Fenton氧化和MAP化学沉淀工艺深度处理垃圾渗滤液
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摘要
卫生填埋方式会产生大量的垃圾渗滤液。由于垃圾渗滤液的成分极其复杂,含有大量的重金属离子和难生物降解的有机物,是一种有毒有害的高浓度有机废水,而且垃圾渗滤液的水质水量受多种因素影响,变化很大,因此仅采用单个的生物处理工艺技术很难实现垃圾渗滤液的达标排放。因此,要实现垃圾渗滤液处理达标排放的目的,必须经过深度处理。
首先研究了在联合工艺处理垃圾渗滤液中污染物组成的变化。通过对渗滤液中溶解性有机物质(DOM)的分离以及采用GC-MS联用仪对垃圾渗滤液中的有机微污染物的鉴定,以及对各工艺处理的渗滤液出水中金属离子组分的分离、鉴定和Visual MINTEQ模型拟合预测,结果表明,经过联合处理工艺,尽管出水水质达到国家一级排放标准,但最后出水中的总的金属离子浓度和无机阴离子浓度仍高于周围的水体环境。因此,渗滤液出水中的重金属和无机污染物仍是对环境造成污染的主要污染源,由此可能带来的环境风险不可忽视。
此外,着重研究探讨了Fenton反应过程中的氧化作用和混凝作用分别对以化学需氧量(COD)为代表的渗滤液总污染物浓度,以及渗滤液中分离出的腐殖酸为代表的单个污染物的去除特性。采用单因素实验和响应曲面优化设计实验(RSM),分析了试验影响因素,优化了反应条件。结果表明,渗滤液中腐殖酸的去除对整体污染物的去除具有决定性的作用。COD的变化曲线与腐殖酸的相似,但腐殖酸的去除率要高于COD大约30%。渗滤液中大部分的腐殖酸被Fenton试剂氧化降解为低分子的有机物而不是完全矿化生成CO2和水。Fenton的氧化作用对混凝去除作用有显著的影响。在一定的投量范围内,氧化和混凝作用分别与双氧水和Fe~(2+)投量呈线性关系。在较低的双氧水与Fe~(2+)摩尔比([H_2O_2]/[Fe~(2+)]<3.0)条件下,Fe~(2+)投量对混凝作用有显著影响,而当[H_2O_2]/[Fe~(2+)]摩尔比过高,Fe~(2+)投量对混凝作用的影响不显著。氧化作用对混凝去除腐殖酸的作用影响很小。在低Fe~(2+)投量时,温度与氧化去除率成正比,但高Fe~(2+)投量时,温度对氧化作用影响不大。
在优化工艺的基础上,首先使用经典的羟氧自由基氧化腐殖酸的化学动力学模型描述Fenton氧化降解腐殖酸过程,同时采用新建的数学统计表观动力学模型探讨Fenton试剂有效处理难生化降解的反渗透浓缩渗滤液的动力学规律。结果表明,Fenton试剂投量、污染物初始浓度、初始pH值以及温度显著地影响Fenton氧化降解污染物的速率与氧化去除率。随着Fenton试剂投量的增大,双氧水和Fe~(2+)将会达到一个饱和的临界浓度状态。通过对模型的实验验证,表明模型与实验值吻合最好,能够从数学和化学的角度对Fenton氧化降解过程进行过程描述和工艺优化。
最后,采用响应曲面法(Response surface methodology,RSM)设计优化鸟粪石化学沉淀法对废水中氨氮去除的工艺参数,并在最佳工艺参数条件下,使用化学平衡软件Visual MINTEQ计算拟合磷酸铵镁平衡体系中Mg~(2+),NH_4~+-N和PO_4~(3-)-P各组分在不同pH条件下的分布变化及饱和指数(SI)的变化。实验和预测结果表明化学模型对MAP沉淀平衡体系拟合良好。本研究的pH范围内(8.0~11.0),在低浓度氨氮废水中,pH是显著的影响因素。而高浓度氨氮废水中,P/N摩尔比是主要的限制因素。在本实验研究范围内,能够使用化学平衡模型Visual MINTEQ预测人工模拟氨氮废水中通过磷酸铵镁沉淀而去除的NH_4~+-N;二次响应RSM模型能预测本实验研究的敞开体系中所有氨氮的去除,包括通过MAP沉淀和氨气挥发而去除的氨氮。
Sanitary landfills are the primary method currently used for municipal solid waste disposal in many countries. Landfill leachate is defined as a high-strength wastewater exhibiting acute and chronic toxicity percolating through deposited waste and emitted within a landfill or dump site through external sources. The characterization of the leachate composition of municipal landfill leachate exhibits noticeably temporal and site-specific variation by the fact that its production and composition may vary as a function of landfill age. However, a biological process alone is not effective enough to remove the bulk of refractory pollutants in landfill leachate. Hence, the advanced treatment of landfill leachate needs to be specific concentrated.
