Permanganate/sulfite(Mn(VII)/S(IV))process is a promising pre-oxidation technology for sequestering the emerging organic contaminants in drinking water treatment plant.Iopamidol(IPM),a representative of iodinated X-ra...Permanganate/sulfite(Mn(VII)/S(IV))process is a promising pre-oxidation technology for sequestering the emerging organic contaminants in drinking water treatment plant.Iopamidol(IPM),a representative of iodinated X-ray contrast media,has been widely detected in water sources and has the risk of forming iodinated disinfection byproducts(I-DBPs)in water treatment system.In this study,we investigated the evolution of iodine species during the IPM degradation by the Mn(VII)/S(IV)process and its effect on the subsequent formation of I-DBPs during chlorination at pH 7.0 and 8.0.IPM could be effectively degraded in the Mn(VII)/S(IV)process at environmentally relevant pH(pH 7.0 and 8.0).The results of quenching and competitive oxidation kinetic experiments revealed that SO^(·-)_(4)was the major reactive oxidizing species contributing to the degradation of IPM whereas the contributions of HO·and reactive manganese species were negligible in the Mn(VII)/S(IV)process.I–and IO–3were generated while no HOI was detected during the degradation of IPM in the Mn(VII)/S(IV)process.The effects of IPM oxidation by Mn(VII)/S(IV)on the subsequent formation of chlorinated disinfection by-products(Cl-DBPs)during chlorination were related to the category of Cl-DBPs.The pre-oxidation of IPM by Mn(VII)/S(IV)resulted in the generation of I-DBPs during the disinfection process although no I-DBPs were detected if no pre-oxidation was applied.The finding of this study suggested that attention should be paid to the toxicity of DBPs when water containing iodinated organic contaminants is treated by Mn(VII)/S(IV)process or other pre-oxidation technologies.展开更多
Chloramines,in practice,are formed onsite by adding ammonia to chlorinated drinking water to achieve the required disinfection.While regulated disinfection byproducts(DBPs)are reduced during chloramine disinfection,ot...Chloramines,in practice,are formed onsite by adding ammonia to chlorinated drinking water to achieve the required disinfection.While regulated disinfection byproducts(DBPs)are reduced during chloramine disinfection,other DBPs such as iodinated(iodo-)DBPs,that elicit greater toxicity are formed.The objective of this study was to investigate the impact of prechlorination time on the formation of both halogen-specific total organic halogen(TOX)and iodo/chlorinated(chloro-)DBPs during prechlorination/chloramination in source waters(SWs)containing iopamidol,an X-ray contrast medium.Barberton SW(BSW)and Cleveland SW(CSW)containing iopamidol were prechlorinated for 5–60 min and afterwards chloraminated for 72 hr with ammonium chloride.Chlorine contact time(CCT)did not significantly impact total organic iodine(TOI)concentrations after prechlorination or chloramination.Concentrations of total organic chlorine(TOCl)formed during prechlorination did not significantly change regardless of pH and prechlorination time,whileTOClappearedtodecreaseafter 72 hrchloraminationperiod.Dichloroiodomethane(CHCl_2I)formation during prechlorination did not exhibit any significant trends as a function of p H or CCT,but after chloramination,significant increases were observed at pHs 6.5 and 7.5 with respect to CCT.Iodo-HAAs were not formed during prechlorination but were detected after chloramination.Significant quantities of chloroform(CHCl_3)and trichloroacetic acid(TCAA)were formed during prechlorination but formation ceased upon ammonia addition.Therefore,prechlorination studies should measure TOX and DBP concentrations prior to ammonia addition to obtain data regarding the initial conditions.展开更多
This study investigated the speciation of halogen-specific total organic halogen and disinfection byproducts(DBPs) upon chlorination of natural organic matter(NOM) in the presence of iopamidol and bromide(Br^-).Experi...This study investigated the speciation of halogen-specific total organic halogen and disinfection byproducts(DBPs) upon chlorination of natural organic matter(NOM) in the presence of iopamidol and bromide(Br^-).Experiments were conducted with low bromide source waters with different NOM characteristics from Northeast Ohio,USA and varied spiked levels of bromide(2-30 μmol/L) and iopamidol(1-5 μmol/L).Iopamidol was found to be a direct precursor to trihalomethane(THM) and haloacetic acid formation,and in the presence of Br^-favored brominated analogs.The concentration and speciation of DBPs formed were impacted by iopamidol and bromide concentrations,as well as the presence of NOM.As iopamidol increased the concentration of iodinated DBPs(iodo-DBPs) and THMs increased.However,as Br^-concentrations increased,the concentrations of nonbrominated iodo-and chloro-DBPs decreased while brominated-DBPs increased.Regardless of the concentration of either iopamidol or bromide,bromochloroiodomethane(CHBrClI) was the most predominant iodo-DBP formed except at the lowest bromide concentration studied.At relevant concentrations of iopamidol(1 μmol/L) and bromide(2 μmol/L),significant quantities of highly toxic iodinated and brominated DBPs were formed.However,the rapid oxidation and incorporation of bromide appear to inhibit iodoDBP formation under conditions relevant to drinking water treatment.展开更多
