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1.
Crocin (saffron bioactive) loaded protein nanoparticles were prepared from three underutilised cereal varieties viz., sorghum (SPCN), foxtail millet (FPCN) and pearl millet (PPCN) using ultrasonication technique. The particle size of crocin loaded protein complex was attained in the nano range with reduced polydispersity index and negative zeta potential. The encapsulation efficiency of crocin in protein nanoparticles was found to be 83.78% (FPCN), 78.74 % (SPCN) and 70.01% (PPCN). The topographical images of crocin loaded protein nano complex was revealed using field emission-scanning electron microscopy (FE-SEM). The attenuated total reflectance fourier transform infra-spectroscopy (ATR-FTIR) analysis showed the characteristic peaks of crocin at 956, 1700 and 3350 cm−1 in protein-crocin nanocomplex as a confirmatory test for nanoencapsulation. The antimicrobial activity of crocin loaded protein nanocomplex against three strains (Escherichia coli, Staphylococcus aureus and Fusarium oxysporium) were also evaluated. In vitro release studies showed higher content of crocin released in simulated intestinal conditions ensuring its controlled release at target site. Bioactivity (anti-cancerous and anti-hypertensive) of crocin upon in-vitro digestion were well retained indicating that protein nanoparticles can act as an effective wall material. Our results suggest that protein nanoparticles prepared in this study can act as an effective oral delivery vehicle for crocin that could be used for development of functional foods.  相似文献   

2.
Ultrasonication, redox-pair generated free radical method and their combination (Ultrasonication/redox-pair method) was used for production of camel whey-quercetin conjugates. FTIR and SDS-PAGE confirmed successful production of whey-quercetin conjugates using ultrasonication and ultrasonication/redox-pair method. FTIR suggested existence of covalent (appearance of new peak at 3399 cm−1) and non-covalent linkages (shifting of peak at 3271 cm−1, 1655 cm−1 (amide I), 1534 cm−1 and 1422 cm−1 (Amide II)) in the whey-quercetin conjugates. Moreover, SDS-PAGE of conjugates produced by ultrasonication as well redox-pair method indicated shifting of protein bands slightly towards high molecular weight due to increase in the mass of proteins due to the binding of polyphenols. All conjugates showed improved techno-functional and bioactive properties in comparison to whey proteins. Conjugates produced through ultrasonication showed smaller particle size, improved solubility, emulsifying and foaming properties while conjugates produced through ultrasonication/redox-pair method depicted superior antioxidant properties in comparison to whey. Furthermore, conjugated samples showed higher inhibition of enzymatic markers involved in diabetes and obesity with highest potential recorded in conjugates produced using ultrasonication. Therefore, ultrasonication can be successfully used individually as well as in combination with redox-pair for production of whey-quercetin conjugates with enhanced bioactive and techno-functional properties.  相似文献   

3.
In this study, modified citrus pectin treated with a combination of microfluidization and ultrasonication was compared to the original and ultrasonication treated pectin on hydrodynamic diameter, molecular weight, polydispersity, zeta potential, apparent viscosity, Fourier-transform infrared spectroscopy (FTIR), 2,2-diphenyl-1-picryl hydrazyl (DPPH) radical scavenging capacity, scanning electron microscope (SEM), atomic force microscopy (AFM), their emulsifying properties and encapsulation properties. Modified pectin treated with a combination of microfluidization and moderate ultrasonication (MUB) was found to have lowest hydrodynamic diameter (418 nm), molecular weight (237.69 kDa) and polydispersity (0.12), and relatively low apparent viscosity among all pectin samples. Furthermore, it showed significantly higher DPPH radical scavenging capacity than the original pectin although only slightly higher than that of ultrasonication treated one (UB). MUB showed a thin fibrous morphology and decreased degree of branching from SEM and AFM. Emulsion stabilized by MUB had highest centrifugal and thermal stability compared to emulsions stabilized by UB and the original pectin. This could be attributed to higher interfacial loading of MUB (17.90 mg/m2) forming more compact interfacial layer observed by confocal laser scanning microscopy (CLSM). Moreover, both MUB and UB exhibited improved encapsulation functionality to protect cholecalciferol (vitamin D3) from UV degradation compared to the original pectin.  相似文献   

