膨润土、褐煤及其混合添加对铅污染土壤钝化修复效应研究
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摘要
土壤重金属污染原位钝化修复是通过向土壤中添加一些钝化修复材料,通过溶解沉淀、离子交换吸附、氧化还原、有机络合等反应来改变土壤中重金属的赋存形态,降低土壤中重金属的生物有效性,在重金属污染修复中具有重要意义。为探究膨润土与褐煤单一及其复配材料对Pb污染土壤的钝化修复效果,以采自河南省济源市某铅冶炼企业周边0-20 cm表层重金属污染土壤为研究材料,设置盆栽玉米(Zea mays L.)试验,采用正交试验处理将膨润土(S)和褐煤(P)按1.5%、3%、5%的浓度梯度单独添加,以及将二者正交混合添加,采用BCR连续提取法研究不同钝化剂处理对Pb污染土壤的修复效应。结果表明,膨润土单一施用对土壤中Pb的有效态含量降低不明显,而褐煤的单一施用能显著降低土壤中Pb的有效态含量,其中添加5%褐煤的处理中弱酸提取态含量降幅达48.7%。膨润土与褐煤混合处理使土壤中Pb的弱酸提取态含量降幅达19.1%-50.8%,残渣态含量增幅达4.8%-40.5%,其中1.5%膨润土+5%褐煤的复配处理对Pb污染土壤的钝化修复效果最佳。膨润土与褐煤配施处理使玉米茎叶中Pb含量降幅为3.4%-33.7%,而膨润土与褐煤的单一钝化处理效果不明显。膨润土与褐煤单一及其配施处理均能显著降低玉米根中Pb含量,降幅为41.5%-66.0%,对玉米根部富集Pb有良好的抑制效果。褐煤单一施用对Pb污染土壤的钝化修复效果整体优于膨润土,两者配施的修复效果因其配施比例而异。
In situ immobilization of heavy metal in contaminated soils with amendments can decrease the bioavailability of heavy metals by changing occurrence state of heavy metals in soils, caused by the reactions of dissolution/precipitation, exchange/adsorption, oxidation/reduction and organic complex. This method has been considered as a non-replaceable and important measure for contaminated soil remediation. In this work, pot experiments were conducted to investigate the effects of bentonite(S) and lignite(P) addition on immobilization and remediation of Pb contaminated soils sampled from Jiyuan City, Henan Province. The addition amounts of bentonite(S) and lignite(P) were 1.5%, 3%, 5% respectively, and the mixture treatment was based on the orthogonal experimental design. BCR(European Community Bureau of Reference) sequential extraction method was used to assess the remediation effects of amendments on soils polluted by Pb after incubation and seedling stage. The results indicated that adding lignite alone could significantly reduce the weak acid extractable content of Pb, while there was no significant difference by bentonite addition alone. Among lignite treatments, 5% lignite treatment decreased the weak acid extractable content of Pb by48.7%. The mixed treatment of bentonite(S) and lignite(P) worked well, which decreased the weak acid extractable content of soil Pb by 19.1%-50.8%, and increased the residual content of Pb by 4.8%-40.5%. The mixed treatment of bentonite(S) and lignite(P)reduced by 3.4%-33.7% of Pb content in stems and leaves in contrast to the CK, but bentonite(S) or lignite(P) alone made no difference. All the treatments, mixed addition or alone, can significantly reduce Pb content in roots by 41.5%-66.0% in contrast to the CK. For the immobilization and remediation effect, lignite treatment works better than bentonite treatment, and the effects of the combinations of these two amendments are different due to each proportion.
