Latest ArticlesUp to date, solid-state carbon dots (CDs) with bright red fluorescence have scarcely achieved due to aggregation-caused quenching (ACQ) effect and extremely low quantum yield in deep-red to near infrared region. Here, we report a novel fluorine-defects induced solid-state red fluorescence (λem = 676 nm, the absolute fluorescence quantum yields is 4.17%) in fluorine, nitrogen and sulfur co-doped CDs (F, N, S-CDs), which is the first report of such a long wavelength emission of solid-state CDs. As a control, CDs without fluorine-doping (N, S-CDs) show no fluorescence in solid-state, and the fluorescence quantum yield/emission wavelength of N, S-CDs in solution-state are also lower/shorter than that of F, N, S-CDs, which is mainly due to the F-induced defect traps on the surface/edge of F, N, S-CDs. Moreover, the solid-state F, N, S-CDs exhibit an interesting temperature-sensitive behavior in the range of 80-420 K, with the maximum fluorescence intensity at 120 K, unveiling its potential as the temperature-dependent fluorescent sensor and the solid-state light-emitting device adapted to multiple temperatures.
The electrode/electrlyte interface is of great signifance to photoelectrochemical (PEC) water oxidation as the reaction mainly occur here. Herein, we focus on the effect of supercapactance of the electrode/electrlyte interface on the performance of PEC. It is discovered that the supercapacitor on the interface is crucial because it links the charge transport and solution ion adsorption on its two sides. In this study, we demonstrate an approach to promote the performance of TiO2 nanowire array (TiO2 NWs) photoanode in photoelectrochemical cells (PECs) by increasing its supercapacitance. A 2−5 nm carbon layer was coated and the interface supercapacitance increases by about 150 times. This enhances the separation rate of electron-hole pairs by collecting more holes. Meanwhile, it also promotes the water oxidation rate by adsorbing more OH− on its surface. As a result, the photocurrent density of C-TiO2 NWs was about 8 times higher than that of its carbon-free counterpart. This approach of increasing the supercapacitance of photoanodes would be attractive for enhancement of the efficiency of PECs and this work demonstrate the importance of supercapacitance of the interface for PECs.
H2O2 has been widely applied in the fields of chemical synthesis, medical sterilization, pollutant removal, etc., due to its strong oxidizing property and the avoidable secondary pollution. Despite of the enhanced performance for H2O2 generation over g-C3N4 semiconductors through promoting the separation of photo-generated charge carriers, the effect of migration orientation of charge carriers is still ambiguous. For this emotion, surface modification of g-C3N4 was employed to adjust the migration orientation of charge carriers, in order to investigate systematically its effect on the performance of H2O2 generation. It was found that ultrathin g-C3N4 (UCN) modified by boron nitride (BN), as an effective hole-attract agent, demonstrated a significantly enhanced performance. Particularly, for the optimum UCN/BN-40% catalyst, 4.0-fold higher yield of H2O2 was obtained in comparison with the pristine UCN. As comparison, UCN modified by carbon dust demonstrated a completely opposite tendency. The remarkably improved performance over UCN/BN was ascribed to the fact that more photo-generated electrons were remained inside of triazine structure of g-C3N4, leading to the formation of larger amount of 1, 4-endoxide. It is anticipated that our work could provide new insights for the design of photocatalyst with significantly improved performance for H2O2 generation.
High responsivity and sensitivity play essential roles in the development of organic field-effect transistors (OFETs)-based biosensors with regard to biological detections, particularly for disease diagnosis. Nonetheless, how to design a biosensor which improves these two outstanding properties while achieving low cost, easy processing, and time saving is a daunting challenge. Herein, a novel biosensor based on OFET with copolymer thin film, whose surface is illuminated with a suitable light beam is reported. This film can be used as both an organic semiconductor material and as a photoelectric active material. Due to amplification of signals as a result of the film's strong response to light, the biosensor possesses higher responsivity and sensitivity compared to dark condition and even realizes a maximum responsivity of up to 103 for alpha-fetoprotein (AFP) detection. The simple combination of light and transistor builds a bridge between photoelectric effect and biological system. In addition, the emergence of more excellent photoelectric active materials is expected to pave a way for ultrasensitive bio-chemical diagnostic tools.
Designing non-noble metal electrocatalysts toward alkaline hydrogen evolution reaction (HER) with high performance at a large current density is urgent. Herein, a CoO/CoP heterostructure catalyst (termed POZ) was designed by a phosphating strategy. The strong electron transfer on the interface of CoO/CoP was experimentally and theoretically proven. POZ showed a low overpotential of 236 mV at 400 mA/cm2, which was 249 mV lower than non-phosphated sample. It also exhibited a remarkable solar-to-hydrogen conversion efficiency of 10.5%. In this work, the construction of CoO/CoP interface realized by a simple phosphating strategy could provide an important reference to boost the HER performance on those materials not merely metal oxides.
