【摘要】：Fenton/類Fenton氧化法在污水預處理和深度處理中有著廣泛應用。然而Fenton/類Fenton法存在應用p H較低,Fe(III)向Fe(II)轉(zhuǎn)化速度慢,Fe(II)利用率低等缺點。乙二胺四乙酸(EDTA)、氨基三乙酸(NTA)與Fe3+/Fe2+形成的絡(luò)合物在中性或弱堿性溶液中較穩(wěn)定,保證了可溶性Fe(III)/Fe(II)濃度。雜環(huán)芳烴衍生物代表阿特拉津(AT)和苯環(huán)芳烴衍生物代表硝基苯(NB)是廣泛存在于各水體中的難降解有機污染物,Fenton/類Fenton法是較理想的降解方法。本研究以EDTA、NTA為絡(luò)合劑分別與AT和NB組成模擬污水,以硫酸鐵溶液和H2O2組成類Fenton體系,研究不同絡(luò)合劑的存在對類Fenton反應降解有機物的影響,并對Fe IIINTA/H2O2反應降解不同目標物進行研究。NTA、EDTA的存在對類Fenton反應降解AT影響實驗結(jié)果:(1)絡(luò)合劑存在時,在p H為7和9時,AT降解效果相對于無絡(luò)合劑存在時明顯提升。(2)當NTA和EDTA存在時,由于p H值的提高改變了Fe(III)絡(luò)合物的形態(tài)結(jié)構(gòu),使Fe IIINTA更容易與過氧化氫絡(luò)合,并且H2O2本身也更容易被分解,p H=3~9時,AT的降解效率隨p H值提升而提升。(3)由于Fe IIINTA和FeIIIEDTA不同p H值下形態(tài)和空間結(jié)構(gòu)差異,p H=7~9范圍內(nèi),NTA存在下類Fenton反應降解AT的效果優(yōu)于EDTA。(4)NTA和EDTA存在時,H2O2和Fe(III)初始濃度增加能提升AT的降解效果。(5)反應體系中叔丁醇濃度的增加對AT的降解抑制明顯,這表明EDTA、NTA存在下類Fenton反應降解有機物的主要活性物種是羥基自由基。(6)Fe IIINTA和Fe IIIEDTA在降解AT的過程中自身均有分解,Fe IIIEDTA能分解成Fe IIINTA,會加快反應速率。FeIIINTA/H2O2反應降解不同結(jié)構(gòu)目標物的研究表明:(1)由于NB降解中間產(chǎn)物的作用以及AT、NB本身結(jié)構(gòu)的差異,NTA存在下,p H=3時,NB的降解效能比AT降解效能高,而p H=7時AT的降解效能更高。(2)除NTA初始濃度以外的其它因素對AT和NB的降解的影響基本相似。(3)NB降解的中間產(chǎn)物與無絡(luò)合劑存在的類Fenton反應降解硝基苯的中間產(chǎn)物相同,降解途徑相似。(4)NB降解中間產(chǎn)物對類Fenton反應自催化作用不明顯,說明NTA阻礙了Fe(III)與中間產(chǎn)物的接觸。
[Abstract]:Fenton/ type Fenton oxidation process is widely used in wastewater pretreatment and advanced treatment. However, the Fenton/ class Fenton method has some disadvantages such as low, Fe (III) conversion speed to Fe (II), low, Fe (II) utilization rate and so on. The complex formed by ethylenediamine tetraacetic acid (EDTA), aminotriacetate (NTA) and Fe3 / Fe2 is stable in neutral or weak alkaline solution, which ensures the concentration of soluble Fe (III) / Fe (II). Heterocyclic aromatic derivatives represent atrazine (AT) and benzene ring aromatic derivatives represent nitrobenzene (NB), which are widely used as refractory organic pollutants in various water bodies. Fenton/ Fenton method is an ideal method for degradation. In this study, EDTA,NTA was used as complexing agent with AT and NB to form simulated sewage, and ferric sulfate and H2O2 were used to form Fenton system to study the effect of different complexing agents on the degradation of organic compounds by Fenton reaction. The effect of NTA,EDTA on the degradation of AT by Fenton reaction was studied. The results were as follows: (1) in the presence of complex agent, pH was 7 and 9, respectively. The degradation effect of AT was significantly improved compared with that without complex agent. (2) in the presence of NTA and EDTA, the morphological structure of Fe (III) complex was changed due to the increase of pH value, which made it easier for Fe IIINTA to complex with hydrogen peroxide. The degradation efficiency of AT increased with the increase of pH value. (3) because of the difference in morphology and spatial structure of Fe IIINTA and FeIIIEDTA under different pH values, the degradation efficiency of AT increased with the increase of pH value. In the presence of NTA, the degradation of AT by Fenton reaction was better than that by EDTA. (4) NTA and EDTA. The increase of initial concentration of H2O2 and Fe (III) could enhance the degradation of AT. (5) the degradation of AT was inhibited obviously by the increase of tert-butanol concentration in the reaction system. It is suggested that the main active species for Fenton reaction degradation of organic compounds in the presence of EDTA,NTA is hydroxyl radical. (6) Fe IIINTA and Fe IIIEDTA decompose, Fe IIIEDTA to Fe IIINTA, in the process of AT degradation. The results show that: (1) due to the effect of NB on degradation of intermediate products and the structure difference of AT,NB itself, in the presence of NTA, pH = 3, The degradation efficiency of NB was higher than that of AT. The degradation efficiency of AT was higher than that of pH = 7. (2) the effect of other factors other than the initial concentration of NTA on the degradation of AT and NB was similar. (3) the intermediate product of NB degradation was similar to Fenton reaction without complexing agent to degrade nitrate. The intermediate products of benzene are the same, The degradation pathway was similar. (4) the autocatalytic effect of the intermediate product of NB degradation on Fenton reaction was not obvious, which indicated that NTA hindered the contact between Fe (III) and the intermediate product.
【學位授予單位】：哈爾濱工業(yè)大學
【學位級別】：碩士
【學位授予年份】：2015
【分類號】：X703

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