The dual-emissive N, S co-doped carbon dots (N, S-CDs) with a long emission wavelength were synthesized via solvothermal method. The N, S-CDs possess relatively high photoluminescence (PL) quantum yield (QY) (35.7%) towards near-infrared fluorescent peak up to 648 nm. With the advanced characterization techniques including X-ray photoelectron spectroscopy (XPS), Fourier transform infrared spectroscopy (FTIR), etc. It is found that the doped N, S elements play an important role in the formation of high QY CDs. The N, S-CDs exist distinct pH-sensitive feature with reversible fluorescence in a good linear relationship with pH values in the range of 1.0–13.0. What is more, N, S-CDs can be used as an ultrasensitive Ag+ probe sensor with the resolution up to 0.4 μM. This finding will expand the application of as prepared N, S-CDs in sensing and environmental fields.
Neutral water splitting is attractive for its use of non-corrosive and environmentally friendly electrolytes. However, catalyst development for hydrogen and oxygen evolution remains a challenge under neutral conditions. Here we report a simple electrodeposition and reductive annealing procedure to produce a highly active Ni-Co-Cr metal/metal oxide heterostructured catalyst directly on Ni foam. The resulting electrocatalyst for hydrogen evolution reaction (HER) requires only 198 mV of overpotential to reach 100 mA/cm2 in 1 M potassium phosphate (pH = 7.4) and can operate for at least two days without significant performance decay. Scanning transmission electron microscopy coupled with electron energy loss spectroscopy (STEM-EELS) imaging reveals a Ni-Co alloy core decorated with blended oxides layers of NiO, CoO and Cr2O3. The metal/metal oxide interfaces are suggested to be responsible for the high HER activity.
All-inorganic cesium lead halide perovskite quantum dots (QDs) have been a promising candidate for optoelectronic devices in recent years, such as light-emitting diodes, photodetectors and solar cells, owing to their superb optoelectronic properties. Still, the stability issue of nanocrystals is a bottleneck for their practical application. Herein, we report a facile method for the synthesis of a series of phosphine ligand modified CsPbBr3 QDs with high PL intensity. By introducing organic phosphine ligands, the tolerance of CsPbBr3 QDs to ethanol, water and UV light was dramatically improved. Moreover, the phosphine ligand modified QD films deposited on the glass subtracts exhibit superior PL intensity and optical stability to those of pristine QD based films.
Graphene-h-BN hybrid nanostructures are grown in one step on the Pt(111) surface by ultra-high vacuum chemical vapor deposition using a single precursor, the dimethylamino borane complex. By varying the deposition conditions, different nanostructures ranging from a fully continuous hybrid monolayer to well-separated Janus nanodots can be obtained. The growth starts with heterogeneous nucleation on morphological defects such as Pt step edges and proceeds by the addition of small clusters formed by the decomposition of the dimethylamino borane complex. Scanning tunneling microscopy measurements indicate that a sharp zigzag in-plane boundary is formed when graphene grows aligned with the Pt substrate and consequently with the h-BN layer as well. When graphene is rotated by 30°, the graphene armchair edges are seamlessly connected to h-BN zigzag edges. This is confirmed by a thorough density functional theory (DFT) study. Angle resolved photoemission spectroscopy (ARPES) data suggests that both h-BN and graphene present the typical electronic structure of self-standing non-interacting materials.
In this work, homogeneous Ni0.33Co0.67Se hollow nanoprisms were synthesized successfully in virtue of Kirkendall effect. It is the first time for bimetallic Ni-Co compounds Ni0.33Co0.67Se to be used in lithium-ion batteries (LIBs). Impressively, the Ni0.33Co0.67Se hollow nanoprisms show superior specific capacity (1,575 mAh/g at the current density of 100 mA/g) and outstanding rate performance (850 mAh/g at 2,000 mA/g) as anode material for LIBs. This work proves the potential of bimetallic chalcogenide compounds as high performance anode materials for LIBs.
