活性炭协同接地极雾化电晕放电特性及预处理采油废水的研究
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摘要
接地极雾化电晕放电技术是一项环境友好型污水处理技术，它处理效率高、反应速度快、不造成二次污染，是值得关注的一项环境治理工艺。本文研究了接地极雾化电晕放电单独作用时和协同活性炭情况下放电特征和对采油废水的预处理效果。本课题涉及到的研究内容和获得的研究结论如下：
1.将雾化放电和电晕放电有机结合在一起，设计了一种新型反应器。放电等离子体的活性物种的存在时间很短，以羟基自由基为例，仅为10-7s。而传统的放电方法并不能使等离子区和反应区相互分离，所以减少了活性物种与污染物的反应时间。该反应器放电等离子区与反应区同步，使放电过程所生成的活性物种能够更有效、充分地作用于水中污染物。同时，在强静电场力和表面张力的作用下，待处理水被雾化成小液滴，从放电反应空间通过，实现了能量的高效利用。
2.为寻求出最佳放电条件提供依据，正负电晕放电、极间距离、流量对于接地极雾化电晕放电的影响进行了研究。研究表明，接地极雾化负电晕放电的放电电流大于接地极雾化正电晕放电的放电电流，更高于传统的电晕放电电流。主要原因是雾化电晕放电中线电极表面形成的泰勒锥缩短了两极之间的距离，另外，形成的泰勒锥的曲率半径也可能促进放电电流的增加。
3.接地极雾化电晕放电放电机理表明：线电极和板电极之间形成了非匀强电场，线电极表面的电场强度最大，当电压超过起晕电压时将在线电极附近形成电晕区，发生放电。并且，覆盖在线电极表面上的水流在强电场力作用下，形成电流体效应，产生液体静电喷雾作用，小液滴会在放电极间发生雾化放电现象。较小的带电液滴在运动的过程中，形成的多锥射流在一定程度上有和较大液滴形成的多锥射流交叉的可能，所以这样的放电形式更有利于形成较为均匀的等离子区，提高其对废水的作用效果。
4.以放电特性为依据，选择了适当的电极间距和电压对高浓度采油废水进行了预处理，并测量了反应前后的BOD、COD、浊度及pH值的变化。接地极雾化电晕放电对采油废水的预处理效果研究表明，接地极雾化电晕放电预处理采油废水可有效提高其可生化性。采油废水可生化性初始值0.079，经处理后上升到0.5以上。COD去除率可达79.64%。
5.活性炭对于放电电流的影响研究表明：活性炭的应用并未使接地极雾化电晕放电电流发生变化，主要原因是活性炭被润湿后和板电极之间形成了良好的导通，从而保证了有无活性炭的情况下，两极之间的距离没有发生变化，所以放电强度没有变化。
6.活性炭协同作用下对采油废水的预处理处理效果表明：活性炭层与接地极雾化电晕放电协同作用后，使采油废水的浊度明显低于无活性炭层时接地极雾化电晕放电处理后的采油废水。同时，活性炭协同作用时，整个处理过程BOD、COD的值均小于无活性炭层时接地极雾化电晕放电处理废水所对应的BOD、COD的值。分析原因活性炭能引发臭氧自由基型链反应，加速臭氧分解生成羟基自由基。而且活性炭层越厚，处理过程中对应的BOD、COD的值越小，说明活性炭越厚时，越有利于污染物的去除，与接地极雾化放电所形成的等离子体产生的协同作用越为明显。
7.不同流量下对于处理结果的影响研究表明，无论是否存在活性炭层，整体来看，流量的增加对降低废水浊度、BOD、COD均产生不利影响。分析原因是流量的增加使放电电流减小，降低了活性物质的产生。故而，反应速率减慢。当电压为13kv，线电极和活性炭层之间的距离为2.5cm，在流量为50ml/min，活性炭厚度为5mm时，处理效果最为理想。
Earthed atomizing corona discharge is an environmental-friendly technology to treatwaste water. This environmental management technology is notable for its high treatmentefficiency, fast reaction and freedom from secondary pollution. This paper studies thecharacteristics of earthed atomizing corona discharge when it is used alone and when it issynergized with activated carbon, as well as their effects of pre-treating of oilfield producedwater. The research contents, results and conclusions are as follows:
1. Corona discharges and atomizing discharges were combined effectively, and anew-style reactor was designed. Active species of discharge plasma exist for quite a short time.Take OH as an example, it only presents for10-7S. Traditional discharge methods are not ableto synchronise the plasma zone and reaction zone completely, so the reaction time betweenactive species and pollutants is cut down. Research indicates that earthed atomizing coronadischarge forms synchronised plasma zones and atomizing liquid drops, as well as theuniform plasma zones, and active species produced by the discharge are able to interact withwaste water from oil extraction directly. Simultaneously, the water to be treated, under theaction of strong electrostatic field force and surface tension, is atomized to small liquid dropsthat pass through the discharge reaction space. The atomizing effect enlarges the reaction areabetween the water and the plasma zone. Thus, compared with other discharge treatmentpatterns, this method can transform the waste water form oil extraction to be biochemicallytreatable with relatively lower energy and realise a higher utilisation rate of energy.
