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The Studies On Structural Regulation And Several Properties Of Carbon Nanomaterials Based On Fullerene,Graphene And Quasi Buckyonion

Posted on:2018-01-05Degree:DoctorType:Dissertation
Country:ChinaCandidate:M S LinFull Text:PDF
GTID:1361330518484566Subject:Inorganic Chemistry
Abstract/Summary:PDF Full Text Request
Carbon nanomaterials are defined as carbon materials which are measured less than 100 nm in at least one dimension,including zero-dimensional fullerenes,one-dimensional carbon nanotubes and carbon fibers,two-dimensional graphenes and others such as bucky onions and nanodiamonds.They usually exhibit distinct electrical,mechanical,thermal and optical properties.Therefore,carbon nanomaterials have shown promising applicable in many scientific and technological areas,such as solar cells,lithium-ion battery,field effect transistors,supercapacitor,catalysis,sensors,biomedicine and composite materials.The dissertation deals with the design and synthesis of the three kinds of carbon nanomaterials,as well as the formation and properties of as-prepared carbon nanomaterials.The main contents are as follows:(1)By nucleophilic substitution reaction,a series of amphiphilic fullerene-based amino acid ester chlorides were synthesized,which could self-assemble as spherical vesicles for drug delayed release.The synthesis condition is relatively moderate rather than extreme conditions such as high temperature,high pressure,oxygen-free or vacuum.Besides,the condition required for self-assembly is also environment friendly.The fullerenes derivatives could easily self-assemble towards drug-containing vesicles in polar solvent by intermolecular forces and ?-? stacking.The size and polarity,as well as the drug loading amount and drug loading(releasing)rates,are dependent on the substituent of amino acid ester.Significantly,the drug loading and average diameter of vesicles were positive correlated,so were the drug releasing rate and polarity of fullerenes.(2)A fullerene photocatalysis evaluation system was established.The current of xenon light was set at 10 A for full spectrum conditions.The temperature was set at 25?,the catalyst concentration was 0.3 mg/mL and the reaction time was 1 h.Through the photocatalytic oxidation of naphthol to naphthoquinone,the catalytic properties of four types of fullerenes were compared,and the mechanism of photocatalytic oxidation process was explored.Notably,the reaction can be carried out at room temperature and under ambient condition.The catalysis results reveal that the activities of fullerenes toward the photocatalytic oxidation are concerned with their LUMO level.C70,for example,has showed the most excellent catalytic activity.The conversion rate of naphthol was 88 ± 2.1%,and the yield of naphthoquinone was 52 ±5.3%.As PCE of organic solar cells conforms the similar order of catalytic activity,this paper proposes an easy and contactless method which does not need device fabrication to qualitative analysis the PCE of organic solar cells.Both organic solar cells and photo oxidation are similarity subjected to the energy level and the density of excitation state.Therefore,the conversion in photo oxidation and the PCE of organic solar cells show a strong linear relationship,on the other hand,it also shows a linear dependence with the product of Jsc and VOC.(3)It was designed and reconstructed the original chemical vapor deposition micro-zone heater instruments.Using single-factor experiment method and orthogonal experiment method,the experimental conditions were optimized and single-layer graphene was successfully prepared with a few defects.Besides,in the synthesis process,the number of layers and defects in as-prepared graphene were under the influence of argon,hydrogen and methane flow rate,as well as the growth time.Thus,different layers and defects of graphene could be obtained by varying the reaction conditions.(4)Nitrogen-doped quasi buckyonions were successfully synthetized from fullerene via radical reaction,which could serve as a substrate material to enhance the activity of loading catalyst that hydrogenate dimethyl oxalate into ethylene glycol.The synthesis reaction was preceded in room temperature and could be mass-produced.The results exhibited that the synthesis path should be classified to radical reaction.Its growth process was accorded with the general debris-fusion-reconstruction of quasi buckyonions.According to the experimental data,the conversion rate could be increased from 14.7%up to 33.7%,and the selectivity rised up to 7.2%as compared to the original 2.49%at a space velocity of 8.4 g g-cat-1 h-1.Furthermore,in the catalysis part,the conversion and selectivity of nitrogen-doped quasi buckyonions supported silicon copper catalyst were improved at a high space velocity.
Keywords/Search Tags:Carbon nanomaterials, Fullerene, Graphene, Buckyonions, Structural regulation, Properties
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