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A Combined Experimental and Theoretical Insights into the Synergistic Effect of Cerium Doping and Oxygen Vacancies into BaZrO <sub/>3-δ</sub> Hollow Nanospheres for Efficient Photocatalytic Hydrogen Production
摘要： The long-standing debate over the influence of oxygen vacancies and various dopants has been the center point in perovskite-based compounds for their photocatalytic applications. Hydrothermally synthesized Cerium doped BaZrO3 (BZO) hollow nanospheres has been systematically studied by experimental and theoretical calculations to understand the effect of Cerium doping and oxygen vacancies on the photocatalytic properties. Compounds synthesized by a template-free route were composed of hollow nanospheres generated by Ostwald ripening of spherical nanospheres, which were formed by agglomeration of nanoparticles. The high alkaline condition and high temperature during the hydrothermal condition may lead to the formation of local disorders and oxygen vacancies in the compounds, confirmed by ultraviolet-visible diffuse reflectance spectroscopy (UV-Vis DRS), X-ray photoelectron spectroscopy (XPS) and electron spin resonance (ESR) analysis and density functional theoretical (DFT) calculations. Combination of oxygen vacancies and progressive doping of Ce onto BZO, BaZr1–xCexO3 (x = 0.00 – 0.04), creates additional energy levels stipulated by vacancy defects and Ce mixed valance states within the band gap of BZO thereby reducing its band gap. The photocatalytic efficacy of the compounds has been examined by photo-driven H2 generation concomitant with oxidation of a sacrificial donor. In this study, BaZr0.97Ce0.03O3 shows the highest efficiency (823 μmol h-1 g-1) with an apparent quantum yield (AQY) of 6% in photocatalytic H2 production among all five synthesized samples. The data obtained from the UV–Vis DRS, XPS, ESR analysis and DFT calculations, the synergistic effect of decreasing the band gap due to Ce doping and the presence of Ce (III)/Ce (IV) pairs along with oxygen vacancies and lattice distortions could be the reasons behind the enhanced photocatalytic efficacy of BaZr1–xCexO3 (x = 0.00 – 0.04) under UV–Visible light.
关键词： Photocatalytic hydrogen production,Cerium doping,Oxygen vacancies,BaZrO3,Hollow nanospheres
更新于2025-11-21 11:01:37
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A fluorescent probe for sequential sensing of MnO <sub/>4</sub><sup>?</sup> and Cr <sub/>2</sub> O <sub/>7</sub><sup>2?</sup> ions in aqueous medium based on a UCNS/TMB nanosystem
摘要： This paper reports the successful design of an UC fluorescence nanosystem for distinguishable and sequential detection of MnO4? and Cr2O72? based on the inner filter effect (IFE) between Gd2O3:Yb,Er upconversion nanospheres (UCNS) and 3,3’,5,5’-tetramethylbenzidine (TMB). The detection of MnO4? was realized by a stoichiometric oxidation reaction between TMB and Mn(VII), which resulted in quenching of the upconversion luminescence (UCL) by the blue product through IFE. The assay of Cr2O72?, in contrast, was based on the formation of complexes and the consumption of the oxidation product of the previous reaction. The sensing of MnO4? and Cr2O72? do not interfere with each other when Pb2+ was added as a masking agent. This provides a new strategy for sensitive and selective detection of MnO4? and Cr2O72?. The detection of MnO4? showed not only a low LOD of 0.243 μM but also high selectivity over other possible interfering ions. The sensitivity assay of MnO4? can be performed in the linear range of 1.85 to 69 μM. An excellent linear relationship was also found in the sensing of Cr2O72?, with a linear range of 18.3 to 250 μM and a LOD of 2.95 μM. The selectivity towards Cr2O72? was also proved to be good. Based on these properties, the UCNS–TMB nanoplatform is a potential chemosensor for both MnO4? and Cr2O72? ions in practical assays for waste water.
