絮凝和氧化—絮凝耦合去除废水中As（Ⅲ）的研究
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摘要
砷的应用范围广、毒性大,尤其是三价砷。随着地表水砷标准的进一步严格,砷污染问题更加突出。
针对水中三价砷(As(Ⅲ))的去除,探讨了铁盐絮凝和铁盐/H_2O_2氧化-絮凝除As(Ⅲ)的效果及相关的机理。
以5mg/L的As(Ⅲ)模拟废水为处理对象,对比了FeSO_4和Fe_2(SO_4)_3絮凝除As(Ⅲ)的效果,结果表明:絮凝除砷时,Fe(Ⅱ)比Fe(Ⅲ)有更高的去除率。红外光谱和Zeta电位分析表明Fe(Ⅱ)和Fe(Ⅲ)水解时产物的结构及表面电位值基本相同,而比表面积和粒度分布测试结果显示Fe(Ⅱ)的水解产物比Fe(Ⅲ)水解产物有更大的比表面积和更小的粒度,因此,能将更多的As(Ⅲ)吸附及共沉淀到表面。
采用Fe(Ⅱ)/H_2O_2(Fenton)及Fe(Ⅲ)/H_2O_2(类Fenton)氧化-絮凝去除水中的As(Ⅲ),结果表明:Fenton氧化-絮凝对As(Ⅲ)的去除率可以达到96%以上,而类Fenton法的去除率仅有70%左右。两种氧化-絮凝除As(Ⅲ)过程的开路电位-时间曲线、以及所形成絮体的红外光谱分析表明:Fenton氧化-絮凝过程中As(Ⅲ)被更有效的氧化为五价砷(As(Ⅴ)),且氧化与絮凝之间形成耦合作用。
用聚合硫酸铁(PFS)替代部分FeSO_4,考察了FeSO_4/PFS、絮凝pH值、氧化剂和絮凝剂投加量,以及不同As(Ⅲ)初始浓度等因素对As(Ⅲ)去除效果的影响。结果表明:按摩尔比FeSO_4/PFS=6/9,絮凝pH=7,氧化剂和絮凝剂的投加量分别为20mg/L和15mg/L(以[Fe]_T计)时,对废水中浓度为0.5~10mg/L砷的去除率均为90%以上,FeSO_4/PFS/H_2O_2氧化-絮凝耦合工艺对水质变化有较强的抗冲击能力,可增强氧化-絮凝工艺絮体的沉降性能,并且对硫酸厂和有色金属冶炼厂的含砷废水的总砷去除率均可达97%以上,对工业含砷废水的去除具有一定使用参考价值。
The arsenic is applied abroad, and is a toxic trace element, especially arsenite. With the arsenic standard of ground water been further stricted, the problem of arsenic contamination is more prominent.
The removal efficiency and mechanisms of As(Ⅲ) were investigated, which was removed by iron flocculation and H_2O_2 oxidation coupled with iron flocculation process.
For the synthetic wastewater that simply contained 5mg/L As(Ⅲ), the removal efficiency of arsenic by FeSO_4 flocculation was higher than Fe_2(SO_4)_3 flocculation. The results of infrared absorption and zeta potential showed that the hydrolysis products forms and surface electric potential of Fe(Ⅱ) and Fe(Ⅲ) hydrolyzing were same, while the results of surface area and particle size distribution showed that the hydrolysis products of Fe(Ⅱ) had bigger surface area and smaller particle size than the hydrolysis products of Fe(Ⅲ), therefore, Fe(Ⅱ) flocculation could adsorb more As(Ⅲ).
Fe(Ⅱ)/H_2O_2(Fenton) and Fe(Ⅲ)/H_2O_2(Fenton-like) oxidation coupled with flocculation were used in removing arsenic, and the removal efficiency of arsenic by Fenton oxidation coupled with flocculation reached more than 96%, while Fenton-like oxidation coupled with flocculation was only about 70%. The results of open circuit potential - time curve and infrared absorption indicated that As(Ⅲ) was oxidized to As(Ⅴ) more effectively by Fenton oxidation coupled with flocculation, and there was a coupled process between oxidation and flocculation.
The part FeSO_4 was replaced by poly ferric sulfate(PFS), and then the influences of FeSO_4/PFS, pH value of flocculation, dosage of oxidant and flocculant, and the different initial concentration of As(Ⅲ) were investigated. The results showed that the mole rate of FeSO_4/PFS was 6/9, and pH value of flocculation was 7, and the dosage of oxidant and flocculant were 20 and 15mg/L, respectively, then the removal efficiency of As(Ⅲ) with 0.5~10mg/L was more than 90%. The FeSO_4/PFS/H_2O_2 oxidation coupled with flocculation process had a stronger capability to suit large concentration change of arsenic, and enhanced the sedimentation performance of flocs. The process could also reach excellent removal effect for arsenic in sulfuric acid plant and non-ferrous smelting plan wastewater, and the removal efficiency was more than 97%, which has a reference value to treat arsenic in the industrial wastewater.
