黄铁矿强化零价铁去除Orange Ⅱ研究
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摘要
零价铁(ZVI)具有价廉易得、安全无毒、还原性较强等特点,能用于去除环境中众多污染物.但其反应活性会随着介质pH值的升高、表面钝化产物的形成而降低,而且反应介质的pH值适用范围较窄.将价廉的黄铁矿(pyrite)与零价铁混合,用于处理合成废水中的偶氮染料Orange Ⅱ,研究了介质的pH值、pyrite/ZVI质量比对Orange Ⅱ去除率的影响,并对协同反应机理进行了初步探讨.结果表明:在相同实验条件下,pyrite协同ZVI对Orange Ⅱ的去除率远高于相同剂量pyrite和ZVI分别对Orange Ⅱ去除率的加和.当初始pH=7.0、pyrite/ZVI质量比为1～4时,与Orange Ⅱ反应的表观速率常数是相应零价铁的9.36～28.0倍.此外,在初始pH值为5.0～10.0时,pyrite/ZVI对Orange Ⅱ均显示了良好的去除效果.机理研究表明:在零价铁去除Orange Ⅱ时,pyrite的存在导致了反应介质pH值的降低,并能将ZVI表面钝化产物转化为高还原活性Fe(Ⅱ),从而显示出显著的强化作用.
Zero valent iron(ZVI) has been widely applied to the removal of diversified contaminants in the environment due to its lower cost,nontoxicity and high reductivity. However,the reactivity of ZVI will decrease quickly due to the pH rise of reaction medium and surface passivation along with the reaction and narrow working pH. In this work,a combination of pyrite with zero valent iron(ZVI) was used to enhance the removal of azo dye Orange Ⅱ,the effects of pH and the mass ratio of pyrite/ZVI on the removal of Orange Ⅱ were investigated,and the synergetic reaction mechanism was also studied. The results show that under the same reaction condition,the removal efficiency of Orange Ⅱ by pyrite/ZVI is much higher than the sum of that by pyrite and ZVI respectively with the same addition. At initial pH 7.0,the rate constant(k_(obs)) of pyrite/ZVI with the mass ratio ranging from 1.0 to 4.0 is enhanced by 9.36 ～ 28.0 folds compared with that of ZVI alone. Moreover,at the pH ranging from 5.0 ～ 10.0,pyrite/ZVI also shows better efficiency for the removal of Orange Ⅱ. The mechanism study reveals that the presence of pyrite could decrease the pH of reaction medium,and prompt the transformation of passive products on ZVI surface to highly reactive Fe(Ⅱ).
Zero valent iron(ZVI) has been widely applied to the removal of diversified contaminants in the environment due to its lower cost,nontoxicity and high reductivity. However,the reactivity of ZVI will decrease quickly due to the pH rise of reaction medium and surface passivation along with the reaction and narrow working pH. In this work,a combination of pyrite with zero valent iron(ZVI) was used to enhance the removal of azo dye Orange Ⅱ,the effects of pH and the mass ratio of pyrite/ZVI on the removal of Orange Ⅱ were investigated,and the synergetic reaction mechanism was also studied. The results show that under the same reaction condition,the removal efficiency of Orange Ⅱ by pyrite/ZVI is much higher than the sum of that by pyrite and ZVI respectively with the same addition. At initial pH 7.0,the rate constant(k_(obs)) of pyrite/ZVI with the mass ratio ranging from 1.0 to 4.0 is enhanced by 9.36 ～ 28.0 folds compared with that of ZVI alone. Moreover,at the pH ranging from 5.0 ～ 10.0,pyrite/ZVI also shows better efficiency for the removal of Orange Ⅱ. The mechanism study reveals that the presence of pyrite could decrease the pH of reaction medium,and prompt the transformation of passive products on ZVI surface to highly reactive Fe(Ⅱ).
引文
[1]张炳亮.硫化与弱磁场加速零价铁去除水体中偶氮染料及机理研究[D].济南:山东大学,2017.
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[3]陆朝阳,王学江,张全兴,等.树脂吸附法处理分散蓝NKF脱磺母液[J].化工环保,2002,22(6):342-346.
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[5]BELTRAN-HEREDIA J,MARTIN J S.Azo dye removal by Moringa oleifera seed extract coagulation[J].Coloration Technology,2008,124(5):310-317.
[6]YAO Y,LI K,CHEN S,et a1.Decolorization of Rhodamine B in a thin-Film photoelectrocatalytic(PEC)reactor with slant-placed Ti O2 nanotubes electrode[J].Chemical Engineering Journal,2012,187(2):29-35.
