渗流式纳米电极电化学反应器处理染料废水研究
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摘要
电化学方法处理有机物由于其没有二次污染和易于控制等优点受到广泛关注,但是由于传质、副反应以及电极消耗等问题,使其运行费用较高。其中传质问题在很多情况下是电化学反应的主要限制因素。目前,对传质的改进办法大都是通过机械搅拌和电极转动等。这些方法虽然对改进溶液间的物质传递有较大的改进,但是对电极表面的传质速率的改进却十分有限。
本课题设计了渗流式纳米电极电化学反应器,通过污染物通过电极时与电极之间的相互作用减小电极表面的传质阻力,从而提高传质效率。本论文以两种模拟染料废水为处理对象对渗流式反应器进行了考察,结果证明通过渗流式的方法确实能较大地提高电化学反应的速率和效率,降低能耗,对电化学方法的广泛应用有很好的借鉴作用。本论文的主要
主要研究工作可以归纳如下:
1.制备了渗流式纳米电极电化学反应器,使反应溶液从电极间穿过,利用穿过时与电极的相互作用减小电极表面的传质阻力。同时,以碳纳米管结合活性炭纤维作为电极,利用其巨大的比表面积和高的催化活性。
2.使用渗流式电化学反应器处理活性艳红X-3B模拟染料废水。当电压为10V,初始pH为中性时,加入3g/L的Na2SO4时,在100 min内X-3B的脱色率达到90%以上,COD去除率达到57.5%。同时,该方法在较大浓度范围(0-200 mg/L)内对X-3B均能达到较好的去除。紫外扫描测定发现X-3B得到了较彻底的降解。在最优实验条件下计算得传质系数在60 min时达到最大值,为1.87×10-3 cm/s。与传统电化学方法进行了对比,传质系数有很大的提高。同时,45 min后反应达到稳定的电流效率,为33.06%,单位能耗为101.34 kWh/kg COD。
3.渗流式电化学反应器处理活性艳蓝X-BR模拟染料废水。当电压为8V,初始pH为2,加入1 g/L的Na2SO4时装置对活性艳蓝的处理效果最佳,脱色率可以达到90%以上,90 min后COD去除率达到51%。在0-500 mg/L浓度范围内的活性艳蓝均能达到很好的去除效率。紫外扫描测试证明,染料分子得到较彻底的破坏。同时,计算得传质系数在15 min时达到最大值1.70×10-3 cm/s,电流效率由15 min时的46.3%降至90 min后的29.3%,同时单位能耗也由57.9 kWh/kg COD提高到91.3 kWh/kg COD。
4.以处理活性艳红为例,对渗流式电化学反应器的电化学过程进行了反应动力学研究,结果显示该反应过程较好的遵循一级反应动力学。
The application of electrochemical techniques in organic wastewater treatment has drawn considerable attention in the last few years, since the electrolytic process is easy to control by potential and current, and such process can operate at low temperature and pressure without adding other reagents. Though electrochemical technique has many advantages, it isn’t widely applied in the wastewater treatment because of its limitations, essentially the high cost and low current efficiency caused mainly by low contaminants mass transfer from water to the electrode surface, secondary reaction and electrode consumption et al. Previous research shows that although the destruction of organic compounds by electrochemical treatment is achieved by oxidation, which can occur directly at the anode and/or indirectly by species (e.g. O?, OH? and O3) generated by the anode, the reaction rates are actually limited by the contaminants diffusion in the external liquid film on electrode surface and in the internal pores. Therefore, contaminants oxidation is controlled by the rate at which organic molecules are carried from the bulk solution to the electrode surface, rather than by the rate at which electrons are delivered to the anode. Reviewing literature, it is fair to say that so far most of the studies carried out on the electrochemical treatment pertain to the experimental conditions, with primary objective of these studies being the development of appropriate parameters for pollutants removal. Although mass transfer has been noticed phenomenally by limited researchers, the work is mainly focused on increasing the contaminants movement in bulk solution or reducing the external liquid film thickness by mechanical stirring. There is a deficiency in the fundamental problem of electrochemical efficiency related to pollutants diffusion in the liquid film.