Colloidal nanoparticles with anisotropic architectures have attracted a variety of interest and attention due to different physical and chemical properties compared with the isotropic counterparts, making them promising candidates in many fundamental studies and practical applications. Particularly, carbon and silica-based anisotropic nanoparticles can be one stand out by combing both intrinsic merits of carbons and silica, such as structural stability, biocompatibility, large surface area, and ease of functionalization with the anisotropic structural complexity. In this review, we aim to provide an updated summary of the research related to the anisotropic carbon and silica-based nanostructures, covering both their synthesis and applications.
Two-dimensional (2D) nanomaterials have attracted a great deal of attention since the discovery of graphene in 2004, due to their intriguing physicochemical properties and wide-ranging applications in catalysis, energy-related devices, electronics and optoelectronics. To maximize the potential of 2D nanomaterials for their technological applications, controlled assembly of 2D nanobulding blocks into integrated systems is critically needed. This mini review summarizes the reported strategies of 2D materials-based assembly into integrated functional nanostructures, from in-situ assembly method to post-synthesis assembly. The applications of 2D assembled integrated structures are also covered, especially in the areas of energy, electronics and sensing, and we conclude with discussion on the remaining challenges and potential directions in this emerging field.
DNA is a self-assembled, double stranded natural molecule that can chelate and align nickel ions between its base pairs. The fabrication of a DNA-guided nickel ion chain (Ni-DNA) device was successful, as indicated by the conducting currents exhibiting a Ni ion redox reaction-driven negative differential resistance effect, a property unique to mem-elements (1). The redox state of nickel ions in the Ni-DNA device is programmable by applying an external bias with different polarities and writing times (2). The multiple states of Ni-DNA-based memristive and memcapacitive systems were characterized (3). As such, the development of Ni-DNA nanowire device-based circuits in the near future is proposed.
Electrochemical N2 reduction offers a promising alternative to the Haber-Bosch process for sustainable NH3 synthesis at ambient conditions, but it needs efficient catalysts for the N2 reduction reaction (NRR). Here, we report that FeOOH quantum dots decorated graphene sheet acts as a superior catalyst toward enhanced electrocatalytic N2 reduction to NH3 under ambient conditions. In 0.1 M LiClO4, this hybrid attains a large NH3 yield rate and a high Faradaic efficiency of 27.3 µg·h−1·mg−1cat. and 14.6% at −0.4 V vs. reversible hydrogen electrode, respectively, rivalling the current efficiency of all Fe-based NRR electrocatalysts in aqueous media. It also shows strong durability during the electrolytic process.
Electrochemical water splitting (EWS) is a highly clean and efficient method for high-purity hydrogen production. Unfortunately, EWS suffers from the sluggish and complex oxygen evolution reaction (OER) kinetics at anode. At present, the efficient, stable, and low-cost non-precious metal based OER electrocatalyst is still a great and long-term challenge for the future industrial application of EWS technology. Herein, we develop a simple and fast approach for gram-scale synthesis of flower-like cobalt-based layered double hydroxides nanosheet aggregates by ultrasonic synthesis, which show outstanding electrocatalytic performance for the oxygen evolution reaction in alkaline media, such as preeminent stability, small overpotential of 300 mV at 10 mA·cm−2 and small Tafel slope of 110 mV·dec−1.
Anisotropy and inhomogeneity are ubiquitous in spark plasma sintered thermoelectric devices. However, the origin of inhomogeneity in thermoelectric nanocomposites has rarely been investigated so far. Herein, we systematically study the impact of inhomogeneity in spark plasma sintered bismuth antimony telluride (BiSbTe) thermoelectric nanocomposites fabricated from solution-synthesized nanoplates. The figure of merit can reach 1.18, which, however, can be overestimated to 1.88 without considering the inhomogeneity. Our study reveals that the inhomogeneity in thermoelectric properties is attributed to the non-uniformity of porosity, textures and elemental distribution from electron backscatter diffraction and energy-dispersive spectroscopy characterizations. This finding suggests that the optimization of bulk material homogeneity should also be actively pursued in any future thermoelectric material research.
We propose a process of quantum-confined ion superfluid (QISF), which is enthalpy-driven confined ordered fluid, to explain the transmission of nerve signals. The ultrafast Na+ and K+ ions transportation through all sodium-potassium pump nanochannels simultaneously in the membrane is without energy loss, and leads to QISF wave along the neuronal axon, which acts as an information medium in the ultrafast nerve signal transmission. The QISF process will not only provide a new view point for a reasonable explanation of ultrafast signal transmission in the nerves and brain, but also challenge the theory of matter wave for ions, molecules and particles.
