石墨相氮化碳的制備及光催化性能調(diào)控
[Abstract]:At present, with the continuous deepening of the process of industrialization, human beings are faced with the great challenge of the rapid deterioration of the earth's environment and the global energy shortage, especially the numerous pollutants in the water. Most of them are organic, toxic and very stable, thus showing the characteristics that are difficult to degrade. Photocatalytic technology has been applied in recent years. The effect of the environmental treatment and sewage treatment is remarkable. The traditional semiconductor titanium dioxide (TiO2) has poor response to visible light and can not be widely used in real life. The new type of photocatalyst graphite phase carbon nitride (g-C_3N_4) has been paid great attention to the advantages of non-toxic, non-toxic and easy to regulate the band gap structure. As a result of small specific surface area, low photocatalytic efficiency and high carrier recombination rate, g-C_3N_4 restricts its wide application. Accordingly, this paper uses composite semiconductors, loaded precious metals, increases specific surface area and doping non-metallic elements to improve the visible photocatalytic performance of graphite phase carbon nitride photocatalyst. As follows: 1. the Bi_2S_3/g-C_3N_4 composite photocatalyst with adjustable Bi_2S_3 content was prepared by in situ formation. Through X- ray diffraction (XRD), Fourier infrared spectroscopy (FT-IR), scanning electron microscope (SEM), transmission electron microscope (TEM), UV visible diffuse reflectance spectroscopy (DRS), photoluminescence (PL), and time resolved fluorescence decay spectra, etc. Analysis was made on the phase, morphology, structure and properties of the prepared photocatalyst. Under visible light, the photocatalytic performance of Bi_2S_3/g-C_3N_4 composite photocatalyst was evaluated with organic dye (Luo Danming B) as degradation model. The results showed that the short rod like Bi_2S_3 was deposited on the surface of g-C_3N_4, and the g-C_3N_4 was significantly enhanced. The photocatalytic performance of the photocatalyst is visible, and with the difference of the Bi_2S_3 content of the narrow band gap semiconductor, the photocatalytic performance of the composite photocatalyst Bi_2S_3/g-C_3N_4 changes. The best visible photocatalytic activity is shown when the Bi_2S_3 content is 5 wt%. Using the capture agent, the NBT conversion, the phenylene two formic acid fluorescence spectroscopy, and the determination of the h+ in the photocatalytic process The main active species in the reaction system, O-2 is a secondary active species in the reaction system. In addition, the mechanism of the enhanced photocatalytic activity of the composite photocatalyst was studied. The addition of Bi_2S_3 significantly enhanced the absorption of visible light by g-C_3N_4, and formed a heterojunction with g-C_3N_4 to promote semiconductor light generation. The effective separation of the sub and hole, prolonging the lifetime of the carrier, and significantly enhancing the photocatalytic performance of g-C_3N_4.2. by three step method to synthesize the g-C_3N_4/PPy/Ag three element composite photocatalyst. First, the calcined melamine was calcined at high temperature to get the graphite phase carbon nitride photocatalyst, and then a series of g-C_3N_4/PPy composite light was obtained by in situ polymerization of pyrrole. At last, Ag was deposited on the surface of g-C_3N_4/PPy to obtain the g-C_3N_4/PPy/Ag composite photocatalyst. The photocatalytic activity of the sample was evaluated by degradation of tetracycline (TC) under visible light. The effect of the load of polypyrrole and Ag on the photocatalytic activity of g-C_3N_4/PPy/Ag was investigated. The optical properties and electronic structures of the samples were obtained by analyzing the photocatalytic activity of the samples. Polypyrrole and silver have synergistic effect on improving the photocatalytic activity of g-C_3N_4/PPy/Ag. Therefore, compared with g-C_3N_4, g-C_3N_4/PPy, g-C_3N_4/Ag degradation of tetracycline, g-C_3N_4/PPy/Ag three element composite photocatalyst has higher photocatalytic activity. In addition, the high effective photocatalytic mechanism of g-C_3N_4/PPy/Ag photocatalyst was analyzed. The matching of pyrrole and g-C_3N_4 energy band accelerates the separation of light generated carriers. The loaded silver has played an important role in the SPR effect as the electron acceptor..3. is coated on the template by mixing the liquid phase with the polyphenol formaldehyde resin. The two times calcined in nitrogen and oxygen, the polymer mold is carried out respectively. The porous structure of g-C_3N_4 (CN) was finally prepared. The structure, morphology and optical properties of the prepared products were analyzed by a series of characterization tests. The results showed that the prepared g-C_3N_4 showed a porous structure, significantly enhanced the visible light and ground absorption, and reduced the recombination rate of the optical carrier significantly. Under visible light, The photocatalytic performance of the synthetic samples was evaluated with RhB as the degradation object. The results showed that the porous g-C_3N_4 obtained after O2 calcined was superior to the calcined samples directly under the N2 atmosphere, and when the input amount of the template was 0.021 g, the photocatalytic performance of the porous carbon (CN-0.021) was the best, which was pure g-C_3N_4 and C/, respectively. 7.8 and 2.2 times of CN-0.021. In addition, the reasons for the enhancement of the photocatalytic performance of porous g-C_3N_4 have been analyzed. It has a larger specific surface area (150.5 m2/g) and internal pore structure, which is the main factor to improve the photocatalytic performance of.4.. On the basis of the synthesis of porous carbon nitride, the phospho diammonium phosphate ((NH4) 2HPO4) is used as the phosphorus source to synchronize the phosphorus. A series of phosphorus doped porous carbon nitride (PCN) photocatalytic materials were prepared by fixing the amount of melamine and template polyphenolic resin balls fixed with melamine and template and changing the amount of (NH4) 2HPO4. The photocatalytic activity of the prepared samples was evaluated by using RhB as degradation model. PCN-0.3 was measured with nitrogen adsorption desorption isotherm. The specific surface area (131.2 m2/g) is less than CN-0.021 (150.5 m2/g), but its photocatalytic activity is not reduced, but the optimum doping amount of phosphorus is discussed. When the input of (NH4) 2HPO4 is 0.3 g, the preparation of phosphorus doped porous carbon nitride (PCN-0.3) is the best catalyst, which is pure g-C_3N_4, phosphorus doped carbon nitride (P-C_3N_4) and porous nitrogen, respectively. By comparing the optical properties of pure g-C_3N_4, P-C_3N_4, CN-0.021 and PCN-0.3 photocatalysts, the reasons for the enhancement of photocatalytic activity of phosphorus doped porous carbon nitride were analyzed by comparing the optical properties of the pure g-C_3N_4, P-C_3N_4, CN-0.021 and PCN-0.3 photocatalysts. The main attributable to the larger surface area provided more reaction sites and the combination of phosphorus doping to reduce the band gap width. The result.
【學(xué)位授予單位】:江南大學(xué)
【學(xué)位級(jí)別】:碩士
【學(xué)位授予年份】:2017
【分類號(hào)】:O643.36;O644.1
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