基金supported by the National Natural Science Foundation of China (Nos.22206050,22025601,21976133 and 52270047)the National Key Research and Development Program of China (No.2019YFC1805202)the State Key Laboratory of Pollution Control and Resource Reuse Foundation (No.PCRRK20014)。
文摘Permanganate/sulfite(Mn(VII)/S(IV))process is a promising pre-oxidation technology for sequestering the emerging organic contaminants in drinking water treatment plant.Iopamidol(IPM),a representative of iodinated X-ray contrast media,has been widely detected in water sources and has the risk of forming iodinated disinfection byproducts(I-DBPs)in water treatment system.In this study,we investigated the evolution of iodine species during the IPM degradation by the Mn(VII)/S(IV)process and its effect on the subsequent formation of I-DBPs during chlorination at pH 7.0 and 8.0.IPM could be effectively degraded in the Mn(VII)/S(IV)process at environmentally relevant pH(pH 7.0 and 8.0).The results of quenching and competitive oxidation kinetic experiments revealed that SO^(·-)_(4)was the major reactive oxidizing species contributing to the degradation of IPM whereas the contributions of HO·and reactive manganese species were negligible in the Mn(VII)/S(IV)process.I–and IO–3were generated while no HOI was detected during the degradation of IPM in the Mn(VII)/S(IV)process.The effects of IPM oxidation by Mn(VII)/S(IV)on the subsequent formation of chlorinated disinfection by-products(Cl-DBPs)during chlorination were related to the category of Cl-DBPs.The pre-oxidation of IPM by Mn(VII)/S(IV)resulted in the generation of I-DBPs during the disinfection process although no I-DBPs were detected if no pre-oxidation was applied.The finding of this study suggested that attention should be paid to the toxicity of DBPs when water containing iodinated organic contaminants is treated by Mn(VII)/S(IV)process or other pre-oxidation technologies.
基金supported by the National Science Founda-tion (NSF, project numbers NSF1124865 and NSF1124844)the German Research Foundation (Deutsche Forschungsgemeinschaft, DFG, project number TE 533/4-1)
文摘Chloramines,in practice,are formed onsite by adding ammonia to chlorinated drinking water to achieve the required disinfection.While regulated disinfection byproducts(DBPs)are reduced during chloramine disinfection,other DBPs such as iodinated(iodo-)DBPs,that elicit greater toxicity are formed.The objective of this study was to investigate the impact of prechlorination time on the formation of both halogen-specific total organic halogen(TOX)and iodo/chlorinated(chloro-)DBPs during prechlorination/chloramination in source waters(SWs)containing iopamidol,an X-ray contrast medium.Barberton SW(BSW)and Cleveland SW(CSW)containing iopamidol were prechlorinated for 5–60 min and afterwards chloraminated for 72 hr with ammonium chloride.Chlorine contact time(CCT)did not significantly impact total organic iodine(TOI)concentrations after prechlorination or chloramination.Concentrations of total organic chlorine(TOCl)formed during prechlorination did not significantly change regardless of pH and prechlorination time,whileTOClappearedtodecreaseafter 72 hrchloraminationperiod.Dichloroiodomethane(CHCl_2I)formation during prechlorination did not exhibit any significant trends as a function of p H or CCT,but after chloramination,significant increases were observed at pHs 6.5 and 7.5 with respect to CCT.Iodo-HAAs were not formed during prechlorination but were detected after chloramination.Significant quantities of chloroform(CHCl_3)and trichloroacetic acid(TCAA)were formed during prechlorination but formation ceased upon ammonia addition.Therefore,prechlorination studies should measure TOX and DBP concentrations prior to ammonia addition to obtain data regarding the initial conditions.
基金supported by the German Research Foundation (Deutsche Forschungsgemeinschaft,DFG,project number TE 533/4-1)the National Science Foundation (NSF,project numbers NSF1124865 and NSF1124844).
文摘This study investigated the speciation of halogen-specific total organic halogen and disinfection byproducts(DBPs) upon chlorination of natural organic matter(NOM) in the presence of iopamidol and bromide(Br^-).Experiments were conducted with low bromide source waters with different NOM characteristics from Northeast Ohio,USA and varied spiked levels of bromide(2-30 μmol/L) and iopamidol(1-5 μmol/L).Iopamidol was found to be a direct precursor to trihalomethane(THM) and haloacetic acid formation,and in the presence of Br^-favored brominated analogs.The concentration and speciation of DBPs formed were impacted by iopamidol and bromide concentrations,as well as the presence of NOM.As iopamidol increased the concentration of iodinated DBPs(iodo-DBPs) and THMs increased.However,as Br^-concentrations increased,the concentrations of nonbrominated iodo-and chloro-DBPs decreased while brominated-DBPs increased.Regardless of the concentration of either iopamidol or bromide,bromochloroiodomethane(CHBrClI) was the most predominant iodo-DBP formed except at the lowest bromide concentration studied.At relevant concentrations of iopamidol(1 μmol/L) and bromide(2 μmol/L),significant quantities of highly toxic iodinated and brominated DBPs were formed.However,the rapid oxidation and incorporation of bromide appear to inhibit iodoDBP formation under conditions relevant to drinking water treatment.
