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51.
    
Current aqueous Zn batteries (ZBs) seriously suffer from dendrite issues caused by rough electrode surfaces. Despite significant efforts in prolonging lifespan of these batteries, little effort has been devoted to dendrite elimination in commercial-grade cathode loading mass. Instead, demonstrations have only been done at the laboratory level (≤2 mg cm−2). Additionally, new dilemmas regarding change of the proton-storage behavior and interface pulverization have emerged in turn. Herein, hydrogen-substituted graphdiyne (HsGDY), with sub-ångström level ion tunnels and robust chemical stability, is designed as an artificial interface layer to address these issues. This strategy prolongs the symmetric cell lifespan to >2400 h (100 days), which is 37 times larger than without protection (63 h). The simulation of dual fields reveals that HsGDY can redistribute the Zn2+ concentration field by spatially forcing Zn2+ to deviate from the irregular electric field. During practical use, the as-assembled full batteries deliver a long lifespan 50 000 cycles and remain stable even at a commercial-grade cathode loading mass of up to 22.95 mg cm−2. This HsGDY-protection methodology represents great progress in Zn dendrite protection and demonstrates enormous potential in metal batteries.  相似文献   
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Graphdiyne (GDY), a 2D carbon allotrope, is predicted to possess high carrier mobility and an intrinsic bandgap. However, the controlled synthesis of mono‐ or few‐layer GDY with good crystallinity remains challenging because of the instability of the monomers. Herein, a rapid and catalyst‐free synthetic method is presented for few‐layer GDY involving the use of a solid/liquid interface and a microwave‐induced temperature gradient. Sodium chloride, which can absorb microwave energy, is used as the solid substrate in a nonabsorbing solvent. A temperature gradient is formed at the solid/liquid interface under microwave irradiation, facilitating the cross‐coupling reaction of monomers at the solid surface and stabilizing the monomers in the bulk solution. Few‐layer GDY with an average thickness of less than 2 nm, a field‐effect mobility of 50.1 cm2 V?1 s?1, and p‐type characteristics is successfully obtained. This wet chemical approach may be extended to the synthesis of other few‐layered 2D materials with improved quality.  相似文献   
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Despite recent progress in 2D nanomaterials‐based biosensing, it remains challenging to achieve sensitive and high selective detection. This study develops few‐layer graphdiyne (GD) nanosheets (NSs) that are used as novel sensing platforms for a variety of fluorophores real‐time detection of DNA with low background and high signal‐to‐noise ratio, which show a distinguished fluorescence quenching ability and different affinities toward single‐stranded DNA and double‐stranded DNA. Importantly, for the first time, a few‐layer GD NSs‐based multiplexed DNA sensor is developed.  相似文献   
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β‐Graphdiyne (β‐GDY) is a member of 2D graphyne family with zero band gap, and is a promising material with potential applications in energy storage, organic electronics, etc. However, the synthesis of β‐GDY has not been realized yet, and the measurement of its intrinsic properties remains elusive. In this work, β‐GDY‐containing thin film is successfully synthesized on copper foil using modified Glaser–Hay coupling reaction with tetraethynylethene as precursor. The as‐grown carbon film has a smooth surface and is continuous and uniform. Electrical measurements reveal the conductivity of 3.47 × 10?6 S m?1 and the work function of 5.22 eV. TiO2@β‐GDY nanocomposite is then prepared and presented with an enhancement of photocatalytic ability compared to pure TiO2.  相似文献   