Firstly, the transformation of pollutions including humic substances, microorganic pollutants, and heavy metals in landfill leachate treated by a combined technology were investigated by fractionation technology of dissolved organic matters (DOM) and gas chromatography-mass spectroscopy (GC-MS) analysis, as well as the physical fraction of metal speciation and prediction using Visual MINTEQ programmer. The observations indicated that leachate treated by the combined process still contained higher concentration of total heavy metals and inorganic anions than the surrounding water environment, though no violation to effluent standard was found. The possible risk in leachate should not be negligible because landfill leachate was still one of the major sources of heavy metals and inorganic pollutants discharged to the surrounding environment.
In addition, our study was focus on the oxidation and coagulation performances of Fenton treatment on chemical oxygen demand (COD) and humic substances removal, where COD was characterized as total organic constituents and the isolated humic substances was characterized as an individual organic contaminant in landfill leachate. The response surface method (RSM) was applied to evaluate and optimize the interactive effects of the operating variables including initial pH and dosages of H_2O_2 and Fe~(2+) on physical and oxidative performances of Fenton process. The change curves of humic acids removal were similar to those of COD. The removal of humic acids was 30% higher than COD removal, which indicated that humic acids was mostly degraded into various intermediate organic compounds but not mineralized by Fenton reagents. The oxidation removal was greatly influenced by initial pH relative to the coagulation removal. The oxidation and coagulation removals were linearly dependent with hydrogen peroxide and ferrous dosages, respectively. Ferrous dosage greatly influenced the coagulation removal of COD at low ratio ([H_2O_2]/[Fe~(2+)]<3.0), but not at extremely high ratio ([H_2O_2]/[Fe~(2+)]>6.0). The coagulation removal of humic acids was not affected obviously by oxidation due to both Fenton oxidation and coagulation remove high molecular weight organics preferentially. Higher temperature gave a positive effect on oxidation removal at low Fe~(2+) dosage, but this effect was not obvious at high Fe~(2+) dosage.
Based on the optimization of Fenton reaction, a new kinetic model was established according to the generally accepted mechanism of high active ?OH oxidation in order to well describe the Fenton oxidation reaction in humic acids aqueous solution, and a mathematics model was derived successfully to describe the two-stage reaction kinetics of Fenton treatment of landfill leachate. Results indicated that the oxidation rate and removal efficiency were strongly dependent on initial pH, initial concentration of Fenton reagents, initial HA concentration and reaction temperature. The experiments demonstrated that hydrogen peroxide and ferrous ion would approach their saturated value with increasing dosage. It was found to be very useful for chemically and mathematically evaluating the performance of Fenton system and/or for process design using these models under various experimental conditions.
Finally, improvement availability for high-level removal of ammonium-nitrogen by struvite using response surface methodology (RSM) was investigated, and chemical equilibrium model Visual MINTEQ, was used to calculate the equilibrium speciation in aqueous solution and solid phases, saturation index (SI), as well as to model the availability of Mg~(2+), NH_4~+, and PO_4~(3-) ions as a function of pH. The predicted and experimental data suggested that the model described the experiments well. The solution pH value was an important parameter in ammonium-nitrogen removal at low initial NH_4~+-N concentration. P/N molar ratio was a limiting factor on struvite precipitation at high initial NH_4~+-N concentration. The quadratic statistical modeling developed using RSM can be used to predict total NH4+-N removal within the ranges of the factors investigated; moreover, the chemical thermodynamics equilibrium model can be used to pre-determine the concentration of ammonium precipitated by struvite.
