HPAA、MSA和SPP 3种可生物降解螯合剂对污染土壤中重金属的淋洗效率
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摘要
【目的】土壤淋洗是快速去除污染土壤中重金属的实用修复技术之一,但成本低廉、高效且环境友好淋洗剂的研究报道仍然较少。【方法】采用振荡淋洗法研究了2-羟基膦酰基乙酸(HPAA)、巯基琥珀酸(MSA)和十水焦磷酸钠(SPP)3种生物易降解螯合剂在不同浓度、pH及时间下对两种污染土壤中重金属的淋洗效率。【结果】3种试剂对土壤Pb、Cd和Zn的去除率随浓度增加而逐渐提升(P<0.05),且总体上HPAA和MSA的去除率优于SPP。在淋洗浓度为0.05 mol/L,p H值为4和时间为60 min条件下,HPAA对两种土壤Pb、Cd和Zn的去除率分别为3.69%～18.44%、21.74%～38.34%和19.17%～52.95%,而MSA相应是25.91%～39.86%、11.84%～17.03%和19.37%～38.25%。它们对重金属的去除率随淋洗液pH值的升高而呈现不同的变化趋势,随淋洗时间的延长呈准一级动力学和准二级动力学反应过程。因此,HPAA和MSA是可适用于去除复合污染土壤中Pb、Cd和Zn的两种淋洗剂。
【Objective】TSoil washing is one of the feasible techniques that remove heavy metals from contaminated soils. However,limited information is available on low cost,high efficiency and eco-friendly washing reagents.【Method】Three biodegradable chelators including 2-hydroxy phosphonoacetic acid(HPAA),mercaptosuccinic acid(MSA) and sodium pyrophosphate decahydrate(SPP) were used to remove cadmium,lead,and zinc from two contaminated soils near the mine under the different chelator concentrations solution p H values and durations.【Result】The removal efficiencies of Cd,Pb and Zn increased with increasing chelator concentrations(P<0.05). Generally,the efficiencies of soil Pb Cd and Zn by HPAA and MSA were higher than that by SPP. Under the conditions of 0.05 mol/L and pH4 of washing solution and duration of 60 min,the removal efficiencies of soil Cd,Pb and Zn by HPAA were 3.69%～39.86%,11.84%～38.34% and 19.17% ～52.95%,respectively. In addition,the removal efficiencies by MSA were 25.91%～39.86%,11.84%～17.03% and 19.37%～38.25%,respectively. They exhibited various changes with increasing p H values. Their reaction processes displayed pseudo-first and pseudo-second order models with prolonging durations.【Conclusion】HPAA and MSA are two relatively efficient biodegradable chelators removing Pb,Cd and Zn from contaminated soils.
【Objective】TSoil washing is one of the feasible techniques that remove heavy metals from contaminated soils. However,limited information is available on low cost,high efficiency and eco-friendly washing reagents.【Method】Three biodegradable chelators including 2-hydroxy phosphonoacetic acid(HPAA),mercaptosuccinic acid(MSA) and sodium pyrophosphate decahydrate(SPP) were used to remove cadmium,lead,and zinc from two contaminated soils near the mine under the different chelator concentrations solution p H values and durations.【Result】The removal efficiencies of Cd,Pb and Zn increased with increasing chelator concentrations(P<0.05). Generally,the efficiencies of soil Pb Cd and Zn by HPAA and MSA were higher than that by SPP. Under the conditions of 0.05 mol/L and pH4 of washing solution and duration of 60 min,the removal efficiencies of soil Cd,Pb and Zn by HPAA were 3.69%～39.86%,11.84%～38.34% and 19.17% ～52.95%,respectively. In addition,the removal efficiencies by MSA were 25.91%～39.86%,11.84%～17.03% and 19.37%～38.25%,respectively. They exhibited various changes with increasing p H values. Their reaction processes displayed pseudo-first and pseudo-second order models with prolonging durations.【Conclusion】HPAA and MSA are two relatively efficient biodegradable chelators removing Pb,Cd and Zn from contaminated soils.
引文
[1]黄川,李柳,黄珊,等.重金属污染土壤的草酸和EDTA混合淋洗研究[J].环境工程学报,2014,8(8):3480-3486.
[2]ZHANG S,LIN H,DENG L,et al. Cadmium tolerance and accumulation characteristics of Siegesbeckia orientalis L.[J]. Ecological Engineering,2013,51(2):133-139.
[3]陈欣园,仵彦卿.不同化学淋洗剂对复合重金属污染土壤的修复机理[J].环境工程学报,2018,12(10):2845-2854.