In situ immobilization of heavy metal in contaminated soils with amendments can decrease the bioavailability of heavy metals by changing occurrence state of heavy metals in soils, caused by the reactions of dissolution/precipitation, exchange/adsorption, oxidation/reduction and organic complex. This method has been considered as a non-replaceable and important measure for contaminated soil remediation. In this work, pot experiments were conducted to investigate the effects of bentonite(S) and lignite(P) addition on immobilization and remediation of Pb contaminated soils sampled from Jiyuan City, Henan Province. The addition amounts of bentonite(S) and lignite(P) were 1.5%, 3%, 5% respectively, and the mixture treatment was based on the orthogonal experimental design. BCR(European Community Bureau of Reference) sequential extraction method was used to assess the remediation effects of amendments on soils polluted by Pb after incubation and seedling stage. The results indicated that adding lignite alone could significantly reduce the weak acid extractable content of Pb, while there was no significant difference by bentonite addition alone. Among lignite treatments, 5% lignite treatment decreased the weak acid extractable content of Pb by48.7%. The mixed treatment of bentonite(S) and lignite(P) worked well, which decreased the weak acid extractable content of soil Pb by 19.1%-50.8%, and increased the residual content of Pb by 4.8%-40.5%. The mixed treatment of bentonite(S) and lignite(P)reduced by 3.4%-33.7% of Pb content in stems and leaves in contrast to the CK, but bentonite(S) or lignite(P) alone made no difference. All the treatments, mixed addition or alone, can significantly reduce Pb content in roots by 41.5%-66.0% in contrast to the CK. For the immobilization and remediation effect, lignite treatment works better than bentonite treatment, and the effects of the combinations of these two amendments are different due to each proportion.
引文
AYARI F,SRASRA E,TRABELSI-AYADI M,2007.Retention of lead from an aqueous solution by use of bentonite as adsorbent for reducing leaching from industrial effluents[J].Desalination,206(1-3):270-278.
BROWN L,SEATON K,MOHSENI R,et a1.,2013.Immobilization of heavy metals on pillared montmorillonite with a grafted chelate ligand[J].Journal of Hazardous Materials,261:181-187.
GUPTA S S,BHATTAEHARYYA K G,2012.Adsorption of heavy metals on kaolinite and montmorillonite:a review[J].Physical Chemistry Chemical Physics,14(19):6698-6723.
HAMIDPOUR M,KALBASI M,AFYUNI M,et a1.,2010.Sorption hysteresis of Cd(Ⅱ)and Pb(Ⅱ)on natural zeolite and bentonite[J].Journal of Hazardous Materials,181(1-3):686-691.
MORERA M T,EEHEVERRIA J C,MAZKIARDN C,et a1.,2001.Isotherms and sequential extraction procedures for evaluating sorption and distribution of heavy metals in soils[J].Environmental Pollution,113(2):135-144.
PUNZ W F,SIEGHARDT H,1993.The response of roots of herbaceous plants species to heavy metals[J].Environmental and Experimental Botany,33(1):85-98.
RAURET G,LóPEZ-SáNCHEZ J F,SAHUQUILLO A,et al.,2000.Application of a modified BCR sequential extraction(three-step)procedure for the determination of extractable trace metal contents in a sewage sludge amended soil reference material(CRM 483),complemented by a three-year stability study of acetic acid and EDTAextractable metal content[J].Journal of Environmental Monitoring,2(3):228-233.
SUN Y B,LI Y,XU Y M,et a1.,2015.In situ stabilization remediation of cadmium(Cd)and lead(Pb)co-contaminated paddy soil using bentonite[J].Applied Clay Science,105-106:200-206.
XI Y H,WU X F,XIONG H,2014.Solidification/stabilization of Pb-contaminated soils with cement and other additives[J].Soil and Sediment Contamination:An International Journal,23(8):887-898.
ZHANG J J,WANG Y,LIU J S,et a1.,2016.Multivariate and geostatistical analyses of the sources and spatial distribution of heavy metals in agricultural soil in Gongzhuling,Northeast China[J].Journal of Soils and Sediments,16(2):634-644.
陈磊,2013.腐植酸液肥、复合肥对“金农丝苗”稻米重金属富集影响的研究[D].长沙:中南大学.CHEN L,2013.Study on the effects of compound fertilizer and humic acid liquid fertilizer amendments on metal contamination accumulation in Rice[D].Changsha:Central South University.
丁满,杨秋云,化党领,等,2017.褐煤基材料对石灰性土壤铅镉生物有效性的影响[J].农业环境科学学报,36(4):678-685.DING M,YANG Q Y,HUA D L,et a1.,2017.Effects of amendments derived from lignite on Pb,Cd bioavailability of lettuce in calcareous soil[J].Journal of Agro-Environment Science,36(4):678-685.
高瑞丽,唐茂,付庆灵,等,2017.生物炭、蒙脱石及其混合添加对复合污染土壤中重金属形态的影响[J].环境科学,38(1):361-367.GAO R L,TANG M,FU Q L,et a1.,2017.Fractions transformation of heavy metals in compound contaminated soil treated with biochar,montmorillonite and mixed addition[J].Environmental Science,38(1):361-367.