An original reactor with seepage electrode made of CNTs has been developed and successfully applied to degrade organics with much higher Current Efficient (CE) and lower Energy Consumption (EC), which let the contaminants go through the electrodes. The reason to employ CNTs is that they are very interesting nano-materials known to exhibit superior and unique electron transfer (ET). The possibility of CNTs utilization for organic oxidation has already been demonstrated, because CNTs electrodes have an extended surface area that promises to provide an additional advantage for chemicals to react. The main contents of this research work can be summarized as follows:
1. Seepage Carbon Nano-tube Electrode (SCNE) Reactor was designed in order to facilitate contaminants mass transfer from the bulk solution to the electrode surface. The innovative concepts behind the reactor design is that the overall mass transfer would be significantly improved while the pollutants seeping through the porous Carbon Nano-tubes (CNTs) electrode. Two kind of SCNE with different electrode combination have been studied.
2. SCNE Reactor treated reactive brilliant red X-3B simulated dye wastewater. The reactor devices used carbon nanotubes-activated carbon fiber electrode as its cathode and anode. The experiment results shows that the optimized conditions for X-3B degradation was potential 10V, initial pH of 7, 3 g/L of Na2SO4. Under this condition, the color removal ratio of X-3B could reach more than 90% within 100 min, which COD removal was more than 57.5%. The results also found that the structure of X-3B had been well degraded. The calculated mass transfer coefficient was improved by 116.01-160.74% compared with conventional electrochemical reactors under same conditions. Further research shows that the Current Efficiency (CE) of the SCNE Reactor is 340.21-519.10% higher than that of the conventional reactors and the Energy Consumption (EC) to mineralize same amount of organics is only 16.51-22.31% of the compared ones.
3. SCNE Reactor treated reactive brilliant blue X-BR simulated dye wastewater. In this study, the reactor using carbon nanotubes electrode as the anode, copper electrode as the cathode. It was found that the condition with potential of 8V, the initial pH of 2, 1 g/L of Na2SO4 was the best condition for degradation of X-BR. And the color removal ratio and COD removal could reach 90% and 51% respectively within 100 min. The reactor can achieve good removal efficiency (70% within 100 min) even when the concentration of X-BR reached 500 mg/L. UV scanning and gas chromatography mass spectrometry test proved that the X-BR molecules have been damaged completely. At the same time, based on the degradation of COD, the mass transfer coefficient 15min when the maximum 1.70×10-3cm/s, current efficiency declined of from 46.3% (15min) to 29.3% (90min), the energy consumption increased from 57.9 kWh / kg COD to 91.3 kWh / kg COD.
4. The results of reaction kinetics showed that the electrochemical process followed the first order reaction kinetics, which was based on the experimental of degradation of X-3B.
本课题设计了渗流式纳米电极电化学反应器,通过污染物通过电极时与电极之间的相互作用减小电极表面的传质阻力,从而提高传质效率。本论文以两种模拟染料废水为处理对象对渗流式反应器进行了考察,结果证明通过渗流式的方法确实能较大地提高电化学反应的速率和效率,降低能耗,对电化学方法的广泛应用有很好的借鉴作用。本论文的主要
主要研究工作可以归纳如下:
1.制备了渗流式纳米电极电化学反应器,使反应溶液从电极间穿过,利用穿过时与电极的相互作用减小电极表面的传质阻力。同时,以碳纳米管结合活性炭纤维作为电极,利用其巨大的比表面积和高的催化活性。
2.使用渗流式电化学反应器处理活性艳红X-3B模拟染料废水。当电压为10V,初始pH为中性时,加入3g/L的Na2SO4时,在100 min内X-3B的脱色率达到90%以上,COD去除率达到57.5%。同时,该方法在较大浓度范围(0-200 mg/L)内对X-3B均能达到较好的去除。紫外扫描测定发现X-3B得到了较彻底的降解。在最优实验条件下计算得传质系数在60 min时达到最大值,为1.87×10-3 cm/s。与传统电化学方法进行了对比,传质系数有很大的提高。同时,45 min后反应达到稳定的电流效率,为33.06%,单位能耗为101.34 kWh/kg COD。
3.渗流式电化学反应器处理活性艳蓝X-BR模拟染料废水。当电压为8V,初始pH为2,加入1 g/L的Na2SO4时装置对活性艳蓝的处理效果最佳,脱色率可以达到90%以上,90 min后COD去除率达到51%。在0-500 mg/L浓度范围内的活性艳蓝均能达到很好的去除效率。紫外扫描测试证明,染料分子得到较彻底的破坏。同时,计算得传质系数在15 min时达到最大值1.70×10-3 cm/s,电流效率由15 min时的46.3%降至90 min后的29.3%,同时单位能耗也由57.9 kWh/kg COD提高到91.3 kWh/kg COD。
4.以处理活性艳红为例,对渗流式电化学反应器的电化学过程进行了反应动力学研究,结果显示该反应过程较好的遵循一级反应动力学。
