本文關(guān)鍵詞：光催化劑的制備與有機(jī)物降解機(jī)理關(guān)系研究　出處：《沈陽理工大學(xué)》2015年碩士論文　論文類型：學(xué)位論文

  更多相關(guān)文章： 氧化鈦 鈦酸鍶 負(fù)載 光催化 降解機(jī)理

【摘要】：在催化劑制備方面,本課題主要采用溶膠-凝膠法制備出了Ti O2和Sr Ti O3兩種粉末光催化劑,對主要的制備條件進(jìn)行優(yōu)化后,分別以0.5HZSM-5和0.3HZSM-5作為二者的載體,制備負(fù)載型催化劑,考察負(fù)載量對光催化劑結(jié)構(gòu)和活性的影響,以獲得性能優(yōu)越的負(fù)載型光催化劑,通過XRD、SEM、FT-IR、BET和BJH等表征手段進(jìn)行深入分析。在有機(jī)物降解機(jī)理方面,本課題主要研究不同負(fù)載量的光催化劑對苯酚和活性艷紅X-3B的降解機(jī)理,通過UV-Vis、FT-IR和TOC等分析手段進(jìn)行深入分析。主要實驗研究分為以下四部分:(1)以鈦酸四丁酯為鈦源,0.5 mol/L的H3PO4改性的HZSM-5為載體,采用溶膠凝膠法制備了純Ti O2以及χTi O2/0.5HZSM-5。結(jié)果表明,樣品中的Ti O2主要以銳鈦礦的形式存在,負(fù)載能夠降低Ti O2的晶粒尺寸。負(fù)載型催化劑具有較大的比表面積,孔徑分布范圍寬。隨著負(fù)載量逐漸增加,催化劑比表面積呈現(xiàn)減小的趨勢。(2)以鈦酸四丁酯為鈦源,硝酸鍶為鍶源,0.3 mol/L的HCl改性的HZSM-5為載體,采用溶膠-凝膠法制備了純Sr Ti O3以及χSr Ti O3/0.3HZSM-5。結(jié)果表明,樣品中的Sr Ti O3主要以鈣鈦礦的形式存在,負(fù)載之后Sr Ti O3晶粒尺寸基本沒有變化。負(fù)載量越大比表面積就越小。負(fù)載之后孔徑分布范圍寬,表現(xiàn)為多級孔道,主要是大孔和介孔結(jié)構(gòu)。(3)采用制備的兩類催化劑對活性艷紅X-3B進(jìn)行光催化降解并研究降解歷程,光照30 min,50%Ti O2/0.5HZSM-5對活性艷紅X-3B的降解率最高,達(dá)到40.7%,比純Ti O2的26.4%提高了14.3%。30%Sr Ti O3/0.3HZSM-5對活性艷紅X-3B的降解率最高,達(dá)到30.6%,比純Sr Ti O3的3.5%提高了27.1%。推測羥基自由基首先攻擊的是-NH-中的N原子,并且分解開的物質(zhì)會繼續(xù)氧化生成醛和酸等小分子物質(zhì);萘醌被氧化為鄰苯二甲酸,然后被降解為小分子酸或醛。含氯基團(tuán)被氧化成含氯有機(jī)物,但延長反應(yīng)時間,大部分有機(jī)氯能完全轉(zhuǎn)化為Cl-,小分子的酸或醛被進(jìn)一步氧化為CO2和H2O,最后剩余不可光催化降解的物質(zhì)。(4)采用制備的兩類催化劑對苯酚進(jìn)行光催化降解并研究降解歷程,光照30min,50%Ti O2/0.5HZSM-5對苯酚溶液的降解率最高,達(dá)到44.4%,比純Ti O2的25.5%提高了18.9%。30%Sr Ti O3/0.3HZSM-5對苯酚溶液的降解率最高,達(dá)到32.2%,比純Sr Ti O3的15.7%提高了16.5%。推測羥基自由基首先攻擊苯酚中的苯環(huán),并附著在苯環(huán)上形成苯二酚,苯二酚被氧化成苯醌,然后苯環(huán)被打開降解成小分子的酸或醛,進(jìn)一步氧化成CO2和H2O,經(jīng)一定時間可完全降解。
[Abstract]:In the aspect of catalyst preparation, two kinds of powder photocatalysts, TIO _ 2 and Sr _ 2O _ 3, were prepared by sol-gel method, and the main preparation conditions were optimized. The supported catalysts were prepared using 0.5HZSM-5 and 0.3HZSM-5 as the supports, respectively. The effects of loading amount on the structure and activity of photocatalyst were investigated. In order to obtain the supported photocatalyst with superior performance, the mechanism of organic matter degradation was analyzed by means of XRDD-SEMT-IRT-BET and BJH. In this paper, the degradation mechanism of phenol and reactive brilliant red X-3B by different amount of photocatalyst was studied, and the degradation mechanism of phenol and reactive brilliant red X-3B was studied by UV-Vis. The main experimental research is divided into the following four parts: 1) using tetrabutyl titanate as titanium source. The pure TIO _ 2 and 蠂 TIO _ 2 / 0.5 HZSM-5 were prepared by sol-gel method on HZSM-5 modified by 0.5 mol/L H _ 3PO _ 4. The results showed that the pure TIO _ 2 and 蠂 _ 2O _ 2 / 0.5 HZSM-5 were prepared. The TIO _ 2 in the sample mainly exists in the form of anatase, and the loading can reduce the grain size of TIO _ 2, and the supported catalyst has a large specific surface area. The pore size distribution range is wide. With the increase of loading amount, the specific surface area of the catalyst decreases. 