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Comparing to other carbon materials, the general graphyne structure is much superior in terms of adaptable bandgap, uniformly distributed pores, more design flexibility, easier for chemical synthesis, pliable electronic properties, and smaller atomic density. Herein, novel γ‐graphdiyne quantum dots (GD QDs) are used in perovskite solar cells as a surface modifier or dopant to TiO2, CH3NH3PbI3, and Spiro‐OMeTAD to realize multiple advantageous effects, in hoping that it would form a more effective carrier transport channel for boosted solar cell performance. First, the presence of GD QDs on TiO2 surface increases perovskite grain size for higher current density and fill factor. Second, the GD QDs at each interface reduce the conduction band offset, passivate the surface for suppressed carrier recombination to attain higher open‐circuit voltage. Third, it improves hydrophobicity and eliminates pinholes in the Spiro‐OMeTAD film for enhanced solar cell stability. As a result, the optimized device shows >15% enhancement in power conversion efficiency (from 17.17 to 19.89%) comparing to the reference device. More significantly, the device stability was improved in harsh environment (moist air, UV irradiation, or thermal conditions). It is expected that GD QDs will find their applications in efficient and stable perovskite solar cells and optoelectronic devices.  相似文献   
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Mixed conducting materials with both ionic and electronic conductivities have gained prominence in emerging applications. However, exploring material with on-demand ionic and electronic conductivities remains challenging, primarily due to the lack of correlating macroscopic conductivity with atom-scale structure. Here, the correlation of proton–electron conductivity and atom-scale structure in graphdiyne is explored. Precisely adjusting the conjugated diynes and oxygenic functional groups in graphdiyne yields a tunable proton–electron conductivity on the order of 103. In addition, a wet-chemistry lithography technique for uniform preparation of graphdiyne on flexible substrates is provided. Utilizing the proton–electron conductivity and mechanical tolerance of graphdiyne, bimodal flexible devices serving as capacitive switches and resistive sensors are created. As a proof-of-concept, a breath–machine interface for sentence-based communication and self-nursing tasks with an accuracy of 98% is designed. This work represents an important step toward understanding the atom-scale structure–conductivity relationship and extending the applications of mixed conducting materials to assistive technology.  相似文献   
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Graphdiyne (GDY) is a fascinating graphene-like 2D carbon allotrope comprising sp and sp2 hybridized carbon atoms. However, GDY materials synthesized by solution-phase methods normally come as thick and porous films or amorphous powders with severely disordered stacking modes that obstruct macroscopic applications. Here, a facile and scalable synthesis of ultrathin holey graphdiyne (HGDY) nanosheets is reported via palladium/copper co-catalyzed homocoupling of 1,3,5-triethynylbenzene. The resulting freestanding 2D HGDY self-assembles into 3D foam-like networks which can in situ anchor clusters of palladium atoms on their surfaces. The Pd/HGDY hybrids exhibit high electrocatalytic activity and stability for the oxygen reduction reaction which outperforms that of Pt/C benchmark. Based on the ultrathin graphene-like sheets and their unique 3D interconnected macrostructures, Pd/HGDY holds great promise for practical electrochemical catalysis and energy-related applications.  相似文献   
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The high activity of nano-sized metal particles (NMPs) makes it easy to appear uncontrolled aggregation, which seriously affects Li/Na storage in electrode materials. Introducing adaptive substrates with proper affinity to NMPs is an effective strategy that optimizes the stability and capacity of the related electrodes. Herein, a comprehensive strategy for the fabrication of adaptive interfacial contacts between metallic Cu nanoparticles (NPs) and triphenyl-substituted triazine graphdiyne (TPTG) substrates is reported. The sp C in the acetylenic linkers and N heteroatoms in the triazine groups synergistically stabilized the Cu NPs loaded onto the TPTG substrates. The stabilizing effect of the TPTG substrate induces a reversible lattice change of the Cu NPs during the charge–discharge process, thus efficiently facilitating the stable transfer of Li+/Na+. Intrinsic mechanism analysis indicates that the heterojunction contact interface of Cu NPs/TPTG provides branched charge transfer pathways from Li/Na to the Cu NPs and TPTG substrates, which synergistically adjusts the affinity to Li/Na atoms and ultimately improves the electrochemical performance in Li/Na storage. The investigation of the structure–property relationship deepens the understanding of the function of heterointerfaces, which is essential for optimizing the performance of energy storage devices.  相似文献   
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