首先研究了在联合工艺处理垃圾渗滤液中污染物组成的变化。通过对渗滤液中溶解性有机物质(DOM)的分离以及采用GC-MS联用仪对垃圾渗滤液中的有机微污染物的鉴定,以及对各工艺处理的渗滤液出水中金属离子组分的分离、鉴定和Visual MINTEQ模型拟合预测,结果表明,经过联合处理工艺,尽管出水水质达到国家一级排放标准,但最后出水中的总的金属离子浓度和无机阴离子浓度仍高于周围的水体环境。因此,渗滤液出水中的重金属和无机污染物仍是对环境造成污染的主要污染源,由此可能带来的环境风险不可忽视。
此外,着重研究探讨了Fenton反应过程中的氧化作用和混凝作用分别对以化学需氧量(COD)为代表的渗滤液总污染物浓度,以及渗滤液中分离出的腐殖酸为代表的单个污染物的去除特性。采用单因素实验和响应曲面优化设计实验(RSM),分析了试验影响因素,优化了反应条件。结果表明,渗滤液中腐殖酸的去除对整体污染物的去除具有决定性的作用。COD的变化曲线与腐殖酸的相似,但腐殖酸的去除率要高于COD大约30%。渗滤液中大部分的腐殖酸被Fenton试剂氧化降解为低分子的有机物而不是完全矿化生成CO2和水。Fenton的氧化作用对混凝去除作用有显著的影响。在一定的投量范围内,氧化和混凝作用分别与双氧水和Fe~(2+)投量呈线性关系。在较低的双氧水与Fe~(2+)摩尔比([H_2O_2]/[Fe~(2+)]<3.0)条件下,Fe~(2+)投量对混凝作用有显著影响,而当[H_2O_2]/[Fe~(2+)]摩尔比过高,Fe~(2+)投量对混凝作用的影响不显著。氧化作用对混凝去除腐殖酸的作用影响很小。在低Fe~(2+)投量时,温度与氧化去除率成正比,但高Fe~(2+)投量时,温度对氧化作用影响不大。
在优化工艺的基础上,首先使用经典的羟氧自由基氧化腐殖酸的化学动力学模型描述Fenton氧化降解腐殖酸过程,同时采用新建的数学统计表观动力学模型探讨Fenton试剂有效处理难生化降解的反渗透浓缩渗滤液的动力学规律。结果表明,Fenton试剂投量、污染物初始浓度、初始pH值以及温度显著地影响Fenton氧化降解污染物的速率与氧化去除率。随着Fenton试剂投量的增大,双氧水和Fe~(2+)将会达到一个饱和的临界浓度状态。通过对模型的实验验证,表明模型与实验值吻合最好,能够从数学和化学的角度对Fenton氧化降解过程进行过程描述和工艺优化。
最后,采用响应曲面法(Response surface methodology,RSM)设计优化鸟粪石化学沉淀法对废水中氨氮去除的工艺参数,并在最佳工艺参数条件下,使用化学平衡软件Visual MINTEQ计算拟合磷酸铵镁平衡体系中Mg~(2+),NH_4~+-N和PO_4~(3-)-P各组分在不同pH条件下的分布变化及饱和指数(SI)的变化。实验和预测结果表明化学模型对MAP沉淀平衡体系拟合良好。本研究的pH范围内(8.0~11.0),在低浓度氨氮废水中,pH是显著的影响因素。而高浓度氨氮废水中,P/N摩尔比是主要的限制因素。在本实验研究范围内,能够使用化学平衡模型Visual MINTEQ预测人工模拟氨氮废水中通过磷酸铵镁沉淀而去除的NH_4~+-N;二次响应RSM模型能预测本实验研究的敞开体系中所有氨氮的去除,包括通过MAP沉淀和氨气挥发而去除的氨氮。
Sanitary landfills are the primary method currently used for municipal solid waste disposal in many countries. Landfill leachate is defined as a high-strength wastewater exhibiting acute and chronic toxicity percolating through deposited waste and emitted within a landfill or dump site through external sources. The characterization of the leachate composition of municipal landfill leachate exhibits noticeably temporal and site-specific variation by the fact that its production and composition may vary as a function of landfill age. However, a biological process alone is not effective enough to remove the bulk of refractory pollutants in landfill leachate. Hence, the advanced treatment of landfill leachate needs to be specific concentrated.