针对水中三价砷(As(Ⅲ))的去除,探讨了铁盐絮凝和铁盐/H_2O_2氧化-絮凝除As(Ⅲ)的效果及相关的机理。
以5mg/L的As(Ⅲ)模拟废水为处理对象,对比了FeSO_4和Fe_2(SO_4)_3絮凝除As(Ⅲ)的效果,结果表明:絮凝除砷时,Fe(Ⅱ)比Fe(Ⅲ)有更高的去除率。红外光谱和Zeta电位分析表明Fe(Ⅱ)和Fe(Ⅲ)水解时产物的结构及表面电位值基本相同,而比表面积和粒度分布测试结果显示Fe(Ⅱ)的水解产物比Fe(Ⅲ)水解产物有更大的比表面积和更小的粒度,因此,能将更多的As(Ⅲ)吸附及共沉淀到表面。
采用Fe(Ⅱ)/H_2O_2(Fenton)及Fe(Ⅲ)/H_2O_2(类Fenton)氧化-絮凝去除水中的As(Ⅲ),结果表明:Fenton氧化-絮凝对As(Ⅲ)的去除率可以达到96%以上,而类Fenton法的去除率仅有70%左右。两种氧化-絮凝除As(Ⅲ)过程的开路电位-时间曲线、以及所形成絮体的红外光谱分析表明:Fenton氧化-絮凝过程中As(Ⅲ)被更有效的氧化为五价砷(As(Ⅴ)),且氧化与絮凝之间形成耦合作用。
用聚合硫酸铁(PFS)替代部分FeSO_4,考察了FeSO_4/PFS、絮凝pH值、氧化剂和絮凝剂投加量,以及不同As(Ⅲ)初始浓度等因素对As(Ⅲ)去除效果的影响。结果表明:按摩尔比FeSO_4/PFS=6/9,絮凝pH=7,氧化剂和絮凝剂的投加量分别为20mg/L和15mg/L(以[Fe]_T计)时,对废水中浓度为0.5~10mg/L砷的去除率均为90%以上,FeSO_4/PFS/H_2O_2氧化-絮凝耦合工艺对水质变化有较强的抗冲击能力,可增强氧化-絮凝工艺絮体的沉降性能,并且对硫酸厂和有色金属冶炼厂的含砷废水的总砷去除率均可达97%以上,对工业含砷废水的去除具有一定使用参考价值。
The arsenic is applied abroad, and is a toxic trace element, especially arsenite. With the arsenic standard of ground water been further stricted, the problem of arsenic contamination is more prominent.
The removal efficiency and mechanisms of As(Ⅲ) were investigated, which was removed by iron flocculation and H_2O_2 oxidation coupled with iron flocculation process.
For the synthetic wastewater that simply contained 5mg/L As(Ⅲ), the removal efficiency of arsenic by FeSO_4 flocculation was higher than Fe_2(SO_4)_3 flocculation. The results of infrared absorption and zeta potential showed that the hydrolysis products forms and surface electric potential of Fe(Ⅱ) and Fe(Ⅲ) hydrolyzing were same, while the results of surface area and particle size distribution showed that the hydrolysis products of Fe(Ⅱ) had bigger surface area and smaller particle size than the hydrolysis products of Fe(Ⅲ), therefore, Fe(Ⅱ) flocculation could adsorb more As(Ⅲ).
Fe(Ⅱ)/H_2O_2(Fenton) and Fe(Ⅲ)/H_2O_2(Fenton-like) oxidation coupled with flocculation were used in removing arsenic, and the removal efficiency of arsenic by Fenton oxidation coupled with flocculation reached more than 96%, while Fenton-like oxidation coupled with flocculation was only about 70%. The results of open circuit potential - time curve and infrared absorption indicated that As(Ⅲ) was oxidized to As(Ⅴ) more effectively by Fenton oxidation coupled with flocculation, and there was a coupled process between oxidation and flocculation.
The part FeSO_4 was replaced by poly ferric sulfate(PFS), and then the influences of FeSO_4/PFS, pH value of flocculation, dosage of oxidant and flocculant, and the different initial concentration of As(Ⅲ) were investigated. The results showed that the mole rate of FeSO_4/PFS was 6/9, and pH value of flocculation was 7, and the dosage of oxidant and flocculant were 20 and 15mg/L, respectively, then the removal efficiency of As(Ⅲ) with 0.5~10mg/L was more than 90%. The FeSO_4/PFS/H_2O_2 oxidation coupled with flocculation process had a stronger capability to suit large concentration change of arsenic, and enhanced the sedimentation performance of flocs. The process could also reach excellent removal effect for arsenic in sulfuric acid plant and non-ferrous smelting plan wastewater, and the removal efficiency was more than 97%, which has a reference value to treat arsenic in the industrial wastewater.
引文
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