2. To provide a basis for the best discharge conditions, the influences of positive/negativeatomizing corona, inter-electrode distance and flux on the earthed atomizing corona dischargeare researched. According to the research finding, on the condition of the same dischargesituation, the discharge current of a negative earthed atomizing corona is greater than that of apositive earthed atomizing corona and exceeds that of a traditional corona even more. Themain reason is that a Taylor Cone formed on the surface of a line electrode during theatomizing corona discharge shortened the inter-electrode distance. Also, there is a possibilitythat the curvature radius of the Taylor Cone will facilitate the aggrandising of the dischargecurrent.
3. In the research, the discharge mechanism of earthed atomizing corona discharge isanalyzed. The research suggests that: a non-uniform electric field is formed between the lineelectrode and the plate electrodes. The highest electric field intensity exists on the surface ofthe line electrode. When the voltage exceeds the onset voltage, a corona zone is formedaround the line electrode and discharges. At the same time, the water flow that covers the surface of the line electrode produces an electric fluid effect under the action of strong electrostatic field force and further acts as a liquid electrostatic spray. The atomized small liquiddrops will discharge in the discharge electrodes. Multiple cone-shaped fluxes formed whensmall electric liquid drops move will, to some extent, be quite likely to make a crossover withthose created by large liquid drops, so this discharge form would be more beneficial forcreating relatively even plasma zone to enhance its effect on waste water.
4. According to I-V characteristics of earthed atomizing corona discharge, appropriateinter-electrode distance and voltage are selected to carry out advanced oxidation treatment onhigh concentration waste water from oil extraction while BOD5, COD, turbidity and pHbefore and after reaction are measured. The study indicates that when consuming little energy,earthed atomizing corona discharge to turns out to be effective on augmenting thebiodegradability of waste water from oil extraction.
The initial value of biodegradability of oilfield produced water was0.079and later roseto over0.5after the treatment. And COD removal rate reached79.64%.
5. The research on activated carbon’s influence on the discharge current suggests that theinvolvement of activated carbon does not cause any change in the current of earthedatomizing corona discharge. The main reason is that a good conduction formed between theactivated carbon and the plate electrodes after the activated carbon is soaked ensures thatthere is no change in the inter-electrode distance with or without activated carbon. As a result,the discharge intensity is unchanged.
6. The research on the effect of pre-treating oilfield produced water with the synergy ofearthed atomizing corona discharge and activated carbon suggests that after the earthedatomizing corona discharge and the activated carbon are synergized, the turbidity of theoilfield produced water is significantly lower than the turbidity of the oilfield produced watertreated by earthed atomizing corona discharge without activated carbon. At the same time,BOD and COD of the oilfield produced water during the pre-treating are both lower thanthose without activated carbon. The reason is that the activated carbon causes ozone freeradical chain reaction which further accelerates the decomposition of ozone into hydroxylradical. The thicker the activated carbon layer, the lower BOD and COD are. This indicatesthat a thicker activated carbon layer is more helpful in removing pollutants and shows moresignificant synergy with the plasma from the earthed atomizing corona discharge.
7. The research on the influences of different water flux on the treatment effect suggeststhat with or without activated carbon, the increase in water flux has a negative influence onlowering the turbidity, BOD and COD of the oilfield produced water. The reason is that theincreased flux reduces the discharge current and thus reduces the generation of active species.As a result, the reaction rate is lowered. When the voltage is13kv, the distance between the line electrode and the activated carbon is2.5cm; when the flux is50ml/min and the thicknessof the activated carbon is5mm, the treatment effect is the best.