Firstly, the transformation of pollutions including humic substances, microorganic pollutants, and heavy metals in landfill leachate treated by a combined technology were investigated by fractionation technology of dissolved organic matters (DOM) and gas chromatography-mass spectroscopy (GC-MS) analysis, as well as the physical fraction of metal speciation and prediction using Visual MINTEQ programmer. The observations indicated that leachate treated by the combined process still contained higher concentration of total heavy metals and inorganic anions than the surrounding water environment, though no violation to effluent standard was found. The possible risk in leachate should not be negligible because landfill leachate was still one of the major sources of heavy metals and inorganic pollutants discharged to the surrounding environment.
In addition, our study was focus on the oxidation and coagulation performances of Fenton treatment on chemical oxygen demand (COD) and humic substances removal, where COD was characterized as total organic constituents and the isolated humic substances was characterized as an individual organic contaminant in landfill leachate. The response surface method (RSM) was applied to evaluate and optimize the interactive effects of the operating variables including initial pH and dosages of H_2O_2 and Fe~(2+) on physical and oxidative performances of Fenton process. The change curves of humic acids removal were similar to those of COD. The removal of humic acids was 30% higher than COD removal, which indicated that humic acids was mostly degraded into various intermediate organic compounds but not mineralized by Fenton reagents. The oxidation removal was greatly influenced by initial pH relative to the coagulation removal. The oxidation and coagulation removals were linearly dependent with hydrogen peroxide and ferrous dosages, respectively. Ferrous dosage greatly influenced the coagulation removal of COD at low ratio ([H_2O_2]/[Fe~(2+)]<3.0), but not at extremely high ratio ([H_2O_2]/[Fe~(2+)]>6.0). The coagulation removal of humic acids was not affected obviously by oxidation due to both Fenton oxidation and coagulation remove high molecular weight organics preferentially. Higher temperature gave a positive effect on oxidation removal at low Fe~(2+) dosage, but this effect was not obvious at high Fe~(2+) dosage.
Based on the optimization of Fenton reaction, a new kinetic model was established according to the generally accepted mechanism of high active ?OH oxidation in order to well describe the Fenton oxidation reaction in humic acids aqueous solution, and a mathematics model was derived successfully to describe the two-stage reaction kinetics of Fenton treatment of landfill leachate. Results indicated that the oxidation rate and removal efficiency were strongly dependent on initial pH, initial concentration of Fenton reagents, initial HA concentration and reaction temperature. The experiments demonstrated that hydrogen peroxide and ferrous ion would approach their saturated value with increasing dosage. It was found to be very useful for chemically and mathematically evaluating the performance of Fenton system and/or for process design using these models under various experimental conditions.
Finally, improvement availability for high-level removal of ammonium-nitrogen by struvite using response surface methodology (RSM) was investigated, and chemical equilibrium model Visual MINTEQ, was used to calculate the equilibrium speciation in aqueous solution and solid phases, saturation index (SI), as well as to model the availability of Mg~(2+), NH_4~+, and PO_4~(3-) ions as a function of pH. The predicted and experimental data suggested that the model described the experiments well. The solution pH value was an important parameter in ammonium-nitrogen removal at low initial NH_4~+-N concentration. P/N molar ratio was a limiting factor on struvite precipitation at high initial NH_4~+-N concentration. The quadratic statistical modeling developed using RSM can be used to predict total NH4+-N removal within the ranges of the factors investigated; moreover, the chemical thermodynamics equilibrium model can be used to pre-determine the concentration of ammonium precipitated by struvite.
引文
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