Study on stabilization of antimony (Sb) in contaminated soil by primary explosives using iron-based and aluminum-based adsorbents
JIANG Yu-cong1,2, XIA Tian-xiang1, JIA Xiao-yang1,3, ZHONG Ming-yu1, WANG Ning-ning1, LI Ning1,2
1. Beijing Key Laboratory for Risk Modeling and Remediation of Contaminated Sites, Beijing Municipal Research Institute of Environmental Protection, Beijing 100037, China; 2. College of Resources, Environment and Tourism, Capital Normal University, Beijing 100048, China; 3. School of Water Science of Beijing Normal University, Beijing 100875, China
Abstract:Iron-based (ferrous sulfate, goethite and iron powder) and aluminum-based (aluminum hydroxide powder) adsorbents were amended to stabilize antimony (Sb) in primary explosives contaminated soils. The stabilizing effects of iron-based adsorbent, aluminum-based adsorbent, and iron-aluminum mixed adsorbent, as well as the changes of specific surface area and the transformation of Sb after stabilization were investigated by sorption isotherm experiments, batch leaching experiments, specific surface area determination and European Community Bureau of Reference (BCR) analysis. Results showed that the isothermal sorption of different iron-based adsorbents for Sb were well described by the Freundlich equation, and the sorption capacity of FeSO4(log Kf = 5.85) was significantly higher than Fe0 (log Kf = 3.21) and goethite (log Kf = 4.32). After 10days, the stabilization efficiency of different iron-based adsorbents for Sb increased with addition, and 10% FeSO4 (97.1%) > 10% Fe0 (72.3%) > goethite (41.0 %). The concentrations of Zn, Cu and Pb in leachates from the soils amended by FeSO4 were 1990.2, 2.8 and 21.6 times higher than control respectively, and it also decreased significantly by aluminum hydroxide amendments. With 4 % addition of aluminum hydroxide, the stabilization efficiencies for Zn, Cu, and Pb was 93.8%、93.5% and 98.3%, respectively. The mixture of 5% FeSO4 sulfate and 4% aluminum hydroxide had the best stabilization effect on Sb, Zn, Cu, and Pb in soil, and the maximum stabilization efficiencies were 94.6%、74.2%、82.2% and 97.6% respectively after 10days. Further analysis revealed that, the specific surface area could reach 1.31~1.67 times that of the original soils and the residual fraction of Sb also increased by 0.037~0.197 times after adding the iron-aluminum mixed adsorbents, which was consistent with the stabilization effect. Our results indicated that using iron-aluminum mixed adsorbent is an effective way to stabilize heavy metals combined contaminated soils.
姜昱聪, 夏天翔, 贾晓洋, 钟名誉, 王宁宁, 李宁. 铁铝吸附剂对起爆药污染土壤中锑的稳定化研究[J]. 中国环境科学, 2020, 40(8): 3520-3529.
JIANG Yu-cong, XIA Tian-xiang, JIA Xiao-yang, ZHONG Ming-yu, WANG Ning-ning, LI Ning. Study on stabilization of antimony (Sb) in contaminated soil by primary explosives using iron-based and aluminum-based adsorbents. CHINA ENVIRONMENTAL SCIENCECE, 2020, 40(8): 3520-3529.
He M, Wang Y, Wang A, et al. Antimony speciation in the environment:Recent advances in understanding the biogeochemical processes and ecological effects[J]. Journal of Environmental Sciences, 2019,75:14-39.
[2]
Wei Y, Su Q, Sun Z, et al. The role ofarbuscular mycorrhizal fungi in plant uptake, fractions, and speciation of antimony[J]. Applied Soil Ecology, 2016,107:244-250.
[3]
Griggs C S, Martin W A, Larson S L, et al. The effect of phosphate application on the mobility of antimony in firing range soils[J]. Science of Total Environment, 2011,409(12):2397-2403.
