TiO2 형태와 도핑방법에 따른 나노물질 초음파 합성 및 환경적 응용 : Study on doping and morphology = Ultrasonic-assisted synthesis and environmental applications of TiO2 based nano-materials
The discovery of photo-electrochemical water splitting using TiO2 electrode by Fujishima and Honda made the way for utilization of TiO2 as a heterogeneous semiconductor photocatalysts for degradation of wide variety of toxic pollutants present in the water and air environment. TiO2 is an inexpensive, abundant and eco-friendly photocatalysts, no photo and chemical corrosion during the reaction and chemically and biologically stable photocatalysts. However the visible-light photocatalytic efficiency of TiO2 was very poor due to its wider band gap and the higher photogenerated electron-hole recombination. Therefore in this present thesis, visible light photocatalytic efficiency of TiO2 was improved by incorporating metals, metal oxides and metal sulfide, respectively and studied their photocatalytic oxidation efficiency towards air pollutants. Zero- (nanoparticle), one- (nanotube, TNT), two-(nanosheet, TNS), and three- (nanoflower, TNF) dimension of TiO2 photocatalytic nanomaterial were synthesized using ultrasonification method. Metals (Ag, Ce, Co, Fe, Mg, and Mn) and metal oxides (Cu2O and WO3) and metal sulphide (CdS) were embedded on different dimensions of TiO2 to improve the visible light photocatalytic efficiency. Furthermore the ultrasonic operational parameters were varied to study their influence on the photocatalytic oxidation efficiency. Subsequently the textural and electronic properties of synthesized photocatalysts were investigated by physicochemical techniques such as XRD, FE-SEM/EDX, TEM, BET, UV-vis and photoluminescence spectroscopy (PL). After successful characterization, the photocatalytic activity of the synthesized photocatalytic nanomaterials (metals-TiO2, metal oxides-TiO2 and metal sulphide-TiO2) were investigated for photocatalytic oxidation efficiency of VOCs and it was compared with that of undoped photocatalyst. First, the highest visible-light photocatalytic degradation efficiency for BTEX was obtained from the WO3-TiO2 among the metals- and metal-oxides-TiO2. Among the WO3-TiO2 photocatalysts according to WO3 contents loaded on TiO2, 1 wt% WO3 loaded TiO2 showed higher photocatalytic degradation for BTEX. Second, in the case of one-dimension single doping photocatalyst, the highest visible-light photocatalytic degradation efficiency for BTEX was obtained from the 10 wt% WO3-TNT among the WO3-to-TiO2 ratio. Third, in the case of two-dimension single doping photocatalyst, the highest visible-light photocatalytic degradation efficiency for BTEX was obtained from the 4 wt% WO3-TNS among the WO3-to-TNS ratio. Fourth, in the case of three-dimension single doping photocatalyst, the highest visible-light photocatalytic degradation efficiency for BTEX was obtained from the 1 wt% WO3-TNF among WO3-to-TNF ratio. Fifth, in the case of one-dimension co-doping photocatalyst, the highest visible-light photocatalytic degradation efficiency for toluene and α-pinene was obtained from the 1 wt% N,Fe-TNT among the Fe-to-TNT ratio. Sixth, in the case of two-dimension co-doping photocatalyst, the highest visible light-activated photocatalytic degradation efficiency for toluene and n-hexane was obtained from the 4 wt% N,WO3-TNS among WO3-to-TNS ratio. Seventh, in the case of three-dimension semiconductor-semiconductor doping photocatalyst, the highest visible-light photocatalytic degradation efficiency for toluene and d-limonene was obtained from the 0.3 wt% CdS-TNF among the CdS-to-TNF ratio. Consequently, the enhanced photocatalytic activity of synthesized nanomaterials is attributed to the increased surface acidity, adsorption ability, and charge separation due to the single or double doping of each dopants and TiO2 (each dimensions) within the synthesized photocatalytic nanomaterials. Additionaly, The generation of byproducts during photocatalytic oxidation of target compounds (toluene, n-hexane, α-pinene, and d-limonene) is a problem for the environmental application of photocatalytic oxidation in indoor environment. In this study, the by products at ppb levels were studied during photocatalytic oxidation degradaton of each target compounds in a pyrex-reactor and identified using GC-MS. The results indicated that a various byproduct were detected in gas phase by GC-MS. It conclues that although some byproducts are formed during photocatalytic oxidation degradation of target compounds, it seems that these byproducts do not have adverse effects (such as carcinogenic) to human health. Because those byproducts at ppb level was detected during photocatalytic oxidation.
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