Removal of antimony from water by potassium ferrate
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摘要: 采用实验室制备的高铁酸钾对水溶液中的三价锑进行去除性能研究. 高铁酸钾对水中三价锑的去除包含2步：一是高铁酸钾对三价锑的氧化，二是原位生成的高铁酸钾分解产物对锑的吸附. XRD和FTIR检测表明高铁酸钾的分解产物符合无定型的2线水铁矿，比表面积大，孔隙率高. 吸附实验结果表明：低pH值更有利于锑的吸附；而离子强度对锑的吸附，在pH 3.5 ~5.5与pH 5.5~7.0这2个区间有着截然相反的影响；吸附动力学过程拟合以准二级动力学拟合最好(R2=0.999 1)，说明以化学吸附为主；吸附等温线拟合以Freundlich模型最优(R2=0.980 4)，而使用Langmuir-Freundlich模型拟合时最大吸附量的理论值可达到129.93 mg/g. 通过吸附前后样品的FTIR表征表明在吸附锑的过程中形成了内层络合物和外层络合物.
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关键词:
- 吸附
Abstract: The synthesized potassium ferrate (K2FeO4) was used to remove Sb(III) from water. The removal was accomplished via two steps: Sb(III) was first oxidized by ferrate, then Sb was adsorbed onto the ferrate decomposition product (DP/ferrate). XRD and FTIR characterized that ferrate decomposition product was amorphous 2-line ferrihydrite with large surface area and high porosity. Adsorption results shows that low pH favored Sb adsorption, whereas when studying the effect of ionic strength, different adsorption behaviors were found in the range of pH=3.5~5.5 and pH=5.5~7.0. Pseudo-second-order kinetic model described the sorption process very well. The values of correlation coefficient were extremely high (R2=0.999 1), indicating chemical adsorption was primary. The experimental data were found to follow the Freundlich isotherms with the best accuracy (R2=0.980 4). The value of Qmax obtained from the Langmuir-Freundlich model was 129.93 mg (g K2FeO4)-1. FTIR results revealed that in the adsorption of Sb by ferrate decomposition product, two forms of surface complexes: an inner-sphere and an outer-sphere surface complex were formed on the surface of ferrate decomposition product.-
Keywords:
- Adsorption
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[1]OKKENHAU G, ZHU Y G, HE J W, LI X, LUO L, MULDER J.Antimony (Sb) and Arsenic (As) in Sb Mining Impacted Paddy Soil from Xikuangshan,China: Differences in Mechanisms Controlling Soil Sequestration and Uptake in Rice,[J].Environmental Science &Technology, 2012, 46(6):3155-62
[2] Council of the European Communities.Council Directive 76/464/EEC of 4 May 1976 on pollution caused by certain dangerous substances discharged into the aquatic environment of the community[J].Off. J. L, 1976, 129:23-29
[3] USEPA.Water related fate of the 129 priority pollutants[J]., 1979, 1:-
[4] UNGUREANU G, SANTOS S, BOAVENTURA R, BOTELHO C .Arsenic and antimony in water and wastewater: Overview of removal techniques with special reference to latest advances in adsorption[J].Journal of Environmental Management, 2015, 151:326-342
[5] SHARMA V K.Oxidation of inorganic compounds by ferrate(VI) and ferrate(V): One-electron and two-electron transfer steps[J].Environmental Science & Technology, 2010, 44:5148-5152
[6] JIANG Y, GOODWILL J E, TOBIASON J E, RECKHW D A.Effect of different solutes, natural organic matter, and particulate Fe(III) on ferrate(VI) decomposition in aqueous solutions[J].Environmental Science & Technology, 2015, 9:2841-2848
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[8] JAMBOR J L, DUTRIZAC J E.Occurrence and constitution of natural and synthetic ferrihydrite, a widespread iron oxyhydroxide[J].Chemical Reviews, 1998, 98:2549-2585
[9] RUSSELL J D.Infrared spectroscopy of ferrihydrite: evidence for the presence of structural hydroxyl groups[J].Clay Minerals, 1979, 1:109-114
[10] JIA Y, XU L, WANG X, DEMOPOULOS G P.Infrared spectroscopic and X-ray diffraction characterization of the nature of adsorbed arsenate on ferrihydrite[J].Geochimicaet Cosmochimica Acta, 2007, 71:1643-1654
[11] RISTI? M, DE GRAVE E, MUSI? S, PPOVI? S, ORREHOVEC Z.Transformation of low crystalline ferrihydrite to α-Fe2O3 in the solid state[J].Journal of Molecular Structure, 2001, 834-836:454-460
[12] KIRI A, MCCOMB, CRAW D, JAES A, MCQUILLIAN.ATR-IR Spectroscopic Study of Antimonate Adsorption to Iron Oxide[J].Langmuir, 2007, 23:12125-121230
[13]徐伟，刘锐平，曲久辉, 彭若梦.铁锰复合氧化物吸附去除五价锑性能研究[J].环境科学学报, 2012, 32(2):270-275
