類石墨相氮化碳基復(fù)合納米光催化體系構(gòu)筑及可見光降解染料性能研究
本文選題:染料 + 水熱法 ; 參考:《江蘇大學(xué)》2017年碩士論文
【摘要】:隨著經(jīng)濟與社會的發(fā)展,水資源污染越來越嚴重,染料的大量使用更是加劇了水資源的短缺。染料廢水不僅對水資源造成嚴重破壞,對人體健康也構(gòu)成一定的威脅。出于民生和發(fā)展角度來說,必須對染料廢水進行嚴格的處理。除了避免染料廢水的亂排放,還要利用有效的科學(xué)技術(shù)來解決當(dāng)前已造成的染料污染。本文對目前國內(nèi)外染料廢水處理技術(shù)進行簡單分析與歸納總結(jié),提出了最近在環(huán)境與能源領(lǐng)域比較熱點的光催化方法。光催化方法有高效、綠色環(huán)保、操作簡單等優(yōu)點,對未來解決有機物污染有著廣闊的前景。具有適當(dāng)?shù)膸丁?yōu)異的穩(wěn)定性和成本低等特點的非金屬聚合物半導(dǎo)體氮化碳(g-C_3N_4)已經(jīng)引起了科學(xué)家們廣泛關(guān)注。然而,較低的量子效率極大地限制了g-C_3N_4的實際應(yīng)用?梢詫-C_3N_4與合適的光催化劑復(fù)合構(gòu)建異質(zhì)結(jié)。異質(zhì)結(jié)的形成有利于光生電荷的轉(zhuǎn)移與分離,抑制光生電子和空穴的復(fù)合從而提高其量子效率。本論文采用水熱法制備了g-C_3N_4/CdWO_4、MnWO_4/g-C_3N_4、g-C_3N_4/O-doped ZnIn_2S_4三種異質(zhì)結(jié)并通過降解染料來評價其光催化效果。取得的成果主要有以下三個方面:(1)利用水熱法制備了g-C_3N_4/CdWO_4納米復(fù)合材料,通過一系列表征證明了棒狀CdWO_4均勻地負載在層狀g-C_3N_4表面。異質(zhì)結(jié)的形成有利于g-C_3N_4表面光生電子和空穴的分離,讓更多的活性物種參與有機物的氧化還原反應(yīng),從而提高其光催化活性。當(dāng)異質(zhì)結(jié)中CdWO_4的含量為20%時,復(fù)合材料表現(xiàn)出最好的降解效果,在180 min可見光下對羅丹明B的降解率為94%,表現(xiàn)出了很好的脫色效果。經(jīng)過四次循環(huán)后,異質(zhì)結(jié)對羅丹明B的降解沒有明顯地降低依,證明了異質(zhì)結(jié)良好的穩(wěn)定性。通過捕獲實驗和ESR表征實驗我們提出了g-C_3N_4/CdWO_4的降解機理。(2)通過水熱法合成了MnWO_4/g-C_3N_4納米復(fù)合材料,通過一系列表征證明了花狀MnWO_4均勻地負載在層狀g-C_3N_4表面。當(dāng)MnWO_4的負載量為10%時,復(fù)合光催化劑的活性最高,分別是純g-C_3N_4和MnWO_4降解率的2.3倍和12.7倍?梢姽庀,10%MnWO_4/g-C_3N_4異質(zhì)結(jié)在4 h可見光下內(nèi)對羅丹明B的降解率為73%,表現(xiàn)出了很好的脫色效果,經(jīng)過四次循環(huán)實驗,異質(zhì)結(jié)的光催化活性沒有明顯地降低,表現(xiàn)出了催化劑良好的穩(wěn)定性,有利于工業(yè)應(yīng)用。通過捕獲實驗和ESR表征實驗我們提出了MnWO_4/g-C_3N_4的降解機理。(3)通過水熱法制備了g-C_3N_4/O-doped ZnIn_2S_4納米復(fù)合材料,通過XPS證明了Zn In_2S_4中晶格氧的存在。HRTEM驗證了片狀氧摻雜的Zn In_2S_4成功地負載在層狀g-C_3N_4的表面。當(dāng)g-C_3N_4的負載量為20%時,復(fù)合材料對羅丹明B表現(xiàn)出了最好的降解率。在20 min可見光下,20%g-C_3N_4/O-doped Zn In_2S_4對羅丹明B的降解率為97%,表現(xiàn)了很出色的降解效果,且在四次循環(huán)后降解效果沒有明顯地降低,體現(xiàn)了光催化劑良好的穩(wěn)定性。
[Abstract]:With the development of economy and society, water pollution is becoming more and more serious. Dye wastewater is not only a serious damage to water resources, but also a threat to human health. From the point of view of people's livelihood and development, dye wastewater must be treated strictly. Besides avoiding the random discharge of dyestuff wastewater, effective science and technology should be used to solve the dyestuff pollution. In this paper, the dyeing wastewater treatment technology at home and abroad is simply analyzed and summarized, and the photocatalytic method which is a hot spot in the field of environment and energy is put forward in this paper. Photocatalytic method has the advantages of high efficiency, green environmental protection, simple operation and so on. It has broad prospects for solving organic pollution in the future. Non-metallic polymer semiconductors with suitable band gap, excellent stability and low cost have attracted much attention. However, low quantum efficiency greatly limits the practical application of g-C_3N_4. The heterojunction can be constructed by combining g-C_3N_4 with the appropriate photocatalyst. The formation of heterojunction is conducive to the transfer and separation