摘要
伴随着我国经济的快速发展,我们生存所依赖的水环境受到的污染却日趋加剧,为了保护好我们的生存环境,对水污染的控制和治理已刻不容缓。目前,城镇污水处理技术相对成熟,厂矿企业排放的工业废水处理技术也有了长足的进步,但目前国内诸多工业园区,从不同企业流出的各种工业废水混合在一起排放,不仅污染物具有多样性,而且会产生复合污染,致使目前常用的处理工艺难以满足国家要求的达标排放,或处理成本太高,业主难以承受。本论文旨在开发一种处理效果好、运行费用低的处理工艺,能有效地去除工业园区内的含重金属有机物复合废水中的污染物。
本课题来源于“国家水体污染控制与治理科技重大专项”--“湘江水环境重金属污染整治关键技术研究与综合示范性课题”。本课题首先长时间详细地调查了湖南省某工业园区的外排水水质,确定了研究对象。研究了电絮凝作为预处理去除重金属、有机物的去除效率及其影响因素；研究了硅藻土吸附重金属的影响因素,吸附动力学和吸附等温线；对比研究了颗粒生物膜—膜生物反应器和普通的膜生物反应器对低浓度重金属、氨氮、总氮、有机物的去除效率,研究了两种不同反应器的膜通量、污泥颗粒和混合液黏度的不同；研究了电场—膜生物反应器的去除效果。本课题在该工业园区的综合污水处理厂内专门建立了一套中试装置,用于验证本课题研究的应用效果,同时这种平行试验已用于指导处理厂的日常运行管理。试验结果表明：
(1)电絮凝能有效地除去废水中的重金属,对模拟废水的Cu2+、Zn2+、Pb2+去除效率可达到96.0%以上,对Cd2+的去除率能达到82.0%以上。研究了电絮凝工艺去除重金属的最佳条件,结果表明,初始pH值对去除效率有重要的影响,当pH达到6最佳值时,同时电流密度为6A/dm2,极板间距为3cm,电絮凝时间30min,则可达到较理想的处理效果。电絮凝对废水中的COD去除也卓有成效。试验证明,在pH值为7,电流密度为10A/dm2,电絮凝时间为30min时,可以达到75%以上的COD去除率,因此,电絮凝处理工艺作为综合废水的预处理是适当的。
(2)本课题研究了电絮凝除磷的可行性,试验证明,在设定的条件下磷的去除效率可以达到75%以上,因此,电絮凝能有效地去除废水中的磷。
(3)硅藻土能有效地吸附废水中的重金属,同时硅藻土的使用量对重金属废水的处理效果具有重要影响,试验室数据和中试结果都表明,在硅藻土投加量为8g/L时,当进水中Cu2+、Zn2+、Pb2+、Cd2+浓度分别为5.0mg/L、5.Omg/L.2.0mg/L、0.2mg/L时,测定出水中的重金属浓度分别为0.73mg/L、.40mg/L、0.17mg/L、0.07mg/L,即Cu2+、Zn2+、Pb2+、Cd2+的去除率分别达到了85.38%、72.00%、91.70%和65.71%,去除效果显著,为后续的生物处理处理奠定了基础。
(4)影响硅藻土吸附效果的主要因素是pH值和进水中重金属浓度。pH值是影响硅藻土吸附效果的重要因素,实验表明,在酸性条件下吸附效果较差,在中性或弱碱性条件下效果较好,如：在pH值=6±0.2时,Cu2+、Zn2+、Pb2+和Cd2+的去除率分别达到了90.00%、77.54%、94.07%和72.14%,但是进一步提高pH值对去除率的影响不大。吸附量随着重金属离子浓度的升高呈上升趋势变化。在重金属离子浓度超过1.0mmol/L后,吸附量则增加缓慢。
(5)硅藻土对Cu2+、Zn2+和Cd2+的吸附规律相近,数据显示：前30min吸附速率都很快,分别达到85.38%、78.77%和68.57%,基本接近吸附峰值；30min后,增幅开始变小。然而,硅藻土吸附Pb2+体现了不同的变化规律,对Pb2+的吸附速度非常迅速,在5min时,溶液中Pd2+的去除率便达到81.48%,10min时吸附率为88.15%,基本接近饱和值。
(6)当硅藻土对Cu2+、Zn2+、Cd2+、Pb2+四种金属离子吸附达到稳定平衡时,改性硅藻土对Pb2+的吸附量明显大于对Cu2+、Zn2+、Cd2+的吸附。如在吸附时间为5min时,硅藻土对Cu2+、Zn2+、Cd2+、Pb2四种重金属的吸附量分别为4.21、3.46、6.80和11.00mg/L,吸附量大小顺序是Pb2+>Cd2+>Cu2+>Zn2+。说明硅藻土吸附剂对重金属离子具有一定的选择性。
(7)研究了硅藻土吸附Cu2+、Zn2+、Cd2+、Pb2+四种不同重金属的吸附等温线,并对其做了回归分析,Langmuir吸附等温线方程拟合的回归系数R2值大于0.94,而Freundlich吸附等温线模型拟合的R2值在0.78-0.81之间,显然Langmuir方程的拟合效果优于Freundlich方程的拟合效果。
(8)对比研究了颗粒生物膜—膜生物反应器和普通膜生物反应器的去除效果,两个反应器对重金属、COD、氨氮的去除效果都很明显,重金属、COD、氨氮的出水浓度都满足《城镇污水处理厂污染物排放标准》(GB18918-2002)的一级B的要求。但两种反应器对总氮的去除效率不高,其主要原因是处理系统采用了连续曝气的运行方式,抑制了反硝化菌的成长。
(9)本实验中,颗粒生物膜—膜生物反应器与普通的膜生物反应器相比,在去除重金属、COD、氨氮和总氮方面都有较好的去除效果,表明投加硅藻土可以强化去除有机物、重金属和氨氮的去除效果。
(10)投加硅藻土可以延缓膜通量的下降速度。投加硅藻土可以改善微生物的生存环境,使污泥浓度增长更快,污泥絮体平均粒径增大了77.37%,污泥黏度减小了41.18%,从而减缓了泥饼层的形成速度,并且使泥饼层变得较疏松、透水性好、可滤性强。因此,投加硅藻土可减缓过膜压力的增长,减轻膜污染,延长了膜组件的使用周期。
(11)电场—膜生物反应器对COD去除效果显著,去除率一直稳定在90.0%以上,改变电流密度对其影响不大。
(12)冲击负荷不会影响电场—膜生物反应器对氨氮的去除效率,表明该系统具有很强的自身调节能力。
(13)电流密度对TN去除率有较大的影响,电流密度从110mA到150mA,TN去除率逐步升高,最高去除效率达到83.8%；但当进一步增加电流密度时,TN去除率开始下降。另外,冲击负荷对TN去除率有一定的影响,系统进水中TN浓度从46mg/L上升到88mg/L,系统去除效果较好；但当TN浓度超过90mg/L后,系统去除率有所下降。
研究结果表明：电絮凝+电场膜生物反应器能有效地处理好工业园区综合废水的复合污染。