[4]冯俊生,张俏晨.土壤原位修复技术研究与应用进展[J].生态环境学报,2014,23(11):1861-1867.
[5]KULIKOWSKA D,GUSIATIN Z M,BULKOWSKA K,et al. Humic substances from sewage sludge compost as washing agent effectively remove Cu and Cd from soil[J]. Chemosphere,2015,136:42-49.
[6]荀志祥,王世泽,王明新,等.超声强化EDDS/EGTA淋洗修复重金属污染土壤[J].环境工程学报,2018,12(6):1766-1774.
[7]FENG C,ZHANG S,LI L,et al. Feasibility of four wastes to remove heavy metals from contaminated soils[J]. Journal of Environmental Management,2018,212:258-265.
[8]朱光旭,郭庆军,杨俊兴,等.淋洗剂对多金属污染尾矿土壤的修复效应及技术研究[J].环境科学,2013,34(9):3690-3696.
[9]朱清清,邵超英,张琢,等.生物表面活性剂皂角苷增效去除土壤中重金属的研究[J].环境科学学报,2010,30(12):2491-2498.
[10]李世业,成杰民.化工厂遗留地铬污染土壤化学淋洗修复研究[J].土壤学报,2015,52(4):869-878.
[11]HU P,YANG B,DONG C,et al. Assessment of EDTA heap leaching of an agricultural soil highly contaminated with heavy metals[J]. Chemosphere,2014,117(1):532-537.
[12]JELUSIC M,LESTAN D. Effect of EDTA washing of metal polluted garden soils. Part I:Toxicity hazards and impact on soil properties[J]. Science of the Total Environment,2014,475:132-141.
[13]王昕,刘振法,高玉华,等.环境友好型海水缓蚀剂的研制及性能研究[J].水处理技术,2012,38(8):37-39.
[14]尚志航,葛欣,隋丽丽,等.巯基琥珀酸包被的CdTe量子点的制备及其在细胞标记中的应用[J].光谱实验室,2013,30(3):1367-1370.
[15]YOON J,EI MOHTAR C S. Rheological properties of sodium pyrophosphate modified bentonite suspensions for seepage control[J]. Engineering Geology,2014,179:32-40.
[16]鲍士旦.土壤农化分析[M].第3版.北京：中国农业出版社，2007.
[17]NEMATI K,BAKAR N K A,ABAS M R,et al.Speciation of heavy metals by modified BCR sequential extraction procedure in different depths of sediments from Sungai Buloh,Selangor,Malaysia[J].Journal of Hazardous Materials,2011,192(1):402-410.
[18]生态环境部，国家市场监督管理总局.土壤环境质量：农用地土壤污染风险管控标准（试行）：GB 15618-2018[S].北京：中国标准出版社，2018.
[19]WANG G,ZHANG S,XU X,et al.Heavy metal removal by GL-DA washing:Optimization,redistribution,recycling,and changes in soil fertility[J].Science of The Total Environment,2016(569/570):557-568.
[20]KAN W,XU J,WEN S,et al.Metal ions directed assembly of two coordination polymers based on an organic phosphonate anion and a multidentate N-donor ligand[J].Journal of Molecular Structure,2017,1128:513-519.
[21]刘磊，胡少平，陈英旭，等.淋洗法修复化工厂遗留地重金属污染土壤的可行性[J].应用生态学报，2010,21(6):1537-1541.
[22]李健民，宋凯伟，章晓林，等.组合抑制剂柠檬酸钠和焦磷酸钠在某铅锌矿分离浮选中的作用[J].过程工程学报，2017,17(3):500-505.
[23]PéREZESTEBAN J,ESCOLáSTICO C,MOLINER A,et al.Chemical speciation and mobilization of copper and zinc in naturally contaminated mine soils with citric and tartaric acids[J].Chemosphere,2013,90(2):276-283.
[24]KULIKOWSK D,KLIK B K,GUSIATIN Z M,et al.Sewage sludge can provide a washing agent for remediation of soil from a metallurgical area[J].Catena,2019,173:22-28.
[25]LIU Y,ZHOU Q,YUAN Y,et al.Hydrothermal synthesis of fluorescent carbon dots from sodium citrate and polyacrylamide and their highly selective detection of lead and pyrophosphate[J].Carbon,2017,115:550-560.
[2]ZHANG S,LIN H,DENG L,et al. Cadmium tolerance and accumulation characteristics of Siegesbeckia orientalis L.[J]. Ecological Engineering,2013,51(2):133-139.