The in vivo spatio-temporal patterns of neovascularization are still poorly understood because it is limited to multi-scale techniques from the cellular level to living animal level. Owing to deep tissue-penetration and zero autofluorescence background, the second near-infrared (NIR-II, 1,000–1,700 nm) fluorescence imaging recently shows promise in breaking through this dilemma by dynamically tracking the pathophysiological process of neovascularization in vivo. Here, NIR-II fluorescence imaging was recruited for monitoring blood vessels in order to visualize the vascular injury and quantitively assess neovascularization in mouse models of acute skeleton muscle contusion and hindlimb ischemia. The temporal analysis of real-time NIR-II fluorescence intensity demonstrated that the blood flow perfusion of ischemia area was able to rapidly restore to 96% of pre-ischemic state within one week. Moreover, the spatial analysis revealed that the lower and outer quadrants of ischemia area in the mouse model of hindlimb ischemia always had relatively high blood flow perfusion compared with other quadrants during three weeks post-ischemia, and even exceeded pre-ischemic quantity at 21 days post-ischemia. In conclusion, this in vivo imaging technique has significant potential utility for studying the spatio-temporal patterns of neovascularization in vivo.
Potassium-ion batteries are regarded as the low-cost alternative to lithium-ion batteries. However, their development is hampered by the lack of suitable electrode materials. In this work, we demonstrate that MoS2 with expanded interlayers represents a promising candidate for the electrochemical storage of potassium ions. Hierarchical interlayer-expanded MoS2 assemblies supported on carbon nanotubes are prepared via a straightforward solution method. The increased interlayer spacing not only enables the better accommodation of foreign ions, but also lowers the diffusion energy barrier and improves diffusion kinetics of ions. When investigated as the anode material of potassium ion batteries, our interlayer-expanded MoS2 assemblies exhibit an excellent electrochemical performance with large capacity (up to ∼ 520 mAhg−1), good rate capability (∼ 310 mAhg−1 at 1,000 mAg−1) and impressive cycling stability, superior to most competitors.
Benzaldehyde byproduct is an imperative intermediate in the production of fine chemicals and additives. Tuning selectivity to benzaldehyde is therefore critical in alcohol oxidation reactions at the industrial level. Herein, we report a simple but innovative method for the synthesis of palladium hydride and nickel palladium hydride nanodendrites with controllable morphology, high stability, and excellent catalytic activity. The synthesized dendrites can maintain the palladium hydride phase even after their use in the chosen catalytic reaction. Remarkably, the high surface area morphology and unique interaction between nickel-rich surface and palladium hydride (β-phase) of these nanodendrites are translated in an enhanced catalytic activity for benzyl alcohol oxidation reaction. Our Ni/PdH0.43 nanodendrites demonstrated a high selectivity towards benzaldehyde of about 92.0% with a conversion rate of 95.4%, showing higher catalytic selectivity than their PdH0.43 counterparts and commercial Pd/C. The present study opens the door for further exploration of metal/metal-hydride nanostructures as next-generation catalytic materials.
A reproducible synthetic strategy was developed for facile large-scale (200 mg) synthesis of surface silanized magnetite (Fe3O4) nanoparticles (NPs) for biological applications. After further coupling a phosphate-specific affinity ligand, these functionalized magnetic NPs were used for the highly specific enrichment of phosphoproteins from a complex biological mixture. Moreover, correlating the surface silane density of the silanized magnetite NPs to their resultant enrichment performance established a simple and reliable quality assurance control to ensure reproducible synthesis of these NPs routinely in large scale and optimal phosphoprotein enrichment performance from batch-to-batch. Furthermore, by successful exploitation of a top-down phosphoproteomics strategy that integrates this high throughput nanoproteomics platform with online liquid chromatography (LC) and tandem mass spectrometry (MS/MS), we were able to specifically enrich, identify, and characterize endogenous phosphoproteins from highly complex human cardiac tissue homogenate. This nanoproteomics platform possesses a unique combination of scalability, specificity, reproducibility, and efficiency for the capture and enrichment of low abundance proteins in general, thereby enabling downstream proteomics applications.