[4]
崔自敏.铁铝复合吸附剂共除地下水中砷和氟的研究[D].哈尔滨:哈尔滨工业大学, 2011. Cui Z M. Simultaneous removal arsenic and of fluoride from groundwater with coprecipitated aluminum-iron hydroxide[D]. Harbin:Harbin Institute of Technology, 2011.
[5]
于冰冰,颜湘华,王兴润,等.不同稳定化材料对废渣中As的固定效果[J].中国环境科学, 2019,39(9):3887-3896. Yu B B, Yan X H, Wang X R, et al. Stabilization effects of different materials on arsenic-containing slag[J]. China Environmental Science, 2019,39(9):3887-3896.
[6]
赵述华,张太平,陈志良等.稳定化处理砷污染土壤对3种修复植物的生态效应[J].中国环境科学, 2019,39(9):3925-3932. Zhao S H, Zhang T P, Chen Z L, et al. Ecological effects of stabilization treatment of As contaminated soils on three remediation plants[J]. China Environmental Science, 2019,39(9):3925-3932.
[7]
卢聪,李青青,罗启仕,等.场地土壤中有效态砷的稳定化处理及机理研究[J].中国环境科学, 2013,33(2):298-304. Lu C, Li Q Q, Luo Q S, et al. Stabilization treatment of available arsenic in contaminated soils and mechanism studies[J]. China Environmental Science, 2013,33(2):298-304.
[8]
álvarez-Ayuso E, Otones V, Murciego A, et al. Evaluation of different amendments to stabilize antimony in mining polluted soils[J]. Chemosphere, 2013,90(8):2233-2239.
[9]
Multani R S, Feldmann T, Demopoulos G P. Antimony in the metallurgical industry:A review of its chemistry and environmental stabilization options[J]. Hydrometallurgy, 2016,164:141-153.
[10]
Spuller C, Weigand H, Marb C. Trace metal stabilisation in a shooting range soil:Mobility and phytotoxicity[J]. Journal of Hazardous Materials, 2007,141(2):378-387.
[11]
Okkenhaug G, Gebhardt G K-A, Amstaetter K, et al. Antimony (Sb) and lead (Pb) in contaminated shooting range soils:Sb and Pb mobility and immobilization by iron based sorbents, a field study[J]. Journal of Hazardous Materials, 2016,307:336-343.
[12]
AlmåsÅ R, Pironin E, Okkenhaug G. The partitioning of Sb in contaminated soils after being immobilization by Fe-based amendments is more dynamic compared to Pb[J]. Applied Geochemistry, 2019,108:104378.
[13]
Tandy S, Hockmann K, Keller M, et al. Antimony mobility during prolonged waterlogging and reoxidation of shooting range soil:A field experiment[J]. Science of Total Environment, 2018,624:838-844.
[14]
GB/T 14848-2017地下水质量标准[S]. GB/T 14848-2017 Standard for ground water quality[S].
[15]
GB 3838-2002地表水质量标准[S]. GB 3838-2002 Environmental quality standards for surface water[S].
[16]
U.S. Environment Protection Agency. Regional screening level summary table[S]. Washington D.C.:U.S. Environment Protection Agency, 2018.
[17]
姜昱聪,贾晓洋,夏天翔,等.起爆药污染场地土壤中锑的环境风险评估[J].环境科学研究, 2020,33(2):485-493. Jiang Y C, Jia X Y, Xia T X, et al. Environmental risk assessment research of antimony in contaminated soil by primary explosives[J]. Research of Environmental Sciences, 2020,33(2):485-493.
[18]
GB 36600-2018土壤环境质量建设用地土壤污染风险管控标准[S]. GB 36600-2018 Soil environmental quality Risk control standard for soil contamination of development land[S].
[19]
Okkenhaug G, Amstatter K, Lassen B H, et al. Antimony (Sb) contaminated shooting range soil:Sb mobility and immobilization by soil amendments[J]. Environmental ence & Technology, 2013,47(12):6431-6439.