4.
Resistant starch type 2 (RS) was isolated from lotus stem using enzymatic digestion method. The isolated RS was subjected to ultrasonication (US) at different sonication power (100–400 W). The US treated and untreated RS samples were characterized using dynamic light scattering (DLS), scanning electron microscopy (SEM), light microscopy and Fourier transform infrared spectroscopy (FT-IR). DLS revealed that particle size of RS decreased from 12.80 µm to 413.19 nm and zeta potential increased from −12.34 mV to −26.09 mV with the increase in sonication power. SEM revealed smaller, disintegrated and irregular shaped RS particles after ultrasonication. FT-IR showed the decreased the band intensity at 995 cm−1 and 1047 cm−1 signifying that US treatment decreased the crystallinity of RS and increased its amorphous character. The bile acid binding, anti-oxidant and pancreatic lipase inhibition activity of samples also increased significantly (p < 0.05) with the increase in sonication power. Increase in US power however increased the values of hydrolysis from 23.11 ± 1.09 to 36.06 ± 0.13% and gylcemic index from 52.39 ± 0.38 to 59.50 ± 0.11. Overall, the non-thermal process of ultrasonic treatment can be used to change the structural, morphological and nutraceutical profile of lotus stem resistant starch which can have great food and pharamaceutical applications.  相似文献   

5.
Ultrasonic technology was applied to release the phenolics bound with starch and protein matrix in order to enhance total phenolic content (TPC) and antioxidant activity (AA) of the sorghum flour. Both the continuous flow and batch ultrasonication were implied with independent variables such as flour to water ratio (FWR), ultrasonication intensity (UI), and ultrasonication time (UT) with an additional variable as flow rate (FR) in continuous flow ultrasonication. All the process variables showed a significant effect on the corresponding ultrasonication process. The optimal conditions for the continuous flow ultrasonication were a FWR of 10% w/v, an UI of 20 W/cm2, an UT of 130 s, and 15 ml/s FR which produced a maximum values of 70.9 mg GAE/100 g dry matter (d.m.) for TPC and 143.9 µmol TE/100 g d.m. for AA. Regarding the batch ultrasonication, the maximum values were 65.6 mg GAE/100 g d.m. and 141.0 µmol TE/100 g d.m. for TPC and AA, respectively at optimum conditions of 10% w/v FWR, 30 W/cm2 UI, and 200 s UT. When comparing with the batch ultrasonication, the continuous flow process saved 35% time and 33% of energy consumption to obtain comparatively higher TPC and AA of the sorghum flour. Ultrasonication improved free phenolic acid content by releasing bound phenolics in the sorghum flour. Impact of various process parameters on specific energy was analyzed during both the processes, and influence of energy on TPC and AA of the sorghum flour was also observed for the batch and continuous flow ultrasonication.  相似文献   

6.
In this research, a sonochemical activation-assisted biosynthesis of Au/Fe3O4 nanoparticles is proposed. The proposed synthesis methodology incorporates the use of Piper auritum (an endemic plant) as reducing agent and in a complementary way, an ultrasonication process to promote the synthesis of the plasmonic/magnetic nanoparticles (Au/Fe3O4). The synergic effect of the green and sonochemical synthesis favors the well-dispersion of precursor salts and the subsequent growth of the Au/Fe3O4 nanoparticles.The hybrid green/sonochemical process generates an economical, ecological and simplified alternative to synthesizing Au/Fe3O4 nanoparticles whit enhanced catalytic activity, pronounced magnetic properties. The morphological, chemical and structural characterization was carried out by high- resolution Scanning electron microscopy (HR-SEM), Energy Dispersive X-Ray Spectroscopy (EDS) and X-Ray diffraction (XRD), respectively. Ultraviolet–visible (UV–vis) and X-ray photoelectron (XPS) spectroscopy confirm the Au/Fe3O4 nanoparticles obtention. The magnetic properties were evaluated by a vibrating sample magnetometer (VSM). Superparamagnetic behavior, of the Au/ Fe3O4 nanoparticles was observed (Ms = 51 emu/g and Hc = 30 Oe at 300 K). Finally, the catalytic activity was evaluated by sonocatalytic degradation of methyl orange (MO). In this stage, it was possible to achieve a removal percentage of 91.2% at 15 min of the sonocatalytic process (160 W/42 kHz). The initial concentration of the MO was 20 mg L−1, and the Fe3O4-Au dosage was 0.075 gL−1. The MO degradation process was described mathematically by four kinetic adsorption models: Pseudo-first order model, Pseudo-second order model, Elovich and intraparticle diffusion model.  相似文献   

