聚醚改性硅油膠束用于制備染料降解催化劑的研究
發(fā)布時(shí)間:2018-07-17 02:40
【摘要】:有機(jī)染料在紡織印染工業(yè)中被廣泛使用,印染廢水中染料的除去一直是紡織印染領(lǐng)域一個(gè)長(zhǎng)期關(guān)注的焦點(diǎn)問(wèn)題。其中,基于高級(jí)氧化法的染料催化降解方法是一主要研究方向,研究開(kāi)發(fā)各種有效的染料降解催化劑也是一個(gè)重點(diǎn)關(guān)注的研究課題。鑒于兩親性聚醚改性硅油獨(dú)特的表面活性,本文創(chuàng)新性的利用聚醚改性硅油膠束作為微納米反應(yīng)器進(jìn)行原位負(fù)載型催化劑的制備,并用于染料降解的研究。本文通過(guò)硅氫加成反應(yīng)制備得到一系列不同結(jié)構(gòu)的聚醚改性硅油,并研究了其在不同溶劑中的自組裝行為,考察了不同因素對(duì)其聚集態(tài)的影響。隨之利用自組裝形成的聚醚改性硅油膠束作為微納米反應(yīng)器,通過(guò)煅燒制得了原位負(fù)載型催化劑Co3O4/SiO2并用于染料降解。主要研究成果如下:一、通過(guò)硅氫加成反應(yīng)合成得到一系列不同結(jié)構(gòu)的聚醚改性硅油(PDMS-g-PEO/PO)接枝共聚物。1、以聚硅氧烷(PHMS)為主鏈,烯丙基聚氧乙烯醚(PEO/PO)為支鏈,鉑為催化劑,60℃反應(yīng)溫度下,通過(guò)硅氫加成法制備得到一系列不同結(jié)構(gòu)的聚醚改性硅油。2、利用傅里葉變換紅外光譜儀(FTIR)和核磁共振氫譜(1H NMR)進(jìn)行表征,發(fā)現(xiàn)產(chǎn)物結(jié)構(gòu)明晰,并與設(shè)計(jì)的分子結(jié)構(gòu)一致。二、通過(guò)PDMS-g-PEO/PO的溶液自組裝,獲得球形、棒狀、囊泡狀等多種形態(tài)的聚集體。1、利用芘(Py)作為熒光探針,測(cè)得了PDMS-g-PEO兩親性共聚物在不同溶劑中的臨界膠束濃度,考察了臨界膠束濃度隨組成的變化規(guī)律。研究表明,疏水性的硅氧烷鏈段越長(zhǎng),親水性的聚醚鏈段越多,其臨界膠束濃度越大。聚合物在丙酮和水的混合溶劑中的臨界膠束濃度值大于在水溶液中的臨界膠束濃度值。2、利用TEM表征手段,考察了兩親性有機(jī)硅接枝共聚物在共聚物分子組成、陳化時(shí)間、溶劑性質(zhì)及溫度等因素對(duì)溶液中自組裝聚集體的形態(tài)變化特征的影響。研究發(fā)現(xiàn),隨著陳化時(shí)間的延長(zhǎng),小囊泡(球狀)聚集融合轉(zhuǎn)變?yōu)榇竽遗莼驈?fù)合囊泡。隨著溫度的升高,膠束的形態(tài)由球狀轉(zhuǎn)變?yōu)榘魻?且尺寸也進(jìn)一步增大。兩親性共聚物在不同的分子組成中和不同的溶劑中,膠束化行為也有所不同。三、利用聚醚改性硅油膠束作為微納米反應(yīng)器,通過(guò)煅燒制備得到Co3O4/SiO2原位負(fù)載型催化劑。1、利用TEM、XPS、XRD考察了催化劑的形貌、元素組成及晶型。與不加催化劑相比較,加入催化劑后,甲基橙的降解率明顯提高。2、考察了煅燒溫度、煅燒時(shí)間、攪拌速率等因素對(duì)催化劑性能的影響。結(jié)果表明,在煅燒溫度為700℃、煅燒時(shí)間為5 h、攪拌速率為500 r/min時(shí),催化劑的催化性能較好。3、考察了制備的催化劑對(duì)不同染料的降解效果。研究結(jié)果表明,Co3O4/SiO2對(duì)酸性染料、活性染料等常見(jiàn)的染料能夠有效地催化氧化。4、經(jīng)過(guò)多次重復(fù)降解后,催化劑仍然保持了穩(wěn)定的催化活性。
[Abstract]:Organic dyes are widely used in textile printing and dyeing industry. The removal of dyes from printing and dyeing wastewater has been a long-term focus in the field of textile printing and dyeing. Among them, the catalytic degradation of dyes based on advanced oxidation method is a main research direction, and the research and development of a variety of effective dye degradation catalysts is also an important research topic. In view of the unique surface activity of amphiphilic polyether modified silicone oil, the in situ supported catalyst was prepared by using polyether modified silicone oil micelle as a micro and nano reactor and used in the degradation of dyes. In this paper, a series of polyether modified silicone oils with different structures were prepared by hydrosilylation reaction. The self-assembly behavior of polyether modified silicone oil in different solvents was studied, and the influence of different factors on the aggregation state was investigated. Then the self-assembled polyether modified silicone oil micelle was used as a micro-nano reactor and the in-situ supported catalyst Co _ 3O _ 4 / Sio _ 2 was prepared by calcination and used for the degradation of dyes. The main results are as follows: first, a series of polyether modified silicone oil (PDMS-g-PEO / PO) grafted copolymers with different structures were synthesized by hydrosilylation reaction. The main chain was polysiloxane (PHMS) and the branching chain was allyl polyoxyethylene oxide ether (PEO / PO). A series of polyether modified silicone oils with different structures were prepared by hydrosilylation at 60 鈩,
本文編號(hào):2128652
[Abstract]:Organic dyes are widely used in textile printing and dyeing industry. The removal of dyes from printing and dyeing wastewater has been a long-term focus in the field of textile printing and dyeing. Among them, the catalytic degradation of dyes based on advanced oxidation method is a main research direction, and the research and development of a variety of effective dye degradation catalysts is also an important research topic. In view of the unique surface activity of amphiphilic polyether modified silicone oil, the in situ supported catalyst was prepared by using polyether modified silicone oil micelle as a micro and nano reactor and used in the degradation of dyes. In this paper, a series of polyether modified silicone oils with different structures were prepared by hydrosilylation reaction. The self-assembly behavior of polyether modified silicone oil in different solvents was studied, and the influence of different factors on the aggregation state was investigated. Then the self-assembled polyether modified silicone oil micelle was used as a micro-nano reactor and the in-situ supported catalyst Co _ 3O _ 4 / Sio _ 2 was prepared by calcination and used for the degradation of dyes. The main results are as follows: first, a series of polyether modified silicone oil (PDMS-g-PEO / PO) grafted copolymers with different structures were synthesized by hydrosilylation reaction. The main chain was polysiloxane (PHMS) and the branching chain was allyl polyoxyethylene oxide ether (PEO / PO). A series of polyether modified silicone oils with different structures were prepared by hydrosilylation at 60 鈩,
本文編號(hào):2128652
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