[20]
Hartley W, Edwards R, Lepp N W. Arsenic and heavy metal mobility in iron oxide-amended contaminated soils as evaluated by short-and long-term leaching tests[J]. Environmental Pollution, 2004,131(3):0-504.
[21]
80-778EEC-1980 Relating to the quality of water intended for human consumption[J].
[22]
BGBI.I,S 2613-1990 Relating to the quality of water intended for human consumption[J].
[23]
HJ 680-2013土壤和沉积物汞、砷、硒、铋、锑的测定微波消解/原子荧光法[S]. HJ 680-2013 Soil and sedimen-determination of mercury, arsenic, selenium, bismuth, antimony-Microwave dissolution/Atomic Fluorescence Spectrometry[S].
[24]
张莹雪,胥思勤.晴隆锑矿区土壤中锑的释放探究[J].贵州大学学报(自然科学版), 2017,34(3):110-114. Zhang Y X, Xu S Q. Study on the release of antimony from soil in Qinglong antimony mine[J]. Journal of Guizhou University (Natural Sciences), 2017,34(3):110-114.
[25]
Eisazadeh A, Kassim K A, Nur H. Morphology and BET surface area of phosphoric acid stabilized tropical soils[J]. Engineering Geology, 2013,154:36-41.
[26]
Fernández-Ondoño E, Bacchetta G, Lallena A M, et al. Use of BCR sequential extraction procedures for soils and plant metal transfer predictions in contaminated mine tailings in Sardinia[J]. Journal of Geochemical Exploration, 2017,172:133-141.
[27]
Wang J, Jiang J, Li D, et al. Removal of Pb and Zn from contaminated soil by different washing methods:the influence of reagents and ultrasound[J]. Environmental Science & Pollution Research, 2015, 22(24):20084-20091.
杜森.土壤分析技术规范[M].二版.北京:中国农业出版社, 2006. Du S. Soil analysis and technical specifications[M]. 2nd edition. Beijing:China Agriculture Press, 2006.
[30]
Elbana T A, Magdi Selim H, Akrami N, et al. Freundlich sorption parameters for cadmium, copper, nickel, lead, and zinc for different soils:Influence of kinetics[J]. Geoderma An International Journal of Soil Science, 2018,324:80-88.
[31]
Shafqat M N, Pierzynski G M. The Freundlich adsorption isotherm constants and prediction of phosphorus bioavailability as affected by different phosphorus sources in two Kansas soils[J]. Chemosphere, 2014,99:72-80.
[32]
唐欢.纳米零价铁对水中As (Ⅲ)和Cd (Ⅱ)的吸附特性研究[D].哈尔滨:哈尔滨工业大学, 2014. Tang H. Characterization of the adsorption behaviour of aqueous As (Ⅲ) and Cd (Ⅱ) ions on nanoparticles of zero-valent iron[D]. Harbin:Harbin Institute of Technology, 2014.
[33]
Xi J, He M, Lin C. Adsorption of antimony (III) and antimony (V) on bentonite:Kinetics, thermodynamics and anion competition[J]. Microchemical Journal, 2011,97(1):85-91.
[34]
Thanabalasingam P, Pickering W F. Specific sorption of antimony (III) by the hydrous oxides of Mn, Fe, and Al[J]. Water, Air, and Soil Pollution, 1990,49(1/2):175-185.
[35]
李小云,王丽萍.氢氧化铝对重金属离子的吸附性能研究[J].光谱实验室, 2010,27(2):408-412. Li X Y, Wang L P. Study on aluminum hydroxide adsorption properties to heavy metal ion[J]. Chinese Journal of Spectroscopy Laboratory, 2010,27(2):408-412.
[36]
龚学臣.SPSS软件在交互效应方差分析中的应用[J].河北北方学院学报(自然科学版), 2015,31(1):19-22. Gong X C. Application of SPSS software in multivariate analysis of variance[J]. Journal of Hebei North University (Natural Science Edition), 2015,31(1):19-22.
