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1.
A series of superabsorbents based on sodium acrylate (NaA), mica (MI), and N,N′-methylene-bis-acrylamide (NMBA) were prepared by inverse suspension polymerization. The influences of the type and content of mica such as pure K+-MI and intercalated-MI (IMI) in the composite gels on the water absorbency and the initial absorption rate in deionized water and salt solutions were investigated. Results showed that the water absorbency and initial absorption rate gradually decrease with increasing amounts of pure K+-MI and intercalated-MI. In addition, the water absorbency and initial absorption rate for the gels prepared by intercalated-MI were lower than those prepared by pure K+-MI.  相似文献   

2.
A novel photocatalytically degradable TiO2/poly[acrylamide-co-(acrylic acid)] composite hydrogel (TiO2/poly[AAm-co-AAc]) was synthesized by polymerization in an aqueous solution with N,N’-methylenebisacrylamide as the crosslinker and ammonium persulphate and TEMED as the initiator pair. The combined and separate effects of photodegradation and adsorption processes for dye removal were evaluated using methylene blue (MB) as the model dye for a photodegradation target, and compared with those of the neat poly[AAm-co-AAc], and a commercially available TiO2 photocatalyst (Degussa P-25). Without photodegradation (i.e. in the dark), the TiO2/poly[AAm-co-AAc] composite adsorbed up to 85% of the MB from a 5 mg L−1 MB solution in 15 min compared to only 10% for the pristine TiO2. The reproducibility in photodegradation of the reused poly[AAm-co-AAc] composite was also investigated, where poly[AAm-co-AAc] was found to be photocatalytically degraded under UV irradiation. Therefore, the TiO2/poly[AAm-co-AAc] composite hydrogel is a good dye adsorber with self-photodegradability and it also can easily be separated from the reaction by simple filtration. With these properties, the TiO2/poly[AAm-co-AAc] hydrogel can be called a green polymer for use in the photodegradation-adsorption process for the abatement of various pollutants.  相似文献   

3.
This paper investigates the degradation of polyhydroxyalkanoates and its biofiber composites in both soil and lake environment. Time-dependent changes in the weight loss of films were monitored. The rate of degradation of poly(3-hydroxybutyrate) [P(3HB)], poly(3-hydroxybutyrate-co-4-hydroxybutyrate) [P(3HB-co-23?mol% 4HB)] and poly(3-hydroxybutyrate-co-3-hydroxyvalerate-co-4-hydroxybutyrate) [P(3HB-co-9?mol% 3HV-co-19?mol% 4HB)] were investigated. The rate of degradation in the lake is higher compared to that in the soil. The highest rate of degradation in lake environment (15.6?% w/w week?1) was observed with P(3HB-co-3HV-co-4HB) terpolymer. Additionally, the rate of degradation of poly(3-hydroxybutyrate-co-3-hydroxyvalerate) [P(3HB-co-38?mol% 3HV)] was compared to PHBV biofiber composites containing compatibilizers and empty fruit bunch (EFB). Here, composites with 30?% EFB displayed the highest rate of degradation both in the lake (25.6?% w/w week?1) and soil (15.6?% w/w week?1) environment.  相似文献   

4.
The development of nanostructured conducting polymers based materials for electrochemical applications has attracted intense attention due to their environmental stability, unique reversible redox properties, abundant electron active sites, rapid electron transfer and tunable conductivity. Here, a phytic acid doped polyaniline nanofibers based nanocomposite was synthesized using a simple and green method, the properties of the resulting nanomaterial was characterized by electrochemical impedance spectroscopy (EIS), Fourier transform infrared spectroscopy (FT-IR), scanning electron microscopy (SEM), and energy dispersive spectroscopy (EDS). A glassy carbon electrode modified by the nanocomposite was evaluated as a new platform for the simultaneous detection of trace amounts of Cd2+ and Pb2+ using differential pulse anodic stripping voltammetry (DPASV). The synergistic contribution from PANI nanofibers and phytic acid enhances the accumulation efficiency and the charge transfer rate of metal ions during the DPASV analysis. Under the optimal conditions, good linear relationships were obtained for Cd2+ in a range of 0.05–60 μg L−1, with the detection limit (S/N = 3) of 0.02 μg L−1, and for Pb2+ in a range of 0.1–60 μg L−1, with the detection limit (S/N = 3) of 0.05 μg L−1. The new electrode was successfully applied to real water samples for simultaneous detection of Cd2+ and Pb2+ with good recovery rates. Therefore, the new electrode material may be a capable candidate for the detection of trace levels of heavy metal ions.  相似文献   

