垃圾渗滤液的预处理方法及其机理研究
摘要
随着工业的发展与人们生活水平的提高,产生的垃圾量成倍增加,由此引起的垃圾渗滤液也成为目前水体污染中备受关注的污染废水。它的主要特点在于恶臭感明显、污染成分复杂且含量高、毒性大而难以采用生化法处理。因此,渗滤液的预处理方法显得尤为重要。在此背景下,本文旨在深入研究经典预处理技术与开发新型预处理技术,分别选用化学混凝法、磷酸铵镁化学法、煤渣吸附法、微波消解法、氧化剂氧化法及联合法预处理垃圾渗滤,旨在寻求高效的处理工艺,探讨其作用机理,为渗滤液的有效治理提供基础数据、理论指导和应用参考。本研究主要包括以下几个方面的内容：
(1)化学混凝法预处理垃圾渗滤液的研究。通常,化学混凝法用于处理老龄垃圾渗滤液,而本试验则采用此方法处理新鲜垃圾渗滤液。试验结果表明,在分别选用氯化铝(AlCl3)、硫酸铝(A12(SO4)3)、氯化铁(FeCl3)、硫酸铁(Fe2(SO4)3)和聚合氯化铝(PAC)作混凝剂预处理垃圾渗滤液的对比研究中,在优化投加量、pH值和反应时间等试验条件下,水质色度的去除效果为：PAC＞AlCl3＞FeCl3> A12(SO4)3=Fe2(SO4)3;总固体残渣量(TS)的去除效果为：PAC＞Fe2(SO4)3＞Al2(SO4)3＞FeCl3＞AICl3;氨氮(NH4+)的去除效果为：FeCl3＞Fe2(SO4)3＞A12(SO4)3＞PAC＞AlC13; CODcr的去除效果为：AICl3＞A12(SO4)3=Fe2(SO4)3＞PAC＞FeCl3。而P043-的去除率均达到100.0%。预处理后的水质经紫外光谱分析,发现其吸收峰比原水的明显减少,强度明显降低,且铝盐的混凝效果明显强于铁盐。反应的沉淀物分别经SEM-EDS分析,证明混凝法不但可以有效去除色度、TS、NH4+、CODcr和PO43-,还可以同时去除渗滤液中的一些无机阴离子和金属离子。并且,再次证明铝盐的去除效果比铁盐的更为显著。在反应动力学机理研究中,污染物的去除均属于二级或三级动力反应模型,反映出化学混凝法在较短时间内去除污染物的效果受限的原因。该方法具有操作简便、反应快速、占地面积小、运行稳定、处理效果较好等特点,但成本较高,容易产生大量的剩余污泥。
(2)磷酸铵镁化学法预处理垃圾渗滤液的研究。试验结果表明,当pH值为9.5、反应温度为20～30℃、[Mg2+]/[NH4+]/[P043-]摩尔比为1：1：1.4、反应时间为15min、静置时间为20min时,其水质最佳去除率为：色度81.3%,TS52.5%,NH4+100.0%,CODcr43.4%,且出水无PO43-。预处理后的水质经紫外光谱分析,发现其吸收峰比原水的明显减少,强度明显降低。试验后的沉淀物经SEM-EDS和XRD分析发现,该灰色沉淀物主要由三种结构组成,即立方型、针状型和圆柱型结构。其中,立方型和针状型结构为磷酸铵镁,圆柱型结构为磷酸镁。此外,结构表面还吸附着其他元素成分,说明该方法不但能有效去除NH4+,还可以通过吸附作用同时去除垃圾渗滤液中的其他污染物质。试验反应经动力学研究分析,属于一级反应动力模型。产物经提纯后,可作为一种缓释肥,加以回收利用。
(3)蜂窝煤渣吸附法预处理垃圾渗滤液的研究。分别选用蒸馏水、氢氧化钠溶液、盐酸溶液、乙醇和乙酸预处理蜂窝煤渣。试验结果表明,盐酸溶液预处理后的蜂窝煤渣,其性状变化最为明显。当其投加量为20.0mg·L-1、pH值为9.5、反应温度为20℃、反应时间为15min、静置时间为20min时,渗滤液中污染物质的去除效果最佳：色度61.3%,TS52.5%,NH4+27.7%,CODcr39.3%,P043-100.0%。预处理后的水质经紫外光谱分析,发现其吸收峰比原水的明显减少,强度明显降低。试验后的沉淀物经SEM-EDS和XRD分析发现,HCl溶液预处理后的蜂窝煤渣的吸附性能最优。通过反应动力学模型研究发现,NH4+和CODcr的吸附均属于三级反应动力模型,色度的吸附属于二、三级反应动力模型。说明其去除速率较慢。该方法具有环境友好、以废治废、操作简便、性能稳定、成本低廉、占地面积小等特点。试验后的剩余沉淀物,可以回收利用。
(4)微波法预处理垃圾渗滤液的研究。试验结果表明,当微波功率为900W,pH值为2.0,反应时间为15min时,其水质最佳去除率为：色度75.0%,CODcr90.6%,PO43-100.0%,而NH4+的去除率很低,仅为6.5%。预处理后的水质经紫外光谱分析,发现其吸收峰比原水的明显减少,强度明显降低。在动力学研究中发现,色度和CODcr的去除均属于一级反应动力模型。该方法操作简便,处理效果好,占地面积小,且处理后的垃圾渗滤液,恶臭味消除,没有剩余残渣沉淀存在,具有进一步开发利用的潜力。
(5)氧化剂氧化法预处理垃圾渗滤液的研究。分别选用高锰酸钾(KMnO4).次氯酸钠(NaCIO).双氧水(H202)和芬顿试剂(Fenton)作氧化剂预处理垃圾渗滤液。试验结果表明,在优化投加量、pH值和反应时间等试验条件下,其水质最佳去除率分别为,KMn04:色度68.8%,NH4+14.4%,CODcr47.6%,PO3-4100.0%:NaClO:色度50.0%,NH4+40.8%,CODcr59.6%,PO3-4100.0%;H2O2:色度68.8%,NH4+3.2%,CODcr53.9%,PO34100.0%；Fenton:色度82.5%,NH4+10.1%,CODcr64.2%,PO3-4100.0%。预处理后的水质经紫外光谱分析,发现其吸收峰均比原水的明显减少,强度明显降低。在动力学研究中,采用KMnO4作氧化剂时,NH4+和CODcr均属于三级反应动力学模型；采用NaClO作氧化剂时,NH4+属于三级反应动力学模型,CODcr属于一级反应动力学模型；采用H202作氧化剂时,NH4+和CODcr的反应动力学模型均拟合得并不理想；采用Fenton作氧化剂时,NH4+属于三级反应动力学模型,CODcr属于二级反应动力学模型。
