Part II. Effect of Surface Properties on Sensitivity of Gas Sensor Using Carbon Nanotube and Graphene
Chapter 6. Estimation of Residual Life of Gas Filtration System
7. Conclusion
Carbon nanotubes and graphene are hexagonal structures of carbon atoms with a one-atom level thickness. The graphene has contact of a conduction band and a valence band at the Dirac point and has a semi-metallic characteristic due to the linear dispersion relation. On the other hand, CNTs have the characteristic of semiconductors or metallics following the (n, m) chirality. With these properties, research into the physical, electrical and mechanical optical properties of graphene and nanotubes have been extensively reported. In particular, it is very important to understand the surface properties of nanotubes and graphene because the optical and electrical properties of the nanotubes and graphene vary greatly depending on the adsorption of molecules or functionalization.
The first part of the thesis in chapter 3 focused on the effect of hydrocarbon and amorphous carbon on Raman signal. Previous researchers have long accepted false conclusions because they failed to recognize that amorphous carbon was deposited on nanotubes and graphene. Hence, there has been a debate as to whether the carbon nanotubes and graphene are damaged by low-energy electron beams due to insufficient results. Many scientists have since accepted that graphene and nanotubes are damaged by low-voltage electron beams without further seeking verification. To understand the effect of low-energy electron beams on carbon nanotubes and graphene, I investigated the effects of carbon nanotube defects, hydrocarbons and amorphous carbon on Raman spectra. The e- beam induced D-mode disappeared after PMMA film coating without any heat treatment, meaning that the e-beam induced D-mode did not indicate a defect of CNTs because it was difficult that carbon-carbon covalent bonding was formed at room temperature. I investigated the hydrocarbon effect, which was inevitably deposited on a sample surface during exposure of the electron beam. The hydrocarbon was a substance consisting only of C and H atoms and increased the background of Raman spectroscopy by 1000 cm-1 to 3000 cm-1. However, the hydrocarbon was not the main cause of e-beam-induced D-mode. Finally, I investigated the effect of amorphous carbon deposited on nanotube surfaces during nanotube synthesis. The amorphous carbon showed an increase in D-mode on Raman spectroscopy when it received low-energy electron beam. After removing the amorphous carbon, the low-energy electron beam was re-irradiated at exactly the same spot, but the intensity of D-mode sharply decreased. This phenomenon has been applied to graphene. Hence, I conclude that low-energy electron beam does not damage carbon nanotubes and graphene.
In the second part in chapter 4, I studied a gas sensor using CNTs. Surface functionalization changes the electrical properties of nanotubes and makes them sensitive to specific gases. The surface functionalization was achieved with an environmentally-friendly plasma treatment using a porous filter electrode with circulation process for uniformity. The plasma-functionalized CNTs showed improved sensitivity to DMMP gas compared to pristine CNTs. While there is a way to intentionally modify surface properties of nanotube through functionalization, surface properties are
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unintentionally changed during the graphene synthesis process. In chapter 5, two factors of graphene synthesis condition were controlled to investigate how the surface properties affect sensor to sensor variation: i) the flowing of CH4 as a carbon precursor during fast cooling, and ii) how to remove the PMMA film using acetone or annealing process. If the carbon precursor is not released during the cooling process, there would be relatively many PMMA residues on the graphene surface. When PMMA was removed by annealing, the 2D/G ratio of the Raman signal was affected by the oxygen doping in the graphene lattice. When graphene was synthesized without releasing carbon precursor and the PMMA film was removed with annealing, the graphene-based sensor showed relatively uniform sensitivity. In addition, the sensitivity of the graphene sensor was improved by heat treatment at 300 °C in air atmosphere. It was investigated on the sensor properties according to the edge ratio of graphene. The ΔR/R0 was similar regardless of different edge ratio. However, as the edge ratio increased, the intensity of the noise increased.
Finally, a CNT-based gas sensor was used to evaluate the residual life of the filtration system.
Four sensors were inserted vertically in the activated carbon and the response of the inserted sensor was checked by exposing DMMP. Using the response curve of inserted CNTs-based sensor, the residual life of activated carbon was evaluated without deterioration of filtration performance.
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