杭小帅,周健民,王火焰,等,2007.粘土矿物修复重金属污染土壤[J].环境工程学报,1(9):113-120.HANG X S,ZHOU J M,WANG H Y,et a1.,2007.Remediation of heavy metal contaminated soils using clay minerals[J].Chinese Journal of Environmental Engineering,1(9):113-120.
景鑫鑫,李真理,程海宽,等,2015.不同固化剂对玉米吸收铅镉的影响[J].中国农学通报,31(15):38-43.JING X X,LI Z L,CHENG H K,et a1.,2015.Effect of different stabilizers on the uptake of cadmium and lead by maize[J].Chinese Agricultural Science Bulletin,31(15):38-43.
李丽君,张强,白光洁,等,2014.改良剂与油菜对土壤重金属有效态的影响[J].水土保持学报,28(1):248-251.LI L J,ZHANG Q,BAI G J,et a1.,2014.The influence of amendments and rape on available heavy metals content in soil[J].Journal of Soil and Water Conservation,28(1):248-251.
刘文庆,2014.纳米羟基磷灰石对铅污染土壤钝化修复效应研究[D].太原:太原理工大学.LIU W Q,2014.The effects of Nano-scale hydroxyapatite on immobilization remediation of Pb-contaminated soil[D].Taiyuan:Taiyuan University of Technology.
刘维涛,周启星,2010.不同土壤改良剂及其组合对降低大白菜镉和铅含量的作用[J].环境科学学报,30(9):1846-1853.LIU W T,ZHOU Q X,2010.Effectiveness of different soil ameliorants in reducing concentrations of Cd and Pb in Chinese cabbage[J].Acta Scientiae Circumstantiae,30(9):1846-1853.
马献发,李伟彤,孟庆峰,等,2016.简述腐植酸在土壤重金属污染修复中的作用[J].腐植酸(6):4-5.MA X F,LI W T,MENG Q F,et a1.,2016.The remediation effect of heavy metals contaminated soil by humic acid[J].Humic Acid(6):4-5.
王成贤,2015.腐植酸对土壤中重金属活性和植物有效性的影响[J].广州化工,43(8):38-40.WANG C X,2015.Effects of humic acid on heavy metal activity and plant availability in soil[J].Guangzhou Chemical Industry,43(8):38-40.
吴烈善,曾东梅,莫小荣,等,2015.不同钝化剂对重金属污染土壤稳定化效应的研究[J].环境科学,36(1):309-313.WU L S,ZENG D M,MO X R,et a1.,2015.Immobilization impact of different fixatives on heavy metals contaminated soil[J].Environmental Science,36(1):309-313.
武瑞平,薛金辉,王中慧,等,2016.腐殖酸对铅污染土壤中油菜生长的影响[J].山东化工,45(23):49-50.WU R P,XUE J H,WANG Z H,et a1.,2016.Effect of humic acid on the growth of rape in lead contaminated soil[J].Shandong Chemical Industry,45(23):49-50.
肖丹丹,2017.腐植酸对铅镉污染土壤中重金属形态及油菜抗氧化酶活性的影响[D].泰安:山东农业大学.XIAO D D,2017.Effects of humic acid on heavy metal forms and antioxidant enzymes activities in soil contaminated by lead and cadmium[D].Tai’an:Shandong Agricultural University.
杨素勤,程海宽,张彪,等,2014.不同品种小麦Pb积累差异性研究[J].生态与农村环境学报,30(5):646-651.YANG S Q,CHENG H K,ZHANG B,et a1.,2014.Differences in Pb accumulation between wheat varieties[J].Journal of Ecology and Rural Environment,30(5):646-651.
于寒,梁煊赫,张玉秋,等,2015.不同秸秆还田方式对玉米根际土壤微生物及酶活性的影响[J].农业资源与环境学报,32(3):305-311.YU H,LIANG X H,ZHANG Y Q,et a1.,2015.Effects of different straw returning models on the soil microorganism and enzyme activity in corn field[J].Journal of Agricultural Resources and Environment,32(3):305-311.
章智明,黄占斌,单瑞娟,2013.腐植酸对土壤改良作用探讨议[J].环境与可持续发展(3):l09-111.ZHANG Z M,HUANG Z B,SHAN R J,2013.Discussion of humic acid on soil amelioration[J].Environment and Sustainable Development(3):l09-111.