(6)微波-氧化剂-磷酸铵镁联合预处理垃圾渗滤液的研究。试验结果表明,在最佳试验条件下,水质的最佳去除效果分别为,微波+KMnO4+磷酸铵镁：色度75.0%,NH4+100.0%,CODcr93.1%,P03-4100.0%,TS99.9%;微波+NaC10+磷酸铵镁：色度75.0%,NH4+100.0%,CODcr91.5%,PO3-4100.0%,TS99.9%;微波+H202+磷酸铵镁：色度100.0%,NH4+100.0%,CODcr90.0%,P043-100.0％,TS99.9%；微波+Fenton+磷酸铵镁：色度100.0%,NH4+100.0%,CODcr92.0%,PO43-100.0%,TS99.9%。预处理后的水质经紫外光谱分析,发现其吸收峰均比原水的明显减少,强度明显降低,且微波+Fenton+磷酸铵镁组合处理后的水质最为显著。
本课题的研究为垃圾渗滤液的经典处理方法提出深层的理论机理,同时为新的处理方法提供了新的探索方向。研究结果丰富了现有垃圾渗滤液的处理技术,并可能开发出简单的物化协同处理工艺,为垃圾渗滤液的处理提供了新的思路与方法。因此,本课题具有重要的理论意义和应用前景。
Along with the development of industry and the remarkable improvement of people's living standard, the domestic garbage has been grown rapidly, which leads to particular attention to landfill leachate. The characteristics of landfill leachate are strong stench, abundance of complicated compositions and high toxicity that are difficult to be disposed by biological treatment methods. Therefore, the pretreatment methods of landfill leachate are particularly important. The aim of this research is to lucubrate the classical technologies and develop new technologies. Chemical coagulation, struvite, adsorption method by honeycomb cinders, microwave digestion method and oxidation method had been used in landfill leachate pretreatment. From these studies, it could be obtained high efficient processes and mechanisms of actions, which could be provided data base, theoretical directions and applications references. The contents of this research mainly included as follows:
(1) Coagulation method. In this research, the coagulation method would be adopted to pretreat fresh landfill leachate, which generally used to pretreat old landfill leachate. AICl3, A12(SO4)3, FeCl3, Fe2(SO4)3and PAC were used as coagulants. Under optimum conditions such as coagulants doses, pH and reaction time, the results of experiments were shown as follows:the color efficiency:PAC＞AlCl3＞FeCl3＞A12(SO4)3=Fe2(SO4)3; the TS efficiency:PAC＞Fe2(SO4)3＞Al2(SO4)3＞FeCl3＞AlCl3; the NH4+efficiency:FeCl3＞Fe2(SO4)3＞Al2(SO4)3>PAC＞AlCl3; the CODcr efficiency:AlCl3>A12(SO4)3=Fe2(S04)3>PAC＞FeCl3. And the PO3-4efficiencies were all obtained at100.0%in this experiment using different coagulants. The UV spectrum analysis of raw/pretreated landfill leachate was manifested that the absorption peaks and intensities of pretreated landfill leachate were even fewer than