三维电极耦合铁碳微电解处理高浓度难降解有机废水
发布时间：2018-09-10 19:38
【摘要】：三维电极-铁碳微电解耦合法是一种新型洁净的高级电化学氧化法。本课题通过三维电极-铁碳微电解耦合法对一种实际高浓度难降解废水进行实验研究。论文通过单因素实验,从电极板材料、填料电极材料、反应时间、极板间距、外电压、初始pH等影响因素分析对处理效果的影响,得出本三维电极-铁碳微电解耦合法实验装置各影响因素的优化条件范围;通过正交实验,进一步对单因素实验得出的优化条件进行深层次的细化组合研究,通过对比对COD、NH3-N、B/C以及其中难降解有机物2,3-二氯吡啶(特征污染物)的处理效果,得出最佳实验条件:阳极不锈钢板、阴极石墨板、填料使用铁碳烧结小球填料、反应时间2.5h、极板间距D=6cm、外加电压10V、初始pH=5;通过对比单独电解、单独微电解以及三维电极耦合铁碳微电解反应处理效果,三维电极耦合铁碳微电解对于COD的处理效果比电解增加了20%,比微电解增加了将近2倍,对于NH3-N的处理效果也要明显优于其它两者,证明了耦合方法的优越性;通过对比反应器在相同反应条件下对不同浓度范围废水的处理效果,探究方法对水处理对象高浓度难降解废水的适用性:原水浓度越高去除效果越好,随着原水浓度降低去除率也随之降低。COD10000时去除率在80%以上;通过对填料消耗产生底泥的回收再反应判断填料消耗再利用的价值:虽然不及装填铁碳烧结填料小球时的处理效果,但相比于一般常用处理方法的效果而言仍较好,具有一定的利用回收价值。本三维电极-铁碳微电解耦合方法装置的电流效率:电流密度J=196.36A/m2,法拉第电流效率η%=232.93%,时空产率=5.25kgCOD/h·m3;动力学分析拟合COD浓度与时间关系,并不完全属于动力学零级或一级反应,而是与反应时间呈三项式关系,相关系数R2为0.99797;污染物COD和NH3-N的氧化机理推测;铁碳烧结填料小球反应前后的形貌结构SEM观察对比,一段时间反复使用后填料内部的空间结构仍然比较紧密,没有出现明显的松散,整体孔隙率仍然高;以及对反应前后填料进行XDS元素能谱分析,经过一段反应时间后的铁碳填料比未使用前增加了Ca、Al、Cu三种新的金属元素;反应过程中对羟基自由基·OH进行了测定,·OH浓度随反应时间逐渐增大,大约在90min后达到平衡;以及金属铜离子和金属铁离子的催化作用分析和反应中絮凝沉淀过程的作用分析,完整阐明了整个三维电极-铁碳微电解耦合方法的反应过程和反应机理。实验结果表明,三维电极-铁碳微电解耦合方法对于高浓度难降解有机废水具有良好的处理效果,对于COD10000的难降解有机废水COD的去除率可达80%以上,对于NH3-N在100-200的难降解有机废水NH3-N的去除率可达60%以上,反应高效快速,不需要额外投加任何试剂,因而具有进一步研究及应用的价值。
[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.
【学位授予单位】：南昌大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：X703
[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.
【学位授予单位】：南昌大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：X703
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