the pure NiMoO 4 nanowire arrays. Such improvements can be ascribed to the characteristic homogeneous hierarchical structure, which not only effectively increases the active surface areas for fast charge transfer, but also reduces the electrode resistance significantly by eliminating the potential barrier at the nanowire/nanosheet junction, an issue usually seen in other reported heterogeneous architectures. We further evaluate the performances of the SOWAs by constructing an asymmetric hybrid supercapacitor (ASC) with the SOWAs and activated carbon (AC). The optimized ASC shows excellent electrochemical performances with 47.2 Wh/kg in energy density of 1.38 kW/kg at 0-1.2 V. Moreover, the specific capacity retention can be as high as 91.4% after 4000 cycles, illustrating the remarkable cycling stability of the NiMoO 4 @NiMoO 4 //AC ASC device. Our results show that this unique NiMoO 4 @NiMoO 4 SOWA has great prospects for future energy storage applications.

Nanoscale self-assembly offers a pathway to realize heterogeneous integration of III-V materials on silicon. However, for III-V nanowires directly grown on silicon, dislocation-free single-crystal quality could only be attained below certain critical dimensions. We recently reported a new approach that overcomes this size constraint, demonstrating the growth of single-crystal InGaAs/GaAs and InP nanoneedles with the base diameters exceeding 1 μm. Here, we report distinct optical characteristics of InP nanoneedles which are varied from mostly zincblende, zincblende/wurtzite-mixed, to pure wurtzite crystalline phase. We achieved, for the first time, pure single-crystal wurtzite-phase InP nanoneedles grown on silicon with bandgaps of 80 meV larger than that of zincblende-phase InP. Being able to attain excellent material quality while scaling up in size promises outstanding device performance of these nanoneedles. At room temperature, a high internal quantum efficiency of 25% and optically pumped lasing are demonstrated for single nanoneedle as-grown on silicon substrate. Recombination dynamics proves the excellent surface quality of the InP nanoneedles, which paves the way toward achieving multijunction photovoltaic cells, long-wavelength heterostructure lasers, and advanced photonic integrated circuits.