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1.
Cellulose gel films were prepared by regeneration process using pre-cooled aq.(8 wt% LiOH + 15 wt% urea) mixture as solvent and ethyl alcohol as non solvent. The Terminus cattapa leaf extract diffused wet cellulose films were then dipped in 1–5 mM aq.AgNO3 solutions to allow in situ generation of silver nanoparticles (AgNPs). Besides the in situ generation, some AgNPs were also formed outside the wet films in the solution. The AgNPs formed outside the films were observed under transmission electron microscope and scanning electron microscope. The nanocomposite films were also characterized by Fourier transform infrared spectroscopy, X-ray diffraction and thermogravimetric analysis and tensile test. The thermal stability of the composite films was lower than that of the matrix up to a temperature of ~300 °C and afterwards showed a reverse trend. The tensile strength of the nanocomposite films was found to be higher than the matrix but decreased with increasing concentration of aq.AgNO3. The cellulose/AgNPs composite films showed good antibacterial activity against E. coli (gram positive) and Bacillus sp. (gram negative). Based on the aforementioned properties, the cellulose/AgNPs composite films can be considered for antibacterial packaging and medical applications.  相似文献   

2.
Polyaniline (PANI) and Ag/PANI nanoporous composite were prepared by an oxidative polymerization method. The oxidation process of PANI nanoparticles was occurred using (NH4)2S2O8 while the oxidation process of Ag/PANI nanoporous composite was occurred using AgNO3 under the effect of artificial radiation. The structural, morphological, and optical properties of the PANI and Ag/PANI nanoporous structures were studied using different characterization tools. The results confirm the formation of polycrystalline nanoporous PANI and spherical nanoporous composite of Ag/PANI particles. Antibacterial activity tests against gram-positive bacteria, Bacillus subtilis and Staphylococcus aureus, and gram-negative bacteria, Escherichia coli, and Salmonella species were carried out using different concentrations of PANI nanoparticles and Ag/PANI nanoporous composites. PANI has not antibacterial effect against all studied pathogens. In contrast, Ag/PANI nanoporous composites possessed antibacterial activity that is identified by the zone of inhibition. The inhibition zones of bacteria are in order; Salmonella species?>?S. aureus?>?B. subtilis?>?E. coli. The inhibition zones of all bacteria increased with increasing concentrations of Ag/PANI nanoporous composites from 200 to 400 ppm then decreased with further increasing of the dose concentrations to 600 ppm. Finally, a simplified mechanism based on the electrostatic attraction is presented to describe the antimicrobial activity of Ag/PANI nanoporous composite.  相似文献   

3.
Cultivation conditions affecting poly(vinyl alcohol) (PVA) degradation by a mixed bacterial culture of Bacillus sp. and Curtobacterium sp. were investigated. Bacterial strains used in this study were isolated from the watercourse and the sewage sludge of vinylonfibre mill by enrichments on PVA as the sole carbon source. The results showed that PVA was greatly degraded under the following conditions: 0.5% PVA as a substrate at the initial medium pH of 8 with 0.15% glucose and urea at C/U ratio 1.5:1 and 1% bacterial inoculum, at a temperature of 35 °C and a shaking speed of 110 rpm. The analysis of FTIR and 1H NMR spectra before and after biodegradation indicate fission of the PVA molecular chain during the incubation.  相似文献   

4.
Sorption of Sr on bentonite was studied using the batch technique. Distribution coefficients (Kd) were determined as a function of contact time, pH, sorbent and sorbate concentration and temperature. The data were interpreted in terms of Freundlich, Langmuir and Dubinin-Radushkevich isotherms. Thermodynamic parameters for the sorption system were determined at three different temperatures. The positive value of the heat of sorption, ΔH° = 30.62 kJ/mol at 298 K, shows that the sorption of strontium on bentonite is endothermic. The negative value of the free energy of sorption, ΔG° = −10.69 kJ/mol at 298 K, shows the spontaneity of the reaction. ΔG° becomes more negative with increasing temperature, which shows that the sorption process is more favorable at higher temperatures. The mean free energy for sorption, E 9 kJ/mol, suggests that ion exchange is the predominant mode of sorption in the Sr concentration range studied, i.e. 0.01 – 0.3 mol/dm3. The presence of complementary cations depresses the sorption of strontium on bentonite in the order Ca2+>Mg2+>K+>Na+. Some organic complexing agents and natural ligands also affect the sorption of strontium. The desorption studies with ground water at low strontium loadings on bentonite show that about 90% of Sr is irreversibly sorbed on the bentonite.  相似文献   

