铝代水铁矿协同吸附砷镉的机制
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摘要
通过室内试验,研究了铝代水铁矿对As(Ⅴ)和Cd(Ⅱ)的协同作用过程及机制.结果表明,溶液体系p H值和重金属加入顺序明显影响铝代水铁矿对砷和镉的协同吸附与共沉淀.在近中性砷镉共存体系下吸附72h(p H为6. 0～6. 5),含20%铝的铝代水铁矿(AF20)对砷和镉的吸附容量达到了60. 9 mg·g~(-1)和17. 1 mg·g~(-1),去除率分别为96. 0%和73. 0%,砷和镉协同吸附到AF20颗粒内部孔隙,AF20对砷和镉的协同吸附效应明显;在砷溶液中加入镉体系下吸附72 h(p H为6. 1～6. 5),AF20对砷和镉的吸附容量分别为58. 1 mg·g~(-1)和12. 4 mg·g~(-1),去除率分别为96. 0%和48. 3%,砷的吸附限制了镉的固定;在镉溶液中加入砷体系下吸附72 h(p H为9. 5～9. 8),AF20对砷和镉固定量分别为20. 9 mg·g~(-1)和24. 4 mg·g~(-1),去除率分别为38. 8%和98. 9%,AF20对砷和镉的共沉淀效应明显,生成的砷镉难溶物通过堵塞孔道使镉呈稀疏条带状分布,同时阻碍砷的进一步吸附.上述结果表明,铝代水铁矿可协同吸附、共沉淀污染环境介质中的砷和镉.
The synergistic process and mechanism of aluminum( Al)-substituted ferrihydrites on arsenic [As( Ⅴ) ] and cadmium[Cd( Ⅱ) ]were studied under laboratory conditions. The results showed that synergistic adsorption and coprecipitation of As and Cd by Al-substituted ferrihydrites was clearly affected by both the p H of solution and the order in which heavy metals were added. The solution in which As co-existed with Cd for 72 hours,at a p H of 6. 0 to 6. 5,the As and Cd adsorption capacity of Al-substituted ferrihydrites containing 20% Al( AF20) reached 60. 9 mg·g~(-1) and 17. 1 mg·g~(-1),respectively. The removal rates of As and Cd were96. 0% and 73. 0%,respectively. Arsenic and Cd were synergistically adsorbed into the internal pores of AF20 particles,and the synergistic adsorption effect of AF20 on As and Cd was clear. Adding Cd to the solution containing As,for 72 hours,and with a p H of6. 1 to 6. 5,the As and Cd adsorption capacity of AF20 was 58. 1 mg·g~(-1) and 12. 4 mg·g~(-1),respectively. The removal rates of As and Cd were 96. 0% and 48. 3%,respectively. Adsorption of As limited the fixation of Cd by AF20. When adding As to the solution containing Cd,for 72 hours,with a p H of 9. 5 to 9. 8,fixed amounts of As and Cd on AF20 were 20. 9 mg·g~(-1) and 24. 4 mg·g~(-1),respectively. The removal rates of As and Cd were 38. 8% and 98. 9%,respectively. The coprecipitation of As and Cd by AF20 was clear. The resulting insoluble As and Cd compounds distributed the Cd distribution in a sparse strip and impeded the further adsorption of As. The results show that Al-substituted ferrihydrites can synergistically adsorb and coprecipitate As and Cd in contaminated environmental media.
