本文選題：苯胺 + 三維電催化氧化法　； 參考：《華東師范大學(xué)》2017年碩士論文

【摘要】：近年來水污染問題日趨嚴(yán)重,其中高濃度含氮有機(jī)污染物由于對(duì)微生物有很強(qiáng)的毒害性,常規(guī)水處理方法難以去除。三維電催化氧化法具有氧化降解能力強(qiáng)、處理效率高、無二次污染等特點(diǎn),且可提高廢水可生化性,非常適用于處理難降解廢水。本文以苯胺這種典型含氮污染物為對(duì)象圍繞三維電催化氧化苯胺開展以下幾個(gè)方面的研究。(1)粒子電極對(duì)苯胺電催化降解效果的影響。活性炭三維電化學(xué)體系中最常用的粒子電極,采用浸漬法將.TiO2-SnO2負(fù)載于活性炭(GranularActivated Carbon,簡稱GAC)中得到一種具有催化活性的新型活性炭-載TiO2-Sn02活性炭(Ti02/SnO2-GAC,簡稱GTSO)。文章選取GAC和GTSO兩種活性炭作為三維粒子電極,通過電鏡掃描、能譜分析、紅外分析、XRD粉末衍射分析以及孔徑-比表面積分析等表征手段來對(duì)兩種活性炭進(jìn)行性能比較,分析發(fā)現(xiàn)在GTSO的表面以及孔道內(nèi)都分布著晶型氧化鈦,而且其比表面積比GAC減小了 390.61 m2·g-1,平均孔徑減小了 0.27 nm,總孔容減小了 0.25 cm3·g-1。通過連續(xù)運(yùn)行實(shí)驗(yàn)發(fā)現(xiàn),兩種活性炭都具有很強(qiáng)的吸附特性,每個(gè)批次實(shí)驗(yàn)進(jìn)行了 2 h,實(shí)驗(yàn)進(jìn)行到60批三維電催化氧化裝置運(yùn)行達(dá)到穩(wěn)定。通過研究粒子電極作用效果發(fā)現(xiàn),以GTSO作為粒子電極對(duì)苯胺的電化學(xué)降解去除率為85%,GAC作為粒子電極的去除率為61%,但是兩者均遠(yuǎn)遠(yuǎn)高于不含粒子電極的二維電解體系中21%的去除率。由此,本文最終確定用GTSO作為三維粒子電極對(duì)苯胺廢水進(jìn)行降解實(shí)驗(yàn),(2)三維電催化降解苯胺實(shí)驗(yàn)條件優(yōu)化。通過單因素法來優(yōu)化電場強(qiáng)度、電解質(zhì)、pH、炭水比等影響因素,最終得到一組最優(yōu)條件進(jìn)行苯胺電解實(shí)驗(yàn)。實(shí)驗(yàn)結(jié)果表明,在實(shí)驗(yàn)條件為電場強(qiáng)度1.2V/cm、電解質(zhì)Na2SO4為0.03mol/L、pH為7、炭水比為0.5,電解120 min條件下進(jìn)行電解實(shí)驗(yàn)?zāi)軌蛉〉阶罴研Ч?此時(shí)苯胺和COD去除率分別為84.5%和60.3%。(3)苯胺電化學(xué)降解途徑分析。實(shí)驗(yàn)通過對(duì)體系中氮元素分析(氨氮、硝態(tài)氮、亞硝態(tài)氮)、羥基自由基含量的測(cè)定,以及通過UV-Vis分光光度法、GC-MS色譜分析等方法對(duì)電解出水的成分解析,從而最終確定苯胺的電化學(xué)氧化途徑。實(shí)驗(yàn)結(jié)果表明,經(jīng)過電解之后配水中氨氮含量由原先的0上升到27.70mg/L,硝態(tài)氮和亞硝態(tài)氮也分別由0上升到2.30 mg/L和0.15 mg/L,而總氮含量卻由原先的126.10mg/L下降到50.30mg/L。這說明由于電解的作用確實(shí)使苯胺得到了有效降解。通過添加叔丁醇和乙醇等羥基自由基抑制劑來進(jìn)行對(duì)比實(shí)驗(yàn)發(fā)現(xiàn):當(dāng)電解時(shí)間進(jìn)行30min時(shí),空白組苯胺去除率為40%左右,而加了叔丁醇的實(shí)驗(yàn)組苯胺去除率僅為20%。另外直接對(duì)體系中·OH的測(cè)定也發(fā)現(xiàn),當(dāng)電解120 min后,出水的吸光度為由原水的0上升到0.35。上述結(jié)果充分證明,經(jīng)過電解作用之后,廢水中產(chǎn)生了-OH這種強(qiáng)氧化性物質(zhì)。通過對(duì)出水的UV-Vis掃描和GC-MS分析可知,由于電解作用使苯胺降解生成了醌類、酚類以及羧酸類物質(zhì),同時(shí)檢測(cè)到有十一烷的產(chǎn)生。由此,本文推導(dǎo)出了苯胺的電化學(xué)降解路徑,為后續(xù)對(duì)于苯胺的研究提供了一定的指導(dǎo)意義。
[Abstract]:In recent years, the problem of water pollution is becoming more and more serious, among which the high concentration of nitrogen containing organic pollutants is very toxic to microorganisms, and the conventional water treatment method is difficult to remove. The three dimensional electrocatalytic oxidation method has the characteristics of high oxidation degradation ability, high treatment efficiency, no two pollution and so on, and can improve the biodegradability of wastewater, which is very suitable for the treatment of difficult to drop. In this paper, the study on the three dimensional electrocatalytic oxidation of aniline is carried out in the following aspects. (1) the effect of the particle electrode on the electrocatalytic degradation of aniline. The most commonly used particle electrode in the three dimensional electrochemical system of activated carbon is loaded on the activated carbon (GranularAct) by impregnation method (.TiO2-SnO2) A new type of active carbon loaded TiO2-Sn02 active carbon (Ti02/SnO2-GAC, GTSO) with catalytic activity was obtained in ivated Carbon (GAC). In this paper, two kinds of activated carbons of GAC and GTSO were selected as three dimensional particle electrodes, and the characterization means, such as electron microscope scanning, energy spectrum analysis, infrared analysis, XRD powder diffraction analysis and pore specific surface area analysis, were used. To compare the performance of the two kinds of activated carbon, it is found that the crystalline