炼油碱水预处理工艺的试验与数值模拟研究
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摘要
炼油碱水是石油炼制过程中油品碱洗精制时产生的一种含有大量硫化物和酚类等有毒有害污染物的碱性废液，是炼油厂主要的恶臭污染源。曝气滤池尤其是循环曝气生物滤池（Circulating BiologicalAerated Filter，简称CBAF）是对这类废水进行预处理的有效装置。基于CBAF的废水处理工艺成本较低，效率较高，是一种值得推广的生物预处理工艺。
但是CBAF反应器的设计、选型以及工程放大，主要依赖于实验数据和个人经验，缺乏理论的指导；CBAF内部的传递（包括质量传递、动量传递）机理较复杂，难以通过普通的实验手段得出接近实际的传递机理，从而难以找到有效提高处理效率的方法；废水各项指标的检测工作量很大，通过实验研究的方法调整操作参数，改进工艺需要耗费大量的人力物力，并且不易找到改进的突破口。
本文采用试验研究与数值模拟相结合的方法，探讨了铁/碳微电解隔离曝气滤池和系列CBAF（单曝气筒CBAF和四曝气筒CBAF）的废水处理性能，模拟了四曝气筒CBAF内部溶解氧浓度、硫化物浓度以及单质硫浓度分布，为四曝气筒CBAF装置及工艺改进提出了思路和方法。
采用铁/碳微电解隔离曝气滤池对炼油废水进行了预处理，当废水中的化学耗氧量（chemical oxygen demand，简称COD）为700mg L-1-1100mg L-1，五日生化需氧量（5-day Biochemical Oxygen Demand，简称BOD5）在70mg L-1-100mg L-1之间，BOD5/COD在0.1左右，氨氮浓度为10mg L-1-30mg L-1，采用隔离曝气及在适宜的操作条件下，COD与氨氮的去除率可分别达到67%和58%。在系统中加入适量的H2O2，可进一步强化废水的降解与提高废水可生化性。
采用三级单曝气筒CBAF对炼油碱水进行生物预处理，当COD、硫化物、酚类和石油类物质的浓度分别不超过1500mg L-1，800mg L-1，15mg L-1和150mg L-1时，水力停留时间(HRT)从7.95h变化到15.90h，气水比从8﹕1变化到12﹕1，上述污染物的总去除率分别达到87.8%，98.0%，96.8%和91.0%。同时，处理系统运行稳定，滤池中的生物质生长良好。生物降解、化学氧化脱硫和曝气吹脱脱硫是硫化物移除的3种主要途径，在有菌条件下，生物降解是其中最重要的一种途径，超过94.5%的硫化物通过生物降解的途径被转化。在有氧情况下，硫化物能转化为不同的形式。当利用循环曝气生物滤池进行废水处理时，在试验条件下平均约有96.5%的硫化物转化为单质硫。
采用计算流体动力学（CFD）技术，选用湍流标准k-ε模型，多相流混合模型（Mixture模型），辅以组分输运模型和壁面函数对CBAF内部的流动进行三维的模拟。
模拟了进水（纯水）流量固定、四种不同气水比下四曝气筒CBAF内部的溶解氧浓度分布。湍流模型选用标准k-ε模型，多相流模型选用混合模型。进水量固定为0.5m3h-1，气水比变化分别为8﹕1、16﹕1、24﹕1和32﹕1。随着气水比增加，溶解氧浓度在z方向、同一水平位置上的分布越来越均匀，气流对于溶解氧浓度分布的扰动越来越强烈，生物滤池下部的溶解氧浓度明显提高，适宜于进行生物氧化反应的区域逐渐增大，填料层溶解氧平均浓度不断上升；填料层、碎石层和曝气筒内水的流动速度不断增大，循环流量可达到进水流量的二十倍以上。通过雷诺数的计算可以知道，填料层、碎石层内的流动为层流，曝气筒内的流动为湍流。
模拟了进水（炼油废水）流量固定，在四种不同气水比情况下四曝气筒CBAF内部的溶解氧浓度、硫化物浓度以及单质硫浓度分布。模拟结果表明，随着气水比增加，气泡对于水的扰动加大，CBAF上部的溶解氧浓度基本一致，下部溶解氧的浓度逐渐增大。硫化物浓度在进水口附近区域较高，在出水口附近区域较低，在同一水平面上的分布不均匀。单质硫主要集中在生物滤池填料层中，并且进水口附近区域浓度较高。出水口附近的填料层中虽然也存在单质硫，但是浓度较低。加大曝气量有利于提高溶解氧浓度，气水比为24﹕1有利于反应物浓度均匀分布。
模拟了曝气量固定，HRT变化（即进水流量变化）的情况下四曝气筒CBAF内部的溶解氧浓度、硫化物浓度以及单质硫浓度分布。模拟结果表明，随着HRT下降，CBAF内溶解氧浓度不断下降，硫化物的浓度不断上升。同一水平面上，随着HRT下降，硫化物浓度梯度逐步减小，出水口处的硫化物浓度逐步增大。无论进水量如何变化，在进水口附近的填料层中，单质硫的浓度总是高于出水口附近填料层中的浓度。
提出了一种改进装置结构的方法，把原来一个进口一个出口改进为两个进口和两个出口的形式。对改进后的CBAF，模拟了进水流量0.5m3h-1，气水比分别为8﹕1、16﹕1、24﹕1和32﹕1等4种气水比情况下的溶解氧、硫化物和单质硫的浓度分布，结果表明，结构的改变能提高硫化物分布的均匀性，从而提高装置的生产能力。
提出了一种改进工艺的方法，通过调节曝气筒曝气量比例来改善硫化物在CBAF内的分布。模拟了进水流量0.5m3h-1，气水比为24﹕1，两组曝气筒曝气量比值分别为8﹕2、7﹕3、6﹕4、4﹕6、3﹕7和2﹕8等6种比例的情况。模拟结果表明，通过调节第一组曝气筒和第二组曝气筒的曝气量比值为2﹕8-4﹕6，均能有效改善原有装置的污染物分布情况，提高生产能力。