5.
Coaxial electrospinning technique was used to fabricate the core–sheath composite nanofibers of ZnO nanoparticle (Nps) (10%, 20% w/w) doped polymethyl methacrylate (PMMA) (as sheath) and polyvinyl alcohol (PVA) (as core). Fourier transform infrared (FT-IR) spectra were confirmed the weak forces arise between ZnO Nps, PMMA and PVA matrixes. The hexagonal (wurtzite) structure of ZnO Nps with ~?30.8 nm of diameter was confirmed from the X-ray diffraction pattern. The morphology and microstructure of core–sheath composite nanofibers were confirmed from the scanning electron microscopy (SEM) and transmission electron microscopy (TEM). It is clearly seen from the TEM images that the PMMA encapsulate the PVA core. Core–sheath composite nanofibers were assessed against Escherichia coli (E. coli) and Bacillus subtilis (B. subtilis) bacteria through quantitative, disk diffusion and viable cell count methods. It was found that ZnO Nps doped core–sheath nanofibers were effectively inhibit the growth of gram positive bacteria, B. subtilis.  相似文献   

6.
High quality graphene sheets (GRP) have been exfoliated using facile one pot method through direct ultrasonication of graphite in the presence of polyvinyl alcohol. The GRP were decorated with silver nanoparticles (AgNPs) producing graphene–silver nanoparticle composites. The effect of variation of graphite and silver salt mass ratios on the morphology and performance of produced composites was studied. The size of AgNPs decorated on GRP has been tuned with synthesis method optimization. The average size of AgNPs was found to be in the range of 8.6–15.6 nm. Cotton–polyester blend textile fabrics were treated with the new smart developed composite as antibacterial agent producing new composites. A significant inhibition of bacterial growth has been observed for graphene–silver nanoparticle composite and the antibacterial efficiency was optimized. The clear inhibition zone for textiles treated with new developed composite and AgNPs alone was recorded as 12 and 1.75 mm respectively, achieving more than six fold improvement.  相似文献   

7.
Styrene (St) was graft-polymerized onto the surfaces of micro-sized silica gel particles, and the surface-grafted composite particles PSt/SiO2 were obtained. With the surface-grafted composite particles PSt/SiO2 as a starting material, water-insoluble antibacterial materials with quaternary ‘onium’ salt-type were synthesized via two polymer reaction steps. The grafted polystyrene was first chloromethylated, resulting in grafted particles CMPS/SiO2, and then quaterisation (QN) and quaternary phosphonium reaction (QP) were conducted with triethylamine, tri-n-butylamine and triphenyl phosphine as reagents, respectively. Two kinds of water-insoluble antibacterial materials, QN-PSt/SiO2 and QP-PSt/SiO2 were prepared. Their antibacterial property was mainly investigated by using Escherichia coli (E. coli) as a model bacterium and by adopting colony count method. The relationship between the chemical structure of the antibacterial group and antimicrobial activity for the water-insoluble antibacterial materials was studied in detail, and their antibacterial mechanism was investigated by TTC-dehydrogenase activity determination and extracellular DNA and RNA measurement methods. The experimental results show that QN-PSt/SiO2 and QP-PSt/SiO2 possess strong antibacterial activity. The main factors affecting the antibacterial ability of the water-insoluble materials are the chemical structure of the antibacterial groups, the bound density of the antibacterial groups on the surface of the water-insoluble antibacterial materials as well as the pH value of the medium. QP-PSt/SiO2 has stronger antibacterial activity than QN-PSt/SiO2; the QN-PSt/SiO2 prepared with tri-n-butylamine has stronger antibacterial activity than that prepared with triethylamine; the water-insoluble material with higher bound density of the antibacterial groups has stronger antibacterial ability; as the pH value of the medium is over the isoelectric point of E. coli, the antibacterial ability is strengthened with the increase of pH value.  相似文献   

8.
Journal of Polymers and the Environment - In this study, we prepared Poly (vinyl alcohol) (PVA)/Guar gum (GG) based nanocomposite films with a different weight ratio of silver nanoparticles (AgNPs)...  相似文献   

9.

