Electrospun Nanoparticle–Nanofiber Composites via a One‐Step Synthesis

A facile approach to synthesize and incorporate metal nanoparticles (NPs) into electrospun polymer nanofibers (NFs) wherein the electrospinning polymer acts as both a reducing agent for the metal salt precursor, as well as a protecting and templating agent for the ensuing NPs, is reported. Such a true one‐step process at ambient conditions and free of organic solvents is demonstrated using a system comprising AgNO₃ and poly(ethylene oxide) (PEO) at electrospinnable molecular weights of 600, 1000, or 2000 kDa. The PEO transforms Ag⁺ into AgNPs, a phenomenon that has not been previously possible at PEO molecular weights less than 20 kDa without the addition of a separate reducing agent and stabilizer or the application of heat. Results from X‐ray photoelectron spectroscopy and UV–Vis absorption spectrophotometry analyses support the formation of pseudo‐crown ethers in high molecular weight PEO as the mechanism in the development of NPs. The AgNPs reduce fiber diameter and enhance fiber quality (reduced beading) due to increased electrical conductivity. Interestingly, several of the NFs exhibit AgNP‐localized nanochain formation and protrusion from the NF surface that can be attributed to the combined effect of applied electrical field on the polymer and the differences between the electrical conductivity and polarizability of the polymer and metal NPs.     

One‐Step Formation of a Single Atomic‐Layer Transistor by the Selective Fluorination of a Graphene Film

In this study, the scalable and one‐step fabrication of single atomic‐layer transistors is demonstrated by the selective fluorination of graphene using a low‐damage CF₄ plasma treatment, where the generated F‐radicals preferentially fluorinated the graphene at low temperature (<200 °C) while defect formation was suppressed by screening out the effect of ion damage. The chemical structure of the C–F bonds is well correlated with their optical and electrical properties in fluorinated graphene, as determined by X‐ray photoelectron spectroscopy, Raman spectroscopy, and optical and electrical characterizations. The electrical conductivity of the resultant fluorinated graphene (F‐graphene) was demonstrated to be in the range between 1.6 kΩ/sq and 1 MΩ/sq by adjusting the stoichiometric ratio of C/F in the range between 27.4 and 5.6, respectively. Moreover, a unique heterojunction structure of semi‐metal/semiconductor/insulator can be directly formed in a single layer of graphene using a one‐step fluorination process by introducing a Au thin‐film as a buffer layer. With this heterojunction structure, it would be possible to fabricate transistors in a single graphene film via a one‐step fluorination process, in which pristine graphene, partial F‐graphene, and highly F‐graphene serve as the source/drain contacts, the channel, and the channel isolation in a transistor, respectively. The demonstrated graphene transistor exhibits an on‐off ratio above 10, which is 3‐fold higher than that of devices made from pristine graphene. This efficient transistor fabrication method produces electrical heterojunctions of graphene over a large area and with selective patterning, providing the potential for the integration of electronics down to the single atomic‐layer scale.     

Synergistic Effect of Mesoporous Co3O4 Nanowires Confined by N‐Doped Graphene Aerogel for Enhanced Lithium Storage

A one‐step multipurpose strategy is developed to realize a sophisticated design that simultaneously integrates three desirable components of nitrogen dopant, 3D graphene, and 1D mesoporous metal oxide nanowires into one hybrid material. This facile synthetic strategy includes a one‐step hydrothermal reaction followed by topotactic calcination. The utilization of urea as the starting reagent enables the precipitation of precursor nanowires and concurrent doping of nitrogen heteroatoms on graphene during hydrothermal reaction, while at the same time the graphene nanosheets are self‐assembled to afford a 3D scaffold. Detailed characterizations on the final calcined product are conducted to confirm the phase purity, porosity, nitrogen composition, and morphology. The integration of two building blocks, i.e., flexible graphene nanosheets and Co₃O₄ nanowires, enables various intertwining behaviors such as seaming, bridging, hooping, bundling, and sandwiching, of which synergistic effect substantially enhances electrical and electrochemical properties of the resultant hybrid. For lithium ion battery application of the hybrid, a remarkably high capacity more than 1200 mA h g^?1 (at 100 mA g^?1) is stabilized over 100 cycles with coulombic efficiency higher than 97%. Even during rapid discharge/charge processes (1000 mA g^?1), a reversible charge capacity of 812 mA h g^?1 is still retained after 230 cycles.     