Alkaline waste water from oil refinery is a kind of alkaline waste liquid containing a largenumber of poisonous and harmful pollutants such as sulphides and phenols produced fromalkaline washing and refining process. It is the main source of fetor in refinery. Aerated filter,especially Circulating Biological Aerated Filter (CBAF) is an effective equipment for alkalinewaste water treatment. Waste water treatment process based on CBAF is worthy of populatingfor its lower cost and higher efficiency.
Until now, design, model selection and engineering enlargement of CBAF reactors relymaily on experimental data and individual experience which is short of theoretical direction.The mechanism of transfer including mass transfer and momentum transfer in CBAF iscomplicated and is hard to get the similar transfer mechanism by common experimentalmeans so it is very difficult to find an effective way to improve the treating efficiency. It costsa great deal of manpower and material resources to adjust the operating parameters throughexperimental research because the detection work of the properties of waste water is veryintensive, and at the same time it is not easy to find a breakthrough for the improvement ofthe reactor and process.
Experimental research combined with numerical simulation is used in this dissertation. Thetreating performance of Fe/C microelectrolysis aerated filter and serial CBAF includingsingle-aerated-tube CBAF and four-aerated-tubes CBAF is studied. The concentrationdistribution of dissolved oxygen, hydrogen sulfide and elemental sulfur in thefour-aerated-tubes CBAF is simulated and the way for the improvement of reactor andprocess is proposed for the four aerated tubes CBAF.
Refinery waste water is pretreated by Fe/C microelectrolysis isolated aerated filter. Whilethe concentration of COD is between700mg L-1-1100mg L-1，which for BOD5between70mg L-1-100mg L-1, the ratio of BOD5/COD is about0.1and the concentration of ammonia-nitrogen is between10mg L-1-30mg L-1, and under suitable operation conditions, theremoval rate of COD and ammonia-nitrogen can reach67%and58%, respectively. Degradation and biodegradability of waste water can be enhanced while moderate H2O2isadded into the system.