Pollution and destruction of the environment due to the accumulation of non-degradable plastics are some of the most important concerns in the world. A significant amount of this waste is related to the polymers used in food packaging. Therefore, experts in the food industry have been looking for suitable biodegradable alternatives to synthetic polymers. Preparing biocompatible and biodegradable films based on starch is a good choice. In this study, various factors affecting films of starch/polyvinyl alcohol (PVA)/containing ZnO nanoparticles such as the amount of starch, PVA, glycerol, and ZnO were evaluated by response surface methodology (RSM). Film formation by solvent casting method, mechanical properties, swelling, solubility, and water vapor permeability (WVP) were selected as responses of RSM. The results showed that hydrogen bonding interactions between polyvinyl alcohol and starch improved the film formation. The effect of glycerol and PVA content on the mechanical strength was contrary to each other. As the amount of PVA increased, the tensile strength first decreased and then increased. The value of WVP was for all Runs from 0 to 6.77?×?10??8 g m??1 s??1 Pa??1. Finally, films with high film formation, maximum tensile strength, and high elongation at break, minimum solubility, permeability, and swelling were optimized.

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10.
The common biodegradable properties of polymer make them an excellent pair for blending, and the water solubility of polyvinyl alcohol (PVA) makes it easy to mix evenly with the starch. In this study, PVAs with different molecular weights were blended with various compositions of cross-linked starch (CLS) to explore the effects of molecular weight of PVA on the biodegradable characteristics of the PVA/starch blends. Comparing the biodegradability of all the various PVA/starch blends, a PVA was singled out from the PVA/starch blends of higher biodegradability. Further, the chosen PVA was then blended with the acid-modified starch (AMS) to systematically investigate the effects of the modified processing of starch on the biodegradable characteristics of the PVA/starch blends. Differential scanning calorimetry (DSC) analysis of PVA and PVA/starch specimens reveal that the Tm values of PVA/starch specimens reduce gradually as their CLS or AMS contents increase. After the CLS is blended in PVAs of different molecular weights, the tensile strength (??f) and elongation at break (??f) values of (P100S0)G20M1 specimen increase and simultaneously reduce, respectively, as their molecular weights of PVA increase from about 80,000 (PVABF-17) to 120,000 (PVABF-26). The ??f and ??f values of the PVA/modified-starch blends decrease with an increase in the modified starch contents. The ??f values of the PVA/AMS specimens decrease with an increase in the concentrations of hydrochloric acid. Comparing the ??f values of the PVA/CLS specimens with those of the PVA/AMS specimens, the ??f values of the PVA/CLS specimens are better than those of the PVA/AMS specimens. On the contrary, the ??f values of the PVA/AMS specimens are better than those of the PVA/CLS specimens. According to the biodegradability of all the PVA/starch blends, PVA with higher molecular weights displays higher biodegradability. The biodegradability of the PVA/modified-starch blends increase as the modified starch contents of the PVA/modified-starch blends increase. As evidenced by the results of the biodegradability test, the biodegradability of the PVA/modified-starch blends, therein PVA is blended with 1N AMS, shows better biodegradability. The result of bio-reaction kinetics experiment can evaluate the decomposition tendency of the PVA/starch blends up to any biodegradable rate under ambient environment. Using the kinetic model of the first order reaction, it is estimated that 16.20?years and 12.47?years will be needed for the PVABF-17/starch blends, containing 20 and 40% of CLS respectively, to be degraded up to 70% under ambient environment. In addition, it is 1.68?years for the PVABF-26 blends with the 40% 2N AMS under decomposition environment while it is 1.94?years for the 40% 1N AMS. Overall, the decomposition potential of PVA/AMS specimens is better than PVA/CLS specimens. Furthermore, the 1N(26P60AS40)100G20M1 specimen is coincidence the biodegradable material criteria of Environmental Protection Administration (EPA) of Taiwan.  相似文献   

