胡敏素和磷酸盐联用对土壤中铜的钝化
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摘要
本文研究了胡敏素和磷酸二氢钾(KH_2PO_4)单独施用以及胡敏素和KH_2PO_4联用等不同情况下,污染土壤中重金属Cu形态的动态变化;采用TCLP(Toxic characteristic leaching procedure)法评价了不同配比钝化剂对污染土壤中Cu的钝化作用,以土壤中典型的根系分泌物酒石酸作为重金属解吸剂来模拟研究土壤中小分子有机酸对Cu钝化后的产物形态变化的影响.结果表明,土壤添加胡敏素和KH_2PO_4能够不同程度地升高土壤pH值,二者联用使酸性土壤pH值从4.90升高到5.22—5.30;添加不同比例的胡敏素和KH_2PO_4均降低了土壤TCLP提取态和酸提取态Cu含量,且P/Cu摩尔比为4∶1时,土壤TCLP提取态和酸提取态Cu含量分别降低了67.8 mg·kg~(-1)和104.5 mg·kg~(-1),而残渣态的Cu含量增加了17.3 mg·kg~(-1).胡敏素和KH_2PO_4联用的效果显著优于二者单独使用;土壤溶液中存在的根系分泌物成分酒石酸对土壤中的Cu具有解吸作用,解吸率随酒石酸浓度增加而提高.胡敏素和KH_2PO_4的联用减少了Cu的解吸,降低了Cu的迁移性.
This study investigated the dynamic change of Cu in contaminated soil under different conditions, including the presence of sole humin and sole potassium dihydrogen phosphate(KH_2PO_4), as well as the presence of humin combined with KH_2PO_4, respectively. The effect of humin and phosphate under different ratios on the passivation of Cu in contaminated soil was evaluated through the toxic characteristic leaching procedure(TCLP). Tartaric acid of typical root exudates in soil was used as a desorbent to stimulate the effect of low molecular weight organic acids on the stability of passivation products. The results indicated that the addition of humin and KH_2PO_4 increased soil pH, e.g, the addition of humin in combination with phosphate enhanced soil pH from 4.90 to 5.22— 5.30. The addition of humin and KH_2PO_4 under different ratios significantly reduced the content of TCLP and acid extraction of Cu from soil. When the P/Cu molar ratio was 4:1, the soil TCLP extraction state and acid extraction Cu content decreased by 67.8 mg·kg~(-1) and 104.5 mg·kg~(-1), respectively, while the residual Cu content increased by 17.3 mg·kg~(-1). The passivation effect on Cu of humin in combination with KH_2PO_4 was better than sole humin or KH_2PO_4. Tartaric acid as a root exudate widely presented in the soil solution, had desorption effect on the passivated Cu in soils, and the desorption increased as the concentration of tartaric acid was increased. In summary, the combination of humin and KH_2PO_4 reduced Cu desorption and hence decreased its migration in soil.
This study investigated the dynamic change of Cu in contaminated soil under different conditions, including the presence of sole humin and sole potassium dihydrogen phosphate(KH_2PO_4), as well as the presence of humin combined with KH_2PO_4, respectively. The effect of humin and phosphate under different ratios on the passivation of Cu in contaminated soil was evaluated through the toxic characteristic leaching procedure(TCLP). Tartaric acid of typical root exudates in soil was used as a desorbent to stimulate the effect of low molecular weight organic acids on the stability of passivation products. The results indicated that the addition of humin and KH_2PO_4 increased soil pH, e.g, the addition of humin in combination with phosphate enhanced soil pH from 4.90 to 5.22— 5.30. The addition of humin and KH_2PO_4 under different ratios significantly reduced the content of TCLP and acid extraction of Cu from soil. When the P/Cu molar ratio was 4:1, the soil TCLP extraction state and acid extraction Cu content decreased by 67.8 mg·kg~(-1) and 104.5 mg·kg~(-1), respectively, while the residual Cu content increased by 17.3 mg·kg~(-1). The passivation effect on Cu of humin in combination with KH_2PO_4 was better than sole humin or KH_2PO_4. Tartaric acid as a root exudate widely presented in the soil solution, had desorption effect on the passivated Cu in soils, and the desorption increased as the concentration of tartaric acid was increased. In summary, the combination of humin and KH_2PO_4 reduced Cu desorption and hence decreased its migration in soil.