Alkaline waste water from oil refinery is biologically pretreated by three-stagesingle-aerated-tube Isolated Aerated Biological Filters. While COD, the concentrations ofsulphides, hydroxybenzene and oil in the waste water are no more than1500mg L-1,800mg L-1,15mg L-1and150mg L-1, respectively, the total removal of these pollutants is87.8%,98.8%,96.8%and91.0%accordingly. The system can run stably and the biomassin the filter grows well. Biodegradation, chemical oxidative desulfurization and aerationdesulfurization are three ways to remove sulphides and under bacterial condition,biodegradation is the most effective one, more than94.5%sulphides are removed bybiodegradation. Under aerobic condition, sulphides can be transformed into different forms.The average value of sulphides transformed into elemental sulfur is about96.5%when thewaste water is treated by CBAF under common operation condition.
The flow inside the CBAF is three-dimentionally simulated based on CFD with k-εmodelfor turbulence model, Mixture model for multiphase flow model, component transport modeland wall function method.
Concentration distribution of dissolved oxygen inside the four-aerated-tubesCBAF issimulated at four different air water volume ratios (AWVRs) and constant influent of water.The k-ε model is chosen for turbulence model and Mixture model for multiphase model. Theinfluent is constant and its value is0.5m3h-1, AWVRs are varied and their values are8﹕1,16﹕1,24﹕1and32﹕1respectively. As AWVR increases, the concentration distribution ofdissolved oxygen becomes more and more uniform in both z direction and the same location.The disturbance of airflow from aerator becomes more and more intense. The concentrationof dissolved oxygen increases obviously at the bottom of the reactor. And the mean value ofthe concentration of dissolved oxygen located in the packing layer increases step by step somore and more zones in packing layer become suitable for biodegradation. The flow velocityof water in packing layer, macadam layer and aerated tubes increases constantly and the flowrate of circular flow can be dozens of times or more than that of inflow. The flow in packing layer and macadam layer is proved to be laminar and that in aerated tubes is turbulent bycalculating Reynolds number.
Concentration distribution of dissolved oxygen, sulphides and elemental sulphur inside thefour-aerated-tubes CBAF is simulated at four different AWVRs and with constant influent ofrefinery waste water. Results show that the disturbance of the bubbles enhance, theconcentration distribution of dissolved oxygen keeps coincident on the top of the CBAF butincreases at the bottom as AWVR increases. The concentration distribution of sulphides is nothomogeneous, and it is high in the area near the inlet and is low in the area near the outlet.The elemental sulphur concentrates upon the packing layer especially near the inlet. Thoughthe elemental sulphur appears in the packing layer near the outlet, its concentration is verylow. Increasing the aeration rate is benificial for increasing the concentration of dissolvedoxygen, and24﹕1is a suitable AWVR for the concentration distribution of reactants.
Concentration distribution of dissolved oxygen, sulphides and elemental sulphur inside thefour-aerated-tubes CBAF is simulated at different Hydraulic Retention Time or HRT for shortand constant AWVR. Results show that the concentration of dissolved oxygen reduces andthat of sulphides increases gradually as HRT decreases. On the same horizontal plane, theconcentration gradient of sulphides reduces and the concentration of sulphides at the outletincreases gradually as HRT decreases. The concentration of sulphur in the packing layer nearthe inlet is always higher than that near the outlet no matter how the HRT varies.
A method that changes the structure of CBAF is proposed. The one-inlet-one-outlet-CBAFis changed into two-inlets-two-outlets-CBAF. The concentration distributions of dissolvedoxygen, sulphides and elemental sulphur are simulated at four different AWVRs which are8﹕1,16﹕1,24﹕1and32﹕1, respectively, while the influent is0.5m3h-1. Results show thatthe changes of the structure of CBAF can improve the distribution of sulphides and increasethe production capacity of CBAF.
A method that changes the technological parameters is proposed which changes theaeration ratio of two sets of aeration tubes so as to improve the concentration distribution ofsulphides inside the CBAF. When the influent is0.5m3h-1and the AWVR is24﹕1, six different aeration ratios of two sets of aeration tubes are simulated which are8﹕2,7﹕3,6﹕4,4﹕6,3﹕7and2﹕8, respectively. Results show that the distribution of pollutants is wellimproved and the production capacity of CBAF is increased by adjusting the aeration ratio ofthe1st set of aeration tubes and the2nd set of aeration tubes from2﹕8to4﹕6.