The synergistic process and mechanism of aluminum( Al)-substituted ferrihydrites on arsenic [As( Ⅴ) ] and cadmium[Cd( Ⅱ) ]were studied under laboratory conditions. The results showed that synergistic adsorption and coprecipitation of As and Cd by Al-substituted ferrihydrites was clearly affected by both the p H of solution and the order in which heavy metals were added. The solution in which As co-existed with Cd for 72 hours,at a p H of 6. 0 to 6. 5,the As and Cd adsorption capacity of Al-substituted ferrihydrites containing 20% Al( AF20) reached 60. 9 mg·g~(-1) and 17. 1 mg·g~(-1),respectively. The removal rates of As and Cd were96. 0% and 73. 0%,respectively. Arsenic and Cd were synergistically adsorbed into the internal pores of AF20 particles,and the synergistic adsorption effect of AF20 on As and Cd was clear. Adding Cd to the solution containing As,for 72 hours,and with a p H of6. 1 to 6. 5,the As and Cd adsorption capacity of AF20 was 58. 1 mg·g~(-1) and 12. 4 mg·g~(-1),respectively. The removal rates of As and Cd were 96. 0% and 48. 3%,respectively. Adsorption of As limited the fixation of Cd by AF20. When adding As to the solution containing Cd,for 72 hours,with a p H of 9. 5 to 9. 8,fixed amounts of As and Cd on AF20 were 20. 9 mg·g~(-1) and 24. 4 mg·g~(-1),respectively. The removal rates of As and Cd were 38. 8% and 98. 9%,respectively. The coprecipitation of As and Cd by AF20 was clear. The resulting insoluble As and Cd compounds distributed the Cd distribution in a sparse strip and impeded the further adsorption of As. The results show that Al-substituted ferrihydrites can synergistically adsorb and coprecipitate As and Cd in contaminated environmental media.
引文
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[14]Huang B,Guo Z H,Xiao X Y,et al.Changes in chemical fractions and ecological risk prediction of heavy metals in estuarine sediments of Chunfeng Lake estuary,China[J].Marine Pollution Bulletin,2019,138:575-583.
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[16]Lock A,Wallschlger D,Belzile N,et al.Rates and processes affecting As speciation and mobility in lake sediments during aging[J].Journal of Environmental Sciences,2018,66:338-347.
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[19]Adra A,Morin G,Ona-Nguema G,et al.Arsenate and arsenite adsorption onto Al-containing ferrihydrites.Implications for arsenic immobilization after neutralization of acid mine drainage[J].Applied Geochemistry,2016,64:2-9.
[20]Mamindy-Pajany Y,Hurel C,Marmier N,et al.Arsenic(V)adsorption from aqueous solution onto goethite,hematite,magnetite and zero-valent iron:Effects of pH,concentration and reversibility[J].Desalination,2011,281:93-99.
[21]Spathariotis E,Kallianou C.Adsorption of copper,zinc,and cadmium on goethite,aluminum-substituted goethite,and a system of kaolinite-goethite:surface complexation modeling[J].Communications in Soil Science and Plant Analysis,2007,38(5-6):611-635.
[22]余贵芬,蒋新,吴泓涛,等.镉铅在粘土上的吸附及受腐殖酸的影响[J].环境科学,2002,23(5):109-112.Yu G F,Jiang X,Wu H T,et al.Adsorption of Cd and Pb on clays and the influence of humic acids[J].Environmental Science,2002,23(5):109-112.
[23]李丽,刘中,宁阳,等.不同类型粘土矿物对镉吸附与解吸行为的研究[J].山西农业大学学报(自然科学版),2017,37(1):60-66.Li L,Liu Z,Ning Y,et al.Study on cadmium adsorptiondesorption behavior of different clay minerals[J].Journal of Shanxi Agricultural University(Natural Science Edition),2017,37(1):60-66.
[24]Schwertmann U,Cornell R M.Iron oxides in the laboratory:preparation and characterization(2nd ed.)[M].New York:Wiley-VCH,2000.
[25]Jiang W,Lv J T,Luo L,et al.Arsenate and cadmium coadsorption and co-precipitation on goethite[J].Journal of Hazardous Materials,2013,262:55-63.
[26]施明哲.扫描电镜和能谱仪的原理与实用分析技术[M].北京:电子工业出版社,2015.196-197.
[27]Yu Y,Yu L,Shih K,et al.Yttrium-doped iron oxide magnetic adsorbent for enhancement in arsenic removal and ease in separation after applications[J].Journal of Colloid and Interface Science,2018,521:252-260.
[28]Zhou Y,Guo H J,Yan G C,et al.Fluidized bed reaction towards crystalline embedded amorphous Si anode with much enhanced cycling stability[J].Chemical Communications,2018,54(30):3755-3758.
