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Fenton氧化降解苯胺的條件優(yōu)化及機(jī)理研究

發(fā)布時間:2018-03-10 10:21

  本文選題:Fenton 切入點(diǎn):難降解有機(jī)物 出處:《中國礦業(yè)大學(xué)》2015年碩士論文 論文類型:學(xué)位論文


【摘要】:苯胺是一種高毒性、不易生物降解的有機(jī)污染物,如何治理苯胺廢水已成為當(dāng)務(wù)之急。國內(nèi)外相關(guān)研究動態(tài)表明Fenton技術(shù)具有氧化性強(qiáng)、反應(yīng)條件簡單、操作方便、不易產(chǎn)生二次污染物等特點(diǎn),在處理難降解有機(jī)污染物時具有獨(dú)特的優(yōu)勢。為了提高Fenton氧化效果應(yīng)該確定最佳反應(yīng)條件。Fenton反應(yīng)的本質(zhì)是氧化還原反應(yīng),而氧化還原電位(ORP)作為氧化還原反應(yīng)的重要參數(shù),理論上能夠較好的指示Fenton反應(yīng)進(jìn)程。因此,系統(tǒng)地分析Fenton反應(yīng)影響因素作用機(jī)制,、實(shí)現(xiàn)Fenton技術(shù)的在線控制有著重要指導(dǎo)意義。通過考察p H、H2O2/Fe2+的摩爾投加比以及絕對投加量等因素對Fenton氧化降解苯胺的影響,通過正交試驗(yàn)優(yōu)化Fenton氧化條件;再根據(jù)不同條件下反應(yīng)過程中ORP及其峰值的變化,篩選出Fenton反應(yīng)體系的主要氧化還原電對,對Fenton氧化苯胺過程中氧化還原電位的變化規(guī)律進(jìn)行研究,以達(dá)到通過ORP表觀值控制Fenton反應(yīng)進(jìn)程的目的;通過檢測Fenton降解苯胺的中間產(chǎn)物對其反應(yīng)機(jī)理進(jìn)行初步的研究和探討。主要研究結(jié)果如下:(1)利用Fenton試劑處理濃度為100mg/L的模擬苯胺廢水,通過單因素及正交試驗(yàn)得出其最優(yōu)操作條件為:p H=3.3,H2O2/Fe2+投加摩爾比為10:1,H2O2和Fe2+的絕對投加量分別為12.5mmol/L及1.25mmol/L;在該條件下反應(yīng)60min,苯胺和CODcr的去除率即可分別達(dá)到87.73%和67.12%。(2)氧化還原電對Fe3+/Fe2+直接決定Fenton反應(yīng)過程中的ORP值,p H值、H2O2投加量和H2O2/Fe2+投加摩爾比等因素均可影響體系中鐵離子形態(tài)轉(zhuǎn)化,其中H2O2投加量的影響最為顯著;根據(jù)Fenton反應(yīng)過程中,ORP的變化規(guī)律指示有機(jī)物的降解程度。(3)借助氣-質(zhì)聯(lián)用儀(GC-MS)分析檢測了苯胺降解的中間產(chǎn)物,對苯胺的降解機(jī)理進(jìn)行了初步探討。苯胺降解的初始產(chǎn)物主要為氨基苯酚,隨著反應(yīng)的進(jìn)行,苯環(huán)開環(huán)生成丁烯二酸。這一反應(yīng)與羥基化經(jīng)典理論相符。在Fenton試劑足夠的條件下,丁烯二酸再同羥基自由基發(fā)生進(jìn)一步反應(yīng),并最終轉(zhuǎn)化為二氧化碳和水。
[Abstract]:Aniline is a highly toxic and not biodegradable organic pollutant. How to treat aniline wastewater has become an urgent matter. The related research trends at home and abroad show that Fenton technology has strong oxidation, simple reaction conditions and convenient operation. In order to improve the oxidation effect of Fenton, it should be determined that the best reaction condition is redox reaction. As an important parameter of redox reaction, redox potential can indicate the process of Fenton reaction in theory. It is important to analyze the mechanism of influencing factors of Fenton reaction and realize the on-line control of Fenton technology. The effects of molar ratio of p H 2O 2 / Fe 2 and absolute dosage on the oxidation and degradation of aniline by Fenton are investigated. The oxidation conditions of Fenton were optimized by orthogonal test, and the main redox electric pairs of Fenton reaction system were selected according to the change of ORP and its peak value during the reaction under different conditions. The change of redox potential in the process of aniline oxidation by Fenton was studied in order to control the process of Fenton reaction through the apparent value of ORP. The reaction mechanism of aniline was studied by detecting the intermediate product of aniline degradation by Fenton. The main results are as follows: 1) the simulated aniline wastewater with 100 mg / L aniline concentration was treated with Fenton reagent. By single factor and orthogonal test, the optimal operating conditions were obtained as follows: molar ratio of 10: 1: 1% H _ 2O _ 2 and Fe2 were 12.5 mmol / L and 1.25 mmol / L, respectively, and the removal rates of aniline and CODcr reached 87.73% and 67.12.1 mmol / L for 60 mins respectively (P < 0.05). The optimum conditions for oxidation of aniline and CODcr were as follows: the molar ratio of H _ 2O _ 2 to H _ 2O _ 2 was 10: 1 / 1 and the absolute dosages of H _ 2O _ 2 and Fe2 were 12.5 mmol / L and 1.25 mmol / L, respectively. Fe3 / Fe _ 2 directly determines the amount of H _ 2O _ 2 and H _ 2O _ 2 and the molar ratio of H _ 2O _ 2 / Fe _ 2 to Fe3 / Fe _ 2 in the Fenton reaction, which can affect the transformation of Fe ~ (2 +) in the system. The effect of H _ 2O _ 2 dosage on the degradation of aniline was the most significant, and the degradation degree of organic matter was indicated according to the variation rule of Fenton. The intermediate product of aniline degradation was detected by GC-MS. The degradation mechanism of aniline was preliminarily discussed. The primary product of aniline degradation was aminophenol. This reaction is consistent with the classical theory of hydroxylation. Under sufficient conditions of Fenton reagent, butene diacid reacts further with hydroxyl radical and is converted to carbon dioxide and water.
【學(xué)位授予單位】:中國礦業(yè)大學(xué)
【學(xué)位級別】:碩士
【學(xué)位授予年份】:2015
【分類號】:X703.1

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