但是CBAF反应器的设计、选型以及工程放大，主要依赖于实验数据和个人经验，缺乏理论的指导；CBAF内部的传递（包括质量传递、动量传递）机理较复杂，难以通过普通的实验手段得出接近实际的传递机理，从而难以找到有效提高处理效率的方法；废水各项指标的检测工作量很大，通过实验研究的方法调整操作参数，改进工艺需要耗费大量的人力物力，并且不易找到改进的突破口。
本文采用试验研究与数值模拟相结合的方法，探讨了铁/碳微电解隔离曝气滤池和系列CBAF（单曝气筒CBAF和四曝气筒CBAF）的废水处理性能，模拟了四曝气筒CBAF内部溶解氧浓度、硫化物浓度以及单质硫浓度分布，为四曝气筒CBAF装置及工艺改进提出了思路和方法。
采用铁/碳微电解隔离曝气滤池对炼油废水进行了预处理，当废水中的化学耗氧量（chemical oxygen demand，简称COD）为700mg L-1-1100mg L-1，五日生化需氧量（5-day Biochemical Oxygen Demand，简称BOD5）在70mg L-1-100mg L-1之间，BOD5/COD在0.1左右，氨氮浓度为10mg L-1-30mg L-1，采用隔离曝气及在适宜的操作条件下，COD与氨氮的去除率可分别达到67%和58%。在系统中加入适量的H2O2，可进一步强化废水的降解与提高废水可生化性。
采用三级单曝气筒CBAF对炼油碱水进行生物预处理，当COD、硫化物、酚类和石油类物质的浓度分别不超过1500mg L-1，800mg L-1，15mg L-1和150mg L-1时，水力停留时间(HRT)从7.95h变化到15.90h，气水比从8﹕1变化到12﹕1，上述污染物的总去除率分别达到87.8%，98.0%，96.8%和91.0%。同时，处理系统运行稳定，滤池中的生物质生长良好。生物降解、化学氧化脱硫和曝气吹脱脱硫是硫化物移除的3种主要途径，在有菌条件下，生物降解是其中最重要的一种途径，超过94.5%的硫化物通过生物降解的途径被转化。在有氧情况下，硫化物能转化为不同的形式。当利用循环曝气生物滤池进行废水处理时，在试验条件下平均约有96.5%的硫化物转化为单质硫。
采用计算流体动力学（CFD）技术，选用湍流标准k-ε模型，多相流混合模型（Mixture模型），辅以组分输运模型和壁面函数对CBAF内部的流动进行三维的模拟。
模拟了进水（纯水）流量固定、四种不同气水比下四曝气筒CBAF内部的溶解氧浓度分布。湍流模型选用标准k-ε模型，多相流模型选用混合模型。进水量固定为0.5m3h-1，气水比变化分别为8﹕1、16﹕1、24﹕1和32﹕1。随着气水比增加，溶解氧浓度在z方向、同一水平位置上的分布越来越均匀，气流对于溶解氧浓度分布的扰动越来越强烈，生物滤池下部的溶解氧浓度明显提高，适宜于进行生物氧化反应的区域逐渐增大，填料层溶解氧平均浓度不断上升；填料层、碎石层和曝气筒内水的流动速度不断增大，循环流量可达到进水流量的二十倍以上。通过雷诺数的计算可以知道，填料层、碎石层内的流动为层流，曝气筒内的流动为湍流。
模拟了进水（炼油废水）流量固定，在四种不同气水比情况下四曝气筒CBAF内部的溶解氧浓度、硫化物浓度以及单质硫浓度分布。模拟结果表明，随着气水比增加，气泡对于水的扰动加大，CBAF上部的溶解氧浓度基本一致，下部溶解氧的浓度逐渐增大。硫化物浓度在进水口附近区域较高，在出水口附近区域较低，在同一水平面上的分布不均匀。单质硫主要集中在生物滤池填料层中，并且进水口附近区域浓度较高。出水口附近的填料层中虽然也存在单质硫，但是浓度较低。加大曝气量有利于提高溶解氧浓度，气水比为24﹕1有利于反应物浓度均匀分布。
模拟了曝气量固定，HRT变化（即进水流量变化）的情况下四曝气筒CBAF内部的溶解氧浓度、硫化物浓度以及单质硫浓度分布。模拟结果表明，随着HRT下降，CBAF内溶解氧浓度不断下降，硫化物的浓度不断上升。同一水平面上，随着HRT下降，硫化物浓度梯度逐步减小，出水口处的硫化物浓度逐步增大。无论进水量如何变化，在进水口附近的填料层中，单质硫的浓度总是高于出水口附近填料层中的浓度。
提出了一种改进装置结构的方法，把原来一个进口一个出口改进为两个进口和两个出口的形式。对改进后的CBAF，模拟了进水流量0.5m3h-1，气水比分别为8﹕1、16﹕1、24﹕1和32﹕1等4种气水比情况下的溶解氧、硫化物和单质硫的浓度分布，结果表明，结构的改变能提高硫化物分布的均匀性，从而提高装置的生产能力。
提出了一种改进工艺的方法，通过调节曝气筒曝气量比例来改善硫化物在CBAF内的分布。模拟了进水流量0.5m3h-1，气水比为24﹕1，两组曝气筒曝气量比值分别为8﹕2、7﹕3、6﹕4、4﹕6、3﹕7和2﹕8等6种比例的情况。模拟结果表明，通过调节第一组曝气筒和第二组曝气筒的曝气量比值为2﹕8-4﹕6，均能有效改善原有装置的污染物分布情况，提高生产能力。
