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This dissertation describes fundamental studies of hollow carbon nanostructures, which may be used as electrodes for practical energy storage applications such as batteries or supercapacitors. Electron microscopy is heavily utilized for the nanoscale characterization. To control the morphology of hollow carbon nanostructures, ZnO nanowires serve as sacrificial templates. The first

This dissertation describes fundamental studies of hollow carbon nanostructures, which may be used as electrodes for practical energy storage applications such as batteries or supercapacitors. Electron microscopy is heavily utilized for the nanoscale characterization. To control the morphology of hollow carbon nanostructures, ZnO nanowires serve as sacrificial templates. The first part of this dissertation focuses on the optimization of synthesis parameters and the scale-up production of ZnO nanowires by vapor transport method. Uniform ZnO nanowires with 40 nm width can be produced by using 1100 °C reaction temperature and 20 sccm oxygen flow rate, which are the two most important parameters.

The use of ethanol as carbon source with or without water steam provides uniform carbonaceous deposition on ZnO nanowire templates. The amount of as-deposited carbonaceous material can be controlled by reaction temperature and reaction time. Due to the catalytic property of ZnO surface, the thicknesses of carbonaceous layers are typically in nanometers. Different methods to remove the ZnO templates are explored, of which hydrogen reduction at temperatures higher than 700 °C is most efficient. The ZnO templates can also be removed under ethanol environment, but the temperatures need to be higher than 850 °C for practical use.

Characterizations of hollow carbon nanofibers show that the hollow carbon nanostructures have a high specific surface area (>1100 m2/g) with the presence of mesopores (~3.5 nm). The initial data on energy storage as electrodes of electrochemical double layer capacitors show that high specific capacitance (> 220 F/g) can be obtained, which is related to the high surface area and unique porous hollow structure with a thin wall.
ContributorsSong, Yian (Author) / Liu, Jingyue (Committee member) / Smith, David (Committee member) / McCartney, Martha (Committee member) / Chen, Tingyong (Committee member) / Arizona State University (Publisher)
Created2016
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Description
This dissertation describes the synthesis and study of porous nanocarbon and further treatment by introducing nitrogen and oxygen groups on nanocarbon, which can be used as electrodes for energy storage (supercapacitor). Electron microscopy is used to make nanoscale characterization. ZnO nanowires are used as the template of the porous nanocarbon,

This dissertation describes the synthesis and study of porous nanocarbon and further treatment by introducing nitrogen and oxygen groups on nanocarbon, which can be used as electrodes for energy storage (supercapacitor). Electron microscopy is used to make nanoscale characterization. ZnO nanowires are used as the template of the porous nanocarbon, and nitrogen doping and oxidation treatment can help further increase the capacitive performance of the nanocarbon.

The first part of this thesis focuses on the synthesis of ZnO nanowires. Uniform ZnO nanowires with ~30 nm in width are produced at 1100℃ in a tube furnace with flowing gases (N2: 500 sccm; O2: 15 sccm). The temperature control is one of the most important parameters for making thin and ultra-long ZnO nanowires.

The second part of the thesis is about the synthesis of nanocarbons. Ultrapure ethanol is used as the carbon source to make carbonaceous deposition on ZnO nanowires. The thickness of the nanocarbons can be controlled by reaction temperature and reaction time. When the reaction time was controlled around 1h, the carbonaceous materials coating the ZnO nanowires become very thin. Then by flowing (1000 sccm) hydrogen at 750℃ through the reaction tube the ZnO nanowires are removed due to reduction and evaporation. Electrochemical evaluation of the produced nanocarbons shows that the nanocarbons possess very high specific surface area (>1400 m2/g) and a capacitance as high as 180 F/g at 10A/g in 6M KOH).

The third part of the thesis is the treatment of the as-synthesized nanocarbons to further increase capacitance. NH3 was used as the nitrogen source to react with nanocarbons at 700℃ to incorporate nitrogen group. Nitric acid (HNO3) is used as the oxidant to introduce oxygen groups. After proper nitrogen doping, the nitrogen doped nanocarbons can show high specific capacitance of 260 F/g at 1A/g in 6M KOH. After further oxidation treatment, the capacitance of the oxidized N-doped nanocarbons increased to 320 F/g at 1A/g in 6M KOH.
ContributorsZhang, Yizhi (Author) / Liu, Jingyue (Thesis advisor) / Wang, Qinghua (Committee member) / Deng, Shuguang (Committee member) / Arizona State University (Publisher)
Created2020