引文
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[16] SHAHID M,XIONG T,MASOOD N,et al.Influence of plant species and phosphorus amendments on metal speciation and bioavailability in a smelter impacted soil:A case study of food-chain contamination[J].Journal of Soils & Sediments,2014,14(4):655-665.
[17] LIU R,ZHAO D.In situ immobilization of Cu(II) in soils using a new class of iron phosphate nanoparticles[J].Chemosphere,2007,68(10):1867-1876.
[18] 钟振宇,赵庆圆,陈灿,等.腐殖酸和含磷物质对模拟铅污染农田土壤的钝化效应[J].环境化学,2018,37(6):1327-1336.ZHONG Z Y,ZHAO Q Y,CHEN C,et al.Passivation of simulated lead contaminated farml and soil using humic acid and phosphate[J].Environmental Chemistry,2018,37(6):1327-1336 (in Chinese).
[19] WANG Y,LI L,ZOU X,et al.Impact of humin on soil adsorption and remediation of Cd(II),Pb(II),and Cu(II)[J].Soil and Sediment Contamination,2016,25(6):700-715.
[20] SAYADI M H,REZAEI M R,REZAEI A.Fraction distribution and bioavailability of sediment heavy metals in the environment surrounding MSW landfill:A case study[J].Environmental Monitoring and Assessment,2015,187(1):4110.
[21] CHEN D,FENG H,LI J.Graphene oxide:Preparation,functionalization,and electrochemical applications[J].Chemical Reviews,2012,112(11):6027-6053.
[22] CHEN B,ZHAO H,CHEN S,et al.A magnetically recyclable chitosan composite adsorbent functionalized with EDTA for simultaneous capture of anionic dye and heavy metals in complex wastewater[J].Chemical Engineering Journal,2019,356:69-80.
[23] REFAT M,MOHAMED G G,IBRAHIM M S,et al.Synthesis and characterization of coordination behavior of diclofenac sodium drug toward Hg(II),Pb(II),and Sn(II) metal ions:Chelation effect on their thermal stability and biological activity[J].Synthesis and Reactivity in Inorganic and Metal-Organic Chemistry,2014,44(2):161-170.
[24] ADEEYO R O,BELLO O S.Use of composite sorbents for the removal of copper (II) ions from aqueous solution[J].Pakistan Journal of Analytical & Environmental Chemistry,2015,15(2):1-12.
[25] SHARMA P,HUSSAIN N,BORAH D J,et al.Kinetics and adsorption behavior of the methyl blue at the graphene oxide/reduced graphene oxide nanosheet-water interface:A comparative study[J].Journal of Chemical & Engineering Data,2013,58(12):3477-3488.
[26] CHEN H,DOU J,XU H.The effect of low-molecular-weight organic-acids(LMWOAs)on treatment of chromium-contaminated soils by compost-phytoremediation:Kinetics of the chromium release and fractionation[J].Journal of Environmental Sciences,2018,70(8):48-56..
[27] 王秀丽,梁成华,马子惠,等.施用磷酸盐和沸石对土壤镉形态转化的影响[J].环境科学,2015,36(4):1437-1444.WANG X L,LIANG C H,MA Z H,et al.Effects of phosphate and zeolite on the transformation of cd speciation in soil[J].Journal of Environmental Sciences,2015,36(4):1437-1444 (in Chinese).
[28] DU,YAN,HU,et al.Affects of mining activities on Cd pollution to the paddy soils and rice-grain in Hunan Province,Central South China[J].Environmental Monitoring & Assessment,2013,185(12):9843-9856.
[29] GAO X,CHEN C T A.Heavy metal pollution status in surface sediments of the coastal Bohai Bay[J].Water Research,2012,46(6):1901-1911.
[30] WANG B,XIE Z,CHEN J,et al.Effects of field application of phosphate fertilizers on the availability and uptake of lead,zinc and cadmium by cabbage (Brassica chinensis L.) in a mining tailing contaminated soil[J].Journal of Environmental Sciences,2008,20(9):1109-1117.
[31] YANG Y,CHEN R,FU G,et al.Phosphate deprivation decreases cadmium (Cd) uptake but enhances sensitivity to Cd by increasing iron (Fe) uptake and inhibiting phytochelatins synthesis in rice (Oryza sativa)[J].Acta Physiologiae Plantarum,2016,38(1):28.
[32] STROBEL B W.Influence of vegetation on low-molecular-weight carboxylic acids in soil solution—a review[J].Geoderma,2001,99(3):169-198.