Along with the rapid development of Chinese economy, water environment which our lives depend on tends worse than ever resulting from pollution. It is urgent to make action for water pollution controlling and handling so as to protect our common homeland. At present, technique for municipal wastewater treatment is relatively abundant, simultaneously substantial progress has been made for treatment technique on industrial wastewater treatment. However, in so many industrial parks of cities or towns, a variety of wastewater is discharged and mixed together from different factories with the complexity and diversity of pollutants. Due to mixture with heavy metals and organic compounds and even resulting in multiplex pollution, it is too difficult to find good solution for handling such complicated wastewater by normal process and fit the national stand, otherwise it will cost too much which the customer cannot stand. Therefor, the purpose of this paper is to develop a treatment process for handling successfully such mixing industrial wastewater with heavy metals and organic compounds, and with high treatment efficiency and lower costs for operation. This study has gotten the support by National Special Water Research named Research For Key Technique and Synthesized Pilot Project For Heavy Metal Pollution Controlling in Xiang River. Firstly the detailed investigation for water quality of the final discharged wastewater has been made for a long time in an industrial park with heavy pollution in Hunan Province so that the study object was defined. In this study, Removal efficiency for heavy metals and organic matter and its influencing factors were researched on electro-flocculation as pretreatment, adsorption kinetics, adsorption isotherms, and its influencing factors on diatomite adsorption for heavy metals has also been researched. Comparative study on removal efficiency between particle biofilm-membrane bioreactor and membrane bioreactor for low concentrations of heavy metals, ammonia nitrogen, total nitrogen and organic matter has been done, as well as the difference about the membrane flux, particles of sludge, viscosity of mixture liquid between the two bioators has been studied. Finally, the study on removal efficiency of the electric field-membrane bioreactor has been done. In order to testify the application purpose for this study, a pilot experimental facility has been build up in the integrated wastewater treatment plant, which is still giving figures as a guidance for daily operation and management of this plant.some achievements of the experiment are shown as below.