[7]KARIYAJJANAVAR P,JOGTTAPPA N,NAYAKA Y A.Studies on degradation of reactive textile dyes solution by electrochemical method[J].Journal of Hazardous Materials,2011,190(1-3):952-961.
[8]TIIRGAY O,ERS6Z G,ATALAY,et a1.The treatment of azo dyes found in textile industry wastewater by anaerobic biological method and chemical oxidation[J].Separation&Purification Technology,2011,79(1):26-33.
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[10]GUAN X,SUN Y,QIN H,et a1.The limitations of applying zero-valent iron technology in contaminants sequestration and the corresponding countermeasures:the development in zero-valent iron technology in the last two decades(1994-2014)[J].Water Research,2015,75:224-228.
[11]LIU H,LI G,QU J,et al.Degradation of azo dye Acid Orange 7 in water by Fe O/granular activated carbon system in the presence of ultrasound[J].Journal of Hazardous materials,2007,144(1):180-186.
[12]DURAN C,OZDES D,GUNDOGDU A,et a1.Kinetics and isotherm analysis of basic dyes adsorption onto almond shell(Prunus dulcis)as a low cost adsorbent[J].Journal of Chemical&Engineering Data,2011,56(5):2136-2147.
[13]KALRA S S,MOHAN,SINHA A,et a1.Advanced oxidation processes for treatment of textile and dye wastewater:A review[C].Singapore:IACSIT Press,2011.
[14]ZHANG W X,WANG C B,LIEN H L,et al.Treatment of chlorinated organic contaminants with nanoscale bimetallic particles[J].Catalysis Today,1998,40(4):387-395.
[15]BARNES R J,RIBA O,GARDNER M N,et al.Inhibition of biological TCE and sulphate reduction in the presence of iron nanoparticles[J].Chemosphere,2010,80(5):554-562.
[16]SCHRICK B,BLOUGH J L,JONES A D,et al.Hydrodechlorination of trichloroethylene to hydrocarbons using bimetallic nickel-iron nanoparticles[J].Chemistry of Materials,2002,14(12):5140-5147.
[17]HU C Y,LO S L,LIOU Y H,et al.Hexavalent chromium removal from near natural water by copper-iron bimetallic particles[J].Water Research,2010,44(10):3101-3108.
[18]ITO D,MIURA K,ICHIMURA T,et al.Removal of As,Cd,Hg and Pb ions from solution by adsorption with bacterially-produced magnetic iron sulfide particles using high gradient magnetic separation[J].IEEE Transactions on Appiled Superconductivity,2004(14):1551-1553.
[19]ZVERDI A,ERDEM M.Cu2+,Cd2+and Pb2+adsorption from aqueous solutions by pyrite and synthetic iron sulphide[J].Journal of Hazardous materials,2006(137):626-632.
[20]WATSON J H P,ELLWOOD D C,DENG Q,et al.Heavy metal adsorption on bacterially produced Fe S[J].Minerals Engineering,1995(8):1097-1108.
[21]CHEN J L,AL-ABED S R,RYAN J A,et al.Effects of p H on dechlorination of trichloroethylene by zero-valent iron[J].Journal of Hazardous materials,2001(83):243-254.
[22]LI X Q,ELLIOTT D W,ZHANG W X.Zero-valent iron nanoparticles for abatement of environmental pollutants:materials and engineering aspects[J].Critical Reviews in Solid State and Materials Sciences,2006(31):111-122.
[23]HENDERSON A D,DEMOND A H.Impact of solids formation and gas production on the permeability of ZVI PRBs[J].Journal of Environmental Engineering,2011(137):689-696.
[24]GUAN X H,SUN Y K,QIN H J,et al.The limitations of applying zero-valent iron technology in contaminants sequestration and the corresponding countermeasures:The development in zero-valent iron technology in the last two decades(1994-2014)[J].Water Research,2015,75:224-248.
[25]FURUKAWA Y,KIM J W,WATKINS J,et al.Formation of ferrihydrite and associated iron corrosion products in permeable reactive barriers of zero-valent iron[J].Environmental Science&Technology,2002,36(24):5469-5475.
[26]PHILLIPS D H,NOOTEN V,BASTIAENS L,et al.Ten Year Performance Evaluation of a Field-Scale ZeroValent Iron Permeable Reactive Barrier Installed to Remediate Trichloroethene Contaminated Groundwater[J].Environmental Science&Technology,2010,44(10):3861-3869.
[27]GONG Y Y,TANG J C,ZHAO D Y,et al.Application of iron sulfide particles for groundwater and soil remediation:A review[J].Water Research,2016,89:309-320.
