铁铈氧化物对土壤As(Ⅴ)和P的稳定化效果
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摘要
本文以铁铈氧化物(Fe-Ce,FC)为研究对象,评估其对中国3种典型砷(As)污染土壤的稳定化修复效果,并通过电子扫描显微镜能散X线分析仪(SEM-EDS)和X射线光电子能谱仪(XPS)等光谱学技术探索FC对As(Ⅴ)的微观吸附特征.结果表明,FC能使土壤毒性浸出As含量显著降低84. 1%～98. 3%,且在碱性土壤中表现出较强的高p H适应性,能显著增加吸附态As(F1+F2)向水合铁铝氧化物结合态(F3+F4)的稳定化. FC能使不同类型土壤的有效态P含量显著下降47. 13%～60. 32%,不仅能缓解P竞争土壤As(Ⅴ)吸附位点,而且能有效预防周边水体的面源污染.通过SEM-EDS和XPS分析,发现As(Ⅴ)吸附产物表面均检测到Fe、Ce和As这3种元素,且As主要吸附于Fe原子表面. FC在我国土壤砷污染稳定化修复领域具有较好地应用前景.
The mining and smelting of arsenic-containing metal minerals,and the large-scale use of chemicals and pesticides,has resulted in the widespread pollution of soils in southwestern and southern China. In this study,the stabilizing effect of Fe-Ce oxide( FC) on three representative arsenic-contaminated soils was evaluated. The microscopic adsorption characteristics of FC and As( Ⅴ)were explored by scanning electron microscopy and energy disperse spectroscopy( SEM-EDS) and X-ray photoelectron spectroscopy( XPS). The results showed that FC can significantly reduce arsenic concentrations by 84. 1%-98. 3% during the Toxicity Characteristic Leaching Procedure( TCLP),and showed strong p H adaptability in alkaline soil. It efficiently transformed( non-)specifically sorbed arsenic( F1 + F2) into hydrous oxides phases of Fe and Al( F3 + F4). FC also significantly reduced available P by47. 13%-60. 32% in different types of soil. FC can not only release As( Ⅴ) adsorption sites occupied by P in soils,but also effectively prevents non-point source pollution of the surrounding water. SEM-EDS and XPS analysis detected Fe,Ce,and As on the surface of As( Ⅴ) adsorption products,and As was mainly adsorbed on the surface of Fe atoms. The results of this study provide a scientific basis for soil arsenic stabilization in China.
The mining and smelting of arsenic-containing metal minerals,and the large-scale use of chemicals and pesticides,has resulted in the widespread pollution of soils in southwestern and southern China. In this study,the stabilizing effect of Fe-Ce oxide( FC) on three representative arsenic-contaminated soils was evaluated. The microscopic adsorption characteristics of FC and As( Ⅴ)were explored by scanning electron microscopy and energy disperse spectroscopy( SEM-EDS) and X-ray photoelectron spectroscopy( XPS). The results showed that FC can significantly reduce arsenic concentrations by 84. 1%-98. 3% during the Toxicity Characteristic Leaching Procedure( TCLP),and showed strong p H adaptability in alkaline soil. It efficiently transformed( non-)specifically sorbed arsenic( F1 + F2) into hydrous oxides phases of Fe and Al( F3 + F4). FC also significantly reduced available P by47. 13%-60. 32% in different types of soil. FC can not only release As( Ⅴ) adsorption sites occupied by P in soils,but also effectively prevents non-point source pollution of the surrounding water. SEM-EDS and XPS analysis detected Fe,Ce,and As on the surface of As( Ⅴ) adsorption products,and As was mainly adsorbed on the surface of Fe atoms. The results of this study provide a scientific basis for soil arsenic stabilization in China.
引文
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[24]钟松雄,尹光彩,陈志良,等.Eh、p H和铁对水稻土砷释放的影响机制[J].环境科学,2017,38(6):2530-2537.Zhong S X,Yin G C,Chen Z L,et al.Influencing mechanism of Eh,p H and Iron on the release of arsenic in paddy soil[J].Environmental Science,2017,38(6):2530-2537.
[25]雷鸣,曾敏,廖柏寒,等.含磷物质对水稻吸收土壤砷的影响[J].环境科学,2014,35(8):3149-3154.Lei M,Zeng M,Liao B H,et al.Effects of phosphoruscontaining substances on arsenic uptake by rice[J].Environmental Science,2014,35(8):3149-3154.
[26]Dou X M,Zhang Y,Zhao B,et al.Arsenate adsorption on an Fe-Ce bimetal oxide adsorbent:EXAFS study and surface complexation modeling[J].Colloids and Surfaces A:Physicochemical and Engineering Aspects,2011,379(1-3):109-115.
[2]肖细元,陈同斌,廖晓勇,等.中国主要含砷矿产资源的区域分布与砷污染问题[J].地理研究,2008,27(1):201-212.Xiao X Y,Chen T B,Liao X Y,et al.Regional distribution of arsenic contained minerals and arsenic pollution in China[J].Geographical Research,2008,27(1):201-212.
[3]Duan Q N,Lee J C,Liu Y S,et al.Distribution of heavy metal pollution in surface soil samples in China:a graphical review[J].Bulletin of Environmental Contamination and Toxicology,2016,97(3):303-309.
[4]环境保护部,国土资源部.全国土壤污染状况调查公报[EB/OL].http://www.gov.cn/foot/site1/20140417/782bcb88840814ba158d01.pdf,2014.