7.
The objective of this work was to develop a simple and efficient method to prepare waxy maize starch nanoparticles (SNPs) by hydrochloric acid (HCl) vapor hydrolysis combined with ultrasonication treatment. The size, morphology, thermal property, and crystal structure of the SNPs were systematically studied. HCl treatment introduces a smaller particle diameter of starch particles from 13.73 ± 0.93 μm to 1.52 ± 0.01–8.32 ± 0.63 μm. Further ultrasonication treatment formed SNPs that displayed desirable uniformity and near-perfect spherical and ellipsoidal shapes with a diameter of 150.65 ± 1.91–292.85 ± 0.07 nm. The highest yield of SNPs was 80.5%. Compared with the native starch, the gelatinization enthalpy changes of SNPs significantly decreased from 14.65 ± 1.58 J/g to 7.40 ± 1.27 J/g. Interestingly, the SNPs showed a wider melting temperature range of 22.77 ± 2.35 °C than native starch (10.94 ± 0.87 °C). The relative crystallinity of SNPs decreased to 29.65%, while long-time ultrasonication resulted in amorphization. HCl vapor hydrolysis combined with ultrasonication treatment can be an affordable and accessible method for the efficient large-scale production of SNPs. The SNPs developed by this method will have potential applications in the food, materials, and medicine industries.  相似文献   

8.
Graft polymerization of acrylic acid (AA) onto poly(l-lactide) (PLLA) film by UV irradiation was carried out to develop surfaces for N-methylene phosphonic chitosan (NMPC) immobilization. The properties of modified films were discussed by colorimetric method, attenuated total reflection-Fourier transform infrared spectroscopy (ATR-FTIR), contact angles, atomic force microscopy (AFM) and osteoblast incubation. The results showed that AA solution concentration and irradiation time had effect on the graft carboxyl densities. Comparing the ATR-FTIR images, two new peaks at 1561 cm−1 and 1632 cm−1 proved that NMPC was immobilized on the film surface successfully. The water contact-angles were decreased from 90 ± 5° to 37 ± 5° after modification. The AFM images indicated that the surface of the combined film was rougher than that of untreated film. The grafted film provided an excellent substrate for the growth of osteoblast.  相似文献   

9.
This study was designed to compare the properties of myofibrillar protein (MP) stabilized soybean oil-in-water emulsions fabricated by ultrasound-assisted emulsification (UAE), high-pressure homogenization (HPH) and high-speed homogenization (HSH). The emulsion properties, droplet characteristics, interfacial proteins, protein exposure extent, microrheological properties, multiple light scattering results, and 7 d storage stabilities of the three emulsions were specifically investigated. Our results indicate that UAE and HPH were better emulsification methods than HSH to obtain high-quality emulsions with higher emulsifying activity index (UAE 20.73 m2·g−1, HPH 11.76 m2·g−1 and HSH 6.80 m2·g−1), whiteness (UAE 81.05, HPH 80.67 and HSH 74.09), viscosity coefficient (UAE 0.44 Pa·sn, HPH 0.49 Pa·sn and HSH 0.22 Pa·sn), macroscopic viscosity index (UAE 2.31 nm−2·s, HPH 0.38 nm−2·s and HSH 0.34 nm−2·s), and storage stability, especially for the UAE. Furthermore, UAE was a more efficient emulsification method than HPH to prepare the fine MP-soybean oil emulsion. The protein-coated oil droplets were observed in the three emulsions. The emulsion droplet size of the UAE-fabricated emulsion was the lowest (0.15 μm) while the interfacial protein concentration (93.37%) and the protein exposure extent were the highest among the three emulsions. During the 7 d storage, no separation was observed for the UAE-fabricated emulsion, while the emulsions fabricated by HPH and HSH were separated after storage for 5 d and 2 h. Therefore, this work suggests that UAE could be a better method than HPH and HSH to fabricate MP-soybean oil emulsion.  相似文献   

