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Flexible three-dimensional interconnected carbon nanotubes on the carbon cloth (3D-CNTs/CC) were obtained through simple magnesium reduction reactions. According to the Nernst equation, the cell voltage based on these pure carbon electrodes without any additives could reach 1.5 V due to the higher di-hydrogen evolution over potential in neutral 3.5 M LiCl electrolytes. In order to improve the electrochemical performance of the electrodes, 3D-CNTs/CC electrodes covered with polyaniline barrier layer (3D-PANI/CNTs/CC) were prepared by in situ electropolymerization using interfacial engineering method. The assembled symmetric supercapacitors display a broadened voltage of 1.8 V, high areal capacitance of 380 mF cm−2, outstanding areal energy density of 85.5 μWh cm−2 and 84% of its initial capacitance after 20 000 charge-discharge cycles. This work demonstrated that the interface engineering strategy provides a promising way to improve the energy density of carbon-based aqueous supercapacitors by widening the voltage and boosting the capacitance simultaneously.

Precise control of the structure and bonds of doped carbon dots (CDs) is important, so that their fluorescence can be tuned as desired. Up until now, there has been a lack of effective ways to control the bonds of doped CDs. In this article, we show that the fluorescence of B/N-doped carbon dots (B/N-CDs) can be precisely tuned just by controlling their precursors’ pH values. The prepared B/N-CDs exhibit two emission bands, including one emission peak at around 450 nm due to the defect state caused by low sp2 hybridization of carbon atoms, as well as another emission peak at around 360 nm caused by the B-N bond. The results for the ratio of the maximum intensity of the two emission peaks above show a linear relationship. Meanwhile, the role of the pH value of the precursors on the luminescence of B/N-CDs is deeply studied. On the one hand, the pH value affects the bonding process of CDs. N-H bonds tend to form at a low pH value, while more competitive B-N bonds exist at much higher pH value, leading to the pH-dependent intensity of the 360 nm emission band. On the other hand, a high pH value causes higher crystallinity, thus suppressing defect-state fluorescence at 450 nm. The dual effects of pH lead to precisely controlled dual-emission intensities as well as ratiometric fluorescence.

Large-size luminescent solar concentrators (LSCs), which act as a complement to silicon-based photovoltaic (Si-PV) systems, still suffer from low power conversion efficiency (PCE). How to improve the performance of LSCs, especially large ones, is currently a hot research topic. Traditional LSCs have only a single transmission mode of fluorescence from the luminescent materials to the Si-PV, but here we introduce a new idea to improve the absorption of Si-PV by employing dual transmission modes of both fluorescence and scattering light. To prepare LSCs with dual mode transmission, Si-PV systems are coupled around the edges of a light-harvesting slice, which is prepared by ultraviolet light-induced polymerization of methyl methacrylate (MMA) solution containing both luminescent CsPbBr3 and TiO2 nanocrystals (NCs). When the sun light or incident light is coupled into the light-harvesting slice, CsPbBr3 NCs can convert the incident light into fluorescence, and then partly transmit to Si-PV at the edges, where the light is finally converted into electrical energy. Besides the traditional fluorescence transmission mode, the addition of TiO2 brings another transmission mode, namely the scattering of incident light to Si-PV, leading to an increase in PCE. In comparison to that of pure CsPbBr3-based LSCs without the addition of TiO2 (0.97%), the PCE of TiO2-doped LSCs with a large size of 20 cm × 20 cm is improved to 1.82%. The maximal PCE appears for LSCs with a size of 5 cm × 5 cm, reaching 2.62%. The reported method of dual transmission modes is a new alternative way to improve the performance of LSC devices, which does not need to change the optical properties of luminescent materials. Moreover, the production process is simple, low-cost and suitable for preparing large area LSCs, further promoting the application of LSCs.

Amongst the different graphene fabrication techniques, bipolar electrochemistry (BPE) has been recently reported as a simple, controllable, low cost, eco-friendly, and scalable method. It consists of a wirelessly placed carbon source between two feeding electrodes subjected to direct current (DC) voltage in a deionized water bath. Although the physicochemical characteristics of produced graphene have been evaluated, the exfoliation and deposition mechanisms are still unclear. In this study, a novel modified BPE system with an electrically-connected graphite-platinum couple acting as the bipolar electrode has been designed in order to decouple and investigate the contribution of anodic/cathodic exfoliation and deposition of graphene in the BPE process. Electron microscopy and Fourier transform infrared spectroscopy results indicate that both anodic and cathodic exfoliation of graphene could take place regardless of the type of polarization; however, the morphology and deposition rate highly depend on the polarization. Furthermore, the graphene fabricated by anodic exfoliation was found to show higher levels of oxidation compared to the graphene produced by cathodic exfoliation.