5.
A novel kind of salt-resistant superabsorbent composite, polyacrylamide/attapulgite, from acrylamide (AM) and attapulgite (APT) was prepared by free-radical aqueous polymerization, using N,N′-methylenebisacrylamide (MBA) as a crosslinker and ammonium persulfate (APS) as an initiator. The organification of APT with hexadecyltrimethyl ammonium bromide (HDTMABr) was proved by FTIR and XRD. The effects of acidified APT (H+-APT), organo-APT (HDTMABr-APT) and the content of APT in the superabsorbent composite on the water absorbency and the initial swelling rate for the superabsorbent composite in distilled water and in various saline solutions were studied. The effects of incorporated HDTMABr-APT and H+-APT on the reswelling ability of the superabsorbent composites were investigated. The results indicate that the incorporation of APT had remarkable influence on the improvement of water absorbency and swelling rate of the composites. Comparing with the composite doped with H+-APT, the water absorbency for the composite doped with 10 wt% HDTMABr-APT was enhanced from 2140 g g−1 to 2800 g g−1 in distilled water and from 100 g g−1 to 121 g g−1 in 0.9 wt% NaCl solution, respectively. The water absorbency of the composites in various saline solutions decreased with the increasing concentration, especially for the multivalent cations. In addition, the reswelling ability of the superabsorbent composites is also improved evidently by adding a small amount of HDTMABr-APT into the composite, comparing with that of incorporated with H+-APT.  相似文献   

6.
An extracting medium based on chitosan–polypyrrole (CS–PPy) magnetic nanocomposite was synthesized by chemical polymerization of pyrrole at the presence of chitosan magnetic nanoparticles (CS-MNPs) for micro-solid phase extraction. In this work, magnetic nanoparticles, the modified CS-MNPs and different types of CS–PPy magnetic nanocomposites were synthesized. Extraction efficiency of the CS–PPy magnetic nanocomposite was compared with the CS-MNPs and Fe3O4 nanoparticles for the determination of naproxen in aqueous samples, via quantification by spectrofluorimetry. The scanning electron microscopy images obtained from all the prepared nanocomposites revealed that the CS–PPy magnetic nanocomposite possess more porous structure. Among different synthesized magnetic nanocomposites, CS–PPy magnetic nanocomposite showed a prominent efficiency. Influencing parameters on the morphology of CS–PPy magnetic nanocomposite such as weight ratio of components was also assayed. In addition, effects of different parameters influencing the extraction efficiency of naproxen including desorption solvent, desorption time, amount of sorbent, ionic strength, sample pH and extraction time were investigated and optimized. Under the optimum condition, a linear calibration curve in the range of 0.04–10 μg mL−1 (R2 = 0.9996) was obtained. The limits of detection (3Sb) and limits of quantification (10Sb) of the method were 0.015 and 0.04 μg mL−1 (n = 3), respectively. The relative standard deviation for water sample spiked with 0.1 μg mL−1 of naproxen was 3% (n = 5) and the absolute recovery was 92%. The applicability of method was extended to the determination of naproxen in tap water, human urine and plasma samples. The relative recovery percentages for these samples were in the range of 56–99%.  相似文献   

7.
吴飞鹏 《高分子科学》2011,29(3):352-359
A series of cationic surfmers with benzyl groups(QARBCs)with different R groups on the benzene ring were synthesized and characterized by IR,1H-NMR,13C-NMR.The aggregation of QARBCs was studied by the steady-state fluorescence technique.It turned out that QARBCs had surface activity and their critical micelle concentration(CMC)values varied in the range of 10-2—10-3mol/L with slight increase with temperature.The copolymerization of acrylamide(M1)and QARBCs(M2)was studied below and above CMC,their reactivity ratios were determined by the Finemann-Ross method.It was found that below CMC,copolymerization took place in a homogeneous system and reactivity ratios of acrylamide and QARBCs were less than 1;while above CMC,reactivity ratios of QARBCs were greater than 1.The copolymerization mechanism of QARBC was observed to be similar to that of micellar polymerization.QARBCs tended to homopolymerization,which gave rise to micro-blocky sequences in the polymer backbone.The Q and e values of QARBCs were calculated according to the Alfrey-Price equation by using r1(AM)and r2(qarBC).Samples of poly(AM-co-QARBC) were prepared above and below CMC and their hydrophobic associations were studied by the steady-state fluorescence spectra and 2D NOESY spectra,and their critical associating concentrations(CAC)were estimated.The results showed that samples of poly(AM-co-QARBC)prepared above CMC had stronger hydrophobic association in aqueous solution than those prepared below CMC.  相似文献   