[33] DING Y Z,SONG Z G,FENG R W,et al.Interaction of organic acids and pH on multi-heavy metal extraction from alkaline and acid mine soils[J].International Journal of Environmental Science & Technology,2014,11(1):33-42.
[34] PONGE J.Plant-soil feedbacks mediated by humus forms:A review[J].Soil Biology and Biochemistry,2013,57:1048-1060.
[35] KAUR C,SELVAKUMAR G,GANESHAMURTHY A N.Organic Acids in the Rhizosphere:Their Role in Phosphate Dissolution[M].Springer India,2016.
[2] LUO Y,TU C.Twenty Years of Research and Development on Soil Pollution and Remediation in China[M].Beijing,Science Press,2018.
[3] GANG W,KANG H,ZHANG X,et al.A critical review on the bio-removal of hazardous heavy metals from contaminated soils:Issues,progress,eco-environmental concerns and opportunities[J].Journal of Hazardous Materials,2010,174(1):1-8.
[4] NEBBIOSO A,VINCI G,DROSOS M,et al.Unveiling the molecular composition of the unextractable soil organic fraction (humin) by humeomics[J].Biology & Fertility of Soils,2015,51(4):443-451.
[5] WANG Y,LI L,ZOU X,et al.Impact of Humin on Soil Adsorption and Remediation of Cd(II),Pb(II),and Cu(II)[J].Journal of Soil Contamination,2016,25(6):700-715.
[6] 王雅辉,邹雪刚,舒冉君,等.胡敏素对Pb2+吸附的响应面优化及机理[J].中国环境科学,2017,37(5):1814-1822.WANG Y H,ZOU X G,SHU R J,et al.Adsorption of Pb(II) from aqueous solutions by humin:Optimization and mechanism[J].Chinese Environmental Science,2017,37(5):1814-1822(in Chinese).
[7] 王雅辉.胡敏素对土壤中Cu、Pb的钝化作用研究[D].广州:广东工业大学,2017.WANG Y H.Passivation of Cu and Pb in soils by humin[D].Guangzhou:Guangdong University of Technology,2017 (in Chinese).
[8] CONTRERAS C,DE L R G,PERALTA-VIDEA J R,et al.Lead adsorption by silica-immobilized humin under flow and batch conditions:assessment of flow rate and calcium and magnesium interference[J].Journal of Hazardous Materials,2006,133(1):79-84.
[9] APPEL C,MA L Q,RHUE R D,et al.Sequential sorption of lead and cadmium in three tropical soils[J].Environmental Pollution,2008,155(1):132-140.
[10] CAO X,WAHBI A,MA L,et al.Immobilization of Zn,Cu,and Pb in contaminated soils using phosphate rock and phosphoric acid[J].Journal of Hazardous Materials,2009,164(2):555-564.
[11] ZHANG J,WANG S,WANG Q,et al.First determination of Cu adsorption on soil humin[J].Environmental Chemistry Letters,2013,11(1):41-46.
[12] REN Z,SIVRY Y,THARAUD M,et al.Speciation and reactivity of lead and zinc in heavily and poorly contaminated soils:Stable isotope dilution,chemical extraction and model views[J].Environmental Pollution,2017,225:654-662.
[13] HUANG G,SU X,RIZWAN M S,et al.Chemical immobilization of Pb,Cu,and Cd by phosphate materials and calcium carbonate in contaminated soils[J].Environmental Science and Pollution Research,2016,23(16):16845-16856.
[14] KNOX A S,KAPLAN D I,PALLER M H.Phosphate sources and their suitability for remediation of contaminated soils[J].Science of the Total Environment,2006,357(1):271-279.
[15] CHEN S,XU M,MA Y,et al.Evaluation of different phosphate amendments on availability of metals in contaminated soil[J].Ecotoxicol Environ Saf,2007,67(2):278-285.
[16] SHAHID M,XIONG T,MASOOD N,et al.Influence of plant species and phosphorus amendments on metal speciation and bioavailability in a smelter impacted soil:A case study of food-chain contamination[J].Journal of Soils & Sediments,2014,14(4):655-665.
[17] LIU R,ZHAO D.In situ immobilization of Cu(II) in soils using a new class of iron phosphate nanoparticles[J].Chemosphere,2007,68(10):1867-1876.
