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Hypothesis The ability to control the assembly of micro/nanosized particles at liquid-liquid interface with external inputs promises new opportunities in nanofabrication and biomedicines. This work aims to demonstrate a way to control of dynamic assembly of nanoparticles at liquid-liquid interface by light and magnetic field, which consequently enables the formation of dynamic emulsion droplets. Experiments Magnetic Fe 3 O 4 nanoparticles functionalized with azobenzene moieties (Fe 3 O 4 @AZO) were synthesized and were dispersed in toluene/(N, N -dimethylformamide, DMF) binary solvent. After irradiation with UV or visible light , the assembly behavior of these Fe 3 O 4 nanoparticles were evaluated by electron microscopy and fluorescent microscopy. Findings Under UV light , Fe 3 O 4 @AZO nanoparticles were self-assembled due to the increase of dipolar interaction from the photoisomerization of azobenzene and polar molecules , DMF, were harvested from a binary solvent of DMF/toluene. While under visible light, a relief of dipolar interactions between Fe 3 O 4 @AZO nanoparticles can induce the secondary assembly of these Fe 3 O 4 @AZO nanoparticles at DMF-toluene interface, resulting in DMF droplets covered by a layer of nanoparticle superlattices . More importantly, coupled with a magnetic field, these emulsion droplets can be shaped into one dimensional ones during the interfacial assembly process, thereby giving rise to dynamic emulsions controlled by light and magnetic field.
Organic–inorganic hybrid lead halide perovskites are potential candidates for next-generation light-emitting diodes (LEDs) in terms of tunable emission wavelengths, high electroluminescence efficiency, and excellent color purity. However, the device performance is still limited by severe non-radiative recombination losses and operational instability due to a high degree of defect states on the perovskite surface. Here, an effective surface engineering method is developed via the assistance of guanidinium iodide (GAI), which allows the formation of surface-2D heterophased perovskite nanograins and surface defect passivation due to the bonding with undercoordinated halide ions. Efficient and stable red-emission LEDs are realized with the improved optoelectronic properties of GAI-modified perovskite nanograins by suppressing the trap-mediated non-radiative recombination loss. The champion device with a high color purity at 692 nm achieves an external quantum efficiency of 17.1%, which is 2.3 times that of the control device. Furthermore, the operational stability is highly improved, showing a half-lifetime of 563 min at an initial luminance of 1000 cd m−2. The proposed GAI-assisted surface engineering is a promising approach for defect passivation and phase engineering in perovskite films to achieve high-performance perovskite LEDs.
Direct conversion of carbon dioxide (CO 2 ) into lower olefins (C 2 -C 4 = ) is highly attractive as a sustainable production route for its great significance in greenhouse gas emission control and fossil fuel substitution. Fe-based catalysts have been extensively studied in CO 2 hydrogenation, which usually show unsatisfactory selectivity toward lower olefins. Here we present a high-dispersion catalyst precursor CoFe 2 O 4 with Na (Na-CoFe 2 O 4 ) that offers C 2 -C 4 = space time yield as high as 2.88 μmol C2-C4= g cat −1 s -1 and olefin to paraffin ratio about 6 at CO 2 conversion higher than 41 %. High dispersion and the intimate contact between Fe and Co sites help inhibit the formation of methane, and favor a higher selectivity of C 2 + hydrocarbons, especially lower olefins. The presence of Na further promotes chain growth and suppresses the direct hydrogenation of Fe-(CH 2 ) n intermediates. A superior stability over 100 h was observed, demonstrating the promising potential of this catalyst for industrial applications.
The present work focus on the measurement of viscosity and interfacial tension of n -heptane ( n -C 7 H 16 ) with dissolved carbon dioxide (CO 2 ) by the surface light scattering. The method allows an absolute determination of both properties in a contactless way. The experiments were conducted in macroscopic thermodynamic equilibrium at temperatures from (298 to 473) K and saturation pressures up to 5.5 MPa. For sample preparation of binary mixtures of n -C 7 H 16 with dissolved CO 2 after its addition, the equilibration process could be checked to be completed by showing that viscosity and interfacial tension are independent on time. For reaching equilibrium, at least two hours were elapsed between the addition of CO 2 and the start of the measurement. For both viscosity and interfacial tension, typical expanded uncertainties are 3% on a confidence level of 95%. The viscosity results were correlated with an empirical equation, where the absolute average deviation (AAD) and the maximum absolute deviation (MAD) between experiments and correlation were 1.9% and 7.2%, respectively. For the viscosity, a data comparison was hindered because of the lack of literature data. For the interfacial tension, which can also be represented by an empirical correlation and good agreement with literature can be found.