关键词： upconversion nanospheres,aqueous medium,UCNS/TMB nanosystem,Cr2O72?,MnO4?,TMB,fluorescent probe,inner filter effect,sequential sensing
更新于2025-11-14 17:03:37
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Prussian blue nanosphere-embedded in situ hydrogel for photothermal therapy by peritumoral administration
摘要： To establish an injectable hydrogel containing prussian blue (PB) nanospheres for photothermal therapy against cancer, PB nanospheres were prepared by one-pot synthesis and the thermosensitive Pluronic F127 was used as the hydrogel matrix. The PB nanospheres and the hydrogel were characterized by shape, particle size, serum stability, photothermal performance upon repeated 808 nm laser irradiation, as well as the rheological features. The effect of the PB nanospheres and the hydrogel were evaluated qualitatively and quantitatively in 4T1 mouse breast cancer cells. The retention, photothermal efficacy, therapeutic effects and systemic toxicity of the hydrogel were assessed in a tumor-bearing mouse model. The PB nanospheres had a diameter of about 150 nm and exhibited satisfactory serum stability, photo-heat convert ability and repeated laser exposure stability. The hydrogel encapsulation did not negatively influence the above features of the photothermal agent. The nanosphere-containing hydrogel showed a phase transition at body temperature and, as a result, a long retention time in vivo. The photothermal agent-embedded hydrogel displayed promising photothermal therapeutic effects in the tumor-bearing mouse model with little-to-no systemic toxicity after peritumoral administration.
关键词： PB,In situ,Thermosensitive,Hydrogel,Photothermal,Injectable,Nanospheres
更新于2025-09-23 15:23:52
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Preparation of humidity, abrasion, and dust resistant antireflection coatings for photovoltaic modules via dual precursor modification and hybridization of hollow silica nanospheres
摘要： Antire?ection (AR) coatings on solar glass, used in photovoltaic (PV) modules, generally encounter harsh environments, which demands that AR coatings must hinder moisture penetration, scratch damage, and dust accumulation. Though chemical modi?cation generally bene?ts the multi-functionalization of AR coatings, it is likely to bring about a degradation of optical and mechanical properties. We demonstrated that a well-controlled dual precursor modi?cation/hybridization process of hollow silica nanospheres was the key to achieve the robust multifunctional AR coatings. The dual precursor-derived AR coatings exhibited an increase of 5.08% in average transmittance at wavelengths from 300 to 1200 nm and a small relative reduction below 0.6% after an ultra-long highly-accelerated humidity and temperature stress test duration of 120 h, equivalent to a 5000 h damp heat test at a temperature and a relative humidity of 85 °C and 85%, respectively, as well as the excellent abrasion and dust resistance. The e?ects of the dual precursor-derived AR coatings on PV devices were evaluated by the encapsulated crystalline silicon mini-modules, where the improvements of 2.45% and 3.20% in the short-circuit current and the power conversion e?ciency (Jsc and PCE) on average, respectively, relative to the bare glass encapsulated mini-modules were observed; meanwhile, the dust resistance of the AR coatings brought about the less degradations of 1.01% and 1.15% in Jsc and PCE, respectively, after the dust settling and removal tests, while the mini-modules with bare glass were 3.45% and 4.40%. It was believed that the dual-precursor, potentially, multi-precursor protocols would pave the way towards developing mechanically robust AR coatings with various fascinating functionalities, such as anti-?ngerprint, anti-soiling, anti-fogging, and anti-icing.
关键词： Dual precursors,Hollow silica nanospheres,Antire?ection coatings,Dust resistance,Abrasion,Humidity
更新于2025-09-23 15:23:52
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Bumpy Hollow Gold Nanospheres for Theranostic Application: Effect of Surface Morphology on Photothermal Conversion Efficiency
摘要： The combination of hollow core and rugose surface morphology is highly attractive for photoactive near-infrared (NIR) nanomaterials. Here, we present a facile pH modification to hollow gold nanosphere (HGN) synthesis to enable controlled tuning of the surface morphology from smooth to very bumpy. Unlike other methods, the synthetic protocol does not require harsh surfactants, secondary reducing agents, or organic solvents. The resultant bumpy HGNs (bHGNs) are highly monodisperse with little variation in protrusion length from particle to particle. Mechanistic studies suggest that surface rugosity is mainly controlled by the presence of free OH- ions in solution. We also present the first systematic investigation into the effect of surface morphology on the photothermal conversion efficiency (PCE) of bumpy as well as smooth HGNs, with a maximum PCE reaching 99%. Although expected to have a higher scattering component, the bHGNs retain the excellent PCE of their smooth counterparts, which may be due to efficient reabsorption of scattered light.