Alkaline waste water from oil refinery is a kind of alkaline waste liquid containing a largenumber of poisonous and harmful pollutants such as sulphides and phenols produced fromalkaline washing and refining process. It is the main source of fetor in refinery. Aerated filter,especially Circulating Biological Aerated Filter (CBAF) is an effective equipment for alkalinewaste water treatment. Waste water treatment process based on CBAF is worthy of populatingfor its lower cost and higher efficiency.
Until now, design, model selection and engineering enlargement of CBAF reactors relymaily on experimental data and individual experience which is short of theoretical direction.The mechanism of transfer including mass transfer and momentum transfer in CBAF iscomplicated and is hard to get the similar transfer mechanism by common experimentalmeans so it is very difficult to find an effective way to improve the treating efficiency. It costsa great deal of manpower and material resources to adjust the operating parameters throughexperimental research because the detection work of the properties of waste water is veryintensive, and at the same time it is not easy to find a breakthrough for the improvement ofthe reactor and process.
Experimental research combined with numerical simulation is used in this dissertation. Thetreating performance of Fe/C microelectrolysis aerated filter and serial CBAF includingsingle-aerated-tube CBAF and four-aerated-tubes CBAF is studied. The concentrationdistribution of dissolved oxygen, hydrogen sulfide and elemental sulfur in thefour-aerated-tubes CBAF is simulated and the way for the improvement of reactor andprocess is proposed for the four aerated tubes CBAF.
Refinery waste water is pretreated by Fe/C microelectrolysis isolated aerated filter. Whilethe concentration of COD is between700mg L-1-1100mg L-1，which for BOD5between70mg L-1-100mg L-1, the ratio of BOD5/COD is about0.1and the concentration of ammonia-nitrogen is between10mg L-1-30mg L-1, and under suitable operation conditions, theremoval rate of COD and ammonia-nitrogen can reach67%and58%, respectively. Degradation and biodegradability of waste water can be enhanced while moderate H2O2isadded into the system.