these of raw landfill leachate. And the effects on the pretreatment of landfill leachate by aluminum salt as coagulants were better than that of ferric salt as coagulants. The SEM-EDS analysis of precipitates after experiments was demonstrated that the coagulation methods were not only used to effectively remove color, TS, NH4+, CODcr and PO3-4, but also used to effectively remove some inorganic and metal anions in raw landfill leachate. Furthermore, It was certified that the coagulation performance of aluminum salt coagulants were better than that of ferric salt coagulants for pretreatment of landfill leachate once again. In kinetics of reactions, the results were shown that the rates of reactions were closer to the second/third order kinetic model, which could explain the reasons of low removal efficiencies of pollutants in raw landfill leachate with short time. This method was characteristics of operate simple, rapid reaction, small occupied area, steady performance and great treatment efficiencies, et al. However, the disadvantages of this method were high cost and abundant of excess sludge produced.
(2) Pretreatment of landfill leachate by struvite method. In this research, when pH was9.5, reaction temperature was20-30℃, the molar ratio of [Mg2+]/[NH4+]/[PO43-] was1:1:1.4, the reaction time was15min and the settling time was20min, the efficiencies of color, TS, NH4+and CODcr were obtained at81.3%,52.5%,100.0%and43.4%, respectively. And no surplus PO3-4existed in pretreated landfill leachate. The UV spectrum analysis of raw/pretreated landfill leachate was manifested that the absorption peaks and intensities of pretreated landfill leachate were even fewer than these of raw landfill leachate. The SEM-EDS analysis of precipitates after struvite method was demonstrated that the structures of precipitate mainly included cubic, acicular and cylinder crystals. In particularly, the cubic and acicular crystals were identified as struvite, and the cylinder crystals were identified as magnesium phosphate. In addition, the surface of crystals was surrounded by other elements, which confirmed that this method could not only remove NH4+, but also remove other pollutant in raw landfill leachate. In kinetics of reactions, the results were shown that the rate of reaction were closer to the first order kinetic model. The precipitates after experiment could be reused as slow release fertilizer by purification.
