Diamond coating using hot-filament chemical vapor deposition (HFCVD) is now widely used in many fields. The quality of the diamond film and many factors determine the success of the coating, such as temperature, time, and pressure during coating. The purpose of this study was to produce coated boron-doped diamond (BDD) films by doping boron in the diamond film and to assess them through comparative analysis with foreign acid BDD, which is widely used as a water-treatment electrode in the present industry. The bending of the titanium substrate due to the high temperature during the diamond deposition was avoided by adding an intermediate layer with a columnar structure to niobium film. The filament temperature and pressure were determined through preliminary experiments, and BDD films were coated. The BDD film deposition rate was confirmed to be 100 nm/h, and the potential window increased with increasing thickness. The electrochemical activation and catalytic performance were confirmed according to the surface characteristics. Although the high deposition rate of the BDD coating is also an important factor, it was confirmed that conducting coating so that amorphous carbonization does not occur by controlling the temperature during coating can improve the electrochemical properties of BDD film.
To optimize the deposition parameters of diamond films, the temperature, pressure, and distance between the filament and the susceptor need to be considered. However, it is difficult to precisely measure and predict the filament and susceptor temperature in relation to the applied power in a hot filament chemical vapor deposition (HF-CVD) system. In this study, the temperature distribution inside the system was numerically calculated for the applied powers of 12, 14, 16, and 18 kW. The applied power needed to achieve the appropriate temperature at a constant pressure and other conditions was deduced, and applied to actual experimental depositions. The numerical simulation was conducted using the commercial computational fluent dynamics software ANSYS-FLUENT. To account for radiative heat-transfer in the HF-CVD reactor, the discrete ordinate (DO) model was used. The temperatures of the filament surface and the susceptor at different power levels were predicted to be 2512–2802 K and 1076–1198 K, respectively. Based on the numerical calculations, experiments were performed. The simulated temperatures for the filament surface were in good agreement with the experimental temperatures measured using a two-color pyrometer. The results showed that the highest deposition rate and the lowest deposition of non-diamond was obtained at a power of 16 kW.
In this study, acetone was used as a carbon source to deposit diamond films using tantalum filaments by hot filament chemical vapor deposition (HFCVD). For acetone fluxes of 80, 90, 130 and 170 standard cubic centimeters per min (sccm) and the respective hydrogen fluxes of 420, 410, 370, and 330 sccm, film thickness appeared to increase with increasing acetone, and high quality diamonds were deposited with well-defined facets of (111) and (100). For acetone fluxes of 210 and 250 sccm and the respective hydrogen fluxes of 290 and 250 sccm, however, the diamond quality was degraded with cauliflower-shaped structures evolving and the film thickness decreased with increasing acetone. The degradation of diamond quality was confirmed by Raman spectra and X-ray diffraction (XRD). Many diamond crystals grown at acetone fluxes of 80, 90, 130 and 170 sccm consisted of five (111) facets, indicating an icosahedral structure. At the corner where the five (111) facets met, there were pentagonal dimples, which implied that diamond crystals must have been etched. The decrease in film thickness at high acetone fluxes of 210 and 250 sccm also implied that the deposited film must have been etched. These results indicate that the two irreversible processes of deposition and etching occur simultaneously, which would violate the second law of thermodynamics from the classical concept of crystal growth by an individual atom. These puzzling results could be successfully explained by non-classical crystallization, where the building blocks for diamond films are nanoparticles formed in the gas phase.
In this study, boron-doped diamond (BDD) film was deposited by hot-filament chemical vapor deposition (HFCVD) using acetone as the carbon source and trimethyl borate (TMB) as the boron source with the aim of lowering the manufacturing cost of BDD electrodes. The BDD film was deposited for 12 and 60 h to observe changes in the morphological behavior of the film as well as subsequent changes in the electrochemical properties. The morphology of the BDD film was not affected by the deposition time, but the thickness increased with increasing deposition time. As the deposition time increased, the deposition rate of the BDD film did not increase or decrease; rather, it remained constant at 100 nm/h. As the thickness of the BDD film increased, an increase in the potential window was observed. On the other hand, no distinct change was observed in the electrochemical activation and catalytic activity depending on the thickness, and there were not many differences. Chemical oxygen demand (COD) was measured to determine the practical applicability of the deposited BDD film. Unlike the potential window, the COD removal rate was almost the same and was not affected by the increase in the thickness of the BDD film. Both films under the two deposition conditions showed a high removal rate of 90% on average. This study confirms that BDD electrodes are much more useful for water treatment than the existing electrodes.