1.将雾化放电和电晕放电有机结合在一起，设计了一种新型反应器。放电等离子体的活性物种的存在时间很短，以羟基自由基为例，仅为10-7s。而传统的放电方法并不能使等离子区和反应区相互分离，所以减少了活性物种与污染物的反应时间。该反应器放电等离子区与反应区同步，使放电过程所生成的活性物种能够更有效、充分地作用于水中污染物。同时，在强静电场力和表面张力的作用下，待处理水被雾化成小液滴，从放电反应空间通过，实现了能量的高效利用。
2.为寻求出最佳放电条件提供依据，正负电晕放电、极间距离、流量对于接地极雾化电晕放电的影响进行了研究。研究表明，接地极雾化负电晕放电的放电电流大于接地极雾化正电晕放电的放电电流，更高于传统的电晕放电电流。主要原因是雾化电晕放电中线电极表面形成的泰勒锥缩短了两极之间的距离，另外，形成的泰勒锥的曲率半径也可能促进放电电流的增加。
3.接地极雾化电晕放电放电机理表明：线电极和板电极之间形成了非匀强电场，线电极表面的电场强度最大，当电压超过起晕电压时将在线电极附近形成电晕区，发生放电。并且，覆盖在线电极表面上的水流在强电场力作用下，形成电流体效应，产生液体静电喷雾作用，小液滴会在放电极间发生雾化放电现象。较小的带电液滴在运动的过程中，形成的多锥射流在一定程度上有和较大液滴形成的多锥射流交叉的可能，所以这样的放电形式更有利于形成较为均匀的等离子区，提高其对废水的作用效果。
4.以放电特性为依据，选择了适当的电极间距和电压对高浓度采油废水进行了预处理，并测量了反应前后的BOD、COD、浊度及pH值的变化。接地极雾化电晕放电对采油废水的预处理效果研究表明，接地极雾化电晕放电预处理采油废水可有效提高其可生化性。采油废水可生化性初始值0.079，经处理后上升到0.5以上。COD去除率可达79.64%。
5.活性炭对于放电电流的影响研究表明：活性炭的应用并未使接地极雾化电晕放电电流发生变化，主要原因是活性炭被润湿后和板电极之间形成了良好的导通，从而保证了有无活性炭的情况下，两极之间的距离没有发生变化，所以放电强度没有变化。
6.活性炭协同作用下对采油废水的预处理处理效果表明：活性炭层与接地极雾化电晕放电协同作用后，使采油废水的浊度明显低于无活性炭层时接地极雾化电晕放电处理后的采油废水。同时，活性炭协同作用时，整个处理过程BOD、COD的值均小于无活性炭层时接地极雾化电晕放电处理废水所对应的BOD、COD的值。分析原因活性炭能引发臭氧自由基型链反应，加速臭氧分解生成羟基自由基。而且活性炭层越厚，处理过程中对应的BOD、COD的值越小，说明活性炭越厚时，越有利于污染物的去除，与接地极雾化放电所形成的等离子体产生的协同作用越为明显。
7.不同流量下对于处理结果的影响研究表明，无论是否存在活性炭层，整体来看，流量的增加对降低废水浊度、BOD、COD均产生不利影响。分析原因是流量的增加使放电电流减小，降低了活性物质的产生。故而，反应速率减慢。当电压为13kv，线电极和活性炭层之间的距离为2.5cm，在流量为50ml/min，活性炭厚度为5mm时，处理效果最为理想。
Earthed atomizing corona discharge is an environmental-friendly technology to treatwaste water. This environmental management technology is notable for its high treatmentefficiency, fast reaction and freedom from secondary pollution. This paper studies thecharacteristics of earthed atomizing corona discharge when it is used alone and when it issynergized with activated carbon, as well as their effects of pre-treating of oilfield producedwater. The research contents, results and conclusions are as follows:
1. Corona discharges and atomizing discharges were combined effectively, and anew-style reactor was designed. Active species of discharge plasma exist for quite a short time.Take OH as an example, it only presents for10-7S. Traditional discharge methods are not ableto synchronise the plasma zone and reaction zone completely, so the reaction time betweenactive species and pollutants is cut down. Research indicates that earthed atomizing coronadischarge forms synchronised plasma zones and atomizing liquid drops, as well as theuniform plasma zones, and active species produced by the discharge are able to interact withwaste water from oil extraction directly. Simultaneously, the water to be treated, under theaction of strong electrostatic field force and surface tension, is atomized to small liquid dropsthat pass through the discharge reaction space. The atomizing effect enlarges the reaction areabetween the water and the plasma zone. Thus, compared with other discharge treatmentpatterns, this method can transform the waste water form oil extraction to be biochemicallytreatable with relatively lower energy and realise a higher utilisation rate of energy.