8.
We isolated 5 mesophilic microorganisms that form clear zones around the colony on an opaque medium containing the aliphatic-aromatic copolyester poly(60 mol% butylene adipate-co-40 mol% butylene terephthalate) (PBAT). Among all strains, the fungal strain NKCM1712 degraded PBAT at the fastest rate (3.5 ± 0.3 μg cm−2 h−1). Genetic and morphological analyses revealed that this strain was closely related to Isaria fumosorosea (phylum Ascomycota). Mass spectroscopic analysis revealed that the degradation products were T, AB, TB, BAB, and ABT (T, terephthalic acid unit; A, adipic acid unit; B, 1,4-butanediol unit)] in the culture of the strain that used PBAT as the sole carbon source. Furthermore, the PBAT degradation ability of this strain in terms of BOD suggested that it could utilize the PBAT degradation products as growth substrates. This is the first report of a mesophilic strain that can mineralize an aliphatic-aromatic polyester into carbon dioxide on its own.  相似文献   

9.
In this present work a method for the determination of Ca, Fe, Ga, Na, Si and Zn in alumina (Al2O3) by inductively coupled plasma optical emission spectrometry (ICP OES) with axial viewing is presented. Preliminary studies revealed intense aluminum spectral interference over the majority of elements and reaction between aluminum and quartz to form aluminosilicate, reducing drastically the lifetime of the torch. To overcome these problems alumina samples (250 mg) were dissolved with 5 mL HCl + 1.5 mL H2SO4 + 1.5 mL H2O in a microwave oven. After complete dissolution the volume was completed to 20 mL and aluminum was precipitated as Al(OH)3 with NH3 (by bubbling NH3 into the solution up to a pH ~ 8, for 10 min). The use of internal standards (Fe/Be, Ga/Dy, Zn/In and Na/Sc) was essential to obtain precise and accurate results. The reliability of the proposed method was checked by analysis of alumina certified reference material (Alumina Reduction Grade-699, NIST). The found concentrations (0.037% w w−1 CaO, 0.013% w w−1 Fe2O3, 0.012% w w−1 Ga2O3, 0.49% w w−1 Na2O, 0.014% w w−1 SiO2 and 0.013% w w−1 ZnO) presented no statistical differences compared to the certified values at a 95% confidence level.  相似文献   

10.
A novel, sensitive and high selective flow-injection chemiluminescence (FI-CL) method for the determination of phenol is reported, based upon its decreasing effect on the CL reaction of luminol with hydrogen peroxide catalyzed by manganese (III) deuteroporphyrin [MnDP, Scheme 1, 3] in alkaline solution. Under the selected optimized experimental conditions, the relative CL intensity was linear with phenol in the range of 4.0 × 10−9 to 4.0 × 10−7 g mL−1. The detection limit (3σ) was 6.3 × 10−10 g mL−1 and the relative standard deviation for 1.0 × 10−7 g mL−1 phenol (n = 11) was 2.99%. The regression equation was I = 120.79 + 1.14 × 1010c (R = 0.9936). This method has been applied to the determination of phenol in water with satisfactory results.  相似文献   

11.
Poly(acrylamide-co-itaconic acid) (P(AM-co-IA)) hydrogel microspheres were prepared via inverse suspension polymerization method. DLS results showed the formation of the monodispersed hydrogel microspheres. The size of the hydrogel microspheres could be controlled by polymerization parameters. Absorbencies of P(AM-co-IA) microspheres in water and saline were investigated and calculated by size changes of each particle before and after swelling. The results showed that P(AM-co-IA) had high absorbencies, the weight of swollen particles was above 4000 times to that of the original dried microspheres. The superabsorbent hydrogel microspheres might find the potential applications in the fields of soil amendments, water shutoff agents, and drug delivery carriers.  相似文献   