[3]陈欣园,仵彦卿.不同化学淋洗剂对复合重金属污染土壤的修复机理[J].环境工程学报,2018,12(10):2845-2854.
[4]冯俊生,张俏晨.土壤原位修复技术研究与应用进展[J].生态环境学报,2014,23(11):1861-1867.
[5]KULIKOWSKA D,GUSIATIN Z M,BULKOWSKA K,et al. Humic substances from sewage sludge compost as washing agent effectively remove Cu and Cd from soil[J]. Chemosphere,2015,136:42-49.
[6]荀志祥,王世泽,王明新,等.超声强化EDDS/EGTA淋洗修复重金属污染土壤[J].环境工程学报,2018,12(6):1766-1774.
[7]FENG C,ZHANG S,LI L,et al. Feasibility of four wastes to remove heavy metals from contaminated soils[J]. Journal of Environmental Management,2018,212:258-265.
[8]朱光旭,郭庆军,杨俊兴,等.淋洗剂对多金属污染尾矿土壤的修复效应及技术研究[J].环境科学,2013,34(9):3690-3696.
[9]朱清清,邵超英,张琢,等.生物表面活性剂皂角苷增效去除土壤中重金属的研究[J].环境科学学报,2010,30(12):2491-2498.
[10]李世业,成杰民.化工厂遗留地铬污染土壤化学淋洗修复研究[J].土壤学报,2015,52(4):869-878.
[11]HU P,YANG B,DONG C,et al. Assessment of EDTA heap leaching of an agricultural soil highly contaminated with heavy metals[J]. Chemosphere,2014,117(1):532-537.
[12]JELUSIC M,LESTAN D. Effect of EDTA washing of metal polluted garden soils. Part I:Toxicity hazards and impact on soil properties[J]. Science of the Total Environment,2014,475:132-141.
[13]王昕,刘振法,高玉华,等.环境友好型海水缓蚀剂的研制及性能研究[J].水处理技术,2012,38(8):37-39.
[14]尚志航,葛欣,隋丽丽,等.巯基琥珀酸包被的CdTe量子点的制备及其在细胞标记中的应用[J].光谱实验室,2013,30(3):1367-1370.
[15]YOON J,EI MOHTAR C S. Rheological properties of sodium pyrophosphate modified bentonite suspensions for seepage control[J]. Engineering Geology,2014,179:32-40.
[16]鲍士旦.土壤农化分析[M].第3版.北京：中国农业出版社，2007.
[17]NEMATI K,BAKAR N K A,ABAS M R,et al.Speciation of heavy metals by modified BCR sequential extraction procedure in different depths of sediments from Sungai Buloh,Selangor,Malaysia[J].Journal of Hazardous Materials,2011,192(1):402-410.
[18]生态环境部，国家市场监督管理总局.土壤环境质量：农用地土壤污染风险管控标准（试行）：GB 15618-2018[S].北京：中国标准出版社，2018.
[19]WANG G,ZHANG S,XU X,et al.Heavy metal removal by GL-DA washing:Optimization,redistribution,recycling,and changes in soil fertility[J].Science of The Total Environment,2016(569/570):557-568.
[20]KAN W,XU J,WEN S,et al.Metal ions directed assembly of two coordination polymers based on an organic phosphonate anion and a multidentate N-donor ligand[J].Journal of Molecular Structure,2017,1128:513-519.
[21]刘磊，胡少平，陈英旭，等.淋洗法修复化工厂遗留地重金属污染土壤的可行性[J].应用生态学报，2010,21(6):1537-1541.
[22]李健民，宋凯伟，章晓林，等.组合抑制剂柠檬酸钠和焦磷酸钠在某铅锌矿分离浮选中的作用[J].过程工程学报，2017,17(3):500-505.
[23]PéREZESTEBAN J,ESCOLáSTICO C,MOLINER A,et al.Chemical speciation and mobilization of copper and zinc in naturally contaminated mine soils with citric and tartaric acids[J].Chemosphere,2013,90(2):276-283.
[24]KULIKOWSK D,KLIK B K,GUSIATIN Z M,et al.Sewage sludge can provide a washing agent for remediation of soil from a metallurgical area[J].Catena,2019,173:22-28.
[25]LIU Y,ZHOU Q,YUAN Y,et al.Hydrothermal synthesis of fluorescent carbon dots from sodium citrate and polyacrylamide and their highly selective detection of lead and pyrophosphate[J].Carbon,2017,115:550-560.