朱海军,廖家莉,张东,等,2015.土壤腐殖酸的提取及其对U(VI)的吸附[J].原子能科学技术,9(12):5788-5794.ZHU H J,LIAO J L,ZHANG D,et a1.,2015.Adsorption of U(VI)by humic acid extracted from soil[J].Atomic Energy Science and Technology,9(12):5788-5794.
邹德乙,2007.腐植酸对防治土壤重金属污染的作用[J].腐植酸环保应用(3):50-51.ZOU D Y,2007.Effect of humic acid on soil heavy metal pollution control[J].Humic Acid Environmental Protection Application(3):50-51.
BROWN L,SEATON K,MOHSENI R,et a1.,2013.Immobilization of heavy metals on pillared montmorillonite with a grafted chelate ligand[J].Journal of Hazardous Materials,261:181-187.
GUPTA S S,BHATTAEHARYYA K G,2012.Adsorption of heavy metals on kaolinite and montmorillonite:a review[J].Physical Chemistry Chemical Physics,14(19):6698-6723.
HAMIDPOUR M,KALBASI M,AFYUNI M,et a1.,2010.Sorption hysteresis of Cd(Ⅱ)and Pb(Ⅱ)on natural zeolite and bentonite[J].Journal of Hazardous Materials,181(1-3):686-691.
MORERA M T,EEHEVERRIA J C,MAZKIARDN C,et a1.,2001.Isotherms and sequential extraction procedures for evaluating sorption and distribution of heavy metals in soils[J].Environmental Pollution,113(2):135-144.
PUNZ W F,SIEGHARDT H,1993.The response of roots of herbaceous plants species to heavy metals[J].Environmental and Experimental Botany,33(1):85-98.
RAURET G,LóPEZ-SáNCHEZ J F,SAHUQUILLO A,et al.,2000.Application of a modified BCR sequential extraction(three-step)procedure for the determination of extractable trace metal contents in a sewage sludge amended soil reference material(CRM 483),complemented by a three-year stability study of acetic acid and EDTAextractable metal content[J].Journal of Environmental Monitoring,2(3):228-233.
SUN Y B,LI Y,XU Y M,et a1.,2015.In situ stabilization remediation of cadmium(Cd)and lead(Pb)co-contaminated paddy soil using bentonite[J].Applied Clay Science,105-106:200-206.
XI Y H,WU X F,XIONG H,2014.Solidification/stabilization of Pb-contaminated soils with cement and other additives[J].Soil and Sediment Contamination:An International Journal,23(8):887-898.
ZHANG J J,WANG Y,LIU J S,et a1.,2016.Multivariate and geostatistical analyses of the sources and spatial distribution of heavy metals in agricultural soil in Gongzhuling,Northeast China[J].Journal of Soils and Sediments,16(2):634-644.
陈磊,2013.腐植酸液肥、复合肥对“金农丝苗”稻米重金属富集影响的研究[D].长沙:中南大学.CHEN L,2013.Study on the effects of compound fertilizer and humic acid liquid fertilizer amendments on metal contamination accumulation in Rice[D].Changsha:Central South University.
丁满,杨秋云,化党领,等,2017.褐煤基材料对石灰性土壤铅镉生物有效性的影响[J].农业环境科学学报,36(4):678-685.DING M,YANG Q Y,HUA D L,et a1.,2017.Effects of amendments derived from lignite on Pb,Cd bioavailability of lettuce in calcareous soil[J].Journal of Agro-Environment Science,36(4):678-685.
高瑞丽,唐茂,付庆灵,等,2017.生物炭、蒙脱石及其混合添加对复合污染土壤中重金属形态的影响[J].环境科学,38(1):361-367.GAO R L,TANG M,FU Q L,et a1.,2017.Fractions transformation of heavy metals in compound contaminated soil treated with biochar,montmorillonite and mixed addition[J].Environmental Science,38(1):361-367.
杭小帅,周健民,王火焰,等,2007.粘土矿物修复重金属污染土壤[J].环境工程学报,1(9):113-120.HANG X S,ZHOU J M,WANG H Y,et a1.,2007.Remediation of heavy metal contaminated soils using clay minerals[J].Chinese Journal of Environmental Engineering,1(9):113-120.
景鑫鑫,李真理,程海宽,等,2015.不同固化剂对玉米吸收铅镉的影响[J].中国农学通报,31(15):38-43.JING X X,LI Z L,CHENG H K,et a1.,2015.Effect of different stabilizers on the uptake of cadmium and lead by maize[J].Chinese Agricultural Science Bulletin,31(15):38-43.