[29]Zhang D N,Wang S F,Wang Y,et al.The transformation of two-line ferrihydrite into crystalline products:effect of pH and media(sulfate vs.nitrate)[J].ACS Earth and Space Chemistry,2018,2(6):577-587.
[30]马玉玲,马杰,陈雅丽,等.水铁矿及其胶体对砷的吸附与吸附形态[J].环境科学,2018,39(1):178-186.Ma Y L,Ma J,Chen Y L,et al.Arsenic adsorption and its species on ferrihydrite and ferrihydrite colloid[J].Environmental Science,2018,39(1):178-186.
[31]Li H C,Shan C,Zhang Y Y,et al.Arsenate adsorption by hydrous ferric oxide nanoparticles embedded in cross-linked anion exchanger:Effect of the host pore structure[J].ACS Applied Materials&Interfaces,2016,8(5):3012-3020.
[32]Maiti A,Basu J K,De S.Experimental and kinetic modeling of As(Ⅴ)and As(Ⅲ)adsorption on treated laterite using synthetic and contaminated groundwater:Effects of phosphate,silicate and carbonate ions[J].Chemical Engineering Journal,2012,191:1-12.
[33]Wang Y H,Morin G,Ona-Nguema G,et al.Arsenite sorption at the magnetite-water interface during aqueous precipitation of magnetite:EXAFS evidence for a new arsenite surface complex[J].Geochimica et Cosmochimica Acta,2008,72(11):2573-2586.
[34]吴萍萍,曾希柏.人工合成铁、铝矿对As(Ⅴ)吸附的研究[J].中国环境科学,2011,31(4):603-610.Wu P P,Zeng X B.Study on arsenate adsorption by synthetic iron and aluminum oxides/hydroxides[J].China Environmental Science,2011,31(4):603-610.
[35]Freitas E T F,Montoro L A,Gasparon M,et al.Natural attenuation of arsenic in the environment by immobilization in nanostructured hematite[J].Chemosphere,2015,138:340-347.
[36]Masquelier C,d'Yvoire F,Collin G.Crystal structure of Na7Fe4(As O4)6andα-Na3Al2(As O4)3,two sodium ion conductors structurally related toⅡ-Na3Fe2(As O4)3[J].Journal of Solid State Chemistry,1995,118(1):33-42.
[37]He S R,Li Y T,Weng L P,et al.Competitive adsorption of Cd2+,Pb2+and Ni2+onto Fe3+-modified argillaceous limestone:Influence of pH,ionic strength and natural organic matters[J].Science of the Total Environment,2018,637-638:69-78.
[38]黄可龙,雷家珩,王林山.无机化学[M].北京:科学出版社,2007.301-306.
[2]Ekstrom E B,Learman D R,Madden A S,et al.Contrasting effects of Al substitution on microbial reduction of Fe(Ⅲ)(hydr)oxides[J].Geochimica et Cosmochimica Acta,2010,74(24):7086-7099.
[3]Hofmann A,Vantelon D,Montargès-Pelletier E,et al.Interaction of Fe(Ⅲ)and Al(Ⅲ)during hydroxylation by forced hydrolysis:The nature of Al-Fe oxyhydroxy co-precipitates[J].Journal of Colloid and Interface Science,2013,407:76-88.
[4]Cao S S,Kang F F,Yang X,et al.Influence of Al substitution on magnetism and adsorption properties of hematite[J].Journal of Solid State Chemistry,2015,228:82-89.
[5]Hansel C M,Learman D R,Lentini C J,et al.Effect of adsorbed and substituted Al on Fe(Ⅱ)-induced mineralization pathways of ferrihydrite[J].Geochimica et Cosmochimica Acta,2011,75(16):4653-4666.
[6]Hu Y D,Li Q Y,Lee B,et al.Aluminum affects heterogeneous Fe(Ⅲ)(hydr)oxide nucleation,growth,and Ostwald ripening[J].Environmental Science&Technology,2014,48(1):299-306.