[14]XU W, LIU R P, QU J H, PENG R M.The adsorption behaviors of Fe-Mn binary oxide towards Sb(V)[J].Acta Scientiae Circumstantiae, 2012, 32(2):270-275
[15] XU W, WANG H J, LIU R P, ZHAO X, QU J H.The mechanism of antimony(III) removal and its reactions on the surfaces of Fe-Mn Binary Oxide[J].Journal of Colloid and Interface Science, 2011, 363:320-326
[16] LI X H, DOU X M, LI J Q.Antimony(V) removal from water by iron zirconium bimetal oxide: performance and mechanism[J].Journal of Environment Science-China, 2012, 24:1197-1203
[17] Q. Wang, M.C. He, C.Y. Lin, Y.X. Gao, L. Zheng. Antimony(III) oxidation and antimony(V) adsorption reactions on synthetic manganite. [J].Chemie Der Erde-Geochemisty, 2012, 72:41-47
[18] KOLBE F, WEISS H, MORGENSTERN P, WENNRICH R, LORENZ W, SCHURK K, STAJEK H, DAUS B.Sorption of aqueous antimony and arsenic species onto akaganeite[J].Colloid Interface Science, 2011, 357:460-465
[1]OKKENHAU G, ZHU Y G, HE J W, LI X, LUO L, MULDER J.Antimony (Sb) and Arsenic (As) in Sb Mining Impacted Paddy Soil from Xikuangshan,China: Differences in Mechanisms Controlling Soil Sequestration and Uptake in Rice,[J].Environmental Science &Technology, 2012, 46(6):3155-62
[2] Council of the European Communities.Council Directive 76/464/EEC of 4 May 1976 on pollution caused by certain dangerous substances discharged into the aquatic environment of the community[J].Off. J. L, 1976, 129:23-29
[3] USEPA.Water related fate of the 129 priority pollutants[J]., 1979, 1:-
[4] UNGUREANU G, SANTOS S, BOAVENTURA R, BOTELHO C .Arsenic and antimony in water and wastewater: Overview of removal techniques with special reference to latest advances in adsorption[J].Journal of Environmental Management, 2015, 151:326-342
[5] SHARMA V K.Oxidation of inorganic compounds by ferrate(VI) and ferrate(V): One-electron and two-electron transfer steps[J].Environmental Science & Technology, 2010, 44:5148-5152
[6] JIANG Y, GOODWILL J E, TOBIASON J E, RECKHW D A.Effect of different solutes, natural organic matter, and particulate Fe(III) on ferrate(VI) decomposition in aqueous solutions[J].Environmental Science & Technology, 2015, 9:2841-2848
[7] JOHNSON M, LORENZ B.Antimony remediation using ferrate(VI)[J].Separation Science Technology, 2015, 50:1611-1615
[8] JAMBOR J L, DUTRIZAC J E.Occurrence and constitution of natural and synthetic ferrihydrite, a widespread iron oxyhydroxide[J].Chemical Reviews, 1998, 98:2549-2585
[9] RUSSELL J D.Infrared spectroscopy of ferrihydrite: evidence for the presence of structural hydroxyl groups[J].Clay Minerals, 1979, 1:109-114
[10] JIA Y, XU L, WANG X, DEMOPOULOS G P.Infrared spectroscopic and X-ray diffraction characterization of the nature of adsorbed arsenate on ferrihydrite[J].Geochimicaet Cosmochimica Acta, 2007, 71:1643-1654
[11] RISTI? M, DE GRAVE E, MUSI? S, PPOVI? S, ORREHOVEC Z.Transformation of low crystalline ferrihydrite to α-Fe2O3 in the solid state[J].Journal of Molecular Structure, 2001, 834-836:454-460
[12] KIRI A, MCCOMB, CRAW D, JAES A, MCQUILLIAN.ATR-IR Spectroscopic Study of Antimonate Adsorption to Iron Oxide[J].Langmuir, 2007, 23:12125-121230
[13]徐伟，刘锐平，曲久辉, 彭若梦.铁锰复合氧化物吸附去除五价锑性能研究[J].环境科学学报, 2012, 32(2):270-275
[14]XU W, LIU R P, QU J H, PENG R M.The adsorption behaviors of Fe-Mn binary oxide towards Sb(V)[J].Acta Scientiae Circumstantiae, 2012, 32(2):270-275
[15] XU W, WANG H J, LIU R P, ZHAO X, QU J H.The mechanism of antimony(III) removal and its reactions on the surfaces of Fe-Mn Binary Oxide[J].Journal of Colloid and Interface Science, 2011, 363:320-326
[16] LI X H, DOU X M, LI J Q.Antimony(V) removal from water by iron zirconium bimetal oxide: performance and mechanism[J].Journal of Environment Science-China, 2012, 24:1197-1203
[17] Q. Wang, M.C. He, C.Y. Lin, Y.X. Gao, L. Zheng. Antimony(III) oxidation and antimony(V) adsorption reactions on synthetic manganite. [J].Chemie Der Erde-Geochemisty, 2012, 72:41-47
[18] KOLBE F, WEISS H, MORGENSTERN P, WENNRICH R, LORENZ W, SCHURK K, STAJEK H, DAUS B.Sorption of aqueous antimony and arsenic species onto akaganeite[J].Colloid Interface Science, 2011, 357:460-465
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