(3) Pretreatment of landfill leachate by honeycomb cinders adsorption method. The honcycomb cinders were pretreated by distilled water, NaOH solution, HCl solution, CH3CH2OH and CH3COOH, respectively. The results of this experiment showed that the color, TS, NH4+, CODcr and PO3-4removal efficiencies were61.3%,52.5%,27.7%,39.3%and100.0%when honeycomb cinders pretreated by HCl solution doses of20.0mg·L-1, pH of9.5, reaction temperature of20℃, reaction time of15min and settling time of20min. The UV spectrum analysis of raw/pretreated landfill leachate was manifested that the absorption peaks and intensities of pretreated landfill leachate were even fewer than these of raw landfill leachate. SEM-EDS analysis and XRD analysis of precipitates after experiment illustrated that the adsorption ability of honeycomb cinders pretreated by HCl solution was better than that of honeycomb cinders pretreated by other solutions. In kinetics of reactions, the results were shown that the rates of NH4+and CODcr reactions were closer to the third order kinetic model, and the rate of color reaction was closer to second/third order kinetic model. The honeycomb cinders adsorption method was characteristic of friendly environment, waste control by waste, simple operation, steady performance, low cost, occupying small area, et al. The precipitates after experiment could be reused.
(4) Pretreatment of landfill leachate by microwave digestion method. The color, CODcr and PO3-4removal efficiencies were obtained at75.0%,90.6%and100.0%, respectively, when microwave power of900W, pH of2.0and reaction time of15min. However, the NH4+removal efficiency was only6.5%. The UV spectrum analysis of raw/pretreated landfill leachate was manifested that the absorption peaks and intensities of pretreated landfill leachate were even fewer than these of raw landfill leachate. In kinetics of reactions, the results were shown that the rates of color and CODcr reactions were closer to the first order kinetic model. This method was advantages of good treatment effect, simple operation, occupying small area, none stench of the pretreated landfill leachate, none precipitates produced, which could be further developed and used.
(5) Pretreatment of landfill leachate by oxidation method using oxidants. In this research, KMnO4, NaClO, H2O2and Fenton were used as oxidants to pretreated raw landfill leachate. The results were demonstrated that the treatment efficiencies of landfill leachate using KMnO4as oxidant were as follows:color68.8%, NH4+14.4%, CODcr47.6%and PO3-4100.0%; the treatment efficiencies of landfill leachate using NaCIO as oxidant were as follows:color50.0%, NH4+40.8%, CODcr59.6%and PO3-4100.0%; the treatment efficiencies of landfill leachate using H2O2as oxidant were as follows:color68.8%, NH4+3.2%, CODcr53.9%and PO3-4100.0%; the treatment efficiencies of landfill leachate using Fenton as oxidant were as follows:color82.5%, NH4+10.1%, CODcr64.2%and PO3-4100.0%. The UV spectrum analysis of raw/pretreated landfill leachate was manifested that the absorption peaks and intensities of pretreated landfill leachate were even fewer than these of raw landfill leachate. In kinetics of reactions, the rates of NH4+and CODcr reactions were closer to third order kinetic model when KMnO4used as an oxidant. When NaCIO was used as an oxidant, the rate of NH4+reaction was closer to third order kinetic model, and the rate of CODcr reaction was closer to first order kinetic model. When H2O2was used as an oxidant, the rates of NH4+and CODcr reactions did not go well. When Fenton was used as an oxidant, the rate of NH4+reaction was closer to the third order kinetic model, and the CODcr reaction was closer to the second order kinetic model.
(6) Pretreatment of landfill leachate by microware-oxidants-struvite. Under the optimum conditions, the color, NH4+, CODcr, PO3-4and TS efficiencies of landfill leachate using microware-KMnO4-struvite were75.0%,100.0%,93.1%,100.0%and99.9%, respectively. The color, NH4+, CODcr, PO3-4and TS efficiencies of landfill leachate using microware-NaClO-struvite were75.0%,100.0%,91.5%,100.0%and99.9%, respectively. The color, NH4+, CODcr, PO3-4and TS efficiencies of landfill leachate using microware-H2O2-struvite were100.0%,100.0%,90.0%,100.0%and99.9%, respectively. The color, NH4+, CODcr, PO3-4and TS efficiencies of landfill leachate using microware-Fenton-struvite were100.0%,100.0%,92.0%,100.0%and99.9%, respectively. The UV spectrum analysis of raw/pretreated landfill leachate was manifested that the absorption peaks and intensities of pretreated landfill leachate were even fewer than these of raw landfill leachate. Moreover, the treatment effect of landfill leachate using microware-H2O2-struvite was the better than that of other combined methods.