[28]CHARLET L,KANG M L,BARDELLI F,et al.Nanocomposite Pyrite-Greigite Reactivity toward Se(IV)/Se(VI)[J].Environmental Science&Technology,2012,46(9):4869-4876.
[29]KANTAR C,ARI C,KESKIN S,et al.Cr(VI)removal from aqueous systems using pyrite as the reducing agent:Batch,spectroscopic and column experiments[J].Journal of Contaminant Hydrology,2015,174:28-38.
[30]DIAO Z H,SHI T H,WANG S Z,et al.Silane-based coatings on the pyrite for remediation of acid mine drainage[J].Water Research,2013,47(13):4391-4402.
[31]张杰,吴爱祥.排土场黄铁矿促进黄铜矿浸出研究[J].金属矿山,2008(3):39-41.
[32]LUO F,YANG D,CHEN Z L,et al.One-step green synthesis of bimetallic Fe/Pd nanoparticles used to degrade Orange II[J].Journal of Hazardous Materials,2016,303:145-153.
[33]CHAKRABORTY S,FAVRE F,BANERJEE D,et al.U(VI)sorption and reduction by Fe(II)sorbed on montmorillonite[J].Environmental Science&Technology,2010,44(10):3779-3785.
[34]LYU Y,LI J F,LIA Y M,et al.The roles of pyrite for enhancing reductive removal of nitrobenzene by zerovalent iron[J].Applied Catalysis B:Environmental,2019,242:9-18.
[35]LYU Y,LI Z,LI J F,et al.Synergetic effect of pyrite on Cr(VI)removal by zero valent iron in column experiments:An investigation of mechanisms[J].Chemical Engineering Journal,2018,349:522-529.
[2]HAI F I,YAMAMOTO K,FUKUSHI K.Hybrid treatment systems for dye wastewater[J].Critical Reviews in Environmental Science and Technology,2007,37(4):315-377.
[3]陆朝阳,王学江,张全兴,等.树脂吸附法处理分散蓝NKF脱磺母液[J].化工环保,2002,22(6):342-346.
[4]REIS L G T D,ROBAINA N F,PACHECO W F,et a1.Separation of Malachite Green and Methyl Green cationic dyes from aqueous medium by adsorption on Amberlite XAD-2 and XAD-4 resins using sodium dodecylsulfate as carrier[J].Chemical Engineering Journal,2011,171(2):532-540.
[5]BELTRAN-HEREDIA J,MARTIN J S.Azo dye removal by Moringa oleifera seed extract coagulation[J].Coloration Technology,2008,124(5):310-317.
[6]YAO Y,LI K,CHEN S,et a1.Decolorization of Rhodamine B in a thin-Film photoelectrocatalytic(PEC)reactor with slant-placed Ti O2 nanotubes electrode[J].Chemical Engineering Journal,2012,187(2):29-35.
[7]KARIYAJJANAVAR P,JOGTTAPPA N,NAYAKA Y A.Studies on degradation of reactive textile dyes solution by electrochemical method[J].Journal of Hazardous Materials,2011,190(1-3):952-961.
[8]TIIRGAY O,ERS6Z G,ATALAY,et a1.The treatment of azo dyes found in textile industry wastewater by anaerobic biological method and chemical oxidation[J].Separation&Purification Technology,2011,79(1):26-33.
[9]SUN Y K,LI J X,HUANG T,et al.The influences of iron characteristics,operating conditions and solution chemistry on contaminants removal by zero-valent iron:A review[J].Water Research,2016,100:277-295.
[10]GUAN X,SUN Y,QIN H,et a1.The limitations of applying zero-valent iron technology in contaminants sequestration and the corresponding countermeasures:the development in zero-valent iron technology in the last two decades(1994-2014)[J].Water Research,2015,75:224-228.
[11]LIU H,LI G,QU J,et al.Degradation of azo dye Acid Orange 7 in water by Fe O/granular activated carbon system in the presence of ultrasound[J].Journal of Hazardous materials,2007,144(1):180-186.
[12]DURAN C,OZDES D,GUNDOGDU A,et a1.Kinetics and isotherm analysis of basic dyes adsorption onto almond shell(Prunus dulcis)as a low cost adsorbent[J].Journal of Chemical&Engineering Data,2011,56(5):2136-2147.
[13]KALRA S S,MOHAN,SINHA A,et a1.Advanced oxidation processes for treatment of textile and dye wastewater:A review[C].Singapore:IACSIT Press,2011.
[14]ZHANG W X,WANG C B,LIEN H L,et al.Treatment of chlorinated organic contaminants with nanoscale bimetallic particles[J].Catalysis Today,1998,40(4):387-395.