[5]Suda A,Makino T.Functional effects of manganese and iron oxides on the dynamics of trace elements in soils with a special focus on arsenic and cadmium:a review[J].Geoderma,2016,270:68-75.
[6]Singh R,Singh S,Parihar P,et al.Arsenic contamination,consequences and remediation techniques:a review[J].Ecotoxicology and Environmental Safety,2015,112:247-270.
[7]Masue Y,Loeppert R H,Kramer T A.Arsenate and arsenite adsorption and desorption behavior on coprecipitated aluminum:iron hydroxides[J].Environmental Science&Technology,2007,41(3):837-842.
[8]Sahu U K,Sahu M K,Mohapatra S S,et al.Removal of As(V)from aqueous solution by Ce-Fe bimetal mixed oxide[J].Journal of environmental chemical engineering,2016,4(3):2892-2899.
[9]Lin L Y,Yan X L,Liao X Y,et al.Migration and arsenic adsorption study of starch-modified Fe-Ce oxide on a siliconbased micromodel observation platform[J].Journal of Hazardous Materials,2017,338:202-207.
[10]Lin L Y,Zhong L R,Yan X L,et al.Reducing arsenic concentration in Panax notoginseng via contaminant immobilization in soil using Fe-Ce oxide[J].Journal of Environmental Quality,2018,47(2):312-317.
[11]Arco-Lázaro E,Agudo I,Clemente R,et al.Arsenic(V)adsorption-desorption in agricultural and mine soils:effects of organic matter addition and phosphate competition[J].Environmental pollution,2016,216:71-79.
[12]龚娟,马友华,胡宏祥,等.农田土壤磷的环境指标研究进展[J].中国农学通报,2016,32(2):112-117.Gong J,Ma Y H,Hu H X,et al.Research advances on environmental indicator of soil phosphorus in Farmland[J].Chinese Agricultural Science Bulletin,2016,32(2):112-117.
[13]陈寻峰,李小明,陈灿,等.砷污染土壤复合淋洗修复技术研究[J].环境科学,2016,37(3):1147-1155.Chen X F,Li X M,Chen C,et al.Mixture leaching remediation technology of arsenic contaminated soil[J].Environmental Science,2016,37(3):1147-1155.
[14]Baken S,Verbeeck M,Verheyen D,et al.Phosphorus losses from agricultural land to natural waters are reduced by immobilization in iron-rich sediments of drainage ditches[J].Water Research,2015,71:160-170.
[15]Fink J R,Inda A V,Tiecher T,et al.Iron oxides and organic matter on soil phosphorus availability[J].Ciência e Agrotecnologia,2016,40(4):369-379.
[16]An B,Zhao D Y.Immobilization of As(Ⅲ)in soil and groundwater using a new class of polysaccharide stabilized Fe-Mn oxide nanoparticles[J].Journal of Hazardous Materials,2012,211-212:332-341.
[17]鲍士旦.土壤农化分析[M].(第三版).北京:中国农业出版社,2000.
[18]US EPA.Method 1311:Toxicity characteristic leaching procedure[S].EPA SW-846:Test Methods for Evaluating Solid Waste,Physical/Chemical Methods,1992.
[19]于冰冰,阎秀兰,廖晓勇,等.用于表征三七种植区土壤中可利用态砷的化学提取剂的筛选[J].农业环境科学学报,2011,30(8):1573-1579.Yu B B,Yan X L,Liao X Y,et al.Screening of chemical extracting agents for characterizing soil bio-effective arsenic on Panax Notoginseng[J].Journal of Agro-Environment Science,2011,30(8):1573-1579.
[20]Wenzel W W,Kirchbaumer N,Prohaska T,et al.Arsenic fractionation in soils using an improved sequential extraction procedure[J].Analytica Chimica Acta,2001,436(2):309-323.
[21]Hafeznezami S,Zimmer-Faust A G,Dunne A,et al.Adsorption and desorption of arsenate on sandy sediments from contaminated and uncontaminated saturated zones:kinetic and equilibrium modeling[J].Environmental Pollution,2016,215:290-301.
[22]Han Y H,Yang G M,Fu J W,et al.Arsenic-induced plant growth of arsenic-hyperaccumulator Pteris vittata:impact of arsenic and phosphate rock[J].Chemosphere,2016,149:366-372.
[23]田桃,雷鸣,周航,等.两种钝化剂对土壤Pb、Cd、As复合污染的菜地修复效果[J].环境科学,2017,38(6):2553-2560.Tian T,Lei M,Zhou H,et al.Effects of two amendments on remedying garden soil complexly contaminated with Pb,Cd and As[J].Environmental Science,38(6):2553-2560.
[24]钟松雄,尹光彩,陈志良,等.Eh、p H和铁对水稻土砷释放的影响机制[J].环境科学,2017,38(6):2530-2537.Zhong S X,Yin G C,Chen Z L,et al.Influencing mechanism of Eh,p H and Iron on the release of arsenic in paddy soil[J].Environmental Science,2017,38(6):2530-2537.
[25]雷鸣,曾敏,廖柏寒,等.含磷物质对水稻吸收土壤砷的影响[J].环境科学,2014,35(8):3149-3154.Lei M,Zeng M,Liao B H,et al.Effects of phosphoruscontaining substances on arsenic uptake by rice[J].Environmental Science,2014,35(8):3149-3154.
[26]Dou X M,Zhang Y,Zhao B,et al.Arsenate adsorption on an Fe-Ce bimetal oxide adsorbent:EXAFS study and surface complexation modeling[J].Colloids and Surfaces A:Physicochemical and Engineering Aspects,2011,379(1-3):109-115.
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