共存重金属离子对针铁矿活化过硫酸盐去除水中磺胺吡啶的影响
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摘要
基于硫酸根自由基的高级氧化技术能有效降解水中磺胺类药物残留。由于在自然环境中共存重金属会对环境修复效果产生一定影响,文中重点研究了不同pH环境条件下不同重金属离子对针铁矿活化过硫酸盐(PS)去除水中磺胺吡啶(SPY)的影响。不同类型重金属离子(Cu~(2+)、Pb~(2+)、Cd~(2+),0.2mmol/L)在反应体系(初始条件:针铁矿,1.0g/L;PS,4mmol/L;SPY,10mg/L;pH=8.2)中对SPY的降解对比研究发现:在无重金属共存的条件下,针铁矿/PS体系降解SPY的去除率为25.2%;Pb~(2+)和Cd~(2+)对针铁矿/PS体系的影响较弱,去除率分别为30.8%和34.8%;Cu~(2+)的促进作用很大,可以使SPY被完全降解(100%)。机理分析认为,在针铁矿/PS体系中Pb~(2+)和Cd~(2+)主要通过影响吸附作用导致磺胺吡啶被去除,而Cu~(2+)主要通过自身活化PS的作用。不同pH条件(3.0,8.0,12.0)实验证实弱碱性条件下,Cu~(2+)/针铁矿/PS能够发挥较高的活性从而降解SPY。本文结果为采用针铁矿活化过硫酸盐技术修复类似复合污染地下水环境提供了实验依据。
Sulfonamides(SAs)can be degraded effectively by the sulfate radical based advanced oxidation processes(SR-AOPs)in aqueous solutions.The remediation efficiency could be affected by the coexisting heavy metal ions in the natural environment.Accordingly in the present study,we focused on the effects of different metal ions on the activation of persulfate(PS)by goethite for the sulfapyridine(SPY)removal under different pH conditions.The experiments were conducted in systems(initial conditions:goethite,1.0g/L;PS,4mmol/L;SPY,10mg/L;pH=8.2)containing coexisting heavy metal ions(Cu~(2+),Pb~(2+)and Cd~(2+),0.2mmol/L)and SPY degradation was monitored.The results showed that the removal of SPY in the goethite/PS system without heavy metal ions was 25.2%,and the effects of Pb~(2+)and Cd~(2+)were small(Pb~(2+),30.8%;Cd~(2+),34.8%).Comparingly,SPY degradation was enhanced to a complete removal(100%)by Cu~(2+).Mechanistic analysis indicated that Pb~(2+)and Cd~(2+)mainly affected the adsorption of SPY in the goethite/PS system,but Cu~(2+)by itself could activate PS.Under different pH conditions(3.0,8.0and 12.0),we confirmed that the Cu~(2+)/goethite/PS system could remove SPY completely from a weak alkaline solution.This study therefore provided experimental evidence in supporting the use of goethite for perfulfate activation in the remediation of complex pollutants in aqueous media.
Sulfonamides(SAs)can be degraded effectively by the sulfate radical based advanced oxidation processes(SR-AOPs)in aqueous solutions.The remediation efficiency could be affected by the coexisting heavy metal ions in the natural environment.Accordingly in the present study,we focused on the effects of different metal ions on the activation of persulfate(PS)by goethite for the sulfapyridine(SPY)removal under different pH conditions.The experiments were conducted in systems(initial conditions:goethite,1.0g/L;PS,4mmol/L;SPY,10mg/L;pH=8.2)containing coexisting heavy metal ions(Cu~(2+),Pb~(2+)and Cd~(2+),0.2mmol/L)and SPY degradation was monitored.The results showed that the removal of SPY in the goethite/PS system without heavy metal ions was 25.2%,and the effects of Pb~(2+)and Cd~(2+)were small(Pb~(2+),30.8%;Cd~(2+),34.8%).Comparingly,SPY degradation was enhanced to a complete removal(100%)by Cu~(2+).Mechanistic analysis indicated that Pb~(2+)and Cd~(2+)mainly affected the adsorption of SPY in the goethite/PS system,but Cu~(2+)by itself could activate PS.Under different pH conditions(3.0,8.0and 12.0),we confirmed that the Cu~(2+)/goethite/PS system could remove SPY completely from a weak alkaline solution.This study therefore provided experimental evidence in supporting the use of goethite for perfulfate activation in the remediation of complex pollutants in aqueous media.