[7]Freitas E T F,Stroppa D G,Montoro L A,et al.Arsenic entrapment by nanocrystals of Al-magnetite:The role of Al in crystal growth and As retention[J].Chemosphere,2016,158:91-99.
[8]曾鹏,郭朝晖,肖细元,等.芦竹和木本植物间种修复重金属污染土壤[J].环境科学,2018,39(11):5207-5216.Zeng P,Guo Z H,Xiao X Y,et al.Intercropping Arundo donax with woody plants to remediate heavy metal-contaminated soil[J].Environmental Science,2018,39(11):5207-5216.
[9]封文利,郭朝晖,史磊,等.控源及改良措施对稻田土壤和水稻镉累积的影响[J].环境科学,2018,39(1):399-405.Feng W L,Guo Z H,Shi L,et al.Distribution and accumulation of cadmium in paddy soil and rice affected by pollutant sources control and improvement measures[J].Environmental Science,2018,39(1):399-405.
[10]Hu Y A,Cheng H F,Tao S.The challenges and solutions for cadmium-contaminated rice in China:A critical review[J].Environment International,2016,92-93:515-532.
[11]Teng Y G,Wu J,Lu S J,et al.Soil and soil environmental quality monitoring in China:A review[J].Environment International,2014,69:177-199.
[12]Zhang X W,Yang L S,Li Y H,et al.Impacts of lead/zinc mining and smelting on the environment and human health in China[J].Environmental Monitoring and Assessment,2012,184(4):2261-2273.
[13]郭朝晖,涂卫佳,彭驰,等.典型铅锌矿区河流沿岸农田土壤重金属分布特征及潜在生态风险评价[J].农业环境科学学报,2017,36(10):2029-2038.Guo Z H,Tu W J,Peng C,et al.Distribution characteristics and potential ecological risk assessment of heavy metals in paddy soil along both sides of river from typical lead/zinc mine area[J].Journal of Agro-Environment Science,2017,36(10):2029-2038.
[14]Huang B,Guo Z H,Xiao X Y,et al.Changes in chemical fractions and ecological risk prediction of heavy metals in estuarine sediments of Chunfeng Lake estuary,China[J].Marine Pollution Bulletin,2019,138:575-583.
[15]Huang B,Guo Z H,Tu W J,et al.Geochemistry and ecological risk of metal(loid)s in overbank sediments near an abandoned lead/zinc mine in central south China[J].Environmental Earth Sciences,2018,77:68.
[16]Lock A,Wallschlger D,Belzile N,et al.Rates and processes affecting As speciation and mobility in lake sediments during aging[J].Journal of Environmental Sciences,2018,66:338-347.
[17]Luevano J,Damodaran C.A review of molecular events of cadmium-induced carcinogenesis[J].Journal of Environmental Pathology,Toxicology and Oncology,2014,33(3):183-194.
[18]Sharma V K,Sohn M.Aquatic arsenic:Toxicity,speciation,transformations,and remediation[J].Environment International,2009,35(4):743-759.
[19]Adra A,Morin G,Ona-Nguema G,et al.Arsenate and arsenite adsorption onto Al-containing ferrihydrites.Implications for arsenic immobilization after neutralization of acid mine drainage[J].Applied Geochemistry,2016,64:2-9.
[20]Mamindy-Pajany Y,Hurel C,Marmier N,et al.Arsenic(V)adsorption from aqueous solution onto goethite,hematite,magnetite and zero-valent iron:Effects of pH,concentration and reversibility[J].Desalination,2011,281:93-99.
[21]Spathariotis E,Kallianou C.Adsorption of copper,zinc,and cadmium on goethite,aluminum-substituted goethite,and a system of kaolinite-goethite:surface complexation modeling[J].Communications in Soil Science and Plant Analysis,2007,38(5-6):611-635.
[22]余贵芬,蒋新,吴泓涛,等.镉铅在粘土上的吸附及受腐殖酸的影响[J].环境科学,2002,23(5):109-112.Yu G F,Jiang X,Wu H T,et al.Adsorption of Cd and Pb on clays and the influence of humic acids[J].Environmental Science,2002,23(5):109-112.