Perovskite quantum-dot-based light-emitting diodes (QLEDs) possess the features of wide gamut and real color expression, which have been considered as candidates for high-quality lightings and displays. However, massive defects are prone to be reproduced during the quantum dot (QD) film assembly, which would sorely affect carrier injection, transportation and recombination, and finally degrade QLED performances. Here, we propose a bilateral passivation strategy through passivating both top and bottom interfaces of QD film with organic molecules, which has drastically enhanced the efficiency and stability of perovskite QLEDs. Various molecules were applied, and comparison experiments were conducted to verify the necessity of passivation on both interfaces. Eventually, the passivated device achieves a maximum external quantum efficiency (EQE) of 18.7% and current efficiency of 75 cd A −1 . Moreover, the operational lifetime of QLEDs is enhanced by 20-fold, reaching 15.8 h. These findings highlight the importance of interface passivation for efficient and stable QD-based optoelectronic devices.
White-light-emitting materials have attracted wide interest for potential applications in information displays and lighting. To date, the majority of reported white-light-emitting materials have been multicomponent systems that are typically processed with organic solvents. These features are associated with complex processing, poor white-light quality, and environmental pollution. Herein, a white-light-emitting aqueous system is realized by encapsulating a fluorophore, which has a vibration-induced emission effect, in Pluronic F127 micelles. Tunable multicolor fluorescence is achieved by changing the temperature, and the use of organic solvents is effectively avoided. Through this process, white-light emission with Commission Internationale de l’Eclairage coordinates of (0.3351, 0.3326) is obtained, which is very close to pure white light, and its color rendering index is as high as 89. The fluorescence color tunability of this system could be performed in a wide temperature range, rendering it a potential material in optical thermometry. Besides, the aqueous system also allows for the application of the material as a fluorescent ink and white-light-emitting hydrogels. Information could be embedded in paper-based materials and hydrogels through the fluorescence quenching effect of iron ions (Fe3+) on the fluorophore. Fluorescence could then be recovered upon removal of Fe3+ by adenosine 5′-triphosphate. Thus, fluorescent patterning and triple-mode anti-counterfeiting could be expected due to the temperature-sensitive emission, fluorescence quenching, and recovering properties.
Elimination of antibiotics such as tetracycline hydrochloride (TC) from wastewater is of great significance, but still faces challenges. Herein, for the first time, I and P co-doped TiO 2 catalysts were prepared via a hydrolysis method. We also reported a simple method to prepare I and P co-doped TiO 2 photoelectrodes, which exhibited preeminent photoelectrocatalytic (PEC) performance for the decomposition of TC. The synergistic effect of I and P co-doping could significantly improve the charge separation rate and enhance the light absorption capacity of TiO 2 , leading to an enhancement of PEC activity. The main factors affecting the PEC performance were investigated, and the highest degradation rate constant (4.20 × 10 −2 min −1 ) was achieved when the doping content of P was 4 at% (ITP-4 photoelectrode) at pH 11.02 under visible light. The Langmuir–Hinshelwood kinetic model and active species trapping experiments were selected to investigate the degradation mechanism of TC. The results suggest that the hydroxyl radicals and photogenerated holes were the main active species that were responsible for the decomposition of TC. Moreover, the degradation pathways of TC based on the intermediates also demonstrated that the hydroxyl radicals and holes showed a principal role in degrading TC.
