本文選題：Keggin多酸　切入點(diǎn)：光敏劑　出處：《東北師范大學(xué)》2017年碩士論文　論文類型：學(xué)位論文

【摘要】：雜多酸是一種綠色催化劑,具有活性高、選擇性好、無毒性、不腐蝕設(shè)備等優(yōu)點(diǎn)。大量的研究工作表明在光激發(fā)作用下,激發(fā)態(tài)的多酸具有很強(qiáng)的氧化能力,可以有效地降解有機(jī)污染物。然而,該類催化劑易溶于水且在催化反應(yīng)條件下穩(wěn)定性差,這使其不易回收重復(fù)利用。其中,Keggin型鎢系多酸盡管具有很好的光催化活性,但是其只能利用太陽光中的紫外光,這限制了其在實(shí)際中的應(yīng)用。制備基于多酸有機(jī)無機(jī)雜化物是當(dāng)前解決這一缺陷的有效途徑之一。通過引入有機(jī)物光敏劑,與多酸形成一種雜化物,這樣既能夠形成非均相的催化劑,實(shí)現(xiàn)催化劑的循環(huán)再利用,又能增加其在可見光下的催化活性。因此,尋找合適的光敏劑備受人們的關(guān)注。本論文則選用黃色的有機(jī)物2,4,6-三(1-咪唑基)-1,3,5-三嗪(TIT)作為光敏劑,經(jīng)酸化后,分別與Keggin型磷鎢酸和硅鎢酸通過簡單的共沉淀法,制備了兩個(gè)黃色的非水溶性的有機(jī)無機(jī)雜化物:TITH-PW12和TITH-SiW12。我們通過使用UV-vis,FT-IR,SEM等手段對其組成進(jìn)行了表征,探究了在可見光照射下對甲基橙溶液(MO)催化降解活性,并初步探討了它們的催化降解機(jī)理。實(shí)驗(yàn)結(jié)果表明,雜化物中多酸(PW12和SiW12)在沉淀過程中結(jié)構(gòu)是保持完整的,同時(shí),發(fā)現(xiàn)所得的雜化物在可見光區(qū)的吸收大大增加。在可見光的照射下,化合物TITH-PW12和TITH-Si W12不需加任何氧化劑就能夠?qū)⒓谆?MO)溶液完全降解,顯示了很好的催化活性。催化劑易于從反應(yīng)體系分離、回收,而且重復(fù)利用四次后,其結(jié)構(gòu)及催化活性仍保持不變,催化降解滿足一級動力學(xué)方程。同時(shí)發(fā)現(xiàn),當(dāng)選用同一種光敏劑而改變Keggin型雜多酸不同時(shí),所形成的復(fù)合物的催化活性沒有明顯的變化。因此,光敏劑的選擇對降解染料催化活性起著至關(guān)重要的作用。
[Abstract]:Heteropoly acid is a kind of green catalyst with high activity, good selectivity, non-toxicity, non-corrosive equipment and so on. A large number of studies show that excited polyacids have strong oxidation ability under photoexcitation. However, this kind of catalyst is easy to dissolve in water and has poor stability under the condition of catalytic reaction, which makes it difficult to recover and reuse. However, it can only use ultraviolet light in the sun, which limits its practical application. The preparation of polyacid-based organic-inorganic hybrids is one of the effective ways to solve this defect. A hybrid is formed with polyacid, which can form heterogeneous catalysts, recycle the catalysts, and increase their catalytic activity under visible light. In this paper, the yellow organic compounds (2x4, 6-, 3-triamidazolyl) were chosen as Guang Min. After acidification, they were treated with Keggin phosphotungstic acid and silicotungstic acid by simple coprecipitation method, respectively. Two yellow insoluble organic-inorganic hybrids: TITH-PW12 and TITH-SiW12were prepared. Their composition was characterized by UV-vis-FT-IR SEM, and the catalytic degradation activity of methyl orange solution (MOO) under visible light irradiation was investigated. The experimental results show that the structures of the polyacids PW12 and SiW12 in the hybrids remain intact during the precipitation process. It was found that the absorption of the resulting hybrids in the visible region was greatly increased. Under visible light irradiation, compounds TITH-PW12 and TITH-Si W12 could completely degrade the methyl Orange MOA solution without adding any oxidant. The catalyst is easy to be separated and recovered from the reaction system, and its structure and catalytic activity remain unchanged after being reused for four times, and the catalytic degradation satisfies the first-order kinetic equation. When the same Guang Min was used to change the Keggin heteropoly acid, the catalytic activity of the complex formed did not change obviously. Therefore, the selection of Guang Min played an important role in the degradation of dye catalytic activity.
【學(xué)位授予單位】：東北師范大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2017
【分類號】：O643.36;O644.1

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