含氮石墨烯量子点的制备及其光学性质研究

采用水热法一步合成了含氮石墨烯量子点(NGQDs), 通过原子力显微镜(AFM)、透射电镜(TEM)、X射线光电子能谱(XPS)等对NGQDs的形貌和组成进行表征, 并进一步通过紫外-可见光谱(UV-Vis)、荧光光谱(PL)等手段研究了NGQDs的光学性质。AFM和TEM分析结果表明, NGQDs尺寸约为8.9 nm、厚度为0.6 ~2.0 nm (即1~3个碳原子层)。XPS分析结果表明NGQDs中氮含量约为17%, 且氮元素主要以“吡咯N”形式存在。光谱学实验表明, NGQDs的激发光谱与吸收光谱基本一致, 且其发射光谱与激发波长之间不存在依赖关系。此外, NGQDs的量子产率为~18%, 并随着含氮量的增加而增加, 且其荧光寿命衰变曲线可以被拟合成很好的双指数衰变曲线(τ₁=2.93 ns, τ₂=9.00 ns), 表明NGQDs有两种发色源, 即边缘富有含氧官能团的sp²碳簇和含氮五元环-吡咯环。     

Low‐Coordinate Step Atoms via Plasma‐Assisted Calcinations to Enhance Electrochemical Reduction of Nitrogen to Ammonia

The electrochemical N₂ reduction reaction (NRR) is emerging as a promising alternative to the industrial Haber–Bosch process for distributed and modular production of NH₃. Nevertheless, developing high‐efficiency catalysts to simultaneously realize both high activity and selectivity for the development of a sustainable NRR is very critical but extremely challenging. Here, a unique plasma‐assisted strategy is developed to synthesize iridium diphosphide nanocrystals with abundant surface step atoms anchored in P,N‐codoped porous carbon nanofilms (IrP₂@PNPC‐NF), where the edges of the IrP₂ nanocrystals are extremely irregular, and the ultrathin PNPC‐NF possesses a honeycomb‐like macroporous structure. These characteristics ensure that IrP₂@PNPC‐NF delivers superior NRR performance with an NH₃ yield rate of 94.0 µg h^?1 mg^?1_cat. and a faradaic efficiency (FE) of 17.8%. Density functional theory calculations reveal that the unique NRR performance originates from the low‐coordinate step atoms on the edges of IrP₂ nanocrystals, which can lower the reaction barrier to improve the NRR activity and simultaneously inhibit hydrogen evolution to achieve a high FE for NH₃ formation. More importantly, such a plasma‐assisted strategy is general and can be extended to the synthesis of other high‐melting‐point noble‐metal phosphides (OsP₂@PNPC‐NF, Re₃P₄@PNPC‐NF, etc.) with abundant step atoms at lower temperatures.     

Defect‐Enriched Nitrogen Doped–Graphene Quantum Dots Engineered NiCo2S4 Nanoarray as High‐Efficiency Bifunctional Catalyst for Flexible Zn‐Air Battery

Flexible Zn‐air batteries have recently emerged as one of the key energy storage systems of wearable/portable electronic devices, drawing enormous attention due to the high theoretical energy density, flat working voltage, low cost, and excellent safety. However, the majority of the previously reported flexible Zn‐air batteries encounter problems such as sluggish oxygen reaction kinetics, inferior long‐term durability, and poor flexibility induced by the rigid nature of the air cathode, all of which severely hinder their practical applications. Herein, a defect‐enriched nitrogen doped–graphene quantum dots (N‐GQDs) engineered 3D NiCo₂S₄ nanoarray is developed by a facile chemical sulfuration and subsequent electrophoretic deposition process. The as‐fabricated N‐GQDs/NiCo₂S₄ nanoarray grown on carbon cloth as a flexible air cathode exhibits superior electrocatalytic activities toward both oxygen reduction reaction (ORR) and oxygen evolution reaction (OER), outstanding cycle stability (200 h at 20 mA cm^?2), and excellent mechanical flexibility (without observable decay under various bending angles). These impressive enhancements in electrocatalytic performance are mainly attributed to bifunctional active sites within the N‐GQDs/NiCo₂S₄ catalyst and synergistic coupling effects between N‐GQDs and NiCo₂S₄. Density functional theory analysis further reveals that stronger OOH* dissociation adsorption at the interface between N‐GQDs and NiCo₂S₄ lowers the overpotential of both ORR and OER.     