10.
A persistent ultrasound-assisted hydrothermal method has been developed to prepare cobalt oxide incorporated nitrogen-doped graphene (Co3O4/N-GO) hybrids. The electrochemical behaviors and catalytic activity of the prepared hybrids have been systematically investigated as cathode materials for Al-air battery. The results show that ultrasonication can promote the yield ratio of Co3O4 from 63.1% to 70.6%. The prepared Co3O4/N-GO hybrid with ultrasonication exhibits better ORR activity over that without ultrasonication. The assembled Al-air battery using the ultrasonicated Co3O4/N-GO hybrid exhibited an average working voltage of 1.02 V in 4 M KOH electrolyte at 60 mA∙cm−2, approximately 60 mV higher than that using hybrid without ultrasonication. This should be attributed to large number density of fine Co3O4 particles growing on the dispersed GO sheets under the persistent ultrasonication. The related ultrasonic mechanism has been discussed in details.  相似文献   

11.
We investigate selective patterning of ultra-thin 20 nm Indium Tin Oxide (ITO) thin films on glass substrates, using 343, 515, and 1030 nm femtosecond (fs), and 1030 nm picoseconds (ps) laser pulses. An ablative removal mechanism is observed for all wavelengths at both femtosecond and picoseconds time-scales. The absorbed threshold fluence values were determined to be 12.5 mJ cm2 at 343 nm, 9.68 mJ cm2 at 515 nm, and 7.50 mJ cm2 at 1030 nm for femtosecond and 9.14 mJ cm2 at 1030 nm for picosecond laser exposure. Surface analysis of ablated craters using atomic force microscopy confirms that the selective removal of the film from the glass substrate is dependent on the applied fluence. Film removal is shown to be primarily through ultrafast lattice deformation generated by an electron blast force. The laser absorption and heating process was simulated using a two temperature model (TTM). The predicted surface temperatures confirm that film removal below 1 J cm−2 to be predominately by a non-thermal mechanism.  相似文献   

12.
In this work, a cost-effective and facile method was adopted for the fabrication of graphene oxide nanoscrolls (GONS) by low frequency (20 kHz) ultrasonication with tunable dimensions. The graphene oxide (GO) was synthesized by modified Hummer’s method using synthetic graphite as a base material. Later, GO suspension (0.05 g L−1) were made using methanol as solvent and subjected to different ultrasonication conditions. It was found that GO sheets curls themselves into nanoscrolls by overcoming the energy barrier for scrolling with the help of bubble cavitation energy provided by ultrasonication. Also, the effect of ultrasonication power (100–150 W) for irradiation time (0.5–3 h) over the GONS dimensions were investigated. The spiral wounded GONS structures were shown using electron microscopy. Raman Spectroscopy, Thin-film X-Ray Diffraction, Energy Dispersive X-Ray, FT Infrared Spectroscopic analysis were also done to endorse GONS formation. Factors affecting GONS formation such as sonication power and solvent selection were studied as scrolling of GO sheets are strongly dependent on sonication parameters and solvent characteristics. It was found that GONS length varies inversely with irradiation time for identical power density. Also, a solvent with relatively large Hansen solubility parameter, lower dipole movement and less negative value of zeta potential support GONS formation of longer length. Raman analysis overlays the rapid oxygen-defect site cleavage mechanism. The obtained GONS unlocks further developments in various engineering applications like adsorption, drug delivery and filtration membrane.  相似文献   

13.
In this reports the facile and green synthesis of rutile-type titanium dioxide nanoparticles decorated graphene oxide nanocomposite via the ultrasonication process (frequency: 50 kHz, Power: 100 W/cm2 and Ultrasonic type: Ti-horn). Because, the sonochemical synthesis method is simple, non-explosive and harmless method than other conventional technique. Furthermore, the synthesized material was characterized by various analytical techniques including FESEM, EDX, XRD, EIS and electrochemical methods. Then, the synthesized TiO2 MPs@GOS composite was applied for the electrocatalytic detection of theophylline (TPL) using CV and amperometric (current-time) techniques. Captivatingly, the modified sensor has excellent electrocatalytic performance with the wider linear range from 0.02 to 209.6 µM towards the determination of theophylline and the LOD and sensitivity of the modified sensor was calculated as 13.26 nM and 1.183 μA·µM−1·cm−2, respectively. In addition, a selectivity, reproducibility and stability of the TiO2 MPs@GOS modified GCE were analyzed towards the determination of theophylline molecule. Finally, the real time application of TiO2 MPs@GOS modified theophylline sensor was established in serum and drug samples.  相似文献   