Antimony (Sb) anode has attracted increasing attention given its high theoretical capacity and suitable working potential. Nonetheless, its practical application is largely hindered by huge volume changes during the cyclic process, resulting in unsatisfactory long-term cycled stabilities at high current density. In this work, large-scale ultrafine Sb nanoparticles are functionally designed to encapsulate into a 3D carbon microfiber framework (CMF) via a scalable electrospinning approach followed by a thermal treatment process. This fabrication strategy effectively avoids the change in the volume of the Sb anode and provides a fast conductive network to serve as an efficient 3D e/Li+ transport pathway. Benefiting from this novel structural design, an ultrafine Sb nanoparticles@carbon microfiber framework (U-Sb-NPs@CMF) composite anode used for lithium-ion batteries (LIBs) delivers a high reversible capacity of 622 mAh g-1 after 200 cycles at 0.5 A g-1 and 507 mAh g-1 after 2000 cycles at 2 Ag-1 and a high-capacity retention of 350 mAh g-1 even after 5000 long-term cycles. These outstanding charge-discharge performances suggest that the U-Sb-NPs@CMF composite is a promising candidate for an anode material in the application of LIBs.

Graphene fibers are promising candidates in portable and wearable electronics due to their tiny volume, flexibility and wearability. Here, we successfully synthesized macroscopic graphene composite fibers via a two-step process, i.e. first electrospinning and then chemical vapor deposition (CVD). Briefly, the well-dispersed PAN nanofibers were sprayed onto the copper surface in an electrified thin liquid jet by electrospinning. Subsequently, CVD growth process induced the formation of graphene films using a PAN-solid source of carbon and a copper catalyst. Finally, crumpled and macroscopic graphene composite fibers were obtained from carbon nanofiber/graphene composite webs by self-assembly process in the deionized water. Temperature-dependent conduct behavior reveals that electron transport of the graphene composite fibers belongs to hopping mechanism and the typical electrical conductivity reaches 4.59 × 103 S m-1. These results demonstrated that the graphene composite fibers are promising for the next-generation flexible and wearable electronics.

CH

CH3NH3PbBr3 perovskite nanocrystals (NCs) suffer from poor stability because of their high sensitivity to environmental moisture and water. To solve this problem, previous works mainly focus on embedding perovskite NCs into water-resistant matrix to form large composites (size of microns or larger). As an alternative solution without serious changing of NC size, enhancing the stability of perovskite NCs themselves by ligand engineering is rarely reported. In this work, we used hyperbranched polyamidoamine (PAMAM) dendrimers with two different generations (G0 and G4) to synthesize CH3NH3PbBr3 perovskite NCs with high photoluminescence (PL) quantum yields (QY) above 70% and a new record stability. A novel dendrimers generation-dependent stability of perovskite NCs was observed. The water-resistance time is 18 h (27 h) for perovskite NCs capped by G0 (G4) generation of PAMAM, which is 7 times (11 times) longer than that of traditional oleic acid-capped NCs. Similar PAMAM generation-related stability is also observed in moisture-resistance tests. The stability time against moisture is 500 h (800 h) for G0 (G4) generation of PAMAM-capped perovskite NCs, which is a new record stability time against moisture for CH3NH3PbBr3 perovskite NCs. In addition, our results also indicate that PAMAM ligands outside perovskite NCs can dramatically slow down the speed of halide exchange. Even for the mixture of perovskite NCs with two different halide composition, the original luminescence properties of PAMAM-capped perovskite NCs can retain after mixing. In view of slow halide exchange speed, excellent water and moisture stability, PAMAM dendrimers-capped perovskite NCs and their mixture are available as color conversion single layer in fabrication of light-emitting diodes (LED).

Graphene nanomeshes (GNMs), new graphene nanostructures with tunable bandgaps, are potential building blocks for future electronic or photonic devices, and energy storage and conversion materials. In previous works, GNMs have been successfully prepared on Cu foils by the H2 etching effect. In this paper, we investigated the effect of Ar on the preparation of GNMs, and how the mean density and shape of them vary with growth time. In addition, scanning electron microscopy (SEM) and high resolution transmission electron microscopy (TEM) revealed the typical hexagonal structure of GNM. Atomic force microscopy (AFM) and x-ray photoelectron spectroscopy (XPS) indicated that large copper oxide nanoparticles produced by oxidization in purified Ar can play an essential catalytic role in preparing GNMs. Then, we exhibited the key reaction details for each growth process and proposed a growth mechanism of GNMs in purified Ar.