Drug-resistant bacterial infections have stolen the spotlight in recent years as stubborn diseases intimidating public health, thus urgently requiring the development of innovative treatment strategies with high antibacterial efficiency and low bacterial resistance. Here, a polymeric antimicrobial with synergistic chemo-photodynamic therapy function is fabricated to combat drug-resistant bacterial infections. In this strategy, polymeric micelles based on amphiphilic poly(aspartic acid)-block-poly(ε-caprolactone) (PAsp-b-PCL) are used as nanocarriers to encapsulate a photosensitizer protoporphyrin IX (PpIX) in the micellar core, which then undergo silver nanoparticle decoration on the micellar shell through an in situ reduction method. Compared with mono-therapy, the combination of silver nanoparticle decoration and light-activatable PpIX enables the resulting polymeric antimicrobial to exert chemo-photodynamic activity to kill drug-resistant bacteria more potently in vitro. Furthermore, the prepared polymeric antimicrobials with synergistic antibacterial activity show robust eradication efficacy against subcutaneous infections induced by drug-resistant Staphylococcus aureus in a murine model. Therefore, our study provides a simple and potent strategy to realize combination therapy for eradicating drug-resistant bacterial infections.
Abstract We report herein a versatile new approach for improving the photodegradation performance of UiO-66 by introducing 2-methylimidazole through a straightforward in situ one-pot solvothermal method. The resultant complex UiO-66-M-0.7 has demonstrated a reaction rate constant of 0.0183 min −1 in the photodegradation of rhodamine B under visible light, which is 69.4% higher than that with unmodulated UiO-66. Further investigation has confirmed that the improved activity can be attributed to enhanced adsorption of the dye by the photocatalyst during the adsorption–desorption equilibrium. The main active species involved in the photodegradation process have been identified as h + and O 2 − ·. In addition, the complex has shown ideal stability in recycling tests and excellent activity in the degradation of methylene blue. This study provides a novel perspective for the future design of various photocatalysts with superior performance. Graphic abstract 2-Methylimidazole-modulated UiO-66 exhibits increased catalytic performance in the photodegradation of rhodamine B (RhB) under visible light because of enhanced adsorption of RhB on the catalyst during the adsorption-desorption equilibrium.
In this study, 3D Fe 3 O 4 micro-flowers were synthesized by the self-assembly approach, then rhombic dodecahedral Cu 2 O was successfully loaded onto their surface by wet chemical method . Ag nanocrystals were reduced in situ on the surface of Fe 3 O 4 /Cu 2 O composites to prepare novel Fe 3 O 4 /Cu 2 O/Ag composites. The composites were characterized by SEM, TEM, XRD , XPS, VSM and UV–Vis diffuse reflectance spectroscopy. The effect of Ag nanocrystals on the photocatalytic performance of the Fe 3 O 4 /Cu 2 O composites was investigated by the degradation of methyl orange under visible light irradiation, and the Fe 3 O 4 /Cu 2 O/Ag composites showed higher photocatalytic efficiency than the Fe 3 O 4 /Cu 2 O composites. Photoelectrochemical and PL measurements were carried out to investigate the synergistic effect between the semiconductors and Ag nanocrystals and it was confirmed that the Fe 3 O 4 /Cu 2 O/Ag composites effectively inhibited the recombination of electron-hole pairs, thus improving the photocatalytic activity. The fact that the Fe 3 O 4 /Cu 2 O/Ag composites could be magnetically recycled and that they retained more than 90% of their original activity after six repeated experiments indicates, that they show great potential for wastewater treatment applications.
Nano-TiO2 is a type of environment-friendly and inexpensive substance that could be used for photocatalytic degradation processes. In this study, the multi-type carbon species doped and modified anatase nano-TiO2 was innovatively synthesized and developed to overcome the deficiency of common nano-TiO2 photocatalysts. The multi-type carbon species were derived from tetrabutyl titanate and ethanol as the internal and external carbon sources, respectively. Meanwhile, diverse characterization methods were applied to investigate the morphology and surface properties of the photocatalyst. Finally, the visible-light photocatalytic degradation activity of the collected samples was evaluated by using methyl orange as a model pollutant. The promotion mechanism of multi-type carbon species in the photocatalytic process was also discussed and reported. The results in this work show that the doping and modification of multi-type carbon species successfully narrows the bandgap of nano-TiO2 to expand the light absorption range, reduces the valence band position to improve the oxidation ability of photogenerated holes, and promotes the separation of photogenerated charge carriers to improve quantum efficiency. In addition, the further modification of the external carbon source can promote the surface adsorption of MO and stabilize the multi-type carbon species on the surface of nano-TiO2.
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