The application of electrochemical techniques in organic wastewater treatment has drawn considerable attention in the last few years, since the electrolytic process is easy to control by potential and current, and such process can operate at low temperature and pressure without adding other reagents. Though electrochemical technique has many advantages, it isn’t widely applied in the wastewater treatment because of its limitations, essentially the high cost and low current efficiency caused mainly by low contaminants mass transfer from water to the electrode surface, secondary reaction and electrode consumption et al. Previous research shows that although the destruction of organic compounds by electrochemical treatment is achieved by oxidation, which can occur directly at the anode and/or indirectly by species (e.g. O?, OH? and O3) generated by the anode, the reaction rates are actually limited by the contaminants diffusion in the external liquid film on electrode surface and in the internal pores. Therefore, contaminants oxidation is controlled by the rate at which organic molecules are carried from the bulk solution to the electrode surface, rather than by the rate at which electrons are delivered to the anode. Reviewing literature, it is fair to say that so far most of the studies carried out on the electrochemical treatment pertain to the experimental conditions, with primary objective of these studies being the development of appropriate parameters for pollutants removal. Although mass transfer has been noticed phenomenally by limited researchers, the work is mainly focused on increasing the contaminants movement in bulk solution or reducing the external liquid film thickness by mechanical stirring. There is a deficiency in the fundamental problem of electrochemical efficiency related to pollutants diffusion in the liquid film.
An original reactor with seepage electrode made of CNTs has been developed and successfully applied to degrade organics with much higher Current Efficient (CE) and lower Energy Consumption (EC), which let the contaminants go through the electrodes. The reason to employ CNTs is that they are very interesting nano-materials known to exhibit superior and unique electron transfer (ET). The possibility of CNTs utilization for organic oxidation has already been demonstrated, because CNTs electrodes have an extended surface area that promises to provide an additional advantage for chemicals to react. The main contents of this research work can be summarized as follows:
1. Seepage Carbon Nano-tube Electrode (SCNE) Reactor was designed in order to facilitate contaminants mass transfer from the bulk solution to the electrode surface. The innovative concepts behind the reactor design is that the overall mass transfer would be significantly improved while the pollutants seeping through the porous Carbon Nano-tubes (CNTs) electrode. Two kind of SCNE with different electrode combination have been studied.
2. SCNE Reactor treated reactive brilliant red X-3B simulated dye wastewater. The reactor devices used carbon nanotubes-activated carbon fiber electrode as its cathode and anode. The experiment results shows that the optimized conditions for X-3B degradation was potential 10V, initial pH of 7, 3 g/L of Na2SO4. Under this condition, the color removal ratio of X-3B could reach more than 90% within 100 min, which COD removal was more than 57.5%. The results also found that the structure of X-3B had been well degraded. The calculated mass transfer coefficient was improved by 116.01-160.74% compared with conventional electrochemical reactors under same conditions. Further research shows that the Current Efficiency (CE) of the SCNE Reactor is 340.21-519.10% higher than that of the conventional reactors and the Energy Consumption (EC) to mineralize same amount of organics is only 16.51-22.31% of the compared ones.
3. SCNE Reactor treated reactive brilliant blue X-BR simulated dye wastewater. In this study, the reactor using carbon nanotubes electrode as the anode, copper electrode as the cathode. It was found that the condition with potential of 8V, the initial pH of 2, 1 g/L of Na2SO4 was the best condition for degradation of X-BR. And the color removal ratio and COD removal could reach 90% and 51% respectively within 100 min. The reactor can achieve good removal efficiency (70% within 100 min) even when the concentration of X-BR reached 500 mg/L. UV scanning and gas chromatography mass spectrometry test proved that the X-BR molecules have been damaged completely. At the same time, based on the degradation of COD, the mass transfer coefficient 15min when the maximum 1.70×10-3cm/s, current efficiency declined of from 46.3% (15min) to 29.3% (90min), the energy consumption increased from 57.9 kWh / kg COD to 91.3 kWh / kg COD.
4. The results of reaction kinetics showed that the electrochemical process followed the first order reaction kinetics, which was based on the experimental of degradation of X-3B.
引文
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