[15]BARNES R J,RIBA O,GARDNER M N,et al.Inhibition of biological TCE and sulphate reduction in the presence of iron nanoparticles[J].Chemosphere,2010,80(5):554-562.
[16]SCHRICK B,BLOUGH J L,JONES A D,et al.Hydrodechlorination of trichloroethylene to hydrocarbons using bimetallic nickel-iron nanoparticles[J].Chemistry of Materials,2002,14(12):5140-5147.
[17]HU C Y,LO S L,LIOU Y H,et al.Hexavalent chromium removal from near natural water by copper-iron bimetallic particles[J].Water Research,2010,44(10):3101-3108.
[18]ITO D,MIURA K,ICHIMURA T,et al.Removal of As,Cd,Hg and Pb ions from solution by adsorption with bacterially-produced magnetic iron sulfide particles using high gradient magnetic separation[J].IEEE Transactions on Appiled Superconductivity,2004(14):1551-1553.
[19]ZVERDI A,ERDEM M.Cu2+,Cd2+and Pb2+adsorption from aqueous solutions by pyrite and synthetic iron sulphide[J].Journal of Hazardous materials,2006(137):626-632.
[20]WATSON J H P,ELLWOOD D C,DENG Q,et al.Heavy metal adsorption on bacterially produced Fe S[J].Minerals Engineering,1995(8):1097-1108.
[21]CHEN J L,AL-ABED S R,RYAN J A,et al.Effects of p H on dechlorination of trichloroethylene by zero-valent iron[J].Journal of Hazardous materials,2001(83):243-254.
[22]LI X Q,ELLIOTT D W,ZHANG W X.Zero-valent iron nanoparticles for abatement of environmental pollutants:materials and engineering aspects[J].Critical Reviews in Solid State and Materials Sciences,2006(31):111-122.
[23]HENDERSON A D,DEMOND A H.Impact of solids formation and gas production on the permeability of ZVI PRBs[J].Journal of Environmental Engineering,2011(137):689-696.
[24]GUAN X H,SUN Y K,QIN H J,et al.The limitations of applying zero-valent iron technology in contaminants sequestration and the corresponding countermeasures:The development in zero-valent iron technology in the last two decades(1994-2014)[J].Water Research,2015,75:224-248.
[25]FURUKAWA Y,KIM J W,WATKINS J,et al.Formation of ferrihydrite and associated iron corrosion products in permeable reactive barriers of zero-valent iron[J].Environmental Science&Technology,2002,36(24):5469-5475.
[26]PHILLIPS D H,NOOTEN V,BASTIAENS L,et al.Ten Year Performance Evaluation of a Field-Scale ZeroValent Iron Permeable Reactive Barrier Installed to Remediate Trichloroethene Contaminated Groundwater[J].Environmental Science&Technology,2010,44(10):3861-3869.
[27]GONG Y Y,TANG J C,ZHAO D Y,et al.Application of iron sulfide particles for groundwater and soil remediation:A review[J].Water Research,2016,89:309-320.
[28]CHARLET L,KANG M L,BARDELLI F,et al.Nanocomposite Pyrite-Greigite Reactivity toward Se(IV)/Se(VI)[J].Environmental Science&Technology,2012,46(9):4869-4876.
[29]KANTAR C,ARI C,KESKIN S,et al.Cr(VI)removal from aqueous systems using pyrite as the reducing agent:Batch,spectroscopic and column experiments[J].Journal of Contaminant Hydrology,2015,174:28-38.
[30]DIAO Z H,SHI T H,WANG S Z,et al.Silane-based coatings on the pyrite for remediation of acid mine drainage[J].Water Research,2013,47(13):4391-4402.
[31]张杰,吴爱祥.排土场黄铁矿促进黄铜矿浸出研究[J].金属矿山,2008(3):39-41.
[32]LUO F,YANG D,CHEN Z L,et al.One-step green synthesis of bimetallic Fe/Pd nanoparticles used to degrade Orange II[J].Journal of Hazardous Materials,2016,303:145-153.
[33]CHAKRABORTY S,FAVRE F,BANERJEE D,et al.U(VI)sorption and reduction by Fe(II)sorbed on montmorillonite[J].Environmental Science&Technology,2010,44(10):3779-3785.
[34]LYU Y,LI J F,LIA Y M,et al.The roles of pyrite for enhancing reductive removal of nitrobenzene by zerovalent iron[J].Applied Catalysis B:Environmental,2019,242:9-18.
[35]LYU Y,LI Z,LI J F,et al.Synergetic effect of pyrite on Cr(VI)removal by zero valent iron in column experiments:An investigation of mechanisms[J].Chemical Engineering Journal,2018,349:522-529.
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