14.
α-lactalbumin was modified by ultrasound (US, 20 kHz, 43 ± 3.4 W/cm−2) pre-treatments (0, 15, 30 and 60 min) and laccase cross-linking of sonicated α-lactalbumin was used to evaluate the physical and oxidative stability of conjugated linoleic acid (CLA) emulsions. The emulsions prepared with laccase cross-linking US-α-lactalbumin (α-lactalbumin treated with US pre-treatment) and US-α-lactalbumin were scrutinized for oxidative and physical stability at room temperature for two weeks of storage. Laccase cross-linking US-α-lactalbumin (Lac-US-α-lactalbumin) revealed improved physical stability in comparison with US-α-lactalbumin, specified by droplet size, structural morphology, adsorbed protein, emulsifying properties and creaming index. SDS-PAGE analysis showed that there was formation of polymers in Lac-US-α-lactalbumin emulsion. Surface hydrophobicity of Lac-US-α-lactalbumin was higher than that of US-α-lactalbumin, and gradually enhanced with the increase of ultrasound time. More importantly, the measurements of peroxide values and conjugated dienes were used to study the oxidative stability of the CLA emulsions. The Lac-US-α-lactalbumin emulsion proved to be reducing the synthesis of fatty acid hydroperoxides and less conjugated dienes compared to the native and US-α-lactalbumin emulsions. This study revealed that the combination of US pre-treatment and laccase cross-linking might be an effective technique for the modification of CLA emulsions.  相似文献   

15.
《Current Applied Physics》2010,10(5):1255-1260
A new type of inorganic–organic hybrid solid state polymer electrolyte consisting of heteropolytungsticacid impregnated polyepichlorohydrin with iodine/iodide and TiO2 nanofiller have been prepared for their potential application in dye sensitized solar cells. The prepared polymer electrolytes were well characterized by FT-IR, Scanning electron microscopy (SEM), X-ray diffraction (XRD), Electrochemical Impedance analysis (EIS) and Thermal analysis (TGA). The prepared polymer electrolyte with TiO2 nanofiller shows reasonable ionic conductivity (20.4 × 10−6 S cm−1) compared to pure polyepichlorohydrin (2.0 × 10−9 S cm−1) at ambient temperature. The presence of negatively charged redox species heteropolytungsticacid in the polymer matrix prevents the photo reduction of iodide (back electron transfer) and the presence of TiO2 nanofiller increases the degree of amorphousity of the polymer which in turn prolongs the stability of the fabricated dye sensitized solar cell over a long period compared to bare polymer electrolyte.  相似文献   

16.
High quality indium tin oxide (ITO) thin films (In2−xSnxO3: x = 0, 0.1 and 0.2) have been grown by using pulsed laser deposition technique on quartz substrates. The structural, morphological, optical and electrical investigations of deposited films have been studied as a function of substrate deposition temperatures and the Sn compositions. X-ray diffraction (XRD) and high-resolution transmission electron microscopy (HRTEM) patterns affirm that each film is polycrystalline in nature with cubic bixbyite single phase structure which preferentially oriented along (222) Miller plane. The existence of chemical bonding and functional groups was investigated by FTIR spectroscopy. The TEM micrograph of films (@450°C) for x = 0.1 and x = 0.2 reveal spherical morphology with average particle size 63 nm and 51 nm, respectively. The SEM and AFM images show uniform flower like surface morphology and well-demonstrated nanosized spherical particles, respectively. The widening of the band gap of all the films were exclusively defined by Burstein-Moss shift. The Hall measurement reveals that each film is degenerate with n-type semiconducting nature along with high mobility. Low resistivity (2.024 × 10−4 Ω-cm) and high transparency (92.58%) along with high carrier concentration (8.915 × 1020 cm−3) were optimized for x = 0.1 film at 450°C deposition temperature.  相似文献   