Alkaline waste water from oil refinery is biologically pretreated by three-stagesingle-aerated-tube Isolated Aerated Biological Filters. While COD, the concentrations ofsulphides, hydroxybenzene and oil in the waste water are no more than1500mg L-1,800mg L-1,15mg L-1and150mg L-1, respectively, the total removal of these pollutants is87.8%,98.8%,96.8%and91.0%accordingly. The system can run stably and the biomassin the filter grows well. Biodegradation, chemical oxidative desulfurization and aerationdesulfurization are three ways to remove sulphides and under bacterial condition,biodegradation is the most effective one, more than94.5%sulphides are removed bybiodegradation. Under aerobic condition, sulphides can be transformed into different forms.The average value of sulphides transformed into elemental sulfur is about96.5%when thewaste water is treated by CBAF under common operation condition.
The flow inside the CBAF is three-dimentionally simulated based on CFD with k-εmodelfor turbulence model, Mixture model for multiphase flow model, component transport modeland wall function method.
Concentration distribution of dissolved oxygen inside the four-aerated-tubesCBAF issimulated at four different air water volume ratios (AWVRs) and constant influent of water.The k-ε model is chosen for turbulence model and Mixture model for multiphase model. Theinfluent is constant and its value is0.5m3h-1, AWVRs are varied and their values are8﹕1,16﹕1,24﹕1and32﹕1respectively. As AWVR increases, the concentration distribution ofdissolved oxygen becomes more and more uniform in both z direction and the same location.The disturbance of airflow from aerator becomes more and more intense. The concentrationof dissolved oxygen increases obviously at the bottom of the reactor. And the mean value ofthe concentration of dissolved oxygen located in the packing layer increases step by step somore and more zones in packing layer become suitable for biodegradation. The flow velocityof water in packing layer, macadam layer and aerated tubes increases constantly and the flowrate of circular flow can be dozens of times or more than that of inflow. The flow in packing layer and macadam layer is proved to be laminar and that in aerated tubes is turbulent bycalculating Reynolds number.
Concentration distribution of dissolved oxygen, sulphides and elemental sulphur inside thefour-aerated-tubes CBAF is simulated at four different AWVRs and with constant influent ofrefinery waste water. Results show that the disturbance of the bubbles enhance, theconcentration distribution of dissolved oxygen keeps coincident on the top of the CBAF butincreases at the bottom as AWVR increases. The concentration distribution of sulphides is nothomogeneous, and it is high in the area near the inlet and is low in the area near the outlet.The elemental sulphur concentrates upon the packing layer especially near the inlet. Thoughthe elemental sulphur appears in the packing layer near the outlet, its concentration is verylow. Increasing the aeration rate is benificial for increasing the concentration of dissolvedoxygen, and24﹕1is a suitable AWVR for the concentration distribution of reactants.
Concentration distribution of dissolved oxygen, sulphides and elemental sulphur inside thefour-aerated-tubes CBAF is simulated at different Hydraulic Retention Time or HRT for shortand constant AWVR. Results show that the concentration of dissolved oxygen reduces andthat of sulphides increases gradually as HRT decreases. On the same horizontal plane, theconcentration gradient of sulphides reduces and the concentration of sulphides at the outletincreases gradually as HRT decreases. The concentration of sulphur in the packing layer nearthe inlet is always higher than that near the outlet no matter how the HRT varies.
A method that changes the structure of CBAF is proposed. The one-inlet-one-outlet-CBAFis changed into two-inlets-two-outlets-CBAF. The concentration distributions of dissolvedoxygen, sulphides and elemental sulphur are simulated at four different AWVRs which are8﹕1,16﹕1,24﹕1and32﹕1, respectively, while the influent is0.5m3h-1. Results show thatthe changes of the structure of CBAF can improve the distribution of sulphides and increasethe production capacity of CBAF.
A method that changes the technological parameters is proposed which changes theaeration ratio of two sets of aeration tubes so as to improve the concentration distribution ofsulphides inside the CBAF. When the influent is0.5m3h-1and the AWVR is24﹕1, six different aeration ratios of two sets of aeration tubes are simulated which are8﹕2,7﹕3,6﹕4,4﹕6,3﹕7and2﹕8, respectively. Results show that the distribution of pollutants is wellimproved and the production capacity of CBAF is increased by adjusting the aeration ratio ofthe1st set of aeration tubes and the2nd set of aeration tubes from2﹕8to4﹕6.
引文
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