超声电化学处理难降解有机物的工艺和机理研究
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摘要
由于难降解的有机化合物,用常规方法处理,往往经济耗费大,处理效果不佳。本实验选用超声电化学法处理难降解有机物,比较了单独超声波、电化学法和超声电化学法对氯苯、硝基苯和刚果红的降解能力,并结合紫外光谱分析刚果红的超声电化学降解历程和降解原理。实验证明,此方法是一种处理水中难降解有机物的有效方法。
第一部分研究了钯修饰钛电极的电化学性能。实验结果表明,钯修饰钛电极对氯苯和硝基苯等难降解有机物具有良好的电催化性能,与未修饰的钛电极相比,循环伏安过程都出现新的氧化峰和还原峰,反应过程峰电流明显增大。
第二部分考察了超声电化学参数对降解过程的影响,如超声波声强、槽电压、溶液初始pH值、处理时间和电解质的投量等。其中槽电压、处理时间和电解质投加量对超声电化学降解效果的影响较为显著,氯苯和硝基苯的表观反应速率随三个因素的增加迅速增大,而后趋于不变。酸性和碱性条件下超声电化学降解能力好于其他pH(超声电化学降解时最优槽电压为15伏,最优初始pH值为12,最佳处理时间60分钟,最优电解质投量为0.1mol/L。)。同时比较了单独超声波、电化学法和超声电化学法的降解结果。超声波几乎无降解效果;超声电化学相对于电化学,在电压15伏时氯苯和硝基苯CODCr去除效率分别提高1.2倍和2.2倍,处理60分钟后CODCr去除率达到75.02%和78.7%,而电化学使180分钟也无法达到这个效果,相同pH值条件下,CODCr去除率提高倍数约为1.7和2.0。
第三部分以刚果红为例,研究了超声电化学法对难降解有机物的超声电化学降解机理。实验结果表明,超声电化学对刚果红的降解效果很好,脱色率达到99.03%,CODCr去除率达到97.51%。紫外光谱分析表明刚果红经超声电化学降解作用下,逐渐完全降解成CO2和水。超声电化学技术有效处理废水的过程是声化学和电化学协同作用的结果,两者彼此影响和相互促进。
本文研究了一种基于超声和纳米电催化技术的超声电化学水处理方法。研究表明,超声电化学法对有机物特别是特种废水,如难降解有机物和持久性有机污染物(POPs)具有很好降解能力,在废水的深度处理领域具有很好的应用前景。
It is expensive and inefficient with the general method in refractory organics because of their particularity. A new method that sonoelectrochemical on the degradation of refractory organics by Pd modified Ti electrode was selected. Meanwhile, the degradation ability and effect factors of organics on the sonochemical, electrochemical or sonoelectrochemical were compared, and the degradation process and mechanism of refractory organic on the sonoelectrochemical was researched. Our experiments have proved that it is an effective method in the degradation of organics.
The first part of dissertation, we prepared the Pd modified Ti electrodes (Pd/Ti electrode) and studied it catalytic performance by cyclic voltammetry. The results showed that the Pd/Ti electrodes had better catalytic ability for chlorobenzene and nitrobenzene than pure Ti electrodes. Their cyclic voltammetries of Pd/Ti electrode all showed new reduction peak or oxidation peak, and the reduction and oxidation currents of reaction were significantly higher than pure Ti electrode.
The second part of dissertation, the effects of ultrasonic intensity, cell voltage, pH value, reaction time and the dosage of electrolyte etc on the sonoelectrochemical were studied. The cell voltage, reaction time and the dosage of electrolyte are the main effect parameters of sonoelectrochemical. The apparent reaction rate of chlorobezene and nitrobenzene increased with cell voltage, reaction time and the dosage of electrolyte, but it began to keep invariant after an especially numerical value. The degradation ability of sonoelectrochemical for chlorobenzene or nitrobenzene was better in acidic or alkaline than others pH value. The result of experiments showed that the best remove condition was cell voltage 15 V, pH value 12, reaction time 60 minute and electrolyte concentration 0.1 mol/L.
The CODCr removal rates of chlorobenzene and nitrobenzene wastewater on the sonochemical, electrochemical and sonoelectrochemical were compared. Although ultrasound could not produce signigicant chemical degradation for chlorobenzene and nitrobenzene, it greatly improved the electrochemical reaction rate. Comparing to electrochemical, the CODCr removal rates of chlorobenzene and nitrobenzene waste water are 1.2 times and 2.2 times when cell voltage is 15 V, and 1.7 times and 2 times when pH value is 12 on the sonoelectrochemical. Meanwhile, the CODCr removal rate got to 75.02% or 78.7% when reaction time is 60 minutes for sonoelectrochemical degradation process, but it could’t reach to this rate until to 180 minutes on the electrochemical degradation process.
The third part of dissertation, take congored as an example, we discussed the elementary degradation mechanism of refractory organics by sonoelectrochemical method. From experimental results, the degradation ability of sonoelectrochemical for Congo Red was very well. The decoloration rate reached 99.03% and the CODCr removal rate reached 97.51%. Through ultraviolet spectrum analysis, the Congo Red had been degraded to CO2 and water by sonoelectrochemical. Meanwhile, through analysis and research the experimental results, they showed that the elementary degradation mechanism of organics by sonoelectrochemical treatment is the synergistic effect of sonochemical and electrochemical, and they are mutual influence and improve.