[23]李丽,刘中,宁阳,等.不同类型粘土矿物对镉吸附与解吸行为的研究[J].山西农业大学学报(自然科学版),2017,37(1):60-66.Li L,Liu Z,Ning Y,et al.Study on cadmium adsorptiondesorption behavior of different clay minerals[J].Journal of Shanxi Agricultural University(Natural Science Edition),2017,37(1):60-66.
[24]Schwertmann U,Cornell R M.Iron oxides in the laboratory:preparation and characterization(2nd ed.)[M].New York:Wiley-VCH,2000.
[25]Jiang W,Lv J T,Luo L,et al.Arsenate and cadmium coadsorption and co-precipitation on goethite[J].Journal of Hazardous Materials,2013,262:55-63.
[26]施明哲.扫描电镜和能谱仪的原理与实用分析技术[M].北京:电子工业出版社,2015.196-197.
[27]Yu Y,Yu L,Shih K,et al.Yttrium-doped iron oxide magnetic adsorbent for enhancement in arsenic removal and ease in separation after applications[J].Journal of Colloid and Interface Science,2018,521:252-260.
[28]Zhou Y,Guo H J,Yan G C,et al.Fluidized bed reaction towards crystalline embedded amorphous Si anode with much enhanced cycling stability[J].Chemical Communications,2018,54(30):3755-3758.
[29]Zhang D N,Wang S F,Wang Y,et al.The transformation of two-line ferrihydrite into crystalline products:effect of pH and media(sulfate vs.nitrate)[J].ACS Earth and Space Chemistry,2018,2(6):577-587.
[30]马玉玲,马杰,陈雅丽,等.水铁矿及其胶体对砷的吸附与吸附形态[J].环境科学,2018,39(1):178-186.Ma Y L,Ma J,Chen Y L,et al.Arsenic adsorption and its species on ferrihydrite and ferrihydrite colloid[J].Environmental Science,2018,39(1):178-186.
[31]Li H C,Shan C,Zhang Y Y,et al.Arsenate adsorption by hydrous ferric oxide nanoparticles embedded in cross-linked anion exchanger:Effect of the host pore structure[J].ACS Applied Materials&Interfaces,2016,8(5):3012-3020.
[32]Maiti A,Basu J K,De S.Experimental and kinetic modeling of As(Ⅴ)and As(Ⅲ)adsorption on treated laterite using synthetic and contaminated groundwater:Effects of phosphate,silicate and carbonate ions[J].Chemical Engineering Journal,2012,191:1-12.
[33]Wang Y H,Morin G,Ona-Nguema G,et al.Arsenite sorption at the magnetite-water interface during aqueous precipitation of magnetite:EXAFS evidence for a new arsenite surface complex[J].Geochimica et Cosmochimica Acta,2008,72(11):2573-2586.
[34]吴萍萍,曾希柏.人工合成铁、铝矿对As(Ⅴ)吸附的研究[J].中国环境科学,2011,31(4):603-610.Wu P P,Zeng X B.Study on arsenate adsorption by synthetic iron and aluminum oxides/hydroxides[J].China Environmental Science,2011,31(4):603-610.
[35]Freitas E T F,Montoro L A,Gasparon M,et al.Natural attenuation of arsenic in the environment by immobilization in nanostructured hematite[J].Chemosphere,2015,138:340-347.
[36]Masquelier C,d'Yvoire F,Collin G.Crystal structure of Na7Fe4(As O4)6andα-Na3Al2(As O4)3,two sodium ion conductors structurally related toⅡ-Na3Fe2(As O4)3[J].Journal of Solid State Chemistry,1995,118(1):33-42.
[37]He S R,Li Y T,Weng L P,et al.Competitive adsorption of Cd2+,Pb2+and Ni2+onto Fe3+-modified argillaceous limestone:Influence of pH,ionic strength and natural organic matters[J].Science of the Total Environment,2018,637-638:69-78.
[38]黄可龙,雷家珩,王林山.无机化学[M].北京:科学出版社,2007.301-306.
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