titanium oxide is distributed in the surface and channel of GTSO, and the specific surface area is reduced by 390.61 m2. G-1. The average pore size decreases by 0.27 nm and the total pore volume decreases by 0.25 cm3. G-1.. The two kinds of activated carbons have strong adsorption properties. The experiment carried out 2 h for each batch, and the experiment carried out the 60 batch of three dimensional electrocatalytic oxidation device to achieve stability. By studying the effect of particle electrode, the removal rate of electrochemical degradation of aniline by GTSO as particle electrode was 85%, and the removal rate of GAC as particle electrode was 61%, but both were far higher than that of non particle electrodes. The removal rate of 21% in the two-dimensional electrolysis system was obtained. Thus, this paper finally determined that GTSO was used as a three-dimensional particle electrode to degrade aniline wastewater. (2) the optimization of the experimental conditions of aniline degradation by three-dimensional electrocatalysis was optimized. The factors such as electric field strength, electrolyte, pH, carbon water ratio and other factors were optimized by single factor method, and a group of optimal conditions were finally obtained for aniline. The experimental results show that the experimental conditions are electric field strength 1.2V/cm, electrolyte Na2SO4 0.03mol/L, pH 7, carbon water ratio 0.5, electrolysis 120 min electrolysis experiment can get the best effect. At this time, the removal rate of aniline and COD is 84.5% and 60.3%. (3) aniline electrochemical degradation pathway analysis. The experiment passed to the system. The analysis of nitrogen elements (ammonia nitrogen, nitrate nitrogen, nitrite state nitrogen), the determination of hydroxyl radical content, and the analysis of the composition of the electrolysis effluent by UV-Vis spectrophotometric method and GC-MS chromatography analysis, and finally determine the electrochemical oxidation pathway of aniline. The experimental results show that the ammonia nitrogen content in water is increased from 0 to 2 after electrolysis. 7.70mg/L, the nitrate nitrogen and nitrite nitrogen also increased from 0 to 2.30 mg/L and 0.15 mg/L respectively, while the total nitrogen content decreased from the original 126.10mg/L to 50.30mg/L., indicating that the effect of electrolysis did effectively degrade aniline. The comparison experiment with the addition of tert butyl alcohol and ethanol and other hydroxyl radical inhibitors was found to be used as an electrolysis. When the time was 30min, the removal rate of aniline was about 40% in the blank group, but the removal rate of aniline was only 20%. in the experimental group with the addition of TERT butanol in addition to the determination of OH in the system. When the electrolysis was 120 min, the absorbance of the effluent from 0 of the raw water to the 0.35. was fully proved. After electrolysis, the wastewater produced -OH By UV-Vis scanning and GC-MS analysis of the effluent, it is known that the degradation of aniline by electrolysis can produce quinones, phenols and carboxylic acids, and the production of eleven alkanes is detected at the same time. Therefore, the electrochemical degradation path of aniline is derived, which provides a certain reference for the follow-up study of aniline. Guide meaning.

【學(xué)位授予單位】：華東師范大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：X703

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