【摘要】：三維電極-鐵碳微電解耦合法是一種新型潔凈的高級電化學氧化法。本課題通過三維電極-鐵碳微電解耦合法對一種實際高濃度難降解廢水進行實驗研究。論文通過單因素實驗,從電極板材料、填料電極材料、反應時間、極板間距、外電壓、初始pH等影響因素分析對處理效果的影響,得出本三維電極-鐵碳微電解耦合法實驗裝置各影響因素的優(yōu)化條件范圍;通過正交實驗,進一步對單因素實驗得出的優(yōu)化條件進行深層次的細化組合研究,通過對比對COD、NH3-N、B/C以及其中難降解有機物2,3-二氯吡啶(特征污染物)的處理效果,得出最佳實驗條件:陽極不銹鋼板、陰極石墨板、填料使用鐵碳燒結(jié)小球填料、反應時間2.5h、極板間距D=6cm、外加電壓10V、初始pH=5;通過對比單獨電解、單獨微電解以及三維電極耦合鐵碳微電解反應處理效果,三維電極耦合鐵碳微電解對于COD的處理效果比電解增加了20%,比微電解增加了將近2倍,對于NH3-N的處理效果也要明顯優(yōu)于其它兩者,證明了耦合方法的優(yōu)越性;通過對比反應器在相同反應條件下對不同濃度范圍廢水的處理效果,探究方法對水處理對象高濃度難降解廢水的適用性:原水濃度越高去除效果越好,隨著原水濃度降低去除率也隨之降低。COD10000時去除率在80%以上;通過對填料消耗產(chǎn)生底泥的回收再反應判斷填料消耗再利用的價值:雖然不及裝填鐵碳燒結(jié)填料小球時的處理效果,但相比于一般常用處理方法的效果而言仍較好,具有一定的利用回收價值。本三維電極-鐵碳微電解耦合方法裝置的電流效率:電流密度J=196.36A/m2,法拉第電流效率η%=232.93%,時空產(chǎn)率=5.25kgCOD/h·m3;動力學分析擬合COD濃度與時間關系,并不完全屬于動力學零級或一級反應,而是與反應時間呈三項式關系,相關系數(shù)R2為0.99797;污染物COD和NH3-N的氧化機理推測;鐵碳燒結(jié)填料小球反應前后的形貌結(jié)構SEM觀察對比,一段時間反復使用后填料內(nèi)部的空間結(jié)構仍然比較緊密,沒有出現(xiàn)明顯的松散,整體孔隙率仍然高;以及對反應前后填料進行XDS元素能譜分析,經(jīng)過一段反應時間后的鐵碳填料比未使用前增加了Ca、Al、Cu三種新的金屬元素;反應過程中對羥基自由基·OH進行了測定,·OH濃度隨反應時間逐漸增大,大約在90min后達到平衡;以及金屬銅離子和金屬鐵離子的催化作用分析和反應中絮凝沉淀過程的作用分析,完整闡明了整個三維電極-鐵碳微電解耦合方法的反應過程和反應機理。實驗結(jié)果表明,三維電極-鐵碳微電解耦合方法對于高濃度難降解有機廢水具有良好的處理效果,對于COD10000的難降解有機廢水COD的去除率可達80%以上,對于NH3-N在100-200的難降解有機廢水NH3-N的去除率可達60%以上,反應高效快速,不需要額外投加任何試劑,因而具有進一步研究及應用的價值。
[Abstract]:Three-dimensional electrode-iron-carbon microelectrolysis is a new clean advanced electrochemical oxidation method. In this paper, a practical high concentration refractory wastewater was studied by three-dimensional electrode-iron-carbon microelectrolysis coupling method. In this paper, the influence factors of electrode plate material, filler electrode material, reaction time, plate distance, external voltage, initial pH and so on are analyzed by single factor experiment. The optimum conditions of the three dimensional electrode and iron carbon microelectrolysis coupling device are obtained, and the optimized conditions of single factor experiment are further studied by orthogonal experiment. By comparing the treatment effect of COD,NH3-N,B/C and the non-degradable organic matter 2C 3-dichloropyridine (characteristic pollutant), the optimum experimental conditions were obtained: anode stainless steel plate, cathode graphite plate, and iron carbon sintered pellet filler. When the reaction time is 2.5 h, the electrode spacing is 6 cm, the applied voltage is 10 V, the treatment effect of initial pH=5; is compared with that of single electrolysis, single microelectrolysis and three dimensional electrode coupled iron-carbon microelectrolysis. Three-dimensional electrode coupled iron-carbon microelectrolysis is 20 times more effective than electrolysis in treating COD and nearly 2 times higher than that in micro-electrolysis. The treatment effect of NH3-N is obviously better than that of the other two, which proves the superiority of the coupling method. By comparing the treatment effect of the reactor on wastewater of different concentration range under the same reaction conditions, the applicability of the method to the high concentration refractory wastewater of the water treatment object is explored: the higher the raw water concentration, the better the removal effect. With the decrease of raw water concentration, the removal rate is more than 80% when the concentration of raw water is reduced. COD10000. The value of reutilization of filler consumption is judged by the recovery and rereaction of sediment produced by packing consumption: although it is not as effective as the treatment effect when filling iron carbon sintered filler pellets, But compared with the common treatment methods, the effect is still better, and has a certain value of utilization and recovery. The current efficiency of the three-dimension electrode-iron / carbon microelectrolysis system is as follows: current density J _ (196.36) A / m ~ (2), Faraday current efficiency 畏 ~ (232.93), space-time yield 5.25 kg COD / h ~ (-3). The kinetic analysis fits the relationship between COD concentration and time and does not belong to the zero order or first order reaction of kinetics. There was a trinomial relationship between reaction time and reaction time, the correlation coefficient R2 was 0.997977.The oxidation mechanism of pollutants COD and NH3-N was inferred. The morphology and structure SEM of iron carbon sintered pellets before and after reaction were observed and compared. After repeated use for a period of time, the space structure inside the packing is still relatively close, there is no obvious looseness, the overall porosity is still high, and the energy spectrum analysis of XDS elements is carried out on the packing before and after the reaction. Three new metal elements of Ca,Al,Cu were added to the iron-carbon filler after a period of reaction time, the hydroxyl radical OH was determined during the reaction, and the concentration of OH gradually increased with the reaction time and reached equilibrium after 90min. The catalytic action of copper ion and iron ion and the effect of flocculation and precipitation in the reaction were analyzed. The reaction process and reaction mechanism of the three dimensional electrode-iron / carbon microelectrolysis coupling method were fully explained. The experimental results show that the coupling method of three-dimensional electrode and iron-carbon microelectrolysis has a good effect on the treatment of high concentration refractory organic wastewater, and the removal rate of COD for the refractory organic wastewater of COD10000 can reach more than 80%. The removal rate of NH3-N from refractory organic wastewater with NH3-N in 100-200 can reach more than 60%, the reaction is efficient and fast, and no additional reagent is needed, so it has the value of further research and application.
【學位授予單位】：南昌大學
【學位級別】：碩士
【學位授予年份】：2017
【分類號】：X703

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