In this dissertation, we studied an novel water treatment method: sonoelectro- chemical wastewater treatment. The results showd that sonoelectrochemical can degrade and remove organic very well, especially refractory organics and persistent organic pollutants. In the field of wastewater advanced treatment, the sonoelectro- chemical has an well application prospect.
第一部分研究了钯修饰钛电极的电化学性能。实验结果表明,钯修饰钛电极对氯苯和硝基苯等难降解有机物具有良好的电催化性能,与未修饰的钛电极相比,循环伏安过程都出现新的氧化峰和还原峰,反应过程峰电流明显增大。
第二部分考察了超声电化学参数对降解过程的影响,如超声波声强、槽电压、溶液初始pH值、处理时间和电解质的投量等。其中槽电压、处理时间和电解质投加量对超声电化学降解效果的影响较为显著,氯苯和硝基苯的表观反应速率随三个因素的增加迅速增大,而后趋于不变。酸性和碱性条件下超声电化学降解能力好于其他pH(超声电化学降解时最优槽电压为15伏,最优初始pH值为12,最佳处理时间60分钟,最优电解质投量为0.1mol/L。)。同时比较了单独超声波、电化学法和超声电化学法的降解结果。超声波几乎无降解效果;超声电化学相对于电化学,在电压15伏时氯苯和硝基苯CODCr去除效率分别提高1.2倍和2.2倍,处理60分钟后CODCr去除率达到75.02%和78.7%,而电化学使180分钟也无法达到这个效果,相同pH值条件下,CODCr去除率提高倍数约为1.7和2.0。
第三部分以刚果红为例,研究了超声电化学法对难降解有机物的超声电化学降解机理。实验结果表明,超声电化学对刚果红的降解效果很好,脱色率达到99.03%,CODCr去除率达到97.51%。紫外光谱分析表明刚果红经超声电化学降解作用下,逐渐完全降解成CO2和水。超声电化学技术有效处理废水的过程是声化学和电化学协同作用的结果,两者彼此影响和相互促进。
本文研究了一种基于超声和纳米电催化技术的超声电化学水处理方法。研究表明,超声电化学法对有机物特别是特种废水,如难降解有机物和持久性有机污染物(POPs)具有很好降解能力,在废水的深度处理领域具有很好的应用前景。
It is expensive and inefficient with the general method in refractory organics because of their particularity. A new method that sonoelectrochemical on the degradation of refractory organics by Pd modified Ti electrode was selected. Meanwhile, the degradation ability and effect factors of organics on the sonochemical, electrochemical or sonoelectrochemical were compared, and the degradation process and mechanism of refractory organic on the sonoelectrochemical was researched. Our experiments have proved that it is an effective method in the degradation of organics.
The first part of dissertation, we prepared the Pd modified Ti electrodes (Pd/Ti electrode) and studied it catalytic performance by cyclic voltammetry. The results showed that the Pd/Ti electrodes had better catalytic ability for chlorobenzene and nitrobenzene than pure Ti electrodes. Their cyclic voltammetries of Pd/Ti electrode all showed new reduction peak or oxidation peak, and the reduction and oxidation currents of reaction were significantly higher than pure Ti electrode.
The second part of dissertation, the effects of ultrasonic intensity, cell voltage, pH value, reaction time and the dosage of electrolyte etc on the sonoelectrochemical were studied. The cell voltage, reaction time and the dosage of electrolyte are the main effect parameters of sonoelectrochemical. The apparent reaction rate of chlorobezene and nitrobenzene increased with cell voltage, reaction time and the dosage of electrolyte, but it began to keep invariant after an especially numerical value. The degradation ability of sonoelectrochemical for chlorobenzene or nitrobenzene was better in acidic or alkaline than others pH value. The result of experiments showed that the best remove condition was cell voltage 15 V, pH value 12, reaction time 60 minute and electrolyte concentration 0.1 mol/L.
The CODCr removal rates of chlorobenzene and nitrobenzene wastewater on the sonochemical, electrochemical and sonoelectrochemical were compared. Although ultrasound could not produce signigicant chemical degradation for chlorobenzene and nitrobenzene, it greatly improved the electrochemical reaction rate. Comparing to electrochemical, the CODCr removal rates of chlorobenzene and nitrobenzene waste water are 1.2 times and 2.2 times when cell voltage is 15 V, and 1.7 times and 2 times when pH value is 12 on the sonoelectrochemical. Meanwhile, the CODCr removal rate got to 75.02% or 78.7% when reaction time is 60 minutes for sonoelectrochemical degradation process, but it could’t reach to this rate until to 180 minutes on the electrochemical degradation process.
The third part of dissertation, take congored as an example, we discussed the elementary degradation mechanism of refractory organics by sonoelectrochemical method. From experimental results, the degradation ability of sonoelectrochemical for Congo Red was very well. The decoloration rate reached 99.03% and the CODCr removal rate reached 97.51%. Through ultraviolet spectrum analysis, the Congo Red had been degraded to CO2 and water by sonoelectrochemical. Meanwhile, through analysis and research the experimental results, they showed that the elementary degradation mechanism of organics by sonoelectrochemical treatment is the synergistic effect of sonochemical and electrochemical, and they are mutual influence and improve.
In this dissertation, we studied an novel water treatment method: sonoelectro- chemical wastewater treatment. The results showd that sonoelectrochemical can degrade and remove organic very well, especially refractory organics and persistent organic pollutants. In the field of wastewater advanced treatment, the sonoelectro- chemical has an well application prospect.
引文
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