关键词： surface plasmon resonance,photothermal conversion efficiency,heat generation,surface morphology,hollow gold nanospheres
更新于2025-09-23 15:23:52
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Resonance Coupling in Heterostructures Composed of Silicon Nanosphere and Monolayer WS <sub/>2</sub> : A Magnetic-Dipole-Mediated Energy Transfer Process
摘要： Light?matter resonance coupling is a long-studied topic for both fundamental research and photonic and optoelectronic applications. Here we investigated the resonance coupling between the magnetic dipole mode of a dielectric nanosphere and 2D excitons in a monolayer semiconductor. By coating an individual silicon nanosphere with a monolayer of WS2, we theoretically demonstrated that, because of the strong energy transfer between the magnetic dipole mode of the nanosphere and the A-exciton in WS2, resonance coupling evidenced by anticrossing behavior in the scattering energy diagram was observed, with a mode splitting of 43 meV. In contrast to plexcitons, which involve plasmonic nanocavities, the resonance coupling in this all-dielectric heterostructure was insensitive to the spacing between the silicon nanosphere core and the WS2 shell. Additionally, the two split modes exhibited distinct light-scattering directionality. We further experimentally demonstrated the resonance coupling effect by depositing silicon nanospheres with different diameters onto a WS2 monolayer and collecting the scattering spectra of the resulting heterostructures under ambient conditions. We further demonstrated active control of the resonance coupling by temperature scanning. Our findings highlighted the potential of our all-dielectric heterostructure as a solid platform for studying strong light?matter interactions at the nanoscale.
关键词： magnetic dipole modes,two-dimensional materials,resonance coupling,two-dimension excitons,silicon nanospheres
更新于2025-09-23 15:23:52
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Growth of Spherical Gold Satellites on the Surface of Au@Ag@SiO <sub/>2</sub> Core–Shell Nanostructures Used for an Ultrasensitive SERS Immunoassay of Alpha-Fetoprotein
摘要： The identification and detection of cancer biomarkers in early stages is an important issue for the therapy of cancer. However, most methods are time-consuming, limited sensing sensitivity and specificity. In this work, we prepared a novel plasmonic multilayered core–shell-satellite nanostructure (Au@Ag@SiO2-AuNP) consisting of an gold nanosphere with silver coating core (Au@Ag), an ultrathin continuous silica (SiO2) shell and high coverage of gold nanospheres (AuNPs) satellites. Au@Ag core is prominent surface enhanced Raman scattering (SERS) platform and the thin SiO2 layer exhibits a long-range plasmon coupling between Au@Ag core to AuNPs satellites further leading to enhanced Raman scattering. Meanwhile, the outer AuNPs satellites have a high biocompatibility and long-term stability. Combining the above advantages, the well-designed metallic nanoassemblies would be a promising candidate for SERS-based applications in biochemistry. For specific detection of alpha-fetoprotein (AFP), we utilized the SERS-active core-shell-satellite nanostructures modified with AFP antibody as immune probes and nitrocellulose membrane (NC) stabilized captured anti-AFP antibodies as solid substrate. To improve the detection performance, we further systematically optimized the parameters, including silver coating thickness of Au@Ag core, the density and size of satellite AuNPs. Under the optimized conditions, AFP could be detected by the SERS-based sandwich immunoassay with an ultralow detection limit of 0.3 fg/mL, and the method exhibited a wide linear response from 1 fg/mL to 1 ng/mL. The limit of detection (LOD) was considerably lower than conventional methods in literature. This work relies on the unique Au@Ag@SiO2-AuNP nanostructures as immune probe develops a new outlook for the application of multilayered nanoassemblies and demonstrates the great potential in early tumor markers detection.