The aim of this research was to propose deeper theory mechanism of classical method for landfill leachate, and provide new study directions of new pretreatment methods. The results of this research enriched techniques which we currently use, and could provide simply new combined physicochemical methods, which could supply new thinkings and processes for landfill leachate pretreatment. Thus, this research is provided with important theoretical significance and wide application.
(1)化学混凝法预处理垃圾渗滤液的研究。通常,化学混凝法用于处理老龄垃圾渗滤液,而本试验则采用此方法处理新鲜垃圾渗滤液。试验结果表明,在分别选用氯化铝(AlCl3)、硫酸铝(A12(SO4)3)、氯化铁(FeCl3)、硫酸铁(Fe2(SO4)3)和聚合氯化铝(PAC)作混凝剂预处理垃圾渗滤液的对比研究中,在优化投加量、pH值和反应时间等试验条件下,水质色度的去除效果为：PAC＞AlCl3＞FeCl3> A12(SO4)3=Fe2(SO4)3;总固体残渣量(TS)的去除效果为：PAC＞Fe2(SO4)3＞Al2(SO4)3＞FeCl3＞AICl3;氨氮(NH4+)的去除效果为：FeCl3＞Fe2(SO4)3＞A12(SO4)3＞PAC＞AlC13; CODcr的去除效果为：AICl3＞A12(SO4)3=Fe2(SO4)3＞PAC＞FeCl3。而P043-的去除率均达到100.0%。预处理后的水质经紫外光谱分析,发现其吸收峰比原水的明显减少,强度明显降低,且铝盐的混凝效果明显强于铁盐。反应的沉淀物分别经SEM-EDS分析,证明混凝法不但可以有效去除色度、TS、NH4+、CODcr和PO43-,还可以同时去除渗滤液中的一些无机阴离子和金属离子。并且,再次证明铝盐的去除效果比铁盐的更为显著。在反应动力学机理研究中,污染物的去除均属于二级或三级动力反应模型,反映出化学混凝法在较短时间内去除污染物的效果受限的原因。该方法具有操作简便、反应快速、占地面积小、运行稳定、处理效果较好等特点,但成本较高,容易产生大量的剩余污泥。
(2)磷酸铵镁化学法预处理垃圾渗滤液的研究。试验结果表明,当pH值为9.5、反应温度为20～30℃、[Mg2+]/[NH4+]/[P043-]摩尔比为1：1：1.4、反应时间为15min、静置时间为20min时,其水质最佳去除率为：色度81.3%,TS52.5%,NH4+100.0%,CODcr43.4%,且出水无PO43-。预处理后的水质经紫外光谱分析,发现其吸收峰比原水的明显减少,强度明显降低。试验后的沉淀物经SEM-EDS和XRD分析发现,该灰色沉淀物主要由三种结构组成,即立方型、针状型和圆柱型结构。其中,立方型和针状型结构为磷酸铵镁,圆柱型结构为磷酸镁。此外,结构表面还吸附着其他元素成分,说明该方法不但能有效去除NH4+,还可以通过吸附作用同时去除垃圾渗滤液中的其他污染物质。试验反应经动力学研究分析,属于一级反应动力模型。产物经提纯后,可作为一种缓释肥,加以回收利用。
(3)蜂窝煤渣吸附法预处理垃圾渗滤液的研究。分别选用蒸馏水、氢氧化钠溶液、盐酸溶液、乙醇和乙酸预处理蜂窝煤渣。试验结果表明,盐酸溶液预处理后的蜂窝煤渣,其性状变化最为明显。当其投加量为20.0mg·L-1、pH值为9.5、反应温度为20℃、反应时间为15min、静置时间为20min时,渗滤液中污染物质的去除效果最佳：色度61.3%,TS52.5%,NH4+27.7%,CODcr39.3%,P043-100.0%。预处理后的水质经紫外光谱分析,发现其吸收峰比原水的明显减少,强度明显降低。试验后的沉淀物经SEM-EDS和XRD分析发现,HCl溶液预处理后的蜂窝煤渣的吸附性能最优。通过反应动力学模型研究发现,NH4+和CODcr的吸附均属于三级反应动力模型,色度的吸附属于二、三级反应动力模型。说明其去除速率较慢。该方法具有环境友好、以废治废、操作简便、性能稳定、成本低廉、占地面积小等特点。试验后的剩余沉淀物,可以回收利用。
(4)微波法预处理垃圾渗滤液的研究。试验结果表明,当微波功率为900W,pH值为2.0,反应时间为15min时,其水质最佳去除率为：色度75.0%,CODcr90.6%,PO43-100.0%,而NH4+的去除率很低,仅为6.5%。预处理后的水质经紫外光谱分析,发现其吸收峰比原水的明显减少,强度明显降低。在动力学研究中发现,色度和CODcr的去除均属于一级反应动力模型。该方法操作简便,处理效果好,占地面积小,且处理后的垃圾渗滤液,恶臭味消除,没有剩余残渣沉淀存在,具有进一步开发利用的潜力。
(5)氧化剂氧化法预处理垃圾渗滤液的研究。分别选用高锰酸钾(KMnO4).次氯酸钠(NaCIO).双氧水(H202)和芬顿试剂(Fenton)作氧化剂预处理垃圾渗滤液。试验结果表明,在优化投加量、pH值和反应时间等试验条件下,其水质最佳去除率分别为,KMn04:色度68.8%,NH4+14.4%,CODcr47.6%,PO3-4100.0%:NaClO:色度50.0%,NH4+40.8%,CODcr59.6%,PO3-4100.0%;H2O2:色度68.8%,NH4+3.2%,CODcr53.9%,PO34100.0%；Fenton:色度82.5%,NH4+10.1%,CODcr64.2%,PO3-4100.0%。预处理后的水质经紫外光谱分析,发现其吸收峰均比原水的明显减少,强度明显降低。在动力学研究中,采用KMnO4作氧化剂时,NH4+和CODcr均属于三级反应动力学模型；采用NaClO作氧化剂时,NH4+属于三级反应动力学模型,CODcr属于一级反应动力学模型；采用H202作氧化剂时,NH4+和CODcr的反应动力学模型均拟合得并不理想；采用Fenton作氧化剂时,NH4+属于三级反应动力学模型,CODcr属于二级反应动力学模型。
(6)微波-氧化剂-磷酸铵镁联合预处理垃圾渗滤液的研究。试验结果表明,在最佳试验条件下,水质的最佳去除效果分别为,微波+KMnO4+磷酸铵镁：色度75.0%,NH4+100.0%,CODcr93.1%,P03-4100.0%,TS99.9%;微波+NaC10+磷酸铵镁：色度75.0%,NH4+100.0%,CODcr91.5%,PO3-4100.0%,TS99.9%;微波+H202+磷酸铵镁：色度100.0%,NH4+100.0%,CODcr90.0%,P043-100.0％,TS99.9%；微波+Fenton+磷酸铵镁：色度100.0%,NH4+100.0%,CODcr92.0%,PO43-100.0%,TS99.9%。预处理后的水质经紫外光谱分析,发现其吸收峰均比原水的明显减少,强度明显降低,且微波+Fenton+磷酸铵镁组合处理后的水质最为显著。