17.
In this study, the starch molecules were modified with ultrasonication at two different time intervals by using starch molecules from corn and cassava. This research aimed to examine the effect of the high power ultrasound of 40 kHz voltage and frequency with short time duration on structural and physical properties of corn and cassava starch. Morphology of ultrasonically treated starch granules was observed by scanning electron microscopy (SEM), FTIR, differential scanning calorimetry (DSC), and X-ray diffraction (XRD) and compared with untreated samples. After the ultrasound treatment groove and notch appeared on the surface of the starch granules. The results showed that gelatinization temperature did not change with ultrasound treatments, but enthalpy value decreased from 13.15 ± 0.25 J/g to 11.5 ± 0.29 J/g and 12.65 ± 0.32 J/g to 10.32 ± 0.26 J/g for sonicated corn and cassava starches, respectively. The XRD results revealed a slight decreased in the crystallinity degree (CD) of sonicated corn (25.3,25.1) and cassava starch (21.0,21.4) as compared to native corn (25.6%) and cassava starch (22.2%). This study suggests that non-thermal processing techniques have the potential to modify the starch from different sources and their applications due to starch’s versatility, low cost, and comfort of use after processing with altered physicochemical properties.  相似文献   

18.
Rhenium oxide nanoparticles have been prepared using ultrasonication at 20 kHz. Samples characterization was committed via SEM-EDX, TEM, XRD, and Raman spectroscopy. Various experimental parameters were examined, including precursor/substrate amounts, ultrasonication intensity, and type of solvent used. Insights to the agglomeration of the prepared nanoparticles depending on the preparation parameters are given. As ultrasonic source we used either an ultrasonic probe by Sonics & Materials Inc. (20 kHz, 750 W net output) or a Bandelin SONOPULS HD 3200 ultrasound generator (20 kHz, 200 W net output) at intensities between 30 and 100 W/cm2. The rhenium oxide nanoparticles haven been decorated on state-of-the-art anode materials (NiO/GDC) for solid oxide fuel cells (SOFCs) in order to prepare catalytically more active anode powders. These experiments revealed that ultrasonication intensity and solvents used are able to affect final nanoparticles size distribution and morphology. At the same time, ratio of precursor and substrate compounds amounts as well as ultrasonication intensity and duration were all found to affect the decoration loading extend of nanoformations on substrate powders. The results showing the influence of the above-mentioned parameters allowed for the quantification of the effects on the loading and the preferable sites of the decoration.  相似文献   

19.
Multiwalled carbon nanotubes (MWCNTs) and Vulcan carbon (VC) decorated with SnO2 nanoparticles were synthesized using a facile and versatile sonochemical procedure. The as-prepared nanocomposites were characterized by means of transmission electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy, and Fourier transform infra red spectroscopy. It was evidenced that SnO2 nanoparticles were uniformly distributed on both carbon surfaces, tightly decorating the MWCNTs and VC. The electrochemical performance of the nanocomposites was evaluated by cyclic voltammetry and galvanostatic charge/discharge cycling. The as-synthesized SnO2/MWCNTs nanocomposites show a higher capacity than the SnO2/VC nanocomposites. Concretely, the SnO2/MWCNTs electrodes exhibit a specific capacitance of 133.33 F g−1, whereas SnO2/VC electrodes exhibit a specific capacitance of 112.14 F g−1 measured at 0.5 mA cm−2 in 1 M Na2SO4.  相似文献   

20.
Metallic gold nanoparticles have been synthesized by the reduction of chloroaurate anions [AuCl4] solution with hydrazine in the aqueous starch and ethylene glycol solution at room temperature and at atmospheric pressure. The characterization of synthesized gold nanoparticles by UV–vis spectroscopy, high resolution transmission electron microscopy (HRTEM), electron diffraction analysis, X-ray diffraction (XRD), and X-rays photoelectron spectroscopy (XPS) indicate that average size of pure gold nanoparticles is 3.5 nm, they are spherical in shape and are pure metallic gold. The concentration effects of [AuCl4] anions, starch, ethylene glycol, and hydrazine, on particle size, were investigated, and the stabilization mechanism of Au nanoparticles by starch polymer molecules was also studied by FT-IR and thermogravimetric analysis (TGA). FT-IR and TGA analysis shows that hydroxyl groups of starch are responsible of capping and stabilizing gold nanoparticles. The UV–vis spectrum of these samples shows that there is blue shift in surface plasmon resonance peak with decrease in particle size due to the quantum confinement effect, a supporting evidence of formation of gold nanoparticles and this shift remains stable even after 3 months.  相似文献   

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