11.
In this study, we have showed a facile route for fabrication of a novel microporous material based on chitosan (CS) and poly(vinyl alcohol) (PVA) biodegradable nanofibers that have high specific surface area, considerable porosity, and small diameter. Scanning electron microscopy, thermogravimetric analysis, differential scanning calorimetry, fourier transform infrared spectroscopy, Brunauer–Emmett–Teller surface area analysis, and CHNS/O elemental analyser were applied to characterize the fabricated CS/PVA composite nanofibers. Moreover, the influences of spinning conditions including concentration, voltage, electrospinning distance, and flow rate, on size distribution and pore diameter of the final product were systematically studied using 2k?1 factorial design experiments, and the response surface optimization was used for determining the best synthesis parameter. The results obtained from 2K?1 factorial design experiments showed that electrospinning parameters influenced the size distribution and pore diameter of the CS/PVA microporous material. Based on the response surface methodology, the CS/PVA product could be obtained with a high microporous diameter of 1.8 nm and a small diameter distribution of 15.0 nm under optimized conditions. The obtained results showed that the fabricated samples could be utilized in different applications.  相似文献   

12.
A novel Fe3O4/cellulose–polyvinyl alcohol (PVA) aerogel was successfully synthesized by an eco-friendly and facile method in this work. Cellulose/PVA matrix was prepared through an environmental friendly physical cross-linking process and further in-situ decorated with Fe3O4. Series of Fe3O4 decorated aerogels were prepared and the effects of Fe3O4 nanoparticles (NPs) on the aerogels were systematic investigated. As-prepared aerogels exhibited desirable properties including nanostructure, relatively high porosity, improved mechanical and superparamagnetism. The TEM results showed that Fe3O4 NPs were integrated in the three-dimensional matrix of cellulose/PVA with a diameter of 9–12 nm. Furthermore, the mechanical strength of the aerogels was significantly enhanced after the introduction of Fe3O4 NPs. Meanwhile, the obtained Fe3O4/cellulose/PVA aerogel exhibited excellent adsorption performance toward methyl blue dye, and can be reused through fenton-like catalysts oxidative degradation of organic dye in H2O2 solution. Therefore, they will have a great potential application as eco-friendly and economical adsorbents.  相似文献   

13.
In this study, polyvinyl alcohol-chitosan-cysteine-functionalized graphene oxide (PCCFG) hydrogel was synthesized from l -cysteine-functionalized graphene oxide (CFG), chitosan (CS), and polyvinyl alcohol (PVA). The hydrogel was characterized by Fourier transform infrared spectroscopy, scanning electron microscopy, and energy-dispersive X-ray spectroscopy and employed for removing lead ion (Pb2+) and cadmium ion (Cd2+) from aqueous solution. The effects of initial metal ion concentration, hydrogel dose, pH, time, and temperature were studied. The experimental data were well described by a pseudo-second-order kinetic model and Langmuir isotherm with maximum adsorption capacities of 250 and 192 mg g−1 at 25°C for Pb2+ and Cd2+, respectively. The adsorption capacity of the PCCFG hydrogel increased with an increase in temperature. The value of ∆G° was negative, which shows the spontaneity of the reaction (electron exchange or ion exchange) between the metal ion and electron-rich atoms (–N, –S, –O). The positive ∆H° shows that the adsorption reaction consumes energy and the positive ∆S° shows the strong affinity of PCCFG toward the Pb2+ and Cd2+ ions. Pb2+ had better affinity and less spontaneity than Cd2+. The results show that the coexistence of Pb2+, Cd2+, and Cu2+ in the solution inhibits the adsorption capacity of PCCFG.  相似文献   

14.
In this study, a synthetic filter material with nutrients (PVA/peat/KNO3 composite bead) was developed for biofilteration. The optimal preparing condition was each of the peat and PVA aqueous solutions mixed with 6.4 g KNO3, and the minimum nitrogen content in the boric and phosphate aqueous solutions was 3.94 and 1.52 g-N/l, respectively. The equilibrium amount of inorganic nitrogen extracted by leaching from the prepared composite bead was between 7.95 and 8.21 mg N/g dry solid. The path of inorganic nitrogen extracted by leaching was the inorganic nitrogen dispersed in the peat phase firstly diffused into the outer PVA phase and then it diffused out of the bead surface for the A-type bead; and that was the inorganic nitrogen dispersed in both the peat and PVA phases simultaneously diffuses into the outer PVA phase and out of the bead surface, respectively, for the H-type bead. The microbial growth rate k g of the H-type composite bead was higher than that of the A-type composite bead about 1.09–1.58 times, and the maximum value of k g was at the H-type composite bead immersed in 0.384 M KNO3 aqueous solution. The percentage of removed VOCs retained at more than 98% during the biofilter operating 230 days as the composite bead immersed in KNO3 aqueous solution before packing. This composite bead bed was without the further addition of nutrients during the operating period.  相似文献   