Graphene films have been attracting great interest owing to their unique physical properties. In this paper, we develop an efficient method to prepare large-area monolayer graphene (97.5% coverage) by atmospheric pressure chemical vapor deposition on Cu foils using polystyrene in a short time (3 min). Raman spectroscopy, transmission electron microscopy and scanning electron microscopy are employed to confirm the thickness and uniformity of the graphene films. Graphene films on glass substrates show high optical transmittance and electrical conductivity. Magnetic transport studies demonstrate that the as-grown monolayer graphene exhibits a high carrier mobility of 3395 cm2 V-1 s-1 at 25 K. On the basis of the analysis, it is concluded that our method is a simple, safe and versatile approach for the synthesis of monolayer graphene.

In the conventional synthesis of aqueous ZnSe quantum dots (QDs), highly reactive Se monomers are rapidly injected into a Zn-thiol complexes solution at room temperature, resulting in a poor excitionic luminescence and a serious trap emission of as-prepared ZnSe QDs. In this paper, we develop a novel cation-inverting-injection method to prepare aqueous ZnSe QDs with a bright excitionic luminescence. In this method, highly reactive Se monomers are first diluted in the reaction solution, followed by low-reaction Zn-thiol complexes slowly dropped at a high reaction temperature (90 °C). The inverting monomer injection order, the suppressed monomer reactivity and the high nucleation temperature in the cation-inverting-injection method can contribute to low-concentration but high-quality ZnSe nuclei, thereby promoting the formation of ZnSe QDs with large-sized particles, a high excitionic emission and a weak trap emission. As-prepared ZnSe QDs exhibit an intense deep-blue excitionic emission, which is the first reported case of a visible excitionic emission instead of a trap emission resulting from ZnSe QDs that are directly synthesized in an aqueous media. Using three types of dyes, via two measuring methods, the accurate photoluminescence quantum yield of the as-prepared ZnSe QDs is measured as 15%, which is a new record for mercaptocarboxylic acid stabilized ZnSe QDs synthesized in an aqueous media.

In this work, highly luminescent quaternary CuNiInS nanocrystals (NCs) are put forward as a good prototype for investigating defect-induced room temperature ferromagnetism. A ferromagnetic Ni cation can preserve the strong luminescence of NCs without introducing intermediate energy levels in the center of the forbidden band. The strong luminescence of NCs is used as an indicator for monitoring the concentration of vacancy defects inside them, facilitating the investigation of the origin of room temperature ferromagnetism in CuNiInS NCs. Our results reveal that the patching of Cu vacancies [Formula: see text] with Ni will result in bound magnetic polarons composed of both [Formula: see text] and a substitution of Cu by Ni [Formula: see text] giving rise to the room temperature ferromagnetism of CuNiInS NCs. Either the ferromagnetic Ni or the non-ferromagnetic Cu cation can tune the magnetism of CuNiInS NCs because of the change of bound magnetic polaron concentration at the altered concentration ratio of [Formula: see text] and [Formula: see text].

Using ZnSe nanocrystals (NCs) as starting material, Ag-doped or Cu-doped ZnCdSe ternary NCs were prepared by hydrazine-promoted sequential cation exchange in aqueous media. The composition of the NCs can be flexibly controlled by varying the amount of intermediate Ag or Cu cation addition, thus changing the emission of the ternary NCs while preserving the NC size. According to Vegard's law, the as-prepared ternary NCs possess an alloyed structure. In addition, the ternary NCs obtained have a high quantum yield, strong stability and a broad optical tuning range.

In this work, we used Ag- and Mn-doped ZnInS/ZnS quantum dots (QDs) acting as a new generation of nontoxic dual-emission QDs with simultaneous tunable emission wavelengths and dual-emission ratiometric, which makes nontoxic dual-emission QDs with broad zone tunability in the color coordinate. The Ag-doped ZnInS ternary QDs can give rise to largely tunable emission wavelengths from 497 nm to 631 nm. The ratiometric of Ag and Mn dual emissions can be tuned by controlling Ag–Mn and Mn–Mn dopant coupling. With increased Mn doping amount, the increased Ag–Mn dopant coupling leads to increased Mn emission at the expense of lowered Ag emission and Ag fluorescence lifetime. The Mn–Mn coupling can be controlled by using different doping manners: co-doping Ag and Mn in ZnInS core or separate-doping Ag in ZnInS core and Mn in ZnS shell. Compared with co-doping, separate doping has weaker Mn–Mn interactions, an increased Mn irradiative recombination rate constant, and bright Mn photoluminescence.

