铁锰氧化物在不同水分条件下对土壤As的稳定化作用
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摘要
本文以铁锰氧化物(Fe-Mn,FM)为研究对象,评估其在不同水分条件下对我国南方3种砷(As)污染土壤的稳定化修复效果.结果表明,添加一定比例(质量分数30%)水分对于抑制土壤As的毒性浸出具有积极作用,但水分过高(淹水条件)则会引发As的大量活化释放.淹水条件下,FM对As污染土壤具有明显的应用优势,能使韶关、河池和常德这3种土壤毒性浸出质量浓度均显著下降99. 00%以上,使其土壤有效态As含量分别显著降低55. 40%、40. 05%和16. 92%,并增加专性和非专性吸附态As向水合铁铝氧化物结合态的稳定化. FM能使韶关、河池和常德土壤有效态磷(P)含量分别降低0. 60%～6. 67%、15. 74%～50. 00%和32. 48%～40. 39%,这有可能会限制缺P区域农产品对酸性或中性土壤的P摄取. FM对3种供试土壤p H值影响的变化幅度仅为0. 04～0. 07,对土壤环境的影响非常小. FM在我国淹水As污染土壤稳定化修复领域具有较好的应用前景.
Fe-Mn oxide( FM) was used to evaluate its stabilization effects on three typical arsenic( As)-contaminated soils in southern China under different water conditions( dry soil,moist soil,and flooded soil). With an increase in moisture content,the toxicity characteristic leaching procedure( TCLP) results for As decreased by 34. 78%,47. 62%,and 13. 64%,respectively,in Shaoguan,Hechi,and Changde,and then increased by 310. 34%,185. 22%,and 23. 38%,respectively. The results showed that adding a certain amount of water( 30%) had a positive effect on decreasing the As concentration in the TCLP,but excessive amounts( 80%)led to As re-release into the soil. The application of FM under flooding conditions has obvious advantages. In the three soils of Shaoguan,Hechi,and Changde,FM significantly reduced the As concentration in the TCLP by more than 99. 00%,and reduced the soil available As content by 55. 40%,40. 05%,and 16. 92%,respectively. FM increased the specificandnon-specific adsorption of As to stabilize the bound fractions of hydrated iron-aluminum oxide,thus significantly reducing the biological effectiveness of soil As and soil environmental risk. FM reduced the available P in the soil in Shaoguan,Hechi,and Changde by 0. 60%-6. 67%,15. 74%-50. 00%,and 32. 48-40. 39%,respectively. Our study revealed that FM can absorb a small amount of available P,which may limit P uptakeby agricultural products in P-deficient areas,while effectively inhibiting the non-point source pollution of soil to surrounding water bodiesin P-rich areas. The variation in p H after FM application in the three soils was only 0. 04-0. 07,which had little effect on the soil environment. FM has good prospects for stabilization of flooded As-contaminated soil. The results of this study provide an important scientific basis for soil As stabilization in China.
Fe-Mn oxide( FM) was used to evaluate its stabilization effects on three typical arsenic( As)-contaminated soils in southern China under different water conditions( dry soil,moist soil,and flooded soil). With an increase in moisture content,the toxicity characteristic leaching procedure( TCLP) results for As decreased by 34. 78%,47. 62%,and 13. 64%,respectively,in Shaoguan,Hechi,and Changde,and then increased by 310. 34%,185. 22%,and 23. 38%,respectively. The results showed that adding a certain amount of water( 30%) had a positive effect on decreasing the As concentration in the TCLP,but excessive amounts( 80%)led to As re-release into the soil. The application of FM under flooding conditions has obvious advantages. In the three soils of Shaoguan,Hechi,and Changde,FM significantly reduced the As concentration in the TCLP by more than 99. 00%,and reduced the soil available As content by 55. 40%,40. 05%,and 16. 92%,respectively. FM increased the specificandnon-specific adsorption of As to stabilize the bound fractions of hydrated iron-aluminum oxide,thus significantly reducing the biological effectiveness of soil As and soil environmental risk. FM reduced the available P in the soil in Shaoguan,Hechi,and Changde by 0. 60%-6. 67%,15. 74%-50. 00%,and 32. 48-40. 39%,respectively. Our study revealed that FM can absorb a small amount of available P,which may limit P uptakeby agricultural products in P-deficient areas,while effectively inhibiting the non-point source pollution of soil to surrounding water bodiesin P-rich areas. The variation in p H after FM application in the three soils was only 0. 04-0. 07,which had little effect on the soil environment. FM has good prospects for stabilization of flooded As-contaminated soil. The results of this study provide an important scientific basis for soil As stabilization in China.
