DBD等离子体—活性炭联用降解碱性品红的实验研究
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摘要
随着我国印染行业的快速发展,印染废水己经成为重点的水环境污染源之一,是水污染治理的重点和难点。开展对印染废水处理技术的研究正受到国内外有关专家的高度关注。
由于活性炭具有巨大的比表面积和化学稳定性等优点,活性炭吸附法一度成为人们研究的焦点,但随着对这种技术的深入研究发现：活性炭吸附法只是将污染物从一相转移到另一相,本质上并没有彻底去除污染物,而且活性炭需要再生,目前其再生方法又存在许多不足,从而限制了该技术的广泛应用。DBD(Dielectric Barrier Discharge)等离子体技术作为一种新兴的高级氧化技术,虽然在难降解废水处理中表现出极大的优势,但是存在设备复杂、能耗高的等问题,成为其工业化应用的瓶颈。针对这两种技术存在的问题,本论文将DBD等离子体技术与活性炭吸附相结合,应用于印染废水的降解,一方面,利用活性炭的吸附性能将污染物截留,延长污染物与活性粒子的接触时间,可提高DBD等离子体的降解效率；另一方面,随着活性炭上污染物的降解,活性炭同步得到再生。本论文主要研究结果如下：
(1)在相同放电电压、电源频率、初始浓度、pH值和循环流量的实验条件下,考查了活性炭吸附法、DBD等离子体处理法及DBD等离子体-活性炭联用三种处理方法对碱性品红的降解效果。结果表明：DBD等离子体-活性炭联用可大大提高碱性品红模拟印染废水的脱色率及COD去除率。
(2)考查了反应装置的工艺参数(如放电电压、电源频率等)、活性炭添加量及循环流量等因素对DBD等离子体-活性炭联用降解碱性品红的影响。结果表明：在电源频率f=-8kHz和10kHz的条件下,碱性品红的脱色率较好；碱性品红溶液在酸性和中性条件下的降解效果要优于碱性条件；循环流量过大或过小均不利于碱性品红的降解；碱性品红的脱色率基本随着活性炭添加量的增加而升高；碱性品红溶液初始浓度越高,脱色率越差。
(3)通过降解前后碱性品红的pH值、CODcr值及紫外光谱图的变化,可初步推断出碱性品红的降解机理,即在DBD等离子体产生的03、·OH等活性粒子作用下,碱性品红苯环结构首先发生羟基化,并进一步开环,然后再按照脂肪族有机物氧化途径逐步被氧化,最终矿化成CO2和H2O。
(4)通过改变不同的实验条件,考查了DBD等离子体再生后活性炭吸附等温线及吸附动力学的变化。结果表明,DBD等离子体再生后活性炭对碱性品红的吸附等温线略低于新活性炭,但对于饱和活性炭,其吸附能力有很大的提高；当U-d=8kV-6mm时,再生后活性炭吸附速率最接近于新活性炭,当U-d=9kV-8mm时,活性炭再生效果最差；在电源频率f=8kHz和10kHz的条件下再生后活性炭的吸附速率均高于f=9kHz;再生后活性炭吸附速率随着活性炭添加量的增大而减小,说明活性炭量越少,再生效果越好。
Along with the rapid development of the dyeing and printing industry, printing and dyeing wastewater has become the main pollution sources of the water, the treatment of which is the emphasis and difficulty of the water pollution treatment. Research on printing and dyeing wastewater treatment technology is being highly concerned by the domestic and foreign experts.
As the activated carbon with large specific surface area and chemical stability, active carbon absorption method has become the focus of research, but with in-depth study of this technology, the researchers found that:The method of Activated carbon adsorption only transfered the pollutants from one phase to another, in essence, did not completely remove the contaminants, and activated carbon regeneration is required, but now the regeneration methods have many disadvantages, thus limited the wide application of the technology. DBD (Dielectric Barrier Discharge) plasma technology is a new and advanced oxidation technology, although it showed great advantage in hard-degradation waste water processing, the need of complex equipment and high energy consumption become the bottleneck of its industrial application. In the view of these two kind of technical problems, this paper will combine the DBD plasma technology with activated carbon adsorption, used in the degradation of printing and dyeing wastewater, on one hand, the use of activated carbon adsorption can be extend the pollutants and active particles contact time and improve the degradation efficiency of DBD plasma; on the other hand, with the degradation of pollutants on the activated carbon, the activated carbon can be regenerated simultaneously. In this paper, the main results are as follows:
(1) At the same experimental conditions (discharge voltage, power frequency, initial concentration, pH and circulating flow), The experiment investigated the activated carbon adsorption method,DBD plasma method and DBD plasma-activated carbon treatment three different treatment methods on the degradation of fuchsin basic.The results showed that:DBD plasma-activated carbon treatment can greatly improve the decolorization rate and COD removal of basic fuchsin simulated dyeing wastewater.