引文
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[21]余涛,杨忠芳,钟坚,等.土壤中重金属元素Pb、Cd地球化学行为影响因素研究[J].地学前缘,2008,15(5):67-73.
[22]李晓艳,吴超.湖南某铅锌矿土壤重金属形态分析及淋溶液pH值对其淋滤的影响[J].环境工程,2017,35(5):172-176.
[23]赵胜男,史小红,张汉蒙,等.乌梁素海水体重金属元素赋存形态模拟分析[J].生态环境学报,2018,27(2):341-349.
[24]JI Y,SHI Y,WANG L,et al.Sulfate radical-based oxidation of antibiotics sulfamethazine,sulfapyridine,sulfadiazine,sulfadimethoxine,and sulfachloropyridazine:formation of SO2extrusion products and effects of natural organic matter[J].Science of the Total Environment,2017,593:704-712.
[25]DO S H,KWON Y J,KONG S H.Effect of metal oxides on the reactivity of persulfate/Fe(Ⅱ)in the remediation of diesel-contaminated soil and sand[J].Journal of Hazardous Materials,2010,182(1):933-936.
[26]ZHANG Y,ZHANG Q,DONG Z,et al.Degradation of acetaminophen with ferrous/copperoxide activate persulfate:Synergism of iron and copper[J].Water Research,2018,146:232-243.
[27]SWEDLUND P J,WEBSTER J G,MISKELLY G M.Goethite adsorption of Cu(Ⅱ),Pb(Ⅱ),Cd(Ⅱ),and Zn(Ⅱ)in the presence of sulfate:properties of the ternary complex[J].Geochimica et Cosmochimica Acta,2009,73(6):1548-1562.
[28]PAN X,YAN L,QU R,et al.Degradation of the UV-filter benzophenone-3in aqueous solution using persulfate activated by heat,metal ions and light[J].Chemosphere,2018,196:95-104.
[29]马莹莹,吴跃辉,李锦卫,等.镀铜废水中Cu2+-H2O2体系氧化降解硝基苯[J].环境工程学报,2016,10(9):4775-4782.
[2]KUMMERER K.Antibiotics in the aquatic environment:a review(partⅡ)[J].Chemosphere,2009,75(4):435-441.
[3]REEMTSMA T,WEISS S,MUELLER J,et al.Polar pollutants entry into the water cycle by municipal wastewater:a European perspective[J].Environmental Science and Technology,2006,40(17):5451-5458.
[4]BARAN W,ADAMEK E,ZIEMIANSKA J,et al.Effects of the presence of sulfonamides in the environment and their influence on human health[J].Journal of Hazardous Materials,2011,196(1):1-15.
[5]RIZZO L,MANAIA C,MERLIN C,et al.Urban wastewater treatment plants as hotspots for antibiotic resistant bacteria and genes spread into the environment:a review[J].Science of the Total Environment,2013,447(9):345-360.
[6]VIDAL J,HUILINIR C,SANTANDER R,et al.Effective removal of the antibiotic nafcillin from water by combining the photoelectro-Fenton process and anaerobic biological digestion[J].Science of the Total Environment,2018,624:1095-1105.
[7]CHOI K J,SON H J,KIM S H.Ionic treatment for removal of sulfonamide and tetracycline classes of antibiotic[J].Science of the Total Environment,2007,387(1):247-256.
[8]GHOLAMI M,MIRZAEI R,KALANTARY R R,et al.Performance evaluation of reverse osmosis technology for selected antibiotics removal from synthetic pharmaceutical wastewater[J].Iranian Journal of Environmental Health Science and Engineering,2012,9(12):1-10.
[9]TIAN Y,GAO B,MORALES V L,et al.Removal of sulfamethoxazole and sulfapyridine by carbon nanotubes in fixedbed columns[J].Chemosphere,2013,90(10):2597-2605.
[10]WEI X,GAO N,LI C,et al.Zero-valent iron(ZVI)activation of persulfate(PS)for oxidation of bentazon in water[J].Chemical Engineering Journal,2016,285:660-670.
[11]ZHOU T,ZOU X,MAO J,et al.Decomposition of sulfadiazine in a sonochemical Fe0-catalyzed persulfate system:parameters optimizing and interferences of wastewater matrix[J].Applied Catalysis B Environmental,2016,185:31-41.