Hierarchical 3D All‐Carbon Composite Structure Modified with N‐Doped Graphene Quantum Dots for High‐Performance Flexible Supercapacitors

Flexible supercapacitors have shown enormous potential for portable electronic devices. Herein, hierarchical 3D all‐carbon electrode materials are prepared by assembling N‐doped graphene quantum dots (N‐GQDs) on carbonized MOF materials (cZIF‐8) interweaved with carbon nanotubes (CNTs) for flexible all‐solid‐state supercapacitors. In this ternary electrode, cZIF‐8 provides a large accessible surface area, CNTs act as the electrical conductive network, and N‐GQDs serve as highly pseudocapactive materials. Due to the synergistic effect and hierarchical assembly of these components, N‐GQD@cZIF‐8/CNT electrodes exhibit a high specific capacitance of 540 F g^?1 at 0.5 A g^?1 in a 1 m H₂SO₄ electrolyte and excellent cycle stability with 90.9% capacity retention over 8000 cycles. The assembled supercapacitor possesses an energy density of 18.75 Wh kg^?1 with a power density of 108.7 W kg^?1. Meanwhile, three supercapacitors connected in series can power light‐emitting diodes for 20 min. All‐solid‐state N‐GQD@cZIF‐8/CNT flexible supercapacitor exhibits an energy density of 14 Wh kg^?1 with a power density of 89.3 W kg^?1, while the capacitance retention after 5000 cycles reaches 82%. This work provides an effective way to construct novel electrode materials with high energy storage density as well as good cycling performance and power density for high‐performance energy storage devices via the rational design.     

One‐Step Transfer and Integration of Multifunctionality in CVD Graphene by TiO2/Graphene Oxide Hybrid Layer

We present a straightforward method for simultaneously enhancing the electrical conductivity, environmental stability, and photocatalytic properties of graphene films through one‐step transfer of CVD graphene and integration by introducing TiO₂/graphene oxide layer. A highly durable and flexible TiO₂ layer is successfully used as a supporting layer for graphene transfer instead of the commonly used PMMA. Transferred graphene/TiO₂ film is directly used for measuring the carrier transport and optoelectronic properties without an extra TiO₂ removal and following deposition steps for multifunctional integration into devices because the thin TiO₂ layer is optically transparent and electrically semiconducting. Moreover, the TiO₂ layer induces charge screening by electrostatically interacting with the residual oxygen moieties on graphene, which are charge scattering centers, resulting in a reduced current hysteresis. Adsorption of water and other chemical molecules onto the graphene surface is also prevented by the passivating TiO₂ layer, resulting in the long term environmental stability of the graphene under high temperature and humidity. In addition, the graphene/TiO₂ film shows effectively enhanced photocatalytic properties because of the increase in the transport efficiency of the photogenerated electrons due to the decrease in the injection barrier formed at the interface between the F‐doped tin oxide and TiO₂ layers.     

N2‐Plasma‐Assisted One‐Step Alignment and Patterning of Graphene Oxide on a SiO2/Si Substrate Via the Langmuir–Blodgett Technique

Precise control of the placement and patterning of graphene on various substrates has tremendous impact in many fields, such as nanoscale electronics, multifunctional optoelectronic devices, and molecular sensing. A one‐step facile technique involving N₂‐plasma promotes surface modification and enhances the surface wettability of the substrate. The technique is employed to create partially hydrophilic surfaces on SiO₂/Si substrate with the aid of various templates, enabling the selective deposition, alignment, and formation of patterns comprising monolayer graphene oxide (GO) sheets; it successfully uses the Langmuir–Blodgett (LB) deposition technique over a large area without the need of any sophisticated equipment. Various characterization techniques are carried out in order to understand the possible mechanism behind the pinning of the GO on the partially treated areas. It is a relatively easy and swift process that can reliably accomplish specific surface modification with high bonding strength between GO and the substrate. This technique allows the creation of patterns with controllable dimensions. For example, the thickness of the GO sheets can be controlled; this is particularly important in creating arrays and devices at wafer‐scale. Being simple yet effective and inexpensive, this technique holds tremendous potential that can be exploited for numerous applications in the field of bio‐nanoelectronics.     