2. To provide a basis for the best discharge conditions, the influences of positive/negativeatomizing corona, inter-electrode distance and flux on the earthed atomizing corona dischargeare researched. According to the research finding, on the condition of the same dischargesituation, the discharge current of a negative earthed atomizing corona is greater than that of apositive earthed atomizing corona and exceeds that of a traditional corona even more. Themain reason is that a Taylor Cone formed on the surface of a line electrode during theatomizing corona discharge shortened the inter-electrode distance. Also, there is a possibilitythat the curvature radius of the Taylor Cone will facilitate the aggrandising of the dischargecurrent.
3. In the research, the discharge mechanism of earthed atomizing corona discharge isanalyzed. The research suggests that: a non-uniform electric field is formed between the lineelectrode and the plate electrodes. The highest electric field intensity exists on the surface ofthe line electrode. When the voltage exceeds the onset voltage, a corona zone is formedaround the line electrode and discharges. At the same time, the water flow that covers the surface of the line electrode produces an electric fluid effect under the action of strong electrostatic field force and further acts as a liquid electrostatic spray. The atomized small liquiddrops will discharge in the discharge electrodes. Multiple cone-shaped fluxes formed whensmall electric liquid drops move will, to some extent, be quite likely to make a crossover withthose created by large liquid drops, so this discharge form would be more beneficial forcreating relatively even plasma zone to enhance its effect on waste water.
4. According to I-V characteristics of earthed atomizing corona discharge, appropriateinter-electrode distance and voltage are selected to carry out advanced oxidation treatment onhigh concentration waste water from oil extraction while BOD5, COD, turbidity and pHbefore and after reaction are measured. The study indicates that when consuming little energy,earthed atomizing corona discharge to turns out to be effective on augmenting thebiodegradability of waste water from oil extraction.
The initial value of biodegradability of oilfield produced water was0.079and later roseto over0.5after the treatment. And COD removal rate reached79.64%.
5. The research on activated carbon’s influence on the discharge current suggests that theinvolvement of activated carbon does not cause any change in the current of earthedatomizing corona discharge. The main reason is that a good conduction formed between theactivated carbon and the plate electrodes after the activated carbon is soaked ensures thatthere is no change in the inter-electrode distance with or without activated carbon. As a result,the discharge intensity is unchanged.
6. The research on the effect of pre-treating oilfield produced water with the synergy ofearthed atomizing corona discharge and activated carbon suggests that after the earthedatomizing corona discharge and the activated carbon are synergized, the turbidity of theoilfield produced water is significantly lower than the turbidity of the oilfield produced watertreated by earthed atomizing corona discharge without activated carbon. At the same time,BOD and COD of the oilfield produced water during the pre-treating are both lower thanthose without activated carbon. The reason is that the activated carbon causes ozone freeradical chain reaction which further accelerates the decomposition of ozone into hydroxylradical. The thicker the activated carbon layer, the lower BOD and COD are. This indicatesthat a thicker activated carbon layer is more helpful in removing pollutants and shows moresignificant synergy with the plasma from the earthed atomizing corona discharge.
7. The research on the influences of different water flux on the treatment effect suggeststhat with or without activated carbon, the increase in water flux has a negative influence onlowering the turbidity, BOD and COD of the oilfield produced water. The reason is that theincreased flux reduces the discharge current and thus reduces the generation of active species.As a result, the reaction rate is lowered. When the voltage is13kv, the distance between the line electrode and the activated carbon is2.5cm; when the flux is50ml/min and the thicknessof the activated carbon is5mm, the treatment effect is the best.
引文
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