pH-sensitive photoluminescence (PL) is an important property of aqueous nanocrystals (NCs) towards NCs-based intelligent applications. Previous works mainly focused on the effect of pH during NC growth process on PL of the aqueous NCs. The effect of pH during application process on PL of as-prepared NCs is still not fully understood. In this work, we brought out a general mechanism for the pH-sensitive PL behaviors of as-prepared aqueous CdTe NCs capped by aqueous thiol ligands, such as carboxylic-acid-terminated 3-mercaptopropionic acid (MPA) and thioglycolic acid (TGA) ligands, hydroxyl-terminated 1-thioglycerol (TG) ligands and amine-terminated 2-mercaptoethylamine (MA) ligands. A major contribution of this work is finding the key role of ligand terminal groups in the diffuse process of free Cd–ligand complexes toward NCs. This terminal group effect is the main reason for PL alteration of NCs during pH adjustment process. Besides the terminal group effect, PL of aqueous NCs is also affected by the aggregation effect, the thiol group effect and the counter ion effect. These effects make different contributions to PL of NCs at different pH ranges. By using this mechanism, we successfully explained the complex pH-sensitive PL behaviors of MPA, TGA, TG and MA-capped CdTe NCs.

To prepare biologically available Zn-based NCs in aqueous solution, we herein reported the synthesis of aqueous Cu:ZnSe/ZnS NCs with internally doped aqueous Cu:ZnSe NCs as the core template. Due to the dual protection of Cu impurities by the ZnSe core and ZnS shells, the as-prepared Cu:ZnSe/ZnS NCs show excellent stability in the open air, which overcomes the intrinsic instability of traditional aqueous Cu:ZnSe NCs. The as-prepared Cu:ZnSe/ZnS NCs possess extremely good stability, good biocompatibility and lower cytotoxicity, and thus can be used as a promising candidate for fluorescent NC-based biological applications.

Synthesis of internally doped Cu:ZnSe QDs in an aqueous solution still suffers from narrow tunable emissions from the blue to green light window. In this work, we extended the emission window of aqueous Cu:ZnSe QDs to the yellow light window. Our results show that high solution pH, multiple injections of Zn precursors, and nucleation doping strategy are three key factors for preparing yellow emitted Cu:ZnSe QDs. All these factors can depress the reactivity of CuSe nuclei and Zn monomers, promoting ZnSe growth outside CuSe nuclei rather than form ZnSe nuclei separately. With increased ZnSe QD size, the conduction band and nearby trap state energy levels shift to higher energy sites, causing Cu:ZnSe QDs to have a much longer emission.

This work wants to give a caution for monitoring the surface modification of dually emitted ZnSe quantum dots (QDs) by using time-resolved photoluminescence (PL). Aqueous ZnSe QDs have two emission bands: namely ZnSe band gap emission centered at 395 nm and ZnSe trap emission centered at 470 nm. By fitting the measured PL spectra by two peaks, serious overlapping of two emission bands can be found in the range of 360-430 nm. As a result, the measured PL lifetimes at 395 nm (the peak position of ZnSe band gap emission) is just an apparent value, composing of both ZnSe band emission (contribution proportion about 80%) and ZnSe trap emission (contribution proportion about 20%). Due to the much smaller PL lifetime of ZnSe band gap emission (less than 20 ns) than that of ZnSe trap emission (about 50-70 ns), the elevated contribution proportion of ZnSe band gap emission at improved QD surface modification will lead to the decreased average PL lifetime at 395 nm. This result is completely opposite to the traditional result where improved QD surface modification leads to increased PL lifetimes on the basis of single emitted QDs. Hence, when time-resolved PL is used for monitoring the surface modification of dually emitted QDs, the emission bands overlapping should be taken into consideration with caution.

A simple one-step process was developed for the preparation of stable Ag nanoparticles with high yield. Direct solvothermal treatment of an ethanol solution of AgNO3 and dodecanethiol (DT) resulted in the formation of Ag nanoparticles. X-ray powder diffraction (XRD) analysis indicated that the solid was composed of fcc-structured metal Ag. Infrared (IR) spectroscopy analysis demonstrated the presence of DT in the products. Transmission electron microscopy (TEM) showed that the particle size could be tuned from 5?nm to 100?nm by changing the synthesis parameters. The samples were stable (no irreversible precipitation) in the solid state for more than 8 months and could be redispersed into nonpolar organic solvent (cyclohexane) to form stable colloidal dispersions. A possible formation and size evolution mechanism is proposed.