15.
Chain-extension reactions were carried out using titanium-iso-propoxide (TIP) as a catalyst for a series of polyesters or copolyesterethers with low molecular weights (M n =1500–10,000) synthesized by the ring-opening copolymerization of succinic anhydride (SA) with ethylene oxide (EO). The copolymers having aM n from 25,000 to 50,000 of different properties were obtained. Both the melting point (T m ) and the fusion heat (H), which indicate the crystallinity of the copolymers, rose with an increase in SA content in the copolymers. Semitransparent films were prepared by compression molding of the copolymers. The biodegradation of the copolymer films was evaluated by enzymatic hydrolysis by lipases and by an aerobic gas evolution test in standard activated sludge. The hydrolyzability of these copolymers by three kinds of lipases was affected by their copolymer composition SA/EO, form, andM n . The copolyesterether (SA/EO=43/57,M n =48,900) was more easily biodegraded by standard activated sludge compared to the polyester (SA/EO=47/53,M n =36,300).Presented at the Pacifichem-95, December 17–22, 1995, Honolulu, Hawaii.  相似文献   

16.
This study refers to two chemical leaching systems for the base and precious metals extraction from waste printed circuit boards (WPCBs); sulfuric acid with hydrogen peroxide have been used for the first group of metals, meantime thiourea with the ferric ion in sulfuric acid medium were employed for the second one. The cementation process with zinc, copper and iron metal powders was attempted for solutions purification. The effects of hydrogen peroxide volume in rapport with sulfuric acid concentration and temperature were evaluated for oxidative leaching process. 2 M H2SO4 (98% w/v), 5% H2O2, 25 °C, 1/10 S/L ratio and 200 rpm were founded as optimal conditions for Cu extraction. Thiourea acid leaching process, performed on the solid filtrate obtained after three oxidative leaching steps, was carried out with 20 g/L of CS(NH2)2, 6 g/L of Fe3+, 0.5 M H2SO4, The cross-leaching method was applied by reusing of thiourea liquid suspension and immersing 5 g/L of this reagent for each other experiment material of leaching. This procedure has lead to the doubling and, respectively, tripling, of gold and silver concentrations into solution. These results reveal a very efficient, promising and environmental friendly method for WPCBs processing.  相似文献   

17.
A gram-negative psychrophilic bacterium, with potential for biodegradation of long-chain n-alkanes was isolated from ice samples collected in Spitzbergen, Denmark. On the basis of results of biochemical and morphological tests and sequence analysis of 16S rRNA, the strain was identified as Pseudomonas frederiksbergensis. In this work, a short-chain NAD+-dependent alcohol dehydrogenase (alcDH) (Accession number: AAR13804) from the P. frederiksbergensis was cloned and transformed in E. coli BL21 (3DE) competent cells. The alcDH activity was highest in the crude extract of cells induced with 1.0 mM IPTG. The recombinant alcDH enzyme was purified to 93.4% homogeneity using three consecutive purification steps including ammonium sulphate, Q-Sepharose Fast Flow column and gel filtration chromatography employing Superdex 200 10/30 HR column. Enzyme enrichment and yield levels of 31.4 folds and 25.5%, respectively, were achieved. While the subunit molecular mass of the enzyme was determined on SDS-PAGE to be ~38 kDa, the aggregated native form of the enzyme had a molecular mass of ~238 kDa by gel filtration analysis. Reaction conditions optima for the recombinant alcDH were determined with propan-1-ol as the substrate. While the optimum pH was 9, the optimum temperature was 35 °C. The alcDH enzyme exhibited moderate thermal stability with half-lives of 150 min at 55 °C, 27 min at 65 °C and 8 min at 75 °C. Results for kinetic parameters indicated that the apparent K m value for alcDH with propan-1-ol as the substrate was found to be 1.42 mM and the V max value was 0.63 mmol mg−1 min−1. Experimental evidence revealed that the recombinant alcDH exhibited a wide range of substrate specificity, with higher levels of specific activity for aliphatic alcohols as compared to secondary alcohols. Taken together, the present study highlights the potential of alcDH as a member of cold-adapted enzymes in several key biotechnological applications including environmental bioremediation and biotransformations. It is envisaged that, with the ongoing screening of microorganisms and metagenomes, directed evolution approaches and the subsequent overexpression of recombinant proteins, more enzymes will be found that are suitable for bioremediation purposes.  相似文献   