本课题的研究为垃圾渗滤液的经典处理方法提出深层的理论机理,同时为新的处理方法提供了新的探索方向。研究结果丰富了现有垃圾渗滤液的处理技术,并可能开发出简单的物化协同处理工艺,为垃圾渗滤液的处理提供了新的思路与方法。因此,本课题具有重要的理论意义和应用前景。
Along with the development of industry and the remarkable improvement of people's living standard, the domestic garbage has been grown rapidly, which leads to particular attention to landfill leachate. The characteristics of landfill leachate are strong stench, abundance of complicated compositions and high toxicity that are difficult to be disposed by biological treatment methods. Therefore, the pretreatment methods of landfill leachate are particularly important. The aim of this research is to lucubrate the classical technologies and develop new technologies. Chemical coagulation, struvite, adsorption method by honeycomb cinders, microwave digestion method and oxidation method had been used in landfill leachate pretreatment. From these studies, it could be obtained high efficient processes and mechanisms of actions, which could be provided data base, theoretical directions and applications references. The contents of this research mainly included as follows:
(1) Coagulation method. In this research, the coagulation method would be adopted to pretreat fresh landfill leachate, which generally used to pretreat old landfill leachate. AICl3, A12(SO4)3, FeCl3, Fe2(SO4)3and PAC were used as coagulants. Under optimum conditions such as coagulants doses, pH and reaction time, the results of experiments were shown as follows:the color efficiency:PAC＞AlCl3＞FeCl3＞A12(SO4)3=Fe2(SO4)3; the TS efficiency:PAC＞Fe2(SO4)3＞Al2(SO4)3＞FeCl3＞AlCl3; the NH4+efficiency:FeCl3＞Fe2(SO4)3＞Al2(SO4)3>PAC＞AlCl3; the CODcr efficiency:AlCl3>A12(SO4)3=Fe2(S04)3>PAC＞FeCl3. And the PO3-4efficiencies were all obtained at100.0%in this experiment using different coagulants. The UV spectrum analysis of raw/pretreated landfill leachate was manifested that the absorption peaks and intensities of pretreated landfill leachate were even fewer than these of raw landfill leachate. And the effects on the pretreatment of landfill leachate by aluminum salt as coagulants were better than that of ferric salt as coagulants. The SEM-EDS analysis of precipitates after experiments was demonstrated that the coagulation methods were not only used to effectively remove color, TS, NH4+, CODcr and PO3-4, but also used to effectively remove some inorganic and metal anions in raw landfill leachate. Furthermore, It was certified that the coagulation performance of aluminum salt coagulants were better than that of ferric salt coagulants for pretreatment of landfill leachate once again. In kinetics of reactions, the results were shown that the rates of reactions were closer to the second/third order kinetic model, which could explain the reasons of low removal efficiencies of pollutants in raw landfill leachate with short time. This method was characteristics of operate simple, rapid reaction, small occupied area, steady performance and great treatment efficiencies, et al. However, the disadvantages of this method were high cost and abundant of excess sludge produced.