In Situ Grown Monolayer N‐Doped Graphene on CdS Hollow Spheres with Seamless Contact for Photocatalytic CO2 Reduction

Photocatalytic CO₂ reduction is an effective way to simultaneously mitigate the greenhouse effect and the energy crisis. Herein, CdS hollow spheres, on which monolayer nitrogen‐doped graphene is in situ grown by chemical vapor deposition, are applied for realizing effective photocatalytic CO₂ reduction. The constructed photocatalyst possesses a hollow interior for strengthening light absorption, a thin shell for shortening the electron migration distance, tight adhesion for facilitating separation and transfer of carriers, and a monolayer nitrogen‐doped graphene surface for adsorbing and activating CO₂ molecules. Achieving seamless contact between a photocatalyst and a cocatalyst, which provides a pollution‐free and large‐area transport interface for carriers, is an effective strategy for improving the photocatalytic CO₂ reduction performance. Therefore, the yield of CO and CH₄, as dominating products, can be increased by four and five times than that of pristine CdS hollow spheres, respectively. This work emphasizes the importance of contact interface regulation between the photocatalyst and the cocatalyst and provides new ideas for the seamless and large‐area contact of heterojunctions.     

Controlled Synthesis of One‐Dimensional Inorganic Nanostructures Using Pre‐Existing One‐Dimensional Nanostructures as Templates

Template‐directed strategy has become one of the most popular methods for the fabrication of one‐dimensional (1D) nanostructures with uniform size and controllable physical dimensions in recent years. This Review article describes the recent progress in the synthesis of 1D inorganic nanostructures by using suitable templates. A brief survey on the templating method based on the organic templates and porous membrane is firstly given. Then, the article is focused on recent emerging synthetic strategies by templating against the pre‐existing 1D nanostructures using different physical and chemical transformation techniques, including epitaxial growth, nonepitaxial growth, direct chemical transformation, solid‐state interfacial diffusion reaction, and so on. The important reactivity role of the 1D nanostructures will be emphasized in such transformation process. Finally, we conclude this paper with some perspectives and outlook on this research topic.     

Photoconductivity of Bulk‐Film‐Based Graphene Sheets

Time‐resolved photoconductivity measurements are carried out on graphene films prepared by using soluble graphene oxide. High photocurrent generation efficiency is observed for these graphene‐based films, and the relationships between their photoconductivity and different preparation methods, incident light intensity, external electric field, and photon energies are investigated. Higher photoconductivity is observed with higher photon energy at same incident light intensity. By fitting the experimental data to the Onsager model, the primary quantum yields for charge separation to generate bound electron–hole pairs and the initial ion‐pair thermalization separation distance are calculated.     

Polyphenol/FeIII Complex Coated Membranes Having Multifunctional Properties Prepared by a One‐Step Fast Assembly

The membrane filtration process has received much attention as one of the most promising water purification techniques. However, it still has several disadvantages, such as organic‐, oil‐, and biofouling, membrane contamination by microorganisms, and the difficulty in rejecting heavy metal ions, which are closely related to the membrane surface properties. Various approaches have been used to prepare membranes with antifouling, antimicrobial, or heavy metal ion removal properties on their surfaces. However, membranes with all these properties have not yet been reported. It might be possible to prepare membranes with such multifunctional properties by modifying the membrane surfaces with various organic and/or inorganic functional materials using multiple chemical/physical modification procedures, though the process should be very tedious, costly, and time consuming. Here, a multifunctional filtration membrane is prepared by a rapid one‐step assembly coating of tannic acid and iron ion (Fe^III) on a commercial poly(ether sulfone) membrane. The catechol‐ and gallol‐rich surfaces combine all of the desirable properties such as antifouling against proteins, oils, and microorganisms, as well as antimicrobial and heavy metal ion removal properties. This study provides a facile approach to prepare multifunctional filtration membranes that have potential applications in practical water purification.