[18] 钟振宇,赵庆圆,陈灿,等.腐殖酸和含磷物质对模拟铅污染农田土壤的钝化效应[J].环境化学,2018,37(6):1327-1336.ZHONG Z Y,ZHAO Q Y,CHEN C,et al.Passivation of simulated lead contaminated farml and soil using humic acid and phosphate[J].Environmental Chemistry,2018,37(6):1327-1336 (in Chinese).
[19] WANG Y,LI L,ZOU X,et al.Impact of humin on soil adsorption and remediation of Cd(II),Pb(II),and Cu(II)[J].Soil and Sediment Contamination,2016,25(6):700-715.
[20] SAYADI M H,REZAEI M R,REZAEI A.Fraction distribution and bioavailability of sediment heavy metals in the environment surrounding MSW landfill:A case study[J].Environmental Monitoring and Assessment,2015,187(1):4110.
[21] CHEN D,FENG H,LI J.Graphene oxide:Preparation,functionalization,and electrochemical applications[J].Chemical Reviews,2012,112(11):6027-6053.
[22] CHEN B,ZHAO H,CHEN S,et al.A magnetically recyclable chitosan composite adsorbent functionalized with EDTA for simultaneous capture of anionic dye and heavy metals in complex wastewater[J].Chemical Engineering Journal,2019,356:69-80.
[23] REFAT M,MOHAMED G G,IBRAHIM M S,et al.Synthesis and characterization of coordination behavior of diclofenac sodium drug toward Hg(II),Pb(II),and Sn(II) metal ions:Chelation effect on their thermal stability and biological activity[J].Synthesis and Reactivity in Inorganic and Metal-Organic Chemistry,2014,44(2):161-170.
[24] ADEEYO R O,BELLO O S.Use of composite sorbents for the removal of copper (II) ions from aqueous solution[J].Pakistan Journal of Analytical & Environmental Chemistry,2015,15(2):1-12.
[25] SHARMA P,HUSSAIN N,BORAH D J,et al.Kinetics and adsorption behavior of the methyl blue at the graphene oxide/reduced graphene oxide nanosheet-water interface:A comparative study[J].Journal of Chemical & Engineering Data,2013,58(12):3477-3488.
[26] CHEN H,DOU J,XU H.The effect of low-molecular-weight organic-acids(LMWOAs)on treatment of chromium-contaminated soils by compost-phytoremediation:Kinetics of the chromium release and fractionation[J].Journal of Environmental Sciences,2018,70(8):48-56..
[27] 王秀丽,梁成华,马子惠,等.施用磷酸盐和沸石对土壤镉形态转化的影响[J].环境科学,2015,36(4):1437-1444.WANG X L,LIANG C H,MA Z H,et al.Effects of phosphate and zeolite on the transformation of cd speciation in soil[J].Journal of Environmental Sciences,2015,36(4):1437-1444 (in Chinese).
[28] DU,YAN,HU,et al.Affects of mining activities on Cd pollution to the paddy soils and rice-grain in Hunan Province,Central South China[J].Environmental Monitoring & Assessment,2013,185(12):9843-9856.
[29] GAO X,CHEN C T A.Heavy metal pollution status in surface sediments of the coastal Bohai Bay[J].Water Research,2012,46(6):1901-1911.
[30] WANG B,XIE Z,CHEN J,et al.Effects of field application of phosphate fertilizers on the availability and uptake of lead,zinc and cadmium by cabbage (Brassica chinensis L.) in a mining tailing contaminated soil[J].Journal of Environmental Sciences,2008,20(9):1109-1117.
[31] YANG Y,CHEN R,FU G,et al.Phosphate deprivation decreases cadmium (Cd) uptake but enhances sensitivity to Cd by increasing iron (Fe) uptake and inhibiting phytochelatins synthesis in rice (Oryza sativa)[J].Acta Physiologiae Plantarum,2016,38(1):28.
[32] STROBEL B W.Influence of vegetation on low-molecular-weight carboxylic acids in soil solution—a review[J].Geoderma,2001,99(3):169-198.
[33] DING Y Z,SONG Z G,FENG R W,et al.Interaction of organic acids and pH on multi-heavy metal extraction from alkaline and acid mine soils[J].International Journal of Environmental Science & Technology,2014,11(1):33-42.
[34] PONGE J.Plant-soil feedbacks mediated by humus forms:A review[J].Soil Biology and Biochemistry,2013,57:1048-1060.
[35] KAUR C,SELVAKUMAR G,GANESHAMURTHY A N.Organic Acids in the Rhizosphere:Their Role in Phosphate Dissolution[M].Springer India,2016.
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