18.
The high surface area of porous nanofibers enhances their performance for many applications. The present study investigated electrospinning and dye adsorption properties of polymeric nanofibers which were porous by various types of salts. The salt/polyacrylonitrile/polyvinylidene fluoride composite nanofibers were electrospun, and the inexpensive salts such as sodium chloride (NaCl), sodium bicarbonate (NaHCO3), or calcium chloride (CaCl2) was used to manufacture the porous fibers. Subsequently, the salt was removed by a selective dissolution, and salt extraction of nanofibers was performed with the solution of hydrochloric acid (10 wt%). Salt/PVDF/PAN and porous PVDF/PAN composite nanofibers have been applied to dye adsorption of solution. The characteristics of nanofibers were studied by Fourier transform infrared microscopy (FTIR) and scanning electron microscopy (SEM) analysis. FTIR showed that the salt was extracted from PVDF/PAN nanofibers successfully, and SEM indicated that many pores were aligned with the nanofibers. The adsorption capacity of salt nanofibers webs and porous nanofibers webs for Basic Blue 41 were compared with each other, and porous fibers were obtained from NaHCO3 having the highest dye adsorption value. Adsorption of dyes follows the Langmuir isotherm and pseudo-second order kinetics.  相似文献   

19.
This study presents a photochemical kinetics model to describe the degradation of water-soluble PVA (Polyvinyl Alcohol) polymer in a UV/H2O2 batch reactor. Under the effect of UV light, the photolysis of hydrogen peroxide into hydroxyl radicals can generate a series of polymer scission reactions. For a better understanding and analysis of the UV/H2O2 process in the cracking of the PVA macromolecules, a chemical reaction mechanism of the degradation process and a relevant photochemical kinetics model are developed to describe the disintegration of the polymer chains. Taking into account the probabilistic fragmentation of the polymer, the statistical moment approach is used to model the molar population balance of live and dead polymer chains. The model predicts the PVA molecular weight reduction, the acidity of the solution, and hydrogen peroxide residual. In addition to previously published data collected in this laboratory, a new set of experiments were conducted using a 500 mg/L PVA aqueous for different hydrogen peroxide/PVA ratios for model validation. Measurements of average molecular weights of the polymer, hydrogen peroxide concentrations and pH of the PVA solution were determinant factors in constructing a reliable photochemical model of the UV/H2O2 process. Experimental data showed a decrease in the PVA molecular weight and a buildup of the solution acidity. The experimental data also served to determine the kinetics rate constants of the PVA photochemical degradation and validate the model whose predictions are in good agreement with data. The model can provide a comprehensive understanding of the impact of the design and operational variables.  相似文献   

20.
To solve the recycling challenge for aqueous binder based lithium-ion batteries (LIBs), a novel process for recycling and resynthesizing LiNi1/3Co1/3Mn1/3O2 from the cathode scraps generated during manufacturing process is proposed in this study. Trifluoroacetic acid (TFA) is employed to separate the cathode material from the aluminum foil. The effects of TFA concentration, liquid/solid (L/S) ratio, reaction temperature and time on the separation efficiencies of the cathode material and aluminum foil are investigated systematically. The cathode material can be separated completely under the optimal experimental condition of 15 vol.% TFA solution, L/S ratio of 8.0 mL g?1, reacting at 40 °C for 180 min along with appropriate agitation. LiNi1/3Co1/3Mn1/3O2 is successfully resynthesized from the separated cathode material by solid state reaction method. Several kinds of characterizations are performed to verify the typical properties of the resynthesized LiNi1/3Co1/3Mn1/3O2 powder. Electrochemical tests show that the initial charge and discharge capacities of the resynthesized LiNi1/3Co1/3Mn1/3O2 are 201 mAh g?1 and 155.4 mAh g?1 (2.8–4.5 V, 0.1 C), respectively. The discharge capacity remains at 129 mAh g?1 even after 30 cycles with a capacity retention ratio of 83.01%.  相似文献   

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