(2) Examined reactor process parameters (such as discharge voltage, power frequency, etc), add the amount of activated carbon and recycle flow rate and other factors on DBD plasma-activated carbon degradation of basic fuchsin.The results showed that:in the power frequency f=8kHz and 10kHz conditions, can obtian a good decolorization rate; The degradation effect of Basic fuchsin solution under acidic and neutral conditions is superior to the alkaline conditions; Too large or too small recycle flow is not conducive to the degradation of basic fuchsin;The increase of the decolorization rate of Basic fuchsin basic is with the activated carbon dosage increase; Basic fuchsin solution initial concentration is higher, the decolorization rate is worse.
(3) Through the degradation of pH value, CODcr value and spectrum variation of fuchsin basic,can be inferred the degradation mechanism of Basic fuchsin, under the action of O3,·OH and other active particles generated in the DBD plasma, the hydroxylated benzene ring structure of basic fuchsin occurs first, and further open-loop, and then the organic matter was oxidized with fat family Organic oxidation way, eventually mineralized into CO2 and H2O.
(4) By varying the experimental conditions, investigate the change of DBD plasma regeneration of activated carbon adsorption isotherms and adsorption.The results showed that, DBD plasma regeneration of activated carbon on adsorption isotherms of Fuchsin Basic slightly below the new activated carbon, but for saturated activated carbon, adsorption capacity has greatly improved; As U-d=8KV-6mm, the adsorption rate of regenerated activated carbon is closest to the new activated carbon, As U-d=9KV-8mm, activated carbon regeneration effect is the worst; In the power frequency f=8kHz and 10kHz, the regenerated activated carbon adsorption rate is higher than the f=9kHz; the adsorption rate of regenerated activated carbon diminished with the added amount of carbon, indicated that the smaller use of activated carbon, the regeneration rate is better.
由于活性炭具有巨大的比表面积和化学稳定性等优点,活性炭吸附法一度成为人们研究的焦点,但随着对这种技术的深入研究发现：活性炭吸附法只是将污染物从一相转移到另一相,本质上并没有彻底去除污染物,而且活性炭需要再生,目前其再生方法又存在许多不足,从而限制了该技术的广泛应用。DBD(Dielectric Barrier Discharge)等离子体技术作为一种新兴的高级氧化技术,虽然在难降解废水处理中表现出极大的优势,但是存在设备复杂、能耗高的等问题,成为其工业化应用的瓶颈。针对这两种技术存在的问题,本论文将DBD等离子体技术与活性炭吸附相结合,应用于印染废水的降解,一方面,利用活性炭的吸附性能将污染物截留,延长污染物与活性粒子的接触时间,可提高DBD等离子体的降解效率；另一方面,随着活性炭上污染物的降解,活性炭同步得到再生。本论文主要研究结果如下：
(1)在相同放电电压、电源频率、初始浓度、pH值和循环流量的实验条件下,考查了活性炭吸附法、DBD等离子体处理法及DBD等离子体-活性炭联用三种处理方法对碱性品红的降解效果。结果表明：DBD等离子体-活性炭联用可大大提高碱性品红模拟印染废水的脱色率及COD去除率。
(2)考查了反应装置的工艺参数(如放电电压、电源频率等)、活性炭添加量及循环流量等因素对DBD等离子体-活性炭联用降解碱性品红的影响。结果表明：在电源频率f=-8kHz和10kHz的条件下,碱性品红的脱色率较好；碱性品红溶液在酸性和中性条件下的降解效果要优于碱性条件；循环流量过大或过小均不利于碱性品红的降解；碱性品红的脱色率基本随着活性炭添加量的增加而升高；碱性品红溶液初始浓度越高,脱色率越差。
(3)通过降解前后碱性品红的pH值、CODcr值及紫外光谱图的变化,可初步推断出碱性品红的降解机理,即在DBD等离子体产生的03、·OH等活性粒子作用下,碱性品红苯环结构首先发生羟基化,并进一步开环,然后再按照脂肪族有机物氧化途径逐步被氧化,最终矿化成CO2和H2O。
(4)通过改变不同的实验条件,考查了DBD等离子体再生后活性炭吸附等温线及吸附动力学的变化。结果表明,DBD等离子体再生后活性炭对碱性品红的吸附等温线略低于新活性炭,但对于饱和活性炭,其吸附能力有很大的提高；当U-d=8kV-6mm时,再生后活性炭吸附速率最接近于新活性炭,当U-d=9kV-8mm时,活性炭再生效果最差；在电源频率f=8kHz和10kHz的条件下再生后活性炭的吸附速率均高于f=9kHz;再生后活性炭吸附速率随着活性炭添加量的增大而减小,说明活性炭量越少,再生效果越好。
Along with the rapid development of the dyeing and printing industry, printing and dyeing wastewater has become the main pollution sources of the water, the treatment of which is the emphasis and difficulty of the water pollution treatment. Research on printing and dyeing wastewater treatment technology is being highly concerned by the domestic and foreign experts.