2) tetrabutyl titanate is used as titanium source and strontium nitrate as strontium source. The HCl modified HZSM-5 of 0.3 mol/L was used as the carrier. Pure Sr TIO 3 and 蠂 Sr TIO 3 / 0.3 HZSM-5 were prepared by sol-gel method. Sr TIO 3 in the sample mainly exists in the form of perovskite. After loading, the grain size of Sr TIO 3 does not change. The larger the loading amount is, the smaller the specific surface area is. The pore size distribution range is wide after loading, and the pore size distribution is multistage. The photocatalytic degradation of reactive brilliant red X-3B was carried out with macroporous and mesoporous structure. The photocatalytic degradation of reactive brilliant red X-3B was studied under light irradiation for 30 min. The degradation rate of reactive brilliant red X-3B by 50 TIO _ 2 / 0.5 HZSM-5 was the highest, reaching 40.7%. Compared with pure TIO _ 2 26.4%, the degradation rate of active brilliant red X-3B was the highest (30.6%). The degradation rate of 0.3HZSM-5 was higher than that of pure TIO _ 2. 30 Sr TIO _ 3 / 0.3HZSM-5 was higher than that of pure TIO _ 2. Compared with 3.5% of pure Sr TIO 3, it is suggested that the first attack of hydroxyl radical is the N atom in -NH-. And decomposed substances will continue to oxidize to aldehydes and acids and other small molecules; Naphthoquinone was oxidized to phthalic acid and then degraded to small molecular acid or aldehydes. Chlorinated groups were oxidized to chlorinated organic compounds but most of the organic chlorine could be completely converted to Cl- when the reaction time was prolonged. The acids or aldehydes of small molecules were further oxidized to CO2 and H _ 2O. Finally, the remaining non-photocatalytic degradation of phenol was carried out using two kinds of catalysts prepared and the degradation process was studied. The degradation rate of phenol solution was the highest (44.4%) after 30 min irradiation with 50% TIO _ 2 / 0.5 HZSM-5. Compared with pure TIO _ 2 25.5%, the degradation rate of phenol solution by 18.90.30Sr TIO _ 3 / 0.3HZSM-5 was the highest, up to 32.2%. It is suggested that hydroxyl radicals attack the benzene ring in phenol at first and attach to the benzene ring to form dihydroxybenzene, which is oxidized to benzoquinone. Then the benzene ring was opened and degraded to a small molecule of acid or aldehydes, which was further oxidized to CO2 and H _ 2O, and could be completely degraded after a certain time.
【學(xué)位授予單位】：沈陽理工大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2015
【分類號】：TQ426;X703

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