[37]
陈皓菁.生活垃圾焚烧飞灰中Zn、Pb、Cu的浸出特性[J].上海应用技术学院学报(自然科学版), 2008,8(4):307-310. Chen H J. Leaching behavior of Zn, Pb and Cu from MSWI fly ash[J]. Journal of Shanghai Institute of Technology:Natural Science, 2008, 8(4):307-310.
[38]
李娟英,陈洁芸,曹宏宇,等. pH对污水污泥中污染物浸出的影响[J].环境工程学报, 2013,7(12):4983-4989. Li J Y, Chen J Y, Cao H Y, et al. Influence of pH on leaching of pollutants from sewage sludge[J]. Chinese Journal of Environmental Engineering, 2013,7(12):4983-4989.
[39]
Denys S, Tack K, Caboche J, et al. Bioaccessibility, solid phase distribution, and speciation of Sb in soils and in digestive fluids[J]. Chemosphere, 2009,74(5):711-716.
[40]
Gál J, Gál J, Hursthouse A S, et al. Chemical availability of arsenic and antimony in industrial soils[J]. Environmental Chemistry Letters, 2006,3(4):149-153.
[41]
陈秋平.干湿交替过程锑矿土壤中As、Sb及氧化铁变化研究[D].贵阳:贵州大学, 2015. Chen Q P. Variation of arsenic (As), antimony (Sb) and Fe oxide in the soils in wet-dry rotation environment[D]. Guiyang:Guizhou University, 2015.
[42]
韩春梅,王林山,巩宗强,等.土壤中重金属形态分析及其环境学意义[J].生态学杂志, 2005,(12):1499-1502. Han C M, Wang L X, Gong Z Q, et al. Chemical forms of soil heavy metals and their environmental significance[J]. Chinese Journal of Ecology, 2005,(12):1499-1502.
[43]
何孟常,万红艳.环境中锑的分布、存在形态及毒性和生物有效性[J].化学进展, 2004,(1):131-135. He M C, Wan H Y. Distribution, speciation, toxicity and bioavailability of antimony in the environment[J]. Progress in chemistry, 2004,(1):131-135.
[44]
李平,王兴祥,郎漫等.改良剂对Cu、Cd污染土壤重金属形态转化的影响[J].中国环境科学, 2012,32(7):1241-1249. Li P, Wang X X, Lang M, et al. Effects of amendments on the fraction transform of heavy metals in soil contaminated by copper and cadmium[J]. China Environmental Science, 2012,32(7):1241-1249.
[45]
葛英勇,秦贵平.利用七水硫酸亚铁生产一水硫酸亚铁及聚合硫酸铁[J].无机盐工业, 1999,(5):29-30,2. Ge Y Y, Qin G P. The process for producing monohydrate ferrous sulfate and PolyFerric sulfate from ferrous sulfate[J]. Inorganic Chemicals Industry, 1999,(5):29-30,2.
[46]
陈鑫蕊.针铁矿/水界面Cd (Ⅱ)/Pb (Ⅱ)竞争吸附及CD-MUSIC模型模拟[D].武汉:华中农业大学, 2018. Chen X R. Competitive adsorption of Cd (Ⅱ) and Pb (Ⅱ) on goethite and CD-MUSIC modeling[D]. Wuhan:Huazhong Agricultural University, 2018.
[47]
潘霖霖.零价铁/活性炭组合工艺去除地下水中氯乙烯类污染物试验研究[D].济南:山东建筑大学, 2017. Pan L L. Experimental study on removal of vinyl chloride pollutants in groundwater by zero valent iron/activated carbon process[D]. Jinan:Shandong Jianzhu University, 2017.
[48]
范文峰,朱广斌,田兴凯.可溶性废氢氧化铝重溶回收的技术应用[J].有色冶金节能, 2014,30(1):16-18,37. Fan W F, Zhu G B, Tian X K. Application of redissolving and recycling technology of dissolved waste aluminum hydroxide[J]. Energy Saving of Nonferrous Metallurgy, 2014,30(1):16-18,37.