of photogenerated charges and the inhibition of the combination of photogenerated electrons and holes to improve their quantum efficiency. In this paper, we have prepared g-C _ S _ 3N _ 3N _ 3N _ 3N _ 2O _ 4 / C _ 3N _ 3C _ 3N _ 3C _ 3N _ 3N _ 3C _ 3N _ 3N _ 3 heterojunction by hydrothermal method and evaluated its photocatalytic effect by the degradation of dyes. The main achievements are as follows: 1) g-C_3N_4/CdWO_4 nanocomposites were prepared by hydrothermal method. A series of characterization proved that rod-shaped CdWO_4 was uniformly loaded on the surface of layered g-C_3N_4. The formation of heterojunction is conducive to the separation of photogenerated electrons and holes on the surface of g-C_3N_4, and more active species are involved in the redox reaction of organic compounds, thus enhancing their photocatalytic activity. When the content of CdWO_4 in the heterojunction was 20, the composite showed the best degradation effect, and the degradation rate of Rhodamine B was 94 under 180 min visible light, showing a good decolorization effect. After four cycles, the degradation of Rhodamine B by heterojunction was not significantly reduced, which proved the good stability of the heterojunction. The degradation mechanism of g-C_3N_4/CdWO_4 was proposed by trapping experiment and ESR characterization experiment. (2) MnWO_4/g-C_3N_4 nanocomposites were synthesized by hydrothermal method. A series of characterization showed that the MnWO_4 was uniformly loaded on the surface of layered g-C_3N_4. When the loading amount of MnWO_4 is 10, the activity of the composite photocatalyst is the highest, which is 2.3 times and 12.7 times higher than that of pure g-C_3N_4 and MnWO_4, respectively. In the visible light, the degradation rate of Rhodamine B by 10MnWOS 4 / g-C3Nac 4 heterojunction was 73% under visible light for 4 h, showing a very good decolorization effect. After four cycle experiments, the photocatalytic activity of the heterojunction did not decrease significantly. The catalyst shows good stability and is favorable for industrial application. The degradation mechanism of MnWO_4/g-C_3N_4 was proposed by trapping experiment and ESR characterization experiment. (3) g-C_3N_4/O-doped ZnIn_2S_4 nanocomposites were prepared by hydrothermal method. The existence of lattice oxygen in Zn In_2S_4 was proved by XPS. HRTEM proved that the sheet oxygen doped Zn In_2S_4 was successfully loaded on the surface of layered g-C_3N_4. When the loading of g-C_3N_4 is 20, the composite exhibits the best degradation rate of Rhodamine B. The degradation rate of Rhodamine B by 20g-C _ 3N _ 3N _ 3N _ 2O _ 4 / O _ doped Zn In_2S_4 was 97% under 20 min visible light, which showed that the degradation effect of Rhodamine B was excellent, and the degradation effect was not obviously decreased after four cycles, which reflected the good stability of photocatalyst.
【學(xué)位授予單位】:江蘇大學(xué)
【學(xué)位級別】:碩士
【學(xué)位授予年份】:2017
【分類號】:X791;O643.36
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