At present, frequent outbreaks of bacteria and viruses have seriously affected people's normal lives. Therefore, the study of broad-spectrum antibacterial nanocomposites is very promising. However, most antibacterial materials have some disadvantages, such as single bactericidal mechanisms and unrepeatable use. Based on the current situation, a kind of nanocomposite with three structures of graphene oxide (GO), quaternary ammonium salt (QAs) and N-halamine was prepared, which showed synergistic effect to improve antibacterial activity and combined with a variety of sterilization mechanisms. Meanwhile, GO can provide richer ways of sterilization and high specific surface area, which is conducive to the grafting of quaternarized N-halamine. The advantages of physical sterilization of GO, charge adsorption of QAs, reuse of N-halamine and efficient sterilization are fully utilized. The results showed that the quaternarized N-halamine-grafted GO was obtained successfully. GO grafted with quaternarized N-halamine polymer showed strong speedy bactericidal activity against Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus) (99%). It had good storage and regeneration properties.
As an emerging thermal-driven membrane technology, membrane distillation (MD) has attracted immense attention for desalination and water purification. The membranes for MD generally have hydrophobic or superhydrophobic properties to enable vapor permeation without liquid passage (e.g., wetting). However, conventional MD membranes cannot undergo long term stable operations due to gradual wetting in practical applications where the feed solution often contains multiple low-surface tension contaminants (e.g., oil). Recently, omniphobic membranes repelling all sorts of liquids and typically having ultralow surface energy and re-entrant structures have been developed for robust MD to mitigate wetting and fouling. In this paper, we aim to provide a comprehensive review of recent progress on omniphobic membranes. Fundamentals, desirable properties, advantages and applications of omniphobic membranes are discussed. We also summarize the research efforts and methods to engineer omniphobic membranes. Finally, the challenges and future research directions on omniphobic membranes are discussed.
Nanodiamond (ND) polarizer can be used for dynamic nuclear polarization (DNP), owing to unpaired electrons provided by surface defects. However, 1H enhancement via Overhauser DNP (ODNP) using ND in-situ liquid has been found much smaller than traditional radicals. Herein, we study the surface properties of ND using electron spin resonance (ESR) and Raman methods firstly. Then the enhancement of 1H ODNP is explored using ND as polarizer with different nanoparticle sizes and concentrations at home-built 0.06 T DNP spectrometer. The surface of ND with the size of 30 nm is further modification via high temperature air oxidized and the enhancement was measured. The results show that nanoparticle sizes and Raman peak intensity ratio of sp2/sp3 hybridization are approximate negative correlation and positive correlation to enhancement, respectively. Furthermore, there is no significant enhancement in the oxidation group, and a −22.5-fold 1H ODNP enhancement is achieved in-situ liquid at room temperature, which demonstrate the ND can be used as an efficient enhancer. We expect ND to play a greater role in biomedical research, especially for multimodal imaging with improving the performance of ND surface.
Spatial isolation of different functional sites at the nanoscale in multifunctional catalysts for steering reaction sequence and paths remains a major challenge. Herein, we reported the spatial separation of dual-site Au and RuO2 on the nanosurface of TiO2 (Au/TiO2/RuO2) through the strong metal-support interaction (SMSI) and the lattice matching (LM) for robust photocatalytic hydrogen evolution. The SMSI between Au and TiO2 induced the encapsulation of Au nanoparticles by an impermeable TiOx overlayer, which can function as a physical separation barrier to the permeation of the second precursor. The LM between RuO2 and rutile-TiO2 can increase the stability of RuO2/TiO2 interface and thus prevent the aggregation of dual-site Au and RuO2 in the calcination process of removing TiOx overlayer of Au. The photocatalytic hydrogen production is used as a model reaction to evaluate the performance of spatially separated dual-site Au/TiO2/RuO2 catalysts. The rate of hydrogen production of the Au/TiO2/RuO2 is as high as 84 μmol h−1g−1 under solar light irradiation without sacrificial agents, which is 2.5 times higher than the reference Au/TiO2 and non-separated Au/RuO2/TiO2 samples. Systematic characterizations verify that the spatially separated dual-site Au and RuO2 on the nanosurface of TiO2 can effectively separate the photo-generated carriers and lower the height of the Schottky barrier, respectively, under UV and visible light irradiation. This study provides new inspiration for the precise construction of different sites in multifunctional catalysts.
Mixed metal sulfides have been widely used as anode material of sodium-ion batteries (SIBs) because of their excellent conductivity and sodium ion storage performance. Herein, ReS2@NiS2 heterostructures have been triumphantly designed and prepared through anchoring ReS2 nanosheet arrays on the surface of NiS2 hollow nanosphere. Specifically, the carbon nanospheres was used as hard template to synthesize NiS2 hollow spheres as the substrate and then the ultrathin two-dimensional ReS2 nanosheet arrays were uniformly grown on the surface of NiS2. The internal hollow property provides sufficient space to relieve the volume expansion, and the outer two-dimensional nanosheet realizes the rapid electron transport and insertion/extraction of Na+. Owing to the great improvement of the transport kinetics of Na+, NiS2@ReS2 heterostructure electrode can achieve a high specific capacity of 400 mAh/g at the high current density of 1 A/g and still maintain a stable cycle stability even after 220 cycles. This hard template method not only paves a new way for the design and construct binary metal sulfide heterostructure electrode materials with outstanding electrochemical performance for Na+ batteries but also open up the potential applications of anode materials of SIBs.
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