(2) Pretreatment of landfill leachate by struvite method. In this research, when pH was9.5, reaction temperature was20-30℃, the molar ratio of [Mg2+]/[NH4+]/[PO43-] was1:1:1.4, the reaction time was15min and the settling time was20min, the efficiencies of color, TS, NH4+and CODcr were obtained at81.3%,52.5%,100.0%and43.4%, respectively. And no surplus PO3-4existed in pretreated landfill leachate. The UV spectrum analysis of raw/pretreated landfill leachate was manifested that the absorption peaks and intensities of pretreated landfill leachate were even fewer than these of raw landfill leachate. The SEM-EDS analysis of precipitates after struvite method was demonstrated that the structures of precipitate mainly included cubic, acicular and cylinder crystals. In particularly, the cubic and acicular crystals were identified as struvite, and the cylinder crystals were identified as magnesium phosphate. In addition, the surface of crystals was surrounded by other elements, which confirmed that this method could not only remove NH4+, but also remove other pollutant in raw landfill leachate. In kinetics of reactions, the results were shown that the rate of reaction were closer to the first order kinetic model. The precipitates after experiment could be reused as slow release fertilizer by purification.
(3) Pretreatment of landfill leachate by honeycomb cinders adsorption method. The honcycomb cinders were pretreated by distilled water, NaOH solution, HCl solution, CH3CH2OH and CH3COOH, respectively. The results of this experiment showed that the color, TS, NH4+, CODcr and PO3-4removal efficiencies were61.3%,52.5%,27.7%,39.3%and100.0%when honeycomb cinders pretreated by HCl solution doses of20.0mg·L-1, pH of9.5, reaction temperature of20℃, reaction time of15min and settling time of20min. The UV spectrum analysis of raw/pretreated landfill leachate was manifested that the absorption peaks and intensities of pretreated landfill leachate were even fewer than these of raw landfill leachate. SEM-EDS analysis and XRD analysis of precipitates after experiment illustrated that the adsorption ability of honeycomb cinders pretreated by HCl solution was better than that of honeycomb cinders pretreated by other solutions. In kinetics of reactions, the results were shown that the rates of NH4+and CODcr reactions were closer to the third order kinetic model, and the rate of color reaction was closer to second/third order kinetic model. The honeycomb cinders adsorption method was characteristic of friendly environment, waste control by waste, simple operation, steady performance, low cost, occupying small area, et al. The precipitates after experiment could be reused.