引文
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[8]Zhang G S,Qu J H,Liu H J,et al.Preparation and evaluation of a novel Fe-Mn binary oxide adsorbent for effective arsenite removal[J].Water Research,2007,41(9):1921-1928.
[9]An B,Zhao DY.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.
[10]Mc Cann C M,Peacock C L,Hudson-Edwards K A,et al.In situ arsenic oxidation and sorption by a Fe-Mn binary oxide waste in soil[J].Journal of Hazardous Materials,2018,342:724-731.
[11]费杨,阎秀兰,李永华.铁锰双金属材料在不同pH条件下对土壤As和重金属的稳定化作用[J].环境科学,2018,39(3):1430-1437.Fei Y,Yan X L,Li Y H.Stabilization effects of Fe-Mn binary oxide on arsenic and heavy metal co-contaminated soils under different p H conditions[J].Environmental Science,2018,39(3):1430-1437.
[12]南京农业大学.土壤农化分析[M].(第二版).北京:中国农业出版社,1981.
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[14]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.
[15]Wongrod S,Simon S,van Hullebusch E D,et al.Assessing arsenic redox state evolution in solution and solid phase during As(Ⅲ)sorption onto chemically-treated sewage sludge digestate biochars[J].Bioresource Technology,2019,275:232-238.
[16]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):179-186.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):179-186.
[17]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.
[18]Catalano J G,Park C,Fenter P,et al.Simultaneous inner-and outer-sphere arsenate adsorption on corundum and hematite[J].Geochimica et Cosmochimica Acta,2008,72(8):1986-2004.
[19]Zhang G S,Qu J H,Liu H J,et al.Removal mechanism of As(Ⅲ)by a novel Fe-Mn binary oxide adsorbent:oxidation and sorption[J].Environmental Science&Technology,2007,41(13):4613-4619.
[20]Ociński D,Jacukowicz-Sobala I,Mazur P,et al.Water treatment residuals containing iron and manganese oxides for arsenic removal from water-Characterization of physicochemical properties and adsorption studies[J].Chemical Engineering Journal,2016,294:210-221.
[21]Wang Y A,Zeng X B,Lu Y H,et al.Dynamic arsenic aging processes and their mechanisms in nine types of Chinese soils[J].Chemosphere,2017,187:404-412.
[22]Huang G X,Chen Z Y,Zhang Y,et al.Changes of arsenic fractionation and bioaccessibility in wastewater-irrigated soils as a function of aging:influence of redox condition and arsenic load[J].Geoderma,2016,280:1-7.
[23]Liu CY,Tian H X,Li H Y,et al.The accuracy in the assessment of arsenic toxicity using soil alkaline phosphatase depends on soil water contents[J].Ecological Indicators,2019,102:457-465.
[24]Wan X,Dong H C,Feng L,et al.Comparison of three sequential extraction procedures for arsenic fractionation in highly polluted sites[J].Chemosphere,2017,178:402-410.
[25]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.
[26]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.
[27]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.
[2]Shi Y L,Chen W Q,Wu S L,et al.Anthropogenic cycles of arsenic in mainland China:1990-2010[J].Environmental Science&Technology,2017,51(3):1670-1678.