关键词： surface enhanced Raman scattering (SERS),Au-Ag bimetallic nanospheres,alpha-fetoprotein,core-shell-satellite nanostructure,gold nanospheres
更新于2025-09-23 15:22:29
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Optical response of heterogeneous polymer layers containing silver nanostructures
摘要： This work is focused on the study of the optical properties of silver nanostructures embedded in a polymer host matrix. The introduction of silver nanostructures in polymer thin films is assumed to result in layers having adaptable optical properties. Thin film layers with inclusions of differently shaped nanoparticles, such as nanospheres and nanoprisms, and of different sizes, are optically characterized. The nanoparticles are produced by a simple chemical synthesis at room temperature in water. The plasmonic resonance peaks of the different colloidal solutions range from 390 to 1300 nm. The non-absorbing, transparent polymer matrix poly(vinylpyrrolidone) (PVP) was chosen because of its suitable optical and chemical properties. The optical studies of the layers include spectrophotometry and spectroscopic ellipsometry measurements, which provide information about the reflection, transmission, absorption of the material as well as the complex optical indices, n and k. Finite difference time domain simulations of nanoparticles in thin film layers allow the visualization of the nanoparticle interactions or the electric field enhancement on and around the nanoparticles to complete the optical characterization. A simple analysis method is proposed to obtain the complex refractive index of nanospheres and nanoprisms in a polymer matrix.
关键词： nanospheres,thin film layers,plasmonic nanoparticles,nanoprisms,spectroscopic ellipsometry
更新于2025-09-23 15:22:29
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Enhanced photocatalytic activity of g-C3N4 quantum dots/Bi3.64Mo0.36O6.55 nanospheres composites
摘要： In this research, heterostructured g-C3N4 quantum dots (CNQDs)/Bi3.64Mo0.36O6.55 nanospheres have been fabricated trough an in situ precipitation process. Compared to the pure Bi3.64Mo0.36O6.55, the as-fabricated CNQDs/Bi3.64Mo0.36O6.55 nanocomposites exhibited significantly improved photocatalytic performance for the photodegradation of rhodamine B (Rh B) and bisphenol A (BPA). In addition, 5 wt% CNQDs/Bi3.64Mo0.36O6.55 sample showed the highest photocatalytic efficiency under visible-light irradiation (λ > 420 nm). The effective separation and transmission of photogenerated electron-hole pairs caused by CNQD loading as well as the improved BET surface area are associated with the enhancement of the photocatalytic activity of the CNQDs/Bi3.64Mo0.36O6.55 photocatalyst.
关键词： Water purification,Bi3.64Mo0.36O6.55 nanospheres,Binary heterostructure,g-C3N4 quantum Dots,Photocatalytic activity
更新于2025-09-23 15:21:01
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Facile Preparation of Highly Luminescent Nitrogen-Doped Carbonaceous Nanospheres and Potential Application in Intracellular Imaging of Quercetin
摘要： Highly luminescent nitrogen-doped carbonaceous nanospheres (LNCNs) were synthesized by a one-pot hydrothermal reaction of b-cyclodextrin (b-CD) and branched polyethylenimine (BPEI). Both the N-doping and amino-functionalisation of LNCNs were achieved simultaneously. The prepared LNCNs display excellent properties such as high physical and chemical stability, excitation wavelength-independent emission, and high photoluminescence quantum yields. Importantly, the LNCNs exhibit a quenching of photoluminescence in the presence of quercetin (Qc) based on the simple static quenching mechanism, making it possible to quantify concentrations from 0.5 to 80 mg mL(cid:1)1 with a detection limit of 0.21 mg mL(cid:1)1. Furthermore, the LNCNs probe was further used for imaging Qc in living cells.
关键词： quercetin,photoluminescence quenching,nitrogen-doped carbonaceous nanospheres,intracellular imaging
更新于2025-09-23 15:21:01