[12]OH S Y,KIM H W,PARK J M,et al.Oxidation of polyvinyl alcohol by persulfate activated with heat,Fe2+,and zero-valent iron[J].Journal of Hazardous Materials,2009,168(1):346-351.
[13]AHMAD M,TEEL A L,WATTS R J.Persulfate activation by subsurface minerals[J].Journal of Contaminant Hydrology,2010,115(1/2/3/4):34-45.
[14]SATAPANAJARU T,CHOKEJAROENRAT C,SAKULTHAEWC,et al.Remediation and restoration of petroleum hydrocarbon containing alcohol-contaminated soil by persulfate oxidation activated with soil minerals[J].Water Air and Soil Pollution,2017,228(9):345.
[15]刘雅莉,刘菲,黄伟英.菱铁矿催化过氧化氢-过硫酸钠修复地下水中TCE时对微生物的影响[J].地学前缘,2014,21(4):186-190.
[16]CHENG M,WU L,HUANG Y,et al.Total concentrations of heavy metals and occurrence of antibiotics in sewage sludges from cities throughout China[J].Journal of Soils and Sediments,2014,14(6):1123-1135.
[17]ZHANG Z Z,ZHANG Q Q,XU J J,et al.Long-term effects of heavy metals and antibiotics on granule-based anammox process:granule property and performance evolution[J].Applied Microbiology and Biotechnology,2016,100(5):2417-2427.
[18]INYANG M,GAO B,ZIMMERMAN A,et al.Sorption and cosorption of lead and sulfapyridine on carbon nanotube-modified biochars[J].Environmental Science and Pollution Research,2015,22(3):1868-1876.
[19]XIE M,CHEN W,XU Z,et al.Adsorption of sulfonamides to demineralized pine wood biochars prepared under different thermochemical conditions[J].Environmental Pollution,2014,186:187-194.
[20]WANG Y,CHEN S,YANG X,et al.Degradation of 2,2',4,4'-tetrabromodiphenyl ether(BDE-47)by a nano zerovalent iron-activated persulfate process:the effect of metal ions[J].Chemical Engineering Journal,2017,317:613-622.
[21]余涛,杨忠芳,钟坚,等.土壤中重金属元素Pb、Cd地球化学行为影响因素研究[J].地学前缘,2008,15(5):67-73.
[22]李晓艳,吴超.湖南某铅锌矿土壤重金属形态分析及淋溶液pH值对其淋滤的影响[J].环境工程,2017,35(5):172-176.
[23]赵胜男,史小红,张汉蒙,等.乌梁素海水体重金属元素赋存形态模拟分析[J].生态环境学报,2018,27(2):341-349.
[24]JI Y,SHI Y,WANG L,et al.Sulfate radical-based oxidation of antibiotics sulfamethazine,sulfapyridine,sulfadiazine,sulfadimethoxine,and sulfachloropyridazine:formation of SO2extrusion products and effects of natural organic matter[J].Science of the Total Environment,2017,593:704-712.
[25]DO S H,KWON Y J,KONG S H.Effect of metal oxides on the reactivity of persulfate/Fe(Ⅱ)in the remediation of diesel-contaminated soil and sand[J].Journal of Hazardous Materials,2010,182(1):933-936.
[26]ZHANG Y,ZHANG Q,DONG Z,et al.Degradation of acetaminophen with ferrous/copperoxide activate persulfate:Synergism of iron and copper[J].Water Research,2018,146:232-243.
[27]SWEDLUND P J,WEBSTER J G,MISKELLY G M.Goethite adsorption of Cu(Ⅱ),Pb(Ⅱ),Cd(Ⅱ),and Zn(Ⅱ)in the presence of sulfate:properties of the ternary complex[J].Geochimica et Cosmochimica Acta,2009,73(6):1548-1562.
[28]PAN X,YAN L,QU R,et al.Degradation of the UV-filter benzophenone-3in aqueous solution using persulfate activated by heat,metal ions and light[J].Chemosphere,2018,196:95-104.
[29]马莹莹,吴跃辉,李锦卫,等.镀铜废水中Cu2+-H2O2体系氧化降解硝基苯[J].环境工程学报,2016,10(9):4775-4782.