Graphene nanosheets are a promising scaffold to accommodate S for achieving high performance Li/S battery. Nanosheet activation is used as a viable strategy to induce a micropore system and further improve the battery performance. Accordingly, chemical activation methods dominate despite the need of multiple stages, which slow down the process in addition to making them tiresome. Here, a three-dimensional (3D) N-doped graphene specimen was physically activated with CO2, a clean and single step process, and used for the preparation of a sulfur composite (A-3DNG/S). The A-3DNG/S composite exhibited outstanding electrochemical properties such as an excellent rate capability (1,000 mAh·g−1 at 2C), high reversible capacity and cycling stability (average capacity ~ 800 mAh·g−1 at 1C after 200 cycles), values which exceed those measured in chemically activated graphene. Therefore, these results support the use of physical activation as a simple and efficient alternative to improve the performance of carbons as an S host for high-performance Li-S batteries.
Atomically thin transition metal dichalcogenides (TMDs) have distinct opto-electronic properties including enhanced luminescence and high on-off current ratios, which can be further modulated by making more complex TMD heterostructures. However, resolution limits of conventional optical methods do not allow for direct nanoscale optical-structural correlation measurements in these materials, particularly of buried interfaces in TMD heterostructures. Here we use, for the first time, electron beam induced cathodoluminescence in a scanning transmission electron microscope (CL-STEM) to measure optical properties of monolayer TMDs (WS2, MoS2 and WSSe alloy) encapsulated between layers of hBN. We observe dark areas resulting from localized (~ 100 nm) imperfect interfaces and monolayer folding, which shows that the intimate contact between layers in this application-relevant heterostructure is required for proper inter layer coupling. We also realize a suitable imaging method that minimizes electron-beam induced changes and provides measurement of intrinsic properties. To overcome the limitation of small electron interaction volume in TMD monolayer (and hence low photon yield), we find that encapsulation of TMD monolayers with hBN and subsequent annealing is important. CL-STEM offers to be a powerful method to directly measure structure-optical correspondence in lateral or vertical heterostructures and alloys.
Subtle structural changes during electrochemical processes often relate to the degradation of electrode materials. Characterizing the minute-variations in complementary aspects such as crystal structure, chemical bonds, and electron/ion conductivity will give an in-depth understanding on the reaction mechanism of electrode materials, as well as revealing pathways for optimization. Here, vanadium pentoxide (V2O5), a typical cathode material suffering from severe capacity decay during cycling, is characterized by in-situ X-ray diffraction (XRD) and in-situ Raman spectroscopy combined with electrochemical tests. The phase transitions of V2O5 within the 0–1 Li/V ratio are characterized in detail. The V–O and V–V distances became more extended and shrank compared to the original ones after charge/discharge process, respectively. Combined with electrochemical tests, these variations are vital to the crystal structure cracking, which is linked with capacity fading. This work demonstrates that chemical bond changes between the transition metal and oxygen upon cycling serve as the origin of the capacity fading.
Platinum (Pt)-based electrocatalyst with low Pt content and high electrocatalytic performance is highly desired in fuel cell applications. Herein, we demonstrated that platinum-nickel (Pt-Ni) nanowires with an average composition of PtNi3 and a fishbone structure can be readily synthesized and used as an efficient electrocatalyst toward methanol oxidation reaction (MOR). The PtNi3 fishbone-like nanowires (PtNi3-FBNWs) present features such as richer Pt on the surface than in the bulk, high-index facets on the rough surface, and polyhedral facets at the ends of side chains. Such compositional and structural features could be determinative to the enhanced performance in the electrocatalysis of MOR. Compared with commercial 20% Pt/carbon black (Pt/C), the specific activity and mass activity of the PtNi3-FBNWs are enhanced by approximately 4.76 and 3.02 times, respectively. The stability of electrocatalysis is significantly improved as well. Such comprehensive enhancement indicates that the PtNi3-FBNWs would be a promising candidate toward MOR in fuel cells.