(1) It is effective for electric flocculation to remove heavy metals, and the removal efficiency is more than96.0%of Cu2+, Zn2+, Pb2+, as well as more than82.0%of Cd2+from simulated wastewater. The optimal condition for electric flocculation process to remove heavy metals has been studied, it is shown that the initial pH value is much important for removal efficiency and the optimal pH is6, current density is6A/dm2, plate space is3cm, and the time for electric flocculation is30min. It is proved that electric flocculation process has excellent removal efficiency for COD removal. The efficiency for COD removal can be more than75%under the conditions with pH7, current density10A/dm2, flocculation30min. Therefore, the the process of electric flocculation as a pre-treatment unit is appropriate for mixed industrial wastewater treatment.
(2) The feasibility for electric flocculation to remove phosphorus from simulated wastewater was also studied. It is proved that phosphorus removal efficiency can be more than75%under optimized condition.
(3)Diatomite can adsorb heavy metals effectively from wastewater, meanwhile the dosage of diatomite has an important impact on the efficiency for heavy metal removal. It is proved that the removal efficiency for heavy metals of Cu2+, Zn2+, Pb2+and Cd2+are85.38%,72.00%,91.70%and65.71%respectively, when thr dosage of diatomite is8g/L. That is, the efficiency is very high. An example can be shown more clearly. When the concentration of Cu2+, Zn2+, Pb2+and Cd2+were5.0mg/L,5.0mg/L,2.0mg/L and0.2mg/L in the influent wastewater, respectively, the corresponding concentration of heavy metals were tested in the effluent as0.73mg/L,1.40mg/L,0.17mg/L and0.07mg/L, respectively, through the electric flocculation process. Thus it gives a good foundation for further removal of heavy metals by subsequent biological treatment.
(4)The main influence factors on adsorption efficiency for heavy metal by diatomite were pH value and concentration of heavy metals in the influent wastewater, and especially for pH value. Normally the dsorption effect is poor under acidic condition, whereas ideal result can be gotten under neutral or weakly alkaline condition. An example can be shown. When pH value is given6±0.2, the removal efficiency for Cu2+, Zn2+, Pb2+and Cd2+will be90.00%,77.54%,94.07%and72.14%, respectively. However, the removal efficiency is almost no change along with the pH value further increasing. When the concentration of heavy metal ion in solution is low, the adsorption amount for a diatomite unit is also low reasonably. Along with increasing of the concentration of heavy metal, more space of diatomite starts to make action with heavy metal ions until tending adsorption saturation point. This means that the adsorption amount will keep increasing along with the concentration ascending of heavy metal. However, once the concentration of heavy metal ion is over1.0mmol/L, the increasing extent of adsorption amount is slowdown.