李丽君,张强,白光洁,等,2014.改良剂与油菜对土壤重金属有效态的影响[J].水土保持学报,28(1):248-251.LI L J,ZHANG Q,BAI G J,et a1.,2014.The influence of amendments and rape on available heavy metals content in soil[J].Journal of Soil and Water Conservation,28(1):248-251.
刘文庆,2014.纳米羟基磷灰石对铅污染土壤钝化修复效应研究[D].太原:太原理工大学.LIU W Q,2014.The effects of Nano-scale hydroxyapatite on immobilization remediation of Pb-contaminated soil[D].Taiyuan:Taiyuan University of Technology.
刘维涛,周启星,2010.不同土壤改良剂及其组合对降低大白菜镉和铅含量的作用[J].环境科学学报,30(9):1846-1853.LIU W T,ZHOU Q X,2010.Effectiveness of different soil ameliorants in reducing concentrations of Cd and Pb in Chinese cabbage[J].Acta Scientiae Circumstantiae,30(9):1846-1853.
马献发,李伟彤,孟庆峰,等,2016.简述腐植酸在土壤重金属污染修复中的作用[J].腐植酸(6):4-5.MA X F,LI W T,MENG Q F,et a1.,2016.The remediation effect of heavy metals contaminated soil by humic acid[J].Humic Acid(6):4-5.
王成贤,2015.腐植酸对土壤中重金属活性和植物有效性的影响[J].广州化工,43(8):38-40.WANG C X,2015.Effects of humic acid on heavy metal activity and plant availability in soil[J].Guangzhou Chemical Industry,43(8):38-40.
吴烈善,曾东梅,莫小荣,等,2015.不同钝化剂对重金属污染土壤稳定化效应的研究[J].环境科学,36(1):309-313.WU L S,ZENG D M,MO X R,et a1.,2015.Immobilization impact of different fixatives on heavy metals contaminated soil[J].Environmental Science,36(1):309-313.
武瑞平,薛金辉,王中慧,等,2016.腐殖酸对铅污染土壤中油菜生长的影响[J].山东化工,45(23):49-50.WU R P,XUE J H,WANG Z H,et a1.,2016.Effect of humic acid on the growth of rape in lead contaminated soil[J].Shandong Chemical Industry,45(23):49-50.
肖丹丹,2017.腐植酸对铅镉污染土壤中重金属形态及油菜抗氧化酶活性的影响[D].泰安:山东农业大学.XIAO D D,2017.Effects of humic acid on heavy metal forms and antioxidant enzymes activities in soil contaminated by lead and cadmium[D].Tai’an:Shandong Agricultural University.
杨素勤,程海宽,张彪,等,2014.不同品种小麦Pb积累差异性研究[J].生态与农村环境学报,30(5):646-651.YANG S Q,CHENG H K,ZHANG B,et a1.,2014.Differences in Pb accumulation between wheat varieties[J].Journal of Ecology and Rural Environment,30(5):646-651.
于寒,梁煊赫,张玉秋,等,2015.不同秸秆还田方式对玉米根际土壤微生物及酶活性的影响[J].农业资源与环境学报,32(3):305-311.YU H,LIANG X H,ZHANG Y Q,et a1.,2015.Effects of different straw returning models on the soil microorganism and enzyme activity in corn field[J].Journal of Agricultural Resources and Environment,32(3):305-311.
章智明,黄占斌,单瑞娟,2013.腐植酸对土壤改良作用探讨议[J].环境与可持续发展(3):l09-111.ZHANG Z M,HUANG Z B,SHAN R J,2013.Discussion of humic acid on soil amelioration[J].Environment and Sustainable Development(3):l09-111.
朱海军,廖家莉,张东,等,2015.土壤腐殖酸的提取及其对U(VI)的吸附[J].原子能科学技术,9(12):5788-5794.ZHU H J,LIAO J L,ZHANG D,et a1.,2015.Adsorption of U(VI)by humic acid extracted from soil[J].Atomic Energy Science and Technology,9(12):5788-5794.
邹德乙,2007.腐植酸对防治土壤重金属污染的作用[J].腐植酸环保应用(3):50-51.ZOU D Y,2007.Effect of humic acid on soil heavy metal pollution control[J].Humic Acid Environmental Protection Application(3):50-51.
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