12.
A facile method to fabricate tough and highly stretchable polyacrylamide (PAM) nanocomposite physical hydrogel (NCP gel) was proposed. The hydrogels are dually crosslinked single network with the PAM grafted vinyl hybrid silica nanoparticles (VSNPs) as the analogous covalent crosslinking points and the reversible hydrogen bonds among the PAM chains as the physical crosslinking points. In order to further elucidate the toughening mechanism of the PAM NCP gel, especially to understand the role of the dual crosslinking points, the PAM hybrid hydrogels (H gels) and a series of poly(acrylamide-co-dimethylacrylamide) (P(AM-co-DMAA)) NCP gels were designed and fabricated. Their mechanical properties were compared with those of the PAM NCP gels. The PAM H gels are prepared by simply mixing the PAM chains with bare silica nanoparticles (SNPs). Relative to the poor mechanical properties of the PAM H gel, the PAM NCP gel is remarkably tough and stretchable and also generates large number of micro-cracks to stop notch propagation, indicating the important role of PAM grafted VSNPs in toughening the NCP gel. In the P(AM-co-DMAA) NCP gels, the P(AM-co-DMAA) chains are grafted on VSNPs and the polydimethylacrylamide (PDMAA) only forms very weak hydrogen bonds between themselves. It is found that mechanical properties of the PAM NCP gel, such as the tensile strength and the elongation at break, are enhanced significantly, but those of the P(AM-co-DMAA) NCP gels decreased rapidly with decreasing AM content. This result reveals the role of the hydrogen bonds among the grafted polymer chains as the physical crosslinking points in toughening the NCP gel.  相似文献   

13.
Two negatively charged polyelectrolyte complex colloidal nanoparticles (PEC) and one positively charged nanoparticle (PEC+) were prepared and used as novel layer-by-layer (LbL) building blocks. These PEC nanoparticles include poly(2-methacryloyloxy ethyl trimethylammonium chloride)/sodium carboxymethyl cellulose (PDMC/CMCNa PEC), poly(diallyldimethylammonium chloride)/CMCNa (PDDA/CMCNa PEC) and PDDA/poly(sodium-p-styrenesulfonate) (PDDA/PSS PEC+). LbL multilayer films based on (PEC+/PEC) were constructed on both quartz slides and modified polyamide (MPA) reverse osmosis support membranes. UV–vis spectroscopy, quartz crystal microbalance (QCM), field emission scanning microscopy (FESEM) and atomic force microscopy (AFM) were utilized to follow the thickness growth and morphology evolution of these multilayer films with increasing bi-layer numbers. LbL multilayer films deposited on MPA support membranes were subjected to pervaporation dehydration of 10 wt% water–isopropanol and effect of bi-layer numbers and feed temperature on pervaporation performance was studied. Generally, PEC+/PEC can be LbL self-assembled successfully on both substrates with a thickness growth rate ca. 200 nm/bi-layer. Moreover, PEC+/PEC multilayer films show high pervaporation performance with film thickness up to several micrometers. For example, performance of the multilayer films in dehydrating 10 wt% water–isopropanol at 50 °C is J = 1.18 kg/m2 h, α = 1013 for (PEC+/PDMC-CMCNa PEC)24 and J = 1.36 kg/m2 h, α = 938 for (PEC+/PDMC-CMCNa PEC)25, respectively.  相似文献   

14.
Superabsorbent polymer acrylamide (AM)/itaconic acid (IA) and its nanocomposite were synthesized by redox polymerization in an aqueous solution of both monomers with mica used as an inorganic additive. The influences of IA concentration, mica content, and crosslinker concentration on the water absorption and physical properties of the superabsorbent polymer and its nanocomposite were examined. Water absorbency in artificial urine by the synthesized copolymers, and the gel strength of the superabsorbent copolymers and their nanocomposites, were tested with loads of 0.28 or 0.70 psi. Transmission electron micrographs and X‐ray diffraction confirmed that the polymer chains were successfully intercalated into the silicate layers in the mica. The water absorbency and the artificial urine absorbency of the composite with an AM‐to‐IA mole ratio of 95:5, 0.2% mol N‐MBA, and 5% w/w mica were 748 ± 5 and 76 ± 2 g g?1, respectively, whilst the neat copolymer achieved only 640 ± 7 and 72 ± 2 g g?1 in water and artificial urine, respectively. The viscoelastic behavior suggested that the swollen gel of the nanocomposites exhibited mechanical stability and elasticity. Copyright © 2009 John Wiley & Sons, Ltd.  相似文献   