(5)The adsorption trend is similar for diatomite to adsorb Cu2+, Zn2+and Cd2+, that is, the adsorption efficiency for the three ions are85.38%,78.77%and68.57%, respectively, in the first30minutes. Subsequently, the increasing extend starts to decrease. However, the adsorption trend for diatomite to adsorb Pb2+is so different compared with the above three ions. The action is very rapid so that the adsorption efficiency is more than81.48%in the first5minutes and88.15%in10minutes, which is tending the utmost for removal.
(6)When the stable equilibrium is reached for diatomite adsorbing the four heavy metal ions of Cu2+, Zn2+、Cd2+、Pb2+, it is shown that the adsorbed amount of Pb2+is much more than the others. For example, when the adsorption amount for the four heavy metal ions of Cu2+、Zn2+、Cd2+、Pb2+is tested in the first5minutes, it will be4.21,3.46,6.80and11.0mg/L, respectively, that is, the sequence of adsorption amount for the four heavy metals is Pb2+> Cd2+>Cu2+>Zn2+.This is also means that diatomite as an adsorbent has an obvious selectivity for different heavy metal ions.
(7)Experimental study on adsorption isotherms for diatomite adsorbing the above4heavy metals was done, and regression analysis was also made with Langmuir and Freundlich Equation in the same time. It is shown that Langmuir adsorption isotherm equation can fit the result better than Freundlich adsorption isotherm, with the fitting regression coefficient R2value0.94, and among0.78to0.81, respectively.
(8)The comparative study has been done on the removal effect on particulate biofilm-membrane bioreactor and ordinary membrane bioreactor. Experimental result is shown that both of them have an outstanding effect for pollutants removal including heavy metals, COD and ammonia, and can fit the demand of the national standard--Discharge Standard of Pollutants for Municipal Wastewater Treatment Plant (GB18918-2002). However, both of bioreactors have a low efficiency for TN removal, resulting from the continuous aeration and prohibiting the growth of denitrifying bacteria.
(9)In this study, compared with ordinary membrane bioreactor, particulate biofilm-membrane bioreactor has gotten a more efficient effect on heavy metal, COD, ammonia and TN removal, due to the enhancement of adding diatomite.
(10)The rate of decline of membrane flux can be delayed by adding diatomite in the MBR reactor. It is proved that adding diatomite can improve the living environment for microorganism, so that the sludge concentration can increase faster with average particle size of flocs increasing up to77.37%, sludge viscosity reducing with41.18%. Thus it will decrease the formation velocity for sludge cake layer. In the meantime, adding diatomite can make sludge cake layer more loosen, permeable, and filterable. In a word, it is important for adding diatomite to decrease the growth rate of enduring pressure for membrane, slow down pollution of membrane, and extend the life cycle for membrane module.
(11)Electricity-membrane bioreactor has a higher efficiency for COD removal and the removal rate can keep more than90.0%. There is no much influence for removal effect by changing current density.
(12)Even with impact load, there is little influence on the efficiency for electricity-membrane bioreactor removing ammonia. It is shown such system has a very strong capacity of self regulation.
(13)It has a great influence on the efficiency for electricity-membrane bioreactor to remove TN by changing current density. For example, current density is changed from110mA to150mA, the remove rate will be improved until the maximum83.8%. If keeping increasing current density, the remove rate for TN starts to decline. Impact load will have some influence for the removal rate of TN. It is shown that the system can keep ideal operation when the concentration of TN of influent wastewater is changed from46mg/L to88mg/L. but when the value of TN is up to90mg/L, efficiency for the system removing TN starts to decline. The experiment result is shown that the assembled unit within electric flocculation and electric membrane bioreactor can treat effectively complicated wastewater discharged from industrial zone.
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