As the activated carbon with large specific surface area and chemical stability, active carbon absorption method has become the focus of research, but with in-depth study of this technology, the researchers found that:The method of Activated carbon adsorption only transfered the pollutants from one phase to another, in essence, did not completely remove the contaminants, and activated carbon regeneration is required, but now the regeneration methods have many disadvantages, thus limited the wide application of the technology. DBD (Dielectric Barrier Discharge) plasma technology is a new and advanced oxidation technology, although it showed great advantage in hard-degradation waste water processing, the need of complex equipment and high energy consumption become the bottleneck of its industrial application. In the view of these two kind of technical problems, this paper will combine the DBD plasma technology with activated carbon adsorption, used in the degradation of printing and dyeing wastewater, on one hand, the use of activated carbon adsorption can be extend the pollutants and active particles contact time and improve the degradation efficiency of DBD plasma; on the other hand, with the degradation of pollutants on the activated carbon, the activated carbon can be regenerated simultaneously. In this paper, the main results are as follows:
(1) At the same experimental conditions (discharge voltage, power frequency, initial concentration, pH and circulating flow), The experiment investigated the activated carbon adsorption method,DBD plasma method and DBD plasma-activated carbon treatment three different treatment methods on the degradation of fuchsin basic.The results showed that:DBD plasma-activated carbon treatment can greatly improve the decolorization rate and COD removal of basic fuchsin simulated dyeing wastewater.
(2) Examined reactor process parameters (such as discharge voltage, power frequency, etc), add the amount of activated carbon and recycle flow rate and other factors on DBD plasma-activated carbon degradation of basic fuchsin.The results showed that:in the power frequency f=8kHz and 10kHz conditions, can obtian a good decolorization rate; The degradation effect of Basic fuchsin solution under acidic and neutral conditions is superior to the alkaline conditions; Too large or too small recycle flow is not conducive to the degradation of basic fuchsin;The increase of the decolorization rate of Basic fuchsin basic is with the activated carbon dosage increase; Basic fuchsin solution initial concentration is higher, the decolorization rate is worse.
(3) Through the degradation of pH value, CODcr value and spectrum variation of fuchsin basic,can be inferred the degradation mechanism of Basic fuchsin, under the action of O3,·OH and other active particles generated in the DBD plasma, the hydroxylated benzene ring structure of basic fuchsin occurs first, and further open-loop, and then the organic matter was oxidized with fat family Organic oxidation way, eventually mineralized into CO2 and H2O.
(4) By varying the experimental conditions, investigate the change of DBD plasma regeneration of activated carbon adsorption isotherms and adsorption.The results showed that, DBD plasma regeneration of activated carbon on adsorption isotherms of Fuchsin Basic slightly below the new activated carbon, but for saturated activated carbon, adsorption capacity has greatly improved; As U-d=8KV-6mm, the adsorption rate of regenerated activated carbon is closest to the new activated carbon, As U-d=9KV-8mm, activated carbon regeneration effect is the worst; In the power frequency f=8kHz and 10kHz, the regenerated activated carbon adsorption rate is higher than the f=9kHz; the adsorption rate of regenerated activated carbon diminished with the added amount of carbon, indicated that the smaller use of activated carbon, the regeneration rate is better.
引文
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