[3]Zhou Y T,Niu L L,Liu K,et al.Arsenic in agricultural soils across China:distribution pattern,accumulation trend,influencing factors,and risk assessment[J].Science of the Total Environment,2018,616-617:156-163.
[4]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.
[5]Xu XW,Chen C,Wang P,et al.Control of arsenic mobilization in paddy soils by manganese and iron oxides[J].Environmental Pollution,2017,231:37-47.
[6]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.
[7]王欣,钟松雄,陈志良,等.厌氧条件水稻土铁对砷释放的影响[J].环境科学,2018,39(6):2911-2918.Wang X,Zhong S X,Chen Z L,et al.Effect of iron on the release of arsenic in flooded paddy soils[J].Environmental Science,2018,39(6):2911-2918.
[8]Zhang G S,Qu J H,Liu H J,et al.Preparation and evaluation of a novel Fe-Mn binary oxide adsorbent for effective arsenite removal[J].Water Research,2007,41(9):1921-1928.
[9]An B,Zhao DY.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.
[10]Mc Cann C M,Peacock C L,Hudson-Edwards K A,et al.In situ arsenic oxidation and sorption by a Fe-Mn binary oxide waste in soil[J].Journal of Hazardous Materials,2018,342:724-731.
[11]费杨,阎秀兰,李永华.铁锰双金属材料在不同pH条件下对土壤As和重金属的稳定化作用[J].环境科学,2018,39(3):1430-1437.Fei Y,Yan X L,Li Y H.Stabilization effects of Fe-Mn binary oxide on arsenic and heavy metal co-contaminated soils under different p H conditions[J].Environmental Science,2018,39(3):1430-1437.
[12]南京农业大学.土壤农化分析[M].(第二版).北京:中国农业出版社,1981.
[13]SW-846,Method 1311:toxicity characteristic leaching procedure[S].
[14]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.
[15]Wongrod S,Simon S,van Hullebusch E D,et al.Assessing arsenic redox state evolution in solution and solid phase during As(Ⅲ)sorption onto chemically-treated sewage sludge digestate biochars[J].Bioresource Technology,2019,275:232-238.
[16]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):179-186.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):179-186.
[17]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.
[18]Catalano J G,Park C,Fenter P,et al.Simultaneous inner-and outer-sphere arsenate adsorption on corundum and hematite[J].Geochimica et Cosmochimica Acta,2008,72(8):1986-2004.
[19]Zhang G S,Qu J H,Liu H J,et al.Removal mechanism of As(Ⅲ)by a novel Fe-Mn binary oxide adsorbent:oxidation and sorption[J].Environmental Science&Technology,2007,41(13):4613-4619.
[20]Ociński D,Jacukowicz-Sobala I,Mazur P,et al.Water treatment residuals containing iron and manganese oxides for arsenic removal from water-Characterization of physicochemical properties and adsorption studies[J].Chemical Engineering Journal,2016,294:210-221.
[21]Wang Y A,Zeng X B,Lu Y H,et al.Dynamic arsenic aging processes and their mechanisms in nine types of Chinese soils[J].Chemosphere,2017,187:404-412.
[22]Huang G X,Chen Z Y,Zhang Y,et al.Changes of arsenic fractionation and bioaccessibility in wastewater-irrigated soils as a function of aging:influence of redox condition and arsenic load[J].Geoderma,2016,280:1-7.
[23]Liu CY,Tian H X,Li H Y,et al.The accuracy in the assessment of arsenic toxicity using soil alkaline phosphatase depends on soil water contents[J].Ecological Indicators,2019,102:457-465.
[24]Wan X,Dong H C,Feng L,et al.Comparison of three sequential extraction procedures for arsenic fractionation in highly polluted sites[J].Chemosphere,2017,178:402-410.
[25]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.
[26]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.
[27]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.
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