15.
Segura R  Pradena M  Pinto D  Godoy F  Nagles E  Arancibia V 《Talanta》2011,85(5):2316-2319
A sensitive procedure is presented for the voltammetric determination of nickel. The procedure involves an adsorptive accumulation of nickel 1-nitroso-2-napthol (NN) complex on a bismuth film electrode prepared ex situ by electrodeposition. The most suitable operating conditions and parameters such as pH, ligand concentration (CNN), adsorptive potential (Eads), adsorptive time (tads), scan rate and others were selected and the determination of nickel in aqueous solutions using the standard addition method was possible. The adsorbed Ni-NN complex gives a well defined cathodic stripping peak current at −0.70 V, which was used for the determination of nickel in the concentration range of 10.0-70.0 μg L−1 (pH 7.5; CNN 6.5 μmol L−1; Eads −0.30 V; tads 60 s) with a detection limit of 0.1 μg L−1. The relative standard deviation for a solution containing 10.0 μg L−1 of Ni(II) was 3.5% (n = 4). The proposed method was validated determining Ni(II) in certified reference waste water (SPS-WW1) and Certified Reference Water for Trace Elements (TMDA 51.3) with satisfactory results. Then lake water samples were analyzed.  相似文献   

16.
Low column efficiency for small molecules in reversed-phase chromatography is a major problem commonly encountered in polymer-based monoliths. Herein, a novel highly crosslinked porous polymeric monolith was in situ prepared by using a multi-acrylate monomer, dipentaerythritol penta-/hexa-acrylate (DPEPA), as crosslinker, which copolymerized with lauryl methacrylate (LMA) as functional monomer in a UV-transparent fused-silica capillary via photo-initiated free-radical polymerization within 5 min. The mechanical stability and permeability of the resulting poly(LMA-co-DPEPA) monolith were characterized in detail. One series of highly crosslinked poly(LMA-co-DPEPA) columns were prepared with relatively higher content of crosslinker (63.3%) in the precursor. Although they exhibited lower permeability, high column efficiency for alkylbenzenes was acquired in cLC, and the minimum plate height (column B) was in the range of 6.04–9.00 μm, corresponding to 111,000–165,000 N m−1. Meanwhile, another series of poly(LMA-co-DPEPA) columns prepared with relatively lower content of crosslinker (52.7%) in the precursor exhibited higher permeability, but the minimum plate height (column E) was relatively low in the range of 10.75–20.04 μm for alkylbenzenes, corresponding to 50,000–93,000 N m−1. Compared with common poly(LMA-co-EDMA) columns previously reported, the highly crosslinked poly(LMA-co-DPEPA) columns using a multi-acrylate monomer as crosslinker possessed remarkably high column efficiency for small molecules in cLC. By plotting of plate height (H) of alkylbenzenes versus the linear velocity (u) of mobile phase, the results revealed a retention-independent efficient performance of small molecules in the isocratic elution, indicating that the use of multi-functional crosslinker possibly prevents the generation of gel-like micropores in the poly(LMA-co-DPEPA) monolith, reducing the mass transfer resistance (C-term).  相似文献   

17.
Tie-line data for the water, ethanol, and cyclohexane [{w1H2O + w2C2H5OH + (1−w1w2)C6H12}] ternary system, where w is the mass fraction, was investigated at T=303.15 K. A quaternary system containing these three compounds and benzene {w1C2H5OH + w2C6H6 + w3C6H12 + (1−w1w2w3)H2O} was also studied at the same temperature, while data on its other two partially miscible ternary systems were taken from the literature [the fourth {w1C2H5OH + w2C6H6 + (1−w1w2)C6H12} is not partially miscible]. From our experimental results we conclude that this quaternary system presents a very small water tolerance and that phase separation could produce a considerable loss of C2H5OH drawn into the aqueous phase. On the other hand, the results also show that the aqueous phase generally contains a higher concentration of C6H6 than of C6H12. A comparison with other similar quaternary systems investigated in our laboratory was also made. The ternary experimental results were correlated with the UNIQUAC equation, and predicted with the UNIFAC group contribution method. As previously, the equilibrium data of the three ternary systems (including those taken from the literature) were used to determine interaction parameters for the UNIQUAC equation. These parameters were then averaged in order to predict equilibrium data of this quaternary system. The UNIFAC method was also used with the same purpose. The UNIQUAC equation appears to be more accurate than the UNIFAC method for this ternary system. However, this last model is slightly better for the quaternary system, as can be seen from the values of both residuals.  相似文献   