(4) Pretreatment of landfill leachate by microwave digestion method. The color, CODcr and PO3-4removal efficiencies were obtained at75.0%,90.6%and100.0%, respectively, when microwave power of900W, pH of2.0and reaction time of15min. However, the NH4+removal efficiency was only6.5%. The UV spectrum analysis of raw/pretreated landfill leachate was manifested that the absorption peaks and intensities of pretreated landfill leachate were even fewer than these of raw landfill leachate. In kinetics of reactions, the results were shown that the rates of color and CODcr reactions were closer to the first order kinetic model. This method was advantages of good treatment effect, simple operation, occupying small area, none stench of the pretreated landfill leachate, none precipitates produced, which could be further developed and used.
(5) Pretreatment of landfill leachate by oxidation method using oxidants. In this research, KMnO4, NaClO, H2O2and Fenton were used as oxidants to pretreated raw landfill leachate. The results were demonstrated that the treatment efficiencies of landfill leachate using KMnO4as oxidant were as follows:color68.8%, NH4+14.4%, CODcr47.6%and PO3-4100.0%; the treatment efficiencies of landfill leachate using NaCIO as oxidant were as follows:color50.0%, NH4+40.8%, CODcr59.6%and PO3-4100.0%; the treatment efficiencies of landfill leachate using H2O2as oxidant were as follows:color68.8%, NH4+3.2%, CODcr53.9%and PO3-4100.0%; the treatment efficiencies of landfill leachate using Fenton as oxidant were as follows:color82.5%, NH4+10.1%, CODcr64.2%and PO3-4100.0%. The UV spectrum analysis of raw/pretreated landfill leachate was manifested that the absorption peaks and intensities of pretreated landfill leachate were even fewer than these of raw landfill leachate. In kinetics of reactions, the rates of NH4+and CODcr reactions were closer to third order kinetic model when KMnO4used as an oxidant. When NaCIO was used as an oxidant, the rate of NH4+reaction was closer to third order kinetic model, and the rate of CODcr reaction was closer to first order kinetic model. When H2O2was used as an oxidant, the rates of NH4+and CODcr reactions did not go well. When Fenton was used as an oxidant, the rate of NH4+reaction was closer to the third order kinetic model, and the CODcr reaction was closer to the second order kinetic model.
(6) Pretreatment of landfill leachate by microware-oxidants-struvite. Under the optimum conditions, the color, NH4+, CODcr, PO3-4and TS efficiencies of landfill leachate using microware-KMnO4-struvite were75.0%,100.0%,93.1%,100.0%and99.9%, respectively. The color, NH4+, CODcr, PO3-4and TS efficiencies of landfill leachate using microware-NaClO-struvite were75.0%,100.0%,91.5%,100.0%and99.9%, respectively. The color, NH4+, CODcr, PO3-4and TS efficiencies of landfill leachate using microware-H2O2-struvite were100.0%,100.0%,90.0%,100.0%and99.9%, respectively. The color, NH4+, CODcr, PO3-4and TS efficiencies of landfill leachate using microware-Fenton-struvite were100.0%,100.0%,92.0%,100.0%and99.9%, respectively. The UV spectrum analysis of raw/pretreated landfill leachate was manifested that the absorption peaks and intensities of pretreated landfill leachate were even fewer than these of raw landfill leachate. Moreover, the treatment effect of landfill leachate using microware-H2O2-struvite was the better than that of other combined methods.
The aim of this research was to propose deeper theory mechanism of classical method for landfill leachate, and provide new study directions of new pretreatment methods. The results of this research enriched techniques which we currently use, and could provide simply new combined physicochemical methods, which could supply new thinkings and processes for landfill leachate pretreatment. Thus, this research is provided with important theoretical significance and wide application.
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