本文選題：吡啶氮氧化物　切入點(diǎn)：金屬配合物　出處：《東華大學(xué)》2017年碩士論文

【摘要】：隨著我國(guó)經(jīng)濟(jì)高速發(fā)展,印染行業(yè)廢水排量大幅度增長(zhǎng),占綜合排水量60%左右。根據(jù)具體印染工藝,對(duì)印染廢水的處理方法主要有物理法、生物法和化學(xué)法。物理法一般指簡(jiǎn)單的界面吸附;化學(xué)法一般指加入強(qiáng)氧化劑對(duì)有機(jī)污染物進(jìn)行氧化降解;生物法主要利用好氧生物酶和厭氧生物酶對(duì)廢水中有機(jī)污染物進(jìn)行氧化脫色,效果好,但是由于其生物活性難以保證,且使用條件較為苛刻,因此研究應(yīng)用人工合成的仿酶催化劑,用于化學(xué)法中催化氧化處理印染廢水是一種趨勢(shì)。均相催化劑使用便捷,催化效率高,但是回收困難,容易產(chǎn)生二次污染。因此,催化劑固化技術(shù)近年來(lái)受到廣泛關(guān)注。吡啶類氮氧化物中與雜環(huán)N原子直接相連的氧原子電子云密度較大,易與金屬離子配位形成新穎的結(jié)構(gòu),且金屬配合物具有更好的催化活性。本文首先合成了三種同分異構(gòu)體配體1,4-二(2-N氧化吡啶)甲氧基苯(L_1),1,4-二(3-N氧化吡啶)甲氧基苯(L_2),1,4-二(4-N氧化吡啶)甲氧基苯(L_3)作為配體,分別與CuCl_2、CoCl_2、MnCl_2配位合成了9種金屬配合物。并通過(guò)核磁、紅外、元素分析確定了配體和配合物的結(jié)構(gòu)。在此基礎(chǔ)上,以過(guò)氧化氫為氧化劑,比較了9種配合物對(duì)于活性藍(lán)-19的催化脫色效果,研究配合物的活性和配體結(jié)構(gòu)及金屬種類的關(guān)系。結(jié)果表明,與配體L_3配位的金屬配合物具有較高的活性,而三種不同的金屬中,Co鹽活性最高,所以得到金屬配合物CoL_3的催化效率最高。以此配合物為研究對(duì)象,研究了催化劑用量,pH值,過(guò)氧化氫用量,底物濃度對(duì)染料降解效果的影響。得到最佳催化降解條件:30 mL染料溶液(濃度500 mg/L),56 mL蒸餾水,14 mL 1 mol/L Na_2CO_3/NaHCO_3緩沖溶液(pH=10.2),加入過(guò)氧化氫使其濃度為0.1 mol/L,CoL_3 10 mg,室溫下進(jìn)行反應(yīng),15 min脫色率可達(dá)到95%以上。采用微膠囊技術(shù)對(duì)選出的最優(yōu)催化劑CoL_3進(jìn)行負(fù)載,將催化劑和磁性粉末包覆在明膠壁材中,使用戊二醛交聯(lián),得到了包覆配合物的磁性微膠囊。催化活性測(cè)試實(shí)驗(yàn)表明,包覆CoL_3的磁性配合物微膠囊依然能夠很好地催化降解活性藍(lán)19。溶液中的磁性配合物微膠囊可通過(guò)外加磁場(chǎng)進(jìn)行回收,并且可以重復(fù)利用。通過(guò)循環(huán)實(shí)驗(yàn)可知循環(huán)使用5次后,其脫色率仍保持到90%以上;重復(fù)使用8次后,其脫色率仍保持到60%以上。
[Abstract]:With the rapid development of China's economy, the discharge of printing and dyeing wastewater has increased by a large margin, accounting for about 60% of the comprehensive discharge. According to the specific printing and dyeing process, the main treatment methods for printing and dyeing wastewater are physical methods. Biological and chemical methods. Physical methods generally refer to simple interfacial adsorption. Chemical methods generally refer to the oxidation and degradation of organic pollutants by adding strong oxidants. The biological method mainly uses aerobic and anaerobic biological enzymes to decolorize organic pollutants in wastewater, but its biological activity is difficult to guarantee, and the application conditions are harsh. Therefore, it is a trend to study the application of synthetic imitating enzyme catalyst to the treatment of printing and dyeing wastewater by catalytic oxidation in chemical method. The homogeneous catalyst is convenient to use, the catalytic efficiency is high, but the recovery is difficult, and it is easy to produce secondary pollution. In recent years, the curing technology of catalyst has attracted wide attention. The electron cloud of oxygen atoms directly connected with heterocyclic N atoms in pyridine nitrogen oxides has a high density and is easily coordinated with metal ions to form novel structures. The metal complexes have better catalytic activity. Firstly, three isomer ligands, 1H 4- dioxy 2-N oxide pyridine) methoxy benzene-L _ 1C _ (1) -dioxy _ 3-N pyridine) were synthesized as ligands, and their ligands were used as ligands, and their ligands were as follows: (1) the ligands of the three isomer ligands, 1 ~ (4) -dioxy (2-N) pyridine) were synthesized as ligands, and (1) methoxybenzenes were synthesized as ligands. Nine metal complexes were synthesized by coordination with CuCl2COCl2MnCl2 respectively. The structures of ligand and complexes were determined by NMR, IR and elemental analysis. On this basis, hydrogen peroxide was used as oxidant. The catalytic decolorization effects of 9 complexes on active blue 19 were compared, and the relationship between the activity of the complexes, the structure of ligands and the kinds of metals was studied. The results showed that the metal complexes coordinated with ligand L3 had higher activity. The catalytic efficiency of the metal complex CoL_3 was the highest because of its highest activity among the three different metals. The amount of catalyst, pH and hydrogen peroxide were studied. Effect of substrate concentration on the degradation of dyes. The optimum catalytic degradation conditions were obtained: 30 mL dye solution (500mg 路L ~ (-1) L ~ (-1)) distilled water (#number0# mg 路L ~ (-1)) distilled water / 1 mol/L Na_2CO_3/NaHCO_3 buffer solution (pH = 10.2), adding hydrogen peroxide to 0.1 mol / L CoL3 ~ (10 mg / L), at room temperature. The decolorization rate of 15 min can reach more than 95%. The optimum catalyst CoL_3 was supported by microencapsulation technique. The magnetic microcapsules coated with catalyst and magnetic powder were prepared by glutaraldehyde crosslinking. The magnetic complex microcapsules coated with CoL_3 can still catalyze the degradation of active blue 19.The magnetic complex microcapsules in the solution can be recovered by external magnetic field and can be reused. The decolorization rate remained above 90%, and the decolorization rate remained above 60% after repeated use for 8 times.
【學(xué)位授予單位】：東華大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：O643.36;X791

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