18.
New poly (vinylidenefluoride-co-hexafluoro propylene) (PVDF-HFP)/CeO2-based microcomposite porous polymer membranes (MCPPM) and nanocomposite porous polymer membranes (NCPPM) were prepared by phase inversion technique using N-methyl 2-pyrrolidone (NMP) as a solvent and deionized water as a nonsolvent. Phase inversion occurred on the MCPPM/NCPPM when it is treated by deionized water (nonsolvent). Microcomposite porous polymer electrolytes (MCPPE) and nanocomposite porous polymer electrolytes (NCPPE) were obtained from their composite porous polymer membranes when immersed in 1.0 M LiClO4 in a mixture of ethylene carbonate/dimethyl carbonate (EC/DMC) (v/v = 1:1) electrolyte solution. The structure and porous morphology of both composite porous polymer membranes was examined by scanning electron microscope (SEM) analysis. Thermal behavior of both MCPPM/NCPPM was investigated from DSC analysis. Optimized filler (8 wt% CeO2) added to the NCPPM increases the porosity (72%) than MCPPM (59%). The results showed that the NCPPE has high electrolyte solution uptake (150%) and maximum ionic conductivity value of 2.47 × 10−3 S cm−1 at room temperature. The NCPPE (8 wt% CeO2) between the lithium metal electrodes were found to have low interfacial resistance (760 Ω cm2) and wide electrochemical stability up to 4.7 V (vs Li/Li+) investigated by impedance spectra and linear sweep voltammetry (LSV), respectively. A prototype battery, which consists of NCPPE between the graphite anode and LiCoO2 cathode, proves good cycling performance at a discharge rate of C/2 for Li-ion polymer batteries.  相似文献   

19.
Poly[acrylamide-co-(2-acrylamido-2-methylpropane sodium sulfonate)] superabsorbents and superabsorbent composites (SAPCs) with zinc borate and/or melamine as fire retardants were synthesized. Water absorbencies decreased inversely to added amount of fire retardant. Thermal stability of SAPC/zinc borate increases with increasing zinc borate. Incorporating melamine improved thermal stability of the SAPC until 300 °C. Flammability analysis demonstrated that wood surface coated with SAP or SAPC emulsions extended time to ignition of the wood. Peak heat release rate and total heat release are smallest in specimens coated with SAPC/30% melamine. Wood coated with SAPC incorporating 20% zinc borate/10% melamine mixture gave the longest time to ignition at 4½ min.  相似文献   

20.
A novel Fe3O4–poly(aniline-naphthylamine)-based nanocomposite was synthesized by chemical oxidative polymerization process as a magnetic sorbent for micro solid phase extraction. The scanning electron microscopy images of the synthesized nanocomposite revealed that the copolymer posses a porous structure with diameters less than 50 nm. The extraction efficiency of this sorbent was examined by isolation of rhodamine B, a mutagenic and carcinogenic dye, from aquatic media in dispersion mode. Among different synthesized polymers, Fe3O4/poly(aniline-naphthylamine) nanocomposite showed a prominent efficiency. Parameters including the desorption solvent, amount of sorbent, desorption time, sample pH, ionic strength, extraction time and stirring rate were optimized. Under the optimum condition, a linear spiked calibration curve in the range of 0.35–5.00 μg L−1 with R2 = 0.9991 was obtained. The limits of detection (3Sb) and limits of quantification (10Sb) of the method were 0.10 μg L−1 and 0.35 μg L−1 (n = 3), respectively. The relative standard deviation for water sample with 0.5 μg L−1 of RhB was 4.2% (n = 5) and the absolute recovery was 92%. The method was applied for the determination of rhodamine B in dishwashing foam, dishwashing liquid, shampoo, pencil, matches tips and eye shadows samples and the relative recovery percentage were in the range of 94–99%.  相似文献   

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